Efficient parallel strategy for molecular plasmonics -- a numerical tool for integrating Maxwell-Schrodinger equations in three dimensions

TL;DR

This paper introduces a parallel computational method for simulating the optical behavior of large ensembles of quantum emitters in complex electromagnetic environments, enabling detailed analysis of collective effects and dissociation dynamics.

Contribution

It presents a load-balanced, three-dimensional domain decomposition approach integrated into Maxwell-Schrodinger simulations, allowing for efficient handling of hundreds of thousands of molecules.

Findings

Achieved significant speedup in simulations of large molecular ensembles.

Demonstrated the impact of strong coupling on molecular dissociation rates.

Enabled detailed study of collective optical effects in complex nanostructures.

Abstract

An efficient parallelization approach to simulate optical properties of ensembles of quantum emitters in realistic electromagnetic environments is considered. It relies on balancing computing load of utilized processors and is built into three-dimensional domain decomposition methodology implemented for numerical integration of the Maxwell equations. The approach employed enables directly accessing dynamics of collective effects as the number of molecules in simulations can be drastically increased. Numerical experiments measuring speedup factors demonstrate the efficiency of the proposed methodology. As an example, we consider dynamics of nearly 700,000 diatomic molecules with ro-vibrational degrees of freedom explicitly accounted for coupled to electromagnetic radiation crafted by periodic arrays of split-ring resonators and triangular nanoholes. As an application of the approach, dissociation dynamics under strong coupling conditions is scrutinized. It is demonstrated that the dissociation rates are significantly affected near polaritonic frequencies.