Tensor Network Simulation of Non-Markovian Dynamics in Organic Polaritons
Tensor Network Simulation of Non-Markovian Dynamics in Organic Polaritons
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DOI：
10.1103/physrevlett.121.227401
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发表时间：
2018-11-26
影响因子：
8.6
通讯作者：
Garcia-Vidal, Francisco J.
中科院分区：
文献类型：
--
作者：
del Pino, Javier;Schroder, Florian A. Y. N.;Garcia-Vidal, Francisco J.
我们计算了由有机分子填充的光腔支持的极化激元态的精确多体时间动力学。光学，振动和辐射过程被视为平等的基础上采用随时间变化的矩阵产品状态算法。我们证明了签名的非马尔可夫振动动力学和它的指纹在远场光子发射光谱在任意的光-物质相互作用的尺度，范围从弱到强的耦合制度。我们分析了单分子和多分子的情况下，分子核和暗态的集体运动在确定极化激元动力学和随后的光子发射中发挥了至关重要的作用。
We calculate the exact many-body time dynamics of polaritonic states supported by an optical cavity filled with organic molecules. Optical, vibrational, and radiative processes are treated on an equal footing employing the time-dependent variational matrix product states algorithm. We demonstrate signatures of non-Markovian vibronic dynamics and its fingerprints in the far-field photon emission spectrum at arbitrary light-matter interaction scales, ranging from the weak to the strong coupling regimes. We analyze both the single-and many-molecule cases, showing the crucial role played by the collective motion of molecular nuclei and dark states in determining the polariton dynamics and the subsequent photon emission.