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MASTER

TITLE RAMAN SPECTROSCOPES IN SHOCK-COMPRESSED MATERIA1,S

AUTHC)R(S) 3. C. Schmidt, M-6D. S. Moore, CHM-4J. W. Shaner, M-6

NOTICEPORTIONS OFTHIS RHWRTAI’IEIL l.EfilBLE.-.—-.. -— -.-— . . ----- — --— -- --It h:ts h?en ~Cpr(J!!UC??d from iho bestwailabk cupy to Ijet’mit the broadestpossible availability. . . ..-

SUBMITTED TO Proceedings of the American Physical Society 1983 Topical

Cmfcrence on Shock Wave= in Comlensc>d Matter, 18-JI July 19~3,Santa Fe, NM

INS(’I.AINII(K

lftt,III% AIm?ttI- )4aloIIlInl Iml, ttnlt*l) ImILIw. ril~ lhnl !hr. LIt,lIIIbhmt I(lmti!ll) II*o% aflotle M* aawb IIr.,ltIImtId tIIMl*I lll@auBil#C*S u*lhell S [)mllafln!orllclfne!gy—— .—. — .—. . . ..— ____ ____ _______ . . ________ . . . ..__ _______ —. —

~~~ ~b~~~ LosAlamo.,NewMexico87545‘~ Los Alamos National Laboratory

%

HAMiN SPECTROSCOPII?S IN SHOCK-COMPRESSED NATI?RIALs*

S. C. Schmidt. D. S. Mooro and J. U. Shnner

Los AlantoII National Laborntr)ryLoH AliwnnH, New Mexico

:’.

spm’ttnn~nus R.nman mpectroscnpy, stimulated Itamnn sc/lttt.rinR nnd cohcrcnt anti-StokesRaman scnttertng hnve hecn used tc measure tempcrdturus ilnd changes in moleeul~rvi bratinnnl ErequvncleH for deton.nclng nnd nhocked materlalq. Inverse Ramwirr andRnmilu Lr?dll(!cd K,.rr eft’ect speccrowcople~ hnve hecn stIggr?.*!t!d :1.q dlngnuntlc prdbes for

dctcrmlnln% thu phennmenolugy of shnck-lndilced cht=mlc;il reucr,tnnn. The pr.qct[cnllty,.qd”~antl~es, .nnd Jlsnrlv.qnt.lycs nf uHing Ramnn r4catc0rlnK rcchntqucs i19 dl.l~noatlcpr,]hcs ot mtcr,tticnplc pllc.nonm.rro lrr!;y thr,jugh .Xn,l lmmedl.lrely bi.hlnr.l the shrrck front IIEshriek-cnmpr,,HHed mulecul,lr system,] ,Ire dl.scuflscd.

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wavu~ mre hellrv(,d tn ho of the nrder of 1 11111or Lena in thlrknrqs. 1 The pd9.911~e t lmr.

tnrn!l~h thr front II” n shock whostq vI=l,.cfcy 1s5 km/qcu 1s thuq IJE the nrdur i~f ?00 FVL?C n r

lL!uH. qcllrl? , if wu Jt!slru ternporxl and

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(I(IL.1 pnlnL+r), th(~ dlagnost lC technl,l, ie *I. -

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example, Fig. 2 de~i.cte Cwr image -intert9ifi -cr-camera pictures- of the shock-front of drt -onat Lng nitromathane and an 80% nltromechane/20% acetone mixture. Liquids are oftenthctllght to be homogeneous mater {als, howevar,these picturoa show Lhut microstructure exl~tain che vicl,llty of the shock-front. Nurh Lng1s known about thm mlcroatructure Ln theregion Lmmediat+.ly behind the front. WhenperfnrmLnq experiment on nitrmathane orGimtlar :Jirstances. eapeclally experimentsuti LLztng opticml ttichniques where spatialre~olut tona of tenH of d~L’ort~ arc desired,one mumt be award that results may actuallyreflact an avera~~m ovm r a etnlallcrchar,ncteristtc mLcrOatr,lcturu. Conver9cly, aatngLc rlenqurem nc with apatlsl ranolutionauaLler than tbc micr(,atructurc may bemlsi,lturprettirL an rcprcaentattvc OF thonvcrago mttarlai.

