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0 0 1 552.72 76.32 Tm <7765616B6572> Tj ET endstream endobj 4 0 obj 7330 endobj 5 0 obj << /Type /Font /Subtype /Type1 /BaseFont /Helvetica /Encoding /WinAnsiEncoding >> endobj 6 0 obj << /Length 7 0 R >> stream L6 CHAPTER II EXPERIT'TENTAL TECTINIQUE AND APPARATUS Eigh Resolutlon Infrared EpectroscopyThroughout the course of this Ph'D' work theinfrared absorption spectra of a wide range of van derWaaIs complexes have been studied' Results from ATDCI1'NeDCll , ( Dcl ) ,''' , Hcl-DcI1 , DcI-HcI1, and (HcI ) 22'5 arepresented in this thesis' AlI studies reported hereinprobe either the HCI or DCl vibration within the complex'As the HCI and DCI vibrational frequencies aresubstantially different (2885.97 cm'1 and 2091'06 c'o-1,respectively), different infrared spectrometers are usedto probe the two chromophores' The HCl vibrations (3'46pm) are investigated with a difference frequency Iaserspectrometer (tunabre from 2.2 4.2 Fm), and the DCrvibrations(4.78pm)withaPb-saltdiodelaser(tunablefrom 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362.16 87.84 Tm <74686520> Tj 1 0 0 1 391.68 87.36 Tm <726573756C74696E67> Tj ET endstream endobj 15 0 obj 7792 endobj 16 0 obj << /Length 17 0 R >> stream L7than the high frequency intramolecular fundarnentalvibrations. This is because these vibrations are onryinfrared active by virtue of a nonzero anharaonicity, dsdiscussed in chapter r. As wilr be seen in numerousexanpres in this text, however, these spectrorneterspossess the requisite sensitivity for such observations.we shalr spend some tirne discussing both of thesespectroneters. The first section dears with the pb-sal,tdiode spectrometer, which was constructed as part of thisdissertation. This is forlowed by a shorter discussionof the difference freguency spectrometer, d, apparatuswhich has been discussed previously in detai16-8. A shortdiscussion folrows regarding the operating principres ofthe slit pulsed valve and gas handling serup. Thechapter concludes with a discussion of the technigue usedto obtain infrared line shapes. fnfrared Spectroneters Diode Laser Spectrometer operating PrinciplesA Pb-salt diode laser issources of tunable radiationThis section will discuss, inprinciples of a pb-salt diode one of the rnost generalin near to rnid-IR regions.some detail, the operatinglasere, and the resulting endstream endobj 17 0 obj 1125 endobj 18 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 19 0 obj << /Length 45 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj13 Do Q endstream endobj 20 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj13 13 0 R >> /Subtype 16 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 18 0 R 19 0 R 14 0 R ] >> endobj 21 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 38748 >> stream ɱh &ku@"j@pYDH4Dp EhrΜg%Dp D@fl4U$h ZEy ˁl5DlP  %a7PPĔPB@l@ HalX[ `wf`(-P;kˆadpk#HP2s"r0 ,4 B#p&q'BD8$i3K L f@apB88Ghf :#p6`.@L05a`jD440' *$! ‰ / $ . 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nid-rR spectroneter (shonn in Figure 2.L) vhichwe devel0ped within our laboratory. This spectrometer isbased around a r,aser photonics sp5goo-2 r.aser sourceassernbly' Briefly, these rasers are composed of a p-njunction which is forward biased. The injected erectronscombine with hores and radiate photons with energiesdeterrnined by the seniconductor band gap, about 21oo cm-'for the studies presented herein.The gain medium for a pb-salt diode laser is formedat a p-n junction in semiconductor naterials. The p_typelayer is characterized by an electron deficiency suchthat the prirnary charge carriers are electron holes. Then-type layer, on the other hand, contains excesselectrons which serve as the charge carriers. When theselayers are placed in contact, electrons and hores in thearea of the junction will combine. This will occur untila self induced electric field across the p-n junctionbalances the charge separation of the electrons andholes' At this point no further reconbination occurs(see Figure 2.2) .When an external bias is applied across thejunction, erectrons are reintroduced to the n-type layerand rernoved from the p-type layer causing eLectrons toonce again recombine with holes. This recourbinationresults in either a radiative (see Figure 2.3) ornonradiative release of energy. The radiative process is endstream endobj 25 0 obj 1340 endobj 26 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 27 0 obj << /Length 45 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj21 Do Q endstream endobj 28 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj21 21 0 R >> /Subtype 24 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 26 0 R 27 0 R 22 0 R ] >> endobj 29 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 32962 >> stream ̅6b72мuoA,"ug,\"qzDzc/Mw{?蒋fQ; h40޻_4C. ]CQzk Q Km9|Z";A~݆CBOAz^Ga, F>W $#mmYT Po$kWoxJ(TGO'ҿ lW$@AӻICJԉ:*BD[MBnTVmp<a= m.<[ך: aV/NKTzot&u{hr h4?Z߿JI4iP~+'KKא";a(i#xanb=&$;K{bTsv?a:N&<% iXh L&!~&4 %0B5N݅CL4*35C_mo*ڄC] "1hN頜)&MHx(jҵTu 黴L0_okjI kh8LBݤLhi^6!_ X0M2 H_nb_naB._WQ6EDJᐐ n%I 2'$lvUSDx-45AbC. cӠ[|@(wx[בCO.7\V>Ä P;쎩 Aڥ X:,bk":;o(p[[W#n-T#ACDuh<9 ATp]0 :0#!i à(a Aam u~A0h0nPà0{V0$\0AeaH0L: `#a#0dt`WI0]a 8 D}CpP0I0҆H0äa۠ú* 8MCw/aH0]Su00A$ 8tçAU a 8Jpo =Jî} ;Ն6: aa70tPX;~@a@WA$=.j#0m=0mb'Pa0X0 :9a8@`n . > Ha# =@ 6-BP8* :E0a{P3gaZh p ;^D6uu 0>]5bl0aBA5m"A =XPavml0a0 >aEl0 al0taapa _ 0a Ilaӯ 0uCu`< a~  6{0C0m6ZG[a0m{! 0[ے a6it0m]' 6\/a0alPm롯aza_^,}mçl6UH/m&0Aa첚M5u]40 aפBcAaK&[)}xvbH D6 mZoU@a$?a];k@o=&N |k}ViEE8U V jaP?m;m6? 07? t/󯷷{}paUP 4?w[a{4 myaMa҆WaCzl-v }M4aޘi Ӡe:M1  AC6 =z+!&m*aaå^mnm+aK 7]Pửk_vw^ݥ_ m׳^l>#"O Jtégs]dr3ۥw !MiIۄ^I7 3m*|067ȶ ? y|77tChr}[,5f`[w2/>g3v~ْ_~Cߦ )aA~w `۳@DH|7*~AGӸOm 6w2p1'htHسMӴҤmMeV޿;d   Dp|zmz 0뒁 (mB&M4&Kmv=Apն5]^ZIvҭi!!/P/W~RKazA-f^M$I~X ;i' * B 6qpۤ:NJ2;H[~!A JJ i|𝤯|/oӂ gkI*i-wF;Mu_ {OῚvGή/[TnBI|_]Z JT~Z_I^_f*V6ÖkKkjj߷iOukIzUl%uo]^>nVdQȸ 4aWKAv8a&!`I~Z{{}Ni'4!_ +_^.+ȖBRm.[ҾPa*`TՐ L2-r7pwVNI;@ !DuL ~0T6+!r$rN}QV`F$ˀaT;VS xB[0i'2iW~MA#k^76jFt4C[/5]5Z]z-%tXaK}1zOou|7*0uޯ ?VæptKmo0wwK^Xau/aF@ݿuuaUXmWJ5L [Tpj 6߆"KwZ jlL7iRAa0>T ARiU.wCW ;zUIPnE6U]*ZX`{oTaU ;RT$pݿ֫ wjL;თI$npþWIUmZav%X0.i*XaT0{--kIUC{ҨT>R꫆Kd/1蓥!I,1]/I.[iUIT=dgcU%w Ik@jo:IVn$P@UJo}j$;TU5EuU-Ѿ %I~&^$KݠKuzI%{qi~.I߮ڤ=i-]]I*KWT|_?v꿼{_rU7pV*!l? }Z]*TIiEV-oo iuI/ \hPV)~,5D|$B:I/?H) ˨;q䁭$x)k^ @J=!K<4I%K KVֽtK6J}4Iz֪`I$Z _,+z}aXI[pKOæ*ւ@,zmRT9%JIoA2iuZI^[z/>*T߽ItuIzүMR^V }DTJҪVkګuI$zI}*a*}y mU%IoK]W/kI$Oio;!KLfA0MoI$lnAZUTN" =*KY(s{$TW-R?mViiorTK[ޒ\KL%*iw}uCJ$I&ҥ+BIVK T~{ XXVt$o֒ZKA%.vX֋o)#RZ[H A8o*K." 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Themonochromator pictured is not reguired forthese studies due to the near singlelongitudinal mode characteristics of thediode used. Each beam splitter (B.S.)pictured is a pelIicIe splitter whichreflects approximately 10* of the bean andtransrnits the renainder. The nultipass usedfor these studies involves six passesthrough the slit expansion and not three asis scheroatically shown in this figure. 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Fo*'ard Biased Diode Laser EnergY Levels Level Band GaP = Pg IIArea /Ort^i Level Electron and Hole DensitY -._-Tffi+II-.^hv=EaYAn approximate picture of the energly levelsof a diode laser. As the diode is forrrardbiased, electrons are injected into then-tlpe naterial which can reconbine in theregion of the interface with holes in thep-type naterial. The recourbination releasesenergy either radiatively or nonradiatively.The radiative recombination results inphotons of energy given by the band gap. 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The photonenergy is determined by the band gap or energy differencebetween the conduction and varence revels. This band gapis very dependent on the choice of semiconductormateri-alr ?s welr as diode tenperature and bias current.rnfrared tunabre diode rasers are typicarry composed of Pb-sa1ts, such as pbr-rSnrTe and pbSr-rEurSerTer-r. By varying x and y in these semiconductor rnateriars, theband gaps can be adjusted from about 4 to 30 pm. otherPb-sal-ts are also avairabre which extend this tuningrange srightly in each direction. The diode used for al_Ithe Dcl studies discussed herein was purchased from r,aserPhotonics (rnodel number sp5615), and has a composition ofPbo.ca,rEro.ooesS"o.eeosTeo.ooss. The dirnensions of the activeregion of this diode are 1 pm X 22 pm X 25O pm. Theoutput frequency is centered around 2ogo c['1, with atuning rate of 1150 WIz/r,A.Lasing is not possible without feedback, which isprovided by forming a cavity around the semiconductormaterial by cleaving the facets. At applied currentsless than a threshold value, the photons are emittedincoherently. As the forward bias current is increased,a threshord condition is reached in which the round tripcavity gain exactly eguals the losses: l,n.=oint+ct (2 .L) endstream endobj 57 0 obj 1290 endobj 58 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 59 0 obj << /Length 45 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj53 Do Q endstream endobj 60 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj53 53 0 R >> /Subtype 56 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 58 0 R 59 0 R 54 0 R ] >> endobj 61 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 32064 >> stream @u.":#6L 8l@. 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364.08 526.80 Tm <53747269706520> Tj 1 0 0 1 414.72 527.52 Tm <67656F6D6574727920> Tj 1 0 0 1 482.64 527.04 Tm <28736565> Tj 1.68 Tc 1 0 0 1 112.80 503.28 Tm <692D3B2E3A3A6520> Tj 1 0 0 1 162.48 503.52 Tm <322E34292E20> Tj 1 0 0 1 212.40 503.28 Tm <5468697320> Tj 1 0 0 1 248.64 503.28 Tm <64657369676E20> Tj 1 0 0 1 298.80 503.52 Tm <706C6163657320> Tj 1 0 0 1 349.68 502.80 Tm <616E20> Tj 1 0 0 1 371.52 502.80 Tm <61637469766520> Tj 1 0 0 1 422.40 502.56 Tm <726567696F6E20> Tj 1 0 0 1 472.80 502.56 Tm <6265747765656E> Tj 1.44 Tc 1 0 0 1 112.32 479.04 Tm <3A623A20> Tj 1 0 0 1 140.64 479.28 Tm <636C616464696E6720> Tj 1 0 0 1 205.68 479.28 Tm <6C61796572732C20> Tj 1 0 0 1 263.04 479.04 Tm <6561636820> Tj 1 0 0 1 299.28 478.80 Tm <6F6620> Tj 1 0 0 1 320.16 478.80 Tm <776869636820> Tj 1 0 0 1 363.84 478.56 Tm <6861766520> Tj 1 0 0 1 400.56 478.56 Tm <6120> Tj 1 0 0 1 414.72 478.56 Tm <68696768657220> Tj 1 0 0 1 466.56 478.32 Tm <696E64657820> Tj 1 0 0 1 509.52 478.08 Tm <6F66> Tj 1.44 Tc 1 0 0 1 112.56 455.04 Tm <3A653A3A616374696F6E20> Tj 1 0 0 1 190.80 455.52 Tm <616E6420> Tj 1 0 0 1 220.08 455.28 Tm <6C617267657220> Tj 1 0 0 1 270.00 455.28 Tm <62616E6420> Tj 1 0 0 1 306.00 455.52 Tm <67617020> Tj 1 0 0 1 335.04 454.80 Tm <7468616E20> Tj 1 0 0 1 371.28 455.04 Tm <74686520> Tj 1 0 0 1 400.32 454.80 Tm <61637469766520> Tj 1 0 0 1 451.44 454.56 Tm <726567696F6E2E> Tj 1.44 Tc 1 0 0 1 111.60 431.28 Tm <3A2D3165736520> Tj 1 0 0 1 154.08 431.76 Tm <74656E6420> Tj 1 0 0 1 190.08 431.76 Tm <746F20> Tj 1 0 0 1 212.40 431.52 Tm <6C6F63616C697A6520> Tj 1 0 0 1 276.96 431.52 Tm <74686520> Tj 1 0 0 1 305.52 431.76 Tm <70686F746F6E7320> Tj 1 0 0 1 363.84 431.28 Tm <616E6420> Tj 1 0 0 1 392.64 431.04 Tm <656C656374726F6E732C> Tj 1.44 Tc 1 0 0 1 111.60 407.52 Tm <3A6573706563746976656C792C20> Tj 1 0 0 1 212.64 407.76 Tm <696E20> Tj 1 0 0 1 233.76 407.76 Tm <6120> Tj 1 0 0 1 248.40 407.76 Tm <736D616C6C657220> Tj 1 0 0 1 305.76 407.76 Tm <61637469766520> Tj 1 0 0 1 356.40 407.52 Tm <726567696F6E2C20> Tj 1 0 0 1 414.24 407.28 Tm <7468757320> Tj 1 0 0 1 450.96 407.04 Tm <7265647563696E67> Tj 1.92 Tc 1 0 0 1 111.60 383.76 Tm <613A736F727074696F6E2E> Tj 1.44 Tc 1 0 0 1 145.92 360.00 Tm <54686520> Tj 1 0 0 1 174.96 360.00 Tm <7472616E736D697373696F6E20> Tj 1 0 0 1 269.76 359.76 Tm <6C6F737320> Tj 1 0 0 1 307.44 360.24 Tm <286F7229> Tj 1.44 Tc 1 0 0 1 110.64 335.76 Tm <3A2E3A6520> Tj 1 0 0 1 138.72 335.76 Tm <746F20> Tj 1 0 0 1 161.28 335.76 Tm <66696E69746520> Tj 1 0 0 1 211.44 335.76 Tm <6F757470757420> Tj 1 0 0 1 262.08 335.76 Tm <636F75706C696E672C> Tj 1.44 Tc 1 0 0 1 109.92 313.44 Tm <706F746820> Tj 1 0 0 1 145.68 311.76 Tm <74686520> Tj 1 0 0 1 174.96 311.76 Tm <63617669747920> Tj 1 0 0 1 226.08 311.52 Tm <6C656E67746820> Tj 1 0 0 1 278.40 312.24 Tm <287B2920> Tj 1 0 0 1 305.28 311.52 Tm <616E64> Tj 1.92 Tc 1 0 0 1 110.64 287.52 Tm <666163657420> Tj 1 0 0 1 153.12 287.76 Tm <656E647320> Tj 1 0 0 1 191.52 288.00 Tm <28527220> Tj 1 0 0 1 215.28 289.68 Tm <3D20> Tj 1 0 0 1 229.68 287.76 Tm <527A292E> Tj 1.20 Tc 1 0 0 1 338.64 359.76 Tm <617420> Tj 1 0 0 1 360.00 359.76 Tm <74686520> Tj 1 0 0 1 389.28 359.52 Tm <636C656176656420> Tj 1 0 0 1 447.36 359.52 Tm <656E647320> Tj 1 0 0 1 484.56 359.28 Tm <6973> Tj 1.44 Tc 1 0 0 1 333.60 335.76 Tm <776869636820> Tj 1 0 0 1 378.24 335.28 Tm <697320> Tj 1 0 0 1 399.36 335.28 Tm <6120> Tj 1 0 0 1 414.48 335.28 Tm <66756E6374696F6E20> Tj 1 0 0 1 479.28 335.04 Tm <6F66> Tj 1.20 Tc 1 0 0 1 333.84 311.52 Tm <74686520> Tj 1 0 0 1 363.12 311.28 Tm <7265666C656374616E636520> Tj 1 0 0 1 450.24 311.04 Tm <6F6620> Tj 1 0 0 1 471.84 311.04 Tm <746865> Tj 3.60 Tc 1 0 0 1 402.00 222.24 Tm <512E3229> Tj 1.20 Tc 1 0 0 1 348.72 155.28 Tm <697320> Tj 1 0 0 1 369.84 155.28 Tm <617070726F7869726E6174656C7920> Tj 1 0 0 1 472.56 154.56 Tm <32354F20> Tj 1 0 0 1 500.64 155.52 Tm <706E> Tj 1.68 Tc 1 0 0 1 342.00 131.28 Tm <342D362E20> Tj 1 0 0 1 384.00 131.04 Tm <546875732C20> Tj 1 0 0 1 427.68 130.80 Tm <746865> Tj 2.40 Tc 1 0 0 1 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181.68 131.52 Tm <6120> Tj 1 0 0 1 196.32 131.52 Tm <7265667261637469766520> Tj 1 0 0 1 276.48 131.28 Tm <696E64657820> Tj 1 0 0 1 319.20 131.28 Tm <6F66> Tj 1.20 Tc 1 0 0 1 109.68 107.28 Tm <7265666C656374616E636520> Tj 1 0 0 1 196.08 107.52 Tm <617420> Tj 1 0 0 1 217.68 107.28 Tm <74686520> Tj 1 0 0 1 246.72 107.28 Tm <636C656176656420> Tj 1 0 0 1 304.56 107.28 Tm <656E6473> Tj 1.44 Tc 1 0 0 1 109.68 83.28 Tm <4C6F737320> Tj 1 0 0 1 145.20 83.52 Tm <6F6620> Tj 1 0 0 1 167.04 83.52 Tm <61626F757420> Tj 1 0 0 1 211.20 83.28 Tm <313420> Tj 1 0 0 1 232.08 84.00 Tm <70657220> Tj 1 0 0 1 261.12 83.28 Tm <636D2E> Tj ET endstream endobj 63 0 obj 8653 endobj 64 0 obj << /Length 65 0 R >> stream 23=:e, fth. is the gain at threshold, oint represents the---,-,e:nal losses and o, the transmission losses at thei::e--s. The internal losses include those due to.-s:rption of light in both the active and cladding:e;:cn and scattering at each heterogeneous interface.l-----e=pts are made to niniroize these internal losses. One:: --:ie approaches utilized by Laser Photonics is:r:::cation of the diode in a Mesa Stripe geometry (seei-;.::e 2.4). This design places an active region between:b: cladding layers, each of which have a higher index of:e::action and larger band gap than the active region.:-1ese tend to localize the photons and electrons,:espectively, in a smaller active region, thus reducinga:sorption. The transmission loss (or):.:e to finite output coupling,poth the cavity length ({) andfacet ends (Rr = Rz). at the cleaved ends iswhich is a function ofthe reflectance of the Q.2) is approxirnately 25O pn4-6. Thus, theis about 0.71, i.e. a or= + (t\lnl - |--'l nt n, / The diode used for these studieslong with a refractive index ofreflectance at the cleaved endsLoss of about 14 per cm. endstream endobj 65 0 obj 1107 endobj 66 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 67 0 obj << /Length 45 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj61 Do Q endstream endobj 68 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj61 61 0 R >> /Subtype 64 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 66 0 R 67 0 R 62 0 R ] >> endobj 69 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 29632 >> stream D"T#4ĕpb@pbE@,Dp2 4\ ċKH( -= ZA:BDe$PZ@e-b*-} SĉH4` HUwF E[F`ul)0@jJg@9aL) i,+,4  р& DGDp&$S#,6Ċ#(D|)!<\ "Ep6ؑ H1p5 b#+@\`f I-C$ .Z! 