Ultrafast Phenomena XIX (eBook)

Preface 6
Contents 8
Contributors 32
Part I Attosecond and High-Order HarmonicGeneration and Applications 82
1 Attosecond Control of Electron Emission in Two-Color Ionization of Atoms 83
Abstract 83
1 Introduction 83
2 Results and Discussion 84
3 Conclusions 86
Acknowledgments 86
References 86
2 Probing Xenon Electronic Structure by Two-Color Driven High-Order Harmonic Generation 87
Abstract 87
1 Introduction 87
2 The Giant Resonance in Xenon 88
3 Experimental Results 88
4 Conclusions 90
References 90
3 Strong Field Applications of Gigawatt Self-compressed Pulses from a Kagome Fiber 91
Abstract 91
References 95
4 Intense Attosecond Pulses for Probing Ultrafast Molecular Dynamics 96
Abstract 96
1 Introduction 96
2 Nonlinear Fourier Transformation Spectroscopy with Intense Attosecond Pulse Train 97
3 Generation of Multi-gigawatt Isolated Attosecond Pulses 98
References 98
5 Disentangling Structural and Dynamical Effects via Multidimensional High Harmonic Spectroscopy 100
Abstract 100
1 Introduction 100
2 Experimental Setup and Results 101
References 103
6 Attosecond Frequency Resolved Momentum Imaging of Two-Photon Dissociative Ionization Dynamics of Nitrogen Molecule 104
Abstract 104
1 Introduction 104
2 Experimental Setup 105
3 Results and Discussion 105
Acknowledgments 107
References 107
7 High-Order Harmonics Fourier Transform Spectroscopy of Two-Photon Dissociative Ionization of Hydrogen Molecules 108
Abstract 108
1 Introduction 108
2 Experimental 109
3 Results and Discussion 110
Acknowledgments 111
References 111
8 Simultaneous Observation of Vibrational Wavepackets of Nitrogen Molecule in Neutral and Singly-Charged Manifolds 112
Abstract 112
1 Introduction 112
2 Experimental Setup 113
3 Results and Discussion 113
Acknowledgments 115
References 115
9 Photo Ionization Time Delay in Molecular Hydrogen 116
Abstract 116
1 Introduction 116
2 Setup 117
3 Results 117
References 119
10 Ultrafast Relaxation and Photodissociation Dynamics of 1,3-Butadiene Studied by Probing Molecular Orbitals 120
Abstract 120
References 123
11 Ultrafast and Photodissociation Dynamics of 1,2-Butadiene Studied by Photoelectron Spectroscopy 124
Abstract 124
References 127
12 Direct Comparison of Multi-photon and EUV Single-Photon Probing of Molecular Relaxation Processes 128
Abstract 128
1 Introduction 128
2 Experimental 129
3 Results and Discussion 129
Acknowledgments 130
References 131
13 Sub-4-fs Charge Migration in Phenylalanine 132
Abstract 132
Acknowledgments 134
References 135
14 Recombination-Induced Autoionization Process in Rare-Gas Clusters 136
Abstract 136
1 Introduction 136
2 Experiment 137
3 Results and Discussion 137
References 139
15 X-Ray Magnetic Circular Dichroism Probed Using High Harmonics 140
Abstract 140
References 143
16 Extreme Ultraviolet Transient Grating Measurement of Insulator-Metal Transition Dynamics in VO2 144
Abstract 144
1 Introduction 144
2 Experiment 145
3 Results 145
Acknowledgments 147
References 147
17 Delayed Core-Level Photoemission from the van der Waals Crystal WSe2 148
Abstract 148
1 Introduction 148
2 Experimental Setup 149
3 Results and Discussion 149
References 151
18 Optimization of Quantum Trajectories Driven by Strong-Field Waveforms 152
Abstract 152
References 157
19 Phase-Matched Generation of High Order Harmonic for Study of Molecular Dynamics 158
Abstract 158
1 Introduction 158
2 Experimental Results and Discussions 159
References 161
20 Multiphoton Transitions for Robust Delay-Zero Calibration in Attosecond Transient Absorption 163
1 Introduction 163
2 Results 164
3 Conclusion and Outlook 164
References 166
21 Infrared Double Optical Gating for Generating Submicrojoule Isolated Attosecond Pulses 167
Abstract 167
1 Introduction 167
2 High-Energy Continuum Harmonic Spectra 168
References 170
22 Generation of Isolated Soft X-Ray Pulses Around the Carbon K-Edge Using CEP-Stabilized Few-Cycle IR Pulses 171
Abstract 171
1 Introduction 171
2 CEP-Dependent HHG 172
3 Pressure Dependence of HH Spectra 173
4 Conclusion 174
References 174
23 Bright Isolated Attosecond Soft X-Ray Pulses 175
Abstract 175
Acknowledgement 178
References 178
24 Strong-Field-Enhanced Forward Scattering of High-Order Harmonics 179
Abstract 179
References 182
Part II Atomic, Molecular and OpticalSciences—Gas Phase 183
25 Non-adiabatic Effects in Electron Momenta 184
Abstract 184
1 Strong Field Ionization 184
2 Field Intensity Calibration 185
3 Quantitative Comparison of Theory and Experiment 185
4 Conclusion and Outlook 186
Acknowledgements 186
References 187
26 Determination of Absolute Cross-Sections of Nonresonant EUV-UV Two-Color Two-Photon Ionization of He 188
Abstract 188
1 Introduction 188
2 Experimental 189
3 Results and Discussion 190
References 191
27 Attosecond Spatial Control of Electron Wave Packet Emission Dynamics 192
Abstract 192
1 Introduction 192
Acknowledgements 195
