Polariton Chemistry
John Wiley & Sons Inc (Verlag)
9781119783299 (ISBN)
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Polaritons are hybrid excitations formed when confined electromagnetic modes form strong couplings with dipole active transitions in a dielectric medium. They have long been a fixture of research in inorganic semiconductor optics but have recently also been taken up as an object of study in molecular science, where their prospective applications are many. The tunability of their molecular properties and processes have given rise to an interdisciplinary field of polariton chemistry, with important potential ramifications for a huge range of fields.
Polariton Chemistry provides a pedagogical overview of this research subject, in which optical cavities are used to control the physiochemical properties and dynamics of molecular systems. The book emphasizes the interdisciplinary nature of this burgeoning field and the need for a shared language and set of fundamentals across many research disciplines. With no existing rival in the current literature, it’s a must-own for researchers in almost any of the physical sciences.
Polariton Chemistry readers will also find:
Analysis of prospective applications including long-range excitation energy transfer, enhanced charge conductivity, and more
Detailed discussion of topics including single molecule strong light-matter coupling, ultrastrong light-matter coupling, and many more
Coverage of key theoretical and experimental techniques
Polariton Chemistry is ideal for any scientist in the fields of physical chemistry, materials science, photonics, quantum optics, and engineering.
Joel Yuen-Zhou, PhD is Associate Professor in the Department of Chemistry and Biochemistry at the University of California, San Diego. His research focuses on the theoretical description of novel interactions between light and molecular matter in the weak, strong, and ultrastrong coupling regimes. His pioneering work on polariton chemistry has been recognized with several awards including a Sloan Fellowship as well as the NSF CAREER, DOE Early Career and Camille-Dreyfus Teacher Scholar awards. Noel C. Giebink, PhD, is a Professor in the Department of Electrical Engineering and Computer Science at the University of Michigan. His research focuses on light-matter interaction and the physics of organic semiconductor materials and devices. He is a senior member of IEEE, Optica, and SPIE, and has been recognized with the DARPA YFA, AFOSR YIP, and NSF CAREER awards. Raphael F. Ribeiro, PhD is Assistant Professor in the Department of Chemistry at Emory University, Atlanta since 2020. His research is focused on theoretical models and simulation of equilibrium and non-equilibrium chemical dynamics in mesoscopic materials. His work has been recognized with awards that include NSF CAREER award and a Young Investigator Award by the Physical Chemistry Division of the American Chemical Society.
Preface xi
Acknowledgments xvii
Part I Basic Concepts 1
1 Ultrafast Dynamics Under Electronic Strong Light–Matter Coupling 3
Courtney DelPo and Gregory Scholes
1.1 Introduction: Energy Levels – Central to Science 3
1.2 Electronic Strong Coupling in Transient Absorption and Reflection Spectroscopy 7
1.2.1 Description of Transient Absorption and Reflection Spectroscopy 7
1.2.2 Polariton Signatures in Transient Absorption and Reflection Spectroscopy 7
1.3 Electronic Strong Coupling in Broadband and Two-dimensional Electronic Spectroscopy 10
1.4 Electronic Strong Coupling in Applications 11
1.5 Future Outlook of Ultrafast Dynamics in Electronic Strong Coupling 13
References 13
2 Molecular Strong Coupling: The Quantum to Classical Transition 17
William L. Barnes
2.1 Introduction 17
2.2 Interaction Strength and the Bulk Material Response 19
2.3 Comparing Quantum and Classical 24
Acknowledgments 25
References 26
3 The Role of Cavity in Polaritonics: Plasmonic Nanoparticles, Self-hybridized Polaritons, and Casimir Self-assembly 29
Oleg V. Kotov and Timur O. Shegai
3.1 Plasmonic Resonators 30
3.1.1 Light–Matter Interactions Using Plasmonic Resonators and Their Arrays 30
3.1.2 Single Plasmonic Resonators 33
3.1.3 The Single-emitter Limit 34
3.1.4 Plexcitonic Photophysics and Photochemistry 37
3.2 Self-hybridized Polaritons 41
