Cavity Born-Oppenheimer Approximation for Correlated Electron-Nuclear-Photon Systems.
Cavity Born-Oppenheimer Approximation for Correlated Electron-Nuclear-Photon Systems.
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DOI：
10.1021/acs.jctc.6b01126
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发表时间：
2017-04-11
影响因子：
5.5
通讯作者：
Rubio A
中科院分区：
文献类型：
--
作者：
Flick J;Appel H;Ruggenthaler M;Rubio A
在这项工作中，我们详细说明了最近引入的腔玻恩-奥本海默近似概念[Flick等人，]相关的电子-核-光子问题。我们演示了如何在条件电子和光子核子波函数的扩展准确地描述强相关的光物质系统的本征态。对于GaAs量子环模型与光子模式共振，我们强调如何基态电子势能面改变通常的谐波电位的自由光子模式的修饰模式与双阱结构。这种变化伴随着电子基态密度的分裂。对于光子模式与振动跃迁共振的模型，我们在激发态电子势能面中观察到从单个最小值到双最小值的分裂。此外，对于一个随时间变化的设置，我们展示了如何在相关的光物质系统的动态可以理解的势能面之间的人口转移。这项工作在量子化学和量子光学的接口铺平了道路，为完整的从头计算描述的物质-光子系统。
In this work, we illustrate the recently introduced concept of the cavity Born–Oppenheimer approximation [Flick et al. , ] for correlated electron–nuclear-photon problems in detail. We demonstrate how an expansion in terms of conditional electronic and photon-nuclear wave functions accurately describes eigenstates of strongly correlated light-matter systems. For a GaAs quantum ring model in resonance with a photon mode we highlight how the ground-state electronic potential-energy surface changes the usual harmonic potential of the free photon mode to a dressed mode with a double-well structure. This change is accompanied by a splitting of the electronic ground-state density. For a model where the photon mode is in resonance with a vibrational transition, we observe in the excited-state electronic potential-energy surface a splitting from a single minimum to a double minimum. Furthermore, for a time-dependent setup, we show how the dynamics in correlated light-matter systems can be understood in terms of population transfer between potential energy surfaces. This work at the interface of quantum chemistry and quantum optics paves the way for the full ab initio description of matter-photon systems.