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o 93 (199 ACTA PHYSICA POLONICA A o 1

oceeigs o e Ieaioa Coeece "Quaum Oics I" asowiec oa 1997

EMOSECO IG WAE ACKES

C. RADZEWICZ

Isiue o Eeimea ysics Wasaw Uiesiy oża 9 -1 Wasaw oa

M IEAC YΒ A

eame o Cemisy a ysics e-Guio Uiesiy ee Sea Isae

A J.S. KASISKI

Cee o ase a ooics eseac Okaoma Sae Uiesiy Siwae OK 77 USA

We aaye oagaio o ua so ig uses i a asae is- esie oiea meium A geea omua o emoseco wae acke eouio is eeoe a aie o seciic oems eoeica a eeimea esus o wae acke isoio y eses wae acke o- aio i ieige meia a gou eociy macig i sum equecy geeaio ae esee umeica esus o siig o emoseco wae ackes i isesie Ke meia ae aso esee ACS umes 5 5e

1 Ioucio eeomes i ase moe-ockig eciques uig e as ecae e o geeaio o uses as so as 75 s (1 s = 1 -15 s iecy om isaie ase [1] y emoyig use comessio eciques oe ca aciee ee soe uses wi e cue eco a ess a 5 s ee [ 3] ogess i is ie as ee ey as eseciay i e 7-ies a -ies as iusae i ig 1 wic eses e isoy o ua so use geeaio i e as 5 yeas Oigiay e mos commo emoseco sysems wee ase o ogaic yes as ase mae- ias owee wi a ae o s isaie ases [] i e eay 9-ies a soi sae ecoogy is aaiae Cuey sysems oeaig a -3 s age ae ouie a commecia sysems wi su- s caaiiies ae o e make A emoseco ig use oagaig i a gie meium ca e isuaie as a wae acke o eeco-mageic aiaio a moes wi is gou eociy a a e same ime cages is sae ue o e ieacio wi e meium We i e wae acke icue aeaig a we wi use e wae acke aguage ougou is ae Oe o e simes eeimes wi emoseco ig uses ioes oagaio o suc wae ackes oug a asae meium

(37 238 C. Radzewicz et al.

o eame a oica wiow mae o gass Suc eeimes ae omiese ey ae eome eey ay i ua as oics aoaoies oe wiou a coscious oug o e eeimeais a weee a uaso ig use as o e eiee om e ase sysem o e same a o is way asses oug a es o a gass ce wiow Sice e esu o may eeimes wi ua so ig uses eseciay i a oiea egime sogy ees o e eais o e use suc as is ime a/o saia oeies i is quie imoa o uesa wa aes o suc a use o is way om e ase sysem o e same We cosieig oagaio o a ow iesiy moocomaic ig eam i a ieecic oe oy as o accou o is ie o eacio wic moi- ies e iacio o e eam y cagig e oagaio cosa wi esec o a o acuum Wa makes e oagaio o emoseco uses iee? is y e iue o ei eiy e emoseco uses ae oa secum ecause o a a sigiica use saig is osee weee ey oagae i a isesie meium Seco e eak iesiy ca e quie ig ee wi a moeae use eegy a aeage owe eeoe 3- oe ocesses (aowe i a meium o ay symmey cao e egece o isace iesiy ee- e eacio ie gies ise o se-ase mouaio a se-ocusig wic iuece e secum o e use a is saio-emoa caaceisics esec- iey I is a we-kow eomeo eaig amog oe igs o omaio o oica soios i ies [5 ] a wie ig coiuum geeaio [7] As is oe e case i oiea oems ee eomea iacio isesio a se-ocusig ae eage; oe ca suy ei eecs seaaey oy i a imie ume o cases we oe o em omiaes owee i mos cases umeica meos ae o e emoye as a meo o souio is ae is ogaie as oows I Sec 2 we ese a geea om o e oagaio equaio o a em- emoseco ig Wae ackes 39