References 196
28 Probing Elastic Rescattering Through Half-Cycle Cutoffs in Above-Threshold Ionization Spectra 197
Abstract 197
1 Introduction 197
2 Experimental Setup 198
3 Analysis and Conclusions 198
References 200
29 Experimental Signature of Light Induced Conical Intersections in Diatomics 201
Abstract 201
Acknowledgments 203
References 203
30 Sub-femtosecond Steering of Carbon Hydrogen Bonds 205
Abstract 205
1 Introduction 205
2 CEP Dependent Asymmetry of the Deprotonation in Acetylene Dication 206
3 Mechanism of the Directional Control via the CEP 207
References 208
31 Tabletop Imaging of Structural Evolutions in Chemical Reactions 209
Abstract 209
1 Introduction 209
2 Results and Discussion 210
References 212
32 Structure Dependence of Kinetic Energy Released in X-ray-Induced Fragmentation 213
Abstract 213
Acknowledgments 215
References 216
33 Controlling Fragmentation Reactions of Polyatomic Molecules with Impulsive Laser Alignment 217
Abstract 217
Acknowledgments 221
References 221
34 Intense Field Ionization of C2H2 and 12C13CH2 Aligned in Field-Free Space 222
Abstract 222
1 Introduction 222
2 Experiment 223
3 Results and Discussion 223
References 225
35 Ionization of Aligned O2 by Intense Laser Pulse 226
Abstract 226
1 Introduction 226
2 Experiment 227
3 Results and Discussion 227
References 228
36 Strong-Field Electronic Control of Multiple-Bond Breaking Dynamics in Ethylene 229
Abstract 229
Acknowledgments 233
References 233
37 Electronic Pre-determination of Ethylene Fragmentation Dynamics 234
Abstract 234
Acknowledgments 237
References 238
38 Long-Lived Neutral H _{2} in Hydrogen Migration Within Hydrocarbon Dication 239
Abstract 239
1 Introduction 239
2 Results and Discussion 240
References 242
39 Pump-Probe Photoelectron Imaging with 90-nm Excitation Pulses 243
Abstract 243
1 Introduction 243
2 Experiments and Results 244
3 Conclusions 246
References 246
40 Time-Resolved Coulomb Explosion Imaging of Ultrafast Fragmentation of CS2 in Highly Charged States 247
Abstract 247
1 Introduction 247
2 Experiment 248
3 Results and Discussion 249
4 Conclusion 249
References 249
41 Initial Phase Shifts in the Quantum Beat Resulting from the Ultrafast Internal Conversion of Pyrazine 251
Abstract 251
1 Introduction 251
2 Results 252
3 Conclusions 253
References 254
42 Ab Initio Quantum Dynamical Study on Ultrafast Nonradiative Transition Pathways of Pyrazine 255
Abstract 255
1 Introduction 255
2 Computational Outline 256
3 Results and Discussion 257
References 258
43 The Ultrafast Wolff Rearrangement in the Gas Phase 259
Abstract 259
1 Introduction 259
2 Experimental Results 259
3 Conclusion 261
References 261
44 Time-Resolved Photoelectron Spectroscopy and Ab Initio Multiple Spawning Studies of Hexamethylcyclopentadiene 263
Abstract 263
1 Introduction 263
2 Methods 264
3 Results and Discussion 264
References 266
45 Laser-Assisted Electron Diffraction for Probing Femtosecond Nuclear Dynamics of Gas-Phase Molecules 267
Abstract 267
1 Introduction 267
2 Experiment 268
3 Results and Discussion 268
4 Conclusion 269
References 270
46 Filament-Driven Lasing Action for Combustion Diagnosis 271
Abstract 271
1 Introduction 271
2 Experimental Results and Discussion 272
3 Summary 273
References 273
Part III Solid State Physics and Chemistry 275
47 Anomalous Phase Change in [(GeTe)2/(Sb2Te3)]20 Superlattice Observed by Coherent Phonon Spectroscopy 276
Abstract 276
1 Introduction 276
2 Experiment 277
3 Result 277
4 Discussion 278
5 Conclusion 278
References 278
48 Dynamical Coupling of Rabi Oscillation to Coherent Phonon in Semiconductor Microcavities 279
Abstract 279
1 Introduction 279
2 Experiment 280
3 Experimental Results and Discussion 280
References 282
49 Coherent Control Over Two-Dimensional Lattice Vibrational Trajectories in alpha -Quartz Using Polarization Pulse Shaping 283
Abstract 283
1 Introduction 283
2 Methods 284
3 Results 285
4 Discussion and Conclusion 285
References 286
50 Ultrafast Lattice Dynamics of Phase-Change Materials Monitored by a Pump-Pump-Probe Technique 287
Abstract 287
1 Introduction 287
2 Experimental 288
3 Results and Discussion 288
4 Summary 289
Acknowledgement 289
References 290
51 Enhancement of Superconducting Coherence in YBa2Cu3Ox by Resonant Lattice Excitation 291
Abstract 291
References 294
52 Coherent Phonon Dynamics in Singlet Fission of Rubrene Single Crystal 295
Abstract 295
1 Introduction 295
2 Experimental Methods 296
3 Results and Discussion 296
Acknowledgments 297
References 298
53 Acceleration of Ultrafast Singlet Fission in Aza-Derivative of TIPS-Pentacene 299
Abstract 299
1 Introduction 299
2 Experimental Details 300
3 Results and Discussion 300
References 302
54 Vibrational Coherence Reveals the Role of Dark Multiexciton States in Ultrafast Singlet Exciton Fission 303
Abstract 303
References 306
55 Ultrafast Carriers Dynamics in Silicon: A Joint Experimental and Theoretical Study 307
