Ultrafast Structural Changes Decomposed from Serial Crystallographic Data.
Ultrafast Structural Changes Decomposed from Serial Crystallographic Data.
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从连续晶体学数据分解的超快结构变化。
DOI：
10.1021/acs.jpclett.9b02375
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发表时间：
2019
期刊：
影响因子：
--
通讯作者：
Ren,Zhong
中科院分区：
文献类型：
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作者：
Ren,Zhong
生化反应过程中电子和分子事件的直接可视化对于机械洞察至关重要。这封信对 Barends 和 Schlichting 等人收集的系列晶体学数据集进行了深入分析。 (Science2015, 350, 445) 探测碳单氧肌红蛋白中的配体光解离。该分析揭示了光解时血红素铁的高自旋 3d 原子轨道的形成引起的电子密度变化及其在最初几皮秒内的动态行为。发现血红素铁连续从血红素平面弹出并弹回血红素平面。这些发现为之前使用超快光谱和分子动力学模拟的工作提供了期待已久的视觉验证。在低频振荡的第一个周期期间，在溶剂中也发现了很大的电子密度变化。这项工作证明了分析方法在检测和隔离化学反应产生的电子变化的微弱瞬态信号方面的重要性。
Direct visualization of electronic and molecular events during biochemical reactions is essential to mechanistic insights. This Letter presents an in-depth analysis of the serial crystallographic data sets collected by Barends and Schlichting et al. (Science2015, 350, 445) that probe the ligand photodissociation in carbonmonoxy myoglobin. This analysis reveals electron density changes caused by the formation of high-spin 3d atomic orbitals of the heme iron upon photolysis and their dynamic behaviors within the first few picoseconds. The heme iron is found popping out of and recoiling back into the heme plane in succession. These findings provide long-awaited visual validations for previous works using ultrafast spectroscopy and molecular dynamics simulations. Electron density variations are also found largely in the solvent during the first period of a low-frequency oscillation. This work demonstrates the importance of the analytical methods in detecting and isolating weak, transient signals of electronic changes arising from chemical reactions.