Cavity-Correlated Electron-Nuclear Dynamics from First Principles
Cavity-Correlated Electron-Nuclear Dynamics from First Principles
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DOI：
10.1103/physrevlett.121.113002
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发表时间：
2018-09-12
影响因子：
8.6
通讯作者：
Narang, Prineha
中科院分区：
文献类型：
--
作者：
Flick, Johannes;Narang, Prineha
极化子化学和量子光学领域的迅速发展和融合需要一种统一的方法来预测原子尺度分辨率的强相关光-物质相互作用。为了实现这一总体目标，我们引入了一个一般的含时密度泛函理论来研究相关的电子，核，光子相互作用在同一量子化的基础上。我们补充我们的理论公式与第一从头计算的相关电子-核-光子系统。对于一个CO2分子在光学腔中，我们构建的红外光谱表现出拉比分裂之间的上，下极化激元分支，时间依赖的量子电动力学观测，如电位移场，并观察腔调制的分子运动。我们的工作开辟了一条重要的新途径，将从头算方法引入集体强振动光物质相互作用的新生领域。
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.