Empirical bond-order potential for hydrocarbons: Adaptive treatment of van der Waals interactions
Empirical bond-order potential for hydrocarbons: Adaptive treatment of van der Waals interactions
复制标题
DOI：
10.1002/jcc.20817
复制
发表时间：
2008-03-01
影响因子：
3
通讯作者：
Stuart, Steven J.
中科院分区：
文献类型：
--
作者：
Liu, Aining;Stuart, Steven J.
键序势为模拟具有经典势的化学反应系统提供了一类强大的模型。在这些模型中，共价键相互作用适应环境，允许键强度随局部化学变化而变化。然而，非键相互作用也应该适应化学变化，这在当前的键序势中被忽略了。在这里，airbo势被扩展到包括自适应Lennard-Jones项，允许范德华相互作用随化学环境自适应地变化。由此产生的势能面及其梯度保持连续，允许它用于动力学模拟。这一新势对烃类进行了参数化，并适用于各种缩合相分子烃类的能量学和密度。该模型对芳烃和其他不饱和烃的模拟更为准确，而原始的AIREBO势在这方面存在一定的不足。对拟合过程中未使用的化合物的测试表明，新模型在预测冷凝相分子碳氢化合物的汽化热和压力（或密度）方面表现得更好。(c) 2007 Wiley期刊公司
Bond-order potentials provide a powerful class of models for simulating chemically reactive systems with classical potentials. In these models, the covalent bonding interactions adapt to the environment, allowing bond strength to change in response to local chemical changes. However, the non-bonded interactions should also adapt in response to chemical changes, an effect which is neglected in current bond-order potentials. Here the AIREBO potential is extended to include adaptive Lennard-Jones terms, allowing the van der Waals interactions to vary adaptively with the chemical environment. The resulting potential energy surface and its gradient remain continuous, allowing it to be used for dynamics simulations. This new potential is parameterized for hydrocarbons, and is fit to the energetics and densities of a variety of condensed phase molecular hydrocarbons. The resulting model is more accurate for modeling aromatic and other unsaturated hydrocarbon species, for which the original AIREBO potential had some deficiencies. Testing on compounds not used in the fitting procedure shows that the new model performs substantially better in predicting heats of vaporization and pressures (or densities) of condensed-phase molecular hydrocarbons. (c) 2007 Wiley Periodicals, Inc.