Polariton Technologies#

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Nonlinear mesoscale polariton dynamics#

Vibrational strong coupling (VSC) experiments are usually performed in planar Fabry-Pérot cavities, where a macroscopic number of molecules couples collectively to a continuum of cavity modes. By contrast, current theoretical treatments simplify this setting to a handful of molecules coupled to a single cavity mode. Hence, developing theoretical frameworks for VSC beyond the single-mode approximation is crucial for a comprehensive understanding of these experiments.

To this end, we have developed the mesoscale cavity molecular dynamics (CavMD) scheme to attack this challenge. With this approach, we achieve real-space imaging of vibrational polariton transport in 2D, which involves self-consistent propagation of approximately 20,000 realistic molecular simulation cells coupled to a multimode cavity. Beyond the well-known ballistic-to-diffusive turnover in the linear response regime, we find a nonlinear freezing mechanism of polariton transport under strong pumping.

Under strong pumping, the initially ballistic upper polariton wavepacket freezes and localizes energy.

References

  1. 29.

    Mesoscale Molecular Simulations of Fabry-Pérot Vibrational Strong Coupling

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

  2. 40.

    Nonlinear Freezing of Vibrational Polariton Transport via Mesoscale Simulations

    Xinwei Ji, Tao E. Li. Nano Lett. acs.nanolett.6c03367 (2026).

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CHE-2502758