The quantum mechanics-based polarizable force field for water simulations.
The quantum mechanics-based polarizable force field for water simulations.
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用于水模拟的基于量子力学的极化力场。
DOI：
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发表时间：
2018
影响因子：
4.4
通讯作者：
W. Goddard
中科院分区：
文献类型：
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作者：
Saber Naserifar;W. Goddard
我们在这里报道了一种新的水的力场，完全基于量子力学(QM)计算，没有经验数据。用X3LYP密度泛函理论(DFT)计算了19个较大的水团簇，在所有取向和距离下，QM都处于较高水平，耦合团簇为单双三元。此外，我们还包括了基于极化电荷平衡法的电荷和极化，以及用DFT-D3方法计算的H2和O2晶体上的非键相互作用。该模型与水的固相和液态实验(Expr)数据符合得很好：T熔体=273.3 K(Expr=273.15 K)，298K时的性质：ΔH VAP=10.36kcal/mo1(Expr=10.52)，密度=0.9965 gr/cm~3(Expr=0.9965)，熵=68.4J/m o l/K(Expr=69.9)，介电常数=76.1(Expr=78.4)，和ln D S(自扩散系数)=-10.08(指数=-11.24)。我们相信，水的这种准确的力场将有助于电催化的全溶剂计算，在这种计算中，我们可以将QM水限制在涉及反应的前一层或两层，使用RexPoN为更远的溶剂提供极化。此外，RexPoN可以更好地描述蛋白质、DNA、聚合物和无机体系的溶剂，这些体系应用于生物分子、制药、电催化(燃料电池和水分解)和电池，其中与显性水分子的相互作用起着重要作用。
We report here a new force field for water based solely on quantum mechanics (QM) calculations with no empirical data. The QM was at a high level, coupled cluster single double triple, for all orientations and distances for water dimer plus X3LYP density functional theory (DFT) on 19 larger water clusters. In addition, we included charge and polarization based on the polarizable charge equilibration method and nonbond interactions from DFT-D3 calculations on the H2 and O2 crystal. This model, denoted as RexPoN, provides quite excellent agreement with experimental (expr) data for the solid and liquid phase of water: T melt = 273.3 K (expr = 273.15 K) and properties at 298 K: ΔH vap = 10.36 kcal/mol (expr = 10.52), density = 0.9965 gr/cm3 (expr = 0.9965), entropy = 68.4 (J/mol)/K (expr = 69.9), dielectric constant = 76.1 (expr = 78.4), and ln D s (self-diffusion coef) = -10.08 (expr = -11.24). Such an accurate force field for water will, we believe, be useful for full solvent calculations of electrocatalysis, where we can restrict QM water to just the first one or two layers involving reactions, using RexPoN to provide the polarization for a more distant solvent. Also, RexPoN may provide a better description of the solvent for proteins, DNA, polymers, and inorganic systems for applications to biomolecular, pharma, electrocatalysis (fuel cells and water splitting), and batteries where interaction with explicit water molecules plays a significant role.
影响因子：
4.4
作者：
Habershon, Scott;Markland, Thomas E.;Manolopoulos, David E.
通讯作者：
Manolopoulos, David E.