Ultrafast Phenomena V Proceedings of the Fifth O S A Topical Meeting Snowmass, Colorado, June 16-19,1986

Editors: G.R. Fleming and A.E . Siegman

With 427 Figures

Springer-Verlag Berlin Heidelberg New York London Paris Tokyo

Contents

P a r t I M o d e L o c k i n g and U l t r a s h o r t Pulse Generat ion

Passive and H y b r i d Femtosecond O p e r a t i o n o f a L inear A s t i g m a t i s m Compensated Dye Laser B y J . - C . Die ls , N . Jamasb i , and L . Sarger ( W i t h 1 F igure ) 2

G e n e r a t i o n of 55-fs Pulses and Var iab le Spectra l W i n d o w i n g i n a L i n e a r - C a v i t y Synchronously P u m p e d cw Dye Laser B y M . D . D a w s o n , T . F . Boggess, D . W . Garvey, and A . L . S m i r l ( W i t h 4 Figures ) 5

C a v i t y - M i r r o r Dispers ion Dependence of Pulse D u r a t i o n Generated f r o m a Simple C P M Laser: A n E x p e r i m e n t a l Study B y M . Y a m a s h i t a , K . Tor i zuka , T . Sato, and M . Ishikawa ( W i t h 2 Figures) 8

Femtosecond Pulse Generat ion f r o m Passively M o d e Locked Cont inuous Wave Dye Lasers 550-700 n m B y P M . W . French and J .R . Tay lo r ( W i t h 3 Figures) 11

S t a b i l i s a t i o n o f a C P M Dye Laser Synchronously P u m p e d by a Frequency D o u b l e d M L Y A G Laser B y J . Chesnoy and L . F i n i ( W i t h 3 Figures) 14

F l u c t u a t i o n s and C h i r p in Co l l id ing -Pulse Mode-Locked D y e Lasers. B y D . Kühlke, Τ . Bonkho fer , U . Herpers , a n d D . von der L i n d e ( W i t h 2 Figures) 17

E x p e r i m e n t a l Observat ion o f H i g h O r d e r Solitons in a C o l l i d i n g Pulse Mode-Locked Laser B y F . Sa l in , P. Grang ier , G. Roger, and A . B r u n ( W i t h 4 Figures) 20

Advances in the T h e o r y of M o d e - L o c k i n g by Synchronous P u m p i n g . B y G . H . C . New and J . M . C a t h e r a l l ( W i t h 3 Figures) . . . 24

Col lect ive Modes - A n A n a l y t i c a l M o d e l for A c t i v e M o d e L o c k i n g i n the Transient Case B y P. Aechtner , P. He inz , and A . Laubereau ( W i t h 2 Figures) 27

VII

G e n e r a t i o n of Picosecond Pulses f r o m a Cont inuous Wave N e o d y m i u m : P h o s p h a t e Glass Laser B y L . Y a n , J . D . L i n g , P . -T . H o , a n d C . H . Lee ( W i t h 3 F igures ) . . . . 30

P a r t I I U l tra fast O p t i c a l G e n e r a t i o n and M e a s u r e m e n t Techniques

F o u r i e r T r a n s f o r m Picosecond Pulse Shaping and Spec t ra l Phase Measurement i n a G r a t i n g Pulse-Compressor . B y J .P. H e r i t a g e , A . M . Weiner , and R . N . T h u r s t o n ( W i t h 4 F igures ) 34

Picosecond Pulse A m p l i f i c a t i o n U s i n g Pulse Compress ion Techniques. B y D . S t r i c k l a n d , P. M a i n e , M . B o u v i e r , S. W i l l i a m s o n , and G. M o u r o u ( W i t h 4 Figures) 38

New O p t i c a l Design for a Jet A m p l i f i e r . B y O. S e d d i k i , A . G o d d i , R. M o u n e t , J . - F . M o r h a n g e , and C. H i r l i m a n n ( W i t h 2 F igures ) . . . 43

F i b e r R a m a n A m p l i f i c a t i o n So l i ton Laser ( F R A S L )

B y M . N . I s l a m , L . F . Mo l l enauer , a n d R . H . Stolen ( W i t h 4 Figures ) 46

Dispers ion Compensated F i b e r R a m a n Osc i l la tor B y J . D . K a f k a , D . F . H e a d , and T . Baer ( W i t h 2 F igures ) 51 80-fs So l i ton - l ike Pulses f r o m an O p t i c a l N o n l i n e a r F i b e r Resonator . B y B . Zysset, P. B e a u d , W . Hödel , a n d H . P Weber ( W i t h 4 Figures) 54

T h e Stabi l i zed So l i ton Laser B y F . M . Mi t s chke and L . F . M o l l e n a u e r ( W i t h 4 F igures ) 58

T h e So l i ton Self Frequency Shi f t . B y F . M . M i t s c h k e , L . F . M o l l e n a u e r , and J . P G o r d o n ( W i t h 2 F igures ) 62

Sol i tons at t h e Zero Dispers ion Wavelength o f S ing le -Mode Fibers B y P . K . A . W a i , C R . M e n y u k , H . H . C h e n , and Y . C . Lee ( W i t h 1 F i g u r e ) 65

A c t i v e M o d e - L o c k i n g of an I n G a A s P O p t i c a l - F i b e r R i n g Laser B y G . Eisenste in , R . M . Jopson, M . S . W h a l e n , K . L . H a l l , a n d G. R a y b o n ( W i t h 4 Figures ) 68

Femtosecond Resolved Fluorescence B y W . R u d o l p h a n d J . - C . Diels ( W i t h 2 F igures ) 71

P a r a m e t r i c A m p l i f i c a t i o n S a m p l i n g Spectroscopy (PASS) : A New Technique for Reso lv ing N e a r - I n f r a r e d Luminescence on a Subpicosecond T i m e Scale. B y D . H u l i n , A . M i g u s , A . A n t o n e t t i , I . L e d o u x , J . B a d a n , a n d J . Zyss ( W i t h 3 F igures ) 75