IINCOHERENT SMI.4N SCA~EK[NG

Spont,lncnu8 damnn apc.:trnncmp; in ❑hock-cntc-pr@srIcd nystcms waM flr.rt pr?rtormt!d In rfntoc -t[ng cryatal!lnu Hrxngcnt? (Iu)x) . ?

Suh.iequt, ntIy the tet!hnlqu.? haw burn 1191!G tomennurv the Lcmpcr+tturc of detonltln~ nLtro -❑et!,anc” ,Iml to look JI. rl-,c ; rcqllerrcy ql)ltt nfVl!)r:ltln,l.11(PETN) nnd llD~$~g” A,,’’lJt~~~~~At\~H p~~~~~~yjlln(l,.r wny tn por[rrrm R,?mnn nc, !tttirlng m,.nqllr,!-mrntu In n medttlm whlr!i~ 1s $h,u-k -cnmprcnnedu!ll[l~ :1 Il[gh Vclorlty gnH gun.

...

.,

STOKES,ANTI-STOKESINTENSITYRATIO

RAMAN WECITLJM

Figllri! 3. Spont,?nc,,t,~-6R,lmln Scnttcrlng llx-prrlmcrrta. ‘

St, )ke~-.lnf. L-Strikes [Irttvltllty rnr lo- Jnll

vlhr;lt lon Jl frt.llll(,ocv qhl rr~ f~~r ‘~lltJt”k-c(lm-

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of reeonancc Eluoreecence. In addltton, fordisfirece resonance Raman .mcatterin~, sincelbqcr radlatlan ia being ab~orbed by thesnmp Le, complicate.ona from phocochemlscry andsample he.atlng can be expecceti. Tim resolved

E~m~iZm8~7fi I%H% ‘J~~~o~~~tr””cOpy ‘x-in diluteeolutLonb at ambterrc conrl{. ttorra. Gene fally~Lgnnl xvcrag,ing was uBed to Lmprove sLg-nal-ro-nn!.+e ratins. Pulee[i reeonance Rarian❑cnttertn~ mcn.9uremcrtC9 may he possible inchock-cnmprewl?o aystzm~ to dtitermincvibrntlnrral fundnm.ent~ 10 nnd overtones ofamaLL cfinccntra:Lon species. !!owvcr, Aatingnf the dctoctor might be required cfi ellmll,atf!flunredcenca effe: s. AlYo, rc~,,l:e of F-:mglepulse erperlments, 5 while tmproved cnmparpd tonpnnt.lnenuti Ramnn scntrerLng I.ntenslcte donot sl, ow ql~n.nl-tn-nolsc ration -e.1 Iargu m

obeervcd ufling tho cob{ rent technlquv~disc[ls!icd Later in thlm paper (Tnb Le 1).

cmmwr WN sptxrrww:opy

.qevi?ral cnh,!rent Rantnn acatteclnu tcchniqlics

havo bcl?n tlemonatrec[!d (Fig. 6). Advnntnnesn! tl)oqft t4.chnLqlles, prlmnrlly dllr Cn 1.1r~oncilttl.rfllR lntrnnttles (Tahl,. 1) and mlnlnvll~xp,.rLmont.11 f!a>mpllcnl[on ia, :fir,: Lncru,l.qud dlJ -

tl?[!rl,lll MWrHLtivtty, ccmpnr~l retiolutlorr

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III,, SII t)h:b,. rvo, tl III sh(],:k-cuml,r~,a :1 1,1~:::!::!l~’i” Stllm,l.,11(1 U:llmlll ,,,!i,t,t!r,,,ql~s~~(Fj,:, /4! ,,,:,., jr,l w)),.;> f]lt~ in,. l,h. nL flH, Br llll.,*!l -

wlry III ,1 m, 1111IIIn (.xri,.(lr j, r,hr(.~hol,l 1,. v,.I 111[1

