生物系统扩展跳跃位点中熵主导电荷传输的闪烁共振简并：静态到动态无序转变的作用
A Flickering Resonance Degeneracy on Entropy-Ruled Charge Transport in the Extended Hopping Sites for Biological Systems: Role of Static-to-Dynamic Disorder Transition
中文总结 AI 辅助
研究生物系统电荷传输，提出闪烁共振耦合熵主导电荷传输理论，用于计算转移速率和扩散迁移率，考虑动态无序相关简并对电子转移速率和扩散迁移率的影响，揭示超快动力学和简并情况下迁移率的转变。
中文摘要 AI 辅助
生物系统中的电荷传输因其在光生物学、生物能量学、氧化还原催化和其他代谢活动等各种功能活动中的作用而备受关注。各种研究观察到生物分子中动态无序的存在促进了中间传输区域的电荷动力学。此前，分子中动态无序对电荷传输的影响在测量从小范围到长程有序的分子电导率时尚未明确确立。在此动机下，我们提出了用于转移速率和基于扩散的迁移率计算的闪烁共振耦合熵主导电荷传输理论。所提出的分析形式主义纳入了动态无序相关简并对熵主导电子转移速率和扩散迁移率的影响，该影响以闪烁共振方式存在，适用于局域跳跃、离域能带传输以及两者之间的区域。通过这种方法，观察到动力学驱动的电子位点匹配概率增强了简并性，这由微分熵量化。分析清楚地表明，对于超快动力学和简并情况，熵主导迁移率转变为能带迁移率，而不是热激活跳跃或扩散过程。
英文摘要
Charge transport (CT) in biological systems is of great interest due to its role in various functional activities like photobiology, bioenergetics, redox catalytic and other metabolic activities, etc. It has been observed by various studies that the presence of a dynamic disorder in biomolecules facilitates charge dynamics in the intermediate transport regime, i.e., far from hopping and towards a bank-like mechanism. Hitherto, the dynamic disorder (in a time scale, coupling between electronic and nuclear dynamics) weightage on CT in molecules is not well-established for the measurement of molecular conductivity from small to long-range ordering. With this motivation, we propose the flickering resonance-coupled entropy-ruled charge transport theory for transfer-rate and diffusion-based mobility (D/μ) calculations. The proposed analytical formalism incorporates the impact of dynamic disorder-correlated degeneracy (in a flickering-resonance manner) on the entropy-ruled electron transfer rate and diffusion-mobility, which are valid for localized hopping, delocalized band transport, and regimes in between. By this approach, it has been observed that the dynamics-driven electronic site matching probability enhances the degeneracy, which is quantified by the differential entropy. The analysis clearly shows that for ultra-fast dynamical and degenerate cases, the entropy-ruled mobility is transformed as band mobility, rather than the thermally activated hopping or diffusion process.
