发表机构
Gauhati University; Indian Institute of Science（古瓦哈提大学; 印度科学学院）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究通过协同隧穿效应，在光系统II反应中心模型中揭示了被动态排序的微观重排，并利用ergotropy和能量电容量化了能量再分布机制。
AI 中文摘要
我们研究了协同隧穿如何影响光系统II反应中心（建模为非平衡分子结）中的被动态排序。我们使用完整的色素激发流形，其中激子态和电荷转移速率在Nakajima-Zwanzig形式下利用实际谱密度计算。协同隧穿通过微观构造的双重还原受体态引入，该态由相关的醌侧双电子构型获得，而光激发允许进入完整的激子流形。被动态置换通过ergotropy和能量电容进行量化。我们发现，ergotropy和能量电容中的热力学平滑性可能掩盖微观态重排。协同隧穿将可提取的非平衡能量在醌受体、供体-脱镁叶绿素自由基对以及来自非活性分支色素贡献显著的激子态之间重新分布。在高库仑相互作用下，协同隧穿不产生被动态重排。ergotropy、能量电容和平均能量之间的分段线性关系进一步揭示了协同隧穿产生的种群重排。
英文摘要
We investigate how cotunneling affects passive-state ordering in a Photosystem II reaction center modelled as a nonequilibrium molecular junction. We use a full pigment excitation manifold, with excitonic and charge-transfer rates computed within a Nakajima-Zwanzig formalism using realistic spectral densities. Cotunneling is introduced through a microscopically constructed doubly reduced acceptor state obtained from relevant quinone-side two-electron configurations, while photoexcitation is allowed into the full excitonic manifold. Passive-state permutations are quantified through ergotropy and energetic capacitance. We find that thermodynamic smoothness in ergotropy and energetic capacitance can conceal microscopic state rearrangements. Cotunneling redistributes the extractable nonequilibrium energy among the quinone acceptor, the donor-pheophytin radical pair, and excitonic states with strong contributions from pigments on the inactive branch. At high Coulomb interaction, cotunneling produces no passive-state reordering. Piecewise-linear relations among ergotropy, energetic capacitance, and mean energy further reveal the population reorderings generated by cotunneling.
CommentsContains Supplementary Information. Suggestions on references are welcome