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<6865616420> Tj 1 0 0 1 451.92 302.64 Tm <617373656D626C792C> Tj 1.44 Tc 1 0 0 1 118.80 282.24 Tm <73686F776E20> Tj 1 0 0 1 162.72 281.52 Tm <696E20> Tj 1 0 0 1 184.08 281.52 Tm <46696775726520> Tj 1 0 0 1 234.96 280.80 Tm <322E362C20> Tj 1 0 0 1 271.44 280.56 Tm <697320> Tj 1 0 0 1 292.32 280.32 Tm <63617061626C6520> Tj 1 0 0 1 350.16 279.60 Tm <6F6620> Tj 1 0 0 1 372.00 279.36 Tm <636F6F6C696E6720> Tj 1 0 0 1 430.56 278.64 Tm <666F757220> Tj 1 0 0 1 466.56 278.16 Tm <6C61736572> Tj 1.20 Tc 1 0 0 1 118.32 258.00 Tm <64696F64657320> Tj 1 0 0 1 168.96 257.52 Tm <746F20> Tj 1 0 0 1 191.04 257.28 Tm <617070726F78696E726174656C7920> Tj 1 0 0 1 292.80 256.08 Tm <6C5F3520> Tj 1 0 0 1 313.68 255.84 Tm <4B2E> Tj 1.20 Tc 1 0 0 1 154.08 233.52 Tm <54686520> Tj 1 0 0 1 183.36 233.28 Tm <6F757470757420> Tj 1 0 0 1 234.72 232.56 Tm <6672656775656E637920> Tj 1 0 0 1 306.24 232.08 Tm <6F6620> Tj 1 0 0 1 327.84 231.60 Tm <74686520> Tj 1 0 0 1 356.64 231.36 Tm <64696F646520> Tj 1 0 0 1 400.56 230.64 Tm <6C6173657220> Tj 1 0 0 1 444.48 230.16 Tm <697320> Tj 1 0 0 1 465.60 229.92 Tm <74756E656420> Tj 1 0 0 1 508.80 229.44 Tm <6279> Tj 1.20 Tc 1 0 0 1 117.84 209.76 Tm <61646A757374696E6720> Tj 1 0 0 1 190.08 209.04 Tm <74686520> Tj 1 0 0 1 219.12 208.80 Tm <64696F646520> Tj 1 0 0 1 262.56 208.32 Tm <74656D706572617475726520> Tj 1 0 0 1 349.20 207.36 Tm <616E6420> Tj 1 0 0 1 378.24 206.88 Tm <63757272656E742E20> Tj 1 0 0 1 450.72 205.92 Tm <54686520> Tj 1 0 0 1 480.00 208.32 Tm <70622D73614974> Tj 1.20 Tc 1 0 0 1 117.12 186.00 Tm <64696F646520> Tj 1 0 0 1 160.56 185.76 Tm <62616E6420> Tj 1 0 0 1 196.80 186.00 Tm <67617020> Tj 1 0 0 1 226.08 185.04 Tm <6368616E67657320> Tj 1 0 0 1 283.44 184.56 Tm <7769746820> Tj 1 0 0 1 319.92 183.84 Tm <74656D70657261747572652C20> Tj 1 0 0 1 414.24 182.64 Tm <617320> Tj 1 0 0 1 435.60 182.40 Tm <6D75636820> Tj 1 0 0 1 472.32 181.92 Tm <617320> Tj 1 0 0 1 496.32 181.68 Tm <326F6F> Tj 1.20 Tc 1 0 0 1 117.12 162.24 Tm <636D2D3120> Tj 1 0 0 1 148.08 161.76 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endstream endobj 79 0 obj 9354 endobj 80 0 obj << /Length 81 0 R >> stream 25Both of these loss channels i.ncrease withtemperature, thus the gain (and therefore the threshordcurrent) needed to overcorne these Losses increases withincreasing ternperature. This effect is demonstrated inFigrure 2.5, which shows the threshord current versustemperature for the diode used in these studies. Atternperatures above about Loo K, the loss channers are sogreat that lasing is irnpossible for this diode.Consequently, one needs to operate at very lowtenperatures, which are achieved with a commercial closedcycle He refrigerator. This cooling system operates onthe principle of adiabatic cooring which accompaniesexpansion of a gas through a smalr orifice. The gas iscompressed and forced through the orifice by pistonswhich run at 3 Hz. As wirr be discussed below, it isthis mechanicar vibration which is primarily responsiblefor the laser freguency noise. The cord head assembly,shown in Figure 2.6, is capable of cooling four laserdiodes to approxinrately l_5 K.The output freguency of the diode laser is tuned byadjusting the diode temperature and current. The pb-saItdiode band gap changes with temperature, as much as 2oocm-1 for r-oo K ternperature change. Additionarly, thefreguency of the rasing mode acquires temperaturedependence via a temperature dependent index ofrefraction. endstream endobj 81 0 obj 1304 endobj 82 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 83 0 obj << /Length 45 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj77 Do Q endstream endobj 84 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj77 77 0 R >> /Subtype 80 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 82 0 R 83 0 R 78 0 R ] >> endobj 85 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 22880 >> stream d "8N3쏜 DD%l(+e! Dv^aPA 1q!#x2=.DxvG,㌆@jX"?<@jlتduqZ/d2Y.C @5ж%"d>G@#|d2Lx˯2PGt6^׽AR 9b$ tGX< UuqXkD2V#6ͬXEӻ!led~AP? 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The four horizontalholes in the front are the locations of thefour diodes which can be mounted at onetine . The srnaIl cyl indrical tube whichprotmdes vertically up from the cold headis a I'Iodion ion pump. This punp extends thetine necessary between vanning tne aioaes toroorn ternperature. This is a desirableaddition to the laser since repeated cyclingto roon tenperature degrades the diodecharacteristics . 27 gE{ TEFFr' Id: \I Figure 2.6 endstream endobj 97 0 obj 526 endobj 98 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 99 0 obj << /Length 45 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj93 Do Q endstream endobj 100 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj93 93 0 R >> /Subtype 96 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 98 0 R 99 0 R 94 0 R ] >> endobj 101 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 34450 >> stream hfHAJ(ATh":`GGYuG[2$2']bƈdnmR# c~g!O!$GXA*=28A2`b /ccGϮ ,16C #KdPCC 6d. ~(ǐ t_0d251C 2%ж.pDs C ~ Ih$Gx.Paj y K5r: GXpV!Q s @h 1Dx4 ":a [P ՈVC G>,Ʌ1Dž7ʅa2:K‚h4#45}c ir8g tDt]t,FVC 4W'C PxĎSHl|@iàh.#N[ XF,h4ZCC # r;*! 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The diode ternperature is controlled bothby external heating of the diode and Joure heating due tothe current flowing through the diode. As can be seen inFigure 2.7 , the spectral modes scan with current in afairly well defined manner. Figure 2.9 shows a prot oflasing freguency of the diode used in these studies, ds afunction of both the diode temperature and current.Instead of a single continuous scan, typically scans ofno more than about r-z cm-l in length are possibre. Thisis because the underlying gain curve does not scan at thesame rate with temperature as does the band gap. AIsothe gain curve is broad enough (10-20 cm'l) to supportmore than one longitudinal cavity mode. The frequency ofthese spectral modes can be predicted from Eq. 2.3knowing the index of refraction and length of the cavity.The spacing between longitudinal rnodes is sirnply v, - vt,conpricated onry by the fact that the index of refractionof the diode is frequency dependent (dispersive). Thus,including this dependence, the spacing between adjacentmodes becomes. endstream endobj 105 0 obj 1183 endobj 106 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 107 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj101 Do Q endstream endobj 108 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj101 101 0 R >> /Subtype 104 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 106 0 R 107 0 R 102 0 R ] >> endobj 109 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 25600 >> stream )^>2c߰1GG"Ʊճ.u膱<~]XtaG<(aL '  n5|dJ vG_i- (u#P+~b.=kR?ƞRuIhvKVcO zxW#G-뎈=e ]x*ۮ.GA@.ucSJàs c__TG$uP@_ca]q#B"=#i,~(V:!Z1#tD˪.WFT M:/wDǂM GWƶjOI^ N9 o aK[iAQT8ǵ MA¨} %!`9t[DAQE1-L ; ?EA9v"ъAזH`-4zt.?iZhM)YNe:8h<+3B'<2a4\2z"!8ڦ H8Fv}y kmV+#NC; { õM>dz'wj2 p`_b2rS6[12.PikVu?lql0iȖvOu, }a5iR_kф  ڪw%o{8wv"; Y! 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nodes for oneof the diode lasers which we checked out(not the diode with which these studies werecarried out) . As for all of the dj.odelasers we investigated, the laser operateson more than one longitudinal mode.Addj-tionalIy, the laser frequency scans tohigher frequency with increasing current.It is also worth noting that any partj-cularcavity mode grows in intensity and thenshrinks. This is due to the differentialscanning rates of the cavity modes and theunderlying gain curve. Also note that atlow current (200 nA for this diode) thelaser only enits a single longitudinal mode.This is a general trend for nearly alldiodes investigated. 29 \1v\.-1 AfIIVlJl Figure 2.7 endstream endobj 113 0 obj 794 endobj 114 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 115 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj109 Do Q endstream endobj 116 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj109 109 0 R >> /Subtype 112 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 114 0 R 115 0 R 110 0 R ] >> endobj 117 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 28020 >> stream H LB#l#h6Dh,TT0Z %Sq"`S DGmLB8*$Am.6IXb#\`"KHd ``\5M! 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AII spectra reported in ifrl=thesis were takln betweeii- 2060 2r2o cm-1which is in the heart of the scanning regionfor this diode.. 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O cm-1 separation measured for thisdiode. However, the index of refraction does varysignificantly over the tenperature range of the diode,and thus the longitudinal mode spacing changes with diodetemperature. This mode structure is not always easilypredictable, as can be seen in Figure 2.9. The figurepresents two temperature regions of the same diode. AtT=105 K, only one longitudinal mode is present, but only20' lower (T=85 K) at least 13 different longitudinalrnodes are supporting gain.While one can typically elirninate aII but one of thelongitudinal modes with a nonochromator, a more favorablesolution is for the diode to lase in a single spectralmode. Newer diodes being produced with such techniquesas rnolecular beam epitaxial growth show prornise forsingle mode operation. 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0 0 1 283.92 72.72 Tm <616E20> Tj 1 0 0 1 305.76 72.96 Tm <6162736F725074696F6E20> Tj 1 0 0 1 385.20 73.92 Tm <61726F73652E> Tj 1.44 Tc /F3 23.0 Tf 1 0 0 1 256.56 547.20 Tm <5C6E66696C742D6F6F6F2A6F> Tj 0.72 Tc /F3 57.0 Tf 1 0 0 1 287.04 510.48 Tm <6C6C7527> Tj 1.92 Tc /F3 11.0 Tf 1 0 0 1 138.24 204.00 Tm <46696775726520> Tj 1 0 0 1 189.36 204.72 Tm <322E39> Tj ET endstream endobj 135 0 obj 4834 endobj 136 0 obj << /Length 137 0 R >> stream TemperatureT=85K Dependent Laser Operation l60mA = 105KltIItII-rII 180mA 800mA 200mA 220mA 14 ul timode Near Single ModeA demonstration of very reasonable andunusable node characteristics, both on thesame diode and only 20 K separated internperature. The higher temperaturechaiacteristics are very favorable sinceonly a single longitudinal mode is present.However, the rnultirnode region is unusablesince about 6 of Dore spectral modes havenearly equal intensities, resulting inobsenration of transitions from each with noa priori Eanner of deternining from whichmode an absorPtion arose. \nfilt-ooo*ollu' Figure 2.9 endstream endobj 137 0 obj 617 endobj 138 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 139 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj133 Do Q endstream endobj 140 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj133 133 0 R >> /Subtype 136 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 138 0 R 139 0 R 134 0 R ] >> endobj 141 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 37832 >> stream "ȳ ⷯ/fE:6GG5 C>Q"GECq":#!؅ Jݎ"e Qz!F!Ջ hjB# xYCK؂~<; xxTzW(r^:_.:P[p\(wew@Xq޼7 NClwW"D wKzXP APcDu(pTat:nPc#~#aTبx\": 7/=Z 3^TaC#(qЅړY,2 ~A}4beh;V=8WyA ]zxKVzZJ %PJQ(@ᾖ%oI¥i' .C HikTª: a5a3B5x[ D~DŽGT;Z#㭽Bp<+tVGV*0+wwJnAUHKvg`LNө0PR rY v}a=5 &-4ivT9<swid eXPD# L2:*/hE̎;W 6W+CAA#ԄMS U =< „ BtqET A!lH[(0DAf o Sҿۜ CCh3bl"A*u$aR\RLvL/ MaiqMb k`At d`a3Q"3 IS#awMa;`A)T#٤ Dgt%HdRsUe]Vh4Mi N 0@ $A"꟧M!Sl$Bc ȮðMvniCIA 0@ G4 i5v;o_AA #.GФYpdgwITELA܏,7m xnp~7'*`"[jT4I1}߰zz鴮jt=Vڱ봡=:<,:#'dUy~E'{m5!7o޿[ְx[u[, i&"a ̀GeWeb&܎Ӿ}@ʳh5Ӵp+w} þbeP ,n6g3).Xr a9'waa`p\!3‚!R)2u@ix[‹04  0h2 62TG2 vxe<[qwІ fd\ A4"!9p*LghwrnM1Ӡ- U q "!il!AGP@>e83d4|H{yK{bh6ӫ u ݄ !p `AL 7 .IMhl22(ݻo;qń,$ӥAB{#zm'I 4:dNlg KtnA7" nrE7/Vx AO=@SRzȸXa Fpp%TͰAzapO A AHtH9A!ݰȰA}h>GWC!Wm;OIꞩCAx9 ^'|#Z`_Iu $DЃ!_~_^C/޴_'[{h$p`G6tZ_ ZO AE/׺JBzz9ǩ1]l?_K$֓p$!B#D-u %]ӒO$;l~j  Yye,AKA.Mtl$MC c&-d,4*4ۭ#@H4!0LL'mm!bP;piwDDDDDI4Y.MOA 0im /aiD4{MжJ vhllGIEN2Aa 0[ڪ}a8  g V`#." dK'vBF#ӱN0؈`0B ΀L&L(B4IMDDDDDihᅤCȮ!V&`hܼ$!ل饏0 *-%Ƽ-2:4a\ke{7 EDuC·G^O۠WN¥,Z +It 4̖2 <">hTˍn/CIԳ5an|D35?̪&DPZ `*j΂CPO S&4!vp a s%k a6-8&4 N5uf4ddFhǑ& '4 „a L` `ȱ"fjeC}ntD 2(=4q Pq  0Da\B!ԏt8B[m@r?# 3{inM?Az e:SA= m^Bj ^B4*v0aSNA !# 26QXt=EdN  n F oINkۡɎ0(AMմmҦ Af Ih%9#&dLT2u azZ!m )\%DDDpe&h2S GPjd$C!6ۧDDDhDD2h aPd^Lu0B""*":MMm2n"""#ˮJ jcneɰ q.§R"DuFr?Qծۂ)nu],(-\2Si}AAmRv{A ttvNhv۷WNO8B 4 C]i4MuoA65ae {#>uBqڧa0@?}~ګߧ@'MnW]a5tiz3}'zt DT5 i3!-O"  F=~[ PKl|{nW@F{=`ȠY!/׽:MBx!\4# u_u[ ־}zuސkj mP_k N*-ֈA_^>rZzxi c ~u}lTKW"jD[L>} rЅtֽo_}?AIaZqj kuﮛgGޓV K@ci~W`al{H~VΚQ A?fO]nkߡئ)~/Oa^ H0OO%u^u36Y~<-C:jӄiS@"-5b}g]=wON·^fx^VM8m&MЩl2lN w TUj.V +kI]űlY@vǰ`9CVհ[Jӿ.M0M4&`^&>!PWvƇ\*|iC(=om^dA^8A2Z`c* wձIC4'gφ]w0#2ᐯ~4µji4J2ظqg  2>M+ M0Wa[Q s0Ϧ@.n:h0AAA#0M4R K ^"""""&ԉY$L!L,5kŨ~(2:0U""""#H'?MCCA*YC_.4 q? uUcUTtSY-DAqI%4ؙe%zTӰoEߝ?E} ^ﵾv@(̔HӴdZ [ )̫G<2$ *_bba0B 2  x@ N.jR <+b{aB 4 >,a adFQh!4dZoM":UPj}&A`AGB!P՘2CʄTͧ]74BW xM6T#M0`8M p~N!P@7DQ$z"cd$4Go`mMot-3fKR(*Tά!<x@97m!Xd mAR$;|!k0D0Xz9ˑESu_I:N]6 _(tY#2!*:a6nذkA I`+JIm' !9B  l<-HȷvQA4AńTC-?k*|RxBӻ B'8A9V"e Ti~k 5t[gBjUjIwFO~mWKKmW~gw^gDVaS_wUK)_Z>9 [VD{`W{jڰvڭI]JixUTbzkqQr;0 (ivv)w)NmCWmcNMՃ_J I Bi{v li+ UK[N׶DWmA+0Mav  4"΂qȯU]^5Y1ɫ0AIg@&d(o &Da<& 6P=SMt)M%wblZim|0UaPg48 Ș, tpWZ 4hDGZjŠؼ"""" u$M50Xa4. )/Dt&M4Occ{`PMTDDDDDC!, EUM{U#X|DGa MBpd]B h Xl,+]9K*N)CtG_4o]Xu\\v *tKk Ժ܏¿\pwK⨛xL$UD<;[+U^z d-y~v@RVȁ ۷~v&I:M?p D0"&E L&KC!2G&\vN0D? 40T 0Dh0 P51: )t;ńXa4 Z A FLvi0vIaxV!ӈ4A A`ID О 2PiBrO ^&M]5iPŠ!pi@h iH k `!lR"``r{ :?D#=&x2~E"V{i|4;Ań ! а A@rWxMva}=6L/4(@<a;I]iiӦ8i>?xaWM!qm#G4a[CJA޾}]6?ji'A jGdR^h*DjEwm ?OmҶBǥኴtI zv<&kxAGLdPr"S >k]U @~59Z/wI ;POO CBOkd}au$?O!#, 8)*q[Vۤkt[$$]?;T(*)U!0͎a4A<^m[M5UL'Mtӎ4 1>,Sk2rN Иa{Uu{K[A o 4V駦|Zwla682 3?gNհOȣˆ%d A0-l&MZizv6jD@VRƟx[j DhDD0@2-!IPL*2 C a8Mtlifb{DDDDDC4 &B0 <[AWI!h/!i22. `B *Ұa+a\$\L,2Ci0Nd8a#\3Q`"bal j""""#$#ғuIxP &Gě":c#wa E Շ ށJ{.]aՎ&nR!fTUbc;565&mnӆvhH2#; y-OUqR53DUA 0eYg}]] D0D 4L d! y r! 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Absorption peaks due to the renaining <2O* of thepower are rarely obserrred, and provide only a minorinconvenience in data analysis. One such observation ofsecondary mode absorption is shown in Figure 2.10 wheretwo spectral scans through the same region of the NeDCIspectrum are plotted. The large peak in each scan is aDCI monomer transition due to near 1O0t absorption of theweak secondary mode present in the laser beam. As can beseen by comparing the relative transition freguencies ofthe NeDCI absorptions (due to the prirnary mode), and themonomer transitions (due to the secondary mode), thefreguency difference between the two longitudinal modeschanges with temperature, as discussed above. Thus byscanning over all spectral regions at two differenttemperatures, one can discriroinate between absorptionsdue to the prirnary and secondary rnodes.In addition to multiple longitudinal modes, pb-saItdiode laser radiation is often composed of rnultiplespatial modes. These are due to lasing which occurs inseparate rrfilamentsil within the active region, thus thesemodes are referred to as filamentary modes. The presenceof these extra modes produces an astigirnatic beam, i.e. itis irnpossible to focus both horizontal and verticalcomponents of the beam simultaneously. 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This mode is present at1;;; ir,ut 10* the povter of the prinary mode'ir,.-tiiriition is -only obsenrable since theronot.t R(1) transition absorbs essentially.rr Ln. right in that secondary node'iocatea about 3 cm'1 to lower frequency thanine prirnary node. Such an obsen/ationrarely occurs and can be discrininated byi.un.ing over the sane sPectral region moreth; ott6" with different current andtemperature. The relative separationbetween tne prinary and secondary modes ischanged in this lDanner' 2t01 .25 Figure 2.10 L endstream endobj 153 0 obj 808 endobj 154 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 155 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj149 Do Q endstream endobj 156 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj149 149 0 R >> /Subtype 152 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 154 0 R 155 0 R 150 0 R ] >> endobj 157 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 35412 >> stream % |JFh8 x _6le菗6gl)h>G ь#̹8hBG5PDB"""""""""""""""&qA%̾GR;' DIxk(fňZG"&?F$~ ]X">|~!B (O\ D}hoC]GXWxGuEW8#@G3F:#.Ta4buPK0D|a8Dw\=60GuYC[Duhh8DuXbyu@#OzGXvqׄ]X|aS`?GVqG!N;(U)@_)Ք? zpaA< pQvO!u;ZNv`A?򟎊yC_axNU $qca4*R8ɛu.A ӪP+ŭE%طAE݄loN}~uK[) %TEtGim0":0b;#b:V;ZzXv.$td!X"mbh8TW-MMzuqZ+OIGELBineC26UA.BTuo \/v0G!;v4vffa+Ca4 vG3vHtAm:!O?;>ğ( nJCAȪx;VdDK]k?PA0a`ThFK?֘N#tr?l݅4ϊC \=yۭL'fʁHq٫=o = ?N]i<h `2VGP5<}^E菮wи`Z_MF{ ?]mcOp[aӽ6aPY}<mD_~0T!F4riV_< ȳ|l:N=4В@eJHGO EkiŠa4"L3Z~]/d(_za;Rё_!rVw{pCa q_+kzVFb:X M?u%@ SUbEp}.la<&ԕnlVb Пh3Yۯ5{5wpdeȼT b.`Q ɅD4Lb^H@X_mBwi~ 5JN͌Rqtv H&ƺp_0T7!&d}qӠ i$1DC-{KW_W`J_D2! &k5{ZUpE{"{[MhDDL,05L'iZ_@?")X5Ǡ{8;[dA &h E %h7Y @PA=7{[O0b` k_KҐ½wu ޶"7 Ɣ(/A^ A6|(I" =; /tk0UL*N"Dlll."XZ."2P W0<_~]@_UnC  m,-A"q?K۪", Ⱥ;MSCF:cUrk0N{yD3M78"m^Z[}  itj0 :֘ DAa5(^-{h1% i WڵDC!p@h>0P݈֨ckB!8gЧ&`zԉdU]Zj׈[]!LMWցZtR[mZIt,&,(Hm_VpDE:;uia;Gaq]Laqz-Hv̋ĹPp20:Av|ZaB @dJ0fUejj 3c{۵ C6o$4j^HXA䩒'[L `@Zz oUiń a7na Pd0Lh;9Jh5 4-؆ă'ea8[U iLg@'/ AfK$+. 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373.20 89.28 Tm <7265636F7264656420> Tj 1 0 0 1 438.48 88.80 Tm <6F6E20> Tj 1 0 0 1 460.08 88.56 Tm <61> Tj ET endstream endobj 271 0 obj 9069 endobj 272 0 obj << /Length 273 0 R >> stream 49element to reduce the effects of brack body radiation.since this radiation depends on d, a reduction from roomtemperature to 27 K is a significant improvement, arsothe Ge filter is guite srnarr (5 nrn) and placed about a cmaway fron the detector erement thus reducing the clearaperture. Signal Detection and AnalysisThe data acguisition is controlled by a basicprogram called SCANBELL.BAS (see Appendix f for aIisting). This program calls a number of in-housewritten assembry language subroutines which are listed inAppendix rr. Briefry, transient signars are averaged ona digitar oscirloscope and then sent to the computer forintegration.The basic program initializes a scientific sorutions(#8OOO22), D/A board to start a train of pulses. Onceinitiated, those purses run unimpeded. A vortage ramp,suppried by the D/A board, is passed to the vortage tocurrent converter to scan the laser freguency. Anassernbry ranguage subroutine Vour.AsM (see Appendix rr)drives the vortage ramp. The train of purses fron theD/A board triggers both the pulsed valve and the digitaloscilloscope. The AC coupled output of the HgcdTedetector (discussed above) is band pass firtered with5 dB points at l-00 Hz and 3.5 kHz and recorded on a endstream endobj 273 0 obj 1223 endobj 274 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 275 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj269 Do Q endstream endobj 276 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj269 269 0 R >> /Subtype 272 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 274 0 R 275 0 R 270 0 R ] >> endobj 277 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 36434 >> stream 97"eD`d0l #L5[3HT))lDp8vp8@\@P"vtG $p5 @&Ul "'jB8d>_0I d<2\恐 C_B(xE>?