Abstract 307
Acknowledgments 309
References 309
56 Ultrabroadband Infrared Pump-Probe Spectroscopy Using Chirped-Pulse Upconversion 310
Abstract 310
References 312
57 Investigation of Laser-Induced Currents in Large-Band-Gap Dielectrics 314
Abstract 314
1 Introduction 314
2 Experimental Setup and Results 315
3 Conclusion and Outlook 316
References 317
58 Field-Induced Dynamics of Correlated Electrons in LiH and NaBH4 318
Abstract 318
1 Introduction 318
2 Results 319
References 320
59 Spontaneous Formation of Correlated Charge Coherence Induced by 1.5-Cycle Pulse in 1-D Organic Metal (TMTTF)2AsF6 321
Abstract 321
1 Introduction 321
2 Experiment 322
3 Results and Discussions 322
4 Summary 324
References 324
60 Coherent Dynamics of Structural Symmetry During the Ultrafast Melting of a Charge Density Wave 325
Abstract 325
1 Introduction 325
2 Experimental 326
3 Results and Discussion 326
References 327
61 10 fs Dynamics of Photoinduced Magnetic Transition in Double-Layered Charge Ordering in LuFe2O4 Under Interlayer Excitation 329
Abstract 329
1 Introduction 329
2 Experiment 330
3 Results and Discussions 330
4 Summary 332
References 333
62 Magnetically Induced Lattice Dynamics in a Magnetoelectric Antiferromagnet Cr2O3 334
Abstract 334
1 Introduction 334
2 Sample and Experiment 334
3 Result and Discussion 335
References 336
63 Coherent Magnetism: Pushing the Limits of Spin-Photon Interaction 337
Abstract 337
1 Introduction 337
2 9 fs Magneto Optical Four Wave Mixing Experiment 338
3 Microscopic Origin of the Magneto-optical Coherent Emission 339
Acknowledgement 340
References 340
64 Quantum Droplets of Electrons and Holes in GaAs Quantum Wells 341
Abstract 341
References 343
65 Exciton Dynamics in Cu-Doped InAs Colloidal Quantum Dots 344
Abstract 344
1 Introduction 344
2 Experiments 345
3 Conclusions 346
References 347
66 Rabi Oscillations in an InAs Quantum Dot Ensemble Observed in Pre-pulse 2D Coherent Spectroscopy 348
Abstract 348
1 Introduction 348
2 Results and Discussion 349
References 351
67 Slow Electron Cooling Dynamics of Highly Luminescent CdSxSe1-x Alloy Quantum Dot 352
Abstract 352
1 Introduction 352
2 Results and Discussion 353
3 Conclusion 354
References 355
68 Ultrafast Dynamics Related to Spin Crossover Processes in Single Crystal [FeII(bpy)3](PF6)2 356
Abstract 356
1 Introduction 356
2 Experimental Methods 357
3 Results and Discussion 358
References 359
69 Femtosecond Electron Diffraction Study of the Spin Crossover Dynamics of Single Crystal [Fe(PM-AzA)2](NCS)2 360
Abstract 360
1 Introduction 360
2 Experimental Methods 362
3 Results and Discussion 362
Acknowledgements 362
References 363
70 Ab Initio Solution of Structural Dynamics with Ultrafast Electron Diffraction and Charge Flipping 364
Abstract 364
1 Introduction 364
2 Experimental Methods 365
3 Preliminary Results 366
References 367
71 Laser Streaking of Free-Electron Pulses at 25 keV 368
Abstract 368
1 Introduction 368
2 Concept, Experiment, Results 369
3 Conclusions 371
References 371
72 Ultrafast Single-Electron Diffraction 372
Abstract 372
1 Introduction 372
2 Single-Electron Pulse Compression 373
3 Time-Resolved Single-Electron Diffraction 374
4 Conclusions 375
References 375
Part IV Interfacial, Surface, Thin Filmsand Carbon Nanotubes 376
73 Hydrated Phospholipid Surfaces Probed by Ultrafast 2D Spectroscopy of Phosphate Vibrations 377
Abstract 377
References 379
74 Femtosecond Time and Angle Resolved Photoemission Spectroscopy of Liquids 381
Abstract 381
Acknowledgments 383
References 384
75 Ultrafast Vibrational Dynamics of Water at a Zwitterionic Lipid/Water Interface Revealed by Two-Dimensional Heterodyne-Detected Vibrational Sum Frequency Generation (2D HD-VSFG) 385
Abstract 385
1 Introduction 385
2 Experimental Methods 386
3 Results and Discussion 387
References 388
76 Ultrafast Vibrational Spectroscopy at Liquid Interfaces by Heterodyne-Detected Sum-Frequency Generation 389
Abstract 389
1 Introduction 389
2 Infrared-Excited TR-HD-VSFG and 2D HD-VSFG to Study Ultrafast Vibrational Dynamics at Liquid Interfaces 390
3 Ultraviolet-Excited TR-HD-VSFG to Study Ultrafast Photochemical Dynamics at Liquid Interfaces 391
References 392
77 Ultrafast Electron Solvation at the Room Temperature Ionic Liquid/Metal Interface 393
Abstract 393
1 Introduction 393
2 Results and Discussion 394
3 Conclusions 396
References 396
78 Ultrafast Spectroscopy Reveals Bulk Heterojunction Morphology 397
Abstract 397
1 Introduction 397
2 Experimental 398
3 Results 398
References 400
79 Toward Ultrafast In Situ X-ray Studies of Interfacial Photoelectrochemistry 401
Abstract 401
1 Introduction 401
2 Experiments and Results 402
Acknowledgment 404
References 404
80 Ultrafast Dynamics in Epitaxial Silicene on Ag(111) 405
Abstract 405
Acknowledgments 407
References 407
81 Accessing Energy-Dependent Photoemission Delays in Solids 409
Abstract 409