~t.l)a,r;nr,..i .I ,!!.r,)ll~, HI Im, il, lti.,1, Srf)k,..; :,,.,,m.rhl. tllri.,lllolll l,. VI. I I* ,Iot,,rmlll,.,1 ,JV 111,, ll,tm:lllI.ral:l,l-,l,.,.t l,),! ,In{l I Ir)t.wllllll t)!’ I !1,. rr:lnsit II!,,,111,1 IJV I III. I ,1,.tl,tlu” pnr.lm*, rvr~ ,)f tllu 111,.1,1,.,ltl) .,lm. Tvpl,., il l:lrt,,llltlltl IIlth,llqll [,..1 ,Ir,,- 11)- lof) l:w/,.,n ,’. t’lR~lr,. ‘! lll!l.ltr.l(l.~ rh,.,lrr:ll)j:,,m,,llt ,1,,,.,1 I’tilr 1 1).1(.~w:lrfl 41 Imlll.lt,.tlIi.lmlll ,1,.11 li,rlll}~ 0.Nll**rlm4.Utl . AH ~llllmllll,m pr, -jl,l.1111. {If ! ,,, )WII Vf. li)l, l : v (rljm c!‘J[ -mm-,11 .lm. 1. l..m-lti, nN U:lu Nail) Imltni.l,a(l .111 .ll -Ilmlll,lm f:lr~,.1 pl,ll., pr8. d,, Ul,7!: .1 Uhll!. k Wtv!.

Will,-l! r,li) II]rwmr,l ll)t,) ii ‘1 [i) I I-mm -1111,. k l,i, tl -

~~l:;;,,’~mlll,. ‘;l,,,,,l,, r,l ,1.11,, r,.,l,a,.r [,7,, I ,,4.11-,, 111111)! 1)111,1Ivlll. il .IIIII{. L -.. w.lllullv/ pllr -

f 1, 11, -,..(,l, }(,1 f v ‘I,lt ., u,!,,,, ,1,8,1*I I c1 <1,,1 G,rfl, l ,1,. f 1,,,.It II!* III r III, ,Il:,t,.k-, ,Bmpr,u.1.,,.,1 I),vllt,.,, u. A11[11, {14. 11-.11,1-1111,~ 11.,, illl..ll,, v 1,),11,1,.,1 ;I,l-,it,p,.,1VI I rltum ,IIIImlIIItn, ~,,r,b,.1 (w:l, \l;) l:i,l,*rVll ,4

pll I ,41.I ,,,1,,1,.,1 I I)rm,,, !.’, t 11,. 1111,11.! t Wlnlli, w 1,) ;,

polllll Ill Ill,. 1,,.,,8,,,,, s ,, 1s1 h m,,, It) I r,ltl( ,)1 Ill,1,,.11, 1 Iml,l$. W.11I . 1’11,. r lml,l~ v,.811N..j\4,o. w.t. t ,1,, -I,, lnl, l,bal I;v Ill,, 1110,8,1S1l,18! ,)l.,l, .!.1 I 1,. . llll#,f’-,1,,11 t,!!) ,,1 1 Ilt, ”i,, I.r.ll. r I,,,:lm, 1,1 0.,*8nla4118,1~NIII

Ul!ll ,!: 11)111’,,l!l ill,, I 111110,11,1 IV, r, l):)ll. l,.,l Ill,.

1.11,,1 I 1,1.111 I lm,, ,,,,, ,,, ,l,”,ll, ,1., 111(] ;;., ,), 1,,,. l,,

Impact. A ttme-of-arriwnl pin actlvnied justbefore Lmpact and the appropriate tuma tiel.ayserved to Q .wltch the laser just prior to theshock W~V~ striking the quartz windrxl andafter it wae well past the focal pot.nt OF the

Incident Laser Light.

*tretI;Lng’Wif6 !S’’jjJelm-ihFas”’thg)’YJgJSthreshold for ~tlmulatad Raman scattcclngLrrdllced by 532-rim ltght, and was the transi- ~

tion obnerv! d In these experiments. As

depicted In Ftg. 5, the backward atirnulntedRaman beam wa+ separated from c!],! incidentla~er by mama OE a dlchrolc filter and wmrthen f,,..,]ned onto the 10-p+ide cntrancc alitof a i-m Czerny-Turnur spectrograph equtopedwith a 120f)-groovee/mm grating used in firstorder. Figura 6 Hht}ws the reaulttngspectrogram for benzene shock-compressed to0.92 GPn. The raflected incldcnt Laser Ilneand the bnckwnrd simulated llriLlouLn-scatter-ing Ilne ,at 532 nm Are ohser.~able, as JIre thebackward &timuLated Raman-scattering llnc fromthe shockt!d ~nmp.lc and the huckwurrl ntlm~llncl.rl

rhmndArII\riI lJms

p

f’~ ,

. /-)-# “v%

I

-++

i ,!I,,,,. ! I

IWO? I

I “’

+ p---- 100 cm-l

Iy \532 nm

/ \Arnbien’ ShockedBenzene Benzene

Rrman-sc.~ttering llne from ambient benzene.The Latter Eeature resulted as a consequenceof the shock wave having paaaed only abouttwo-thirds of the way through che sample, andhence a sLlmulated Raman signal wa u alsoobtained from the un~hocked Liquid.

The frequency nhiFt of the Raman linewiLl have emall cnntrlhutlnns of approximatelyo-l cm-l bOca”.q@ the light crosees the m(~v~ng