VIII

Measurement o f Opt i ca ] Phase w i t h Subpicosecond Reso lut ion by T i m e D o m a i n In ter f e rometry . B y J . E . R o t h e n b e r g ( W i t h 6 F igures ) 78

Rea l T i m e Picosecond O p t i c a l Oscilloscope B y J . A . V a l d m a n i s ( W i t h 8 Figures) 82

B e a m O v e r l a p for L o n g Delay Lines Us ing A c t i v e Feedback B y C. D o l a n d , W . B . Jackson, and A . Andersson ( W i t h 3 Figures) . 86

U l t r a s h o r t Dye Laser Pulses U s i n g the Sweeping O s c i l l a t o r M e t h o d . B y Y . H . Meyer , M . M . M a r t i n , E . B r e h e r e t , a n d 0 . Benois t d ' A z y ( W i t h 4 Figures) 89

A n I n v e s t i g a t i o n on U l t r a s h o r t L i g h t Pulse G e n e r a t i o n by Trave l l ing -Wave A m p l i f i e d Spontaneous E m i s s i o n B y W . Lee, C. N i n g , Z. H u a n g , a n d W . W a n g ( W i t h 5 Figures) . . . 92

P a r t I I I E lectroopt ic S a m p l i n g Techniques

E l e c t r o o p t i c S a m p l i n g o f G a l l i u m Arsen ide I n t e g r a t e d C i r c u i t s B y K . J . W e i n g a r t e n , M . J . W . R o d w e l l , J . L . F r e e m a n , S.K. D i a m o n d , and D . M . B l o o m ( W i t h 6 F igures ) 98

Picosecond C h a r a c t e r i z a t i o n of U l t r a f a s t Phenomena : New Devices and New Techniques. B y D .R . D y k a a r , R. Sobolewski , J . F . W h i t a k e r , T . Y . Hs iang , G .A . M o u r o u , M . A . H o l l i s , B . J . C l i f t o n , K . B . Nichols , C O . Bozler , and R . A . M u r p h y ( W i t h 4 Figures) 103

Precise Measurement of Signal P r o p a g a t i o n Character is t i cs i n G a A s I n t e g r a t e d C i r c u i t s by Picosecond E l e c t r o - O p t i c Sampl ing B y R . K . J a i n , X . - C . Zhang , M . G . Ressl, and T . J . P ier ( W i t h 2 Figures) 107

P r o p a g a t i o n o f U l t r a s h o r t E lec t r i ca l Pulses on Superconduct ing Transmiss ion Lines B y L N . D u l i n g I I I , C . - C C h i , W . J . Gal lagher , D . Grischkowsky, N . J . Halas , M . B . K e t c h e n , and A . W . Kleinsasser ( W i t h 4 Figures) 110

H i g h R e p e t i t i o n Rate E l e c t r o - O p t i c S a m p l i n g w i t h an I n j e c t i o n Laser. B y A . J . Tay lor , R.S. Tucker , J . M . Wiesenfe ld , G. Eisenste in , and C A . B u r r u s ( W i t h 5 Figures) 114

Picosecond Optoe lec tronic Sampl ing of E l e c t r i c a l Waveforms Produced by an O p t i c a l l y E x c i t e d F i e l d Effect Trans i s tor B y D . E . Cooper and S . C Moss ( W i t h 1 F i g u r e ) 117

IX

Picosecond E l e c t r i c a l Pulses i n Microe lec t ron i cs . B y P G . M a y , G . P L i , J . - M . H a l b o u t , M . B . K e t c h e n , C.-C. C h i , M . Scheuermann, I . N . D u l i n g I I I , D . Grischkowsky, a n d M . S m y t h ( W i t h 3 F igures ) . 120

H i g h Speed C i r c u i t Measurements Us ing Photoemiss ion S a m p l i n g B y J . B o k o r , A . M . Johnson , R . H . Storz , and W . M . S impson ( W i t h 2 Figures ) 123

Photoemiss ive S a m p l i n g o f Picosecond E l e c t r i c a l Waveforms B y A . M . Weiner , R . B . M a r c u s , P.S.D. L i n , a n d J . H . Abeles ( W i t h 5 Figures ) 127

Non l inear Responses o f Picosecond Photode tec tors t o Photogenerated Carr i e r s B y T . F . C a r r u t h e r s a n d J . F . Weiler ( W i t h 3 F igures ) 131

D i r e c t Generat i on o f Picosecond t o Subpicosecond O p t i c a l Pulses U s i n g E l e c t r o o p t i c M o d u l a t i o n M e t h o d s B y T . Kobayash i , A . M o r i m o t o , T . F u j i t a , K . A m a n o , T . U e m u r a , a n d T . Sueta ( W i t h 6 Figures) 134

E l i m i n a t i o n o f D y n a m i c F lash i n a Picosecond Streak Image T u b e B y H u a n w e n Zhang ( W i t h 1 F igure ) 137

P a r t I V Nonl inear Optics and C o n t i n u u m G e n e r a t i o n

P a r a m e t r i c C h i r p Reversal and Enhancement : A p p l i c a t i o n i n Femtosecond Opt i cs . B y A . Piskarskas, D . Podenas, A . Stabinis , A . Umbrasas , A . Varanavichius , A . Yankauskas, and G. Yonushauskas ( W i t h 7 Figures) 142

S u p e r c o n t i n u u m Generat ion i n Gases: A H i g h O r d e r Nonl inear Opt i cs Phenomenon . B y P B . C o r k u m , C. R o l l a n d , and T . Sr inivasan-Rao ( W i t h 3 Figures) 149

New E x c i t a t i o n and Probe C o n t i n u u m Sources for Subpicosecond A b s o r p t i o n Spectroscopy B y J . H . G l o w n i a , J . Misewi ch , and P.P. Sorok in ( W i t h 2 Figures) . 153

I n d u c e d Phase M o d u l a t i o n and Spectral B r o a d e n i n g o f a Weak 530-nm Picosecond Pulse by an Intense 1060-nm Picosecond Pulse i n Glass. B y R .R . A l f a n o , Q .X . L i , T . J i m b o , J . T . Manassah , and P.P. H o ( W i t h 2 Figures) 157

