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Understand the emerging field of polariton chemistry with this accessible introduction 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…mehr
Understand the emerging field of polariton chemistry with this accessible introduction
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.
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Autorenporträt
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.
Inhaltsangabe
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 1.3 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 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 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 3.2 Self-hybridized Polaritons 41 3.3 Casimir Microcavities 44 3.4 Conclusions and Outlook 46 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 4.4 Photophysics of Plexcitons 65 4.5 Spectral Signatures 73 4.6 Applications 75 4.7 Conclusion 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 5.5 Cavity Description for Plasmon Modes 91 5.6 Nanocavities 93 5.7 Light-Matter Coupling 97 5.8 Conclusion 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 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 7.5 Multidimensional Electronic Spectroscopy for Exciton Polaritons: Heisenberg-Langevin Theory 154 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 8.3 Applications 177 8.4 Summary and Outlook 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 9.3 The Influence of Disorder and Semilocalization on Vibrational Dynamics 203 9.4 Conclusion and Outlook 211 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 10.3 Experimental Signatures of Polariton Condensation in Organic Microcavities 225 10.4 The Molecular Medley for Polariton Condensation 227 10.5 Summary 242 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 11.3 Polariton Relaxation Mechanisms 257 11.4 Comparison Between the Experimentally and Theoretically Estimated Wep in BSBCz-EH System 264 11.5 Conclusion 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 12.4 Summary 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 13.3 Nonidealities: That We Must, Nevertheless, Deal with 294 13.4 Current Challenges and Proposed Best Practices 299 13.5 Conclusion 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 14.3 Gauge Relativity 324 14.4 Imperfect Cavities 347 14.5 Conclusions 356 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 15.3 Effective Models in Cavity QED 372 15.4 The Ground States in Cavity QED 377 15.5 Conclusions 382 References 382 Afterword 385 Index 387
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 1.3 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 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 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 3.2 Self-hybridized Polaritons 41 3.3 Casimir Microcavities 44 3.4 Conclusions and Outlook 46 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 4.4 Photophysics of Plexcitons 65 4.5 Spectral Signatures 73 4.6 Applications 75 4.7 Conclusion 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 5.5 Cavity Description for Plasmon Modes 91 5.6 Nanocavities 93 5.7 Light-Matter Coupling 97 5.8 Conclusion 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 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 7.5 Multidimensional Electronic Spectroscopy for Exciton Polaritons: Heisenberg-Langevin Theory 154 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 8.3 Applications 177 8.4 Summary and Outlook 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 9.3 The Influence of Disorder and Semilocalization on Vibrational Dynamics 203 9.4 Conclusion and Outlook 211 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 10.3 Experimental Signatures of Polariton Condensation in Organic Microcavities 225 10.4 The Molecular Medley for Polariton Condensation 227 10.5 Summary 242 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 11.3 Polariton Relaxation Mechanisms 257 11.4 Comparison Between the Experimentally and Theoretically Estimated Wep in BSBCz-EH System 264 11.5 Conclusion 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 12.4 Summary 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 13.3 Nonidealities: That We Must, Nevertheless, Deal with 294 13.4 Current Challenges and Proposed Best Practices 299 13.5 Conclusion 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 14.3 Gauge Relativity 324 14.4 Imperfect Cavities 347 14.5 Conclusions 356 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 15.3 Effective Models in Cavity QED 372 15.4 The Ground States in Cavity QED 377 15.5 Conclusions 382 References 382 Afterword 385 Index 387
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