1 Introduction 409
2 Results 410
3 Conclusion and Outlook 411
References 412
82 Visualization of Ultrafast Electron Dynamics Using Time-Resolved Photoemission Electron Microscopy 413
Abstract 413
1 Introduction 413
2 Experimental 414
3 Results 414
3.1 Carrier Lifetime in a Si Nanowire 415
3.2 Electron Drift Velocity and Mobility on a GaAs Surface [3] 415
References 416
83 A New Regime of Nanoscale Thermal Transport: Collective Diffusion Counteracts Dissipation Inefficiency 417
Abstract 417
1 Introduction 417
2 A New Regime of Nanoscale Thermal Transport 418
3 The Experiment 419
4 Characterizing Phonon Transport in Materials 419
Acknowledgments 420
References 420
84 Laser-Induced Plasma Dynamics Imaged by Femtosecond In-Line Holography 421
Abstract 421
1 Experimental Setup and Numerical Approach 421
2 Results and Discussion 422
Acknowledgments 423
References 423
85 Resonant Optical Kerr Response with Ultrashort Decay Time by Nonlocal Wave Coupling of Light and Excitons 424
Abstract 424
1 Experimental Procedures 425
2 Results and Discussion 425
Acknowledgments 427
References 427
86 Single-Shot Real-Time Observation of Ultrafast Amorphization in Ge2Sb2Te5 Thin Film 428
Abstract 428
1 Introduction 428
2 Experimental Method 429
3 Results and Discussion 430
4 Summary 430
Acknowledgments 430
References 431
87 Electrochemical Control of Coherent Phonon Generations in Single-Walled Metallic Carbon Nanotubes 432
Abstract 432
1 Introduction 432
2 Experiments 433
3 Results and Discussion 433
4 Conclusion 434
References 435
88 Ultrafast Charge Photogeneration and Dynamics in Semiconducting Carbon Nanotubes 436
Abstract 436
Acknowledgments 438
References 438
89 Thickness Dependent Hot-phonon Effects Observed by Femtosecond Mid-infrared Luminescence in Graphene 439
Abstract 439
1 Introduction 439
2 Experiment 440
3 Results and Discussion 440
References 442
Part V Chemistry—Liquid Phase 443
90 Discriminating Racemic from Achiral Solutions with Femtosecond Accumulative Spectroscopy 444
Abstract 444
1 Introduction 444
2 Measurement Principle and Experimental Results 444
3 Discussion and Outlook 446
References 447
91 Quantum Dynamics of Molecular Reactions Directed by Explicit Solvent Environment 448
Abstract 448
1 Ultrafast Chemical Reactions in Solution 448
2 Photochemical Bond Cleavage in Acetonitrile 449
3 Solvent Potential Extracted from Classical Molecular Dynamics Simulations 449
4 Quantum Dynamics in the Combined Potential of the Molecule and Its Surrounding 451
References 452
92 Excited-State Dynamics of Catalytically Active Transition Metal Complexes Studied by Transient Photofragmentation in Gas Phase and Transient Absorption in Solution 453
Abstract 453
1 Introduction 453
2 Results and Discussion 454
3 Conclusions 455
Acknowledgments 456
References 456
93 Coherent Control of the Photodissociation of Triiodide in Solution Reveals New Pathways 457
Abstract 457
1 Introduction 457
2 Experimental Methods 458
3 Results and Discussion 458
Acknowledgments 460
References 460
94 Multidimensional Photochemistry Model: Application to Aminobenzonitrile and Benzopyran 461
Abstract 461
1 Aminobenzonitrile (ABN, R = H) versus Dimethylaminobenzonitrile (DMABN, R = CH3) Charge Transfer 462
2 Photoisomerisation of Benzopyran (the Spiropyran Chromophore) 464
References 465
95 Tuning of Isomerization Rates in Indigo-Based Photoswitches 466
Abstract 466
1 Introduction 466
2 Experimental 467
3 Results and Discussions 467
References 469
96 Bimolecular Reactions on a Timescale Below 1 ps 470
Abstract 470
1 Beating Diffusion to Get Access to the Intrinsic Rates of Bimolecular Reactions 470
2 Tuning Reactivity to Speed up Reaction Times 471
References 473
97 Ultrafast Dynamics of a Bistable Intramolecular Proton Transfer Switch 474
Abstract 474
1 Introduction 474
2 Results 475
3 Discussion 475
References 477
98 Excited State Structural Dynamics Probed with Time-Resolved Sulfur K-Edge X-Ray Absorption Spectroscopy 478
Abstract 478
1 Introduction 478
2 Transient Sulfur K-Edge Spectroscopy 479
3 Summary 481
References 481
99 Solvent Environment Revealed by Positively Chirped Pulses 482
Abstract 482
1 Introduction 482
2 Experimental 483
3 Results and Discussion 483
References 485
100 Coherent Wavepacket Motion in Ultrafast Intermolecular Electron Transfer in Electron-Donating Solvent 486
Abstract 486
1 Introduction 486
2 Results and Discussion 487
3 Conclusion 489
101 Elementary Electron and Ion Dynamics in Ionized Liquid Water 490
Abstract 490
1 Introduction 490
2 Experimental Methods 491
3 Results and Discussion 491
Acknowledgments 492
References 493
102 Signatures of Conical Intersection Mediated Relaxation Dynamics in Time-Resolved Broadband Raman Detection 494
Abstract 494
1 Ultrafast Relaxation Dynamics of RNA and DNA Bases 494
2 Off-Resonant Raman Detection Schemes 495
3 Time-Resolved Raman Signatures of Conical Intersection Mediated Relaxation of Uracil 495