oseco wae acke i a asae isesie a oiea meium Secio 3 oies eames o e wae acke saig eecs i a iea egime — o eoeica a eeimea aa ae oie I Sec we aaye oiea oagaio egime a ese e esus o umeica cacuaios iusaig a come wae acke eouio

oagaio equaio We sa y eeseig e scaa eecic ie E( o e ig wae acke as a iega o is ouie comoes

eac caaceie y is amiue (k wae eco k a equecy ω(k Ou o ou aiaes ie equecy a ee comoes o e wae eco a escie eac ouie comoe oy ee ae ieee ecause o e isesio eaio ω = ω(k e we eese e ie amiue as a ouc o a sowy ayig eeoe (SE a a ase aco wee we assume a e wae ecos ae goue aou a cea aue k a coesoigy e equecies om a a aou e cea equecy ω = ω(k is eas o e oagaio equaio o sowy ayig ee- oe [-11]

I e as equaio a ui eg eco s = k/kassume o e i e iecio o cooiae as ee iouce A aiioa em iγ Α Α as aso ee ae I escies e eec o e 3- oe oieaiy (Ke ye oieaiy o e meium e iega oe k ca e eace y a iega oe ω we e isesio eaio is ake io accou wee is e ie o eacio a s = k/ k is aicua om o eessio o aows aicaio o is aoac o o isooic a aisooic meia Sice o assumios aou e om o A( ae ee mae Eq (3 is eac A aia ieeia equaio o A( ca aso e oaie y usig Eq (3

is is oe y eaig / i owes o k x ky a (ω - ω a eacig ese aiaes wi i∂/∂ i/y a -∂/∂t eseciey Keeig ems u o e seco oe gies o a uiaia ieige meium [11] C. aewic e a

e coeicies ß1 = 1/g = ∂k/∂ω a β = ∂β1/∂ω escie e eecs o gou eociy a gou eociy isesio eseciey γ xx a γyy ae e- sosie o e iacio o e wae acke γx eecs eam wak-o i a ieige meium wie γ was ou o e esosie o e oaio o e wae acke [9] I is wo meioig a e coeicies x a γ ais o isooic meium Oe ca easiy geeaie Eq ( y aig ige oe ems o e sake o caiy we wi o o i ee u ae ee a ieese eae o e oigia aes [-11] Eie o e wo equaios (Eq (3 o e eae esio o Eq ( ca e umeicay iegae I sou e oie ou a Eq ( is a aoimaio o Eq (3 a i oe o make em oay equiae oe wou ae o icue ems o a oes io Eq ( is ceay is o a acica aoac We ou owee a i a cases suie e esus o eie aoac ae amos ieica i e ems u o 3- oe ae icue io Eq ( eoe we ese e esus o suc iegaio e us cosie some sime cases

3 iea oagaio 1 - a 3 - eecs is e us aaye Eq ( i a 1-imesioa case Assume a Α( = A( is is e case weee ig oagaes i a sige moe oica ie o e ase eam oeies ae suc a i ca e moee as a oe-imesioa ae wae I is case a eiaies wi esec o a y ais a we ae e wi a we-kow oiea Scöige equaio o e oowig om

is equaio is easy o soe i we kee oy e is em o e ig sie Oe ca eiy a ay ucio A(z, a as a om A(z, /νg cosiues a oe souio is meas a i e owes oe aoimaio a 1-imesioa wae acke ca e o ay sae a i oagaes wiou isoios wi e see equa o e gou eociy i a gie meium I may seem o e a iia sae- me wic i is u a oe wi sigiica cosequeces i may eeimes We wi iusae is wi wo eames e is eame o e aoc a e gou eociy ca ay wi a eeime is a wae acke isoio y eses I as ee ecogie quie a og ime ago a e ieece ewee ase a gou eociies ca ea o sigiica eecs uo oagaio o emoseco uses oug eses [1-13] I a coimae eam ie a a wae acke is ocuse wi a comaic es e e ase suaces ei e es ae seica u e sae o e wae acke is o I e U-isie age e gou eociy is smae a e ase eociy o oica gasses ecause e wae acke oagaes oug moe gass i e cee o e eam wee e es is e ickes i accumuaes moe gou eay a ase eay ee wie a e eges o e es e wo eays ae amos equa As a esu e wae acke ei e es is isoe; is cea a ags ei e eges is i u causes a e iesiy o ig i e ocus o oge oows e iesiy ime oie o e iu use ecause iee aia oes o e wae acke coiue o i a iee imes I is imoa o e ae o measue is isoio eseciay o come eses suc Femtosecond Wave Packets 241

