Flux-Conserving Diagrammatic Formulation of Optical Spectroscopy of Open Quantum Systems
Flux-Conserving Diagrammatic Formulation of Optical Spectroscopy of Open Quantum Systems
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DOI：
10.1021/acs.jpcc.9b08635
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发表时间：
2019-09
期刊：
影响因子：
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通讯作者：
S. Mukamel;Michael Galperin
中科院分区：
文献类型：
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作者：
S. Mukamel;Michael Galperin
我们提出了一种开放的非平衡系统的光学光谱学的理论方法，它概括了传统的非线性光学光谱学工具，在各级近似下施加电荷和能量守恒。分子和辐射场的自由度进行了量子力学处理。该公式是基于非平衡绿色函数（NEGF）的方法，和双面费曼图表示的光子通量。数值模拟的模型系统。我们的研究桥梁量子输运和光学光谱学的理论方法，并建立了一个坚实的基础，在分子光电子学中的非线性光学光谱的传统工具。
We present a theoretical approach to optical spectroscopy of open nonequilibrium systems, which generalizes traditional nonlinear optical spectroscopy tools by imposing charge and energy conservation at all levels of approximation. Both molecular and radiation field degrees of freedom are treated quantum mechanically. The formulation is based on the nonequilibrium Green’s function (NEGF) approach, and a double sided Feynman diagrammatic representation of the photon flux is developed. Numerical simulations are presented for a model system. Our study bridges the theoretical approaches of quantum transport and optical spectroscopy and establishes a firm basis for applying traditional tools of nonlinear optical spectroscopy in molecular optoelectronics.