Ultrafast Phenomena XVI (eBook)

Paul Corkum: Atomic, Molecular and Optical Science Group Leader at Steacie of the National Research Council, he is a member of the Royal Societies of London and of Canada. He was the recipient of the Optical Society of America's Charles H. Townes award and the IEEE's Quantum electronics award in 2005. In 2006 he received the American Physical Society's Arthur L. Schawlow Prize. Corkum’s research launched attosecond science. After studying the interaction of intense light pulses with atoms and molecules he and his group proposed how atomic and molecular gases can be used to produce attosecond pulses. In 2002 they measured the motion of hydrogen atoms in a hydrogen molecular ion with a timing precision of 200-attoseconds and a spatial precision of 0.02 Angstroms. In 2004 they demonstrated how attosecond technology can be used to image the highest occupied molecular orbital of Nitrogen. More recently they were able to strobe the attosecond motion of an electron in a hydrogen molecule almost instantaneously as the molecule breaks. Sandro De Silvestri: He is professor at the Department of Physics of Politecnico in Milan, Italy. He is presently director of the European Large Scale Infrastructure "Center for Ultrafast Science and Biomedical Optics (CUSBO)", within the program of providing access to europen reasearch groups. He is also director of the "Centre of Ultrafast and Ultraintense Optical Science" (ULTRAS) of CNR-INFM. He is Fellow of the Optical Society of America and he is member of organising committee of several international congress in the field of photonics and ultrafast phenomena. He has made a number of significant contributions to the field of "Ultrafast Phenomena", extending for a period of about 25 years, in a variety of topics such as: (i) coherent vibrational spectroscopy; (ii) development of techniques for the generation of few optical cycle pulses either with high energy or tunable from near-IR to visible; (iii) study of ultrafast dynamics in organic and quantum confined systems; (iv) carrier envelope phase effects on strong field photoionization and high order harmonic generation; (v) generation of attosecond pulses. Keith Nelson: He is professor at the Department of Chemistry of MIT. His research is aimed at time-resolved optical study and control of condensed matter structural changes and the collective modes of motion through which they occur: (i) phase transitions or other collective structural rearrangements in crystalline solids; (ii) dynamics of the lattice vibrational modes; (iii) interactions between reactive molecular modes and lattice vibrations in reaction dynamics. He has developed femtosecond pulse shaping techniques for multiple-pulse excitation and coherent control of crystal lattice vibrations whose motions are involved in ferroelectric phase transitions, and for generation of ultrahigh-frequency acoustic waves whose motions are involved in structural relaxation of viscoelastic fluids and polymers. He has developed novel methods for recording complete femtosecond time-resolved spectroscopy measurements in a single laser shot, with the objective of observing ultrafast, irreversible structural and chemical changes in solids. In the ferroelectric crystals he has studied terahertz (THz) frequency lattice vibrations, by fabricating integrated waveguides and other structures through femtosecond laser machining providing further control over THz waves. He is extending these and other methods and applying them toward study of and control over condensed matter structural changes. Eberhard Riedle: He is professor for experimental physics at the Department for Physics of the Ludwig-Maximilians University of Munich, Germany. His interest and research focuses on the ultrafast dynamics, mechanisms and control of ultrafast chemical reactions, e.g. proton and electron transfer, molecular switches and molecules in zeolites. For these investigations he develops new methods and techniques for the generation and characterisation of extremely short tunable light pulses in the visible, NIR and UV. The research is performed within the framework of the SFB ADLIS in Vienna, the newly founded SFB 749 on "dynamics and intermediates of molecular transformations", the International Max Planck Research School on Advanced Photon Science (IMPRS-APS) and most importantly the newly founded exclellence cluster "Munich-Centre for Advanced Photonics (MAP)". In the latter he coordinates the research area " Molecular dynamics and elementary chemical reactions". He was deputy chair (2001-2004) and chair (2004-2007) of the Molecular Physics division of the Deutsche Physikalische Gesellschaft (DPG). Among a large number of meetings he was the responsible local organizer of the 68. Physikertagung der DPG (2004) and local chair for CLEO-Europe/EQEC (2033, 2005,2007). Robert Schoenlein:  He is Staff Scientist at LBNL. His research included the development of a 8 fs pulse novel laser system in the blue-green spectral region, the application to three-pulse photon echo studies of electronic dephasing and vibrational dynamics in semiconductor nanocrystals and ultrafast dynamics of the first step in vision. In 1994 he received the Adolph Lomb Medal from OSA. He initiated a new research direction in ultrafast x-ray science with the first time generation of 300 fs pulses in the hard x-ray regime (30 keV) via Thomson scattering between relativistic electrons from a LINAC and terawatt femtosecond laser pulses. In 2000, Schoenlein and co-workers demonstrated for the first time, the generation of femtosecond synchrotron pulses via laser manipulation of a stored electron beam. This approach serves as the basis for new femtosecond x-ray beamlines now under construction at the Advanced Light Source, BESSY, and the Swiss Light Source. Current research activities are in the application of ultrafast x-ray techniques to investigate atomic and electronic structural dynamics in condensed matter including photoinduced phase transitions in correlated electron systems, ferroelectrics, transition-metal complexes and molecular dynamics in solution.

Ultrafast Phenomena XVI 3
Preface 5
Contents 6
Part I_Attosecond and High-Order Harmonic Generation andMeasurement, Atomic and Molecular Physics 30
Sub-100-as soft x-ray pulses 31
Introduction 31
Experimental Methods 31
Results and Discussion 32
Conclusions 33
Generation of High-order Harmonics with aNear-IR Self-phase-stabilized ParametricSource 34
QuasiPhaseMatchedHighOrderHarmonicGeneration in the SoftXrayRegime 37
Introduction 37
Experimental Setup 38
Results and Discussion 38
Conclusions 39
Phase Matching and Quasi-Phase Matching ofExtreme High-Order Harmonic Generation 40
Comparison of Parallel and PerpendicularPolarized Counterpropagating Light for Quasi-Phase-Matching High Harmonic Generation 43
Experimental Methods 44
Results and Discussion 44
Conclusions 45
Enhanced Harmonic Generation in Gas Jets withExpanding Clusters 46
Introduction 46
Experiments 46
Conclusion and future directions 48
Observation of Elliptically Polarized HighHarmonic Emission from Molecules Driven byLinearly Polarized Light 49
Polarization-Resolved Pump-Probe Spectroscopywith High Order Harmonics 52
Introduction 52
Experimental Methods 52
Results and Discussion 53
Conclusions 54
Study of quantum-path interferences in thehigh harmonic generation process. 55
Introduction 55
Experimental Methods 55