as microscope objectives for which direct calculations may be quite difficult and which are commonly used in applications such as two- microscopy [14]. We have designed an interferometric method to measure the wave packet distortion in lenses [15]. The experimental set-up is shown in Fig. 2. The main part of the system is a modified Michelson interferometer with one arm serving as a reference arm and the other arm including the tested lens L. A collimated beam from a femtosecond Ti:sapphire was used as an input beam. Its diameter was big enough to fill the aperture of the lens. As indicated in the figure, at the output of the interferometer a flat reference wave packet interferes with a wave packet distorted by a double passage through the lens. The interference fringes are visible only in the regions where the two wave packets overlap for a given delay defined by the position of the mirror M1. As this mirror is scanned the fringes appear and disappear in different radial zones of the output beam. A detector placed behind a smahl pinhole was used to measure the fringe visibility at different distances from the beam center. For any given position of the pinhole we measured the delay corresponding to maximum fringe visibility and thus found the shape (we assume cylindrical symmetry) of the distorted wave packet. An example of the results is presented in Fig. 3. It shows the relative group delay as a function of the radial position on a 40x microscope objective. As one can see the parts of the wave packet propagating close to the edges of the lens are advanced by more than 30 fs with respect to the center of the wave packet. We found it quite amusing a a aiio o a coe gass (17 m ick ewee e es a e cue mirror M2 significantly improved the performance of the objective. Apparently the objective has been designed to work with the cover glass! Asa example, consider a mixing experiment with femtosec- ond laser pulses. A crystal with χ( nonlinearity is illuminated by two collinear ua so ase uses wi equecie ω 1 a ω and a sum frequency at ω3 = ω1 + ω is geeae Sice e ee equecies ioe i e ocess are quite different, the group velocities of the corresponding pulses are differ- 242 C. dzz et Ι

e too. ThiS has a detrimental effect on the sum frequency generation process. If ω 1 ≠ ω e g(ω1) ≠ 1 g ('2) in a dispersive medium. As a result the two input pulses propagate with different speeds. This limits the range over which the input pulses overlap which in turn limits the efficiency of the process. In addition, the ouu use a ω3 oagaes a ye aoe (a usuay ey iee see As a esu e ouu use is oge a e iu uses ecause coiuios om iee sices o e cysa aie a e ouu ace a iee imes e ae eec emais ee i e case o seco amoic geeaio (SG we a sige emoseco use is use o ouce aoe use a wice e iu equecy e oem o gou eociy mismac cou e sigiicay aei- ae i a equecy miig sceme wic esues o ase macig (M a gou eociy macig (GM cou e ou We ou a is ca e acu- ay aciee i some cases we ye I o-coiea sum equecy geeaio sceme is aie [1 17] Figure 4 illustrates the basic idea. In the UV-visible range the group ve- locity in nonlinear crystals decreases with increasing frequency and thus the sum equecy use a ω3 ags ei e iig uses a ω 1 a ω eeoe wi a suitable choice of the angles Ψ1 and ψ the projections of vgl, Vg2 and ßg3 on k3 can be made equal. This means that the three pulses have the same components of the group velocity along the propagation direction and they do not separate as they propagate. It is not obvious that group velocity matching and phase match- ing can be achieved in a given crystal for given of the input pulses. Whether this is possible or not depends on dispersion properties of the particu- lar nonlinear birefringent crystal selected. Figure 5 shows the results of numerical cacuaios o β-aium oae (O cysa i e age o uamea wae- egs coesoig o e uaiiy age o isaie emoseco oscia- o wo ocesses ae ee cosiee o-coiea ye I SG (ω + ω → ω and non-collinear type I third harmonic generation (THG) (ω + ω → 3ω e two cases are quite different. For SHG the problem involves solving two equations (phase matching condition and group velocity matching condition) for two vari- aes ψ = Ψ1 = Ψ and O (Θ is an angle between k3 and the optic axis of the crystal) and the solutions are exact if they exist. In the case of THG there are Femtosecond Light Wave Packets 243

