The Optical Signatures of Stochastic Processes in Many-Body Exciton Scattering.

IF 11.7 1区 化学 Q1 CHEMISTRY, PHYSICAL Annual review of physical chemistry Pub Date : 2023-04-24 DOI:10.1146/annurev-physchem-102822-100922
Hao Li, S A Shah, Ajay Ram Srimath Kandada, Carlos Silva, Andrei Piryatinski, Eric R Bittner
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引用次数: 3

Abstract

We review our recent quantum stochastic model for spectroscopic lineshapes in the presence of a coevolving and nonstationary background population of excitations. Starting from a field theory description for interacting bosonic excitons, we derive a reduced model whereby optical excitons are coupled to an incoherent background via scattering as mediated by their screened Coulomb coupling. The Heisenberg equations of motion for the optical excitons are then driven by an auxiliary stochastic population variable, which we take to be the solution of an Ornstein-Uhlenbeck process. Here, we present an overview of the theoretical techniques we have developed as applied to predicting coherent nonlinear spectroscopic signals. We show how direct (Coulomb) and exchange coupling to the bath give rise to distinct spectral signatures and discuss mathematical limits on inverting spectral signatures to extract the background density of states.

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多体激子散射随机过程的光学特征。
我们回顾了我们最近的量子随机模型,在共同进化和非平稳背景种群的激励下,谱线形状。从相互作用玻色子激子的场论描述出发,我们推导了一个简化模型,其中光学激子通过散射耦合到非相干背景,并通过它们的屏蔽库仑耦合介导。然后,光学激子的海森堡运动方程由一个辅助的随机总体变量驱动,我们将其作为Ornstein-Uhlenbeck过程的解。在这里,我们提出的理论技术的概述,我们已经开发的应用于预测相干非线性光谱信号。我们展示了直接(库仑)和交换耦合如何产生不同的光谱特征,并讨论了反演光谱特征以提取状态背景密度的数学限制。
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来源期刊
CiteScore
28.00
自引率
0.00%
发文量
21
期刊介绍: The Annual Review of Physical Chemistry has been published since 1950 and is a comprehensive resource for significant advancements in the field. It encompasses various sub-disciplines such as biophysical chemistry, chemical kinetics, colloids, electrochemistry, geochemistry and cosmochemistry, chemistry of the atmosphere and climate, laser chemistry and ultrafast processes, the liquid state, magnetic resonance, physical organic chemistry, polymers and macromolecules, and others.
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