Acknowledgments 497
References 498
103 VIPER 2D-IR: Novel Pulse Sequence to Track Exchange Beyond the Vibrational Lifetime 499
Abstract 499
1 Mixed IR/Vis 2D Spectroscopies 499
2 Viper 2D-IR 500
References 502
104 Sagnac Interferometer for Two-Dimensional Spectroscopy in the Pump-Probe Geometry 503
Abstract 503
Acknowledgments 506
References 506
105 Broadband Electronic Two-Dimensional Spectroscopy in the Deep UV 507
Abstract 507
1 Introduction 507
2 Experimental Setup 508
3 Results and Discussion 509
References 510
106 A Non time Ordered Pulse Scanning Protocol for Multidimensional Spectroscopy with Entangled Light 511
Abstract 511
1 Introduction: Spectroscopy with Entangled Light 511
2 LOP---A New Non time Ordered Delay Scanning Protocol 512
3 Probing Intraband Dephasing Rates of Excitons in Aggregates 513
Acknowledgements 514
References 514
107 Ultrafast Interaction of Dark and Bright Electronic States in Open-Chain Carotenoids Investigated by Pump-DFWM 515
Abstract 515
1 Introduction 515
2 Experimental 516
3 Results and Discussion 516
References 518
108 Following the Excited State Dynamics of beta -Apo-82032-Carotenal with Two-Dimensional Electronic-Vibrational Spectroscopy 519
Abstract 519
1 Introduction 519
2 Experimental 520
3 Results and Discussion 521
4 Conclusions 521
Acknowledgments 522
References 522
109 Survival of Nuclear Coherences for a Series of Internal Conversions in Free Base Tetraphenylporphyrin 523
Abstract 523
1 Introduction 523
2 Results and Discussion 524
References 526
110 Distinctive Spectral Features of Exciton and Excimer States in the Ultrafast Electronic Deactivation of the Adenine Dinucleotide 527
Abstract 527
1 Introduction 527
2 Experimental Results 528
3 Discussion and Conclusions 529
Acknowledgments 529
References 529
111 Influence of Intramolecular Hydrogen Bonding on the Photodynamics of 2-(1-Ethynylpyrene)-Adenosine (PyA) 530
Abstract 530
1 Introduction 530
2 Materials and Methods 531
3 Results 531
4 Discussion 532
References 532
112 S2 to S1 Relaxation Dynamics in Perylene Bisimide Dye Aggregates and Monomers 534
Abstract 534
1 Introduction 534
2 Experimental Approach 535
3 Analysis of the Dynamics 535
References 536
113 2D IR Spectroscopy with Phase-Locked Pulse Pairs from a Birefringent Delay Line 537
Abstract 537
Acknowledgments 540
References 540
114 Hydrogen Bond Dynamics in Alcohols Studied by 2D IR Spectroscopy 541
Abstract 541
1 Introduction 541
2 Experiment 542
3 Theory 542
4 Results and Discussion 542
References 545
115 Hydrogen Bond Enhancement of Fermi Resonances Explored with Ultrafast IR Two-Colour Pump-Probe and 2D-IR Spectroscopy 546
Abstract 546
References 548
116 Observation of the Dark State in Ruthenium Complexes Using Femtosecond Infrared Vibrational Spectroscopy 550
Abstract 550
1 Introduction 550
2 Experimental 551
3 Results and Discussion 552
References 553
117 Vibrational Dynamics of Nitrosyl Stretch of Ru Complex in Aqueous Solution Studied by Two-Dimensional Infrared Spectroscopy 554
Abstract 554
1 Introduction 554
2 Results and Discussion 555
References 557
118 Ultrafast IR Spectroscopy of O-H Stretching Modes in 2-Naphthol-Acetonitrile Photoacid-Base Complexes 558
Abstract 558
References 561
119 Vibrational Dynamics of the CN Stretching in the Electronically Excited State by UV and Visible-Pump and Infrared-Probe Spectroscopy 562
Abstract 562
1 Introduction 562
2 Results and Discussion 563
3 Conclusion 565
Part IVInterfacial, Surface, Thin Filmsand Carbon Nanotubes 376
References 565
120 Structural Motifs of Liquid Acetic Acid from Ultrafast CARS Spectroscopy 567
Abstract 567
1 Introduction 567
2 CO Vibration of Acetic Acid 568
References 569
121 Ultrafast Time-Domain Raman Study to Visualize Large-Amplitude Distortions in Copper Complexes 570
Abstract 570
1 Introduction 570
2 Experimental 571
3 Results and Discussion 572
References 573
122 Investigation of Vibrational Dynamics by Femtosecond Time-Resolved CARS 574
Abstract 574
Acknowledgments 577
References 577
123 Two-Dimensional Fourier Transform Infrared-Visible and Infrared-Raman Spectroscopies 578
Abstract 578
Acknowledgments 580
References 580
Part VI Biological Systems 581
124 Ultrafast Intersystem Crossing in SO2 and Nucleobases 582
Abstract 582
1 Introduction 582
2 Methodology 583
3 Results 583
3.1 Dynamics of SO2 584
3.2 Dynamics of DNA Nucleobases 584
4 Conclusion 585
References 586
125 Detection of the G(--H)2022 Radical in the Electronic Deactivation of the G--C Watson-Crick Base Pair 587
Abstract 587
1 Introduction 587
2 Experimental Details 588
3 Results and Discussion 588
Acknowledgments 589
References 589
126 Ultrafast Photoisomerization of Chiral Biomimetic Molecular Switches 590
Abstract 590
1 Introduction 590
2 Results 591
3 Discussion 592
References 593
127 Snapshots of Sub-picosecond Dynamics in Heme-proteins Captured by Femtosecond Stimulated Raman Scattering 594
