质体蓝素的玻璃化蛋白动力学和巨大的溶剂重组能
Glassy protein dynamics and gigantic solvent reorganization energy of plastocyanin
摘要：
报道了天然光合作用中作为电子载体的质体蓝素金属蛋白的电子传递活化参数的分子动力学模拟结果。我们已经发现，缓慢的，非遍历的构象波动的蛋白质，再加上水合水，导致在一个非常广泛的分布供体-受体能隙远远超过所观察到的通常研究的无机和有机供体-受体复合物。斯托克斯位移不受这些波动的影响，可以从溶剂化模型中计算的溶剂偶极极化的响应。大幅度蛋白质/水流动性的非遍历特征打破了电子转移的平衡（遍历）理论的斯托克斯位移和重组能量特征之间的强联系。这种机制可能是负责低活化屏障的天然电子转移蛋白质的特点是低反应自由能。
英文摘要：
We report the results of Molecular Dynamics simulations of electron transfer activation parameters of plastocyanin metalloprotein involved as electron carrier in natural photosynthesis. We have discovered that slow, non-ergodic conformational fluctuations of the protein, coupled to hydrating water, result in a very broad distribution of donor-acceptor energy gaps far exceeding that observed for commonly studied inorganic and organic donor-acceptor complexes. The Stokes shift is not affected by these fluctuations and can be calculated from solvation models in terms of the response of the solvent dipolar polarization. The non-ergodic character of large-amplitude protein/water mobility breaks the strong link between the Stokes shift and reorganization energy characteristic of equilibrium (ergodic) theories of electron transfer. This mechanism might be responsible for low activation barriers in natural electron transfer proteins characterized by low reaction free energy.
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