Simulating anharmonic vibrational polaritons beyond the long wavelength approximation

作者：Dipti Jasrasaria, Arkajit Mandal, David R. Reichman, Timothy C. Berkelbach · 发表于：The Journal of Chemical Physics · 年份：2025 · DOI：10.1063/5.0235584 · 被引用次数：4 · 研究领域：Strong Light-Matter Interactions、Thermal Radiation and Cooling Technologies、Plasmonic and Surface Plasmon Research

In this work, we investigate anharmonic vibrational polaritons formed due to strong light-matter interactions in an optical cavity between radiation modes and anharmonic vibrations beyond the long-wavelength limit. We introduce a conceptually simple description of light-matter interactions, where spatially localized cavity radiation modes couple to localized vibrations. Within this theoretical framework, we employ self-consistent phonon theory and vibrational dynamical mean-field theory to efficiently simulate momentum-resolved vibrational-polariton spectra, including effects of anharmonicity. Numerical simulations in model systems demonstrate the accuracy and applicability of our approach.