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- W2796688500 abstract "The rapidly developing and converging fields of polaritonic chemistry and quantum optics necessitate a unified approach to predict strongly correlated light-matter interactions with atomic-scale resolution. Toward this overarching goal, we introduce a general time-dependent density-functional theory to study correlated electron, nuclear, and photon interactions on the same quantized footing. We complement our theoretical formulation with the first ab initio calculation of a correlated electron-nuclear-photon system. For a ${mathrm{CO}}_{2}$ molecule in an optical cavity, we construct the infrared spectra exhibiting Rabi splitting between the upper and lower polaritonic branches, time-dependent quantum-electrodynamical observables such as the electric displacement field, and observe cavity-modulated molecular motion. Our work opens an important new avenue in introducing ab initio methods to the nascent field of collective strong vibrational light-matter interactions." @default.
- W2796688500 created "2018-04-24" @default.
- W2796688500 creator A5038553566 @default.
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- W2796688500 date "2018-09-12" @default.
- W2796688500 modified "2023-10-16" @default.
- W2796688500 title "Cavity-Correlated Electron-Nuclear Dynamics from First Principles" @default.
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- W2796688500 doi "https://doi.org/10.1103/physrevlett.121.113002" @default.
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