MaxwellLink: A unified framework for self-consistent light-matter simulations

Abstract

A major challenge in light-matter simulations is bridging the disparate time and length scales of electrodynamics and molecular dynamics. Current computational approaches often rely on heuristic approximations of either the electromagnetic (EM) or the material component, hindering the exploration of complex light-matter systems. Herein, MaxwellLink -- a modular, open-source Python framework -- is developed for the massively parallel, self-consistent propagation of classical EM fields interacting with a large heterogeneous molecular ensemble. The package utilizes a robust TCP/UNIX socket interface to couple EM solvers with a wide range of molecular drivers. In this initial release, MaxwellLink supports EM solvers spanning from single-mode cavities to full-feature three-dimensional finite-difference time-domain (FDTD) engines, and molecules described by multilevel open quantum systems, force-field and first-principles molecular dynamics, and nonadiabatic real-time Ehrenfest dynamics. With the socket-based architecture, users can seamlessly switch between levels of theory of either the EM solver or molecules without modifying the counterpart. Moreover, the EM engine and molecular drivers scale independently across multiple high-performance computing (HPC) nodes, facilitating large-scale simulations previously inaccessible to existing numerical schemes. The versatility and accuracy of this code are further demonstrated through applications including superradiance, radiative energy transfer, vibrational strong coupling in Bragg resonators, and plasmonic heating of molecular gases. By providing a unified, extensible engine, MaxwellLink potentially offers a powerful platform for exploring emerging phenomena across the research fronts of spectroscopy, quantum optics, plasmonics, and polaritonics.