Lindsey Rebecca K, Fried Laurence E, Goldman Nir
Physical and Life Sciences Directorate , Lawrence Livermore National Laboratory , Livermore , California 94550 , United States.
Department of Chemical Engineering , University of California , Davis , California 95616 , United States.
J Chem Theory Comput. 2019 Jan 8;15(1):436-447. doi: 10.1021/acs.jctc.8b00831. Epub 2018 Dec 24.
We demonstrate development of the Chebyshev Interaction Model for Efficient Simulation (ChIMES) for molecular systems through application to water under ambient conditions (298 K, 1 g/cm). These models, which are comprised of linear combinations of Chebyshev polynomials explicitly describing two- and three-body interactions, are largely fit by force matching to Kohn-Sham Density Functional Theory (DFT). Protocols for selecting user-specified parameters and inclusion of stress tensor data are investigated, and structural and dynamical property prediction for resulting models is benchmarked against DFT. We show that the present ChIMES force fields yield excellent agreement with DFT without the need for additional terms such as those for Coulomb interactions. Overall, we show that tractable parametrization and subsequent accuracy of the present models make ChIMES an ideal candidate for extension of DFT dynamics to larger system sizes and longer time scales.
我们通过将其应用于环境条件（298 K，1 g/cm³）下的水，展示了用于分子系统的高效模拟切比雪夫相互作用模型（ChIMES）的开发。这些模型由明确描述两体和三体相互作用的切比雪夫多项式的线性组合组成，主要通过与科恩-沙姆密度泛函理论（DFT）进行力匹配来拟合。研究了选择用户指定参数和包含应力张量数据的协议，并将所得模型的结构和动力学性质预测与DFT进行了基准测试。我们表明，当前的ChIMES力场与DFT具有极好的一致性，无需诸如库仑相互作用之类的附加项。总体而言，我们表明，当前模型易于处理的参数化及其后续的准确性使ChIMES成为将DFT动力学扩展到更大系统规模和更长时间尺度的理想候选者。
