Analysis of the Classical Trajectory Treatment of Photon Dynamics for Polaritonic Phenomena

Abstract

Simulating photon dynamics in strong light-matter coupling situations via classical trajectories is proving to be powerful and practical. Here we analyze the performance of the approach through the lens of the exact factorization approach. Since the exact factorization enables a rigorous definition of the potentials driving the photonic motion it allows us to identify that the cause of the underestimation of photon number and intensities observed in earlier work is primarily due to an inadequate accounting of light-matter correlation in the classical Ehrenfest force rather than errors from treating the photons quasiclassically per se. The latter becomes problematic when the number of photons per mode begins to exceed a half.

References in corpus (12)

• How to face the loss in plasmonics and metamaterials
• Quantum Electrodynamical Density-Functional Theory: Bridging Quantum Optics and Electronic-Structure Theory
• Theoretical Challenges in Polaritonic Chemistry
• The exact forces on classical nuclei in non-adiabatic charge transfer
• Large Enhancement of Ferro-Magnetism under Collective Strong Coupling of YBCO Nanoparticles
• Capturing Vacuum Fluctuations and Photon Correlations in Cavity Quantum Electrodynamics with Multi-Trajectory Ehrenfest Dynamics
• Benchmarking Semiclassical and Perturbative Methods for Real-time Simulations of Cavity-Bound Emission and Interference
• Ultrafast dynamics with the exact factorization
• Simulating Photodissociation Reactions in Bad Cavities with the Lindblad Equation
• Cumulant expansion for the treatment of light-matter interactions in arbitrary material structures
• Molecular photodissociation enabled by ultrafast plasmon decay
• Case Studies of the Time-Dependent Potential Energy Surface for Dynamics in Cavities

Cited by in corpus (5)

• QM/MM Modeling of Vibrational Polariton Induced Energy Transfer and Chemical Dynamics
• Semiclassical Real-Time Nuclear-Electronic Orbital Dynamics for Molecular Polaritons: Unified Theory of Electronic and Vibrational Strong Couplings
• Electronic Born-Oppenheimer Approximation in Nuclear-Electronic Orbital Dynamics
• Selective Excitation of IR-Inactive Modes via Vibrational Polaritons: Insights from Atomistic Simulations
• Polariton-induced Purcell effects via a reduced semiclassical electrodynamics approach