Charge Hopping Dynamics along a Disordered Chain in Quantum Environments: Comparative Study of Different Rate Kernels.
Charge Hopping Dynamics along a Disordered Chain in Quantum Environments: Comparative Study of Different Rate Kernels.
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量子环境中沿无序链的电荷跳跃动力学：不同速率内核的比较研究。
DOI：
10.1021/jp511933m
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发表时间：
2015
期刊：
影响因子：
--
通讯作者：
Andrés Montoya
中科院分区：
文献类型：
--
作者：
Seogjoo J. Jang;Andrés Montoya
计算研究了具有高斯位能无序和线性耦合量子浴的一维链上电荷沿着跳跃动力学。直接从Pauli主方程的数值解计算时间相关的平方位移，对于五种不同的速率核：精确费米黄金法则（FGR）速率表达式，固定相位插值（SPI）近似，半经典（SC）近似，经典Marcus速率表达式和Miller-Abrahams表达式。所有结果表明在稳态极限下的扩散行为。基于FGR速率表达式的结果表明，量子浴中的电荷输运可以比经典Marcus表达式的预测更敏感的无序。虽然SPI近似相当好地捕捉到了这一总体趋势，但SC近似在定量和定性水平上都不可靠，并且在某些条件下甚至比经典的Marcus表达式更差。这些结果提供了有用的指导，在选择近似速率内核的大规模模拟，也表现出显着的，但脆弱的积极影响的量子环境上的电荷跳跃动力学。
This work presents a computational study of charge hopping dynamics along a one-dimensional chain with Gaussian site energy disorder and linearly coupled quantum bath. Time-dependent square displacements are calculated directly from numerical solutions of Pauli master equations, for five different rate kernels: exact Fermi golden rule (FGR) rate expression, stationary phase interpolation (SPI) approximation, semiclassical (SC) approximation, classical Marcus rate expression, and Miller-Abrahams expression. All results demonstrate diffusive behavior in the steady state limit. The results based on the FGR rate expression show that the charge transport in the quantum bath can be much more sensitive to the disorder than the prediction from the classical Marcus expression. While the SPI approximation captures this general trend reasonably well, the SC approximation tends to be unreliable at both quantitative and qualitative levels and becomes even worse than the classical Marcus expression under certain conditions. These results offer useful guidance in the choice of approximate rate kernels for larger-scale simulations and also demonstrate significant but fragile positive effects of quantum environments on the charge hopping dynamics.
影响因子：
5.5
作者：
Ruehle, Victor;Lukyanov, Alexander;May, Falk;Schrader, Manuel;Vehoff, Thorsten;Kirkpatrick, James;Baumeier, Bjoern;Andrienko, Denis
通讯作者：
Andrienko, Denis