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Nonlinear optical spectroscopy of single, few, and many molecules; nonequilibrium Green's function QED approach

机译:单个,少数和许多分子的非线性光学光谱;   非平衡格林函数QED方法

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摘要

Nonlinear optical signals from an assembly of N noninteracting particlesconsist of an incoherent and a coherent component, whose magnitudes scale \simN and \sim N(N-1), respectively. A unified microscopic description of bothtypes of signals is developed using a quantum electrodynamical (QED) treatmentof the optical fields. Closed nonequilibrium Green's function expressions arederived that incorporate both stimulated and spontaneous processes. General(n+1)-wave mixing experiments are discussed as an example of spontaneouslygenerated signals. When performed on a single particle, such signals cannot beexpressed in terms of the nth order polarization, as predicted by thesemiclassical theory. Stimulated processes are shown to be purely incoherent innature. Within the QED framework, heterodyne-detected wave mixing signals aresimply viewed as incoherent stimulated emission, whereas homodyne signals aregenerated by coherent spontaneous emission.
机译:来自N个非相互作用粒子的集合的非线性光学信号由非相干分量和相干分量组成,其大小分别为\ simN和\ sim N(N-1)。使用光场的量子电动力学(QED)处理开发了两种信号的统一微观描述。推导了封闭的非平衡格林函数表达式,其中包含了受激过程和自发过程。讨论了一般(n + 1)波混合实验作为自发信号的示例。当在单个粒子上执行时,如这些经典理论所预测的那样,此类信号无法按照n阶极化来表达。刺激过程显示为纯非相干性质。在QED框架内,将外差检测到的混波信号简单地视为非相干受激发射,而零差信号则由相干自发产生。

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