tnrer[nce hetwecn two mudla of dtffurenc re -

fracc Lve Lndlces and bcca, ww the ,,materi~lbehind the shock wnve wne ml-wing . Sincethc~u crrurs Il;e consldcr:lb Ly less th{ln theexpcrLurtt,lL uncrrcalnty of ~ 0.5 cm-l for the❑ensurud f.equcnry shifts nnd nre J smallfraction IJE the sh[ft duo to comprcsslon, nomttvmpt w.Ie mndc to currect the dat.t fo(. CI1OSPrffrctm.

SIRI,;II ht!am lnt(,n~l.tlr~ uHln~ flSkS aroHltfflrif=ntly lnr:~c ch,ll film cnn ho IlnL.d :!s :1

d,. t,, rt, )r. Thu L,lrgc tnrldvnl lnt,,nsltleqr,!~llll r+,d, huwuvl, r, cm rituun~ tlnmn~r to opt [ cn 1c41mpont!nLH ur.lr [ncn 1 pol nts. Spat lnl nndtrmp,lrl I r,.+,]llltl,,n (T,Ihlu 1) nm d,!tormlnrdhy tllo c,~nlrrrnl pnr;iwwter IIt’ tl, o f,:vltnlng LCI,9nnll 1.111. lnc I &IIIt lnna!r PIIISO dur,ltl,,rt. Thatrlstfs tl. rlllllqllo .11 .7,1 mwFfcrq from LhO dlr-

.,

I/● BSRS

1

,OL ~ -J0,5 I,5

l%essu~ (GPa)

lnrlllO!lt l)(,wf.i It,v,.1.i ,.on!ll(ll,r:lhly 1),. low t11,14,.

rl!t{,ll I.,, d r[lr .4t[ml,l lt~,,l R:lmilll .4r;\Lt,.rli)~~, I)y

ov,, rl. ir.l)l n.! t;lt. pllmp i>a..1m wl tl) ;1 h,,; )m, 98uI,,,I IV.1 hril:ld l~:lnll ql>ulr,.a., It 1111. ant l-.:; l.okfi. b l“r,. -qll,. nf. v. R; L#ll, I( IS?U 1.+ .I, s:tlt(. r,. d l“ra,m Ill!. !)v,I,l,I

1):111.: !,),1rr4. (,*pl,4,:hr.4 .1s; -In .vl],a#>rl]t 1,111) Intn)tilt, l),bmp 1r$.qtl,.!l,.v. N(I tllr,. wlllll,l t!lt,.,l!:llv

,.XI ,r: :1!1 I II tll,, (.,1.11, ,,1” ,.ilrllll. lt. ,.l IP,117,11!!I,. ;li L,, r[n p,, 11(.!l (,!.. CI I,. ,.oml)l. ,ti. I{,lmlll-.lrl Iv,.

sp4. u.trlt,n, W[tll .;1111 11. IP,,, [Ill ,,!l:il Lv I ,;

i]vi. rco,:v, r 1111)r8, rlr..l\t,lh ,tn[l ,11 I]r.r 11.1,.k):rill(ll,l

~.rrlt(.t,l. ,1111.111,1 LIIII:I hII ,vt:4Ji)lc. .

‘; [ 111.1~pll.l ,4,. m.tl,,ltl,l): III 11#11 r,,q,l:rl,,l :1:1 [11

m:lll\, !11 t !11. ,,,lll,,rU.lll t#.,.l,,,l #111,1,, b1140.tl!ll#,,lIIilrr, 11,>1.T:II ,{,~tmm.tr{,, ;Irr,l,}j.,,.,m,,ll II ,,l. I. ,,4,., .

5 [111!,. $pml (.11 ,111#1 I +.np(lr:r I r,,,14tl,ll 1<,41(T:tl) l,. 1) .,I),I!lI.I 1,,, 11,,. ,!llrr:t, r 1,111 !Im,l ,,1

ttl,. 111.11[, II I.lll?lll,lnl .111.1 ,11111 1 1,, ! 1.1n4, r 1) Ill.

li, n~th, rv,ll>u.rl 1 .,,1.,. A 1111 1 (,,111 Iv 41,),.< ,Irl.1(,

Wltl, f 11,1 ll.V,l CI!, Uql,n,t,, 1,.,,1, ,11., 11s. Wilt,ll ,1hr,,.l,ll):lt),l .Iv,, 1,1!1,.1 i 1 11.1,,,1 1011. I 1,,, :111, ...

1)...lm, Il,)ll::l)l),,:l,a ,)r lrrt, \:lil lrlll,,,l III l!ll. 111.-

tl.11.litv 411 I Ill. ,.,J1!I Ii!, :, [m, 11,1!, 1 8, l.t 11!111

‘)%~1).,.;!s,l, !)1 I I\*. tll)l 13., \ l)\ I l},, I ,\.i,>r .), )8{ I \j8. r-.

m:il .,,r 1,11,,111 4 Iu !11,, II-r. .4! r,.:lm, ,.:111 l),, ,)1” III,,

!), ,! 1,.1, !,1 I 118, .11),1! rl, l 1,)11 .11,:11, ! i , I 11,1,1 1,1,.,,.r 1,,1 :

affecting spectral resolution and detection

9enaf.ttvity.

Coheren: antt-Stokes Raman scattering (CARS)

