Polariton Assisted Down-Conversion of Photons via Nonadiabatic Molecular Dynamics: A Molecular Dynamical Casimir Effect
Polariton Assisted Down-Conversion of Photons via Nonadiabatic Molecular Dynamics: A Molecular Dynamical Casimir Effect
复制标题
极化子通过非绝热分子动力学辅助光子下转换：分子动力学卡西米尔效应
DOI：
10.1021/acs.jpclett.9b02870
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发表时间：
2019
期刊：
影响因子：
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通讯作者：
Yuen-Zhou, Joel
中科院分区：
文献类型：
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作者：
Pérez-Sánchez, Juan B.;Yuen-Zhou, Joel
从理论上研究了3，3 ′-二乙基-2，2 ′-噻炔碘化物分子在光学微腔中光致异构化的量子动力学。通过量子Rabi哈密顿量将由两个电子态和反应坐标组成的分子模型耦合到单腔模中，并采用多构型含时Hartree方法（MCTDH）求解由纯分子激发出发的含时薛定谔方程.我们表明，对于单分子强耦合的光子模式，非绝热分子动力学产生混合的极化激元流形与不同数量的激发，而不需要反向旋转的光-物质耦合项。因此，在顺式构型的分子的电子激发之后，在反式构型异构化时产生两个光子。讨论了这种现象在集体强光-物质耦合制度下工作的条件，并根据微腔内两个分子的模拟，发现对于本系统是不可行的。然而，我们的发现提出了一种新的机制，即在没有超强耦合的情况下，通过利用极化激元结构中出现的分子动力学来实现光子下转换。
Quantum dynamics of the photoisomerization of a single 3,3′-diethyl-2,2′-thiacynine iodide molecule embedded in an optical microcavity was theoretically studied. The molecular model consisting of two electronic states and the reaction coordinate was coupled to a single cavity mode via the quantum Rabi Hamiltonian, and the corresponding time-dependent Schrödinger equation starting with a purely molecular excitation was solved using the Multiconfigurational Time-Dependent Hartree Method (MCTDH). We show that, for single-molecule strong coupling with the photon mode, nonadiabatic molecular dynamics produces mixing of polariton manifolds with differing number of excitations, without the need of counter-rotating light–matter coupling terms. Therefore, an electronic excitation of the molecule at thecisconfiguration is followed by the generation of two photons in thetransconfiguration upon isomerization. Conditions for this phenomenon to be operating in the collective strong light–matter coupling regime are discussed and found to be unfeasible for the present system, based on simulations of two molecules inside the microcavity. Yet, our finding suggests a new mechanism that, without ultrastrong coupling, achieves photon down-conversion by exploiting the emergent molecular dynamics arising in polaritonic architectures.