论文标题

通过多模式量子模型研究的分子旋转极化子的腔诱导的非绝热动力学和光谱

Cavity-induced Non-Adiabatic Dynamics and Spectroscopy of Molecular Rovibrational Polaritons studied by Multi-Mode Quantum Models

论文作者

Fischer, Eric W., Saalfrank, Peter

论文摘要

从理论上讲,我们研究了由单个旋转式双原子分子组成的模型系统中形成的旋转偏振子的量子动力学和光谱,该模型系统与两个退化,正交极化模式相互作用。我们在长度规代表示中采用了有效的旋转式Pauli-Fierz Hamiltonian,并在二维角度坐标空间中识别三态振动式圆锥形圆锥形交叉点(VPCI)。上部和上部振动极性子具有混合光材料杂种特征,而中间状态本质上是纯粹的光子。 VPCI在单一振兴的振动极性子之间提供有效的种群转移通道,在旋转密度中表现出丰富的干扰模式。从光谱镜上,当外部红外激光场与分子模式和空腔模式均识别出三个明亮的单一兴奋状态。非平凡的VPCI拓扑表现为上振动偏振子的光谱区域的明显多峰进展,该振动区域可追溯到Rovibro-Polaritonic轻质型混合状态的出现。实验上普遍存在的自发发射来自腔模式,引起了强度和峰值扩展的耗散降低,这主要影响纯光子中间状态峰以及rovibro-Polaritonic的进程。

We study theoretically the quantum dynamics and spectroscopy of rovibrational polaritons formed in a model system composed of a single rovibrating diatomic molecule, which interacts with two degenerate, orthogonally polarized modes of an optical Fabry-Pérot cavity. We employ an effective rovibrational Pauli-Fierz Hamiltonian in length gauge representation and identify three-state vibro-polaritonic conical intersections (VPCIs) between singly-excited vibro-polaritonic states in a two-dimensional angular coordinate branching space. The lower and upper vibrational polaritons are of mixed light-matter hybrid character, whereas the intermediate state is purely photonic in nature. The VPCIs provide effective population transfer channels between singly-excited vibrational polaritons, which manifest in rich interference patterns in rotational densities. Spectroscopically, three bright singly-excited states are identified, when an external infrared laser field couples to both a molecular and a cavity mode. The non-trivial VPCI topology manifests as pronounced multi-peak progression in the spectral region of the upper vibrational polariton, which is traced back to the emergence of rovibro-polaritonic light-matter hybrid states. Experimentally ubiquitous spontaneous emission from cavity modes induces a dissipative reduction of intensity and peak broadening, which mainly influences the purely photonic intermediate state peak as well as the rovibro-polaritonic progression.

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