Construction of a Gaussian Process Regression Model of Formamide for Use in Molecular Simulations.
Construction of a Gaussian Process Regression Model of Formamide for Use in Molecular Simulations.
复制标题
DOI：
10.1021/acs.jpca.2c06566
复制
发表时间：
2023-02-23
影响因子：
2.9
通讯作者：
Skelton, Jonathan M.
中科院分区：
文献类型：
--
作者：
Popelier, Paul L. A.;Brown, Matthew L.;Skelton, Jonathan M.
FFLUX是一种基于量子化学拓扑结构的新型力场，可以使用随几何形状变化的柔性多极矩进行分子动力学模拟。这是通过高斯过程回归机器学习模型实现的，该模型可以准确地预测原子能量和多极矩，直到十六进制。我们在B3LYP/ augg -cc- pvtz水平上建立了甲酰胺单体的理论模型，其精度可达亚kJ mol-1，分子的最大预测误差为0.8 kJ mol-1。该模型与Lennard-Jones参数一起用于FFLUX模拟，成功地优化了甲酰胺二聚体的几何形状，与3d校正的B3LYP/ augg -cc- pvtz相比，误差小于0.1 Å。并与由静态多极矩和Lennard-Jones参数构成的力场进行了比较。与文献相比，FFLUX恢复了二聚体的预期能量排序，并且发现与氢键相关的C=O和C - n键长变化与密度泛函理论一致。
FFLUX, a novel force field based on quantum chemical topology, can perform molecular dynamics simulations with flexible multipole moments that change with geometry. This is enabled by Gaussian process regression machine learning models, which accurately predict atomic energies and multipole moments up to the hexadecapole. We have constructed a model of the formamide monomer at the B3LYP/aug-cc-pVTZ level of theory capable of sub-kJ mol–1 accuracy, with the maximum prediction error for the molecule being 0.8 kJ mol–1. This model was used in FFLUX simulations along with Lennard-Jones parameters to successfully optimize the geometry of formamide dimers with errors smaller than 0.1 Å compared to those obtained with D3-corrected B3LYP/aug-cc-pVTZ. Comparisons were also made to a force field constructed with static multipole moments and Lennard-Jones parameters. FFLUX recovers the expected energy ranking of dimers compared to the literature, and changes in C=O and C–N bond lengths associated with hydrogen bonding were found to be consistent with density functional theory.
登录
查看更多内容
影响因子：
2.9
作者：
Gora, RW;Grabowski, SJ;Leszczynski, J
通讯作者：
Leszczynski, J
影响因子：
2.9
作者：
Frey, Jann A.;Leutwyler, Samuel
通讯作者：
Leutwyler, Samuel
影响因子：
4.4
作者：
Cabaleiro-Lago, EM;Ríos, MA
通讯作者：
Ríos, MA
DOI：
10.1016/j.saa.2013.10.059
发表时间：
2015-02-05
影响因子：
4.4
作者：
Hughes, Timothy J.;Kandathil, Shaun M.;Popelier, Paul L. A.
通讯作者：
Popelier, Paul L. A.
影响因子：
4.4
作者：
ESSMANN, U;PERERA, L;PEDERSEN, LG
通讯作者：
PEDERSEN, LG