_w°8+«ㅔ<}WPCVP=EWYCePU>=_]uê?ÄP>?‡ =w?C :V#'P}&J//cъ}iN">P_Դ-Ji&IBaq{lURhYԥa }2; n@hXD38<Wiajʠ.v{B<AQ5"B{ 2pw+IHB'o\ L "TLȝ쐟40*B)8G&4~k!B 01 MzBuRA"d5i&PCOM.^V ݇i߭20ߠ>Ǧ DDЄ |? /%&'IB BoP6!*R[%AWK_#^$w%J#~h8]GZt^kh:rcb}?]4at ii rM~xACaeʭ0T ^_A@#M?T$!F A"$0ÙAJ }PN!,܋?ᦃA&jm AhAƛzRq;^G?]=>NŠӻ"C0DM;Vwfiw'pJ麴Ds poY9NtFNh"/E7vAr#O_﷠"0C:\jnݺ!KMl%k$K:n(4#zl  OL;~ : 3¶:~?^AGASVa7AmMgmiva[?{j߽:ָI=;NOoDv'h h-7uB:ڦմw#DyO֫MD2b ziH;v6^[o Kz)'ܕ>_aS[o!9CN;[/ &*%W nME1A?(%Z~_[ N;NKG\ & !a_a[ _N*Μ0" ` &4 CTpiZI!'?h^w#aU [9 ]uҭ! d@Zvi,biZU>f{+Ian4(Mk""lؽ֫%L?6q LaS AXqi׽?[Y!8AD6? %`!Uvà@UTE]=kKt4%E{ Ke ҿm_ . ڶPBCkVRu~׈`T B.6*Bc3['+>lDC% zm6ŦYؑ0UM~†јM΍'I'f>KpRZ Mȓm3ۧMBjI79 vjꟑK i'%?" 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<646574656374696F6E20> Tj 1 0 0 1 329.76 88.32 Tm <6C696E697420> Tj 1 0 0 1 372.72 88.32 Tm <6F6620> Tj 1 0 0 1 394.56 88.32 Tm <322E4F20> Tj 1 0 0 1 423.12 88.32 Tm <5820> Tj 1 0 0 1 438.24 88.32 Tm <4C4F313020> Tj 1 0 0 1 468.24 88.08 Tm <444349> Tj ET endstream endobj 279 0 obj 10045 endobj 280 0 obj << /Length 281 0 R >> stream f,-digital storage oscirloscope (Tektronix nodel 2430A).The scope is operated in a data averaging mode, i.e. theoscilloscope runs independentry untiL it has averaged aspecified nurnber of slit valve pulses. upon conpletionof this average, the scope signals the computer toacguire the waveforrn, which is sent to the conputer overa GPfB bus in the ilfast transrnit moder option of theTektronix scope.Active baseline subtraction is used as follows:Two baseline gates are positioned on either side of thecentrally located signal gate (see Figure 2.L6). Thesebaseline gates are each 256 channels long and separatedfrorn the signal gate by 1.00 channels. A straight Ij-ne isIeast squares fit to each baseline gate (see subroutineSLIM.ASM in Appendix II). The baseline for integration isdetermined by the Iine connecting the point where thebaseline extrapolated straight lines intersect the signalgate, Iabelled a-b in Figure 2.L6. The actualintegration is also carried out within the subroutineSUM.ASM, and involves sinply adding the value of eachdata point in the signal gate minus the value of thebaseline at that point. This active baseline subtractionyields an output which is insensitive to arnplitude noiseon the -1 msec tine constant or longer. 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1 0 0 1 321.60 114.96 Tm <746F20> Tj 1 0 0 1 343.44 114.72 Tm <636175736520> Tj 1 0 0 1 386.64 114.48 Tm <616E20> Tj 1 0 0 1 408.48 114.24 Tm <6F627365727661626C6520> Tj 1 0 0 1 488.88 113.04 Tm <696E637265617365> Tj 1.44 Tc 1 0 0 1 141.60 92.64 Tm <696E20> Tj 1 0 0 1 163.44 92.40 Tm <6672657175656E637920> Tj 1 0 0 1 234.96 91.92 Tm <6E6F6973652E> Tj ET endstream endobj 295 0 obj 9901 endobj 296 0 obj << /Length 297 0 R >> stream containing conplexes/cm3/quantun state based on atransition moment of the conprex eguar to that of freeDCl. The absolute frequencies for the obserrred absorptionsignars are determined with a conbination of a referencegas absorption celr and a fixed length Fabry-perotcavity. ñ lot of the totar power is used for the gascelI and etalon. This fraction is further split withabout 9z of the totar power going to the reference cerrand Lt to etalon, which represents sufficient power toprovide s/N of >1oo for both reference and etalonsignals. Both are obtained by chopping the rR beam atabout 300 Hz with a mechanicar chopper and colrecting thesignals with lock-in detectors (Stanford Research systemsModel 510). The lock-in reference signar is supplied bya HeNe laser which is chopped sirnultaneousry with thediagnostic beams and focused on an FND-]oo si photodiode.The etalon is formed from 95t reflective flatmirrors spaced (znSe substrate) by about 25 cr, providinga free spectral range (FSR) of about 635 Mltz and afinesse of L0-15. since the back surfaces of the etaronoptics are uncoated, about 3t is refrected back towardthe Iaser. rf roore than about 5t of the totar potrer isput on the etaLon, enough of this reflected light getsback to the laser source to cause an observable increasein frequency noise. endstream endobj 297 0 obj 1314 endobj 298 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 299 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj293 Do Q endstream endobj 300 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj293 293 0 R >> /Subtype 296 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 298 0 R 299 0 R 294 0 R ] >> endobj 301 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 36724 >> stream * nauqqC8"?(pE8,()YC¬0~#_ o,? oxTcxDu?xWc#CqZzaS[noT>/][n~8`GWU*; Ǣ B[T =S<u "?oT?aR"?CՄGT.?nxNTo[[[GU¥ ִP^ku |a1Lv tI'ε >6[<}8@ܺjp7wu뭤a"D⬃` !/a5A "NHp`7O {uq8zSXz~tz覉A ZEIߝՒ]pN̝"H0AAQU`E`cwV]J$D<43ܘ ds* "dCYogk&BY#Ȍ3QM:"FdTA3! @`h0DRq"DB9m%7`.\rNDHG)pB΁`NӸhD0imH82" A E 8@ 0&*]>jV$G]\AAivznIh5ixa4zpՍW24M: ܏2,9 %)n]wQ = " d'7vCdZdф D;ldeȽ%L!wiDsrt;d'&vA!mCᧄALhE20Ed\`ȥ{,5MzI=*M V鷭qA::M? 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304 0 obj << /Length 305 0 R >> stream 53The etalon fringes serve two purposes in thisexperiment. First, the fringes are used to indicate thepresence of ruultiple longitudinal modes when searchingfor optirnal tenperature/current conditions for aparticular freguency region. This search is carried outby scanning the laser current about o.L - 0.5 cm'1 in arapid scan utilizing the internal sawtooth rnode of thecurrent supply. Secondary mode fringes are wellseparated from those of the primary urode and are readilyobservable if the secondary node power is greater thanabout l-Ot of the total power.SecondIy, and more irnportantly, the transmissionfringes are used to interpolate the unknown absorptionpeak frequencies from those of a reference gas. CarbonylSulfide (OCS) absorption freguencies are used for theabsolute freguency standard for all studies reportedherein. The oCS gas j.s contained in a static ceIl, andthe attenuation of the laser beam is rnonitored with aIock-in detector as discussed above. The transitionfreguencies are reported by Hunt et aI.11 to an accuracyof o.ooo3 cm-1. Two such oCS peaks are used to calibratethe etalon FSR for each spectral scan. The unknoltnfreguency positions are then interpolated from two ormore nearby OCS positions. Mu1tiple scans over the samefreq'uency regions are recorded and the results averagedto reduce the effects of random errors. 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<< /Length 313 0 R >> stream provides a reproducibility of tO.OOO5 cD'1, as determr".;by conparisons rrith nultiple OCS reference gastransitions. The convolution of our precision with thequote accuracy of the OCS measurements yield an absoluteaccuracy of +0.0006 cm-1. Difference Frequency Laser Spectrometer The fundamental principle behind the differencefreguency laser spectrorneter (shown in Figure 2.L7) isthe nonlinear mixing of two visible Iasers11. 01=0302 (2.10) The highest freguency (or) laser is a Spectra physics2O2O Ar* laser with an internal temperature stabilizedetalon. Whj-Ie this Laser will lase on either blue (489.0nrn or 20486.8 cm-1) or green (514.5 mn or L94Zg.2 cm-1)transitions, dII spectra herein were taken with the greenline. Single frequency. outputs of 0.8 W with a frequencystability of 1 I'IlIz are routinely available with thisIaser.The output of the Ar* Iaser is nixed with the singlefreguency output of a Spectra Physics 380A dye laser,pumped by a 4 W Spectra Physics 2020-05 Ar* Iaser. Dyelaser output powers of O.2 0.5 w are achieved withRhodarnine 6G dye. 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1 256.08 72.96 Tm <746F20> Tj 1 0 0 1 278.16 73.20 Tm <6120> Tj 1 0 0 1 292.56 73.20 Tm <7472616E7369656E7420> Tj 1 0 0 1 364.80 73.20 Tm <6469676974697A65722E> Tj ET endstream endobj 319 0 obj 4883 endobj 320 0 obj << /Length 321 0 R >> stream 55 Difference Frequency Laser Spectrometer Ar+ Laser Ring DyeLaser LiNbOr cn.\+ l"-meter Compu ter Detector Figure 2.L7 A schenatic layout of the differencefrequency laser spectrometer. The outputsof a single freguency Ar' and ring dyelasers are overlapped and passed into aLiNbor crystal. A small amount of infraredlight- at the difference frequency isproduced. This beam is split with 50t goi-ngto a White ceII rnultipass through the slitjet expansion and the reurainder serving asthe reference beam. The outputs of thesignal detector is subtracted fron that ofthe reference detector, the result beingsent to a transient digitizer. endstream endobj 321 0 obj 634 endobj 322 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 323 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj317 Do Q endstream endobj 324 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj317 317 0 R >> /Subtype 320 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 322 0 R 323 0 R 318 0 R ] >> endobj 325 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 35144 >> stream ɨ&@t {@p5pUrRT .Y-@T ioy0er2@2USG@@hfv@ 6S5@mfd a9i,d @Ii 5@7aMP,PF@ A Q5 @0mI$ `ݴj9mDm)d9my9Zih4v3 L $M2r8M5 P  20'̒`ʠ[ eXGX2<6 C7wWwWW]u_$XO 9 60 ^ׯ 0Aq6Kk x?uָWVC h:cal&ad(1uWW_w_]]_ 9 &ب?zp }H5)H=6*eO1AX("HP 'qsyLN ) Sb :V҆eax@ 6+)Ȍ!gaiv BPArsR|Oz%D5BH&t#vnJz-r3;i~аD+6u_m+a<'SO~ӑ.:AW2HV!a9jkJ٨ixM'KݙaWOWi'LA@`OMc]uU:pD4pLTAU. ڦ 4恒]H[aJ∓0z&C >KzUT̴Ddf 5y`L&YHWx!2JOAh6 !np¯A'׶λ OʆlDxA"\2td"$gm/@Hp@ɓiZ7LBkS_TN%kXְz"[ X6U}Hg)ç'͢G'jt kd;SbM6a4d& AzatEBM]uzNK Ä  ELBj'zQ_V c :ia;@YS1AV ޖ%о뿌iwAG,,AS4]0dT*xjC$:h0"b0L7#~B__o{ ZۄA+a4 sz+AGrmP_]]wf`[ !8߬I+vrP#B=_ ֐Kr7( woD$08d}{C6jmXmm^!DT;h2Tl0^LOv+XjzxCȽYh:A|&dLLݧҷ__h'邏m+:\0N H 'wz\5avX 0E~XlzPڥ@fu}^ TA@@IŴ҆ 29U]'}nlQ@gaS0 Ȏq3IXM4|D&pڰ^4:njDj?l AMF l_ὝWgvo&Si|dA4PȾ XO ńxa0l{) t f`"wL$Xa4B"> hDP?0L!6% ®!w]_uէ@N1`O,I"#9( 2Sne+RN ̆Aٕ[)hVAjv !wa`+ v0 u{B@ A-):W"ԞDH0D6yńi0i4"M8nN֐}$9ٶT ;D(H;~qap2G&rq$@ڠ@r &L;i"Mz_r .=4EAC8L8pAjo%A2R" kIX{ {U|'@Іֈgo~:zM)Ȝ#Mitj]:" V脉autkR&} ;Ti9S_]?[g[ @. aD:Ј"Aa;'k !v km9ߧj64M6@ME P_i_E8 0TdᝥM @!<pr>Amj08":}VV}mrt _G 5MA6W]zm/{[OM48m 6XuVivj24X/GaV+Nݠd"ON_n(ÿd3U/VU  ju~EUtQݓ Bka4 qufCG0Atנ`!%-CL F*-aTVma퍦aa";]A 0A pd!"VSEv hB>ȡ O+eKw Mo &\R 6EYm8 t6:KRTctA/y")y ZLU";: nh>$!ۮ[IT0@ʑIXlJZC>* #wPh7mo< 4-\29K$`޹'Mh6CP@v7UĻ26gA:tEg[[ CuO"r8( ƃ U<'?ӓ$ i i Cjn~ߕ7vvL:#S~1MTT'8ăk #'U#BZdk)f3pah;D?dJ>?P>s! h>{ 7F'OiLi՛܉BWJ%g[s)7 㳁i/0\:di4ڭ0Ӳ,'?v5%{C=`ii0i9Nx_:}{iwCDX)`a y PN*Ȧ?": Azy AAVC xWg"jziCIe,gN!N wW#HhK *Z82cvuVh;cU49f,am0A zm艟تk C) M}Cc 5GF=~և^A~Vύcb! i݂ U5d$0`h&ӮzlTmSj i%tAK%i d}D~A޾-u]oWA&"e";rYzAu*T M`";!qt t_[mLw$ Ť (A hՄ ??;;M4ۤd@}d9~Dv3>>p!ixd3~dJذ@ˠm Vu~k|v6:BK`֡nAݭ0]DWJpN0ZK # sȵ9P!PTll0PDDBYFu3=4n2A[{OA2r 5KH!ga5V2' !6a aꝺ dE0 L7L 0zd8dY2gD^H &@v2@]¿¿QrTB2%ç-N6F\PX>vZErb ?L;B ;A6<đ^=Y$k`Yr&@Mq{Tf^vNܝn_{M->vƑqqWD~AdCB>% izwA c38 p{$dzp8a/-C/v(6ia4t M² {LQ:O[߭_2PexrAx :%#QA []ִG87$J㵃!i$ȕ ~_M[=\A 4 A"2CTmaRXo[+!| CAimKJzjo ["LP3 V-i09 =?*:Y i(xi Kj@Xkgy[ OMCBA>>{gI8a84 lB>!A7NP` 1m0|Љ\69>?4%²;ܦ~C-+m&-iT02B"#ugIVX0` &tu.Di1M2BɴqVӾ coܫ !FڭqEB"+j3]&L0@Ok &l"#ȀjҴXwNޚF0`^µiC3ނIvb͑pbi#D{:+[T⩧k" f66,a;AAy N4IN>=hE2$C',HJ"?[4 a<:kVЊtH ^@T`@M>]rBOdeo#ϒt'QQ[Da D%A4"@A TSLȸ@AIo(.q, qh;Ȱ m;;V0BF@twA '?`/ 0@i!HNztD) L l(!K!NN8/Y܍$Y 4i2sV7 KC\TL&Ӱ=?_[kVA;!j!nnְߚ ha ܘ*oT DLMՓ.E2qé_PL4]ݺA \ Գ+wNql*j I_~=/AZv\8DWa44~ `TlS>CEd(PhC5}V ^ 9  RAN UAmzaӲ! i:'W_md!>v5M * M?"^⠯Dtv]",p7U^"ΐ|]'U]xi{Ha$0rh>ANʌB#Aa]p_D^wՐ݂mXL*#Rl0CT# BznB~붠 Y84T! 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A fraction of the output power ispassed into an external Fabry-Perot etalon which isequipped with a piezo driven end nirror' The dye laseris forced to lock to one side of a cavity etalon fringe'scanning is accomplished by slowty changing the externalcavitylengthviaavoltageramptothePzT.SincethePz:nscanisslightlynonlinear,theresultingspectralscan is nonlinear, ds evidenced by about a 10t differencein channel numbers between dye laser etalon fringes nearthe beginning of a scan and near the end' The frequencyofthedyelaseristhenpulledalongwiththeexternalcavity producing scans of up to about 2.5 cm-1 in length.Thistechniguereducesthefrequencynoiseonthedyelaser from the free running vaLue of about 50 MHz toabout 3 l'1llz in a 2 YJIz bandwidth'The horizontally polarized dye laser and vertj-calIypolarized Ar* laser are combined with a polarization beamsplitter and rendered coLlinear vi-a alignrnent throughvariable diameter irises. The visible lasers are focusedinto a LiNbo3 crystal via a 20 cm focal length achromaticIens. The crystal is cut and positioned for 90' phasenatching of the visible lasers. The correct phasernatching conditions are maintained throughout a spectralscan by adjusting the crystal temperature which iscontrolled to to.o5" via active stabilization by endstream endobj 329 0 obj 1358 endobj 330 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 331 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj325 Do Q endstream endobj 332 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj325 325 0 R >> /Subtype 328 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 330 0 R 331 0 R 326 0 R ] >> endobj 333 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 36696 >> stream ɨLG 8-_#Ftipdx#EFc#:9":6#|˙GDt]J|0GG8!r>82:;]88A u]cD~tQe`>UݺP0e+pD{:޵NOW#E>(?aU莬p7 GV"q#6 }J ] c|"?b~+պ_[խӇN#;S~|,7\; P޸V*=oAV?޾Pw__ %.H t>z]ˑӏKUXx:ݬ bX a:q> K um%u @IۑUJ){Mh0 Ch??p~]q[#H|<'xz[#Hhkޕa{C'A>v,%>!fݽ4䵓s3-ك24O;]Azư·ɾ;ڴ<9n~#[z}rdtMB\BA' c'd1J$٭"R) d ;D_R"fPfG!%!93ʁ h.tdN0D8A" 0A4AA! a2d\!`PD1V " `h4`h8` !Ba08au 8`0iA0L v5>ЇX'=wnqa560iit _PTvM=;OM>u[7pwN?!Gaes݄ԃ &`܋6 Ȗ;pƨnG;+q莙 FDAN8d`5"/ ~HAG6 d1y*}twGA#rP ڄPl* 'ON2PںA|&ޝ&'[@Jz? 67 Izz}ӥB MX,%}+iJ갿K OAK |/|QC\zx?x R:q_뾿[_oDzJ ߧ^/[o9kK #0Ko1knK:?_ ^ UZ?_5":mo}V_Z^1l%a+ K3/d;:~MHp2OaaaL> SN{ 4hӠ8Oaa4S~j l0!axi {)8ؾ=` K6Bu5 E-ӑ@4" 0b &" ;iDi4N -&A.h6MDtMkӢ(NROWt%axa0Oa{ u[P>!0 ka5Nkzam8a{0LMCd$a4Q% ڦ ?_&3$$Zd!e,dA dZ0M"@  " HVzqh+`Q`8* ("""""" ʱQaDu\Pj ˤ  PPO N P:xD>0}nC޵@XxV\:H-^P0BE ^2ܮ-iӄԂ5_B\&v:dZcP\PfHȥTyA tAgj"Vn[Zd,,^m6nVAunL\,y)\́<2> kj85̌ V.% n;25c >N!aA[츈-0@D2D4H**!S3:(#yD9!Њ17!" !TB q0vAOO]04,!4"݂CT`Aj(zm(':-;[Aq 5zO{m[ojWmmCAIa |w&N:`L Sd֛DsӈvB"{w@iBp Qtp<-Lo#r,̅IWKA7=&Ϥ ) ;aA 7/ Pkaz v7Iu&qNA/_Y7}?z~BivO~zR4N =wEX%p5zItJ(vMW׻/ïB jǓ.C=t;WץƾֿK`&?Jj7ŭ?~Z[Jhî~azzȎk('ԧd:7k!ۧG< R[oȀ]*VRvSb}oV0Wʂo/Yk_S%kvaoo-bsk]{K\N҆NL09_kOz_zw]_fiZUI}c`qqmG $ M6.'z /i Z *rdp ߴV$[~EC0WNt  `AŦi CGLRw8<`Hc6(-NjR}4 4C hsY0A;Ѓt᧢&BCB3t8Ӻ iMwM5vէm!Ҥ&M'h:Ox@A2d9ZdW0^l&*A 2zLM4a4M0¦B& D=0d&2))0AjZjRW#21!J (hb 9YJ)tA ;7 n""J j]a:G^<oB626Q2PUqޟ.PaQCS݅oUhl?Žaqa;B޷E8,|6+T'irl-Nu+yB R`DvV2;P} h0AӆgjY.P?]~_ӌ,>뻺|>;(}qՔ4l8s"-Xxi! {n*LfdHrʠ8R[RHguoA  `g=30u AaEЈ &O!% +f! 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endstream endobj 335 0 obj 9966 endobj 336 0 obj << /Length 337 0 R >> stream 57comparison with a reference thermocouple junction.Because LiNbO3 will transnit from visible to only 4.2 1rr,the crystal itself is responsible for the long wavelengthlinit of the difference frequency spectrometer.Conversely, the short wavelength extrerne (2.2 pn) is determined by the lowest ternperature at which the LiNbO, crystal can operate and not suffer index damage due toabsorption of the Ar* laser. This damage is prevented athigher temperatures as a result of self annealing in thecrystal.The resulting IR beam (power < 1O-5 W) is focusedwith a LO cm focal length CaFr lens and then split;approximately 50t is used for a reference beam and 50tfor signal detection. The signal beam is passed into aWhite cel112 multipass arrangement. In this opticalIayout, end mirrors (go1d coated pyrex substrates) areseparated by their radius of curvature (30 cn). The beamis focussed at the input mirror (M1) and refocussed onthis mirror with each pass. The infrared beam istypically nultJ.passed through the White ceII either L2 or1.5 tirnes and then focussed on the signal detector.Both the signal and reference detectors arephotovoltaic InSb with an active area of 0.049 mnz. Thecurrent signals produced by the detectors are convertedto voltages via transirnpedence arnplifiers (identical inprincipal to that shown in Fig 2.L5 with a total gain of endstream endobj 337 0 obj 1348 endobj 338 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 339 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj333 Do Q endstream endobj 340 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj333 333 0 R >> /Subtype 336 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 338 0 R 339 0 R 334 0 R ] >> endobj 341 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 36082 >> stream 1aѶGm_7#>G aGFp#HfGo,8fA#8r.G0Y ج0GdcYAl#p7,ّ `܎5&r"KpC HGxe q4F`8xm #h. 