Results and Discussion 56
Conclusions 56
Interference Patterns in the WavelengthDependence of High-Harmonic Generation 58
Introduction 58
Numerical Model 58
Results and Discussion 59
Conclusions 60
Generation of Polarization-Shaped UltravioletFemtosecond Pulses 61
All-Optical Quasi-PhaseMatching andQuantum Path Selection of High-OrderHarmonic Generation at 140 eV UsingCounterpropagating Light 64
Introduction 64
Experimental Methods 64
Results and Discussion 65
Ultrafast Molecular and Materials Dynamicsprobed by Coherent X-Rays 67
Plasma-Blue-Shift Spectral Shear Interferometryfor Characterization of Ultimately Short OpticalPulses 70
Spatially resolved Ar* and Ar+* imaging as adiagnostic for capillary based high harmonicgeneration 73
Introduction 73
Experimental 73
Results and Discussion 73
Conclusions 75
Internal Momentum State Mapping usingHigh Harmonic Radiation 76
1. Introduction 76
3. Results and Discussion 76
4. Conclusions 78
Attosecond control of electron localization in oneandtwo-color dissociative ionization of H2 and D2 79
Introduction 79
One-color experiment 79
Two-color experiment 80
Simultaneous Description of Electron and NuclearDynamics: A Quantum Approach for Multi-Electron Systems 82
Introduction 82
Results and Discussion 83
Conclusions 84
Attosecond Photoelectron Spectroscopy ofElectron Tunneling in Dissociating HydrogenMolecular Ion 85
Attosecond angular streaking: an ideal techniqueto measure an electron tunneling time? 88
Introduction 88
Experimental part 89
Conclusion and Outlook 90
Probing Dynamics in Polyatomic Molecules UsingHigh Harmonic Generation: the Role of IonizationContinua 91
Introduction 91
Experimental Methods 91
Results and Discussion 92
Conclusions 93
High harmonic generation from multiplemolecular orbitals of N2 94
Introduction 94
Experimental Methods 94
Results and Discussion 94
Conclusions 96
Ultrafast Multiphoton Crystallography 97
Introduction 97
Results and Discussion 97
Conclusions 99
Direct Measurement of Angle-Dependent SinglePhoton Ionization of N2 and CO2 100
Introduction 100
Results and Discussion 101
Conclusions 102
Field-free unidirectional molecular rotation 103
Attosecond coincidence spectroscopy ofdiatomic molecules 106
Introduction 106
Experimental Methods 106
Results and Discussion 107
Conclusions 108
Real-time Evolution of the Valence Orbitals in aDissociating Molecule as Revealed byFemtosecond Photoelectron Spectroscopy 109
Introduction 109
Experimental Methods 109
Results and Discussion 110
Conclusions 111
TransientWaveguiding in a RotationallyExcited Molecular Gas 112
Introduction 112
Experimental Methods 112
Results and Discussion 112
Conclusions 114
Molecular Recollision Interferometry in HighHarmonic Generation 115
Multi-Electron Dynamics in Molecular HighHarmonic Generation 118
Introduction 118
MCTDHF 118
System and Models 118
Results and Discussion 119
Conclusions 120
Probing the dynamics of plasma mirrors on theattosecond time scale 121
Introduction 121
Mutual coherence of harmonic sources generated on plasma mirrors 121
Probing the dynamics of the plasma electrons 122
Shaping Entangled Photon Pairs 124
Introduction 124
Experimental Methods 124
Results and Discussion 125
Conclusions 126
Part II_Ultrafast X-ray and Electron Science 127
Ultrafast Structural Dynamics of Polar SolidsStudied by Femtosecond X-Ray Diffraction 128
Introduction 128
Experimental Techniques 128
Lattice dynamics in ferroelectric nanolayers 129
Structural dynamics of polar dipole solvation 130
Atomic Motion in Laser Excited Bismuth Studiedwith Femtosecond X-Ray Diffraction 131
Introduction 131
Experimental Methods 131
Results and Discussion 132
Acknowledgements. 133
Femtosecond X-ray Diffraction Study of theUltrafast Coupling between Magnetization andStructure in the Ferromagnet SrRuO3 134
Introduction 134
Experiment 134
Results and Discussion 135
Conclusion 136
Electron-Phonon Energy Transfer in BismuthObserved by Ultrafast Electron Diffraction 137
Introduction 137
Experimental Methods 137
Ultrafast Heating of Bismuth 138
Atomic View of the Photoinduced Collapse ofGold and Bismuth 140
Introduction 140
Experimental Methods 140
Results and discussion 141
Four-dimensional Visualization of TransitionalStructures in Phase Transformations by ElectronDiffraction 143
Introduction 143
Ultrafast Electron Crystallography on VO2 Single Crystals 143
Visualization of Atomic Motion in Four Dimensions 144
Perspectives 145
Ultrashort soft x-ray pulses from a femtosecondslicing source for time-resolved laser pump- x-rayprobe experiments 146
Introduction 146
The “Femtoslicing” Source 146
The Laser Pump- X-Ray Probe Experimental Setup 147
Summary 148
Femtosecond X-Ray Absorption Spectroscopy of aPhotoinduced Spin-Crossover Process 149
Introduction 149
Light-driven spin crossover at room temperature in solution 149
Femtosecond X-Ray Absorption Spectroscopy 150
Results 150
Conclusions 150
Probing Reaction Dynamics of Transition-MetalComplexes in Solution via Time-Resolved SoftX-ray Spectroscopy 152
Introduction 152
Experimental Methods 153
Results and Discussion 153
Conclusions 154
Sub-20-fs Optical Pump-X-ray ProbeSpectroscopy beyond the Si K Edge 155
Introduction 155
Experimental Methods 156
Results and Discussion 156
Conclusions 157
Capturing Transient Solute Structures in Solutionby Pulsed X-ray Diffraction 158
Introduction 158
Experimental Methods 158
Results and Discussion 159
Conclusions 160
Structural kinetics in protein-coated goldnanoparticles probed by time-resolved x-rayscattering 161
Introduction 161
Experimental Methods 161
Results and Discussion 162
Conclusions 163
X-ray induced transient optical reflectivityfor fs-X-ray/optical cross-correlationat Free-Electron Lasers 164
Introduction 164
Experimental Methods 164
Conclusions 166
Autocorrelation Experiments with Soft X-ray FELPulses 167
Introduction 167
Experimental 168
Results and Discussion 168
Conclusions 169
Ultrafast coherent X-ray diffractive imaging withthe FLASH Free-Electron Laser 170
Single pulse diffractive imaging 170
Diffractive imaging at FLASH 170
Time-resolved Imaging 171
Lensless Microscopy and Holography with 60 nmResolution using Tabletop Coherent Soft X-Rays 173
Introduction 173
Experimental Setup 173
Results and Discussion 174
Nanoscale Heat Transport Probed with UltrafastSoft X-Rays 176
Relativistic attosecond electron pulses from cascadedacceleration using ultra-intense radially polarized laserbeams 179
Introduction 179
Radially Polarized Laser Beams 179
Electron Acceleration With Radially Polarized Laser Beams 179
Cascaded Electron Acceleration with Radially Polarized Beams 180
Conclusions 181
Attosecond Free Electron Pulsesfor Diffraction and Microscopy 182
Introduction 182
Attosecond Free Electron Pulses from Synthesized Optical Gratings 182
Numerical Simulations and Discussion 183
Perspectives 184
Electronically Driven Structural Dynamics of SiResolved by Femtosecond Electron Diffraction 185
Introduction 185
Experimental methods 185
Excitation of the [001] acoustic phonon modes 185
Non-thermal collapse of the lattice 187
References 187
Picosecond electron deflectometry of optical-fieldionized plasmas 188
Introduction 188
Experimental Methods 188
Results and Discussion 188
Conclusions 190
Part III_Correlated Electron Systems, Magnetization and Spin Dynamics 191
Clocking the Collapse of a Mott Gap 192
Coherent OrbitalWaves in Manganites 195
Ultrafast terahertz response driven by photoinducedinsulator to metal transitionin layered organic salt 198
