De Silva Nisal, Warnakula Tharindu, Gunapala Sarath D, Stockman Mark I, Premaratne Malin
Advanced Computing and Simulation Laboratory (AχL), Department of Electrical and Computer Systems Engineering, Monash University, Clayton, Victoria 3800, Australia.
Jet Propulsion Laboratory, California Institute of Technology, Pasadena, CA 91109, United States of America.
J Phys Condens Matter. 2021 Feb 18;33(14). doi: 10.1088/1361-648X/abe078.
Electronic excitation energy transfer is a ubiquitous process that has generated prime research interest since its discovery. Recently developed variational polaron transformation-based second-order master equation is capable of interpolating between Förster and Redfield limits with exceptional accuracy. Forms of spectral density functions studied so far through the variational approach provide theoretical support for various experiments. Recently introduced ohmic like spectral density function that can account for logarithmic perturbations provides generality and exposition to a unique and practical set of environments. In this paper, we exploit the energy transfer dynamics of a two-level system attached to an ohmic like spectral density function with logarithmic perturbations using a variational polaron transformed master equation. Our results demonstrate that even for a relatively large bath coupling strength, quantum coherence effects can be increased by introducing logarithmic perturbations of the order of one and two in super-ohmic environments. Moreover, for particular values of the ohmicity parameter, the effect of logarithmic perturbations is observed to be insignificant for the overall dynamics. In regard to ohmic environments, as logarithmic perturbations increase, damping characteristics of the coherent transient dynamics also increase in general. It is also shown that, having logarithmic perturbations of the order of one in an ohmic environment can result in a less efficient energy transfer for relatively larger system bath coupling strengths.
电子激发能量转移是一个普遍存在的过程,自发现以来一直是主要的研究热点。最近基于变分极化子变换发展的二阶主方程能够以极高的精度在福斯特极限和雷德菲尔德极限之间进行插值。迄今为止通过变分方法研究的谱密度函数形式为各种实验提供了理论支持。最近引入的能解释对数微扰的类欧姆谱密度函数为一组独特且实用的环境提供了通用性和阐释。在本文中,我们使用变分极化子变换主方程研究了一个与具有对数微扰的类欧姆谱密度函数相连的两能级系统的能量转移动力学。我们的结果表明,即使对于相对较大的浴耦合强度,在超欧姆环境中通过引入一阶和二阶对数微扰也可以增强量子相干效应。此外,对于欧姆性参数的特定值,观察到对数微扰对整体动力学的影响不显著。对于欧姆环境,随着对数微扰增加,相干瞬态动力学的阻尼特性通常也会增加。还表明,在欧姆环境中具有一阶对数微扰对于相对较大的系统 - 浴耦合强度可能导致能量转移效率较低。