~~~RS)~~!fJPnt StOkeg

Raman scattering

(Fig. 4) occur a9 four-wave para-metric processes in which three waves, cwo at

a pump L’requency and onc aL either the Stokesor ant L-StokeB frequency are mixed in a sampleto prcduce u coherent Eeam at the anti-Stokeeor StO1,es frcquenr.y, reapecttvc+ly. The mixingi$l great Ly crhnced Lf the frequeocv

differ~nc~ between the pump ~nd the Stokes or,nntl-Stokee Erequenc lea colncid=s with a Raman&ctlvc mode GE the sample. Lilce [nverf; e Ramen

r3cattertng, CAkS and CSRS can be produced atLncitlent powLr Luvels considerably below thosurequired fot stimulated Ramnn scattering.h..wevcr, since phase matching 1s required,poa~thLe geomutrlc~t arrangementrr are Limtced.

t..,;~<T+.! Ilm ,,1

,’” b,, ,V,v,.,. .,...:

fiw, !,u ;. . :“..;. - -’ .

,, \,.

quenciea of the s!lock-comprus.eed materials are

not preci-el,y known, and sinca we wlahed t>prod[l~e CAM signals f~am tmre than one ❑odeor epeciea, .a brond-band dye lacer, with .ebandwidth equivalent to thethe dye, wa e ‘sin pr0fi155 0:used as the Stokes beam.portion of the 6 n~ Long frequency doubledNd:YAG Laser pulse was used CO puml~ the dye

la9er. The resulting two Laaer beama (dye andremaining pump) were paased through aeparareGalilean telescopes and sent along parallelpatha tovarde the .anmple. The beam wereEocuaed and creased (with ap,>roxLmateLy 1 mmLength of uverhp) tic a point 4 mm in front of

:g:i:::r ;:::::q::!ti”s;:: ;A:::::y::an:;:

(phnse-matchinR angLe) wae tuned hy trdJustLngthe axial distance between the paraLLcL beam~Uei.ng ~ precLsLon translation stage on the dyc

Laser beam turning prL9m. The CARS beam wasreflt?ccetf out cf the shocked sampl.? by the

highly pullshed front surface of the tnrgetplat{! and ~Long n path pnrallel to chc twotncumin~; benms. Aft~r being mcpnrated Eromthe pump and Stokc~ henms IIslng n LrLIIg-wnJc-lemgth-pirss dlchrolc Elltcr, the hen n was thenpaased chrnugh a dove pri~m and Eoc(lsud ontntllc 75um wldc cntrnncc .LLt of the spc(!tronw -ter. The dove prism wrt:; us,!d to rot:ttc theimn~,: OF tl.c CARS st~nnl cn th.lt any bclmmovt>nwnt rnnllltin~ From th~ cll~ngln R pus i t, 1o11

r)f the ref Lectiufl ~\lrCncc rfllr LnE the shock-

tnmpre~slon prort!s~ Wf)ll I d trnnfi l:ltc to

mov?mont ,Il(]ny,, rnrhi,l. tn., n .~craus, tllc spec -trnmctrr tint r. Inra. ,; LLt. TII[! si~nala were

dotcctod Jt. thC Uxlt ,f the .Ipectrnma. f,!r u:tilnu

n HI llcon-l lltt!nsl flt.,1-rnr:,t!t vldl~f)n ( K(:(;-

PLIC 12051)) couplc!l tn JIn i>pLlr;IL m,lltl-rll.ll\n,.l,an~lljfzer (Ot4\) (ECI; -I’AR l? f)5,\) .

Flp!lr,. ‘) :{huw,I till! OHA rVL?Or,lL1d Klllll:AKS

s [ #;rl:l 1,: fnr C[lt. ring-.4tCrLchlnH morfu~ I1f bL!n-za.nc nn(l ht. t)zcnr-,lt, [n .4 bOZ honzt. n,~, 402bonz(. ut. -,lfi (hy voltlm~) mlxtllre, both at

nmh[cnt c,]nd[t [nnfl ,Ind :!llo~:k-t:f~mplt.swt.d tll0.91 C1’n. i,lwl) +lIl(]wn lM th,. 251.fi~l! I]m 11P,

I lnu in :,u.[:1,,1,1 <,r*lt,r ,iMtis,l .1,4 .I w:ii,c lun):tll r~!l -cronci,. Th(. Nporrr,ll Jntn oht:llnt. d .I!III’LKRll HCAl{S Ilh[)W!l III) l, V[dl!lll!l, f,)r tilt. prou,,11u4.