3 aiaes Ψ ι , ψ a θ a oy wo equaios ase macig coiio as to be fuhfilled but then group velocity matching is not exact. However, the results of numerical cahculations indicate that the residual group velocity mismatch in our scheme can be small as one percent of that for a standard collinear THG case. As one can see in Fig. 5 PM and GVM conditions can be achieved for SHG in BBO over an entire tuning range of Ti:sapphire laser. Similarly exact PM and approximate GVM are possible for THG process in a somewhat smaller range of wavelengths. C Radzewicz d ad.

I oe o see e eec o GM o equecy miig wi emoseco uses we ae umeicay iegae e oiea equaios o e amiues o e ee ies

wee Α is e amiue ωi — e equecy ni — e eacio ie o e i- ie a βi = ∂ ki/∂ω Α eeece ame moig wi e gou eociy o e ω 1 use is use a βιi = 1/gi — 1/g 1 o i = 3 e esus o e iegaio ae sow i ig Oe ca ceay see a o easoae eeimea coiios e eec o gou eociy mismac is o egigie Seco amoic uses i a GM o-coiea sceme ca e sigiicay soe a ose acieae i a saa coiea sceme is as ee eiie i a eeime eome wi aoimaey 3 og uses om a isaie ase a a 5 mm og O cysa e seco amoic as ee geeae usig wo iee aoaces a saa coiea Femtosecond Light Wave Packets 5

SG a a o-coiea GM SG I eac case e uaio o e seco amoic use as ee measue y iesiy coss-coeaio wi e iu ase use esus o e coss-coeaio measuemes ae sow i ig 7 o e saa coiea sceme e ouu use uaio is amos wice o a o e ase use A e same ime e esus sow a o e GM sceme seco amoic uses a ae soe a e iu ase uses ca e aciee is is o suisig sice i a iea case o SG wiou sauaio oe sou eec

e seco amoic use o e soe a e iu use y a aco o √

As a ia eame o iea oagaio eecs e us cosie a emoseco wae acke oagaig i a ieige isesie meium I e ig oa- gaes as a eaoiay wae e e ems γ a γ i Eq ( ae o-eo Wie e is oe meas a e oyig eco i suc a meium is o aae o e wae eco (a ac kow o a eas a ceuy e eisece a meaig o e seco oe ae ee ou a eaie oy ecey [ 9] umeica iegaio o Eq ( sows a ecause o is em e wae acke wic is igy ocuse we i ees a uiaia ieige cysa oaes aou e ais a is eeicua o e ae eie y oic ais o e cysa a e k eco e eec ca e eaie i a way ey simia o a emoye o eai e wae acke isoio y eses ecause o e ig ocusig e e- 246 C. Radzewicz et al.

