Computational Polaritonics

We simulate and model molecular polaritons by developing a variety of general-purpose and open-source computational approaches.

Cavity molecular dynamics (CavMD)

Expanding the scope of conventional molecular dynamics, the single-mode CavMD approach can efficiently simulate collective vibrational strong coupling between a single or a few cavity modes coupled to a molecular ensemble in the condensed phase. Beyond single-mode CavMD, the mesoscale CavMD approach aims to simulate vibrational strong coupling for condensed-phase molecules formed in a wide range of cavity geometries, such as the planar Fabry—Pérot cavities employed in experiments.

We are actively examining the boundaries of single-mode and mesoscale CavMD. Please check the Github page for more details.

Representative work

11. Tao E. Li, Joseph E. Subotnik, Abraham Nitzan. "Cavity Molecular Dynamics Simulations of Liquid Water under Vibrational Ultrastrong Coupling"

Proc. Natl. Acad. Sci., 117, 18324–18331 (2020)

27. Tao E. Li. "Mesoscale Molecular Simulations of Fabry-Pérot Vibrational Strong Coupling"

J. Chem. Theory Comput., 20, 7016–7031 (2024)

Reduced semiclassical electrodynamics

While the CavMD approach simulates all molecules explicitly, the reduced semiclassical electrodynamics approach takes a completely different strategy. In this approach, the coupled Maxwell–Schrödinger equations are propagated for simulating local molecular processes in a realistic cavity structure under collective strong coupling. Particularly, only a few molecules, referred to as quantum impurities, are treated quantum mechanically, while the remaining macroscopic molecular layer and the cavity structure are modeled using dielectric functions.

This approach is at its infancy, and we are actively working on improving its performance for studying polariton dynamics.

Representative work

30. Andres Felipe Bocanegra Vargas, Tao E. Li. "Polariton-Induced Purcell Effects via a Reduced Semiclassical Electrodynamics Approach"

J. Chem. Phys., 162, 124104 (2025)

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