Abstract 594
1 Background and Significance 594
2 Methods 595
3 Results 596
References 596
128 Vibrational Dynamics in Photoactive Yellow Protein Revealed by Mid-IR Pump/Visible Probe Spectroscopy 597
Abstract 597
1 Introduction 597
2 Experimental 598
3 Results and Discussion 598
4 Conclusion 599
References 600
129 Probing Ultrafast Structural Dynamics of Photoactive Yellow Protein with Femtosecond Time-Domain Raman Spectroscopy 601
Abstract 601
1 Introduction 601
2 Experimental 602
3 Results and Discussion 602
References 604
130 Vibrational Energy Flow in Hemeproteins 605
Abstract 605
1 Introduction 605
2 Vibrational Energy Flow in Cytochrome c [4] 606
3 Vibrational Energy Flow in Myoglobin 606
4 Advantages of the Present Technique for Studies on Intermolecular Vibrational Energy Transfer in Condensed Phases 607
Acknowledgements 607
References 607
131 Towards Direct Measurement of Ultrafast Vibrational Energy Flow in Proteins 608
Abstract 608
References 611
132 Time-Resolved Impulsive Raman Study of Excited State Structures of Green Fluorescent Protein 612
Abstract 612
1 Introduction 612
2 Experimental Method 613
3 Results and Discussion 613
References 615
133 Nonlinear Fourier-Transform Spectroscopy Using Ultrabroadband Femtosecond Pulses for the Measurement of Photobleaching of Fluorescent Proteins 616
Abstract 616
1 Introduction 616
2 Nonlinear Fourier-Transform Spectroscopy 617
3 Experimental 617
4 Conclusions 619
Acknowledgements 619
References 619
134 Femtosecond Vibrational Spectroscopic Study on Photoexcitation Dynamics of DNO-Bound Myoglobin 620
Abstract 620
1 Introduction 620
2 Experimental Methods 621
3 Results and Discussion 621
References 623
Part VII Charge and EnergyTransfer—Photovoltaicand Light Harvesting 624
135 Interpreting Oscillations in Numerically Exact Simulations of 2D Electronic Spectra 625
Abstract 625
1 Introduction 625
2 Model 626
3 Results and Discussion 627
4 Conclusions 627
Acknowledgments 628
References 628
136 Coherent Ultrafast Charge Transfer in an Organic Photovoltaic Blend 629
Abstract 629
1 Introduction 630
2 Results 630
3 Conclusions 632
References 632
137 Ultrafast Energy and Charge Transfer Processes in a Flexible Molecular Triad Designed for Organic Photovoltaics 633
Abstract 633
1 Introduction 633
2 Results 634
3 Conclusions 635
References 635
138 Ultrafast Electron and Hole Dynamics in Novel Conjugated Star-Shaped Molecules 636
Abstract 636
1 Introduction 636
2 Experimental and Results 637
References 639
139 Photoinduced Charge Transfer Occurs Naturally in DNA 640
Abstract 640
1 Introduction 640
2 Results and Discussion 641
3 Conclusion 643
References 643
140 A Regulation of Energy Flow in Purple Bacterial Photosynthetic Antennas 644
Abstract 644
1 Introduction 644
2 Experimental 645
3 Results and Discussion 646
References 647
141 Elucidation and Control of Ultrafast Intramolecular Charge Transfer Dynamics of Marine Photosynthetic Pigments 648
Abstract 648
1 Introduction 648
2 Experimental 649
3 Results and Discussion 650
References 651
142 The Primary Photosynthetic Energy Conversion in Bacterial Reaction Centers---Stepwise Electron Transfer and the Effect of Elevated Exposure Levels 652
Abstract 652
1 The Primary Reactions of Photosynthetic Reaction Centers 652
2 Techniques 653
3 Results 653
References 654
143 Resonant Stimulated X-Ray Raman Spectroscopy of Molecule Following Core Ionization 656
Abstract 656
1 Introduction 656
2 Results and Discussion 657
Acknowledgments 658
References 658
144 Light Harvesting Dynamics in Gloeobacter Rhodopsin (GR) 659
Abstract 659
1 Introduction 659
2 Experimental Methods 660
3 Results and Discussion 660
4 Conclusion 661
References 662
145 Disentangling Electronic and Vibrational Coherence in the Phycocyanin-645 Light-Harvesting Complex 663
Abstract 663
1 Introduction 663
2 Results and Discussion 664
3 Conclusions 665
References 665
146 Ultrafast Energy Flow and Equilibration Dynamics in Photosynthetic Light-Harvesting Complexes 667
Abstract 667
References 670
147 Primary Process in Light-Harvesting Complex Studied by Pump-Repump-Probe Spectroscopy 671
Abstract 671
1 Introduction 671
2 Experimental 672
3 Results and Discussion 672
4 Conclusion 674
References 674
148 Ultrabroadband Two-Dimensional Spectroscopy by a Birefringent Delay Line 675
Abstract 675
Acknowledgments 677
References 678
Part VIII THz Generation and Application 679
149 Filling the Entire Terahertz Frequency Gap by Single-Cycle MV/Cm Pulses 680
Abstract 680
1 Introduction 680
2 Experimental Results 680
References 682
150 Terahertz Imaging with Optical Resolution by Femtosecond Laser Filament in Air 683
Abstract 683
1 Introduction 683
2 Experimental Results 683
2.1 THz Sub-wavelength Imaging by Femtosecond Laser Filament 683
2.2 Resolution of THz Imaging (Diameter of THz Beam Emission from Femtosecond Laser Filament) 685
3 Numerical Simulation 685