T h e Observat ion of C h i r p e d S t i m u l a t e d R a m a n Scat tered L i g h t i n F ibers . B y A . M . Johnson, R . H . Sto len, a n d W . M . S impson ( W i t h 3 Figures ) 160

X

O b s e r v a t i o n o f 7 .2-THz Beats Between the D-L ines o f A t o m i c R b B y J . E . G o l u b and T . W . Mossberg ( W i t h 1 F i g u r e ) 164

Coherent M u l t i p h o t o n Resonant I n t e r a c t i o n a n d H a r m o n i c G e n e r a t i o n . B y A . Mukher j ee , N . M u k h e r j e e , J . - C . Die ls , a n d G. A r z u m a n y a n ( W i t h 4 Figures) 166

U l t r a f a s t Chaos f r o m Semiconductor Lasers. B y Y . C h o , T . U m e d a , I . J u n Cha , M . K o i s h i , and M . M i w a ( W i t h 5 Figures) . 169

P a r t V Applications to Semiconductors , Q u a n t u m Wells , and Solid State P h y s i c s

T h e r m o d y n a m i c s and Kinet ics o f M e l t i n g , E v a p o r a t i o n and C r y s t a l l i z a t i o n , Induced by Picosecond Pulsed Laser I r r a d i a t i o n B y F . Spaepen ( W i t h 1 F igure ) 174

I n v e s t i g a t i o n o f N o n t h e r m a l P o p u l a t i o n D i s t r i b u t i o n s w i t h 10-fs O p t i c a l Pulses. B y C .V . Shank, R . L . Fork , C . H . B r i t o C r u z , a n d W . K n o x ( W i t h 3 Figures) 179

Superheat ing D u r i n g U l t r a f a s t Laser H e a t i n g o f Semiconductors B y D . v o n der L i n d e , Ν. Fabr ic ius , Β. D a n i e l z i k , a n d P. Hermes ( W i t h 4 Figures) 182

N o n - e q u i l i b r i u m Carr iers in G a A s : Secondary E m i s s i o n D u r i n g t h e F i r s t T w o Picoseconds By J . A . K a s h a n d J . C . Tsang ( W i t h 5 F igures ) 188

U l t r a f a s t C a r r i e r Dynamics i n G a A s and A l x G a 1 _ x A s B y W . Z . L i n , J . G . F u j i m o t o , E.P. I p p e n . and R . A . Logan ( W i t h 4 Figures) 193

Subpicosecond O p t i c a l Non- l inear i t i es i n G a A s M u l t i p l e - Q u a n t u m -Wel l S t r u c t u r e s . B y D . H u l i n , A . A n t o n e t t i , A . M i g u s , A . M y s y r o w i c z , H . M . Gibbs , N . P e y g h a m b a r i a n , W . T . Masse l ink , and H . M o r k o g ( W i t h 5 Figures) 197

Picosecond R e l a x a t i o n of N o n t h e r m a l W a n n i e r E x c i t o n s i n GaAs B y L . Schultheis , J . K u h l , A . H o n o l d , and C . W . T u ( W i t h 1 F igure ) 201

Picosecond Observat ion of the Pho tore f rac t i ve Effect i n GaAs B y A . L . S m i r l , G .C . Valley, M . B . K l e i n , K . B o h n e r t , and T . F . Boggess ( W i t h 2 Figures) 203

XI

Time-Reso lved Photo luminescence Measurements i n A l x G a 1 _ x A s U n d e r Intense Picosecond E x c i t a t i o n B y K . B o h n e r t , Η. K a l t , D . P N o r w o o d , Τ .F . Boggess, A . L . S m i r l , a n d R . Y . L o o ( W i t h 2 Figures) 207

Picosecond E x c i t e - P r o b e and Trans ient G r a t i n g Studies o f G a x I n 1 _ x A s y P 1 _ y . B y R . J . M a n n i n g , A . M i l l e r , A . M . Fox, a n d J . H . M a r s h ( W i t h 2 Figures) 210

U l t r a f a s t D y n a m i c s i n G a A l A s D i o d e Laser A m p l i f i e r s B y M . S . S t i x , M . P Kesler , and E.P. I p p e n ( W i t h 8 F igures ) 213

E l e c t r o n i c Energy R e l a x a t i o n and L o c a l i z a t i o n i n T w o I I - V I C o m p o u n d Semiconductor Q u a n t u m Wel l Structures B y Y . Hefetz , W . C . Goltsos, D . Lee, and A . V . N u r m i k k o ( W i t h 6 Figures ) 218

T r a n s i e n t R a m a n Scat ter ing i n M u l t i p l e Q u a n t u m W e l l S tructures B y D . Y . O b e r l i , D . R . Wake, M . V . K l e i n , J . K l e m , a n d H . M o r k o g ( W i t h 2 Figures) 223

Fast E n e r g y R e l a x a t i o n of H o t Electrons i n B u l k G a A s a n d M u l t i -Q u a n t u m Wells . B y C . H . Yang and S.A. L y o n ( W i t h 2 Figures) . . . 227

Picosecond Photo luminescence and Energy-Loss Rates i n G a A s Q u a n t u m Wells U n d e r H i g h - D e n s i t y E x c i t a t i o n B y T . Kobayash i , H . U c h i k i , Y . A r a k a w a , and H . Sakaki ( W i t h 4 Figures) 231

B r o a d T u n i n g o f the Photo luminescence Energy and L i f e t i m e by t h e Q u a n t u m - C o n f i n e d Stark Effect . B y H . - J . P o l l a n d , L . Schultheis , J . Kühl , E .O . Göbel , and C . W . T u ( W i t h 2 Figures ) 234

A u g e r H e a t i n g of Si l i con-on-Sapphire by Femtosecond O p t i c a l Pulses . B y M . C . D o w n e r and C.V. Shank ( W i t h 2 F igures ) 238

