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arXiv 2312.13618quant-phphysics.chem-ph
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高斯环境下广义系统-浴纠缠定理

Generalized system-bath entanglement theorem for Gaussian environments

Yu Su, Yao Wang, Rui-Xue Xu, YiJing Yan

AI总结:

将系统-浴纠缠定理从线性响应推广到关联函数,利用广义朗之万动力学和Bogoliubov变换,实现复合空间中纠缠关联的计算,并演示于电子转移系统的溶剂化自由能。

摘要:

系统-浴纠缠定理(SBET)在之前的工作中针对高斯环境建立,见J. Chem. Phys. 152, 034102 (2020),该定理以线性响应函数形式表述。此定理将系统-浴纠缠响应与局域系统和裸浴的响应联系起来。在本工作中,我们将其推广到关联函数。推导的关键步骤包括:沿用之前工作中的混合浴模式的广义朗之万动力学,以及通过辅助浴将原始有限温度正则热库映射到有效零温真空的Bogoliubov变换。利用该定理,只要已知裸浴的统计性质并获得约化系统的关联,就可以在全复合空间中计算系统-浴纠缠关联和浴模式关联。我们以具有特定分子内振动模式的电子转移系统的溶剂化自由能计算为例进行了数值演示。

英文摘要:

A system-bath entanglement theorem (SBET) with Gaussian environments was established previously in J. Chem. Phys. 152, 034102 (2020) in terms of linear response functions. This theorem connects the system-bath entanglement responses to the local system and bare bath ones. In this work, we generalize it to correlation functions. Key steps in derivation are the generalized Langevin dynamics for the hybridizing bath modes as in the previous work, together with the Bogoliubov transformation mapping the original finite-temperature canonical reservoir to an effective zero-temperature vacuum via an auxiliary bath. With the theorem, the system-bath entangled correlations and the bath modes correlations in the full composite space can be evaluated as long as the bare-bath statistical properties are known and the reduced system correlations are obtained. Numerical demonstrations are carried out for the evaluation of the solvation free energy of an electron transfer system with a certain intramolecular vibrational modes.

机构、总结、中文摘要均由AI分析而来,可能存在错误,请以论文正文为准。

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