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These aurplifiers are assernbled in-house usingcomponents carefully chosen to rnatch the freguencyresponses as closely as possible. The outputs of thesignal and reference detectors are subtracted, thusreducing the IR anplitude noise to about ]--2 x l-O'a of theincident light leve], within a factor of 2-3 of the shotnoise linit in a 5 kHz band rrridth for about 5 pw of IRpower.Absorption signals are concurrent with the pulsedvalve and are rnonitored via attenuation of light reachingthe signal detector The infrared signal recordedduring each valve pulse is displayed on an oscilloscopeand averaged with a transient digitizer (DSP TechnologyModel 2oo1s). Typically, four pulses are summed togetherto increase the S/N. This sum is then passed to apersonal computer for integration with baselinesubtraction providing a detection sensitivity of 1O-5absorption/ Hz1/2 per single gas pulse in a 5 kllz bandwidth. This corresponds to a detection lirnit of 1 x Lo8Hcl containing complexeslcms/quantum state. Thisdetection limit is 2OO-foId smaller than that for thediode laser. This is due to 1) 5-fold highersensj.tivity, 2) the 2.5-fold larger HCI absorptionstrength, 3) the 2-fo1d narrover line width, 4) the2-fo1d longer pathlength, and 5) the ability to cool allHCI molecules into J=0, but not DCI. 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Thesedata are collected through A-D ports read directly by thecomputer.Once signals are observed, the absolute freguenciesmust be determined for each transition. A home builttraveling Michelson interferometer, referred to as arrlambda meterrr, is used for this task. The apparatus isshown in Figure 2.I8 and is based on the original designof Lee and HaI113. The scheme involves separating thelaser beam of interest with a 50t beam splitter, andpassing each fraction through a different arm of theinterferometer. Interference fringes are collected (seeFigure 2.L9 ) as the cart travels from one extreme to theother (40 cm in our apparatus). The ratio ofinterference fringes counted in a certain time intervalfrom the light of interest to those of a referencepolarization stabilized HeNe laser is egual to the ratioof wavelengths for the two lasers. Since only anintegral number of wavelengths can be measured, the errorassociated with this measurement is as large as 1 countout of about L X 106 total counts, or an error of 1 partin 105. This error is reduced by increasing the numberof counts via a phase lock loop which nultiplies thecount rate by as much as 1-6, thus reducing this error to endstream endobj 353 0 obj 1345 endobj 354 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 355 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj349 Do Q endstream endobj 356 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj349 349 0 R >> /Subtype 352 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 354 0 R 355 0 R 350 0 R ] >> endobj 357 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 25544 >> stream ɨtcЎ@peHQQݞ@pGP#cS5 J` e0:9nGŹmp6AǖyD#clf尵he%-| \m">{#4du-qmqZ±6k8C8Öl &8C,yjB#3`m夦pJ6P(Et\  dr#.|eS#ȎX ߖUl (6r,"8@&HAdް6ɰGh6ܷGˁ9\ @ @\Z #qvGQ9ڄGEPq1Gp%1|%JlTyh)h0`j@@@h@e4FaGK5nTH  VY+(`[*х޿U#[#MP[PX?jjƸvHޖZ[*v_kpOwzezݻ[l.PJ ꗱ _UՇ:ރo?`wڷ_xUðT"?;cJaRa G\wzz#!#dL̗ "HS5#XT \$T߫ x[w9vW.oMAvnV V0p &"]b\iw¤]lwNXXtDu*V<-ޗߵAU#A;]ܺåDu[߽}+:jïպ:G[[96YP\}=gY8xV"?KIv"ޭ} .:~oduG_ǫw#D{\.t@uco,= î–٘>aKl la}5[ia&ؘ"nT[0A}n4 C;A7iFT X?AiؚA :ZtڻA aj u[_ pa0&Qdc[SӢ9vT!aA 40MXtxDCw #o}}5p*# ~d ?PȺPMtd`}OO_:& &]l=}[Az }ӥ|0l$piV ~CDpd5t /܃Cғt] :'o֪NokZ ^mxJV%}.r"ﴟzӶ`}{_kl":ȃczwJ  ?﮾r)ȀmZakK[X` <&۵u:΁bik *iW;t~aݠ0_%Oiu|TCMd!GT3wJp ¡}~Ґ64Ʒiv҆2 idvn[xrM <3 c;Nt@ֹK) x6A(kym l=i@tC,<[Y m[~V}P|o" >޻  ނ =3 7Ƿ 4K;7|":vA_ 7ow"CICݞ M?ս=h5N{!.{ {Ioo]XNv} ?تރ{wսB"O6+c oa9"G_ պ¶Ȁ\+ ۅ^?kCo'vm[mݾoεzoT }VV텿oN %O÷zVx"= ; mSM}/m0}0?ai /VA:3 슃J,#o˫w ?nGV]+xw^o(a߷aڮb?շSuF Ciˆ@aumV |}@k!Ǯ2̂K{ݰ^JhSi_ۧۧm-m[Շ75o;itaCy*"`. 0KGVOa~ x|9 W(6  8Oa_mApK.}C }6b~^6_p`#@ 6# ۽vk۸a[{u}";\A[R׆-s[տoҴ5mRm0']N4V3?L `t?m!aKmIiDb!?A["uza%# 0NOaDno }4w1[aӼ oxmt_VI/{UHmm/~6h%aO!).arlI&:iW\L:o=*o躤m!a GumV^l47٭0]d l$״M ,XaﯶBO%Q |=;H&PiizmA6 *lUGi:qT e|0 ?PImՆh&=#iV a :Li}J(mՆAC % xe?[V4}eu@ЩVaD2  B([D\X0aIPU T CC 0 $GEtu v%t62;{Sh&{t6ÒHn:ob]i.":'All4 cDWUk +#ih0icՄiCMJ$Al8l4 rw[ &AWQai0:a=y$9xaNE@ãڤK4 l. ?4l%ACvXm%&mO[jʂ OIw da0BmAm20P@^m^n4M5Mn_:/!KvA  A]ޒp_aSaY o6%MNumWHhI tu |'zatWu~azR${i.`0I/Ҹ`];u  BMA0Izԁې<MJҦ*AAABLҶA 0ֵl7Ra?N Њ^oaՆ2+Z_m%{kנJWumҾvl%kKҵd=Z CvKJJC\Xm`eO ] 6*ie2G6A i &~m ԉ`a @ѣ# !{mfg3mJatl%_ ghGp ^DCK0Tӆ!abtL6Z 6az#mIxl(l7?m&~ $[J{l0ml oҸa~ՆAa%¶@m]L6*o^ % (aJFh6/A oҢJ:L0][mp~mpP~Mdu[oQ6ީQUl?JMXն w_Ӱo =66ߥ]6V.Km QհߥmJ҇V~6ߥ A҈=6xJ qT6 +PA:(o}҂ (>oK.z ZnPjzT<6aI* |6z_oJ DLU/Vޔ-6 턝)^h-i,6v[ i ABJᰑ.m- +V!]P-8ka Pir:פ?z 'tDPa"ۺ7}XtM,7 Zd . xiYHQݥY oASp)fiޖ1AÅMw5A&- ނpv":xA6qL[k6h-x@ ~xMI8n;=mRk3Y4պ% NDi7}Mb"76,7w /Mm}+H>Åt&#kx|iMa:K㴻w~CV{w&l' x5T?{vò:{qa' um aa7ɽoJana$ooOΎAl=ԐH*ommIl<7Iڄ[{wa$[xa :Vh{Iim2zmm$aII&ICMH%w H-P ! *{lwd PK "Kom#ВMT[ [8A%lu %m%iA8mp[l4 ÷taޒ[mH l:IpJ[mRIl4նCʤAnmM$GV jvR jh}PInmU !Kmԭ `I0@RuEh:Dmۄ 0MmI>?Ah$dUˤ a"YޝÇO-Az[A{ K oK^oM z^A/ U$n?_}$T%߬.I%Km_KaH/m}%U^M]/H% /m.{~NWݝ=$ti]餕m ^VҶJՆǥgUX0ڦJa&a&*B4i$ +T]uP:a4“It B 0M^m&AA)-04a E$6d4ެA%[mu^*6 a%ƐKo#H2 n% -:ISm LF}$aA a"$aIo. mt¤m PI6I w $xTat ":#I6ñH0R: A%m$nR 6tl0I 7H' IPI2pI&AJC:[I0m H& 0ZǒJC5UTA&۱ n8Im0M6b$ᇗTit7 4>6:i[ &ې<5N Fa4tG af>۠A&hM6XI l8tM?@MްIxIdu@ap a &Ɓ l;A o#II u a Iւ aBI0ZI6èIwaAIxH$~0 $4 H6}$nIхA$m4MIA6$màv ݄]BJa m &a$ommm I &ۇA RjMwPval>$ }$lkGTa$n@iH mPI7MoMl+I$OmzGp# Mm 6+`*@l{&nP ā 68H+aí0iT;5 lazA @L0m9Naپ۶*z 4APL7i$}$Em |$E$aCH$I mA$n$l:A܏In$a$aMкH o$a$aMt6A$mI6â?I&A $htL6Iz |$mM 6I&uI&۪AaäaPMT EA$:I0ۺ a֒M.mi aA6A&uI&۪A n$#IU$aDuIVtA &a H&$@B &o$n1A nmI0} mMҠy~I4Il>IH&$}$ PAwI[nL6I&uI&ۄGTmna mh$  #A&pH6 :I0ۂ $u$a Ima  $}$n$ 4Ω7A$ Fuˢ]PAl`mI^Mä 7!9gOmƕ6&  tP6tduH$oGT $oJ+a}$nҬa, –umTaIaS n)z Ky )nm;,$l:JMK}, AI`PIzҴ ޒAh$l7II6ޒA }-mZ}-PM#IRIXA$ 5It$mIn(H(mJM&MD L6% V|$m$ %Iդl0W}-%m]tAZH&zJI%NIX":i$ ,}- mK]-$m, l7.E@åZA"X$Y C 3IXI"n CE8Ft-$7؞m.$Wa-$ AoKtJCMʑM ȫ IKI&6ޗtP4a.${ bt qI+ttaa$I=$mԜRJ& iw u렅P&+}T"4H atjv:KI'TF+M"#Gd#HBH- S! 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1.20 Tc 1 0 0 1 214.32 90.96 Tm <6C617365727320> Tj 1 0 0 1 265.68 90.48 Tm <697320> Tj 1 0 0 1 286.32 90.24 Tm <6465746572726E696E656420> Tj 1 0 0 1 366.96 89.28 Tm <66726F726E20> Tj 1 0 0 1 402.48 88.56 Tm <74686520> Tj 1 0 0 1 432.00 88.08 Tm <726174696F20> Tj 1 0 0 1 475.92 87.36 Tm <6466> Tj 1.44 Tc 1 0 0 1 214.56 78.96 Tm <7A65726F20> Tj 1 0 0 1 250.32 78.48 Tm <636F756E747320> Tj 1 0 0 1 301.44 78.00 Tm <666F7220> Tj 1 0 0 1 329.76 77.76 Tm <746865736520> Tj 1 0 0 1 373.92 77.04 Tm <31617365727320> Tj 1 0 0 1 424.32 76.32 Tm <746F20> Tj 1 0 0 1 446.40 75.60 Tm <7468617420> Tj 1 0 0 1 482.88 75.36 Tm <6F6620> Tj 1 0 0 1 504.48 75.36 Tm <61> Tj 1.44 Tc 1 0 0 1 214.08 66.72 Tm <7265666572656E636520> Tj 1 0 0 1 286.80 66.00 Tm <6672657175656E637920> Tj 1 0 0 1 359.04 65.28 Tm <73746162696C697A656420> Tj 1 0 0 1 438.72 63.84 Tm <48654E6520> Tj 1 0 0 1 475.68 63.12 Tm <6C617365722E> Tj 1.44 Tc 1 0 0 1 106.08 140.40 Tm <4669677275726520> Tj 1 0 0 1 156.96 139.92 Tm <3220> Tj 1 0 0 1 165.60 139.92 Tm <2E3139> Tj ET endstream endobj 367 0 obj 4706 endobj 368 0 obj << /Length 369 0 R >> stream 61 Dye laser ], Meter Fl-inges IFq)fE oo.qgoc)oo$lco OAoIc?oolIqIU:vI 5.0 0.0 r0.0 r5.0 20.0 25.0 30.0Time (ps) 35.0 40.0 45.0 50.0 An example of the l-neter fringes obtainedfor the dye Laser, with sinilai fringesobserved for both the Ar' and HeNe fi-qnt.The freguencies of both the Ar* and dielasers is deterrnined frorn the ratio dfzero counts for these 1asers to that of areference frequency stabilized HeNe laser. 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<542D> Tj 1.92 Tc /F3 11.0 Tf 1 0 0 1 524.40 710.40 Tm <3632> Tj 1.44 Tc 1 0 0 1 124.56 678.72 Tm <6C65737320> Tj 1 0 0 1 160.08 679.44 Tm <7468616E20> Tj 1 0 0 1 197.04 680.16 Tm <4C20> Tj 1 0 0 1 210.48 681.12 Tm <7061727420> Tj 1 0 0 1 247.44 680.88 Tm <696E20> Tj 1 0 0 1 270.48 681.36 Tm <496F372C20> Tj 1 0 0 1 301.44 682.08 Tm <6F7220> Tj 1 0 0 1 323.04 682.56 Tm <61626F757420> Tj 1 0 0 1 366.72 683.28 Tm <6F276F6F3120> Tj 1 0 0 1 409.44 684.00 Tm <636D2D312720> Tj 1 0 0 1 447.60 684.72 Tm <666F7220> Tj 1 0 0 1 475.92 685.20 Tm <65616368> Tj 1.20 Tc 1 0 0 1 124.80 654.72 Tm <72656961696E6720> Tj 1 0 0 1 182.40 655.92 Tm <6F6620> Tj 1 0 0 1 203.76 656.16 Tm <74686520> Tj 1 0 0 1 233.28 656.64 Tm <6C616E62646120> Tj 1 0 0 1 282.48 657.60 Tm <6D6574657220> Tj 1 0 0 1 326.88 658.32 Tm <666F7220> Tj 1 0 0 1 354.96 659.04 Tm <74686520> Tj 1 0 0 1 383.28 659.76 Tm <76697369626C6520> Tj 1 0 0 1 442.08 660.48 Tm <3161736572732E20> Tj 1 0 0 1 506.16 661.68 Tm <4173> Tj 1.20 Tc 1 0 0 1 124.80 631.20 Tm <64697363757373656420> Tj 1 0 0 1 196.80 632.40 Tm <62656C6F772C20> Tj 1 0 0 1 247.92 633.36 Tm <7365766572616C20> Tj 1 0 0 1 305.28 634.08 Tm <7265706574697469766520> Tj 1 0 0 1 384.48 635.76 Tm <72656164696E677320> Tj 1 0 0 1 449.28 636.96 Tm <61726520> Tj 1 0 0 1 477.60 637.44 Tm <6E61646520> Tj 1 0 0 1 514.32 638.64 Tm <746F> Tj 0.96 Tc 1 0 0 1 125.52 607.68 Tm <72656475636520> Tj 1 0 0 1 175.68 608.64 Tm <7468697320> Tj 1 0 0 1 211.68 609.12 Tm <756E6365727461696E747920> Tj 1 0 0 1 298.32 610.56 Tm <6576656E20> Tj 1 0 0 1 335.04 611.04 Tm <6675727468657227> Tj 0.96 Tc 1 0 0 1 161.52 584.64 Tm <546F20> Tj 1 0 0 1 183.60 584.88 Tm <636F6E7665727420> Tj 1 0 0 1 241.20 585.84 Tm <7468697320> Tj 1 0 0 1 276.72 586.56 Tm <776176656C656E67746820> Tj 1 0 0 1 356.16 588.00 Tm <746F20> Tj 1 0 0 1 378.72 588.24 Tm <6672657175656E637920> Tj 1 0 0 1 450.24 589.68 Tm <726567756972657320> Tj 1 0 0 1 515.52 591.12 Tm <616E> Tj 1.20 Tc 1 0 0 1 126.00 560.40 Tm <616363757261746520> 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eachreiaing of the lanbda meter for the visible 1asers. Asdiscussed below, several repetitive readings are nade toreduce this uncertainty even further'To convert this wavelength to frequency reguires anaccurate knowledge of the index of refraction of air,which is far too sensitive a function of temperature andcolor for our purposes. Instead, the absolute infraredfrequency is determined via observation of reference gastransitions (eg. HCIT or HFla) for molecules seeded intothe supersonic expansion' This provides an infraredfreguency correction due to the srnall uncertainties inthe HeNe freguency and index of refraction. since theHeNe f reguency is stable to !2 ltftIz over several hours,and the room ternperature varies only slightly over a day(<5 "C), this freguency correction is useful for anextended period of tirne. one could use a reference gascell similar to that used with the diode laserspectrometer,buttherearenotasmanylikelycandidatesfor reference gases in this region of the spectrum (2 4prn). AdditionalIy, most of the rnolecules (eg' CHlr HF'HzO) which could serve as reference gases have largerotational constants, and thus rotational spacings>1 cm-1. One i,s then forced to interpolate a significantdistance to cover aII of the spectral scan' since lambda meter conditibns (eg. alignrnent and endstream endobj 377 0 obj 1371 endobj 378 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 379 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj373 Do Q endstream endobj 380 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj373 373 0 R >> /Subtype 376 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 378 0 R 379 0 R 374 0 R ] >> endobj 381 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 40220 >> stream 4, s3 Gc#j 68Rs^Tqa51@ m,)992C5.b6E9G8$@rF2ᰎqLNGHѢ5 `~"$!]Wg>Gˌ!p:0A ,*B"""&hDJ2'Gc$#_0Dv].%(#6DDDDDDJ. 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<706F736974696F6E7320> Tj 1 0 0 1 464.40 85.20 Tm <77697468> Tj ET endstream endobj 383 0 obj 9940 endobj 384 0 obj << /Length 385 0 R >> stream 63room ternperature) change from day to day, the lanbdameter must be caribrated daily. This invorves repeatedlymeasuring the apparent transition frequency in the slitjet to deteraine the correction factor, i.e. measuredtransition freguency ninus the true freguencyt,l4. Byaveraging about 40 measurements, a residual standarddeviation of the nean of about o.ooo2 cm'r is obtained fordetermination of the correction factor (0.0416 cn-1).This correction factor changes sJ.ightly from day to day,but is never more than about 1t unless the rarnbda meterj-s realigned in which case it roay vary by up to L_3t.The van der WaaIs transition frequencies can bedetermined using the same procedure as for the referencegas transitions. However, due to the significant numrrerof van der waars transitions observed (eg. over 12oo forHcr dirner alone), not all van der waars transitionfreguencies are measured directry in this manner. Thefrequencies of these absorption peaks are determined byinterpolation from lambda meter determined frequenciesutilizing the dye laser transmission fringes. The freespectrar range of this cavity (ca. 322.3 MlIz) isdetenni-ned by calibration with two peaks on a particularscan which have been neasured interferometrically. Theabsolute frequency accuracy for peak position deterainedin this manner is +o.ooo5 cr'l, or +15 wHz, as deterninedby cornparing interpolated reference gas positions with endstream endobj 385 0 obj 1414 endobj 386 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 387 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj381 Do Q endstream endobj 388 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj381 381 0 R >> /Subtype 384 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 386 0 R 387 0 R 382 0 R ] >> endobj 389 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 31850 >> stream %uup+C?E+ _w|8]W]}w__Wu_U‡W +Pu ̰>PAAzJDe﷒Z!p}ȉ[ ;= եPiq }uP]}_u}Ka8a!)UL*~'J[‚=t4'9C<=+UM3* dKMb&–_Mu w޺ôﯪHʇapPl"lʂ%I `@x\RMق*Efa8D`D,4HЍa tl 5[ /5C-p]v_Ȃ}m^UiUxaBmgBsEh2v}:A75 Qj@%7&{WA^7n?ֿ;FI~n֫[iC߲ B.KdG״6A xt－cz# ZZ]y0PJFD{UҾμ55\?k_׆׻W;OՎ*. %iKXea}S^aBim6 . ='nEc  M>im~'pdP@!Ȱ N^"#&6j !; :șCO""""$ ! 44Ѭ)Ȼ DDDDEwO@ʃ ]Wu]}w}eî.[r[KHQh< a_dł*B AkR*i[΃@PM jj&bD'G{=B ioҢ>;NK `+]3x2T}0Zh9I#,LЌb!s# ݢҰw]X p]PC1N1 L_B  r%DHH K#:dDꚺpqa LA\!"3P͊kY;{M'vqaN!"i[(vڨ:ֿ* 5"8l"'jk:A_HnD }鵗BIPuNv1"(+Zp PL A[yޯ%@0{5z}3k꾱'`/]5yj~ImVÅd0 nyxn/_TJ]d$57ztGtkkdvxpT8?9\j _>ܳGk/0Sݰk՝B &^D"-[It݇P0~߭n@!qw?%J#Lz";n48pm5?Oki AxA'# hM‘>˶4۾r#vZEѬ)'ò$!*<k~CڄPb/}ϧo҅y 0 pzkimN)հKoO QjoW 7~i/d([_ X0Zu۽XdU`-!I]kI.B>JtG:zU k ꟷoz| Z uz 5niVA?__nG7*!z68i}_k֯Y` (6#pa 68cci +ZkgO{]=~jMJtM0x`|20M='kV_vEw$a0nv-Sc:ᅰ<$S 0Almi 4ﰮOmD-\Y@/R}b80>$05djU|21 \34#֩]m>A"# [PAŦqP=qN !^-vaZ "j8" kXDD@i  d% A!}Xa%+=PNfPAa! xaIX& &N4""""4" `&0H !<'40L)/MkZ`i2@EAyC f+8rg F)=|T4,J+է v kJE}J傒bfC_};T ?BP5 $K~>3gA" G qvpva;Ai3͌۫;Ytuq}!) h!80h!"d&UPn6Nm텻[ 4 `@ d!Y 28`BdR@ΌE(z"{F O#>NAL-whafLSA3K("s(3Dy#QBQm}Ͳ$AT{/#{IN|0M?Aah4 Z`!`ʁH1MwI@&Aq莌]y'0ȅȼզMCoiAo qaߤ=?%'y*^ (nK 쾢-M]5iMMt[gP/M᫦v< m"vP@\JmM".6n|'z;UzC~^/wI5֓aIޠb4v<9mD#!9.Gh:ׯPZWi7bcO'%AAHm  ຶC}}=K^55[xj~8O"#R%\ ijHKm^ƽVF4W=8.7 9ZkאiCa _?n%c^}"ȽoW@ k4_m޶C:?r Ȍ2M;L?yGA_Q2!fR#_?nG;ӆdEgNI}hZRKl" m/! 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SIit hrlsed Valve and Gas Handling The study of van der Waals complexes reguires anefficient rneans to synthesize these weakly bound species.A supersonic expansion, with its high number density andlor.r rotational and vibrational temperatures, has provento be one of the most useful means of synthesizing thesecomplexes. AdditionaIIy, the slit jet geometry providesa long absorption pathlength as compared with a pinholeexpansion. The single pass absorption pathlength in theslit used for these experinents (4 cm) provides about a400-fold increase in path length over that of a LOO pmdiarneter pinhole. A multipass, of course, can furtherincrease the path length; 12 passes for a total pathlength of 48 cm are used for these studies.Additionally, since a slit jet only expands perpendicularto the slit axis, the density of gas falls off as I/r,rather than the L/rz drop off in density for a pinholewhich expands in two directions. This provides a highernumber density and more collisions than for the pinholeexpansion with the same backing pressure. The slit hasan additional advantage that the nolecules do not expandalong the long axis, thus the Doppler freguency shiftsare guite small for the slit expansion (eg. 25 ll&tz FWHM endstream endobj 393 0 obj 1256 endobj 394 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 395 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj389 Do Q endstream endobj 396 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj389 389 0 R >> /Subtype 392 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 394 0 R 395 0 R 390 0 R ] >> endobj 397 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 35098 >> stream 25QuXH}#CpX">GqՂ!~C":GXC.GGG##XPE8"?p#p-TcahCnG޾CSpEaڄ>>a+X"X]qx?(x^ YCv=CTA":xKxx_(C֨;+Ԏeoaۥ{qtPP>uU|Kzްx#]P| Lq[u*> *U^," ,ӂåt/tXp;rsBm7tou~ݽOM~EKBD[&**;02؍p.G[ձ T<(x[[GU:޶K#|=H.EarʐRɺ+UTL-ః+LP! *Uԗ}4@zz~K !G@4 E;fDwit$*26d`qlD| 4ҰL`@geiQ 0D ")ȾG;e$FA^M?M a?L a#R@31d",'&8;^ a5Anr3P1:.T8m;v5Tlw` &f] * KFt2C"%MõGO#HNlw[h0MH0* hMA8'n7I]Eݐ܏!ZZv5MjӄC`u +M]Bt82:ȴl<5jOAm];_^@`K?}SPiCATpdE yMd:զ 8:xB@=Aa wI'0/DC =_MkZZ!xkk22_]ý?At>V0J{V}t&ҿȂA!tE~ak=iJPQ' ΈP _C c")C[A>8[zVI@Y կ7z }{n _h#A!H'>[i !$t~} ׇn"4q'kd7{ h}WJkb׮/Oppal/ { :u`說UccY 9Na=_}v7ԫ'ҿDjX" #"QA|&fwk{נ߻oXOwa=<6 0PiZ ^z^Or8AXMKi Shp>N2xƩfoʐA^׆0!~  Om 4C>@iǝM0g_ uίo]2 h0M.dp!HAӊcOk}DDPQ M4`𕭯M;jA șB""""#G4a8a4 /`^4@TUdG2cNL&§vi&@a;c""""dzh0 [ jDDD2j0R, *Ma80@adyԙ !Pq.>P@a?JCG0U uç[  S_Zm3QDc*1 d1GBu5aB (T0Ū{OL0鯴Ɵd;!F܋K"z@#B=òH֞mO mרZU_ W@0; za W8lW O@0nI]; lԓ{{Zh;T^Ω;QA8+ 4a?DGŠ6,0Ui#td&Q! 82(EDDFꃢIƶE*v_ 8Aj/PGPߑGvl*j^ժ{- E# iCAMh %5gj!