期刊
PHYSICAL REVIEW LETTERS
卷 121, 期 11, 页码 -出版社
AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.121.113002
关键词
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资金
- STC Center for Integrated Quantum Materials NSF [DMR-1231319]
- Harvard John A. Paulson School of Engineering and Applied Sciences
- Deutsche Forschungsgemeinschaft [FL 997/1-1]
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 CO2 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.
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