Introduction 198
Experimental Methods 199
Results and Discussion 199
Conclusions 200
Photo-induced macroscopic oscillationbetween insulator and metalin layered organic Mott insulator 201
Introduction 201
Experimental Methods 202
Results and Discussion 202
Conclusions 203
THz Slow Motion of an Ultrafast Insulator-MetalTransition in VO2: Coherent Structural Dynamicsand Electronic Correlations 204
Introduction 204
2D multi-THz study of the ultrafast insulator-metal transition 204
Qualitative model of the ultrafast phase transition 206
Nonthermal Melting of Orbital Order inLa1/2Sr3/2MnO4 by Coherent Excitation of a Mn-OStretching Mode 207
Ultrafast Gigantic Photo-Response in Charge-Ordered Organic Salt (EDO-TTF)2PF6 on 10-fstime scales 210
Introduction 210
Experimental Methods 211
Results and Discussion 211
Conclusions 212
Teasing a Quasiparticle: Ultrafast NonlinearResponse of the Fr¨ohlich Polaron in GaAs 213
Introduction 213
Experiment 213
Discussion 214
Conclusions 215
Time-resolved X-ray Absorption Spectroscopy ofPhotoinduced Insulator-Metal Transition in aColossal Magnetoresistive Manganite 216
X-ray Absorption Spectroscopy on the fs TimeScale: Ultrafast Electron and Spin Dynamicsin Nickel 219
Introduction 219
Experimental Setup 219
Results 219
Discussion 221
Ultrafast Photoinduced Ferromagnetic Orderin a Magnetic Semiconductor Heterostructure 222
Introduction 222
Experimental Methods 222
Results and Discussion 223
Conclusions 224
Non-equilibrium spin-dynamics of Gd(0001)studied by time-resolved SHG and magnetic lineardichroism in 4f core-level photoemission 225
Ultrafast Spin Control by Charge-separatedStates in Colloidal ZnO Quantum Dots 228
Introduction 228
Experimental Methods 228
Results and Discussion 229
Conclusions 230
Ultrafast electronic and spin dynamics in thin ironfilms: electron-magnon and electron-phononinteractions 231
Introduction 231
Experimental Methods 231
Results and Discussion 232
Conclusions 233
Laser Induced Alignment of Water Spin Isomers 234
Introduction 234
Results and Discussion 235
Conclusions 236
Memory Effects in Photo-inducedFemtosecond Magnetization Rotation in aFerromagnetic Semiconductor 237
Introduction 237
Experimental Methods 238
Results and Discussion 238
Conclusions 239
Part IV_Physics - Condensed Phase and Low Dimensional Systems 240
Transient Dielectric Function of Fs-Laser ExcitedBismuth 241
Introduction 241
Experimental 241
Conclusions 243
Coherent A1g and Eg Phonons of Antimony 244
Introduction 244
Experimental Methods 244
Results and Discussion 244
Conclusions 246
Mode selective Excitation of Coherent Phononsin Bismuth by Femotosecond Pulse Pair 247
Introduction 247
Experimental Methods 247
Results and Discussion 248
Conclusions 249
Ultrafast Dynamics of Electron-Hole PlasmaCoupled to Optical Phonons in a ZnO Thin Film 250
Large-amplitude coherent phonons in semimetals 253
Introduction 253
Experimental Methods 253
Results and Discussion 254
Conclusions 255
Laser-Induced Undoing of a Peierls Distortion 256
Introduction 256
Structure of Arsenic 256
Method 257
Effect of Pressure 257
Laser-Induced Phase Transition 258
Conclusion 258
Ultrafast dynamics of coherent optical phononsin a-quartz 259
Introduction 259
Experiment 259
Results and Discussion 259
Conclusions 261
Influence of Lattice Heating Time on Strain WaveDynamics in InSb 262
Introduction 262
Experimental Methods 262
Results and Discussion 263
Conclusions 264
Soft X-Ray Thomson Scattering in Warm DenseMatter at FLASH 265
The Free Electron Laser in Hamburg (FLASH) 265
Thomson Scattering in Warm Dense Matter 265
Experimental Setup 266
Results 267
Magnon-Enhanced Phonon Damping at Gd(0001)and Tb(0001) surfaces 268
Introduction 268
Experimental Methods and Data Analysis 268
Results and Discussion 269
Conclusions 270
Ultrafast Coherent Interactions in QuantumWells Studied by Two-Dimensional FourierTransform Spectroscopy 271
Two-quantum Two-dimensional FourierTransform Electronic Spectroscopy of Biexcitonsin GaAs Quantum Wells 274
Introduction 274
Experimental Methods 274
Results and Discussion 275
Conclusions 276
Three-Pulse Echo Peak Shift Spectroscopy ofDisordered Semiconductor Quantum Wells andDense Atomic Vapors 277
Coherently controlled ballistic charge currentsin unbiased bulk silicon and single-walledcarbon nanotubes 280
Introduction 280
Experimental Methods 280
Results and Discussion 280
Conclusions 282
Ultrafast dynamics of coherent phonons in thealigned single-walled carbon nanotubes 283
Introduction 283
Experimental Methods 284
Results and Discussion 284
Conclusions 285
Evidence for electron correlation in (6,5) carbonnanotubes from pump-probe spectroscopy withbroadband pulses 286
Introduction 286
Experimental Methods 286
Results and Discussion 287
Conclusions 288
Ultrafast Relaxation of Excited Dirac Fermions inEpitaxial Graphene 289
Introduction 289
Experimental Methods 290
Results and Discussion 291
Conclusions 291
Radiationless Transitions and AngularMomentum Transfer in SemiconductorNanocrystals 292
Introduction 292
Results and Discussion 293
Ultrafast Carrier Dynamics in SemiconductorNanowires 295
Introduction 295
Experimental Methods 295
Results and Discussion 296
Conclusions 297
Time-resolved photoemission spectroscopy ingraphite 298
Introduction 298
Experiment 298
Results and Discussion 299
Conclusions 300
Exciton Dephasing in Semiconducting Single-Walled Carbon Nanotubes 301
Introduction 301
Experimental Methods 301
Results and Discussion 302
Conclusions 303
On the Absence of Carrier Multiplication in InAsCore/Shell/Shell Nanocrystals 304
Introduction 304
Experimental Methods 305
Results and Discussion 305
Conclusions 306
Temporal dynamics of polaritons in a stronglycoupledorganic-semiconductor microcavity 307
Introduction 307
Experimental Methods 307
Discussion and Conclusion 308
Three-Dimensional Electronic Four Wave-MixingSpectroscopy in GaAs Quantum Wells 310
Introduction 310
Experimental Methods 311
Results and Discussion 311
Conclusions 312
Ultrafast carrier dynamics in spherical CdSe core/elongated CdS shell nanocrystals 313
Introduction 313
Experimental Methods 313
Results and Discussion 314
Conclusions 315
Time-Resolved Optical Studies of InGaAs/GaAsQuantum Wells in High Magnetic Fields 316
Introduction 316
Experimental Methods 316
Results and Discussion 317
Conclusions 318
Femtosecond Formation of UltrastrongLight-Matter Interaction 319
Introduction: Cavity QED in the ultrastrong coupling regime 319
Multi-THz waveguide with semiconductor quantum wells 319
Non-adiabatic formation of intersubband cavity polaritons 320
Ultrafast Bleaching and Gainin a Single Semiconductor Quantum Dot 322
Introduction 322
Experimental Methods 322
Results and Discussion 323
Conclusions 324
Probing coherent optical phonons by ExtremeUltraviolet radiation based on high-orderharmonic generation 325
Introduction 325
Experimental Methods 326
Results and Discussion 326
Conclusions 327
Part V_Chemistry - Condensed Phase 328
Real-Time Monitoring of Structural Evolution inCis-Stilbene Photoisomerization b y Ult rafastTime-Domain Raman Spectroscopy 329
Introduction 329
Experimental 330
Results and Discussion 330
Origin of Negative and Dispersive Features inResonance Femtosecond Stimulated RamanSpectroscopy 332
Introduction 332
Results and Discussion 332
Conclusions 334
Reactive Dynamics in Nanoscale Water dropletsConfined in Inverse Micelles 335
Introduction 335
Experimental Methods 335
Results and Discussion 336
