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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >The Relaxation Dynamics and Short-Time Optical Response of a Multimode Open System
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The Relaxation Dynamics and Short-Time Optical Response of a Multimode Open System

机译：多模开放系统的弛豫动力学和短时光学响应

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摘要

When dividing a large system into a subsystem and a bath, one sometimes needs to include multiple nuclear coordinates in the subsystem in order to treat the remaining bath modes by Markovian relaxation theory (which assumes fast bath relaxation). This paper examines the effects of Redfield relaxation on the time-resolved fluorescence signal and on the loss of energy from a three-mode system. Simulations are compared for system coordinates coupled to the same bath mode and to independent bath modes, for coupling linear and quadratic in the system coordinates, and for different temperatures. To make these comparisons meaningful, a criterion is proposed for normalization of the coupling strengths in the different cases. The fluorescence Stokes shift and the system energy are shown to be sensitive to different relaxation processes. The coupling of multiple system coordinates to the same bath mode results in a wide range of relaxation rates. Simple descriptions in terms of individual population relaxation and coherence dephasing rates are inadequate due to sequential processes and to coupling between populations and coherences. These results have implications not only for Redfield treatments but also for other relaxation theories such as the Brownian oscillator model.
机译：将大型系统划分为一个子系统和一个浴场时，有时需要在子系统中包含多个核坐标，以便通过马尔可夫松弛理论（假定快速浴场松弛）来处理其余的浴场模式。本文研究了雷德菲尔德弛豫对时间分辨荧光信号和三模系统能量损失的影响。比较了针对耦合到相同水槽模式和独立水槽模式的系统坐标，用于耦合系统坐标中的线性和二次方以及不同温度的仿真。为了使这些比较有意义，提出了在不同情况下标准化耦合强度的标准。荧光斯托克斯位移和系统能量显示出对不同的弛豫过程敏感。将多个系统坐标耦合到相同的沐浴模式会导致宽范围的松弛率。由于顺序的过程以及种群与一致性之间的耦合，因此关于个体种群弛豫和相干移相速率的简单描述是不够的。这些结果不仅对Redfield处理有影响，而且对其他松弛理论（如Brownian振荡器模型）也有影响。

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