Targeted Transferable Machine-Learned Potential for Linear Alkanes Trained on C(14)H(30) and Tested for C(4)H(10) to C(30)H(62)

基于 C(14)H(30) 训练的线性烷烃目标可迁移机器学习势能函数,以及基于 C(4)H(10) 至 C(30)H(62) 测试的线性烷烃目标可迁移机器学习势能函数

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Abstract

Given the great importance of linear alkanes in fundamental and applied research, an accurate machine-learned potential (MLP) would be a major advance in computational modeling of these hydrocarbons. Recently, we reported a novel, many-body permutationally invariant model that was trained specifically for the 44-atom hydrocarbon C(14)H(30) on roughly 250,000 B3LYP energies (Qu, C.; Houston, P. L.; Allison, T.; Schneider, B. I.; Bowman, J. M. J. Chem. Theory Comput. 2024, 20, 9339-9353). Here, we demonstrate the accuracy of the transferability of this potential for linear alkanes ranging from butane C(4)H(10) up to C(30)H(62). Unlike other approaches for transferability that aim for universal applicability, the present approach is targeted for linear alkanes. The mean absolute error (MAE) for energy ranges from 0.26 kcal/mol for butane and rises to 0.73 kcal/mol for C(30)H(62) over the energy range up to 80 kcal/mol for butane and 600 kcal/mol for C(30)H(62). These values are unprecedented for transferable potentials and indicate the high performance of a targeted transferable potential. The conformational barriers are shown to be in excellent agreement with high-level ab initio calculations for pentane, the largest alkane for which such calculations have been reported. Vibrational power spectra of C(30)H(62) from molecular dynamics calculations are presented and briefly discussed. Finally, the evaluation time for the potential is shown to vary linearly with the number of atoms.

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