T h e O r i g i n o f Picosecond P h o t o i n d u c e d A b s o r p t i o n Decays i n H y d r o g e n a t e d A m o r p h o u s Sil icon B y W . B . Jackson, C. D o l a n d , and C.C. T s a i ( W i t h 2 F igures ) 242

Picosecond Decay of P h o t o i n d u c e d A b s o r p t i o n i n H y d r o g e n a t e d A m o r p h o u s Si l i con B y D . M . Rober t s a n d T . L . Gustafson ( W i t h 2 F igures ) 245

Femtosecond Spectroscopy of H o t Carr iers i n G e r m a n i u m B y P . M . Fauchet , D . H u l i n , G . H a m o n i a u x , A . Orszag, J . Kolodzey , a n d S. Wagner ( W i t h 3 Figures) 248

XII

Sp in D ephas i ng Kinet i cs of Free Carr iers i n A l l o y Semimagnet ic Semiconductors C d j _ x M n x S e by One and T w o P h o t o n E x c i t a t i o n B y M . R . J u n n a r k a r and R.R. A l f a n o ( W i t h 1 F igure ) 251

D e t e c t i o n o f Higher Order Fourier Components o f Index G r a t i n g s i n Picosecond Transient G r a t i n g E x p e r i m e n t s B y E . O . Göbe l and H . Saito ( W i t h 3 F igures ) 254

T r a n s i e n t Thermoref lectance Studies of T h e r m a l T r a n s p o r t i n C o m p o s i t i o n a l l y M o d u l a t e d M e t a l F i l m s . B y G . L . Eesley, C . A . Paddock , and B . M . Clemens ( W i t h 2 Figures) 257

Femtosecond Studies of N o n e q u i l i b r i u m Elec t ron i c Processes i n M e t a l s . B y R . W . Schoenlein, W . Z . L i n , J . G . F u j i m o t o , a n d G . L . Eesley ( W i t h 4 Figures) 260

T ime-Reso lved Observat ion of E l e c t r o n - P h o n o n R e l a x a t i o n D u r i n g Femtosecond Laser Heat ing o f Copper . B y H . E l s a y e d - A l i , M . Pessot, T . N o r r i s , and G. M o u r o u ( W i t h 2 F igures ) 264

Femtosecond C a r r i e r Re laxat i on i n Semiconduc tor -Doped Glasses B y M . C Nuss, W . Z i n t h , and W . Kaiser ( W i t h 2 Figures ) 267

Femtosecond Dynamics o f E lec t ron -Ho le P lasma i n Semiconductor M i c r o c r y s t a l l i t e Doped Glass. B y C R . O l b r i g h t , B . D . Fluegel , S .W. K o c h , and N . Peyghambar ian ( W i t h 2 F igures ) 270

H i g h - C o n t r a s t U l t r a f a s t Phase C o n j u g a t i o n i n Semiconductor -D o p e d Glass. B y D . C o t t e r ( W i t h 3 Figures) 274

Femtosecond V i b r a t i o n a l Re laxat i on of the F \ Center i n L i F B y W . H . K n o x , L . F . Mo l l enauer , and R . L . Fork ( W i t h 2 Figures) . 277

D e t e r m i n a t i o n of the R a p i d Quenching Rates of E x c i t e d State F-Centers by O H ~ Defects i n K C l . B y D u - J e o n J a n g , T . C C o r c o r a n , M . A . El -Sayed, L . Gomes, a n d F . L u t y ( W i t h 4 Figures) 280

P r o p a g a t i o n of Coherent Phonon Po lar i tons i n L i T a 0 3 Measured by FIR-Cherenkov-Pulses B y M . C . Nuss and D . H . A u s t o n ( W i t h 3 F igures ) 284

P a r t V I C h e m i c a l React ion D y n a m i c s

Cages, Crossings and Corre lat ions - T h e o r e t i c a l Perspectives on So lut i on React ion D y n a m i c s . B y J . T . Hynes 288

XIII

P o l a r i t y Dependent B a r r i e r s and the P h o t o i s o m e r i z a t i o n D y n a m i c s o f Po lar Molecules i n S o lu t i o n . B y J . M . Hicks , M . T . Vandersa l l , E . V . S i t z m a n n , and K . B . Eisenthal ( W i t h 3 F igures ) 293

D y n a m i c Solvent Effects on Smal l B a r r i e r I somer izat ions B y P .F . B a r b a r a and V . Nagara jan ( W i t h 3 F igures ) 299

Solvat ion D y n a m i c s i n Po lar L i q u i d s : E x p e r i m e n t and S i m u l a t i o n B y M . M a r o n c e l l i , E . W . Castner , J r . , S.P. Webb , a n d G.R. F l e m i n g ( W i t h 4 Figures) 303

Femtosecond S tudy o f E l e c t r o n L o c a l i z a t i o n a n d So lvat ion i n P u r e Water . B y Y . G a u d u e l , J . L . M a r t i n , A . M i g u s , N . Y a m a d a , a n d A . A n t o n e t t i ( W i t h 2 Figures) 308

T i m e - D e p e n d e n t Fluorescence Shi f t i n A lcoho l i c Solvents: A Non-Debye Behav iour Related t o H y d r o g e n Bonds B y C. R u l l i e r e , A . Declemy, and P h . K o t t i s ( W i t h 4 Figures ) 312

Picosecond D y n a m i c s o f P r o t o n - A n i o n I o n P a i r G e m i n a t e R e c o m b i n a t i o n . B y D . H u p p e r t a n d E . Pines ( W i t h 1 F i g u r e ) 315

E x c i t e d State P r o t o n Transfer i n M a t r i x Iso lated W a t e r and M e t h a n o l Complexes o f 2 -Hydroxy -4 ,5 -benzotropone a n d 3 -Hydroxyf lavone B y D . F . Ke l l ey and G . A . Brucker ( W i t h 2 Figures ) 319

Detec t i on o f t h e I n v e r t e d Region i n P h o t o - i n d u c e d I n t r a m o l e c u l a r E l e c t r o n Transfer . B y R . J . H a r r i s o n , G.S. B e d d a r d , J . A . Cowan , and J . K . M . Sanders ( W i t h 2 Figures ) 322

