静态和动态失调对紫细菌光合系统环状触角亚基辐射各向异性的影响
Influence of Static and Dynamic Disorder on the Anisotropy of Emission in the Ring Antenna Subunits of Purple Bacteria Photosynthetic Systems
摘要：
利用约化密度矩阵方法计算了紫色细菌捕光环系统中激子散射的时间依赖性。与Kumble和Hochstrasser（J.Chem.Phys.109（1998）855）的工作相反，考虑了静态无序（位置能量的波动）以及动态无序（耗散）。对于耗散的描述，我们使用Redfield理论在激子本征态没有长期近似。这被证明是等价于马尔可夫极限的Capek的理论在当地的国家。研究了具有18种色素的圆形聚集体，以模拟LH2络合物内细菌叶绿素的B850环。可以证明，耗散对于荧光的时间依赖性各向异性是重要的。与Kumble和Hochstrasser的结果相比，较小的静态无序值足以产生相同的各向异性衰减率。
英文摘要：
Using the reduced density matrix formalism the time dependence of the exciton scattering in light-harvesting ring systems of purple bacteria is calculated. In contrast to the work of Kumble and Hochstrasser (J. Chem. Phys. 109 (1998) 855) static disorder (fluctuations of the site energies) as well as dynamic disorder (dissipation) is taken into account. For the description of dissipation we use Redfield theory in exciton eigenstates without secular approximation. This is shown to be equivalent to the Markovian limit of Capek's theory in local states. Circular aggregates with 18 pigments are studied to model the B850 ring of bacteriochlorophyls within LH2 complexes. It can be demonstrated that the dissipation is important for the time-dependent anisotropy of the fluorescence. Smaller values of static disorder are sufficient to produce the same decay rates in the anisotropy in comparison with the results by Kumble and Hochstrasser.
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