Symmetry Dependent Solvation of Donor-Substituted Triarylboranes 338
1. Contribution of internal charge mobility to solvation 338
2. Solvatochromic shifts in the femtosecond transient absorption spectra 339
Substitution- and Temperature-Effects onHemithioindigo Photoisomerization –The Relevance of Energy Barriers 341
Introduction 341
Experimental Methods 341
Results and Discussion 342
Conclusions 343
Vibrational Coherence Decay in Metal Carbonyls:Solvent Dependence of Coherence LifetimesStudied with MDIR 344
Introduction 344
Experiment 344
Results 345
Generation of Narrowband Ultrashort PulsesTunable in the mid-IR and the Application toVibrational Energy Transfer in a ModifiedAmino Acid 347
Introduction 347
Experimental Methods 347
Results and Discussion 348
Ultrafast Exciton Dynamics of J- and HAggregatesof Porphyrin Catechol in AqueousSolution 350
Introduction 350
Results and Discussion 350
Conclusion: 352
References: 352
Chirp Effect on Vibrational Wave Packets inLarge Molecules: a Multimode Perspective 353
Introduction 353
Theory 353
Experiment 354
Conclusions 355
References: 355
Determining Vibrational Huang-Rhys Factors by PhotonEcho Spectroscopy 356
Introduction 356
Conclusions 358
Observation of High-Frequency CoherentVibrational Motion with Strongly Chirped ProbePulses 359
Coherent Transfer of Molecular Vibrations in theElectronic Excited States 362
Introduction 362
Experimental Methods 363
Results and Discussion 363
Conclusions 364
Ultrafast Isomerization Dynamics of BiomimeticPhotoswitches 365
Introduction 365
Results and discussion 365
Conclusions 367
Broadband femtosecond fluorescenceup-conversion and photon echo experiments in theUV 368
Introduction 368
Results and discussion 368
Conclusions 370
Intramolecular Vibrational Energy RedistributionMeasured by Femtosecond Pump-ProbeExperiments in a Hollow Waveguide 371
Femtosecond Fluorescence Spectroscopy of N6,N6-Dimethyladenine: New Explanation of the “DualFluorescence” Dynamics from Decay and RiseTime Measurements at Threshold 374
Introduction 374
Experimental Method 375
Results 375
Discussion 376
Assignment of the Excited-State Infrared-Spectrain the Course of the Ring Opening Reaction of aPhotochromic Dihydroazulene 377
Introduction 377
Materials and Methods 378
Results and Discussion 378
Conclusions 379
Time-resolved coincidence imaging of ultrafastmolecular dynamics 380
Introduction 380
Experimental Methods 380
Results 381
Discussion 382
Ultrafast time and frequency domain vibrationaldynamics of the CaF2/H2O interface 383
1. Introduction: 383
2. Experimental: 384
3. Results and Discussion 384
4. Conclusion: 385
5. References: 385
Non-Condon vibronic coupling of coherentmolecular vibration in MEH-PPV induced by avisible few-cycle pulse laser 386
Introduction 386
Experimental Methods 386
Results and Discussion 386
Conclusions 388
Specific Channel of Energy Dissipation inCarotenoids: Coherent Spectroscopic Study 389
Introduction 389
Experiments 389
Results and Discussion 390
Conclusions 391
Coherent phonons in cyanine dye monomers andJ-aggregates 392
Introduction 392
Experimental Methods 392
Results and Discussion 393
Conclusions 394
Ultrafast Dynamics in Na-doped water Clusters 395
Introduction 395
Experimental Methods 395
Results and Discussion 396
Conclusions 397
Electronic Excitations in Pentacene Films:Singlet versus Triplet Dynamics 398
Introduction 398
Ultrafast Electronic Dynamics 398
Delayed Triplet Formation 399
Conclusions 400
Photoreaction from a light generatednon-equilibrium state 401
Introduction 401
Materials and Methods 402
Results and Discussion 403
Conclusion 403
Excited-State Nuclear Wavepacket Motion of anUltrafast Inorganic Molecular Switch 404
Introduction 404
Experimental Methods 405
Results and Discussion 405
Conclusions 406
Femtosecond Electronic Dynamics via a ConicalFunnel 407
Introduction 407
Experiment and Results 408
Modeling 409
Discussion and Conclusion 409
A new technique to measure time-resolvedcircular dichroism : ultrafast conformationaldynamics of 1,1'-bi-2-naphthol 410
Introduction 410
Time-Resolved Circular Dichroism 410
Conformational dynamics in excited state Binaphthol 411
Picosecond Time-Resolved Vibrational CircularDichroism Spectroscopy 413
Introduction 413
Experimental Methods 413
Results and Discussion 414
Conclusions 415
Part VI_Chemistry - Advanced Spectroscopy, Molecular Control, HydrogenBonding, Liquids and Interfaces 416
Automated 2D infrared and electronicspectroscopies using pulse shaping 417
1. Introduction 417
2. Experimental Methods 418
3. Results and Discussion 418
4. Conclusions 419
References 419
Relaxation-Assisted Dual-Frequency Two-Dimensional Infrared Spectroscopy: MeasuringDistances and Bond Connectivity 420
Introduction 420
Results and Discussion 420
Triggered-exchange Two-dimensional InfraredSpectroscopy of Metal Carbonyl PhotodissociationDynamics 423
Introduction 423
Experimental Methods 423
Results and Discussion 424
Conclusions 425
Observation of Quantum Coherence in Light-Harvesting Complex II by Two-DimensionalElectronic Spectroscopy 426
Introduction 426
Experimental Methods 426
Results and Discussion 427
Conclusions 428
Vibrational Beating in Two-DimensionalElectronic Spectra 429
Double-Quantum Coherence Spectroscopy ofChromophore Aggregates 432
Chain Length Dependence of Two-DimensionalInfrared Spectral Pattern Characteristic to 310-Helix Peptides 435
Introduction 435
Experimental Methods and Simulations 435
Results and Discussion 436
Two-dimensional infrared spectroscopy ofGlycine-L-Alanine-Methylamide. 438
Introduction 438
Experimental 438
Results and Discussion 439
How do vibrations change their composition uponelectronic excitation? – EXSY-T2D-IRmeasurements challenge DFT calculations. 441
Introduction 441
Results and Discussion 442
Conclusions 443
Propagation and beam geometry effects on 2DFourier transform spectra of multi-level systems 444
Introduction 444
Methods 444
Results and discussion 445
Conclusion 446
References 446
Difference 2D-IR spectroscopy on thechromophore in bacteriorhodopsin 447
Introduction 447
Results 447
Conclusion and outlook 449
Coherent Control of Retinal Isomerization inBacteriorhodopsin in the High Intensity Regime 450
Introduction 450
Experimental Methods 450
Results and Discussion 451
Conclusions 452
Quantum Control of the Photoinduced WolffRearrangement of Diazonaphthoquinone in theCondensed Phase Using Mid-InfraredSpectroscopy 453
Coherent control of matter waves passing througha conical intersection in ß-carotene 456
Introduction 456
Experimental Methods 457
Conclusions 458
Mode selective single-beam coherent anti-Stokes Ramanscattering 459
1. Introduction 459
2. Experimental setup 460
3. Results and Discussion 460
4. References 461
Early Time Vibrationally Hot Ground-StateDynamics in ß-Carotene Investigated with Pump-Degenerate Four-Wave Mixing (Pump-DFWM) 462
Introduction 462
Experimental Methods 462
Results and Discussion 463
Conclusions 464
Surface Femtochemistry: Investigation andOptimization of Bond-Forming ChemicalReactions 465
Coherent Control of the Exciton Dynamics in theFMO Protein 468
Introduction 468
Experimental Methods 468
Results and Discussion 469
Conclusions 470
Coherent Control of Population Transfer in anIonic Multilevel System using Phase- andAmplitude-Shaped Femtosecond Pulses 471
Introduction 471
Experiment and Simulation 472
Results and Discussion 472
Coherent control of the efficiency of anartificial light-harvesting complex 474
