Calculation of Linear and Non-linear Electric Response Properties of Systems in Aqueous Solution: A Polarizable Quantum/Classical Approach with Quantum Repulsion Effects.
Calculation of Linear and Non-linear Electric Response Properties of Systems in Aqueous Solution: A Polarizable Quantum/Classical Approach with Quantum Repulsion Effects.
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DOI：
10.1021/acs.jctc.0c00674
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发表时间：
2020-11-10
影响因子：
5.5
通讯作者：
Cappelli C
中科院分区：
文献类型：
--
作者：
Marrazzini G;Giovannini T;Egidi F;Cappelli C
我们提出了一个计算研究的极化率和超极化率的有机分子在水溶液中，专注于溶质-水的相互作用和它们影响分子的线性和非线性电响应特性的方式。我们采用极化量子力学/分子力学（QM/MM）的计算模型，处理的溶质在QM水平，而溶剂处理经典使用力场，包括极化电荷和偶极子，动态响应溶质的量子力学电子密度。量子限制效应也被处理的装置最近实施的方法，赋予溶剂分子的参数电子密度，施加泡利排斥力的溶质。通过将该方法应用于一组芳香族分子在溶液中，我们表明，极化率和第一超极化率，观察到的溶液值是静电，氢键，和非静电溶质溶剂相互作用之间的微妙平衡的结果。
We present a computational study of polarizabilities and hyperpolarizabilities of organic molecules in aqueous solutions, focusing on solute–water interactions and the way they affect a molecule’s linear and non-linear electric response properties. We employ a polarizable quantum mechanics/molecular mechanics (QM/MM) computational model that treats the solute at the QM level while the solvent is treated classically using a force field that includes polarizable charges and dipoles, which dynamically respond to the solute’s quantum-mechanical electron density. Quantum confinement effects are also treated by means of a recently implemented method that endows solvent molecules with a parametric electron density, which exerts Pauli repulsion forces upon the solute. By applying the method to a set of aromatic molecules in solution we show that, for both polarizabilities and first hyperpolarizabilities, observed solution values are the result of a delicate balance between electrostatics, hydrogen-bonding, and non-electrostatic solute solvent interactions.
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影响因子：
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作者：
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