Year: 2026
Type: article
Abstract: Two-dimensional real-space imaging of vibrational polariton transport in planar Fabry–Pérot microcavities is numerically simulated via the mesoscale cavity molecular dynamics approach, which self-consistently propagates∼2×104 realistic molecular simulation cells on a two-dimensional grid coupled to the same number of cavity modes. Beyond the well-known polariton ballistic-to-diffusive turnover in the linear response regime, these atomistic simulations reveal a nonlinear freezing mechanism of vibrational polariton transport; that is, under strong pumping of the upper polariton, the initially ballistically propagating upper polariton completely freezes and localizes energy to molecules at specific locations. This mechanism originates from pump-induced breaking of the in-plane translation symmetry: significant molecular excitations at the pulse hot spot broaden the polariton density of states, thus funneling population to the k∥ → 0 band edge with vanishing group velocities. Overall, our work provides numerical insights for exploring novel mechanisms of vibrational polaritons.
Source: Nano Letters
Authors: Xinwei Ji, Tao E. Li
Institution: University of Delaware
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: green
Awards: G1453181110, G1555197637, G1787346651, Track 4: Advanced CI Coordination Ecosystem: Monitoring and Measurement Services, G2299875479, G2888034965, G3185749182, G338811424, G3562386289, Computational Polariton Chemistry Beyond the Single-mode Approximation, Track 1: ACCESS Resource Allocations Marketplace and Platform Services (RAMPS), G4010157413, G4071103020, ACO: An Open CI Ecosystem to Advance Scientific Discovery (OpenCI), G485097472, Track 3: COre National Ecosystem for CyberinfrasTructure (CONECT), G5367127336, G5464919783, G731264315, G7916508619, Track 2: Customized Multi-tier Assistance, Training, and Computational Help (MATCH) for End User ACCESS to CI, G878072758, G8994211811
OpenAlex ID: W7166557587