Multiple Interacting Photonic Modes in Strongly Coupled Organic Microcavities
arXiv:2407.04904 · doi:10.1098/rsta.2023.0343
Abstract
Room temperature cavity quantum electrodynamics with molecular materials in optical cavities offers exciting prospects for controlling electronic, nuclear and photonic degrees of freedom for applications in physics, chemistry and materials science. However, achieving strong coupling with molecular ensembles typically requires high molecular densities and substantial electromagnetic field confinement. These conditions usually involve a significant degree of molecular disorder and a highly structured photonic density of states. It remains unclear to what extent these additional complexities modify the usual physical picture of strong coupling developed for atoms and inorganic semiconductors. Using a microscopic quantum description of molecular ensembles in realistic multimode optical resonators, we show that the emergence of a vacuum Rabi splitting in linear spectroscopy is a necessary but not sufficient metric of coherent admixing between light and matter. In low finesse multi-mode situations we find that molecular dipoles can be partially hybridised with photonic dissipation channels associated with off-resonant cavity modes. These vacuum-induced dissipative processes ultimately limit the extent of light-matter coherence that the system can sustain.
13 pages, 4 figures
References in corpus (16)
- Coherent coupling of molecular resonators with a micro-cavity mode
- Quantum Electrodynamical Density-Functional Theory: Bridging Quantum Optics and Electronic-Structure Theory
- Multiple Rabi Splittings under Ultra-Strong Vibrational Coupling
- Unveiling the mixed nature of polaritonic transport: From enhanced diffusion to ballistic motion approaching the speed of light
- Theory of Nanoscale Organic Cavities: The Essential Role of Vibration-Photon Dressed States
- Macroscopic QED for quantum nanophotonics: Emitter-centered modes as a minimal basis for multi-emitter problems
- Disorder-Enhanced and Disorder-Independent Transport with Long-Range Hopping: Application to Molecular Chains in Optical Cavities
- Polariton Localization and Dispersion Properties of Disordered Quantum Emitters in Multimode Microcavities
- A theoretical perspective on molecular polaritonics
- Disorder enhanced vibrational entanglement and dynamics in polaritonic chemistry
- Non-polaritonic effects in cavity-modified photochemistry
- Microscopic Theory of Multimode Polariton Dispersion in Multilayered Materials
- Large Random Arrowhead Matrices: Multifractality, Semi-Localization, and Protected Transport in Disordered Quantum Spins Coupled to a Cavity
- A Lindblad master equation capable of describing hybrid quantum systems in the ultra-strong coupling regime
- Extremely large Lamb shift in a deep-strongly coupled circuit QED system with a multimode resonator
- Exploring the Nature of High-Order Cavity Polaritons under the Coupling-Decoupling Transition