References 686
151 Ultrafast Optical Modulation of Efficiently-Generated Terahertz-Wave in Charge Ordered Organic Ferroelectrics 687
Abstract 687
1 Introduction 687
2 Experiments 688
3 Results and Discussions 688
References 690
152 Ultrafast Terahertz Response of Lithium Niobate in the Nonperturbative Regime 691
Abstract 691
1 Introduction 691
2 Experiment and Results 692
3 Discussion 693
References 693
153 Inherent Resistivity of Graphene to Strong THz Fields 694
Abstract 694
1 Introduction 694
2 Measurement 695
3 Results and Discussion 695
4 Conclusion 696
References 696
154 Nonlinear Carrier Responses in Gold Thin Films Induced by Intense Terahertz Waves 697
Abstract 697
1 Introduction 697
2 Experiments 698
3 Results and Discussion 698
4 Conclusions 700
References 700
155 THz-Controlled Photoelectron Emission from Nanotips 701
Abstract 701
1 Introduction 701
2 Experimental Methods 702
3 Results and Discussion 702
References 703
156 Nonlinear Carrier Dynamics in Semi-metal Bismuth Induced by Intense Terahertz Field 704
Abstract 704
1 Introduction 704
2 Experiment 705
3 Result and Discussion 706
4 Conclusion 706
References 707
157 Ultrafast Insulator-Metal Transition in VO2 Driven by Intense Multi-THz Pulses 708
Abstract 708
References 711
158 Coherent Ultrafast Magnetization Dynamics Non-resonantly Induced in Cobalt by an Intense Terahertz Transient 712
Abstract 712
1 Introduction 712
2 Experimental Results 713
References 715
159 Beating of Terahertz Pulse Induced Spin Precession in ErFeO3 716
Abstract 716
1 Introduction 716
2 Result 717
3 Conclusion 719
References 719
160 Resonant Antiferromagnetic Spin Wave Excitation by Terahertz Magnetic Near-Field with Split Ring Resonator 720
Abstract 720
1 Introduction 720
2 Experimental Setup 721
3 Results 722
4 Summary 723
References 723
161 Ultrafast Spin Dynamics in an Antiferromagnet NiO Observed in Pump-Probe and Terahertz Experiments 724
Abstract 724
1 Introduction 724
2 Sample 725
3 Experiment 725
4 Result and Discussion 725
References 726
Part IX Photoemitted Electron, Plasmonand Nanoplasmas 728
162 Controlling the Motion of Strong-Field, Few-Cycle Photoemitted Electrons in the Near-Field of a Sharp Metal Tip 729
Abstract 729
1 Introduction 729
2 Experimental Setup 730
3 Results 731
4 Conclusion 731
References 732
163 Velocity Map Imaging of Electrons Strong-Field Photoemitted from Si-Nanotip Arrays 733
Abstract 733
Acknowledgments 736
References 736
164 Visualization of Photocurrents in Nanoobjects by Ultrafast Low-Energy Electron Point-Projection Imaging 737
Abstract 737
1 Introduction 737
2 Method 738
3 Results and Discussion 739
4 Conclusions 740
References 740
165 Visualization of Charge Carrier Motion in Semiconductor Nanowires with Ultrafast Pump-Probe Microscopy 741
Abstract 741
1 Introduction 741
2 Pump-Probe Microscopy 741
Acknowledgments 743
References 744
166 Ultrafast Optical Control of Charge Dynamics in Organic and Hybrid Electronic Nanodevices 745
Abstract 745
References 748
167 Ultrafast Non-thermal Response of Plasmonic Resonance in Gold Nanoantennas 749
Abstract 749
References 752
168 Control of Femtosecond Surface Plasmon Coupled onto a Gold Tapered Tip and Its Nonlinear Emission 753
Abstract 753
1 Introduction 753
2 Experimental Setup 754
3 Results and Discussion 755
References 756
169 Ultrafast Optical-Field Controlled Photoemission from Plasmonic Nanoparticle Arrays 757
Abstract 757
References 759
170 Real Space and Real Time Observation of Plasmon Wavepacket Dynamics in Single Gold Nanorod 761
Abstract 761
1 Introduction 761
2 Experiment 762
3 Results and Discussion 762
References 763
171 Vector Pulse Shaped Ultrafast Plasmon Based on Response Functions Measured for Orthogonally Polarized Excitation 764
Abstract 764
1 Introduction 764
2 Experimental Setup 765
3 Results and Discussion 765
References 767
172 Few-Cycle Laser Pulse Induced Plasmon Assisted Thermionic Injection in Metal-Insulator-Metal Junctions 768
Abstract 768
1 Introduction 768
2 Experimental Setup 769
3 Results and Discussion 769
References 771
173 Single Nanoparticles and Nanoplasmas in Femtosecond Laser Fields 772
Abstract 772
1 Introduction and Summary 772
2 Experiment 773
3 Shock Waves in Nanoplasmas 773
4 Mapping Nanoscale Light Absorption with Plasma Explosion Imaging 775
5 Conclusion 776
References 776
Part X Novel Pulsed Sourcesand Application 777
174 Passively CEP-Stable Front End for Frequency Synthesis 778
References 781
175 Tunable Few-Cycle Mid-IR Pulses Towards Single-Cycle Duration by Adiabatic Frequency Conversion 782
Abstract 782
References 785
176 Carrier-Envelope Phase of Single-Cycle Pulses Generated Through Two-Color Laser Filamentation 786
Abstract 786
References 788
177 Phase-Locked Multi-THz High-Harmonic Generation by Dynamical Bloch Oscillations in Bulk Semiconductors 790
Abstract 790
References 793
178 Direct Generation of 7 fs Whitelight Pulses from Bulk Sapphire 794