:;:::::qlk”” “’’”dk “r ““’’)m’’’’’”t’(’” “;;:;;:(,11 conra. nrr:lt lonfl .IIIIIVP tlIII

lCV,. L) havlu}; M:lrnnn net lvr trnlt,+l t Lnno w[ tl)lll

th~! ,vlhr.lt 1,*N4 1 I r,,,~llnncy r<!), lon $lp:lnllt, d hy

thn Hnln pr,}l”t 10 nf the dy,. (1 .,,. hotw,,,.11 HOI)illll Ill]fl ,,m-t). r 11 ,1,1(1I I i,l,l , tll,. !lp,. ,. Lr,l,Iht:l I 11,!,1 for thv mlxtllro:l d,) ll~lr ,.<~nt ,1{,, ,I,,vevldonr,. ror ,1(.1.1,.rlulm oxrh,, nfln. r-,1~.t Intnl!t h,. -

twl. (!n thll hl.nt,!ll,. :Ipa.c 1,.u tlt,r I II,,, th,. .- I ,,:,,Iftor pJtIlnnMIm 1,1 Lhv .!li,~rk . [f I%K,SII:III,:,, 11;1,1

fjcrllrrvd, l’.,~w poak:l W(lllll[ ha. (.q~l,lol)t 111.I WI.ISI\

the 111.II; !ISIIIU;Intl hIUIIt IBIII. -Ii,, I r.ln:l I I 1,.n:~. Fh.11-

n~tro<l vlhr.ltlnnnl rlnp, -nt rot I.11III): fr,,,v,l,.:t,.v

qh! it. % f’or hunl. m,, (dJL.Ilnt,,l ,I,ll!l)! Nllll~. ARS .11!,1

1.11o ~lhi r!.1 m,..l:lllr,.kl 1111[.11: nsn:; ,1:1,: t .Nl,.I [,,,,tlr vhork pr-,l,n,lr,, nrv .,11 bun I 11 )’\;:. l!. ‘rhl.

11.If ~1 :!l(ll,. nL(, q I Ilnl 111!. [WI. Lab,.llll!,llla.,i m#.il!411 r,.

,,(, ,,[., ~l,.,, ( I r,.,lt14.!l,,v !llllrL.. :1t C.II II IJII 14$1)1

Viii,,,’k pr(.~fl[tr{,n. Tempt, r,l I r ..na~ltll la~n I ,1. tllv

I

RBBCARS

$! Shocked

\&

Mixture

Hgcaiibratiarr line

--&_L~ ~

950 900 850

Raman Shift (cm-i)

Fl~llrl? 9. RfLffCARS Spectru 24 “Thn Amhi@nt. PC.I!CPOHttlon# Of The l%o :;puclt?a ,ir[!992 cm-! For Ilt.,lr.rno And qf15 cm-l

For U,:n;:vno-db.

spec Lcs with concencrattons dwm to part-per-

hundred levels shuu!d be poss. ~Le.

~~E;;!4”;:: ~eey::gge,;:fe:: ~’p:;:::::;~:

21technique for performing mea9uremenC.9 in~hock-ccmpreesed 3y9tem9 -xhich may have alarge non-rcsonanr hnckground. Slmllar to Ln-verse-Ram.~n scattering, RIKES requires asingle trequcncy pump b?am. a broad-hand prz.uesource, no phase match. ng nnd lower incidentpower levels than :.tlmulatcd Kammn scattering(Fig. 4). Apprcpri~t: polarlz.ltion of the in-put pump and ,~robe beams results Ln aac#ttl!rcd probe beam whoqe polarization isrotacei -t conditions of Raman reeonancc. An

analyzer placed in ~hc #cattcred probe beamthug .rantimlts light only nt ,ilfferences inErcqumrcy corre-pnnding t,. Raman resonance.This arrnnucment idt=nLly would P,LV.. a largesignll tntennity ~l~ninst a emall brtckg:Jundmaking Lt a good choice For the detrctLon of

9Pacie~ with lMALL concentrations. In shc k.nppLLc,ltion.s, ::nwevt,r, two dlfflcultics could

,arl+c. The strnlnt!d shock-compress{.d silmple

could PxhLbl.c hLreFrlnk,,ncc whicll would rotatethe poL,lr Lzltlorr or’ ;111 nf tic Lncident prnb, !frequenclon, resultln~ Ln n L,lrge unw:lnrv Bi I

backgr.)urlrl. ‘Thu sccnncl pruhlvm arlwt!s in gco - ;

metric ;Irr;]nt:(!mt,nt cnn:)id,:r,nt Lens. Slnco 7poldrlzatlnn ann Lyzur i~ reqllirrd [n thu Ollt -

pllt humm, n ~tralght [lilt! trnnsmisslollarr~w:i’mt,nt l.; thu m(ls t l(,glcnl ch,)l,:c. ,4.~ecnntl CI1OLCU would be :+lmll,ar to Fig. 10 wiLltOptic;ll r.(dnpt)ncnt:i nrr:ln~ed to nll 11 !llly

pnl.lrlz[n~ (.t’fi!t-t.s 0[ tl~~. ruf lrr. cln R :Iurf.n et..

Tompor,~l .In,l spJtl.al rw~,]lutl,ms tor quch .1n

nrr. ttlp.cm,.llt qllnll:ll ht. th,. Iast, r pill 1P ILIIIHLII

,anfl t!lu (11 Ffr. if-rlon Llmlt 111- th(~ nptlc.:11 \.nm-pollrnt,l ll!;l ,11.

