光合蛋白复合体的高压孔燃烧转运动力学研究

G. Small, N. Reddy, R. Jankowiak
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引用次数: 0

摘要

空穴燃烧光谱已被证明是阐明光合作用蛋白质-叶绿素复合物的激发态(Qy)电子结构和输运(能量、电荷)动力学的有力工具。1-3此外,孔燃烧已经证明这种配合物在微观尺度上是玻璃状的,这导致Qy←S0 Chi吸收跃迁的非均匀加宽~50-150 cm-1 (ΓI)。重要的是,研究还表明,同一配合物的不同qy态的零声子线(ZPL)频率分布函数是不相关的,这意味着与能量和电子转移相关的能隙分布函数的宽度为~21/2 ΓI。这就提出了一种可能性,即运输动力学可能是分散的它们是否存在取决于与输运过程相关的电子-声子耦合的强度。幸运的是,孔烧已被证明能够表征这种耦合的性质和强度。需要发展适用于低温极限下任意强电子-声子耦合的整个空穴轮廓(零声子空穴[ZPH] +声子边带空穴)的精确理论。最近,这一理论已被推广到任意温度关键的一点是,ZPH只是整个配置文件的一小部分。对于光合单位的输运动力学问题来说,整个孔的轮廓是重要的。因此,单分子(复合体)检测对能量和电子转移问题的影响不大。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
High Pressure Hole-Burning Studies of Transport Dynamics in Photosynthetic Protein Complex
Hole burning spectroscopies have proven to be powerful tools for the elucidation of the excited state (Qy) electronic structure and transport (energy, charge) dynamics of photosynthetic protein-chlorophyll complexes.1-3 Furthermore, hole burning has proven that such complexes are glass-like on a microscopic scale, which results in inhomogeneous broadenings of ~50-150 cm-1 (ΓI) for the Qy←S0 Chi absorption transitions. Importantly, it has also been shown that the zero-phonon line (ZPL) frequency distribution functions for different Qy-states of the same complex are uncorrelated, meaning that the widths of the distribution functions for energy gaps relevant to energy and electron transfer are ~21/2 ΓI. This raises the possibility that the kinetics for transport could be dispersive.4 Whether or not they are turns out to be dependent on the .strength of the electron-phonon coupling associated with the transport process. Fortunately, hole burning has proven to be capable of characterizing the nature and strength of this coupling. Required was the development of an accurate theory for entire hole profile (zero-phonon hole [ZPH] plus phonon sideband holes) applicable for arbitrarily strong electron-phonon coupling in the low temperature limit. More recently, this theory5 has been extended to arbitrary temperature.6 A key point is that the ZPH is only one small part of the entire profile. It is the entire hole profile that is important to the problem of transport dynamics in the photosynthetic unit. Thus it is that single molecule (complex) detection would be of little consequence to the problem of energy and electron transfer.
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