U l t r a f a s t Studies Designed t o Test t h e F u n d a m e n t a l S t a t i s t i c a l Assumpt ions U n d e r l y i n g Chemica l R e a c t i v i t y i n L i q u i d s B y C .B . H a r r i s , J . K . B r o w n , M . E . Paige, D . E . S m i t h , and D . J . Russell ( W i t h 4 Figures) 326

Geminate R e c o m b i n a t i o n and R e l a x a t i o n o f Condensed Phase Molecu lar Halogens B y D . F . Kel ley and N . A . A b u l H a j ( W i t h 1 F i g u r e ) 330

Fast Photochemica l Processes o f A r o m a t i c N i t r o C o m p o u n d s in So lu t i on . B y B . B . C r a i g , S.K. C h a t t o p a d h y a y , and J . C . M i a l o c q ( W i t h 4 Figures) 334

Cage Recombinat i on and U n i m o l e c u l a r /?-Scission React ions o f Sul fur Centered Free Radicals B y T . W . Scott and S.N. L i u ( W i t h 3 F igures ) 338

XIV

T h e I n f l u e n c e of F r i c t i o n and D e u t e r a t i o n on St i lbene I s o m e r i z a t i o n . B y S.H. Courtney , M . W . B a l k , S. Canonica , S.K. K i m , a n d G.R. F l e m i n g ( W i t h 3 Figures) 341

K r a m e r s - H u b b a r d A p p r o a c h t o the Solvent Dependence of I s o m e r i z a t i o n . B y M . Lee and R . M . Hochstrasser ( W i t h 3 Figures) 344

P h o t o i s o m e r i z a t i o n Studies o f S u b s t i t u t e d Sti lbenes: 4,4 ' -D i h y d r o x y s t i l b e n e and 4 ,4 ' -D imethoxy st i lbene B y D . M . Zeg l insk i and D . H . Waldeck ( W i t h 2 Figures) 347

Picosecond Studies of Barrierless Tors iona l Di f fus ion B y D . B e n - A m o t z and C .B . H a r r i s ( W i t h 2 Figures) 350

T i m e - R e s o l v e d Fluorescence Spectra of E t h i d i u m B r o m i d e B y J . H . S o m m e r , Τ . Μ . N o r d l u n d , Μ. M c G u i r e , a n d G. M c L e n d o n ( W i t h 3 F igures ) 353

Picosecond a n d Femtosecond M o l e c u l a r Beam C h e m i s t r y : Coherence a n d Fragment Recoi l D y n a m i c s By A . H . Zewai l ( W i t h 4 Figures) 356

Picosecond Laser Study of the Collisionless U V Photod issoc ia t i on of E n e r g e t i c M a t e r i a l s By J . - C . M i a l o c q and J . C . Stephenson ( W i t h 3 Figures) 362

E x p e r i m e n t a l S tudy of H a r m o n i c Generat i on w i t h Picosecond 248 n m R a d i a t i o n . B y T .S . L u k , A . M c P h e r s o n , H . J a r a , U . J o h a n n , I . A . M c l n t y r e , A . P . Schwarzenbach, Κ. Boyer , and C . K . Rhodes ( W i t h 2 Figures) 366

T ime -Reso lved Measurement of Laser - Induced D e s o r p t i o n of a M o l e c u l a r Monolayer . B y G . A r j a v a l i n g a m , T . F . H e i n z , and J . H . G l o w n i a ( W i t h 1 F igure ) 370

P a r t V I I D y n a m i c s of Biological Processes

Picosecond E l e c t r o n Transfer and S t i m u l a t e d Emiss ion i n Reac t i on Centers o f Rhodobacter sphaeroides and Chlorofelxus aurantiacus. B y M . Becker, D . M i d d e n d o r f , N . W . W o o d b u r y , W . W . P a r s o n , and R . E . B lankensh ip ( W i t h 4 F igures ) 374

Femtosecond Spectroscopy of the P r i m a r y Events o f B a c t e r i a l Photosynthes is B y W . Z i n t h , J . Dobler , and W . Kaiser ( W i t h 3 Figures) 379

A n A c c u m u l a t e d P h o t o n Echo Study of Sub-picosecond Processes i n P h o t o s y n t h e t i c React ion Centers B y S.R. Meech, A . J . Hoff , and D . A . W i e r s m a ( W i t h 2 Figures) . . . . 384

XV

U l t r a f a s t E l e c t r o n and Energy Transfer in React ion Center and A n t e n n a Prote ins f r o m Photosynthet i c B a c t e r i a B y M . R . Wasie lewski , D . M . T iede , and H . A . F r a n k ( W i t h 5 Figures) 388

Femtosecond Spectroscopy of E x c i t a t i o n Energy Transfer and I n i t i a l Charge Separat ion i n the React ion Center o f t h e Photosynthet i c B a c t e r i u m Rhodopseudomonas sphaeroides B y J . B r e t o n , J . - L . M a r t i n , A . M i g u s , A . A n t o n e t t i , and A . Orszag ( W i t h 4 Figures) 393

Picosecond Trans ient A b s o r p t i o n Spectroscopy of Green P l a n t Photosystem I React ion Centres B y B . L . Gore , L . B . G i o r g i , and G. Por te r ( W i t h 1 F i g u r e ) 398

Femtosecond-Pulse Spectroscopy of P r i m a r y Photoprocesses i n React ion Centers o f Rhodopseudomonas sphaeroides R-26 B y S.V. C h e k a l i n , Y u . A . Matvee ts , and A . P . Yartsev ( W i t h 3 Figures ) 402

Detergent Effects u p o n the Picosecond D y n a m i c s o f H i g h e r P l a n t L i g h t H a r v e s t i n g C h l o r o p h y l l Complex ( L H C ) . B y J .P. I d e , D . R . K l u g , W . K u h l b r a n d t , G. Por ter , and J . B a r b e r ( W i t h 1 F igure ) 406