Introduction 474
Experimental Methods 474
Results and Discussion 475
Conclusions 476
Strong Field Coherent Control Using 2D Spatio-Temporal Mapping 477
Introduction 477
Experimental Methods 477
Results and Discussion 477
Control of Excited-State Population andVibrational Coherence with Shaped-Resonant andNear-Resonant Excitation 480
Introduction 480
Experimental Methods 480
Results and Discussion 481
Conclusions 482
Pump-push-probe transient spectroscopy ofisolated conjugated oligomers 483
Introduction 483
Experimental Methods 484
Results and Discussion 484
Vibrational Energy Relaxation in Liquid-to-Supercritical Ammonia Studied by FemtosecondMid-Infrared Spectroscopy 486
Introduction 486
Results and Discussion 487
Probing Intermolecular Couplings inSimulations of the Two-Dimensional InfraredPhoton Echo Spectrum of LiquidWater 489
Introduction 489
Theory 489
Results and Discussion 490
Conclusions 491
Heterogeneous Dynamics of Coupled Vibrations 492
Introduction 492
Experimental Methods 492
Results and Discussion 493
Immobilized water in hydrophobic hydration 495
Introduction 495
Experiment 495
Results and Discussion 495
Conclusions 497
Collective Breakdown of H-Bonding in Ice 498
Introduction 498
Results and Discussion 498
Conclusions 500
The Dynamics of Aqueous Hydroxide IonTransport Probed via Ultrafast Vibrational EchoExperiments 501
Introduction 501
Nonlinear Infrared Spectroscopy of HOD in NaOD Solution 502
Glasslike Behaviour in Aqueous ElectrolyteSolutions 504
Mid-IR-Induced Nuclear Wavepacket Motion of aHydrogen Bonding System: Effects of Mechanicaland Electrical Anharmonic Couplings 507
Introduction 507
Methods 507
Results and Discussion 508
Ultrafast Photodecomposition of DibenzoylPeroxide studied by Time-Resolved InfraredSpectroscopy 510
Introduction 510
Results and Discussion 511
Electron detachment of OH¯(aq) 513
Introduction 513
Experimental Methods 513
Results and Discussion 514
Conclusions 515
Pathways of Vibrational Relaxation afterN-H Stretching Excitation in IntermolecularHydrogen Bonds 516
Introduction 516
Methods 516
Results and discussions 517
GHz Longitudinal and Transverse AcousticWaves andStructural Relaxation Dynamics in Liquid Glycerol 519
Introduction 519
Experimental Method and Results 519
Discussion 521
References 521
Frequency dependence of the molecularreorientation of liquid water 522
Introduction 522
Experiment 522
Results and Discussion 522
Discussion and Conclusion 524
Ultrafast Temperature Jumps in Liquid WaterStudied by Infrared-Pump and X-ray Absorption-Probe Spectroscopy 525
Influence of the Environment on ReactionDynamics: Excited State Intramolecular ProtonTransfer in the Gas Phase and in Solution 528
Unified probe process in the gas phase and in solution 528
Mechanism of the excited state intramolecular proton transfer: Transfertime and coherent wavepacket motion 529
Internal conversion through a conical intersection 530
Ultrafast 2D-IR spectroscopy of a molecularmonolayer 531
Introduction 531
Experimental Method 531
Results and Discussion 532
Conclusions 533
Frozen Dynamics and Insulation of Water at theLipid Interface 534
Introduction 534
Results and Discussion 534
Conclusions 536
Ultrafast vibrational dynamics of interfacial water 537
Introduction 537
Experimental Methods 537
Results and Discussion 538
Conclusions 539
Ultrafast Dynamics at Liquid InterfacesInvestigated with Femtosecond Time-ResolvedMultiplex Electronic Sum-Frequency Generation(TR-ESFG) Spectroscopy 540
Introduction 540
Experimental Methods 540
Results and Discussion 541
Femtosecond spectral phase shaping for CARSspectroscopy and imaging 543
Introduction 543
Setup 543
Spectroscopy 544
Conclusions 545
Part VII_Biological Systems, Molecular Light Harvesting andCharge-Transfer Complexes 546
Energy transfer along a poly(Pro) - peptide 547
Introduction 547
Materials and Methods 547
Results and Discussion 548
Conclusions 549
Energy transport in peptide helices around theglass transition 550
Introduction 550
Results and Discussion 550
Conclusions 552
Ultrafast Vibrational Dynamics of Adenine-Thymine Base Pairs in Hydrated DNA 553
Introduction 553
Experimental Methods 553
Results and Discussion 555
Ultrafast Vibrational Dynamics in the AppA BlueLight Sensing Protein 556
Introduction 556
Experimental Methods 557
Results and Discussion 557
Direct observation of ligand transfer and bond formationin cytochrome c oxidaseusing mid-infrared chirped-pulse upconversion 559
Introduction 559
Experimental approach: mid-infrared chirped-pulse upconversion 559
Results and Discussion 560
Tryptophan Residues as Natural UltrafastVoltmeters in Retinal Proteins 562
Interrogating Fiber Formation Kinetics withAutomated 2D-IR Spectroscopy 565
1. Introduction 565
2. Experimental Methods 565
3. Results and Discussion 566
4. Conclusions 567
References 567
Coherent Control of Chirality-Induced 2DElectronic Spectroscopy Signals 568
Two-Photon Two-Color Generation ofZeaxanthin Radical Cation in CP29 LightHarvesting Complex 571
Introduction 571
Experimental Methods 572
Results and Discussion 572
Conclusions 573
Rebinding of Proximal Histidine in theCytochrome c' from Alcaligenes xylosoxidansActs as a Molecular Trap for Nitric Oxide 574
Introduction 574
Experimental Methods 574
Results and Discussion 575
Conclusions 576
Two-Dimensional Electronic Spectroscopy of theLow-Light Adapted Light Harvesting Complex 4 577
Introduction 577
Experimental Methods 577
Results and Discussion 578
Conclusions 579
Three-Pulse Photon Echo Spectroscopy as a Probeof Flexibility and Conformational Heterogeneityin Protein Folding 580
Introduction 580
Methods 581
Results and Discussion 581
Ultrafast Rebinding of CO to CarboxymethylCytochrome c Probed by FemtosecondVibrational Spectroscopy 583
Introduction 583
Experimental Methods 583
Results and Discussion 584
Real-time observation of the bond lengthmodulation of carbon double bond during thephotoisomerization of bacteriorhodopsin 586
Introduction 586
Results and Discussion 587
Electron Transfer in Photosynthetic ReactionCenters: Optimization in Model and Nature 589
Introduction 589
Setup of Rate Equations for the Genetic Algorithm 589
Results and Discussion 590
Conclusions 591
Coherently Controlled Release of Drugs inOphthalmology 592
Introduction 592
Experimental Methods 592
Results and Discussion 593
Conclusions 594
Light Harvesting, Energy Transfer andPhotoprotection in the Fucoxanthin-ChlorophyllProteins of Cyclotella meneghiniana 595
Introduction 595
Experimental Methods 595
Results and Discussion 596
Conclusions 597
Primary Reaction Dynamics of Green AbsorbingProteorhodopsin WT and D97N Mutant Observedby fs Infrared and Visible Spectroscopy 598
Introduction 598
Experimental Methods 598
Results and Discussion 599
Conclusion 600
Photodynamics of a Collagen Model Peptide 601
Introduction 601
Experimental Methods 601
Results and Discussion 602
Conclusion 603
Ultrafast Charge Migration FollowingIonization in Oligopeptides 604
Introduction 604
Methodology 604
Results and Discussion 605
Probing Photodynamics of Retinal ProtonatedSchiff-Base with 7 fs Impulsive VibrationalSpectroscopy 607
Introduction 607
Experimental 607
Results 608
Discussion and Conclusion 609
The 2DIR Spectroscopy on C-D Modes of Leucined10Side Chain 610
Introduction 610
Results and Discussion 610
A Time-resolved Vibrational Spectroscopy Studyon Adenine/Thymine Based Nucleic Acid Systems 613
Introduction 613
Results and Discussion 613
