Proton transfer in bulk water using the full adaptive QM/MM method: integration of solute- and solvent-adaptive approaches
Proton transfer in bulk water using the full adaptive QM/MM method: integration of solute- and solvent-adaptive approaches
复制标题
使用完全自适应 QM/MM 方法在散装水中进行质子转移：溶质和溶剂自适应方法的集成
DOI：
10.1039/d1cp00116g
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发表时间：
2021
影响因子：
3.3
通讯作者：
Yohichi Suzuki
中科院分区：
文献类型：
--
作者：
Hiroshi C. Watanabe; Masayuki Yamada;Yohichi Suzuki
量子力学/分子力学（QM/MM）方法是一种混合的分子模拟技术，增加了大系统的局部电子结构的可及性。该技术结合了QM方法中的精度和MM方法中的成本效率的优点。然而，很难直接应用QM/MM方法的溶液系统的动力学，特别是质子转移。正如Grotthuss机制中所解释的，质子转移是水合氢离子和溶剂水分子之间的结构相互转化。因此，当应用QM/MM方法时，需要对溶质和溶剂进行自适应处理，即对分子定义进行即时修订。虽然已经提出了几种溶剂自适应方法，但一个完整的自适应框架，这是一种也考虑溶质自适应的方法，仍未开发。本文提出了一种新的过剩质子坐标的数值表达式及其控制算法。此外，我们证实，该方法可以稳定，准确地模拟质子在体水中的转移动力学。
The quantum mechanical/molecular mechanical (QM/MM) method is a hybrid molecular simulation technique that increases the accessibility of local electronic structures of large systems. The technique combines the benefit of accuracy found in the QM method and that of cost efficiency found in the MM method. However, it is difficult to directly apply the QM/MM method to the dynamics of solution systems, particularly for proton transfer. As explained in the Grotthuss mechanism, proton transfer is a structural interconversion between hydronium ions and solvent water molecules. Hence, when the QM/MM method is applied, an adaptive treatment, namely on-the-fly revisions on molecular definitions, is required for both the solute and solvent. Although several solvent-adaptive methods have been proposed, a full adaptive framework, which is an approach that also considers adaptation for solutes, remains untapped. In this paper, we propose a new numerical expression for the coordinates of the excess proton and its control algorithm. Furthermore, we confirm that this method can stably and accurately simulate proton transfer dynamics in bulk water.