Picosecond C o n f o r m a t i o n a l Intermediates i n t h e B a c t e r i o r h o d o p s i n Photocyc le . B y G . H . A t k i n s o n , T . L . Brack , D . B l a n c h a r d , G . Rumbles , a n d L . Siemankowski ( W i t h 3 F igures ) 409

E l e c t r o n Transfer and R a p i d Restr i c ted M o t i o n i n Homologous A z u r i n s . B y J . W . P e t r i c h , J . W . L o n g w o r t h , and G.R. F l e m i n g ( W i t h 3 Figures ) 413

P r i m a r y Process o f V i s i o n : Hypsorhodops in B y T . Kobayash i , H . O h t a n i , and M . T g u d a ( W i t h 3 F igures ) 416

R e a c t i v i t y and Dynamics of Hemeprote ins i n the Femtosecond a n d Picosecond T i m e Domains . B y D . Houde , J . W . P e t r i c h , O . L Ro jas , C. Poyar t , A . A n t o n e t t i , and J . L . M a r t i n ( W i t h 3 F igures ) 419

Picosecond R a m a n Hole B u r n i n g as a Probe of C o n f o r m a t i o n a l Heterogeneity : A p p l i c a t i o n s t o O x y h e m o g l o b i n B y B . F . C a m p b e l l and J . M . F r i e d m a n ( W i t h 4 F igures ) 423

U l t r a f a s t Studies of N i t r o s y l m y o g l o b i n . B y K . A . J o n g e w a r d , J . C . M a r s t e r s , and D . M a g d e ( W i t h 4 Figures ) 427

Molecu lar D y n a m i c s S tudy of V i b r a t i o n a l C o o l i n g i n O p t i c a l l y E x c i t e d Hemeprote ins . B y E.R. H e n r y , W . A . E a t o n , a n d R . M . Hochstrasser ( W i t h 1 F igure ) 430

XVI

C h e m i c a l React ion in a Glassy M a t r i x : D y n a m i c s o f L i g a n d B i n d i n g t o Pro toheme i n G lycero l :Water . B y J . R . H i l l , M . J . Cote , D . D . D l o t t , J . F . K a u f f m a n , J . D . M c D o n a l d , P . J . Ste inbach, J . R . Berendzen , and H . Frauenfelder ( W i t h 3 F igures ) 433

P a r t V I I I E n e r g y Transfer and R e l a x a t i o n

Energy and E l e c t r o n Transfer of Adsorbed Dyes on M o l e c u l a r Single Crysta l s and O t h e r Substrates . B y K . K e m n i t z , Ν. Nakash ima , and K . Yosh ihara ( W i t h 5 F igures ) 438

O p t i c a l P u m p - P r o b e Spectroscopy of Dyes on Surfaces: G r o u n d -State Recovery of R h o d a m i n e 640 on Z n O a n d Fused Si l i ca B y P .A. A n f i n r u d , T .P . Causgrove, a n d W.S . S t r u v e ( W i t h 1 F igure ) 442

Picosecond Fluorescence Spectroscopy on M o l e c u l a r Assoc iat ion i n L a n g m u i r - B l o d g e t t F i l m s B y I . Y a m a z a k i , N . T a m a i , and T . Y a m a z a k i ( W i t h 3 Figures ) 444

Fluorescence Concentra t i on D e p o l a r i z a t i o n o f D O D C I i n G lycero l : A P h o t o n - C o u n t i n g Test of T h r e e - D i m e n s i o n a l E x c i t a t i o n T r a n s p o r t T h e o r y B y D . E . H a r t , P.A. A n f i n r u d , and W.S . S t ruve ( W i t h 1 F igure ) . . . 447

F r a c t a l Behaviors i n T w o - D i m e n s i o n a l E x c i t a t i o n E n e r g y Transfer o n Vesicle Surfaces. B y N . T a m a i , T . Y a m a z a k i , I . Y a m a z a k i , a n d N . M a t a g a ( W i t h 3 Figures) 449

Trans ient V i b r a t i o n a l H e a t i n g of Molecules A f t e r I n t e r n a l Convers ion. B y A . Seilmeier, U . Sukowski , W . Kaiser , a n d S.F. Fischer ( W i t h 2 Figures) 454

Non l inear A b s o r p t i o n Spectroscopy of L i q u i d s w i t h U l t r a s h o r t I R Pulses B y H . Graener , R. Dohlus , and A . Laubereau ( W i t h 2 Figures) — 458

Femtosecond Re laxat ion Dynamics of Large Organic Molecules B y M . J . Rosker, F . W . Wise , C .L . Tang , and A . J . T a y l o r ( W i t h 4 Figures) 461

P o p u l a t i o n L i f e t imes of O H ( v = l ) and O D ( v = l ) V i b r a t i o n s i n Alcohols , Silanols and C r y s t a l l i n e Micas . B y E . J . H e i l w e i l , Μ.P. Casassa, R .R . Cavanagh, and J . C . Stephenson 465

S 0 - S n T w o - P h o t o n A b s o r p t i o n D y n a m i c s o f R h o d a m i n e Dyes B y P. Sperber, Μ. Weidner , and A . Penzkofer ( W i t h 3 Figures) — 469

XVII

Nonl inear O p t i c a l Response of One -Dimens iona l E x c i t o n s i n Po lydiacety lene . B y B . I . Greene, J . Orens te in , R .R . M i l l a r d , and L . R . W i l l i a m s ( W i t h 2 Figures) 472

Picosecond P h o t o c o n d u c t i v i t y and Non l inear O p t i c a l Phenomena i n i rans -Po lyace ty lene B y D . Moses, M . S inc la ir , and A . J . Heeger ( W i t h 1 F i g u r e ) 475

Singlet E x c i t o n Fusion i n Mo lecu lar Solids B y R .R . M i l l a r d a n d B . I . Greene ( W i t h 2 Figures ) 478

M a t r i x Effect o n V i b r a t i o n a l R e l a x a t i o n i n M o l e c u l a r Crys ta l s B y J .R . H i l l , E . L . C h r o n i s t e r , J . C . Post lewaite , and D . D . D l o t t ( W i t h 1 F i g u r e ) 482