Mapping Parallel Pathways of Energy Flow inLHCII with Broadband 2D ElectronicSpectroscopy 616
Introduction 616
Experimental Methods 616
Results and Discussion 617
Dissecting Exciton Dynamics Pathways inElectronic Multidimensional Spectroscopy byPulse Polarizations 619
Introduction 619
Signatures of density matrix coherences 620
Results and Discussion 620
Photoselection Polarization Experiments RevealUltrafast Electron Hopping Between DistinctAromatic Residues in the Flavoprotein DNAPhotolyase 622
Introduction 622
Experimental Methods 623
Results and Discussion 623
Conclusions 624
Quantum Coherence Accelerating PhotosyntheticEnergy Transfer 625
Introduction 625
Experimental Methods 625
Results and discussion 626
Conclusions 627
References 627
Ultrafast dynamics of light-harvesting function ofß-carotene in carbon nanotube 628
Introduction 628
Experimental Methods 628
Results and Discussion 629
Conclusions 630
Direct Femtosecond Observation of Tight andLoose Ion Pairs upon Photoinduced BimolecularElectron Transfer 631
Ultrafast Dynamics of Dansylated POPAMDendrimers and Energy Transfer in their DyeComplexes 634
Introduction 634
Experimental 635
Results and Discussion 635
Conclusions 636
Electron Transfer in a Donor/Acceptor SystemCoupled to the Surface of Metal Oxide NanoporousFilms: Direct vs. Surface ConfinedElectron Transfer 637
Introduction 637
Experimental Methods 638
Results and Discussion 638
Conclusions 639
Aqueous Proton Transfer Pathways inBimolecular Acid-Base Neutralization 640
The solvated electron dynamics in aqueousbromide studied by three-pulse-spectroscopy 643
Introduction 643
Experimental Methods 643
Results and Discussion 643
References 645
Naphthalene Bisimides: on the Way to UltrafastOpto-electronic Devices 646
Naphthalene bisimides as candidates for opto-electronics 646
Ultrafast processes in the naphthalene bisimides 647
Ultrafast Charge Photogeneration in MEH-PPVCharge-Transfer Complexes 649
Introduction 649
Results and Discussion 649
Conclusions 651
Photomodulation of Interfacial Electron Transferby Optical Switches 652
Introduction 652
Experimental Methods 653
Results and Discussion 653
Conclusions 654
Two-color two-dimensional Fourier transformspectroscopy of energy transfer 655
Introduction 655
Experimental Setup. 656
Electron Injection Dynamics of PeryleneDerivatives into ZnO and TiO2 Particle Films 658
Introduction 658
Results and Discussion 659
Conclusions 660
Part VIII_THz Science and Technology, Nano-Optics and Plasmonics 661
Dynamic Metamaterials at Terahertz Frequencies 662
Introduction 662
Results and Discussion 663
Effect of Spin-Polarized Electrons on THzEmission from Photoexcited GaAs(111) 665
Background and Introduction 665
Experimental Methods 666
Results and Discussion 666
Nonlinear Lattice Response Observed ThroughTerahertz SPM 668
Introduction 668
Experimental Methods 668
Results and Discussion 669
Conclusions 670
Ultrafast Electron Cascades Driven by IntenseFemtosecond THz Pulses 671
Introduction 671
Experimental Methods 671
Results and Discussion 671
Conclusions 673
Rabi Oscillations in a Shallow Donor SystemDriven by Intense THz Radiation 674
Introduction 674
Experiment 674
Results and Discussion 675
Conclusion 676
Nonlinear optical effects in germanium in the THzrange: THz-pump - THz-probe measurement ofcarrier dynamics 677
Introduction 677
Experimental Methods 677
Results and Discussion 678
Conclusions 679
Terahertz Nonlinear Response and CoherentPopulation Control of Dark Excitons in Cu2O 680
Introduction 680
Formation and cooling dynamics of 1s para excitons in Cu2O 680
Terahertz nonlinear control of the internal quantum state of excitons 681
Impact Ionization in InSb studied by THz-Pump-THz-probe spectroscopy 683
Introduction 683
Experimental Methods 683
Results and Discussion 684
Conclusions 685
Single Shot Linear Detection of THzElectromagnetic Fields on the Fs to Ps Scale 686
Electro-Optic Sampling for THz Spectroscopy and e- Bunch Monitoring 686
EO Sampling by Supercontinuum Encoding with Balanced Detection 687
Kerr Effect with an Optical Pulse as Fs Reference 687
Monitoring of Electron Bunches on the Ps Scale 688
Conclusion 688
Intense THz Pulses and 11-fs Electro-opticSampling with a Multi-BranchEr:fiber/Ti:sapphire Hybrid Amplifier 689
Introduction 689
Multi-branch Er:fiber – Ti:sapphire hybrid laser 689
Frequency selective surface sensor for terahertzbio-sensing applications 692
Introduction 692
Surface sensor design and fabrication 692
Experimental set-up 693
Results and discussion 693
Conclusion 694
Single cycle THz pulses in 1D and 2D photoniccrystal structures 695
Introduction 695
Experiment and Simulation 695
Results and Discussion 696
Conclusions 697
Terahertz wave from coherent LO phonon in aGaAs/AlAs multiple quantum well under anelectric field 698
Introduction 698
Experimental Methods 698
Results and Discussion 699
Conclusions 700
Improved Fast Scanning TeraHz Pulse System 701
Introduction 701
Experimental Method and Results 701
Ultrafast photoemission electron microscopy:imaging light with electrons on femto-nano scale 704
Introduction 704
Experimental method 704
Results 704
Summary 706
Ultrafast Electron Dynamics in QuantumWellStates of Pb/Si(111) Investigated byTwo-Photon Photoemission 707
Direct Visualization of Electron Emissionduring Femtosecond Laser Ablation 710
Attosecond Nanoplasmonic Field Microscope 713
1. Introduction 713
2. Calculations and Results 714
3. Conclusions 715
References 715
Coherent Control of Surface Plasmon PropagationDirections 716
Introduction 716
Experimental Methods 716
Results and Discussion 717
References 718
Ultrafast Laser-Induced Electron Emission fromField Emission Tips 719
Introduction 719
Experimental Methods 719
Emission Mechanisms 720
High Current Field Emitters 720
Conclusion 721
Simultaneous Spatial and Temporal Control ofNanooptical Fields 722
Introduction 722
Experiment 722
Results and Discussion 723
Summary 724
Nano-Confined Light and Electron SourcesDriven by Few-Cycle Optical Pulses 725
Introduction 725
Experimental Methods 725
Results and Discussion 726
Nonlinear Optical Responseof Metal Nanoantennas 728
Introduction 728
Experimental Methods 729
Results and Discussion 729
Outlook 730
Near-Field Imaging of Single-Cycle THz PulsesTransmitted Through Sub-WavelengthMetallic Slit Structures 731
Introduction 731
Experiment and Simulation 731
Results 732
Conclusion and Outlook 733
Nanoscale Optical Microscopy in the VectorialFocusing Regime 734
Introduction 734
Experiment 735
Results and Discussion 735
Conclusions 736
Ultrafast Wide-Field Fluorescence Microscopy 737
Introduction 737
Experimental Method 737
Results and Discussion 738
Conclusions 739
Measurement of Dispersion Properties of SilverNanowires Used as Plasmon Waveguides 740
Introduction 740
Experimental Methods 740
Results and Discussion 741
Conclusions and Future Work 742
Part IX_Novel Pulsed Sources: oscillators, amplifiers, nonlinear mixing 743
Pulse energies exceeding 20 mJ directly from afemtosecond Yb:YAG oscillator 744
Introduction 744
Experiment 744
Results and Conclusion 745
Fundamentally Mode-locked 3 GHz FemtosecondErbium Fiber Laser 747
Introduction 747
Design Considerations 748
Experimental Setup 748
Conclusions 749
Ultrabroadband Er:fiber Systemsand Applications 750
Introduction 750
Systems Performance and Applications 750
Conclusions 752
Compact high Power Ytterbium based fs-Oscillator-Amplifier System 753
Introduction 753
Setup 753
Results 754