3.3 Casimir Microcavities 44
3.4 Conclusions and Outlook 46
References 47
4 Plexciton Photophysics 61
Daniel Finkelstein-Shapiro
4.1 Goal of this Chapter 61
4.2 What is a Plexciton and How Is It Different from a Cavity Polariton 61
4.3 Synthesis of Plexcitons and Their Structure: Influence and Consequence on the Photophysics 64
4.3.1 Colloidal Systems-based on Organic Molecules 64
4.3.2 Open Cavities 65
4.3.3 Surface Nanocavities 65
4.4 Photophysics of Plexcitons 65
4.4.1 Emitters 66
4.4.2 Metallic Nanoparticle 67
4.4.3 Plexcitons 69
4.5 Spectral Signatures 73
4.5.1 Suggestions for Approaching Transient Absorption Spectra of Plexcitons 75
4.6 Applications 75
4.6.1 Photostability 75
4.6.2 Hot Electron Hole Generation 75
4.6.3 Chiral Cavities and Phase Transitions 76
4.7 Conclusion 76
Acknowledgments 76
References 76
5 Coupling of Nanocavities to Molecules 83
Rohit Chikkaraddy and Jeremy Baumberg
5.1 Light and Molecules 83
5.2 Optical Cavities 85
5.3 Free-electron Model 87
5.4 Introduction to Plasmons 88
5.4.1 Propagating Surface Plasmon Polaritons 90
5.4.2 Localized Surface Plasmon Polaritons 90
5.5 Cavity Description for Plasmon Modes 91
5.5.1 Qualify Factor 92
5.5.2 Mode Volume 92
5.6 Nanocavities 93
5.6.1 Nanoparticle on Mirror 93
5.6.2 Sensing Molecules in the Gap 96
5.6.3 Effect of Nanoparticle Size and Shape 96
5.7 Light–Matter Coupling 97
5.7.1 Weak-coupling Regime and Purcell Effect 99
5.7.2 Strong Coupling 103
5.7.3 Single-molecule Strong Coupling 107
5.8 Conclusion 109
References 109
Part II Spectroscopy and Dynamics 115
6 Nonlinear Spectroscopy Under Vibrational Strong Coupling 117
Adam D. Dunkelberger, Cynthia G. Pyles and Jeffrey C. Owrutsky
6.1 Introduction 117
6.2 Experimental Considerations 120
6.3 Understanding the Nonlinear Response of MVP 121
6.4 Early Delays 121
6.5 Later Delays 122
6.6 Intermediate Delays 127
6.7 Optical and Photophysical Opportunities 128
6.8 Concluding Remarks 130
Acknowledgments 131
References 131
7 Quantum Dynamics, Optical Signals, and Spectroscopy of Molecular Polaritons 139
Zhedong Zhang
7.1 Introduction 139
7.2 Quantum Electrodynamics of Molecular Polaritons 140
7.3 Pump-probe Spectra for Molecular Polaritons 143
7.4 Multidimensional Infrared Spectroscopy for Vibrational Polaritons: Density-matrix Theory 144
7.4.1 Gateway-window Formalism 144
7.4.2 Cooperativity Versus Localization 147
7.4.3 Stochastic Model for Vibrational Polaritons 148
7.4.4 Simulations of 2DIR Spectra for VPs 150
7.5 Multidimensional Electronic Spectroscopy for Exciton Polaritons: Heisenberg–Langevin Theory 154
7.5.1 Langevin Model for Exciton Polaritons 154
7.5.2 Correlation Functions of Vibrations 157
7.5.3 Absorption Spectrum 158
7.5.4 Time-resolved Emission of Polaritons 159
7.5.5 Two-dimensional Polariton Spectroscopy 159
7.5.6 Connection to Polariton Pump-probe Spectra 162
Acknowledgments 163
References 164
8 Molecular Dynamics Simulations of Exciton–Polaritons in Organic Microcavities 167
Gerrit Groenhof, Ruth H. Tichauer and Ilia Sokolovskii
8.1 Introduction 167
8.2 Molecular Dynamics in the Collective Strong Coupling Regime 168
8.2.1 Born–Oppenheimer Approximation in the Electronic Strong Coupling Regime 169
8.2.2 Quantum Mechanics/Molecular Mechanics 169
8.2.3 Multiscale Tavis–Cummings Hamiltonian 170
8.2.4 Multimode Fabry–Pérot Cavities 172
8.2.5 Semiclassical Molecular Dynamics 174
8.3 Applications 177
8.3.1 Polariton Relaxation 177
8.3.2 Polariton Transport 179
8.3.3 Polaritonic Photochemistry 182
8.4 Summary and Outlook 185
References 185
9 Disorder in Cavity-modified Transport and Chemistry 193
David Hagenmüller, Jérôme Dubail, Francesco Mattiotti, Guido Pupillo and Johannes Schachenmayer
9.1 Introduction 193
9.2 Semilocalization 194
9.2.1 The Disordered TC Model with Hopping 195
9.2.2 Arrowhead Matrix Model and Dark State Multifractality 199
9.3 The Influence of Disorder and Semilocalization on Vibrational Dynamics 203
9.3.1 The Holstein–Tavis–Cummings Model 203
9.3.2 Vibrational Entanglement and Numerical Simulations 205
9.3.3 Dynamics After Photo-excitation 207
9.4 Conclusion and Outlook 211
References 213
Part III Applications 219
10 Engineering Organic Exciton–Polariton Condensates in Microcavities 221
Sitakanta Satapathy and Vinod M. Menon
10.1 Introduction 221
