Molecular Polariton Dynamics in Realistic Cavities

Area of Science:

• Computational Chemistry
• Quantum Dynamics
• Cavity Quantum Electrodynamics

Background:

• Ab initio methods for polaritonic chemistry face high computational costs due to many degrees of freedom.
• Semiclassical approaches treating light classically offer a viable alternative to overcome these limitations.

Purpose of the Study:

• To develop and implement a computational approach for simulating polaritonic chemistry.
• To enable the study of large molecular systems interacting with realistic optical cavities.

Main Methods:

• Numerical propagation of Maxwell's equations for simulating realistic cavities.
• Quantum electron dynamics using the density functional tight-binding (DFTB) theory.
• Coupling classical light simulation with quantum molecular dynamics.

Main Results:

• Successfully simulated polaritonic signals in transmission spectra.
• Observed complex molecular responses influenced by cavity properties and molecular arrangement.
• Enabled atomistic-level simulations of numerous molecules within cavities.

Conclusions:

• The developed method overcomes computational limitations in polaritonic chemistry.
• Provides detailed insights into molecule-cavity interactions at the atomistic level.
• Facilitates the study of systems mimicking experimental setups for polaritonic phenomena.