Exciton-polariton dynamics in multilayered materials

Coupling excitons with quantized radiation has been shown to enable coherent ballistic transport at room temperature inside optical cavities. Previous theoretical works employ a simple description of the material, depicting it as a one-dimensional single-layer placed in the middle of an optical cavity, thereby ignoring the spatial variation of the radiation field. In contrast, in most experiments, the optical cavity is filled with organic molecules or multiple layers of two-dimensional materials. Here, we develop an efficient mixed-quantum-classical approach, introducing a bright layer description, that enables the simulation of exciton-polariton quantum dynamics in all three dimensions. Our simulations reveal that, for the same Rabi splitting, a multilayered material extends the quantum coherence lifetime and enhances transport compared to a single-layer material. We find that this enhanced coherence can be traced to a synchronization of phonon fluctuations over multiple layers, wherein the collective light-matter coupling in a multilayered material effectively suppresses the phonon-induced dynamical disorder. Propagation of exciton-polaritons (EP) within optical cavities often relies on a single material layer approximation, which does not take the full light-matter coupling complexity into account. Here, the authors develop a quantum-classical approach to simulate EP dynamics in multilayered materials, unveiling longer EP coherence lifetimes compared to single-layer materials.