O p t i c a l Damage i n M o l e c u l a r Crysta l s : A Sol id State Exp los i on B y D . D . D l o t t , T . J . Kos ic , and J .R . H i l l ( W i t h 4 F igures ) 485

R o t a t i o n a l R e l a x a t i o n o f Free a n d Solvated Rotors B y A . J . B a i n , C. H a n , P L . H o l t , P J . M c C a r t h y , A . B . M y e r s , M . A . Pere ira , a n d R . M . Hochstrasser ( W i t h 5 Figures ) 489

U l t r a f a s t D y n a m i c s at t h e Inter face : P r o b i n g t h e T r a n s i t i o n f r o m So lu t i on t o Surface In terac t i ons i n Charged Micel les B y E . F . T e m p l e t o n , K . B r i n k e r , S. Paone, a n d G . A . K e n n e y -Wallace ( W i t h 1 F i g u r e ) 495

Shock M o d e r a t e d Photophysics and Photo chemis t ry at M u l t i -k i l o b a r Pressures B y B . L . Justus , A . L . H u s t o n , and A . J . C a m p i l l o ( W i t h 5 Figures ) . 499

P a r t I X Coherent Spectroscopic Techniques

Phase G r a t i n g A p p r o a c h t o Suscept ib i l i ty Tensors: D e t e r m i n a t i o n i n I so t rop i c M e d i a . B y J . Etchepare , G. G r i l l o n , I . T h o m a z e a u , G. H a m o n i a u x , and A . Orszag ( W i t h 4 Figures) 504

Non l inear Response F u n c t i o n for Four-Wave M i x i n g : A p p l i c a t i o n t o Coherent R a m a n Lineshapes i n Po lyatomics and t o t h e O p t i c a l A n d e r s o n T r a n s i t i o n B y S. M u k a m e l , Z. Deng , and R . F . L o r i n g ( W i t h 2 Figures) 510

Picosecond Laser Pulse Shaping and Phase S h i f t i n g for M o l e c u l a r Spectroscopy B y M . Haner , F . Spano, and W.S . W a r r e n ( W i t h 2 Figures) 514

T h i r d - O r d e r Non l inear O p t i c a l Interac t i ons i n T h i n F i l m s o f Organic Po lymers Invest igated by Picosecond and Subpicosecond Four-Wave M i x i n g . B y P . N . Prasad , D . Narayana Rao, J . Swiatk iewicz , P. C h o p r a , and S.K. Ghoshal 518

XVIII

Picosecond Raman- Induced Phase C o n j u g a t i o n Spectroscopy B y R. D o r s i n v i l l e , P. De l fyet t , a n d R.R. A l f a n o ( W i t h 2 Figures) . . 521

P o l a r i z a t i o n Dependence of T ime-Reso lved C A R S i n L i q u i d s B y N . Kohles and A . Laubereau ( W i t h 3 F igures ) 524

D i r e c t Measurement of Wave-Vector -Dependent P o l a r i t o n Energy Ve loc i ty a n d Dephas ing i n N H 4 C 1 B y G . M . Gale , F . Vallee, and C. F ly t zan i s ( W i t h 4 Figures) 528

I m p u l s i v e S t i m u l a t e d Rayle igh , B r i l l o u i n , a n d R a m a n Scat ter ing : E x p e r i m e n t s and T h e o r y of L i g h t Scat ter ing Spectroscopy i n the T i m e D o m a i n . B y M . R . Farrar , L . R . W i l l i a m s , Y o n g - X i n Y a n , L a p - T a k C h e n g , and K . A . Nelson ( W i t h 4 F igures ) 532

U l t r a f a s t Trans ient Spectroscopy w i t h B r o a d b a n d N o n - T r a n s f o r m -L i m i t e d L i g h t Sources B y T . Y a j i m a a n d N . M o r i t a ( W i t h 4 Figures) 536

Picosecond Dephasing T i m e Measurement by CSRS U s i n g T e m p o r a l l y Incoherent Nanosecond Laser w i t h Short C o r r e l a t i o n T i m e B y T . K obayas h i , T . H a t t o r i , and A . Terasaki ( W i t h 3 Figures) . . . 541

A n o m a l o u s Pulse D u r a t i o n Dependence of the Q u a s i c o n t i n u u m A b s o r p t i o n S p e c t r u m B y P. M u k h e r j e e and H.S. K w o k ( W i t h 3 Figures) 544

I n d e x of C o n t r i b u t o r s 549

XIX

Femtosecond Carr ier Relaxation in Semiconductor-Doped Glasses

M.C. Nuss*, W. Zinth, and W. Kaiser

P h y s i k D e p a r t m e n t der Technischen Universität München, A r c i s s t r . 2 1 , D-8000 München 2, Fed. Rep. o f G e r m a n y

Semiconductor-doped g l a s s e s incorporating small CdSxSei - x or CdSexTei -x c r y s t a l l i t e s i n a g l a s s matrix, show strong nonlinear absorption / l / and l a r g e v a l u e s of the nonlinear o p t i c a l s u s c e p t i b i l i t y X3 /2/. The semi-conductor c r y s t a l l i t e system c u r r e n t l y a t t r a c t s i n c r e a s i n g a t t e n t i o n when the semiconductor i n c l u s i o n s are small enough to expect quantum e f f e c t s .

The semiconductor-doped g l a s s f l i t e r s s t u d i ed (Schott RG 830, RG 715, and RG 645) a r e c h a r a c t e r i z e d by an exponential absorption edge ~ three times l e s s s teep than the corresponding bulk semiconductors. The frequency p o s i t i o n of the absorption edge v a r i e s with composition, but i t may as w e l l be i n f l u e n c e d by the s i z e of the semiconductor i n c l u s i o n s . No confinement e f f e c t s a r e observed i n the absorption s p e c t r a at 300 K, most probably due to a c e r t a i n v a r i a t i o n of c r y s t a l l i t e s i z e .