-r;YI_GP4G D"Mr:E4vf]4Dƫï@pgT htGݯ]ut `@#_" ϢxBv6!TXAj c@Ȕ&.>pI?xv\R0! .(L (NF#m=ݾAq Ѓ "h` d49?>l 5wv~hq$ At "ynO@ӷhA =0jti݄]ȡY^ݩ )"C Aڷ!gh5 ȆgKַzz!HNɟ!/%62Mh5;XD ̅B3zڄڶ8idt`)w]OU A .W=N֖N  f!H USCA%u*o}n}Q@e- &hvUUk?[ڴG*ai0魅u @l4꿥^1}*ޕ_d 5kM~tp+V$iֿ3ޱ? 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470.16 522.96 Tm <736C6974> Tj 1.20 Tc 1 0 0 1 108.00 501.60 Tm <657870616E73696F6E7320> Tj 1 0 0 1 187.44 501.12 Tm <68617320> Tj 1 0 0 1 216.48 500.88 Tm <6265656E20> Tj 1 0 0 1 252.96 500.64 Tm <6578706C6F6974656420> Tj 1 0 0 1 325.68 500.16 Tm <696E20> Tj 1 0 0 1 346.56 500.16 Tm <74686520> Tj 1 0 0 1 375.36 499.92 Tm <4843492D44434920> Tj 1 0 0 1 433.20 497.52 Tm <2F20> Tj 1 0 0 1 448.32 499.44 Tm <4443492D484349> Tj 1.20 Tc 1 0 0 1 108.00 477.84 Tm <73797374656D7320> Tj 1 0 0 1 165.60 477.36 Tm <746F20> Tj 1 0 0 1 187.68 477.36 Tm <6F627461696E20> Tj 1 0 0 1 238.32 476.88 Tm <6120> Tj 1 0 0 1 252.24 476.88 Tm <6D65617375726520> Tj 1 0 0 1 310.56 476.64 Tm <6F6620> Tj 1 0 0 1 331.92 476.40 Tm <74686520> Tj 1 0 0 1 361.20 476.16 Tm <656E6572677920> Tj 1 0 0 1 411.60 475.92 Tm <646966666572656E6365> Tj 1.44 Tc 1 0 0 1 107.28 453.36 Tm <6265747765656E20> Tj 1 0 0 1 165.60 453.12 Tm <74686520> Tj 1 0 0 1 194.40 452.88 Tm <74776F20> Tj 1 0 0 1 223.68 452.88 Tm <636F6E666F726D6572732C20> Tj 1 0 0 1 310.32 452.16 Tm <617320> Tj 1 0 0 1 331.44 452.16 Tm <77696C6C20> Tj 1 0 0 1 367.92 451.92 Tm <626520> Tj 1 0 0 1 389.76 451.92 Tm <64697363757373656420> Tj 1 0 0 1 462.96 451.20 Tm <696E> Tj 1.44 Tc 1 0 0 1 107.52 429.36 Tm <4368617074657220> Tj 1 0 0 1 165.12 429.12 Tm <56492E> Tj 1.44 Tc 1 0 0 1 143.28 405.12 Tm <4F6E6520> Tj 1 0 0 1 172.32 404.88 Tm <646973616476616E7461676520> Tj 1 0 0 1 266.88 404.40 Tm <6F6620> Tj 1 0 0 1 288.48 404.16 Tm <6120> Tj 1 0 0 1 302.88 404.16 Tm <736C697420> Tj 1 0 0 1 338.88 403.92 Tm <657870616E73696F6E20> Tj 1 0 0 1 412.08 403.44 Tm <697320> Tj 1 0 0 1 433.20 403.44 Tm <7468617420> Tj 1 0 0 1 470.16 402.96 Tm <666F7220> Tj 1 0 0 1 498.48 402.96 Tm <746865> Tj 1.20 Tc 1 0 0 1 107.52 381.36 Tm <73616D6520> Tj 1 0 0 1 143.04 381.12 Tm <6261636B696E6720> Tj 1 0 0 1 201.12 381.36 Tm <707265737375726520> Tj 1 0 0 1 266.16 380.40 Tm <626568696E6420> Tj 1 0 0 1 317.04 380.16 Tm <74686520> Tj 1 0 0 1 346.08 380.16 Tm 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<696D706F7274616E7420> Tj 1 0 0 1 243.12 92.40 Tm <637269746572696120> Tj 1 0 0 1 308.64 92.16 Tm <697320> Tj 1 0 0 1 329.28 92.16 Tm <7768657468657220> Tj 1 0 0 1 387.84 91.68 Tm <6F7220> Tj 1 0 0 1 409.44 91.44 Tm <6E6F7420> Tj 1 0 0 1 438.48 91.20 Tm <746865> Tj ET endstream endobj 399 0 obj 9911 endobj 400 0 obj << /Length 401 0 R >> stream 65measured for ArHCl transitions with 400 torr backingpressure.One further benefit of the slit jets, discoveredonly after having studied a number of systems, is thatthe vibrationar, rotational, and translationar nodes tendto be in eguilibriurn at a conmon teurperature. Thispresumabry results fron the large number of corrisions inthe slit expansion. This equilibrium property of slitexpansions has been exploited in the HCI-DCI / DCI-HCIsystems to obtain a measure of the energy differencebetween the two conformers, as will be discussed inChapter VI.One disadvantage of a slit expansion is that for thesame backing pressure behind the expansion, the purnpingreguirements for a slit expansion are considerablygreater than those for a pinhole. This is a directresult of the 500-fold larger area for a s1it, 4.O cm X100 pm = O.O4 ch2, than a LOO pm pinhole with area =8 x to-5 cm2. With the o.o4 cm2 slit and 5oo torr backingpressure (optinral for HC1 dirner studies) , the gas flow isabout 400 torr-Liter/sec. The available pumping systemfor the diode laser spectrometer (6t' diffusion pump withrnechanicar backing pump) has a rnaximurn throughput of onry4 torr-liter/sec. Thus, the valve is pulsed at about 20Hz with 400 ps long pulses yielding a Lt duty cycle.The important criteria is whether or not the endstream endobj 401 0 obj 1307 endobj 402 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 403 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj397 Do Q endstream endobj 404 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj397 397 0 R >> /Subtype 400 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 402 0 R 403 0 R 398 0 R ] >> endobj 405 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 36660 >> stream P8m""v_1TD.`"&I$ Ĝ2C$Bꁓtq_ҿtC އP2><#1E}p(z!QkªCu]  Sa\8P0PÄP>P(x*8EPxESQC>CB(xOU |,:༡up(|nkrAQC C(w ](|xrv~w^KRRMf!g:K 4 90%[livBu&mj DT9Ao@FFȟO_ 0@_^M G7% ;D6!-?('H44'l>ŒԝOKtHQCYPE&JBT8LZ D;Pdv?M쉐ӧZ &iϑr*u20Oz j_ Zwqh1dr a?_^ ƞm͆V۽ C3)`CNeO%8h;4C0vFj$DzwTU[WCîr Vfc%C INӿEC[uӽokwvMA/P"a2l}J#}#X&׾˲WEm0( bP!aiVTڴyd@+D6)q*Atva5uתk `?Ol' -:Fk& NY .^'nx0^V\i;w֟y iӵ ;b_)_ ӆqIb/0gOQ d[' tfE.DvZd^ ضAŧ o{NRhx`D"B>6 1a4M_u}|:>/a~V\#'OҼDD4d8 $!cspKqp)pX5E1ivݦ""""!^X ˠV %G2/ B d jݭD'm=DZ}58A OR5{DXM8a+ASs@J*Q!Av"*@ޢ" MnB;ȣCM0>8L0[ 8GpԡA@'iDDXM>0a((@`P?!w‡\8PCJ>P])%x̋ma^Lt;.IhOg_RB5/öM3wtf)B0_H$4AAjg'ar19 (=%ݤ/uuT8mKr7n:c #֭m8!k+DS^ɞi-r#ض6L5{{k7OQ4)8oAkL*r@=v:A[\V6/[i w鳭v 2>`jd`tKC;CiҰW֟Ɲ|aC9a "RA? 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<636E2C20> Tj 1 0 0 1 468.96 91.20 Tm <616E6420> Tj 1 0 0 1 497.52 91.44 Tm <70756C7365> Tj ET endstream endobj 407 0 obj 10725 endobj 408 0 obj << /Length 409 0 R >> stream 6:pressure in the vacuum ehanber is sufficiently 10w toavoid rrshockingtt the expansion. This is accompanied by awarning of the species in the expansion to near roomtemperature, a phenonenon which is not observed with theslit jet under tlpical expansion conditions.Operating the valve in a pulsed manner hassignificant advantages. prinariry, since the varve isonly open for a short period of tirne (typicarly aboutAt=4OO prsec), the absorption signal lies at f/ e*At), orabout r-2 krlz- Moving the signar from near DC to r- krrzpushes this signal above the nain sources of noise on thelasers, such as slow fluctuations in the rR power.The pursed slit varve used in these studies wasdeveloped in our raboratory and has been discussed indetail in previous pubrications15. A schematic of thevalve is shown in Figure 2.2o. The seal is made betweena viton o-ring stretched into a linear channer, and aknife edge stainless steel base plate. The actuar sritis formed by two aruminum half prates borted to thebotton of the stainless base prate. The valve is openedby momentum transfer from a preaccelerated ferrornagneticplug to a rod on which the viton seal is attached. Theviton is then pulred off the knife edge and returned by acompressed spring. A pair of leaf springs attached tothe viton horder maintain its orientation relative to thesrit. slit geometries of 75 or 1oo pn by 4 cn, and pulse endstream endobj 409 0 obj 1391 endobj 410 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 411 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj405 Do Q endstream endobj 412 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj405 405 0 R >> /Subtype 408 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 410 0 R 411 0 R 406 0 R ] >> endobj 413 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 41760 >> stream iр<#4E2#j #N>a2>E 3iB2Ȏ0Fs#62>G!@ǢD|DjFq\R8+yp`?'/" aQA8ĥ"8d"""J0T~H$97)ʲ;<2戎t]3#8s78FD<68xDC(92d\2b>qDĭ#h!Ktc##ѯ*0Ida\COdq d|"> @\2aPdTxn'ct+)\\"!+C$a}W]D =Vz[{(z##E:"9BD).8~ "?e!u+(Bar:ՊE:X?cT;ASP"Q(tGP@@/R~D쎋5]:: \"??~WG˯B88"?8 ~*Tk_GPA(1/<]|}cq"?qoq">GXGኄ: ?B< X[Pq.up׮z(vGV;(pDDupYC jCO~GwvP_tquF.C,(* P@@)y0GJIRSS;%B;>s"ij۱8!ݳˢ+쾱&J´Uھ=a<P|B)?H8N:[H*GWT_VmUj; !GC?:.5.C#U˨CE8"? 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The actual seal is made between aViton o-ring and a raised knife edge at thebottorn of the va1ve. Just above this is acompressed spring which is responsible forclosing the va1ue. The valve is opened viamomentum transfer fron a preaccelaratedferromagnetic plug to the rod connecteo tothe o-ring seal. Three uorn gears labeledD, L and S for delay, pulse length andspring tension respectively are connected tofeedthroughs to allow external adjustnent ofthese parameters. 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<657870616E64696E6720> Tj 1 0 0 1 309.84 327.36 Tm <6761732E20> Tj 1 0 0 1 353.28 325.92 Tm <45697468657220> Tj 1 0 0 1 403.92 324.96 Tm <636F6C6420> Tj 1 0 0 1 439.68 324.48 Tm <7761746572> Tj 1.68 Tc 1 0 0 1 131.28 306.00 Tm <2835276320> Tj 1 0 0 1 165.12 306.96 Tm <3D20> Tj 1 0 0 1 180.72 304.56 Tm <32373820> Tj 1 0 0 1 208.80 304.32 Tm <49282920> Tj 1 0 0 1 230.64 303.84 Tm <6F7220> Tj 1 0 0 1 252.24 303.60 Tm <636F6F6C656420> Tj 1 0 0 1 302.64 302.64 Tm <657468616E6F6C20> Tj 1 0 0 1 362.16 302.16 Tm <282D6F6F2E6320> Tj 1 0 0 1 410.40 302.88 Tm <3D20> Tj 1 0 0 1 427.20 300.48 Tm <32723320> Tj 1 0 0 1 454.08 300.00 Tm <4B2920> Tj 1 0 0 1 476.40 299.52 Tm <697320> Tj 1 0 0 1 497.52 299.04 Tm <75736564> Tj 1.44 Tc 1 0 0 1 129.12 281.52 Tm <666F7220> Tj 1 0 0 1 157.68 281.28 Tm <7468697320> Tj 1 0 0 1 193.68 281.28 Tm <707572706F73652E> Tj 1.44 Tc 1 0 0 1 164.40 257.52 Tm <54686520> Tj 1 0 0 1 193.68 257.04 Tm <736F6C656E6F696420> Tj 1 0 0 1 258.72 256.08 Tm <726571756972657320> Tj 1 0 0 1 323.28 254.88 Tm <617070726F78696D6174656C7920> Tj 1 0 0 1 424.80 252.96 Tm <334F4F20> Tj 1 0 0 1 452.88 252.72 Tm <562C20> Tj 1 0 0 1 475.20 252.00 Tm <343020> Tj 1 0 0 1 496.32 251.76 Tm <41726E70> Tj 1.44 Tc 1 0 0 1 127.68 234.48 Tm <656C656374726963617220> Tj 1 0 0 1 207.12 233.76 Tm <70757273657320> Tj 1 0 0 1 257.76 232.32 Tm <746F20> Tj 1 0 0 1 279.60 231.84 Tm <636F6D7072657465727920> Tj 1 0 0 1 358.80 230.40 Tm <6F70656E20> Tj 1 0 0 1 394.80 229.68 Tm <74686520> Tj 1 0 0 1 423.36 229.44 Tm <76617276652E20> Tj 1 0 0 1 481.68 228.00 Tm <5468657365> Tj 1.20 Tc 1 0 0 1 127.20 210.24 Tm <61726520> Tj 1 0 0 1 156.00 210.24 Tm <70726F766964656420> Tj 1 0 0 1 221.04 208.80 Tm <627920> Tj 1 0 0 1 243.12 208.32 Tm <6120> Tj 1 0 0 1 257.28 208.08 Tm <686F6D6520> Tj 1 0 0 1 293.28 207.36 Tm <627569727420> Tj 1 0 0 1 336.48 206.64 Tm <64726976657220> Tj 1 0 0 1 387.36 205.68 Tm <6369726375697420> Tj 1 0 0 1 444.96 204.48 Tm <626173656420> Tj 1 0 0 1 488.88 204.00 Tm <6F6E> Tj 1.20 Tc 1 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obj << /Length 425 0 R >> stream 58lengths of 400-5oo psec are used for arr studies expectthe NeDCl. Efficient production of this especiarlyweakry bound species requires higher backing pressure andan associated reduction in the purse length to 3oo 350psec in order to ninimize the gas road. Feedthroughs,which connect with worn gears inside the varve per-rnit thepulse length, dS werl as the delay and spring tension, tobe adjusted whire the varve is operating. The turn-onand turn-off tirnes for the gas pulses are approxirnatery50 psecr dS can be seen in Figure 2.L6.Two pairs of r/4" hores drilred through the body ofthe valve wilr accept either tube heaters or pipe threadfittings so that a coorant can be circurated through thevalve. The production of weakly bound van der l{aalscomplexes such as NeDCI1 is enhanced greatly byprecooling the expanding gas. Either cold water(5'c = 278 I() or cooled ethanol (-oo.c = 2r3 K) is usedfor this purpose.The solenoid requires approximately 3OO V, 40 Arnpelectricar purses to compretery open the varve. Theseare provided by a home buirt driver circuit based ondumping a large arnount of charge stored on an g4o ttfcapacitor through the pulsed valve sorenoid. siliconcontror'1ed rectifiers, triggered by a pulse frorn thecomputer, are used to i-nitiate the charge flow. Thiscircuit produces a current pulse of about 2oo ssec in endstream endobj 425 0 obj 1340 endobj 426 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 427 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj421 Do Q endstream endobj 428 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj421 421 0 R >> /Subtype 424 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 426 0 R 427 0 R 422 0 R ] >> endobj 429 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 36874 >> stream ɨfd\5K!p$.0NMG"GHE#! v_#p;"dL   |!#:Āl.F(d|ͣDTaÔ9VHr܈9!8c9Cr1!Qa2:/';rC㐃rT9A S)9ϐ;#9^Pyܧ(r7"X-C4@>q4F>yDgѸ3yGQc+DDDD _D^% DF-GM2Mr x+)6#aι)D8R\ r8v,3c8#y#d`B9 L!Dtdt]Tg|(p@#tat("90BcQ@nLr s qdpPEʀW$Adrx""""tGs#@#8DDDqF"""""DJ#^@Tl2 ;ᯉt$7W.GaGn..4C\0#BٟEւ< BDu xDuA:8躿|Xne!e#"uUqCZ#X@ 6E}ay>AB DžP R}7ytIaoU⎀A4]Kڸ,0%e);t it@ibN1Qt :míɪ*VF:?ZiBV3HĺBby:_Duk\p?@1*!0(|xxO!:T-Ur^TH3,ynUt&v\ .:vL)~ؙْɱv Go;$ nݦDgjvGY'BZM[PӰA丠g)#A-N AA Ȗ鱻XOth4"D!R*?iO4tm nJ|82+MRvTAihԍ_4 _l'I n>Kv!]qh>@02>Z[V]-tz}eQ"*:nA;|/$?+N8a aGH Zn'KUQrQUMnDD_eӠۆo]}i7^R^+`xA" uxOݥ_ڧ!Z{ (?\^mYJ_cvIm`]t܎}]l[_ӫzRI_2~]j:xl[4;{_;H }H}&$o ȃTa^nt7~:~9 `vj bX02sK;UFJ׽G /o};6N)\EXd!t|.'z$a] "hC=wcM687U /Z 00pӧj|ՅV]wDD2"l(@BBkM]HD3,&a;87 ӺJ""" 0 TaO4 űOlpՆC~$"""$!&A  NtoG/u`""S&"*i!liݯHDH̻ A!,&l*k4YB""&%"dLLBiAxׄJӑI@& jIDhAP08QD0%Z +&">k~cĤ6׻鎭#P P`'n oރZ*w&I>2-%lJ^݄A`DuBC@jlC /ah0D9i.Bb\rMv8xM0 Yr*c$MwO i. `wjmҰ]8iQ(G- ߧ OC 䦤K =ScmLxWԇ < _r~l^wwU5t8, i5ߧ 4ǥ]_YR|ժ ?C+)~kJEY 7pMV !H"?]iEzLzA{UB2x>Uӆ;$޽ّF(<"; i/eoZF\\wk$ Ni wTR3; z7A؇J{ d(PMaB"%Z`,Yí&N?FB;!.ӵiXb"*" aL*qɎp4i(e H*A!ؖxp5 xQo GVˬ:ߎ(@0ADuҶGX~XExR:hanYƋ!L",dIR;<"3+J7MBYm8aL'h>I˙A+\2R_&_a3b5o޽b֓0 ٩!oTBl&w;Ly#u"5^i6ŮІ8! !58E `Kiwô4aHr*`du_6Q<4?a0L hA␄V":Myc=.x@ȠV_=5WvPi0A `!Џ.0D.`h;W[XB/i9L p " ̆Jl#N"Ӈtv_5Ɵi5nϤܝ0 HT _7^j?Ib k٥ӒyЌ$,A}=]{VI^ڎ-97 mIB@w0uO!8$6DN2px`l5NA_W$Ih z~5ߏBt h !IAPWuyHSr`n-{M!{V" iN DO^. i|@EBFEoi[UP_QLPNW'&W AS*Zt"#B B d$jjAXDa8(kfn'/be1O#t`TTnnE^00vb""4-F w`PMxl\]ݜ5OmZ`":O' P@&TІUKDC4uA »aikdq` "AL M0-iTgA O؈ZZ9C & 2%U 3H@wgp3i„imՅVDDD]achrӚ2 !k}''taV" ":tA8": 0"1ZMN;5 R^{aػkWEd&CCbSP!>z!>{ud6PW¿!"QKuLnv&Y.[^ӳ u~.B kdQa+M0aV[ T7;H΂nr B9ͰD1Uڼ Tjw i D2ge*7ŧz;d`RTRdbav j{i_ Y !P nիL;}" lQԿ+""qD_x_]ha PC1 5Du2ۮڧdJA}B"E6 ӈh;A0DBED4 ՌҪP)݄>i;v` A_pWmoví5lva}0A )@c% O]}t"9A5 F;ph< i @d)6 1>Ow>\HA 4 H@R!7ڥV* id-ܟ@ZoZlZL 4 dZֺ !Kzm;\0[neqDApX&*w! x`m8dZ!"!MB'"ZM:A+C S1h80{]{"?B"""DŴi =gh !/ iyDE0M45[[Zn8aSh8P Tp݂MlXAC,ePl&=4ZVdwXӻ)aF!@#HԺn"=H~x"}GSC&oPXP#NߠDza7 ڧ a jCFƝHUؑpb\"GuGf^+ӆA;+k|;]qAV}gjw-]A-C恂 )` ̂waBІkA͆yr: @ФA)Q1R,~dX?p¿jDrAA H4">Dl?q 43gP)\$Rgyji>ބCL!"VD+!6qubdHwAA20dՇWęr Y=4Ji=Rw0IN NӶޝ ͑5uDg LD2GEP=?:];TAY5Aa0x @BGA:?ﾓvNӻ/ NPpaApB;%:t /1VM/ +e;oU)ݪl]iń " BPR'ү_C!^ Ƀ:#eBC!`7mA Lɬ} w}kKnb:!9V:kD y#_~ V}4_OO!x&`DNly/ 6qvtKO V(0Jom4pyBeMN[3z#G`\*A Gr,S JiDnw݂446i_?::_U[A>a !}p׃ [>P_z}`{GO>l_lxk)%ސaw@O R _E:lTlruߪ#}ID_/! @}":vݽMniZ޴AK0xq tW4 &ݤ"ذ5ajfnND_i'n[A "a2` H3 j^  }U{4GA궰OJHnQb"8Y3a5ӸhE!^TJPKvbCwG0t"  d+M68K͉v3~}}~FwxOtDAN ZQ8bO{V'<8HDDDC8r224d:^m*icDƩ2u֪iȑab! 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The gas urixtures found toprovide maximum signals for each of the comprexes studiedare presented in each chapter.AII gas lines are stainless steel and only VCR typefittings are used for connections. Needle valves and apressure regurator are used to contror the stagnationpressure. The exception to this is when studying DCIcomplexes,' the regulator is bypassed and only a needlevalve is used to regurate the backing pressure in orderto rninirnize the DcI Ioss. Additionarly, the Dcr studiesreguire seasoning of the gas lines with DF to dispraceany hydrogen containing molecures with those containingdeuterium. DF is chosen since we can easiry synthesizeDF by mixing eximer laser grade F, with an excess of D2 inour rnixing tanks. The DF is then separated from theresidual De by freezing it out in a liquid N, trap.Deuteration of the gas lines and rnixing tank ismaintained by arways keeping them above atmosphericPressure. ..l endstream endobj 433 0 obj 1301 endobj 434 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 435 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj429 Do Q endstream endobj 436 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj429 429 0 R >> /Subtype 432 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 434 0 R 435 0 R 430 0 R ] >> endobj 437 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 34334 >> stream S?2Pr ̀c o,~o#51E9 u ^cS P2D2s Ucg!cJ8P2= ݄S#QD2)ՆGEsC 4jaBEPu B#8?|*4lUeXpC 2ceuUՇ 88dzC7@_a ԏؐ y iO,@f"dPP#uc@u>g }d27w˨H~P2rPj VNPb (pX@Eq#!"? zy k*݂ w/ ]VC Ec,!`Xc;! #1qP">6*G">8ߎ"!5!谲<@5o9~ACQpD2Cd2v0\d2c:f0u i:ˬCXh!XDupPd`|!G:RP=k2,~/a!C 2mw `|zF"F!  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~"1^^hizajMl ~@0"! ;H4V5[={}~m}p*3IM[V5/m 2]< IDG]A}F +h~}^1d.-+m(MAB9I L5Qlk:X~dt 5mGUdAN:Ms |0P/XT=>@uQi i4aV^R{_ڿMDAK,0^M&R A/șCItpLFACcU|?܄rWk§h0P44&Ǽ?p" V 'v ?`´C=j, ?("R1E-v!*!ô׫X[EԵ¨ iY Qft _Wƃ ,S"ilrru "֛Q0Pvw@ a^8-; BpPlpeĆPv"&'5 ;8Lj"4 0a0B Mh> άme +MDtGZt"=ka莵 :Du{;lv#% ʕ;l*e]%tv2u8r6g ˯(D3A a ^ߺS`DD< vBR6 \"a ڤ[θAtEA eXQ wh2, 6ȹD Y6u|y6֝'2>8&B!"n5j!۸avxDTQahRopdm}dp`K;*ot#'X@aNF) Aɩ6D];[\ %6JK2 \"4ILZ!I`zޟvEM8[8gR(IBfC$^馽7^ i d0`ޜo=7tBjL S՚d'vm^u|ˑmi `5S5V~zkّU}Ҿȳl|+jXB ma}Kh_7 H䢘wa]D Պ^Onal7AC`NJN4V^U|%{&s"[ada$u.0Walu{}PEzxMڶa0dR,"AۢjC<G:꜐^nӤԋ6ش !栄ZULCM&ذMOm^]wUWZzv鐜հ0@4DAԺZrL0K5 ad-GFtTD32| a ?cM?u0h#1gAr"$"  %Npv\$%:taDXA H v^׽N]m5%J%I hIb%>2 27vi:_ukA Qiz kz}kTDDvJ%AbjV}{_QVՔ#MvVN;MS"G^2mSLPN¶O}u B d\M4P1pf^ڂIb"zla80);mRm2 _*$ih2;A4; b!D0Zu E' xf=.