Optimization of Exciton Trapping in Energy Transfer Processes

被引:213
作者
Cao, Jianshu [1 ]
Silbey, Robert J. [1 ]
机构
[1] MIT, Dept Chem, Cambridge, MA 02139 USA
基金
美国国家科学基金会;
关键词
OPTICAL-EXCITATIONS; FMO COMPLEX; COHERENCE; PHOTOSYNTHESIS; ABSORPTION; DENDRIMERS; MIGRATION; TRANSPORT; DYNAMICS; SYSTEMS;
D O I
10.1021/jp9032589
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
In this paper, we establish optimal conditions for maximal energy transfer efficiency using solutions for multilevel systems and interpret these analytical Solutions With More intuitive kinetic networks resulting from a systematic mapping procedure. The mapping procedure defines ail effective hopping late as the leading order Picture and nonlocal kinetic Couplings as the quantum correction, hence leading to it rigorous separation of thermal hopping and coherent transfer useful for visualizing pathway connectivity and interference in quantum networks. As a result of these calculations, the dissipative effects of the surrounding environments call be optimized to yield the maximal efficiency, and modulation of the efficiency call be achieved using the cumulative quantum phase along Lilly closed loops. The optimal coupling of the system and its environments is interpreted with the generic mechanisms (i) balancing localized trapping and delocalized coherence, (ii) reducing the effective detuning via homogeneous line-broadening, (iii) Suppressing the destructive interference in nonlinear network configurations, and (iv) controlling phase modulation ill closed loop configurations. Though these results are obtained for simple model systems, the physics thus derived provides insights into the working of light harvesting systems, and the approaches thus developed apply to large-scale computation
引用
收藏
页码:13825 / 13838
页数:14
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