Flflurr 11 show!) twn RIKES .4p,. vrT:l fr#lm tw,ldlrf!,ri,nt a,xl),,rlmc,nt,i Or cI:I. 9,1? ,.m-l V14);1$M1OF he I1,ZIIII, I ~ll(>(:k-(:oml)rc?s:;,.,1 to 1 . 17 [;PJ. ~l)Ltl

‘;~. “,Y!W. .I-,,.,4,..!,,.’,

,, .,., ,, .,,

.,,’,,

&.,.@#b ‘ ., .+.,, ,, ‘: \$’ ;,!,1.’

“IJ7, : *,- , ,.W@ .,!

lm* -.L’*.

Aw!n”al ?.,$!. .--r

,Wti 4HIW:C,* ., “ - .7”,;M4 -,!<,

+4.,.’

Fl~,lr,, If). N.IM III 111,1111.ISRIKI. 1,1’ Ill I ,SI.I :~1.11! l,r-

1:1)! l:mp**rlm#,lll -

traces have spectral featuree, however theyare not consistent and do not exhibit thepreesure-induced frequency shift expected for

the benzene rins atretchlng mode based on

previous BSRS and RaBCARS experfmonta. In

addtt Lon the broadband si~nal at the dyefrequency suggests a shock-induced

polarization rotation of the entire pr “m?

beam. The conclusion reached fron theseexperiments 19 Lhat while it may be possibleto perform RIKES in shock-c(,mpregsed maZerL-

els, the experiment will he considerably moredifficult than techniques not requiringpolarized lacer beans (Table I).

If the output bemm of a parametric mixing

proccs:~ is sufficiently strong, it can ‘,!rthermix with ore of th,. Lncirl[!nt hemms anl~ creutea new ourput beam dt yet a different fre-quency. Higher order Raman 9pectraL excLca-

-—. ~ –._‘r___r__——

Benzene RIKES

A

J--/””\~,_.Lmb!n!_....-..J[~-.J_. .. L.... --—-’d-1 . – .1 ____ .....L_

900 1000

llamon 5hift (cm-l)

TASLE [. RAMAN SPECTROSCOPY

—_Temporal Spatial

Technique Resolution Resolution Difficulties Advantageti(119 ) (P)

IncoherentSpontaneous 10 10 Low aensiclvtcy li!nics

temporai and spatial res-

Cot,eren?

Simulated lp-4_l

Inverse 1O-’’-1I-J

Ant l.-stokewSt,)kes (CARS, 10-’’- 1(1

Difficult In high cmis-aion backgro!lnd ,appl. ica -tiona.

L)i:ficult where Fluores-cence or photochemistry

occurs.

10 May requjre emall specie9conccntrat lonfl.

Could have competingfluorescence effectp.

2300 Spatial reeulutton mar-ginal.

High power levels re-qui :ed.

I.lmitcd docection c.lpa-.

billty (single ,Jodc andspecies).

lo(y) I’hn:lc mntrllLng rcqlllre~i.

Can identify .~ibrat!onal.spectra and species.

Can ciea9ure temperature.

Can ldentiEy ,.,ibrationrtl9pectra and 9pecies.

Increased sensitivity com-pared to spontaneous Ramanscattering.

Can tdcntlfy single vthra-:ional speccra.

Good temporal resolutlod.

Scactered beam come~ backalong incident he:im.

Can identify Vibrat lon~lspecr:a :Ind species.

TJ0e9 rot require phase-macchtn~.

Cood SpatL.~1 resolution.

Good Tempor~t resolur.lon.

AIL Raman ,,ctlvc molecul-sand modes scatter.

Nn nnn-t:stmanr lJack-

Uround.

Cnnd Jetrctlon scnslti-Vtty.

All Rmnn artlve nrnlt.r[l!.~a.Ind mnde~ :+c,lttl, r.

-.

Raman Induced 10-’’-10Rerr Effect(R IKES)

10 Sen9 Lt lve to bir9frln- Can identify Vibrational

gence effects. 9peccra and species.

L es not require p},ase

matching.

Good spatial resoluc~on.

Good temporal resolutlnn.

All Raman actl~e moleculesand mode~ scatter.

Other Complicated.

. .—— — —

tion studLcs (HORSES) (Fig. 4) have been u~cdto genernte co;lercnt Yecond Stoket and secondanti-Stokti.s beamo. Other multi-col.r paramet-

ric mixing processes us[ng polarlzed beams

have been used to observe Raman transitions.These cechnlqucs arv generally used tosuoprcqs non-resonant background effeccs. Ob-servation of any of these more compltc,ltedproc23se!l Ln ~tock-comprc~sed ay~tems wILLprobtibly come after some of the techniques

discussed previ,>usLy are further (cvcloped.

Optic:llall~nmenc for :Iny ?echnlque rcquirlngpol~r Lzed hcams wIL1 suruly be di. Eficu Lt.

