Coupling Polyatomic Molecules to Lossy Nanocavities: Lindblad versus Schrödinger description
arXiv:2403.02890 · doi:10.1063/5.0205048
Abstract
The use of cavities to impact molecular structure and dynamics has become popular. As cavities, in particular plasmonic nanocavities, are lossy and the lifetime of their modes can be very short, their lossy nature must be incorporated into the calculations. The Lindblad master equation is commonly considered as an appropriate tool to describe this lossy nature. This approach requires the dynamics of the density operator and is thus substantially more costly than approaches employing the Schrödinger equation for the quantum wave function when several or many nuclear degrees of freedom are involved. In this work we compare numerically the Lindblad and Schrödinger descriptions discussed in the literature for a molecular example where the cavity is pumped by a laser. The laser and cavity properties are varied over a range of parameters. It is found that the Schrödinger description adequately describes the dynamics of the polaritons and emission signal as long as the laser intensity is moderate and the pump time is not much longer than the lifetime of the cavity mode. Otherwise, it is demonstrated that the Schrödinger description gradually fails. We also show that the failure of the Schrödinger description can often be remedied by renormalizing the wave function at every step of the time propagation. The results are discussed and analyzed.
References in corpus (18)
- Strong coupling between surface plasmon polaritons and emitters
- Molecular polaritonics: Chemical Dynamics under strong Light-Matter Coupling
- Theoretical Challenges in Polaritonic Chemistry
- Resolution of Gauge Ambiguities in Molecular Cavity Quantum Electrodynamics
- Electron transfer in confined electromagnetic fields
- Strong coupling with light enhances the photoisomerization quantum yield of azobenzene
- Cavity-Born-Oppenheimer Hartree-Fock Ansatz: Light-matter Properties of Strongly Coupled Molecular Ensembles
- Entangled Photonic-Nuclear Molecular Dynamics of LiF in Quantum Optical Cavities
- Unraveling a cavity induced molecular polarization mechanism from collective vibrational strong coupling
- Quantum Coherent Control of a Single Molecular-Polariton Rotation
- Simulating Photodissociation Reactions in Bad Cavities with the Lindblad Equation
- Molecular photodissociation enabled by ultrafast plasmon decay
- A quantum optics approach to photoinduced electron transfer in cavities
- Collective response in light-matter interactions: The interplay between strong coupling and local dynamics
- Nonadiabatic phenomena in molecular vibrational polaritons
- Cavity-induced Non-Adiabatic Dynamics and Spectroscopy of Molecular Rovibrational Polaritons studied by Multi-Mode Quantum Models
- Radiative Emission of Polaritons Controlled by Light-Induced Geometric Phase
- Practical guide to the statistical mechanics of molecular polaritons