10.2 Mechanism of Polariton Condensation in Organic Microcavities 223
10.2.1 Radiative Pumping 224
10.2.2 Vibron-assisted Relaxation 225
10.3 Experimental Signatures of Polariton Condensation in Organic Microcavities 225
10.4 The Molecular Medley for Polariton Condensation 227
10.4.1 Single Crystalline Systems 227
10.4.2 Low Molecular Weight Emitters 230
10.4.3 Polymers 235
10.4.4 Host–Guest Systems 238
10.5 Summary 242
References 243
11 Kinetic Models for Polariton Relaxation in Organic Microcavities and Comparison to Experiments 247
Tomohiro Ishii, Stéphane Kéna-Cohen, Felipe Herrera and Chihaya Adachi
11.1 Introduction 247
11.2 Modeling Polariton Kinetics in the Linear and Nonlinear Regime 249
11.2.1 Polariton Kinetics in the Linear Regime 249
11.2.2 Polariton Kinetics in the Nonlinear Regime 254
11.3 Polariton Relaxation Mechanisms 257
11.3.1 Radiative Pumping Process (1): Initial Experiments 257
11.3.2 Radiative Relaxation 260
11.3.3 Nonradiative Relaxation 262
11.4 Comparison Between the Experimentally and Theoretically Estimated W ep in BSBCz-EH System 264
11.5 Conclusion 265
References 265
12 Reactions and Assembly Under Vibrational Strong Coupling 271
Kenji Hirai and Hirohi Uji-i
12.1 Introduction 271
12.2 Vibrational Strong Coupling 272
12.3 Chemical Reactions Under VSC 275
12.3.1 Organic Reactions 276
12.3.2 Enzymatic Reactions Under VSC 280
12.3.3 Symmetry of Molecular Vibrations 281
12.3.4 Interpretation of Vibrational Strong Coupling 281
12.3.5 Self-assembly and Crystallization Under VSC 282
12.4 Summary 283
References 283
13 Controlling and Probing Molecular Polaritons 289
Michael A. Michon and Blake S. Simpkins
13.1 Introduction 289
13.2 Analytical Description of Cavities 289
13.2.1 Treatment of Lossless Mirrors Bounding an Absorbing Medium 289
13.2.2 Semiclassical Coupled Oscillators 293
13.3 Nonidealities: That We Must, Nevertheless, Deal with 294
13.3.1 Details for Dealing with Cavities 294
13.3.2 Spatially Dependent Response 296
13.3.3 Line Broadening 298
13.4 Current Challenges and Proposed Best Practices 299
13.4.1 Current Challenges 300
13.4.2 Measuring Reaction Rates in Optical Cavities 301
13.4.3 Validating Angle-independent Rate Extraction 303
13.4.4 Proposed Cavity System Design 307
13.5 Conclusion 311
References 311
Part IV Frontiers 315
14 A Comparison of Coulomb and Multipolar Gauge Theories of Cavity Quantum Electrodynamics 317
Adam Stokes and Ahsan Nazir
14.1 Introduction 317
14.2 Perfect Cavity 318
14.2.1 Empty Fabry–Pérot Cavity 318
14.2.2 Perfect Cavity Containing Matter 319
14.3 Gauge Relativity 324
14.3.1 Relativity and Invariance 324
14.3.2 Gauge Nonrelativistic Predictions 325
14.3.3 A Case Study in Gauge Relativity and Gauge Ambiguities: Dipolar Photon Emission and Detection 329
14.4 Imperfect Cavities 347
14.4.1 Phenomenological Descriptions 347
14.4.2 Subsystem Gauge Relativity in Macroscopic QED 352
14.5 Conclusions 356
References 357
Appendix A: Computation of K and G, and the Field Canonical Commutation Relation in the Case of a Perfect Parallel Plate Cavity 362
Appendix B: Born–Markov-secular Master Equation for the Dipole in a Fabry–Pérot Cavity 364
Appendix C: Emission Rates of a Dipole Near a Single Plate 367
Appendix D: Proof that the Sum of Imperfect Cavity Lorenztians Gives a Dirac Comb in the Perfect Cavity Limit 368
15 The Vacuum in Ultrastrong Coupling Cavity Quantum Electrodynamics 369
Peter Rabl
15.1 Introduction 369
15.2 The Dicke Model 370
15.2.1 Collective Light–Matter Interactions 370
15.2.2 Superradiant Instability 371
15.3 Effective Models in Cavity QED 372
15.3.1 Cavity QED in the Coulomb Gauge 372
15.3.2 Cavity QED in the Dipole Gauge 374
15.4 The Ground States in Cavity QED 377
15.4.1 Boundary-induced Ferroelectricity 377
15.4.2 Collective Ultrastrong Coupling Regime 378
15.4.3 Nonperturbative Coupling Regime 379
15.4.4 Ground-state Phases in Cavity QED 381
15.5 Conclusions 382
References 382
Afterword 385
Index 387
| Erscheint lt. Verlag | 10.2.2026 |
|---|---|
| Verlagsort | New York |
| Sprache | englisch |
| Themenwelt | Naturwissenschaften ► Chemie |
| Naturwissenschaften ► Physik / Astronomie ► Optik | |
| ISBN-13 | 9781119783299 / 9781119783299 |
| Zustand | Neuware |
| Informationen gemäß Produktsicherheitsverordnung (GPSR) | |
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