aig eam coais wae ecos a om iee ages wi e oic ais o e cysa Sice o a eaoiay wae e ie o eacio ees o is age o ase a gou eociies ae aso ucios o e same age Wa is ee moe imoa e ieece ewee ase eociy a gou e- ociy aies as a ucio o is age As a esu oe sie o e wae acke ags moe ei e ase os a e oe sie wic eas o e wae acke oaio I suc a use is ecoimae ae i eis e cysa i wi ook skewe — wie e ase os wi e eeicua o e iecio o oagaio e wae acke ise wi e o simy ecause e ieece ewee ase a gou eays wi e iee a is oosie sies e eoeica eicios o e wae acke oaio ae ee eiie eeimeay i a se-u [1] simia o e oe sow i ig 2. e se-u as ee ioiie o icue wo ieica 11 eescoes oe i eac am wo 1 mm ick uie cysas ae ee ace oe a e ocus o eac eescoe e wae ackes oagaig i e cysas eeiece oaio as escie aoe We ae ace e cysas i o ams o cace a e isoios o e wae ackes a ae o ue o e oaio i e cysa owee e cysas wee se i suc a way a e wo wae ackes eeiece oaio i oosie iecios a us i o oea eecy i sace y ecoig e ige isiiiy a iee osiios i e ouu eam esus e eay ewee wo ams o e ieeomee we wee ae o measue e wae acke oaio e esus o e eeime (ois ae comae o e eoeicay cacuae wae acke oaio (ie in ig I is cea a ou moe o wae acke oaio is a eas aequae as iicae y e ageeme o is eicios wi e eeimea esus Femtosecond Light Wave Packets 7

o comee ou aaysis o e iea oagaio we sou iey meio e eecs o e gou eociy isesio We e gou eociy isesio em —(i/β∂ Α/∂ is aso icue io e aaysis o Eq (5 e use sae oes o emai cosa uig oagaio Isea ecause iee ouie comoes o e use eeiece iee gou eays e esu is a use wi ayig sae a ime eee equecy I is aoimaio e ig equecy aies ieay wi ime a us e use is sai o ae a iea ci e eec ca e quie seee o isace a 5 s og ouie imie use a 3 m oues is uaio uo oagaio oug 1 mm o use siica e esaig o emoseco uses ue o oagaio i isesie meia meas a i ay gie eeime we cao ake e use uaio o gae Ee i we eiy a e use is so we i eis e ase sysem i ca e quie oge we i ieacs wi ou same simy ecause ee was some gass o e way om e ase o e ieacio egio A aiio o ige oe isesio ems eas o ee moe sigiica use esaig a a oiea ci

oiea oagaio

e us sa agai wi 1-imesioa case e oiea em iγIΑ Α i Eq (5 escies e eec o iesiy eee ie o eacio (A = + γιΑ is iouces a ime eee ase a oiea ci wiou aecig e use sae As a esu ew equecies ae geeae a e use secum oaee Secum oaeig i Ke meia ca e comie wi a gou eociy isesio o ouce uses a ae sigiicay soe a e oigia ase uses i a ecique cae use comessio [19] We o gou eociy isesio a Ke oieaiy ems ae icue e e esu ees o e sigs o β a coeicies I e wo emS ae e same sig e ci ue o isesio a e oe ue o Ke oieaiy ae e same sig oo As a esu e use eeieces esaig a a comie ci O e oe a i sg(β = -sg(γ e ee eis sae souios o e oagaio equaio [5] Suc souios ae cae oica soios ecause ey ca oagae oe og isaces i oica ies wiou cages i sae ey ae o aicua iees o egiees esigig oica commuicaio sysems I oe o e eeimes i is ie icoseco uses ae ee oagae i a ie o eg 1 1 11 m ie ue a om e Ea o e Su [] I a 3- case e ieay ewee isesio a oieaiy is augmee y a aiioa eec amey a comeiio ewee iacio a se-ocusig Wie e is es o icease e asese imesios o e wae acke e ae oes eacy e oosie I as ee kow o a eas 3 yeas [1] a o og uses e uimae ae o a eam oagaig i a Ke meium is eemie y is owe Ρ o P < Pc (Ρc is cae ciica owe a ees o e meium oeies oy iacio wis a e eam eocuses I owee P > Pc se-ocusig eais a caasoic eam coase is osee is is o ue o emoseco uses As as ee oie ou y seea gous [-5] i is case oe as o ake io accou isesio eecs as we ecause o a e wae acke wi a owe ige a e ciica owe oes o coase; C dzz t l isea i uegoes a come eouio o i ime a sace I oe o iusae is eouio e us u ack o Eq ( o a wae acke a is Gaussia o i ime a asese saia isiuio oagaig i a isooic meium i is coeie o ewie Eq ( i a sigy iee om [11]