Femtosecond absorption recovery of a l l three Schott f i l t e r g l a s s e s was studied. I n the experiment, femtosecond l i g h t p u lses of = 60 f s duration and λ = 620 run from a c o l l i d i n g - p u l s e modelocking dye l a s e r generate an e l e c t r o n - h o l e plasma with a c a r r i e r d e n s i t y Ν * 3x1ο 1 7 cm"3 i n the semiconductor i n c l u s i o n s . A weaker probing pulse samples the absorption changes as a function of the delay time between e x c i t i n g and probing pulses. A l l data were recorded at room temperature.

F i g . l a , b shows the time-resolved absorption changes f o r the semiconductor-doped g l a s s f i l t e r s RG 645 and RG 830. The absorption change ΔΑ i s p l o t t e d versus delay time between e x c i t i n g and probing p u l s e s . The dashed curves are the c r o s s - c o r r e l a t i o n t r a c e s determining time zero. In the RG 830 semiconductor-doped g l a s s ( F i g . l b ) the energy of the femtosecond l a s e r pulses i s w e l l above the bandgap, c r e a t i n g c a r r i e r s with an excess energy ΔΕ * 500 meV. A f a s t recovery of the i n i t i a l bleaching i s observed with a time constant of 230 f s . This process can be i d e n t i f i e d with cooling of the i n i t i a l l y hot e l e c t r o n gas to the l a t t i c e temperature. A comparison with the expected energy l o s s r a t e of the e l e c t r o n gas due to the emission of LO-phonons i n c r y s t a l l i n e semiconductors /3/ y i e l d s s i m i l a r r e l a x a t i o n times f o r the absorption recovery. In RG 645 ( F i g , l a ) the o p p o s i t e e x t r e m e i s r e a l i z e d . The excess energy i s only s l i g h t l y l a r g e r than the bandgap. The absorption decreases with the integrated pulse i n t e n s i t y . No f a s t c a r r i e r r e l a x a t i o n process i s observed s i n c e the c a r r i e r s are i n j e c t e d with low excess energy. Consequently, the temperature of the e l e c t r o n gas w i l l not change and no f a s t absorption recovery i s observed. The bleaching i s due to the f i l l i n g of s t a t e s i n the conduction and valence b a n d s a n d remains e s s e n t i a l l y constant over the p l o t t e d time.

•Present address: AT&T B e l l Laboratories, 600 Mountain Ave., Murray H i l l , N.J. 07974, USA

267

A c t u a l l y , ΔΑ decays with a long time constant of ~ 100 ps (not shown i n thee f i g u r e ) . We a t t r i b u t e the 100 ps time constant to e l e c t r o n - h o l e recombination. This short recombination time i s not unreasonable i n the l i g h t of the l a r g e number of s u r f a c e s t a t e s i n the semiconductor-doped g l a s s e s , r e a c t i n g as e f f i c i e n t recombination c e n t e r s .

The most i n t e r e s t i n g case i s the semiconductor-doped g l a s s RG 715 ( F i g . 2 ) , where the i n i t i a l c a r r i e r excess energy ΔΕ i s ~ 300 meV. Here, both the femtosecond decay process as w e l l as the b a n d f i l l i n g can be traced. The three s o l i d curves correspond to d i f f e r e n t e x c i t a t i o n d e n s i t i e s , where the lower curves are f o r two times (curve b) and four times (curve c) attenuated l a s e r pulses, r e s p e c t i v e l y . A semilog p l o t of the data r e v e a l s two time constants; 250 f s f o r the f a s t i n i t i a l absorption recovery and 85 ps f o r the c a r r i e r recombination process. S i g n i f i c a n t i s the s u p e r l i n e a r decrease with c a r r i e r d e n s i t y of ΔΑ f o r times > 1 ps: ΔΑ decreases four times f a s t e r i f the c a r r i e r d e nsity i s reduced by a f a c t o r of 2.

The data can be explained assuming a c a r r i e r d e n s i t y dependent b a n d f i l l i n g process. I n p a r t i c u l a r , we think of energy l e v e l s or t r a p s below the conduction band, a c t i n g as a s i n k f o r the conduction band e l e c t r o n s . I f thee density of these l e v e l s i s about the same as the c a r r i e r d e n s i t y (~ 1 0 1 7 cm - 3) and the trapping time i s s e v e r a l hundfred femtoseconds, the capture of the c a r r i e r s i n t o these l e v e l s becomes saturated, l e a d i n g to the nonlinear dependence of ΔΑ on c a r r i e r d e n s i t y observed i n Fig.2. The f a s t 250 f s r e l a x a t i o n process i s a combination of c o o l i n g of the e l e c t r o n gas due to LO-phonon emission and trapping of charge c a r r i e r s . From there, el e c t r o n - h o l e recombination takes p l a c e v i a s u r f a c e s t a t e s i n the middle o f f the bandgap with a time constant of 85-100 ps.

268

Fig.2 Absorption recovery of the semiconductor-doped g l a s s RG 715

D e l a y T i m e C p s e c l

I n conclusion, we point out that the absorption changes observed f o r the three semiconductor-doped g l a s s e s i n v e s t i g a t e d here can be w e l l explained w i t h i n the framework of bulk semiconductor p h y s i c s . The observed processes are c o o l i n g of a hot e l e c t r o n , e l e c t r o n trapping, and recombination. There i s no i n d i c a t i o n of quantum s i z e e f f e c t s i n the c u r r e n t l y used g l a s s e s . We expect that e x c i t o n i c e f f e c t s w i l l only be apparent f o r semiconductor-doped systems with smaller c r y s t a l l i t e s and with homogeneous s i z e d i s t r i b u t i o n .

1 G. Bret, F. G i r e s , Appl. Phys. L e t t . 4 (1964) 175 B. Dan i e l z i k , K. Nattermann, D. von der Linde, Appl. Phys. B38 (1985), 31

2 R.K. J a i n , R.C. Lind, J . Opt. Soc. Am. 73 (1983) 647 P. Roussignol, D. Ricard, K.C. Rustagi, C. F l y t z a n i s , Optics Commun. 55 (1985) 143

3 J . Shah, S o l i d S t a t e E l e c t r o n . 21 (1978) 43

269