Fenna-Matthews-Olson复合体的约束几何动力学：相关运动在减少激发能量转移中的不确定性中的作用
Constrained geometric dynamics of the Fenna-Matthews-Olson complex: The role of correlated motion in reducing uncertainty in excitation energy transfer
摘要：
绿硫细菌的Fenna Mathews Olson（FMO）复合物是光合色素蛋白质复合物的一个例子，其中色素的电子性质被蛋白质环境改变以促进从天线复合物到反应中心的有效激子能量转移。FMO络合物的许多电子性质可以从静态晶体结构的知识中提取。然而，最近对FMO复合体中持久量子动力学的观察和分析表明，蛋白质动力学是在实验室条件下保护和产生量子相干性的关键因素。虽然快速的分子间和分子内的振动已被广泛研究，慢动力学，有效地确定光学非均匀加宽的实验合奏得到较少的关注。我们的研究采用约束几何动力学研究蛋白质网络的灵活性，有效地产生可访问的构象状态从公布的晶体结构。统计和主成分分析揭示了功能相关元素之间的高度相关的低频运动，包括激子耦合的颜料之间的强相关性。我们的分析揭示了一个层次的结构相互作用，执行这些相关的运动，从单体单体接口的水平下降到α螺旋，β片层和颜料。除了诱导强的空间相关性的构象合奏，我们发现，整体刚性的FMO复杂的是非常高的。我们认为，这些观察结果支持的想法，高度相关的非均匀无序的电子激发态，这是进一步支持的构象合奏的激子耦合的显着低方差。
英文摘要：
The Fenna Mathews Olson (FMO) complex of green sulphur bacteria is an example of a photosynthetic pigment protein complex, in which the electronic properties of the pigments are modified by the protein environment to promote efficient excitonic energy transfer from antenna complexes to the reaction centres. Many of the electronic properties of the FMO complex can be extracted from knowledge of the static crystal structure. However, the recent observation and analysis of long lasting quantum dynamics in the FMO complex point to protein dynamics as a key factor in protecting and generating quantum coherence under laboratory conditions. While fast inter and intra molecular vibrations have been investigated extensively, the slow dynamics which effectively determine the optical inhomogeneous broadening of experimental ensembles has received less attention. Our study employs constrained geometric dynamics to study the flexibility in the protein network by efficiently generating the accessible conformational states from the published crystal structure. Statistical and principle component analysis reveal highly correlated low frequency motions between functionally relevant elements, including strong correlations between pigments that are excitonically coupled. Our analysis reveals a hierarchy of structural interactions which enforce these correlated motions, from the level of monomer monomer interfaces right down to the alpha helices, beta sheets and pigments. In addition to inducing strong spatial correlations across the conformational ensemble, we find that the overall rigidity of the FMO complex is exceptionally high. We suggest that these observations support the idea of highly correlated inhomogeneous disorder of the electronic excited states, which is further supported by the remarkably low variance of the excitonic couplings of the conformational ensemble.
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