ՇaB2?T_jcvk4cOF=T[:? > stream BT 3 Tr 1.20 Tc /F3 12.0 Tf 1 0 0 1 158.64 689.52 Tm <416C7220> Tj 1 0 0 1 188.16 689.04 Tm <7261726520> Tj 1 0 0 1 223.92 689.28 Tm <676173657320> Tj 1 0 0 1 267.12 687.84 Tm <7573656420> Tj 1 0 0 1 303.84 687.12 Tm <696E20> Tj 1 0 0 1 324.72 686.88 Tm <74686520> Tj 1 0 0 1 353.52 686.40 Tm <657870616E73696F6E7320> Tj 1 0 0 1 432.96 684.96 Tm <61726520> Tj 1 0 0 1 461.52 684.48 Tm <7573656420> Tj 1 0 0 1 498.24 684.00 Tm <6173> Tj 1.92 Tc 1 0 0 1 122.16 666.96 Tm <7075726368617365643B20> Tj 1 0 0 1 202.56 664.56 Tm <692E652E20> Tj 1 0 0 1 237.36 664.08 Tm <417220> Tj 1 0 0 1 261.60 664.56 Tm <2839392E3939357420> Tj 1 0 0 1 323.76 663.60 Tm <707572697479292C20> Tj 1 0 0 1 388.56 661.68 Tm <4E6520> Tj 1 0 0 1 412.80 662.16 Tm <2837357420> Tj 1 0 0 1 446.40 660.96 Tm <4E652C20> Tj 1 0 0 1 477.84 660.24 Tm <32352A20> Tj 1 0 0 1 504.24 660.00 Tm <4865292C> Tj 1.44 Tc 1 0 0 1 121.92 642.24 Tm <616E6420> Tj 1 0 0 1 150.48 641.76 Tm <486520> Tj 1 0 0 1 174.72 642.00 Tm <2839392E3939357420> Tj 1 0 0 1 237.12 641.04 Tm <707572697479292E20> Tj 1 0 0 1 309.12 639.12 Tm <54686520> Tj 1 0 0 1 337.92 639.36 Tm <677261646520> Tj 1 0 0 1 381.36 638.16 Tm <6F6620> Tj 1 0 0 1 402.48 637.68 Tm 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510.72 588.48 Tm <616E64> Tj 1.20 Tc 1 0 0 1 120.72 570.96 Tm <44637220> Tj 1 0 0 1 151.68 570.96 Tm <2839397420> Tj 1 0 0 1 186.48 569.52 Tm <69736F746F70696320> Tj 1 0 0 1 250.32 569.28 Tm <7075726974792920> Tj 1 0 0 1 308.16 567.36 Tm <61726520> Tj 1 0 0 1 337.44 566.88 Tm <667265657A652D70756D702D74686177656420> Tj 1 0 0 1 473.76 564.72 Tm <6E756C7469707265> Tj 1.20 Tc 1 0 0 1 120.24 547.20 Tm <74696D657320> Tj 1 0 0 1 163.68 546.48 Tm <746F20> Tj 1 0 0 1 185.52 546.00 Tm <72656D6F766520> Tj 1 0 0 1 235.44 545.28 Tm <766F6C6174696C6520> Tj 1 0 0 1 300.72 544.08 Tm <636F6E74616D696E616E74732E> Tj 1.44 Tc /F3 11.0 Tf 1 0 0 1 244.56 497.52 Tm <4C696E6520> Tj 1 0 0 1 279.84 497.04 Tm <576964746820> Tj 1 0 0 1 322.80 496.08 Tm <4D6561737572656D656E7473> Tj 1.44 Tc 1 0 0 1 155.28 450.96 Tm <726E66726172656420> Tj 1 0 0 1 219.84 450.00 Tm <65786369746174696F6E20> Tj 1 0 0 1 299.28 448.80 Tm <6F6620> Tj 1 0 0 1 320.88 448.32 Tm <44637220> Tj 1 0 0 1 349.44 447.84 Tm <6F7220> Tj 1 0 0 1 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<636F6E736964657261626C7920> Tj 1 0 0 1 212.16 378.24 Tm <6C617267657220> Tj 1 0 0 1 262.08 377.52 Tm <7468616E20> Tj 1 0 0 1 298.08 376.80 Tm <74686520> Tj 1 0 0 1 326.88 376.32 Tm <62696E64696E6720> Tj 1 0 0 1 384.72 375.60 Tm <656E6572677920> Tj 1 0 0 1 436.08 374.64 Tm <666F7220> Tj 1 0 0 1 464.40 374.16 Tm <7468657365> Tj 1.44 Tc 1 0 0 1 117.36 355.92 Tm <636F6D706C6578657320> Tj 1 0 0 1 189.84 354.96 Tm <6F6620> Tj 1 0 0 1 211.20 354.72 Tm <6265747765656E20> Tj 1 0 0 1 270.00 353.76 Tm <316F6F20> Tj 1 0 0 1 312.72 353.04 Tm <356F6F20> Tj 1 0 0 1 341.28 352.56 Tm <636D2D312E20> Tj 1 0 0 1 385.68 351.84 Tm <6F6620> Tj 1 0 0 1 408.24 351.60 Tm <696E74657265737420> Tj 1 0 0 1 473.52 350.40 Tm <697320> Tj 1 0 0 1 494.64 350.16 Tm <746865> Tj 1.44 Tc 1 0 0 1 116.88 332.16 Tm <74696D6520> Tj 1 0 0 1 153.36 331.68 Tm <736361726520> Tj 1 0 0 1 196.80 331.20 Tm <726571756972656420> Tj 1 0 0 1 261.60 330.00 Tm <746F20> Tj 1 0 0 1 283.44 329.52 Tm <72656469737472696275746520> Tj 1 0 0 1 376.80 328.32 Tm <74686520> Tj 1 0 0 1 405.36 327.84 Tm <482844296372> Tj 1.44 Tc 1 0 0 1 116.16 308.16 Tm <766962726174696F6E617220> Tj 1 0 0 1 203.52 306.96 Tm <656E6572677920> Tj 1 0 0 1 254.88 306.00 Tm <696E746F20> Tj 1 0 0 1 289.92 305.52 Tm <74686520> Tj 1 0 0 1 318.48 305.28 Tm <76616E20> Tj 1 0 0 1 347.52 304.56 Tm <64657220> Tj 1 0 0 1 376.08 304.32 Tm <776161727320> Tj 1 0 0 1 419.52 303.60 Tm <626F6E642E20> Tj 1 0 0 1 470.16 302.64 Tm <417320> Tj 1 0 0 1 492.48 302.16 Tm <746865> Tj 1.44 Tc 1 0 0 1 116.64 283.68 Tm <6C69666574696E6520> Tj 1 0 0 1 181.44 282.96 Tm <6F6620> Tj 1 0 0 1 203.28 282.72 Tm <6120> Tj 1 0 0 1 217.68 282.48 Tm <636F6D706C657820> Tj 1 0 0 1 276.00 281.52 Tm <697320> Tj 1 0 0 1 297.12 281.28 Tm <726564756365642C20> Tj 1 0 0 1 361.68 280.32 Tm <74686520> Tj 1 0 0 1 390.72 279.84 Tm <636F72726573706F6E64696E67> Tj 1.44 Tc 1 0 0 1 115.92 259.68 Tm <6162736F727074696F6E20> Tj 1 0 0 1 196.08 258.48 Tm <72696E6520> Tj 1 0 0 1 231.36 258.24 Tm <776964746820> Tj 1 0 0 1 274.56 257.52 Tm <77696C7220> Tj 1 0 0 1 310.80 257.04 Tm <626520> Tj 1 0 0 1 333.12 256.56 Tm <696E637265617365642E20> Tj 1 0 0 1 419.04 255.12 Tm <54686520> Tj 1 0 0 1 448.32 254.64 Tm <6162697269747920> Tj 1 0 0 1 506.16 253.68 Tm <746F> Tj 1.44 Tc 1 0 0 1 115.68 235.68 Tm <61636375726174656C7920> Tj 1 0 0 1 194.88 234.48 Tm <6D65617375726520> Tj 1 0 0 1 252.96 233.76 Tm <74686520> Tj 1 0 0 1 282.48 233.28 Tm <696E63726561736520> Tj 1 0 0 1 347.28 232.32 Tm <696E20> Tj 1 0 0 1 368.88 232.08 Tm <6C696E6520> Tj 1 0 0 1 404.16 231.36 Tm <776964746820> Tj 1 0 0 1 447.84 230.64 Tm <64756520> Tj 1 0 0 1 477.12 230.16 Tm <746F> Tj 1.44 Tc 1 0 0 1 114.96 212.64 Tm <707265646973736F63696174696F6E20> Tj 1 0 0 1 230.88 210.24 Tm <62726F6164656E696E6720> Tj 1 0 0 1 310.56 209.04 Tm <726567756972657320> Tj 1 0 0 1 375.36 207.84 Tm <6120> Tj 1 0 0 1 389.76 207.60 Tm <6B6E6F77726564676520> Tj 1 0 0 1 462.24 206.64 Tm <6F6620> Tj 1 0 0 1 484.08 206.16 Tm <6F74686572> Tj 1.44 Tc 1 0 0 1 115.20 187.92 Tm <736F757263657320> Tj 1 0 0 1 173.04 187.20 Tm <6F6620> Tj 1 0 0 1 195.12 186.72 Tm <6C696E6520> Tj 1 0 0 1 230.40 186.48 Tm <776964746820> Tj 1 0 0 1 273.84 185.76 Tm <62726F6164656E696E672E> Tj 1.20 Tc 1 0 0 1 150.72 163.44 Tm <54686520> Tj 1 0 0 1 179.52 163.20 Tm <726E6F737420> Tj 1 0 0 1 216.72 162.48 Tm <696E72706F7274616E7420> Tj 1 0 0 1 288.24 161.76 Tm <736F7572636520> Tj 1 0 0 1 338.64 160.80 Tm <6F6620> Tj 1 0 0 1 360.00 160.56 Tm <62726F6164656E696E6720> Tj 1 0 0 1 440.64 159.12 Tm <696E20> Tj 1 0 0 1 461.52 158.64 Tm <74686520> Tj 1 0 0 1 490.56 158.16 Tm <64696F6465> Tj 1.44 Tc 1 0 0 1 114.72 140.16 Tm <7370656374726F6D6574657220> Tj 1 0 0 1 209.28 138.72 Tm <697320> Tj 1 0 0 1 230.88 138.48 Tm <6672657175656E637920> Tj 1 0 0 1 302.16 137.28 Tm <6E6F69736520> Tj 1 0 0 1 347.28 134.64 Tm <7434392831302920> Tj 1 0 0 1 402.72 135.84 Tm <746674697A6C2E20> Tj 1 0 0 1 453.84 134.88 Tm <54686520> Tj 1 0 0 1 483.60 134.40 Tm <6C61726765> Tj 1.20 Tc 1 0 0 1 113.76 116.16 Tm <756E6365727461696E747920> Tj 1 0 0 1 201.60 114.96 Tm <696E20> Tj 1 0 0 1 222.48 114.72 Tm <74686520> Tj 1 0 0 1 252.24 114.24 Tm <6672657175656E637920> Tj 1 0 0 1 323.52 113.04 Tm <6E6F69736520> Tj 1 0 0 1 366.96 112.56 Tm <726976616C7320> Tj 1 0 0 1 417.36 111.60 Tm <74686520> Tj 1 0 0 1 446.64 111.12 Tm <6578706563746564> Tj 1.44 Tc 1 0 0 1 113.76 91.92 Tm <636F6E747269627574696F6E20> Tj 1 0 0 1 207.84 90.72 Tm <746F20> Tj 1 0 0 1 229.92 90.24 Tm <6C696E6520> Tj 1 0 0 1 265.20 90.00 Tm <776964746820> Tj 1 0 0 1 308.40 89.04 Tm <62726F6164656E696E6720> Tj 1 0 0 1 387.84 87.84 Tm <627920> Tj 1 0 0 1 409.68 88.32 Tm <707265646973736F63696174696F6E2C> Tj ET endstream endobj 439 0 obj 8839 endobj 440 0 obj << /Length 441 0 R >> stream Alr rare gases used in the expansions are used aspurchased; i.e. Ar (99.995t purity), Ne (75t Ne, 25* He),and He (99.995t purity). The grade of Ne is referred toas nfirst runt and is used since it is substantiarry ressexpensive than high purity Ne. Both HCI (99.9t pure) andDcr (99t isotopic purity) are freeze-pump-thawed nultipretimes to remove volatile contaminants. Line Width Measurements rnfrared excitation of Dcr or HCr within a van derwaals complex deposits approxinrately 2Loo or 2goo cm-1 ofenergy into the respective complex. This energy isconsiderably larger than the binding energy for thesecomplexes of between 1oo 5oo cm-1. of interest is thetime scare required to redistribute the H(D)crvibrationar energy into the van der waars bond. As thelifetine of a complex is reduced, the correspondingabsorption rine width wilr be increased. The abirity toaccurately measure the increase in line width due topredissociation broadening reguires a knowredge of othersources of line width broadening.The rnost inrportant source of broadening in the diodespectrometer is frequency noise t49(10) tftizl. 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<62726F6164656E696E6720> Tj 1 0 0 1 356.40 472.80 Tm <68617320> Tj 1 0 0 1 385.44 472.08 Tm <6265656E20> Tj 1 0 0 1 421.68 472.08 Tm <70726573656E74656420> Tj 1 0 0 1 494.40 469.92 Tm <6279> Tj 1.44 Tc 1 0 0 1 110.64 453.84 Tm <4C6F76656A6F797A20> Tj 1 0 0 1 172.80 452.64 Tm <616E6420> Tj 1 0 0 1 201.36 452.16 Tm <77696C6C20> Tj 1 0 0 1 238.08 451.20 Tm <6F6E727920> Tj 1 0 0 1 273.84 450.48 Tm <626520> Tj 1 0 0 1 295.44 450.00 Tm <6272696566727920> Tj 1 0 0 1 353.28 448.80 Tm <64697363757373656420> Tj 1 0 0 1 425.52 447.12 Tm <686572652E20> Tj 1 0 0 1 476.64 446.16 Tm <546865> Tj 1.44 Tc 1 0 0 1 109.92 429.60 Tm <636F6E747269627574696F6E7320> Tj 1 0 0 1 211.44 427.44 Tm <746F20> Tj 1 0 0 1 233.04 426.96 Tm <74686520> Tj 1 0 0 1 262.32 426.48 Tm <6C696E6520> Tj 1 0 0 1 297.36 425.76 Tm <776964746820> Tj 1 0 0 1 341.28 424.80 Tm <64756520> Tj 1 0 0 1 370.32 424.08 Tm <746F20> Tj 1 0 0 1 391.68 424.32 Tm <7072657373757265> Tj 1.20 Tc 1 0 0 1 109.20 405.60 Tm <62726F6164656E696E6720> Tj 1 0 0 1 189.12 403.92 Tm <616E6420> Tj 1 0 0 1 218.16 403.20 Tm <7472616E73697420> Tj 1 0 0 1 276.00 402.00 Tm <74696D6520> Tj 1 0 0 1 311.52 401.28 Tm <62726F6164656E696E6720> Tj 1 0 0 1 391.44 399.60 Tm <61726520> Tj 1 0 0 1 420.48 399.12 Tm <657870656374656420> Tj 1 0 0 1 486.00 397.68 Tm <746F20> Tj 1 0 0 1 507.36 397.20 Tm <6265> Tj 1.68 Tc 1 0 0 1 108.96 381.60 Tm <6E65676C696769626C6520> Tj 1 0 0 1 189.36 379.92 Tm <666F7220> Tj 1 0 0 1 217.68 379.44 Tm <616C7220> Tj 1 0 0 1 246.48 378.72 Tm <657870616E73696F6E20> Tj 1 0 0 1 318.72 377.52 Tm <636F6E646974696F6E7320> Tj 1 0 0 1 397.92 375.84 Tm <7769746820> Tj 1 0 0 1 434.88 375.36 Tm <3C316F6F6F20> Tj 1 0 0 1 478.08 373.92 Tm <746F7272> Tj 1.44 Tc 1 0 0 1 108.24 358.08 Tm <6261636B696E6720> Tj 1 0 0 1 166.08 357.60 Tm <7072657373757265732E20> Tj 1 0 0 1 252.96 354.96 Tm <486F77657665722C20> Tj 1 0 0 1 318.48 353.76 Tm <446F70706C657220> Tj 1 0 0 1 375.84 352.56 Tm <62726F6164656E696E6720> Tj 1 0 0 1 456.72 350.64 Tm <6973> Tj 1.44 Tc 1 0 0 1 108.00 334.08 Tm <6F6273657276656420> Tj 1 0 0 1 173.76 332.64 Tm <696E20> Tj 1 0 0 1 194.64 332.16 Tm <74686520> Tj 1 0 0 1 224.16 331.68 Tm <736C697420> Tj 1 0 0 1 260.40 332.16 Tm <6A65742C20> Tj 1 0 0 1 296.16 330.24 Tm <617320> Tj 1 0 0 1 317.76 329.76 Tm <65766964656E63656420> Tj 1 0 0 1 389.76 328.32 Tm <627920> Tj 1 0 0 1 412.08 327.84 Tm <323920> Tj 1 0 0 1 434.88 327.12 Tm <4E487A20> Tj 1 0 0 1 462.96 326.64 Tm <6C696E65> Tj 1.20 Tc 1 0 0 1 107.04 310.08 Tm <77696474687320> Tj 1 0 0 1 158.88 308.88 Tm <666F7220> Tj 1 0 0 1 186.48 308.40 Tm <417248437220> Tj 1 0 0 1 230.64 307.44 Tm <617420> Tj 1 0 0 1 252.96 306.96 Tm <722D6F20> Tj 1 0 0 1 273.84 306.48 Tm <4B2E20> Tj 1 0 0 1 302.88 306.00 Tm <446F70706C657220> Tj 1 0 0 1 360.24 304.80 Tm <62726F6164656E696E6720> Tj 1 0 0 1 441.12 303.12 Tm <696E63726561736573> Tj 1.44 Tc 1 0 0 1 106.80 286.08 Tm <74686520> Tj 1 0 0 1 135.60 285.36 Tm <68657465726F67656E656F757320> Tj 1 0 0 1 237.84 283.44 Tm <6C696E6520> Tj 1 0 0 1 273.12 282.96 Tm <77696474682C20> Tj 1 0 0 1 324.00 281.76 Tm <746875732C20> Tj 1 0 0 1 367.20 280.80 Tm <74686520> Tj 1 0 0 1 396.24 280.08 Tm <6566666563747320> Tj 1 0 0 1 454.56 278.88 Tm <6F66> Tj 1.20 Tc 1 0 0 1 106.56 261.84 Tm <446F707072657220> Tj 1 0 0 1 163.92 260.64 Tm <62726F6164656E696E6720> Tj 1 0 0 1 244.08 259.20 Tm <61726520> Tj 1 0 0 1 272.64 258.72 Tm <6D616E6966657374656420> Tj 1 0 0 1 352.80 256.80 Tm <696E20> Tj 1 0 0 1 374.16 256.56 Tm <616E20> Tj 1 0 0 1 396.48 256.08 Tm <696E63726561736564> Tj 1.44 Tc 1 0 0 1 105.60 237.60 Tm <476175737369616E20> Tj 1 0 0 1 171.12 236.40 Tm <636F6D706F6E656E7420> Tj 1 0 0 1 243.36 234.96 Tm <746F20> Tj 1 0 0 1 265.20 234.72 Tm <74686520> Tj 1 0 0 1 294.24 234.00 Tm <6C696E6520> Tj 1 0 0 1 330.48 233.28 Tm <73686170652E20> Tj 1 0 0 1 387.84 231.84 Tm <5468697320> Tj 1 0 0 1 424.56 231.12 Tm <636F6E747269627574696F6E> Tj 1.20 Tc 1 0 0 1 105.84 213.36 Tm <697320> Tj 1 0 0 1 126.96 213.60 Tm <6775616E74696669656420> Tj 1 0 0 1 206.64 211.44 Tm <627920> Tj 1 0 0 1 228.72 211.20 Tm <7363616E6E696E6720> Tj 1 0 0 1 293.52 210.00 Tm <6F76657220> Tj 1 0 0 1 329.76 209.04 Tm <6162736F727074696F6E7320> Tj 1 0 0 1 416.40 207.12 Tm <64756520> Tj 1 0 0 1 445.68 206.40 Tm <746F20> Tj 1 0 0 1 467.52 205.92 Tm <65695F74686572> Tj 1.44 Tc 1 0 0 1 105.12 189.60 Tm <737461626C6520> Tj 1 0 0 1 155.04 188.40 Tm <6D6F6C6563756C657320> Tj 1 0 0 1 230.16 187.68 Tm <2865672E20> Tj 1 0 0 1 264.24 186.48 Tm <63486F20> Tj 1 0 0 1 290.16 186.00 Tm <6F7220> Tj 1 0 0 1 311.52 185.52 Tm <4843722920> Tj 1 0 0 1 348.00 184.80 Tm <6F7220> Tj 1 0 0 1 370.08 184.32 Tm <31306E6720> Tj 1 0 0 1 406.32 183.36 Tm <6C6976656420> Tj 1 0 0 1 449.04 182.40 Tm <76616E20> Tj 1 0 0 1 478.56 181.92 Tm <646572> Tj 1.68 Tc 1 0 0 1 103.92 165.84 Tm <776161727320> Tj 1 0 0 1 147.36 164.88 Tm <6E6F6C6563756C657320> Tj 1 0 0 1 222.48 164.16 Tm <2865672E20> Tj 1 0 0 1 255.84 162.72 Tm <417248436C2920> Tj 1 0 0 1 307.44 161.76 Tm <696E20> Tj 1 0 0 1 328.56 161.28 Tm <74686520> Tj 1 0 0 1 357.84 160.80 Tm <7372697420> Tj 1 0 0 1 394.08 161.28 Tm <6A65742E20> Tj 1 0 0 1 437.76 158.64 Tm <46696775726520> Tj 1 0 0 1 488.88 157.68 Tm <322E3272> Tj 1.44 Tc 1 0 0 1 104.16 141.84 Tm <73686F777320> Tj 1 0 0 1 147.36 140.88 Tm <6120> Tj 1 0 0 1 162.48 140.64 Tm <72696E6520> Tj 1 0 0 1 198.24 140.16 Tm <736861706520> Tj 1 0 0 1 242.16 139.20 Tm <66697420> Tj 1 0 0 1 270.24 138.72 Tm <746F20> Tj 1 0 0 1 292.08 138.24 Tm <6120> Tj 1 0 0 1 306.00 138.00 Tm <6E657468616E6520> Tj 1 0 0 1 364.32 135.36 Tm <5120> Tj 1 0 0 1 378.72 136.56 Tm <6272616E636820> Tj 1 0 0 1 429.84 135.12 Tm <7472616E736974696F6E2E> Tj 1.44 Tc 1 0 0 1 103.20 118.08 Tm <54686520> Tj 1 0 0 1 132.96 117.36 Tm <66697474656420> Tj 1 0 0 1 183.60 116.40 Tm <6C696E6520> Tj 1 0 0 1 219.60 115.92 Tm <736861706520> Tj 1 0 0 1 263.28 114.72 Tm <697320> Tj 1 0 0 1 284.16 114.48 Tm <476175737369616E20> Tj 1 0 0 1 348.96 113.28 Tm <7769746820> Tj 1 0 0 1 385.92 112.32 Tm <6120> Tj 1 0 0 1 400.32 112.08 Tm <465746494D20> Tj 1 0 0 1 436.80 111.12 Tm <6F6620> Tj 1 0 0 1 459.12 110.64 Tm <36332E3828722D3429> Tj 1.44 Tc 1 0 0 1 102.48 93.60 Tm <4D6C6C7A2E20> Tj 1 0 0 1 146.40 92.64 Tm <54686520> Tj 1 0 0 1 175.68 92.16 Tm <6C696E6520> Tj 1 0 0 1 211.92 91.44 Tm <73686170657320> Tj 1 0 0 1 262.32 90.48 Tm <6F6620> Tj 1 0 0 1 283.92 90.24 Tm <746865736520> Tj 1 0 0 1 327.60 89.28 Tm <737461626C6520> Tj 1 0 0 1 378.24 88.08 Tm <7370656369657320> Tj 1 0 0 1 436.80 86.64 Tm <696E20> Tj 1 0 0 1 457.92 86.16 Tm <74686520> Tj 1 0 0 1 487.44 87.12 Tm <6A6574> Tj ET endstream endobj 447 0 obj 9965 endobj 448 0 obj << /Length 449 0 R >> stream 7tand it is therefore very difficurt to quantify thissource of broadening with the diode raser spectrometer.All line width measurements made on the diode raser arepresented as rower linits to the vibrationalry excitedlifetines. Active frequency stabirization has beendemonstrated to reduce the line rvidth by 3-fo1d, whichshould improve these measurements.Accurate rine width neasurements are possible on thedifference frequency spectrometer. A detailed discussionof the sources of line broadening has been presented byLovejoyz and will onry be briefry discussed here. Thecontributions to the line width due to pressurebroadening and transit time broadening are expected to benegligible for alr expansion conditions with <1ooo torrbacking pressures. However, Doppler broadening isobserved in the slit jet, as evidenced by 29 NHz linewidths for ArHCr at r-o K. Doppler broadening increasesthe heterogeneous line width, thus, the effects ofDopprer broadening are manifested in an increasedGaussian component to the line shape. This contributionis guantified by scanning over absorptions due to ei_therstable molecules (eg. cHo or HCr) or 10ng lived van derwaars nolecules (eg. ArHCl) in the srit jet. Figure 2.2rshows a rine shape fit to a nethane Q branch transition.The fitted line shape is Gaussian with a FWFIM of 63.8(r-4)Mllz. The line shapes of these stable species in the jet endstream endobj 449 0 obj 1382 endobj 450 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 451 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj445 Do Q endstream endobj 452 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj445 445 0 R >> /Subtype 448 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 450 0 R 451 0 R 446 0 R ] >> endobj 453 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 16568 >> stream d@PSFv` "M"8PI(R8lH 9#(DH_# ""$jN p44ˁ2G b%,2@$ !@]@dG>M?(u>?uW\8Gp/WW]"xp>=C]u(?u_X#U^2@G] L@0J;_]+뢞AE=Å&ʼnEwUOUE,]~P">"(xCE_"W(x~P(Wuê8+T_u_PE_}wwWWYDZ?PC$!ߐ ` :d@am!ds1bdwx#1!(pVP%sPB(ALvGa-P͐9'2&Gq0L 2B#|& >?2B:#=d2Hx"OtG AA} ӈcH7dw*M-^_J I7PMfuz(xweuA#I,7yR +×CƸ*]:t#{65d0r?TG=W! { ġNcC .|(#AGHd?C DG߂#B7n$F/Z"?q#:Q ?C loG_hFM ~i ~^Lk_֋oމ<0izXB^WՐv"eAT%P[i~ml%][KUf t!^ U^x:_נ#Յ6d}! ץ J(֗du}/MWqi.)}p޴.TtDuJ*:(qUƆurJKZ- ! hARڮ['UZ%#§.{f'A „&fkl,;ވS ^*?j"?fA0Gb::Cc]C(p":0߲ҿ:?Pzd2# C0-<0T ]nBGJ@qQ{L8ai[XT]K0APpD5R0 p֛u".٠%u-d-l܄8(a`]Q@A 5- 7#f'4~ pؑɢt4 >[&{u$>> "_0]/V@fap@akr.