Cavity-Mediated Enhancement of the Energy Transfer in the Reduced Fenna-Matthews-Olson Complex.

IF 5.7 1区 化学 Q2 CHEMISTRY, PHYSICAL
Journal of Chemical Theory and Computation Pub Date : 2024-09-10 Epub Date: 2024-08-27 DOI:10.1021/acs.jctc.4c00626
Luis E Herrera Rodríguez, Aarti Sindhu, Kennet J Rueda Espinosa, Alexei A Kananenka
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Abstract

Strong light-matter interaction leads to the formation of hybrid polariton states and can alter the light-harvesting properties of natural photosynthetic systems without modifying their chemical structure. In the present study, we computationally investigate the effect of the resonant cavity on the efficiency and the rate of the population transfer in a quantum system coupled to the cavity and the dissipative environment. The parameters of the model system were chosen to represent the Fenna-Matthews-Olson natural light-harvesting complex reduced to the three essential sites. The dynamics of the total system was propagated using the hierarchical equations of motion. Our results show that the strong light-matter interaction can accelerate the population transfer process compared to the cavity-free case but at the cost of lowering the transfer efficiency. The transition to the strong coupling regime was found to coincide with the degeneracy of polariton eigenvalues. Our findings indicate the potential and the limit of tuning the energy transfer in already efficient natural light-harvesting systems.

Abstract Image

空腔介导的还原 Fenna-Matthews-Olson 复合物能量转移的增强。
强烈的光物质相互作用会导致混合极化子态的形成,并能在不改变化学结构的情况下改变天然光合系统的光收集特性。在本研究中,我们通过计算研究了谐振腔对与腔体和耗散环境耦合的量子系统中种群转移的效率和速率的影响。我们选择了模型系统的参数来代表芬纳-马修斯-奥尔森自然采光复合体,并将其简化为三个基本位点。利用分层运动方程传播了整个系统的动力学。我们的结果表明,与无空腔情况相比,强光-物质相互作用可以加速种群转移过程,但代价是降低转移效率。向强耦合机制的过渡与极化子特征值的退化相吻合。我们的研究结果表明了在已经高效的自然光收集系统中调整能量转移的潜力和极限。
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来源期刊
Journal of Chemical Theory and Computation
Journal of Chemical Theory and Computation 化学-物理:原子、分子和化学物理
CiteScore
9.90
自引率
16.40%
发文量
568
审稿时长
1 months
期刊介绍: The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.
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