Fiber laser pumped high average power singlecycleTHz pulse source 756
Introduction 756
Experimental Methods 756
Results and Discussion 757
Conclusions 758
Millijoule Pulse Energy High Repetition RateFemtosecond Fiber CPA System: Results,Micromachining Application and Scaling Potential 759
Introduction 759
Experimental Setup and Results 759
Conclusions 761
Femtosecond thin disk lasers with > 10 µJ pulseenergy for high field physics at multi-megahertzrepetition rates
Introduction and motivation 762
Femtosecond thin disk laser 762
Photoelectron imaging spectroscopy (PEIS) 763
Summary and conclusions 764
Ultra-high intensity-High Contrast 300-TW laserat 0.1 Hz repetition rate. 765
1. Introduction 765
2. Laser design 765
3. Experimental results 766
4. Conclusion 767
Highly Efficient, Low-Cost Diode-PumpedFemtosecond Cr3+:LiCAF Lasers 768
Introduction 768
Experimental Setup 769
Results and Discussion 769
Conclusions 770
Environmentally stable 200-fs Yb-doped fiberlaser with dispersion compensation by photoniccrystal fiber 771
1. Introduction 771
2. Photonic crystal fiber 771
3. Environmentally stable mode-locked laser 772
4. Conclusions 773
Noncollinear Optical Parametric AmplificationPumped by the Third Harmonics ofa Ti:sapphire Laser 774
Introduction 774
Experiments 774
Results and Discussion 775
Conclusion 776
Sub-10 fs Pulse Generation in Vacuum UltravioletUsing Chirped Four Wave Mixing in HollowFibers 777
Introduction 777
Results and Discussion 778
Conclusions 779
Generation of High Energy Pulses from a FiberbasedFemtosecond Oscillator 780
Introduction 780
Experimental Methods 780
Results and Discussion 781
Conclusions 782
Femtosecond passively mode-locked fiber lasersusing saturable Bragg reflectors 783
Introduction 783
Experimental Results 783
Linear soliton laser 783
Stretched-pulse laser 784
Discussion and conclusion 785
Noncollinear optical parametric amplification ofcw light, continua and vacuum fluctuations 786
Influence of the seed light on the output of parametric amplifiers 786
Amplification of cw light in femtosecond and picosecond pumped NOPAs 786
Comparison of cw-, continuum- and OPG-seeded NOPAs in the fs-regime 787
Modeling of Octave-Spanning Sub-Two-CycleTitanium:Sapphire Lasers: Simulation andExperiment 789
Introduction 789
Laser Model 789
Experimental Setup 790
Pulse Dynamics in the Laser 790
Conclusions 791
Ultra-Broadband Infrared Pulses from aPotassium-Titanyl Phosphate Optical ParametricAmplifier for VIS-IR-SFG Spectroscopy 792
Chirped-pulse Raman amplification fortwo-color high-intensity laser experiments 795
Introduction 795
Results and Discussion 796
Generation of Broadband mid-infrared Pulsesfrom an Optical Parametric Amplifier 798
References 800
Optimized 2-micron Optical Parametric ChirpedPulse Amplifier for High Harmonic Generation 801
Generation of sub-20-fs, two-colordeep-ultraviolet pulses by four-wave mixingthrough filamentation in gases 804
Efficient ultrafast four-wave opticalparametric amplification in condensed bulkmedia 807
Introduction 807
Experimental Methodology 807
Results and Discussion 808
Conclusions 809
Cascaded four-wave mixing technique for highpowerfew-cycle pulse generation 810
Introduction 810
Experimental setup and results 811
Conclusions 812
2 MHz repetition rate - 15 fs fiber amplifierpumped optical parametric amplifier 813
Introduction 813
Experiment and Results 813
Scaling Considerations 815
Conclusions 815
Octave-wide tunable NOPA pulses at up to 2 MHzrepetition rate 816
Complete spectral coverage for ultrafast spectroscopy 816
Octave-wide tunability with femtosecond UV pumping 817
Investigation of phase dependencies in optical parametric amplification 817
Asymptotic pulse shapes and pulseself-compression in femtosecond filaments 819
Efficient and Highly Coherent Extreme-Ultraviolet High-Harmonic Source 822
Introduction 822
Experimental Methods 822
Results and Discussion 823
Conclusions 824
References 824
Single-stage Pulse Compression and High-EnergySupercontinuum generation from a Chirped-pulseoscillator 825
Introduction 825
Experimental setup 826
Results and Discussion 826
An All-Optical Synchrotron Light Source 828
Introduction and Motivation 828
Results and Prospects 829
Compression of an Ultraviolet Pulse by MolecularPhase Modulation and Self-Phase Modulation 831
Introduction 831
Experimental Methods 831
Results and Discussion 832
Conclusions 833
Temporal Optimization of UltrabroadbandOptical Parametric Chirped Pulse Amplification 834
Third Harmonic X-waves Generation byFilamentation of Infrared Femtosecond LaserPulses in Air 837
Introduction 837
Experimental Methods 837
Results and Discussion 838
Conclusions 839
Generation and control of coherent conical pulsesin seeded optical parametric amplification 840
Introduction 840
Experimental Methods 841
Results and Discussion 841
Conclusions 842
Generation of Ultrashort O ptical Pu lses Us ingMultiple Coherent Anti-Stokes Raman ScatteringSignals in a Crystal and Observation of theRaman Phase 843
Introduction 843
Experimental Setup and Results 843
Discussion 844
Conclusions 845
References 845
Generation of High-power Visible and UV/VUVSupercontinua and Self-compressed Single-cyclePulses in Metal-dielectric HollowWaveguides 846
Part X_Frequency Combs andWaveform Synthesis 849
CEO-Phase Stabilized Few-Cycle FieldSynthesizer 850
Introduction 850
Field Synthesizer 850
Results and Discussion 851
Conclusions 852
High-power, mHz linewidth Yb:fiber opticalfrequency comb for high harmonic generation 853
Introduction 853
Experimental Methods and Results 854
Conclusions 855
High Harmonic Frequency Combs for HighResolution Spectroscopy 856
Introduction 856
Experimental Methods 856
Results and Discussion 857
Conclusions 858
Ultrafast double pulse parametric amplificationfor precision Ramsey metrology 859
Introduction 859
Phase-stable double pulse NOPCPA 860
Results 861
Towards Versatile Coherent Pulse Synthesis usinga Femtosecond Laser and Synchronously PumpedOptical Parametric Oscillator 862
Introduction 862
Experiment 862
Results 863
Conclusions 864
Frequency comb spectroscopy on calcium ionsin a linear Paul trap 865
Introduction 865
Experimental methods 865
Trapping and laser cooling of calcium ions. 865
Spectroscopy on calcium ions 866
Results and Discussion 867
Conclusions 867
Generation of octave-spanning Raman combstabilized to an optical frequency standard 868
Introduction 868
Experimental Methods 868
Results and Discussion 869
Tunable, octave-spannning supercontinuumdriven by X-Waves formation in condensedKerr media. 871
Toward Ultrafast Optical Waveform Synthesiswith a Stabilized Ti:Sapphire Frequency Comb 874
Introduction 874
Setup 874
Results 876
Conclusion 876
References 876
Multimillijoule Optically Synchronized andCarrier-Envelope-Phase-Stable ChirpedParametric Amplification at 1.5 µm 877
5-fs multi-mJ CEP-locked parametric chirpedpulseamplifier at 1 kHz 880
Introduction 880
Gain spectra with several pump wavelengths 880
Experiment 881
Conclusions 882
Sub-two-cycle pulses at 1.6 µm from an opticalparametric amplifier 883
References 885
Carrier envelope offset control of broadRaman sidebands by locking two pump laserfrequencies to a single optical cavity 886
Introduction 886
Experimental Methods 887
Results and Discussion 887
Cancellation of the coherent accumulation inrubidium atoms excited by a train offemtosecond pulses 889
Introduction 889
Experimental Methods 890
Results and Discussion 890
Conclusions 891