-s3I>?NC!;`fA]P;"7;UV և];[ b,P8"?Pp߫n"tZkba1׫PPC/yq^@D~ >sEWCz k~YuxXd" ? n\/յ떈!N#;^_ɺQvL/ "?Dc/E3uږfmtGP.c'ӦGTkdGCOȾ֛kDžm?kYh躵OOa~׮Ö`O M ܳ|4 j 4Bp4dgz܁˳'UIwUG0~":0\3mkQW})fhi<G SŨ:;OWA&DiܡlnZ莺 ؇t? b.*Dd8!Dz>`o`@cN3{DuAuCA3V qv=YB SO|WŔEՙzTSTɌTC[[@'} ³P=CN{ݶZNڍ ֭޿Wu<?\@֟{ ]}gA?O:l7~k~i%YXu[ }?U~(=VHQEi=mT>ՠd g ['t4;tz_u;F96~~ڴKBA2?jvwk0NwiODaEl0dHFMV }i\kC00@"G& iڥEDE[%ŧڽuaj &Wа 4L&KM.b"""]58!AJGAzкU4;[0?G/VZiG(_莈E~/ ޸_m50nB=?U4MG@K^ yۡ~ xwB⮿~zG^3C!7R mG`w~YP7?Tn?٭t&F]0߃R(5MYgeO?YzaLJfA$M;^ _)b O$d%[n}85_.D\O"p!Cj*ДA\ h:qD´, ammG]Ԓ47Su^F@UK !VPEʁU?TT}]At z_Jc߯*#OX~-.tֈmkw᤭_zT Ӳqv8 v5R<4&3@B-0 5V Cn#{\idTDDqv{FnаZaȯk7qN""@ҧ$:}UpMЍ5OGRΠ \~ظohA j.QDDX_6dRֽ_Gl){D?j4>>D\3M C\* " Aau:խVl-R mCC &K GQ@cZ}8 o@DoGH0DY x5}m[hn{񿐣kbFl>ԏ>)'֡#]K8@uؿ"@Ye ^6A{Zo,f?K4G_~?!ow@OZt_4=:yu7d)5Ziw ve(5g˄`ֱ֛a,Q 4Ӣ1Wy u}:Bw[܋_Fmx`݈^~ڵ#\ QEGTh;knTG?%#T waVA*_}a6(i~V "K}쎽i%x1{l _?G^Wod u` /,4 0_æ/WCx#ou_ tiO^i\%i?^_j+Vua1,]|]w/Y˩g.ׇD3wt[*p0I~=,B_![Zvk#_Pw;B>⽿ZAu)k¨kA0{=>;q A>1î<\#?C`׍?[-wKO_ [u,AxtjHxgXX/]4ôj 4Y˃4Aqy;j|2 %~3eB􋨆zGڱ9wpD~8_l"6WcL"ȨkG>Fƈf5KJyNVÈ)g)K\9g ׃U$#! 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<746F692D6F63695F486366> Tj 1.68 Tc 1 0 0 1 219.36 76.08 Tm <7468616E20> Tj 1 0 0 1 255.12 75.36 Tm <4843492D4443492E> Tj ET endstream endobj 463 0 obj 6855 endobj 464 0 obj << /Length 465 0 R >> stream Voigt Line Shape Fits DCI.HCI HCI-DCI ATHCI .opf E-=## fi-'tr 11IJI'lT--+*f +ts'**' fi{t]IIt l-ror- 44.3(5.6)MHzfr.u = 30(3 )l'{Hz FLo, - I6.5(2.8)tr{Hzra., = 3o(3)1"'lHz 1.-- -u -i-- a-t l-lFEEF=#:i'tr3 Fror= <3.0lrlHzrr.,- 29{3)l'{Hz F1cra:-*-a-<+*N '' 'J-3oo -l5o o l5O 3ooFrequency (MHz)Figure z.22 A dernonstration of predissociationbroadening. The rower trace is due to ArHCIwhich is expected to have a very loncrvibrationally excited 1ifetine ii.. 'deterained to be >0.3 ES, which wouldcorrespond to a Lorentzian width of 500 Hz).The niddre trace is due to HCr vibrationarexcitation of Hct-DcI. This ]ine ;h;;" isbroader than that of ArHCr. but narro*.f thanthat HCl excitation of DCI-HCI. as wif:. Uediscussed in Chapter VI, this is au" 1" .significantly shorter tifetine toi-oci_Hcfthan HCI-DCI. endstream endobj 465 0 obj 805 endobj 466 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 467 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj461 Do Q endstream endobj 468 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj461 461 0 R >> /Subtype 464 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 466 0 R 467 0 R 462 0 R ] >> endobj 469 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 26418 >> stream ̈ QdGZd Fdx́PA3 h27P 2&2d 2ĺ_Z$u ^:j!20utaG/|s"PJuCppDz+UPC">@h(.j C# 8$*=iZ7-TV^#o A>W#G̓ Z+/1k1]֔S^$wFIp1J ^GL.0U`4J! q1:Q,pU ]Pf PxwC:M/wtq† !#*D(qǭ>GT"`/.à ?j^NV"?GT|*pC°ztS)OU"ƷnPG!CPGZ(|Z(">B)Wp 8AxXxR:(uDŽS%owmR[CL,4"j|)P|2: =TPu‡ rʣL -#r B!P`º2(2 S0D+a4#A2d1 Y qh{ B75 JqA|'{P &4 =tŲ/h=;$E.t{5t" "w ?OMյOa(k/zNޝ[{"2%DY j=;QA .2ȑDLP8ֵzT@SN_ Aи4'(t]Gۡ^t}}n_8(p~~}9ÿ}ouvtI''=WKCtaT.$TsP/GCdZl]VCD6n59 < XaSPAXE8Bjk;[XjdՂ ф#tA aEYJ/[ ` & `%-:`A ޚpa0[ 7.S1_z[P(u_(nzE4%ܦYDGivl9Њz_[J hAoZ hh}hH>3Q MXtwmrc3'"9]k+x/4id2|2 BxqBY@pZl.?u! 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U.D. Schuder, D.D. Nelson Jr., D.J. Nesbitt, J.Chen. Phys. 9{, 5796 (1991).2. M.D. Schuder, C.M. Lovejoy, D.D. NeIson Jr-, andD.J. Nesbitt, J. Chem. Phys. 91, 44Lg (L989).3. M.D. Schuder, D.D. Nelson Jt., and D.J. Nesbitt, (inpreparation) .4. M.D. Schuder and D.J. Nesbitt (in preparation).5. M.D. Schuder, C.M. Lovejoy, R. Lascola, and D.J.Nesbitt (in preparation) .6. C.ll. Lovejoy and D.J. Nesbi-tt, J. Chem. Phys.86, 3l-s1 (1eB7).7. C.M. LovejoY, PhD.(1eeo). Thesis, University of Colorado 8. A. McIIroy, Ph.D. Thesis, University of Colorado(1ee1).g. G.P. Agrawal and H.K. Dutta, Lonq-WavelengthSemiconductor Lasers (Van Nostrand-Reinhold, NewYork, L986) .10. N. Hunt, S.C. Foster, J.W.C. Johns, and A.R.W.McKellar, J. MoI. Spec. 111, 42 (1985).11. A.S. Pine, J. Opt. Soc. Am. 64, 1683 (L974).L2. J.U. White, J. Opt. Soc. An. 32, 285 (1942).13. J.L. HaLI and S.A. I-ee, Appl. Phys. Ltt. 29, 367(Le76).14. G. GuelachviIi, Opt. Comm. 19, 150 (I976).15. C.M. Lovejoy and D.J. Nesbitt, Rev. Sci. 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This probren is deart with very sinpry bypassing the bearn through a spatiar filter and eliurinatingall but one spatiar roode. we have used a 100 prn hole incu foil for this purpose. The beam is focused into thespatiar filter with an f/2, t, dianeter caF. plano-convexlens. Routinely, about 50* of the rR radiation istransmitted through the spatial filter. The beam enittedfrom the spatial firter is recorrirnated with a f/6, 1rrdiameter CaF, plano-convex 1ens. Frequency Noisern addition to the frequency scanning, output powerand spectral node characteristics discussed above, thenagnitude of both amplitude and freguency noise areextremely important criteria to assess the usefurness ofthis laser for tunable rR spectroscopy. we will deray adiscussion of the diode l-aser amplitude noise until thedata acguisition section.The urain source of freguency noise on the diodelaser is due to nechanicar vibrations which accompanyeach extension of the piston used to coor the cold head.This is shown unambiguously in Figure 2.rr, which is atrace of the laser freguency noise versus tine. The protwas obtained by triggering a storage oscirloscope with amicrophone positioned near the cold head. The frequencynoise is rnapped into anplitude noise by positioning the endstream endobj 161 0 obj 1274 endobj 162 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 163 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj157 Do Q endstream endobj 164 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj157 157 0 R >> /Subtype 160 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 162 0 R 163 0 R 158 0 R ] >> endobj 165 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 31416 >> stream aP Ql)m8#`z# Īv"$G,٨h#45PG[)7Q "*̎#Dds##6D%28["f"vH6&!Pd  f@,n8E8a~Ky\F cƈdT"0 !Ŏɇ(8< _TW!7]U _}W_Wy 뾾xFרE?ǯu2"08]p(zG HëWuÅR R ]y+p޾ "e~a r2G[C}צab*!#__]vC =!G!1>>=]d2A#HqH 5 !#d{B݂) v|d2PU2YC$#$;AVt4# Z|r1'ŎDŽGO(t$u`хC C G @fA(u K8Cڸ'Gcdx,y "f] &CAI@a2 .2) j  n2RO߭Q*  gTp\@iƗMwzkoBK׸d[v&2l$?vmVf @ 2:#SP'eJ ? 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V[ qП CD~ 0Oi/o_b" $14ńKZ7DD0 &" P߿G8 0l u!DtcaB ވGB[~TA&MP qkZANsW(=ixV=Z[Z\D2\>ڶ*v1pMd%miױ  ӿ Dֈ8~;t",JZeL:d[ _an8 g1e#u]2LISaC|SߕM0V=0*BJGw?L`9Hn~8dɯ /cRT|$ӐE;.$z Eރ)Ò lHEDPDAJɓNG }+q 'Dtaдp]!q/X}}| 0i '0Dt] ܩqd`{!SNZeAw*0ut3Ya7"Ƅ)i?[ޝdZ0y}'i ƿN꿫w:E^-p6gbg־%Kr7Adv` "Ro.Sjm@;|0@ʙa߆mRaC<'ng[T*!_[!~LL aݥ ֫N<'b.v,gbBZp/mPH "%a8aH%Adq{hV@n8D~Jpam7 <6PFA[6 kbʰO8 Xa:ރ#ETڠNU6]UӤJ4aH njHi\~$Z{@DpI;`a4\,0~1? &A WLb"^lhR+Z$vAC&Y :3ji_;]q! Al x@]D2) _'O)T!a"ЮuT)~jfp0ۄaDY>L&4ܔ}vF Oz + D3Ҝ2?55E:"AP$XA]T -,8`%=]q4ظ%|i;`'kWxhQ# eLC 'HrvOW R V ̵_!amqp¶CI:{M_Z`frEO&ۻo_a(A!~ dK TGDDD4! C֫.aWu5"KL".5t@a5<ET@Hu{[ړaT82JNm>܏߄ l Q+KAh3!' x`wʀOІAʴ.i#曺a4dP7օZi0 dN ރ"+۝#VLrD_O B͘" Hm~^ kTAd0֌@< M3ϠAk3>ӄyU~* rt|;B 1޷'M/g:!3m_ &Fտ}ZQAt&0A!l)'oh0eC E ar4..+0Bke3A " .8fo{&DQYOw۵wC`fRZ?J9b~&KiDAdٛwAz`)'HK2Xi)"Da^AôZaH?;uj Zw!\T ߬3SZ!PJ\T0Ni=|8w3}8us%DZ$dw "N`ā㰡Mwqz. 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Infact, the trace was obtained by triggeringthe oscilloscope with a micropirone piu".anear the cold head. 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By knowing the slope ofthe etalon fringe one can obtain a rough measure of thisfreguency noise. However, a better nethod to quantifythe freguency noise invorves rneasuring accuratery theline width of a stabre molecure (ocs) in the srit jet.The procedure by which the rine widths are measured wilrbe discussed rater in this chapter and onry the resultswilr be presented here. since the rnajor sources of linewidth broadening of stable morecures (eg. ocs) in thesrit jet are residual Dopprer broadening and freguencynoise, by determini.ng the Doppler width and theabsorption line width, the freguency noise is measurabre.The average FWHM Gaussian absorption rine width for ocstransitions is 52 (4 ) MHz. This is substantiarry largerthan the L6 MlIz predicted for Doppler width at I K.Thus, essentiarry the entire line width can be attributedto freguency noise. However, it should be stressed herethat this measurement is representative of onry a smarrregion of possible lasing freguencies, and that thefreguency noise varies across this region. The magnitudeof this effect is approxirnated to be about tt o MHz.Thus, the freguency noise on the diode laser is bestrepresented as 49(10) MlIz. endstream endobj 177 0 obj 1390 endobj 178 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 179 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj173 Do Q endstream endobj 180 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj173 173 0 R >> /Subtype 176 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 178 0 R 179 0 R 174 0 R ] >> endobj 181 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 37370 >> stream . 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A reduction in the frequency noise has theadditional benefit of inproving the detection sensitivityto lifetine broadening in spectrar transitions. one wayto reduce the freguency noise sampled by the experimentis to sinply shut off the data acguisition during theperiods of excess frequency noise. The disadvantage ofsuch a modification is a loss of about r/3 of possibredata taking time.An alternate rnethod, which does not suffer from thisproblem, is to stabirize actively the }aser output byfeeding a frequency dependent correction back onto theIaser through an external current input. The errorsignal is obtained by selecting the frequency of thediode raser such that it is on the side of a transmissionfringe. This signar is passed to a home built servocircuit composed of proportional and integral gainanprifiers (shown in Figure z.L2). Briefly, the circuitis composed of a pure integrator, which rolrs off atabout 15 kHz. 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The circuitis composed of one stage of pure integrationis included (the second operationalarnplifier (op. anp. ). One stage with a knee(the first op. amp. ) for additionalgai.n at low frequency but the gain rolls offand becones sinply proportional gain of zat about 240 Hz. The last two op. amps.ro11 off the gain near DCI which wouldotherwise be infinite. Also included butnot shown is an adjustable gain proportj-ona1ampl ifier. IR Dctcc tot \- Figure 2.12 Frbry-PcrotELalon Pb-S 8llDrod! 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TxG-r$> stream BT 3 Tr 1.20 Tc /F3 11.0 Tf 1 0 0 1 133.44 690.24 Tm <66696E69746520> Tj 1 0 0 1 183.36 690.00 Tm <6761696E20> Tj 1 0 0 1 219.60 688.56 Tm <617420> Tj 1 0 0 1 240.72 688.08 Tm <7665727920> Tj 1 0 0 1 277.68 687.12 Tm <726F7720> Tj 1 0 0 1 306.48 686.40 Tm <6672657175656E636965732E20> Tj 1 0 0 1 405.84 684.24 Tm <4164646974696F6E617272792C20> Tj 1 0 0 1 507.84 682.08 Tm <6F6E65> Tj 1.20 Tc 1 0 0 1 132.48 666.48 Tm <737461676520> Tj 1 0 0 1 175.92 665.52 Tm <6F6620> Tj 1 0 0 1 197.52 665.04 Tm <61646A7573746162726520> Tj 1 0 0 1 276.24 664.08 Tm <70726F706F7274696F6E616C20> Tj 1 0 0 1 369.84 662.16 Tm <6761696E20> Tj 1 0 0 1 406.80 660.48 Tm <697320> Tj 1 0 0 1 428.40 660.00 Tm <696E63727564656420> Tj 1 0 0 1 495.12 659.28 Tm <286E6F74> Tj 1.20 Tc 1 0 0 1 132.00 642.48 Tm <73686F776E292E20> Tj 1 0 0 1 196.80 641.04 Tm <54686520> Tj 1 0 0 1 225.60 640.32 Tm <6572726F7220> Tj 1 0 0 1 269.04 639.60 Tm <7369676E617220> Tj 1 0 0 1 319.68 638.16 Tm <66726F6D20> Tj 1 0 0 1 354.96 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Additionarry, onestage of adjustabre proportional gain is incruded (notshown). The error signar from this circuit is fed backon the laser via an externar voltage to current input.This input has a flat response to about zo k'z. A pureintegrator has a phase shift of -go. and a frequencyro1l-off of -6 dBloctave. potential probrems arise ifanother source of phase shift is present at freguencieswhere the gain goes through unity. rf this is the case,the circuit wirl be unstabre due to positive feedback.This technigue has been demonstrated to reduce thefree running frequency noise of 50 MlIz to about r.o MlIz.This represents a substantiar reduction in the freguencynoise which is sufficient to prace the freguency noisel0wer than the residual Doppler width. However, it isnot used in everyday data acguisition due to difficurtyin freguency scanningr. whire a piezoerectric crystal isthe element of choice to scan the externar. cavity (andthus the diode laser), one needs to change the cavityrength by L-2 tirnes the waverength of light. This isdifficult to do rapidly (-1 kHz) for 5 pm radiation.Arternatively, a smal1 frequency dither can be applied tothe diode laser, which is an often used technigue.rntracavity caF, galvo plates are capable of changing thecavity length by the reguisite amount, but initialatternpts to incorporate them failed since the resultant endstream endobj 201 0 obj 1405 endobj 202 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 203 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj197 Do Q endstream endobj 204 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj197 197 0 R >> /Subtype 200 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 202 0 R 203 0 R 198 0 R ] >> endobj 205 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 33778 >> stream rbЋðU##;<'JQn]_Pqn[[`}_[_u޿|=:[[h-Oڮ<.U݅zO [ELޤucuC APa40 #]GUG_aDubz޿-l8Jt 6;Xz\+?Wީ۠ƃ¦@H] v4Ӣ \ke!5.h{vֺuWGaHqfӺa0?·(o_u+޷##޷A^t":n*6<+vMj:,pM @_- L;m>6BA7v\OjM4~e0.,#Lշ!T&$}b D B@U#p\!8<< ӴM A%4h0!z N-qМ,4"!CT!ݤꁩK44>aYg@`0@nxiEt[d ͘"H#AP g =Az"gD^Fd?fD1Mdx>΢.\Y\0M0@8{txOPz Ro6ѩB$ gA ` Al6ݠ{ޕS2MB-aBvjW#d9AkkI{[[OO m-M^ Hm:%G'8de O q}!OAwv&EgDd.P =7Nh%{r~=Xk_Njm9ۑ}Ș i}$ t҆Aӛd$A!["uN.}uүp#?__̓$%oZa6:OӴi 1 aC_Q#п9NPLM'j맯oRJ]5i\$SW -q}_zG!kP ૿}]uhŤ?oA5B]5lw{ }ƈ8/}mvGO__ ٬10zN5!{J^M$< 2p&o9!=wpӧ_ ' ¡Ac"phiw)/d?aٙV }D5' Lא('կWNnAv T&{' *#1_ݝR¯d5M--mO"dRa& eQOz{ Э8=VkvL&DG̈́&DDiv5ՎC7M8GpnM>MKfKO#@2a5bPA=M0!M0LMLAC""=8p_ D3phoI Mް>&CL& 1E.0B""= mZvڇ / Av `$ &DGOa76лMF29"NShWa0A馩hpd  q2 @AJ3h0¼ gKB"#DDDDDDDDuڥ™ 8]s=xPѐ/Q[ӵ^G\}ӆ-z{<azu{t%tEm"n7z!5f^w-5l~Y ۆ˗T A4Q|"42n {mLMkËTfqeR!qA X}&Άy!P`Ba aꠢs7vvG-"3CkNIGib qH@\"bqc":>8" q Yx^*yQn-0n RQDwh$G; ̪# FC5 hX@!`}t>8a?O[2G,# ̎   a L }aYDh[H;Z_0dG"eTSB8 < ` iIIՇD Q#;'}nzՂ(͑Ѓ!wOO ń]L+e``CRg=Iz*ծB? 4 'Ӥ:t!"8do ST{WOAh :v74{i891SF\{I'SC߫vT4*~ A8jub(ȿvkx_B?!CZD\m4%K  MW|!Iվ΀-!Gֿ\=0CBϯ Ȃ.PJdp_wV@֫Ҷ> AVzt?^z{T }C5[kl7 %usTZWZVAkVuB(/ӾzZnC8'{TA߰ ZI_c_{}^-5{T߳^V$k`+aS4uBW}8U1A6qh#SNUy&욆맷vO}̈́cN펁 1l*[ `OD樐=U[m/lmc ;ꭶa[[[>PW WNڻpV`0L޿گɆ6D␆XMnh4aZ |0"b 'B#O ]7pI biӨL4@4jmp;ղX" 66A-ҽ+ ݂`aq|ZA+ 0hAVi=UR) c4@g-NjҴXa2!SȸXAkDzZm+/2dHNȢIծ ¦@ɉC2d0L;!2-H4 3'Nm5 TDDDDE}B"#lBvn1a;]kAr%D~XDEU]n^Pwkte7$]9樁 p)); Jܴ_ ibROWr4)3dSy#ROtM _nGwQ7[0DxM;m]? wd,)gSMB/zeXȁ0LA amwoIB M8JNTxDB 4 /NïSPO2gC32 .8i8xMܗ>w`lc pdpa'aVJ!Sȸ#1/A!~3' D4T! h0BuW{!k#rhz^t2yRqH 44kiiw?`H6/zIԨt̉`iP5v 2)r:9n~q;~KL vi۽]wV.6BFGAzzn:߶4ZjTݠh5S!;<6t Btn .Wuݧ ۇEJFE!m^'WYiokDy)E!:ՇuuׯZhk?^DLaGo @5!D-'{EnO^FnBMY+H#$Oݪf7iu0WWlMazXOJmi|/p׭3'$Y>u.?҆궒 mբ,&kjZ+i{@^ԅÕWVﴯT׵v ֗I]_iZᓕpP0l\ZiDu{ix6kR I<(M(C' i\W{O(=U5 " aD6bM߲;k4ΥDR?UᅆNP,UbWJR ikB j]A}ke٣NT*-NiӸM: S[,A!`G { Z{ڶCXal,"i8jOM6i SL8DFmm0a)TqdcL'I4U]laH" !FK 8Xn:Oz ڭ Aj0v,( ֕mv0@ȁ &DF "@{tPLLTHM2<TB""#i7݄2&B`0L *d;ڠȶC8!xi L(LÄЈBe*KEkDtYEi,5i2c8[(~/np`PaC<+t,ޖO,!ZKXL:XB[_;*̠y/j>­YHgj.'iEN׽ZOOy/iMR4V: f BĒz9!dFr,!AoM2f"L;N0L zu"l!* F a5teO)r0d 6@lP@cGAǶ]L"GR4+8pvh Q 0 LC ńL'i'jpTeSD6hAsN@kV&ÆBdsb> T"j )044wkw~6ӠSdT /P0@Ї &T=U0m{`6Yӄ EU|$Z5Ha8 UwojJ.e,9)E$vu<2`vxU_oN'ۮ,dDd$0d`lCAMԄuۇ!SӼnA<v7]w}]w Ȝɟ%Fȿ 4ÿ ?~kL菺#&Cڒ; t ciLd@.pj]K頃\ M[c zx/~n}z4K_]|5/AO ZOZ$IJAVB?vA=;}w~~C=;a菷ވ.&_KT'o>wFORc{ȹwݦ݅p͋ 'uK ?_tp nBsblS_SH>DtPR]c-6|Z#(pLI <}׵laV' C=mVqWnQSw]cL(" hv֡ QCUX0 ,4a?; Ʒ 3i=>E 33 >ΪPPՆP 4*8ش@ΓIa&Umxp#@ɒ""=8fNBSitê{ m:k Ј " P)U^ !j`M Ƌ ML'HdM` F7 5 aS P>@c z & `DDD~V`'h21RB@#: JhDDt?ӸD{2&aW-[7 nkPo_z;C[|PDtYu6O(z_>Mﵡނd&ҩ7Rd GQAo H\&uJf 8AA]O8z0L/NBM$@6D(퐮m à c$ve# tE: [=> ' [ȃ_K- :uA_?tG?a|q6?4ZakuJ*ڴaXaapgV0R\abbv2p#3 & j۰apV)vX`M0] d d4p@0X8d0B"""NiO"] ` n B8 %%E u- putGx":ǿ޸Z#j_}ֽ}}duQպe2G"SblT2,Afvӽ [;Nح3d;BX\"u;8OO7;[,od4'aNeUWm׷mOk%‘H(ALtv KaW @c$"0Bp6p߄y2u @l"0P>'C9 ؀0 O0}$tNC@.AN! ۋTWA4E"d<nGdy!(r0F\%aІ²hwaPtD'8A O6ID$"L0]N>б5D#N`!֣< = MՇdq8A?ݭ^D%H%0Am >UzC0a;v {Fg s@@?Z߄ ?#쾆R>pȋi! ۬&}.M<C: (9 !@ &n֓i2oOO_܏?ȓ` aoWD[_H6vIʰugW 91 QjIwnGPOnl04GɪY$_ -D7=}HO_]Z_]*~B^;_D}oVFrWD]{oZD!ȴxOֿwl5NXe f`K>[38iSGJ/p=uu'!ݬ3`dᆢA wZZgZ/ jf QLY8hBm ׫i>mٽS%t֚e{-M06Zx"$w,zxAS IT;,] 7i{ 0!Z#м&InmX.uSq,;&8 '2@P"'I͑4Bj 0Fp AT%ao!MN krAf9 ЎOOar8`hd~48>a p!d!p#Jni4GDaDBgC4 ;m'G^ar BA ȾS> "+z3&=' 4AC§DL@0D60BLp`i8iaϡDAiâ?umڄL`-ࠁ;hZxA d$;W3ݐ\z*U4Ol(WAKJKS%=l / O +a,.G2ӤAM Boa;WTյD .C*6N C@;^XӤo/]#Ȟ*:p!*OM=ރp:G _<?N;MAڅM]/[p,_?[ɨ#5OO^IukQ-Kc\Ǎ?`{ץMíW㴽a_|Z?׳aCoH, ]=O `=P U={Im; 5N8r`o#c+ZxM5hA} Id #kxr/7ku"XamUrUL1D3@ G"`?RJ޾_[N8M6i \3?iWdߧiViʀwAR70]SMaʡZr{[oPH8g9& i5I)v0i R)QVC [i*{]卍2ERjתiޚ`X`4VdGQR@0Z5vC5d*C] 8^ai* 5L&&Ls DDF*P` p2C0B"""""0X0UA X `nvB$8@Ƞ rƸL\!,A> i!MRﶸa_w#|w_z4r:Sz.TeD&|dz#" %H<@}B2lM7MNV r̓V{5n77Ӥ޸mvTi 9N!#a0Be;m'zOl<׫jk)+rpsD&6D̏&j5A_ơ B;a6 :I{kJ>{lkIz}߯[ǫ 5 |']'oGÅJ;^wr:/Okt} `$c1>_{k8D'c?ӯfLf_ӷ[f ~!ŸOoOYmiӃ.&U>@~ɒW{鰶'&+ ; iXx =P_~IC]u_]VX{g]5dKIBD4h$O_uvd:'a(fb( @i}Y {A>_޾{gIa&g łT=0 pPAwMaOkuT31 JtD-taxd( #.[:}`;-4f 0Id@;B""8[_[(IxfcV68 JNiՄ` vPjڶpUb\; l$ !ds(B""8VN&0N2L&H;L! 