wee ee ew aamees a o eg imesio ae ee iouce is- esio eg s = τ /β iacio eg = γw/ = πw/λ a oiea eg = (γΑ -1 wi τ w a Α eig e uaio as- ese sie a amiue o e wae acke eseciey e aaage o suc scaig is a i oies ee aamees a ca e easiy comae o eac oe wic i u eaes oe o eauae e seg o e ee eomea ey eese (e smae e coeicie e moe imoa e coesoig em i Eq (7 e meaig o ese aamees is as oows Ld is a isace emoseco ig Wae ackes 9

wic akes e use o oue is uaio ecause o e meium isesio Ldf is e isace equie o e use o oue is aea as a esu o iac- io a is e se-ocusig isace o asae meia e iequaiy

Lds » Ln! Ldf yicay os I meas a e isesio eecs cosiue oy a sma coecio o e asic wae acke eouio eie y iacio a se-ocusig owee e esus o iegaio o Eq (7 sow a sma as i is e isesio ays a cucia oe i oagaio o a emoseco wae acke A eame o e wae acke eouio oaie y iec iegaio o Eq (3 is sow i ig 9 (e esus wee ey simia we Eq (7 wi 3- oe ems icue was iegae I is aicua case i was assume a e wae acke sie i ey iecio is muc age a is sie i e iecio is o oy mae e comuaio sime u aso eae us o ese e esus as a 3- gas e oowig aamees ae ee assume maeia — use siica (s = mm use uaio — s use waeeg — m eam sie — 3 m ( = mm use iesiy — 7 GW/c ( = mm e owe o e eam is aou A og use o is owe wou se-ocus a coase owee e emoseco wae acke cosiee ee isays a quie iee eaio I sas o se-ocus as iicae y e eogae sae i ig 9a u e e ocess is aese a e use sis io wo uses as sow i igs 9c a I is isucie o ook a e saio-emoa secum o e wae acke sow i ig 1 Saig om a smoo Guassia sae e 5 C Radzewicz et al. secum eoes oug a "Meica a" sucue (ig 1c a e eeos ee saia oes e cea oe (aou k = coais wo eaks i e equecy isiuio oe a e equecies owe a e iu use equecy a aoe wic is sie owas ige equecies e wo sie oes ae oa seca ceee a e iu use equecy e esus ee as oe mig eec o a oiea oem o a aicua coice o aamees o eame e sig a magiue o e β coemcie u om e umeica iegaio esus some geea cocusios aou e oe o e isesio ca e aw o e case iusae i igs 9 a 1 e ocess sas wi e se-ocusig e se-ocusig is e soges a c = (ig 9a simy ecause e iesiy is e iges ee us e iesiy a e cee o e wae acke iceases aiy a so oes e wi o secum ue o se-ase mo- uaio Oce e secum is oa eoug e isesio sis owe equecies owas e ea o e use a ige equecies owas is ai is owes e iesiy a e cee o e wae acke a ees i om a coase A e same ime e a o e wae acke a as ee ocuse sogy iacs o om e sie oes i e secum as iscusse aoe e use siig sow i ig 9 as ee ecey osee i a eeime [] I cocusio we ae aaye some asecs o iea a oiea o- agaio o emoseco ig wae ackes i asae isesie oiea meia I aicua we ae sow e eecs o gou eociy o oagaio o suc wae ackes oug eses wae acke oaio i ieige meia a sum equecy geeaio wiou gou eociy mismac umeica esus sowig wae acke siig wee aso esee

eeeces

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