Molecular structure and free energy landscape for electron transport in the decahaem cytochrome MtrF
Molecular structure and free energy landscape for electron transport in the decahaem cytochrome MtrF
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DOI：
10.1042/bst20120139
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发表时间：
2012-12-01
影响因子：
3.9
通讯作者：
Rosso, Kevin M.
中科院分区：
文献类型：
--
作者：
Breuer, Marian;Zarzycki, Piotr;Rosso, Kevin M.
利用热力学积分和经典分子动力学方法计算了细菌十血红素细胞色素MtrF中电子流的自由能分布。对两个版本的结构进行的广泛计算有助于验证方法和结果，因为图谱中的差异可能与特定血红素组局部带电氨基酸的差异有关。重组自由能λ的第一次估计产生的范围与部分溶剂暴露的辅因子的预期一致，并揭示了一个活化能范围可克服的电子流。未来的工作将致力于提高可极化力场动力学和量子化学能隙计算，以及电子耦合矩阵元素的量子化学计算的λ的准确性。
The free energy profile for electron flow through the bacterial decahaem cytochrome MtrF has been computed using thermodynamic integration and classical molecular dynamics. The extensive calculations on two versions of the structure help to validate the method and results, because differences in the profiles can be related to differences in the charged amino acids local to specific haem groups. First estimates of reorganization free energies lambda yield a range consistent with expectations for partially solvent-exposed cofactors, and reveal an activation energy range surmountable for electron flow. Future work will aim at increasing the accuracy of lambda with polarizable forcefield dynamics and quantum chemical energy gap calculations, as well as quantum chemical computation of electronic coupling matrix elements.