Part XI_Optics, Optoelectronics, Measurement, Diagnostics andInstrumentation 892
Sub-10-fs XUV Tunable Pulses at the Output of aTime-Delay-Compensated Monochromator 893
Introduction 893
Experimental Results 893
Conclusions 895
First Step Towards a Femtosecond VUVMicroscope: Zone Plate Optics asMonochromator for High-Order Harmonics. 896
Introduction 896
Experimental Set-up 896
Results 897
Conclusions 898
Measurement of Electron Pulse Duration byAttosecond Streaking 899
Introduction 899
Proposed Experiment 899
Numerical Results 900
Conclusion 901
Nanoscale Spatial Effects of Pulse Shaping 902
Introduction 902
Spatio-temporal coupling 902
Spatial shaping effects in a focus 903
Conclusions 904
Designer Femtosecond Pulse Shaping UsingGrating-Engineered Quasi-Phasematching inLithium Niobate 905
Introduction 905
Crystal design and experiment 905
Results and discussion 907
Conclusions 907
Direct Measurement of Spectral Phase forUltrashort Laser Pulses Based on IntrapulseInterference 908
Introduction 908
Experimental Methods 908
Results and Discussion 909
Measurements with an adaptive pulse shaper 909
Measurements without an adaptive pulse shaper 910
Conclusions 910
Two Dimension Spatial Light Modulator with anOver-Two-Octave Bandwidth for High-PoweredMonocycle Optical Pulses 911
1. Introduction 911
2. Structure of 2D-SLM 911
3. Optical damage of 4-f phase compensator with 2D·UV-LC-SLM 911
4. Feedback chirp compensation experiment in the near-infrared (NIR)region 912
5. Feedback chirp compensation experiment in the UV region 912
6. Conclusions 912
References 913
Vector Pulse Shaper Assisted Short PulseCharacterization 914
Introduction 914
Experiment and Simulation 914
Results and Discussion 915
Femtosecond Spectral Interferometry withAttosecond Accuracy by Correction forSpectrometer Resolution Asymmetry 917
Introduction 917
Experiment 917
Analysis 918
Results and Conclusions 918
Spatial phase control and applications of highorderharmonics 920
Introduction 920
EUV spatial phase shaping 920
Applications of high-order harmonic based source 921
Conclusions 922
A New Generalized Projections Algorithm GearedTowards Sub-100 Attosecond PulseCharacterization 923
Introduction 923
Methods 923
Results 924
Conclusion 925
Characterization of Mid-Infrared Pulses by Time-Encoded Arrangement 926
Introduction 926
TEA SPIDER 926
Conclusions 928
Intensity and phase measurements of thespatiotemporal electric field of focusingultrashort pulses 929
Introduction 929
Experimental Results 930
Polarization, ionization and spatial gates in singleattosecond pulse generation 932
Introduction 932
Results and Discussion 933
All dispersive mirrors compressor for femtosecond lasers 935
Introduction 935
High dispersive chirped mirrors 936
Conclusions 937
Optical Mapping of Attosecond IonizationDynamics by Few-Cycle Light Pulses 938
Polarization, Phase and Amplitude Controland Characterization of Ultrafast Laser Pulses 941
Silicon-Chip-Based Single-Shot Ultrafast OpticalOscilloscope 944
Introduction 944
Time-to-Frequency Conversion 944
Silicon-Chip-Based Ultrafast Optical Oscilloscope 945
Time-resolved off-axis digital holography forcharacterization of ultrafast phenomena in water 947
Introduction 947
Method 947
Results and Discussion 948
Conclusions 949
3 GHz RF Streak Camera for Diagnosis of sub-100 fs, 100 keV Electron Bunches 950
Simulations of Frequency-Resolved OpticalGating for measuring very complex pulses 953
Introduction 953
Conclusions 955
References: 955
Electron density gradient measurement for laserwakefield accelerator 956
Introduction 956
Experimental Setup 956
Results and Discussion 957
10-femtosecond Precision, Long-term StableTiming Distribution Over Multiple Fiber Links 959
Two-dimensional pulse shapers capable ofmore than phase & amplitude modulation
Introduction 962
Polarization control along with phase & amplitude modulation usingmulti-pass 2D LC-SLM
Full control over optical e-field superposition of w +2w pulses 963
Adaptive Phase Shaping in a Fiber Chirped PulseAmplification System 965
Introduction 965
Experimental Details 965
Results 967
Conclusions 967
Two-dimensional Fourier transform electronicspectroscopy with a pulse-shaper 968
Introduction 968
Probing Anomalous Spectral Diffusion andExciton Fluctuations by CoherentMultidimensional Spectroscopy 971
1. Introduction 971
2. Anomalous relaxation and 2D lineshapes 971
2.1. Stationary ensembles (1 < a <
2.2. Aging spectral diffusion with (0 <
3. Peaks induced by slow bath fluctuations 973
Noninterferometric Two-Dimensional FourierTransform Spectroscopy 974
Introduction 974
Experimental Methods 974
Results and Discussion 975
Conclusion 976
Part XII_Applications of Ultrashort Pulses 977
Filament-induced electric events in thunderstorms 978
Introduction 978
Experimental methods 978
Results and discussion 979
Conclusion 979
Optimizing laser-induced refractive index changesin “thermal” glasses 981
Introduction 981
Experimental Methods 981
Results and Discussion 981
Conclusions 983
Femtosecond laser fabrication for the integrationof optical sensors in microfluidic lab-on-chipdevices 984
Tailored Femtosecond Pulses for Nanoscale LaserProcessing of Dielectrics 987
Introduction 987
Experiment 987
Results and Discussion 988
Conclusions 989
Electric Field Detection of Near-Infrared LightUsing Photoconductive Sampling 990
Introduction 990
Experimental Methods 990
Results and Discussion 991
Conclusions 992
Fluorescence-Detected Two-DimensionalElectronic Coherence Spectroscopy by Acousto-Optic Phase Modulation 993
Introduction 993
Experimental Methods 993
Results and Discussion 994
Conclusions 995
Single-pulse standoff nonlinear Ramanspectroscopy using shaped femtosecond pulses 996
Introduction 996
Results and Discussion 997
Multiphoton Microscopy by MultiexcitonicLadder Climbing in Colloidal Quantum Dots 999
Introduction 999
Background 999
Experimental demonstration 1000
Conclusions 1001
Real-time wave-packet engineeringusing a sensitive wave-packet spectrometerand a pulse-shaper 1002
Introduction 1002
Experimental Methods 1002
Results 1003
Discussion and Conclusion 1003
Grating Enhanced Ponderomotive Scatteringfor Characterization of Femtosecond ElectronPulses 1005
CARS Microspectrometer with a SuppressedNonresonant Background 1008
Introduction 1008
Experimental Methods 1008
Results and Discussion 1009
Conclusions 1010
Resonant and Nonresonant Stimulated ParametricFluorescence Microscopy 1011
Introduction 1011
Experimental Methods 1012
Results and Discussion 1012
Femtosecond pump-probe spectroscopy as aninstrument for nanostructured materialsinvestigation. 1014
Selective excitation in nonlinear microscopy byusing an ultra-broadband pulse 1017
Introduction 1017
Principle of selective excitation of single vibrational mode 1017
Experimental 1018
Conclusions 1019
Interferometrically Detected Femtosecond CARSin a Single Beam of Shaped Femtosecond Pulses 1020
Introduction 1020
Single-Beam Heterodyne CARS 1020
All-Fibre-Implementation 1022
Advantages of Two-photon Microscopy withUltrashort Pulses 1023
Introduction 1023
Experimental Methods and Results 1023
Summary 1025
Development of laser-based imaging systems formedical diagnostics 1026
Introduction 1026
Laser system with wavelength flexibility 1027
Single-shot optical coherence tomography 1027
Results and prospects 1028
Frequency shifts at the fiber-optical eventhorizon 1029
Introduction 1029
Experiment 1029
Results 1030
Conclusion 1031
Index of Contributors 1032