SUMMAP.Y

Sever,ll spontnn,~oua :Ind coherent Ram,~n 9c it-tering mechnnlgms hnvc buc?n dl.scuascd m+pot-.ntlally vtilu:lblr rfingnostlc tecll,lL~uos fcrdete-mlflf,ng the Str!lctllre anu encrk$, tr:lnsfermech~ni~ms domlnnnt durLng the shnck cnm-prrss inn of cOndenfied-pllnwu mt>ll,ctll.nr systvmsmThu nr~cclc:lllty. n(I-#CIIt. I!:C$+ nn,l ,liq.lllJ.ant,lg,!sof 1,:}1C.\ tt.rl!nlqu,f hnvc been sllmm.lrl .tPv1.

Det,lll,,d !escrlptlun!; of backwnr,l St Lmlll.#ltt,d

Rfiman sc~ltt,?rinb; .Ind r,. f l,~rt,,d l~roa,lb:lnd CII -

hcccnt ant L-Srok, Fq U.lm,ln :;[..ntt,. ring h:i~,e ht.,, ”gi-tcn.

‘rut, f,ln&lm[,ntll Limit.ltl,lns It m,,kln~ ,, Kp,, rt -

mental ma?:lqllrt,ments In thi, r+:filon thr,, ugll .111[1

lmlWdlat!, Ly behinil 4!Inck Fro,lc< ,Ir,, thi, m,l:<l -mum pos Hl!l l., +P(IEI .11 rv9. >1,1[ 11~11w}III-h ,..1,1 h,,

ach Levf>..l .Ind tltl, lncr,>.l:~l,d Il:lu,lti{,ltl] III !.-i~rKempllr 11 lnl..l:lulra.lnaY11t:4. F(~r ~l+[bl,. wm..,,,l,.n; ,,th

(Jpt [Clll m~~.lqilr,, mcntq, tllo l::(. ,( ’tlllll llmit,

,vr ,!p:l~l:li r+.:41>l[ltl,>n, [.4 - l/;? ;,. l.’,1r IIUII!)I -

cnso,:, jnd tt, mp,7r<11 tt.t.hnlqltt.~ , LI)IS !Atl(lwliltll,

,~r ,Ip,.,,tr II r,,:<,l!, Ul ILIII, I .4 tl,lls ,lr

, wa..w.nlt.~l),,r:~ .

In tlII. n,,ir IIltllr.,, +:IV I I..., .:,,.lr+, WI, hl.1 11,:1,I III. rIvI)l IIt ICII1 ,It Unlm.in :1,..art,, v[ni: m,,.la,ll-,,ma,llt,l

I 11 ,., ,,1 ]Ilrl. ,t 1,)11 Wltll ,,11,,,~ .11 ly,llt,,~r II- II, I.l I-,tI,\u,.>* WI 11 on.jl>l~, tIH !.,) I:I,TI ,!rm rll~. I -II I, Iw {II}:,fl,.:l:411rr.,m,lll ,! : (1) ,1,. 1,. rlrll,l,ll 1,,,1 ,)1

/lhr.lti~~n.11 Is ,’r~? 111”.1,.I~ I ‘r m,tny II III,’ i- I. IIm-[,r,..ana.,l mnll,. rl 1,4; (,, ) i 1,.,, [ [! [.,.,, i 1,,,, ,,1 ~,, !,,.

r{ .11 \Ih:I.ll. ~ wtl,,., .al), >,. k -,.,,, n;, ro, .:. <.s. I ; ( 1) I I .,, L I .

f’1 VII 11,1 lclr m,IIIV .mlf,ri II. ,11 ,,lla,,n, a. II

.II).,1.11.:1 r :1111 t IIIP. ! r,)m 11)418.k-[11t1116a, ml #l,”,SBloib#)-

q[l 14111, ll,Jl,;m,,rl.71tl,,ll ,111,1 1.,,,1,. ( 19,,; 1 ‘.) l!. -

terminatf.on of reacrlon-race phenomenology for

shock-compressed materials, (i.e., how dorates and phenomenology change with Iars,G coGl-pre9sLnn.e and high cemperaturea); and (51 mea-surement of some details of shock-front struc-ture possibly providing tnsi2ht regarding theunique features of the shock process. Whenthe result~ of the:;e ❑easurements are couplcclwith pre9ently known information, theposalbilities fo.: Lncrensing our phenomenoloq-ical underwtar.rllng of the shock-~ompresslonprocess are numerous.

The outhorg wish to thank C. W. CaldweLl,R. L. Eaven90n, and C. i. Laguna For theirassistance Ln performing the shockwave u.~peri-mentw and Adele Zlmmermnn and Mnry Ann Lucernfor cyDing the manuscript and preparing manyOr tht: fl~ures.

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