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324.24 91.20 Tm <417070726F78696E6174656C7920> Tj 1 0 0 1 426.96 91.68 Tm <4C302A20> Tj 1 0 0 1 456.00 91.68 Tm <6973> Tj ET endstream endobj 207 0 obj 9459 endobj 208 0 obj << /Length 209 0 R >> stream 4l_ etalon fringe height was reduced to an unusable level.Further work is reguired to make this scheme practicalfor daily use, but it has been shown to be feasible andrepresents substantial benefits for future dataacguisition. Optical LayoutThe optical layout for the Pb-salt diode laserspectrometer is shown in Figure 2.I. The infraredradiation emitted from the diode laser is collected withan off-axis parabolic mirror with a focal length of 1.5rr.The advantages of this mirror over a large diameter lensare near unj-ty reflection over most of the infrared andno dispersion, ds well as being a parabolic element whichwj-I] focus off axis with no stigmatism. It is positionedto collimate the highly divergent (=f/L) diode beam. Anunber of flat gold turning nirrors are used to redirectthe beam (see Figure 2.L). Adjustable irises are used toIocalize the infrared beam and to facilitate overlap wj-tha visible HeNe tracer beam. The only transmission opticsalong the beam path are CaF, lenses used to f-) focus thebeam through a spatial filter (discussed earlier), 2)collirnate the beam following the spatial filter, and 3)focus the bearn (f/2, 1t') onto the infrared detector.Following the spatial filter, the beam is dividedvia a pellicle bean spli-tter. 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Tm <746149492920> Tj 1 0 0 1 321.60 567.36 Tm <697320> Tj 1 0 0 1 342.24 567.60 Tm <7573656420> Tj 1 0 0 1 378.48 567.36 Tm <746F20> Tj 1 0 0 1 400.32 567.36 Tm <73696E706C69667920> Tj 1 0 0 1 465.60 567.36 Tm <6C61736572> Tj 1.20 Tc 1 0 0 1 147.60 543.84 Tm <616C69676E726E656E7420> Tj 1 0 0 1 220.08 543.60 Tm <616C6F6E6720> Tj 1 0 0 1 263.28 543.60 Tm <74686520> Tj 1 0 0 1 292.32 543.36 Tm <736C697420> Tj 1 0 0 1 328.08 543.36 Tm <6178697320> Tj 1 0 0 1 364.08 543.36 Tm <616E6420> Tj 1 0 0 1 392.64 543.36 Tm <746F20> Tj 1 0 0 1 413.76 543.36 Tm <6D617869726E697A6520> Tj 1 0 0 1 479.28 543.84 Tm <70756E70696E67> Tj 1.20 Tc 1 0 0 1 147.84 519.84 Tm <73706565642E20> Tj 1 0 0 1 205.20 519.60 Tm <54686520> Tj 1 0 0 1 234.24 519.60 Tm <646973616476616E7461676520> Tj 1 0 0 1 328.08 519.36 Tm <6F6620> Tj 1 0 0 1 349.68 519.36 Tm <7375636820> Tj 1 0 0 1 385.68 519.36 Tm <6120> Tj 1 0 0 1 400.08 519.36 Tm <736D616C6C20> Tj 1 0 0 1 443.28 519.12 Tm <636861726E62657220> Tj 1 0 0 1 501.84 519.12 Tm <697320> Tj 1 0 0 1 522.96 519.12 Tm <74686174> Tj 1.44 Tc 1 0 0 1 147.36 496.08 Tm <74686520> Tj 1 0 0 1 175.68 496.08 Tm <6D756C74697061737320> Tj 1 0 0 1 248.16 495.84 Tm <6D6972726F727320> Tj 1 0 0 1 306.24 495.84 Tm <63616E20> Tj 1 0 0 1 335.04 495.84 Tm <6E6F7420> Tj 1 0 0 1 363.60 495.84 Tm <626520> Tj 1 0 0 1 385.20 496.32 Tm <706C6163656420> Tj 1 0 0 1 436.56 495.60 Tm <696E7369646520> Tj 1 0 0 1 486.48 495.60 Tm <746865> Tj 1.20 Tc 1 0 0 1 147.36 472.32 Tm <6368616D6265722E20> Tj 1 0 0 1 219.60 472.08 Tm <546875732C20> Tj 1 0 0 1 263.04 472.32 Tm <6561636820> Tj 1 0 0 1 298.56 472.80 Tm <7061737320> Tj 1 0 0 1 335.04 472.08 Tm <726571756972657320> Tj 1 0 0 1 399.60 472.08 Tm <7472616E736D697373696F6E20> Tj 1 0 0 1 493.68 471.84 Tm <7468726F756768> Tj 1.20 Tc 1 0 0 1 147.12 448.32 Tm <74776F20> Tj 1 0 0 1 176.16 448.32 Tm <4361462C20> Tj 1 0 0 1 209.04 448.32 Tm <77696E646F77732E20> Tj 1 0 0 1 281.28 448.32 Tm <54686520> Tj 1 0 0 1 310.56 448.32 Tm <6F707469726E756D20> Tj 1 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Aschematic of the pulsed val.ve (discussed in more detaillater in this chapter), vacuum chamber, and nultipassmirrors is shown in Figure 2.L3. A small vacuum chanber(6" dianeter X 5rr taII) is used to sinplify laseralignrnent along the slit axis and to maxirnize punpingspeed. The disadvantage of such a small charnber is thatthe multipass mirrors can not be placed inside thechamber. Thus, each pass requires transmission throughtwo CaF, windows. The optirnum number of passes usedtherefore represents a balance between longer pathlengthand the reduction in laser power due to additional lossesfor each pass.one can calcuLate the number of passes whichprovides the optimal signals given the transmission ofthe window as follows. First, the observed signalanplitude is expressed in terms of the fR power andnumber of passes. SdP*n (2 .5) where, the signal amplitude is labeled as S, the power asP, and the number of passes as n. 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As is apparent in thisfigure the vacuun chanbei is guite snall,and in fact is only slightly larger than theslit pulsed valve. The slit valve rests onthe vacuum chamber and points downwardsinto a 6'r diffusion punp. The sixpasses typically utilized for these studiesare shorrn. The vacuum chamber windows areeither CaF, or sapphire, both of whichprovide es3entially identical behavior,except sapphire windows (1 nrn) are thinnerthan CaF, (8 nn) . at4v Figrure 2.L3 endstream endobj 225 0 obj 605 endobj 226 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 227 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj221 Do Q endstream endobj 228 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj221 221 0 R >> /Subtype 224 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 226 0 R 227 0 R 222 0 R ] >> endobj 229 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 14624 >> stream ɨ+3`ۓk#Rԕ'ȾGXJևȠ*ې'FA.ZSR!JA\Aw]CEEw?[C}}}}P  ^G zBk '"]A? % b\)ӈ=PweQr16w/qlvGX:"¤嘊2oAKOtOUfh>!IwB, D4OLDJ vla<), VKӑVIh I;F(#x'3Pq PdPD8s3+;q 'aa XC4C_R94 p@Ai `h^ ;A`waS!  vv:nݪR U5U.&4DJnJݺ]/;.CA')2AdOlm" ?+%%ENaGKrh\&inAz@A~G6  ;"TnT $A_]po\5A|5nT!a,W΁i񭊮%pbBqr f"Y~A ?ArOrAr 0g "mS ^% D} L?oEx@{Jplm7K)PĂ9ZxApB $)#HAɨe!Z֯:_Rvx6fݵ$'οi% ~vʹwN׸nav v{%a;J 8d[]= \vP`f8i=ڬ0Yvqr&DvNCi4ᄚ@@/L\hqǦScTzhB?M uOV;K ;L7N/]=4i]5 h`&^ 2ikq(L A &B]Q ()j2Ye@NI4 0Rɂ* DɔvbTGDDq}[O6 z'({ﺅXſ$/6ҿZjVZݩfg4$OSVW$M#gJPL+h:NUk}]MڶKmV'G6HY| ۯXMz}}~m/ޯZU{u&\/b ZڦҿM!U{(A {El WTZ_=Oa_ߤL?m/|~Fw?+Z a/Mzux@\V]r5U= #PF۴b8w >)w)6ku=:Y7vt}M m4+#MuwWW_ê_W S)hRMK:Wi"IM8nNV;l 'tDNA]5Pv]ޘh6M! 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<45712E20> Tj 1 0 0 1 179.04 387.12 Tm <322E3720> Tj 1 0 0 1 208.56 387.12 Tm <697320> Tj 1 0 0 1 228.96 387.12 Tm <6D6178696D697A656420> Tj 1 0 0 1 300.96 387.60 Tm <77697468> Tj 1.44 Tc 1 0 0 1 149.52 363.12 Tm <6465726976617469766520> Tj 1 0 0 1 229.68 363.36 Tm <616E6420> Tj 1 0 0 1 258.72 363.60 Tm <73657474696E6720> Tj 1 0 0 1 316.56 363.60 Tm <6974> Tj 1.20 Tc /F3 11.0 Tf 1 0 0 1 337.68 387.36 Tm <7265737065637420> Tj 1 0 0 1 394.80 387.60 Tm <746F20> Tj 1 0 0 1 416.64 387.60 Tm <6E20> Tj 1 0 0 1 430.80 387.60 Tm <627920> Tj 1 0 0 1 452.64 387.60 Tm <74616B696E6720> Tj 1 0 0 1 504.24 387.60 Tm <697473> Tj 1.68 Tc 1 0 0 1 337.44 363.60 Tm <656775616C20> Tj 1 0 0 1 380.64 363.84 Tm <746F20> Tj 1 0 0 1 402.72 363.84 Tm <302E> Tj 0.00 Tc /F3 16.0 Tf 1 0 0 1 202.80 308.40 Tm <61> Tj 0.00 Tc 1 0 0 1 196.56 294.96 Tm <36> Tj 1.92 Tc /F3 7.0 Tf 1 0 0 1 218.88 306.24 Tm <6C5E712E326E2920> Tj 1 0 0 1 258.24 306.96 Tm <2D273E5E> Tj 1.68 Tc /F3 5.0 Tf 1 0 0 1 218.88 300.00 Tm <6C744A20> Tj 1 0 0 1 231.36 302.88 Tm <4A20> Tj 1 0 0 1 249.12 301.92 Tm <7C20> Tj 1 0 0 1 257.52 305.04 Tm <2D20> Tj 1 0 0 1 269.04 303.12 Tm <4C726C> Tj 1.44 Tc /F3 10.0 Tf 1 0 0 1 288.48 302.88 Tm <746E28546C20> Tj 1 0 0 1 323.28 303.12 Tm <54326E20> Tj 1 0 0 1 346.32 304.56 Tm <2B20> Tj 1 0 0 1 358.80 303.12 Tm <54322720> Tj 1 0 0 1 381.84 305.52 Tm <3D20> Tj 1 0 0 1 393.84 303.12 Tm <41> Tj 1.44 Tc 1 0 0 1 150.00 219.12 Tm <536F6C76696E67> Tj 1.92 Tc /F3 11.0 Tf 1 0 0 1 208.56 219.36 Tm <666F7220> Tj 1 0 0 1 236.88 219.36 Tm <6E20> Tj 1 0 0 1 251.04 220.08 Tm <7969656C64732C> Tj 7.44 Tc /F3 10.0 Tf 1 0 0 1 240.24 160.56 Tm <6E3D2D20> Tj 1 0 0 1 296.16 165.12 Tm <4C> Tj 1.92 Tc 1 0 0 1 276.72 151.68 Tm <3220> Tj 1 0 0 1 289.20 151.44 Tm <516E285429> Tj 3.12 Tc /F3 11.0 Tf 1 0 0 1 488.16 304.56 Tm <283220> Tj 1 0 0 1 502.08 303.36 Tm <2E3829> Tj 3.12 Tc /F3 13.0 Tf 1 0 0 1 442.80 161.04 Tm <28322E6529> Tj 1.44 Tc /F3 11.0 Tf 1 0 0 1 150.00 98.88 Tm <5573696E6720> Tj 1 0 0 1 193.92 99.12 Tm <6120> Tj 1 0 0 1 208.08 99.12 Tm <7479706963616C20> Tj 1 0 0 1 265.92 99.12 Tm <7472616E736D697373696F6E20> Tj 1 0 0 1 359.52 99.36 Tm <7468726F756768> Tj 1.20 Tc 1 0 0 1 417.36 99.36 Tm <6120> Tj 1 0 0 1 431.76 99.36 Tm <4361465E20> Tj 1 0 0 1 464.64 99.36 Tm <77696E646F7720> Tj 1 0 0 1 515.76 99.84 Tm <6F66> Tj 0.00 Tc /F3 5.0 Tf 1 0 0 1 453.36 95.28 Tm <49> Tj ET endstream endobj 231 0 obj 5440 endobj 232 0 obj << /Length 233 0 R >> stream number of passes (n) is expressed as Pn : Po (T)2n (2 .6) fhis loss is due to both absorption of the infrared lightby the optical material and scattering off each of theinterfaces. The exponent is 2n rather than n since eachpass reguires transmission through 2 windows (4surfaces). The signal, dS a function of T and n, isgiven by Eq . 2.7 . scnT2n (2.7) Eq. 2.7 is maximized withderivative and setting it respect to n by taking itsegual to 0. a6 l^q.2n) -'>^ltJ J | - Lrl tn(Tl T2n + T2' = A Solving for n yields, n=- L2 Qn(T) (2 .8) (2.e) Using a typical transmission through a CaF^ window ofI endstream endobj 233 0 obj 596 endobj 234 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 235 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj229 Do Q endstream endobj 236 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj229 229 0 R >> /Subtype 232 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 234 0 R 235 0 R 230 0 R ] >> endobj 237 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 37142 >> stream Ԣ>]nf sT}D4_1hDv\<"""$<.G (v"D0Oȃr1q9 A8 LDtxv]i06Ô809 qYPue9HhS#;G##=!e:fr)Ey88Ac;C9NSg!\S9A6hDDDDDDADO菌D""""$؈0DpS;:#3Ȏ\F""$98 X:E,?;(L\A(#GV 8G)u0E=>#pu:^+Ӿ"[޹O(x. 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endstream endobj 239 0 obj 9854 endobj 240 0 obj << /Length 241 0 R >> stream 45about 94t (T=0.94) leads to a prediction of 8 passes forthe optirnum signal. However, the windows on the vacuumchamber are coated with a thin diffusion punp oil firrnwhile running which can further reduce the transmission.A liguid N, trap is not used since it reduces theeffective purnping speed berow an acceptable rever. Aslight reduction to T=0.9 rowers the optirnun conditionsto 4-5 passes. Thus, six passes hrere used for allexperiments reported herein. Fotrowing the murtipass,which is formed by two flat mirrors as shown in Figure2.1,3, the infrared beam is focussed onto HgCdTedetectors, discussed below. 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1 0 0 1 280.80 569.52 Tm <6261747465726965732E20> Tj 1 0 0 1 367.20 570.48 Tm <54686520> Tj 1 0 0 1 396.24 570.72 Tm <6465746563746F7220> Tj 1 0 0 1 461.52 571.44 Tm <616E64> Tj 1.20 Tc 1 0 0 1 122.64 544.32 Tm <61726E706C696669657220> Tj 1 0 0 1 194.64 545.76 Tm <7061697220> Tj 1 0 0 1 230.88 545.28 Tm <68617320> Tj 1 0 0 1 260.16 545.52 Tm <6120> Tj 1 0 0 1 274.32 545.52 Tm <746F74616C20> Tj 1 0 0 1 317.52 546.00 Tm <726573706F6E73697669747920> Tj 1 0 0 1 411.12 546.96 Tm <6F6620> Tj 1 0 0 1 433.44 547.20 Tm <3320> Tj 1 0 0 1 447.12 547.20 Tm <5820> Tj 1 0 0 1 462.48 547.44 Tm <31303520> Tj 1 0 0 1 487.20 547.68 Tm <562F5720> Tj 1 0 0 1 517.44 547.92 Tm <696E> Tj 1.20 Tc 1 0 0 1 122.88 520.56 Tm <6120> Tj 1 0 0 1 137.04 520.56 Tm <62616E6420> Tj 1 0 0 1 173.04 521.04 Tm <776964746820> Tj 1 0 0 1 217.20 521.52 Tm <6F6620> Tj 1 0 0 1 239.28 521.52 Tm <4C6F20> Tj 1 0 0 1 259.92 521.76 Tm <487A20> Tj 1 0 0 1 281.52 522.00 Tm <746F20> Tj 1 0 0 1 304.08 522.00 Tm <6C2D6F20> Tj 1 0 0 1 324.48 522.24 Tm <4D487A2E20> Tj 1 0 0 1 367.68 522.72 Tm <54686520> Tj 1 0 0 1 396.72 522.96 Tm <6465746563746F7220> Tj 1 0 0 1 461.76 523.44 Tm <68617320> Tj 1 0 0 1 491.04 523.92 Tm <6120> Tj 1 0 0 1 505.20 524.64 Tm <7065616B> Tj 1.20 Tc 1 0 0 1 122.88 496.56 Tm <646574656374697669747920> Tj 1 0 0 1 210.00 497.28 Tm <617420> Tj 1 0 0 1 231.60 497.52 Tm <61626F757420> Tj 1 0 0 1 275.52 497.76 Tm <313020> Tj 1 0 0 1 296.16 498.96 Tm <706D20> Tj 1 0 0 1 318.00 498.24 Tm <6F6620> Tj 1 0 0 1 340.08 498.48 Tm <332E3420> Tj 1 0 0 1 368.40 498.72 Tm <7820> Tj 1 0 0 1 383.52 498.72 Tm <6C2D30313020> Tj 1 0 0 1 413.04 499.20 Tm <636D20> Tj 1 0 0 1 435.12 499.20 Tm <487A6C2F3F2F7720> Tj 1 0 0 1 484.80 499.68 Tm <696E20> Tj 1 0 0 1 505.92 500.16 Tm <61> Tj 1.20 Tc 1 0 0 1 123.84 472.80 Tm <3120> Tj 1 0 0 1 137.76 472.80 Tm <6B487A20> Tj 1 0 0 1 166.56 473.04 Tm <62616E6477696474682E20> Tj 1 0 0 1 252.96 474.00 Tm <417420> Tj 1 0 0 1 275.04 474.24 Tm <61626F757420> Tj 1 0 0 1 318.72 474.48 Tm 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This is a photoconductivedetector, Purchased from Infrared Associates, modelnumber HCT-90, which is inherently AC coupted and is usedwith an amplifier also from fnfrared Associates (nodelPPA-15-10). The arnplifier is powered by l-5 voltrechargeable gel cell batteries. The detector andarnplifier pair has a total responsivity of 3 X 105 V/W ina band width of Lo Hz to l-o MHz. The detector has a peakdetectivity at about 10 pm of 3.4 x l-010 cm Hzl/?/w in a1 kHz bandwidth. At about 5 pnr where these studies arecarried out, the sensitivity per watt is down by about afactor of two.The other detectors used are photovoltaic InSb'These were assembled in-house from InSb elements. Thewafers are fixed to copper base plates (see Figure 2.L4)wj.tn a thin film of indium. These Cu plates also serveas the ground plane for the detectors. The output isamplified by home built transirnpedence amplifiers (seeFigure 2.]5) with a switchable total gain of either 10 knor 1 !n. while the output of these detectors is capableof DC operation, the high gain setting requires Accoupling (at about 5 Hz) due to residual DC offsets inthe anrplifiers. These are large area detectors (abouta 4rt) which saturate with black body radiation frorn thelaboratory. Therefore, an AR coated Ge window, cooled toIiguid N, ternperature, is placed in front of the detector endstream endobj 249 0 obj 1373 endobj 250 0 obj << /Length 27 >> stream % CANON_PFINF_TYPE0_TEXTON endstream endobj 251 0 obj << /Length 46 >> stream q 612.00 0 0 791.76 0.00 0.00 cm /Obj245 Do Q endstream endobj 252 0 obj << /Type /Page /MediaBox [ 0 0 612.00 791.76 ] /Parent 11 0 R /Resources << /Font << /F3 5 0 R >> /XObject << /Obj245 245 0 R >> /Subtype 248 0 R /ProcSet [ /PDF /Text /ImageB /ImageC /ImageI ] >> /Contents [ 250 0 R 251 0 R 246 0 R ] >> endobj 253 0 obj << /Type /XObject /Subtype /Image /Width 2550 /Height 3299 /BitsPerComponent 1 /ColorSpace /DeviceGray /Filter /CCITTFaxDecode /DecodeParms << /K -1 /Columns 2550 >> /Length 19232 >> stream )GgaHWvX|lJwB\OEa1?!8D~"VS* 8(pDzW.\Dwb|anD~ǫuSԺ(|[Yz_8^ ` WS+TnC_xXzu> ;uC-?-jz\ ]C__ C#q;YCjzXt`jǼ-B|-pP8I (u@mnC/ BEձk} GT?a׺|=_ Kfc 4{Yb5QW j*F:KJKHC?zV ]Du}ڪcu[>ժ\~C־޹Hި?GXR8a [~+pHOWpႭ[Du^ت: ߷[[<ީ ?A[ KSmH?|V.޻?zꝭV<oO^HF~GX[m(xN#?"?qa<":tuҿ "p)PP0GVk8;\Jǭ= tjT<" íGU<ռ-a t[z'A jw}[Æ;nKu+u`=tkz:[GUڹuQW ?h4\Վ/|=RHuH݊C\ "r?iq^<*ދcnVj.[´GW#<ucDu 9N?va[B(w{p}cVn3r v˂D~|*5v}:@PG^eK"dSRjWuM.P6?b d@8zI2E-Bڸ0!A&dZ{6B!Ī 㦬iՐ3' 0!k–Cn̻Nw _pVՐ{mw, *wPKp!M5T@0@MoLMn406\ P!j SjvM  \o׾r: $|㨠i z)PL!l Io7 0ӆo?[ k~7y?}C-&ݜTm  J 8koi_F17o`=i6!l?om+[N܋z"߽OXpwPI֒ ~V [J+4maa}LRuJVm߽~(k!Pa_V* ?rU#s5L2 ߿qMAB[K܁ .G_];]dfnzp&_0AiEӮfOoMRD~C'l06MZ }ʰvN骲 LW`00ֵ3ZAXjG@a9^C`AMW#eB ^!M|uп?._S?]_{kk}~#F@S"]#);<'5y62G(D5lRa?`9 qγdm /YnI=_\2zJ]]Z2Sp<~d4o2p< ?nv,m`x2"x3%P`5zKfysAFf&9bf"8 sfVh:d LnhX\6'}" #a_k +Ȃ,}k}%[}}w߽-;}Ok_ڵ}/KֿnvNv_?JɰIzMVK-Kվ[$F}ޱɽ`nn@jd a Czhkb F26}v&26vBk GSt^ )2uw: ;դ~UIc >o6)E 0B4O4ߺ <*m[@u=_O}nt<={B}uM4:M:_+3l_wi޷Bk/f\!릺 󲘎?k؀<_kuײv>GDph 0,dZAwv$)M!>~ܰɄ7kșWGDtGXfdGnd W ^e6@ s>ArqeS$=LWoz|+ޝw#~Cտ": W=e:[dT2΃A{XED!VӺ|h8;2! 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The whole assenrbly isconstruct of Cu to naxinize both theraal andelectrical conduction. A srnall wire isattached to the center of the detectorelement. The back surface of the eleroentsenres as ground and is attached to the Cumount via a thin layer of fn. A Ge windowis placed in front of the detector andcooled to 77 K to reduce black bodyradiation inpinging on the detector. 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587.28 Tm <35307046> Tj 2.16 Tc 1 0 0 1 433.20 469.20 Tm <6C304B20> Tj 1 0 0 1 460.32 466.56 Tm <313030> Tj ET endstream endobj 263 0 obj 5527 endobj 264 0 obj << /Length 265 0 R >> stream InSbPhotodioCe Figure 2.15 In S b Transimpedence Ampl ifier S i gnalOut 4.9 9K g n, 6 Rrrf 49.9K The transinpedance anplifier used for theInSb infrared detectors. The op. anp. shownat top is the actual transinpedancearnplifier with a gain of 10 kn. The othertwo anplifiers provide additional gain if sodesired. The output can be selected to comeeither directly frorn the transinpedanceamplifier or after the two additional. stagesof gain. Since each of these anplifiersprovides a factor of 10 gain, the finaloutput has a gain of either 10 K0 or 1 Un.Due to offset drifts in the two extraarnplifiers, this signal is AC coupled withthe 6. I 1tf capacitor. 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