Bhattacharyya Pallavi, Sebastian K L
Department of Inorganic and Physical Chemistry, Indian Institute of Science, Bangalore 560012, India.
Phys Rev E Stat Nonlin Soft Matter Phys. 2013 Jun;87(6):062712. doi: 10.1103/PhysRevE.87.062712. Epub 2013 Jun 24.
We suggest a method of studying coherence in finite-level systems coupled to the environment and use it for the Hamiltonian that has been used to describe the light-harvesting pigment-protein complex. The method works with the adiabatic states and transforms the Hamiltonian to a form in which the terms responsible for decoherence and population relaxation are separated out. Decoherence is then accounted for nonperturbatively and population relaxation using a Markovian master equation. Almost analytical results can be obtained for the seven-level system, and the calculations are very simple for systems with more levels. We apply the treatment to the seven-level system, and the results are in excellent agreement with the exact numerical results of Nalbach et al. [Nalbach, Braun, and Thorwart, Phys. Rev. E 84, 041926 (2011)]. Our approach is able to account for decoherence and population relaxation separately. It is found that decoherence causes only damping of oscillations and does not lead to transfer to the reaction center. Population relaxation is necessary for efficient transfer to the reaction center, in agreement with earlier findings. Our results show that the transformation to the adiabatic basis followed by a Redfield type of approach leads to results in good agreement with exact simulation.
我们提出了一种研究与环境耦合的有限能级系统中相干性的方法,并将其应用于用于描述光捕获色素 - 蛋白质复合体的哈密顿量。该方法适用于绝热态,并将哈密顿量变换为一种形式,其中导致退相干和布居弛豫的项被分离出来。然后,使用马尔可夫主方程对退相干进行非微扰处理,并对布居弛豫进行处理。对于七能级系统可以得到几乎解析的结果,对于更多能级的系统计算也非常简单。我们将该处理方法应用于七能级系统,结果与纳尔巴赫等人 [纳尔巴赫、布劳恩和索尔瓦特,《物理评论E》84, 041926 (2011)] 的精确数值结果非常吻合。我们的方法能够分别考虑退相干和布居弛豫。结果发现,退相干仅导致振荡的阻尼,而不会导致向反应中心的转移。与早期研究结果一致,布居弛豫对于有效转移到反应中心是必要的。我们的结果表明,转换到绝热基然后采用雷德菲尔德类型的方法得到的结果与精确模拟结果吻合良好。