Abstract 794
1 New Insights into Bulk Filamentation 794
2 Propagation Properties of New Frequencies and Generation of Sub-10-fs Pulses During SCG 795
3 Conclusion and Outlook 797
References 797
179 Ultrafast 2 00B5m Laser Oscillators Based on Thulium-Doped ZBLAN Fibers 798
Abstract 798
References 800
180 Characterizing Phase Fluctuations of Fiber Oscillators by Using External Optical Cavities 801
Abstract 801
1 Introduction 801
2 Experimental Setup and Results 802
3 Conclusion 803
References 804
181 Two Novel Schemes for Photon-Number Squeezed Pulse Generation in Ultrafast Nonlinear Fiber Optics 805
Abstract 805
1 Introduction 805
2 Photon Number Squeezing by Noise Reduced 1.5 mu m EDFA with the CBD Technique 806
3 Photon Number Squeezing by 800 nm Pulses with Spectral Narrowing 807
4 Conclusion 807
References 808
182 Towards a Compact Fiber Laser for Multimodal Imaging 809
Abstract 809
1 Introduction 809
2 Experimental 810
3 Results and Discussion 810
References 812
183 Measurement and Characterization of Sub-5 fs Broadband UV Pulses in the 230--350 nm Range 813
Abstract 813
1 Introduction 813
2 Experimental Layout 814
3 Results and Discussion 815
References 816
184 Generation and Characterization of Tunable 00B5J-Level, Sub-10 fs UV Pulses 818
Abstract 818
References 821
185 Femtosecond Pulses in 375--405 nm Region by Chirped Sum Frequency 822
Abstract 822
1 Introduction 822
2 Experimental 823
3 Results and Discussion 823
4 Conclusions 825
References 825
186 Pushing the NOPA to New Frontiers: Output to Below 400 nm, MHz Operation and ps Pump Duration 826
Abstract 826
1 Optical Parametric Amplifiers Pumped by Yb-Based Lasers 826
2 Fully Utilizing the Tuning Possibility of a 343 nm Pumped NOPA 827
3 Continuum-Seeded NOPA with 1 ps 130 W Pump Pulses 828
4 Towards New Applications of Wavelength-Tunable MHz 10 fs Pulses 829
References 829
187 2 MHz Tunable Non Collinear Optical Parametric Amplifiers with Pulse Durations Down to 6 fs 830
Abstract 830
1 Introduction 830
2 Results 831
3 Conclusions 833
References 833
188 Fiber-Slab-Pumped OPCPA for XUV-Based Time-Resolved Photoelectron Spectroscopy at 500 kHz Repetition Rate 835
Abstract 835
1 Introduction 835
2 Fiber Oscillator and Hybrid Fiber-Slab Amplifier 836
3 OPCPA Results and Discussion 837
References 838
189 Sub-100 fs Mid-Infrared Pulses as Driver for a Table-Top Hard X-Ray Source 839
Abstract 839
1 Introduction 839
2 Results 840
References 842
190 Generation of Stationary On-Axis Optical Filaments by Means of Dammann Lenses 843
Abstract 843
1 Introduction 843
2 Experimental Set-up 844
3 Experimental Results 845
4 Conclusions Results 846
References 846
191 Wavefront Analysis of High-Efficiency, Large-Scale, Thin Transmission Gratings 848
Abstract 848
1 Introduction 848
2 Design and Analysis of Transmission Gratings 849
3 Spatial Distortion and Wavefront Analysis 849
4 Ray Tracing and Summary 851
References 851
Part XI Pulse Shaping and Manipulations 852
192 High-Energy Sub-Optical-Cycle Parametric Waveform Synthesizer 853
Abstract 853
References 856
193 Above-Millijoule Optical Waveforms Compressible to Sub-fs Using Induced-Phase Modulation in a Neon-Filled Hollow-Core Fiber 857
Abstract 857
References 860
194 Isolating Quantum Coherence Using Coherent Multi-dimensional Spectroscopy with Spectrally Shaped Pulses 861
Abstract 861
1 Introduction 861
2 Experimental and Results 862
3 Conclusions 863
References 864
195 Spatiotemporal Dynamics of Femtosecond Pulses Shaped by Diffractive Optical Elements 865
Abstract 865
References 867
196 Spectral Shaping and Continuous Tuning of Multi-color Carrier-Envelope Phase Locked Pulse 869
Abstract 869
1 Introduction 869
2 Experimental 870
3 Results and Discussion 870
4 Summary 871
Acknowledgments 872
References 872
197 Tailoring of High-Field Multi-THz Waveforms with Sub-cycle Precision 873
Abstract 873
References 875
198 Over 1-mJ Intense Ultrashort Optical-Vortex Pulse Generation with Programmable Topological-Charge Control by Chirped-Pulse Amplification 877
Abstract 877
1 Introduction 877
2 Experiments and Results 878
References 880
199 The Influence of Generalized Focusing on Polarization-Shaped Few-Cycle Pulsed Beams 881
Abstract 881
1 Introduction 881
2 Focusing-Induced Polarization-State Changes 882
3 An Example: The Polarization Gating Pulse 882
4 Conclusions 883
Acknowledgement 883
References 883
200 Simultaneous Selective Two-Photon Microscopy Using MHz Rate Pulse Shaping and Quadrature Detection of the Time-Multiplexed Signal 885
Abstract 885
1 Introduction 885
2 Experimental 886
3 Results and Discussion 887
References 888
201 Simultaneous Spatial and Temporal Focusing of Femtosecond Laser Pulses for Directly Writing Optical Waveguides in Pr3+ Doped ZBLAN Glass 889
Abstract 889
1 Introduction 889
2 Experiments and Results 890
3 Conclusion 891
Acknowledgments 891
References 892