论文标题

Deepks+算作为昂贵的量子机械模型与机器学习潜力之间的桥梁

DeePKS+ABACUS as a Bridge between Expensive Quantum Mechanical Models and Machine Learning Potentials

论文作者

Li, Wenfei, Ou, Qi, Chen, Yixiao, Cao, Yu, Liu, Renxi, Zhang, Chunyi, Zheng, Daye, Cai, Chun, Wu, Xifan, Wang, Han, Chen, Mohan, Zhang, Linfeng

论文摘要

最近,机器学习(ML)电位的发展使得以量子力学(QM)模型的准确性进行大规模和长时间的分子模拟成为可能。但是,对于高水平的QM方法,例如在元gga级别和/或具有精确交换的密度功能理论(DFT),量子蒙特卡洛等,生成了足够数量的数据以训练ML潜在的培训由于其高成本而在计算上仍然具有挑战性。在这项工作中,我们证明了基于ML的DFT模型Deep Kohn-Sham(Deepks)可以在很大程度上缓解这个问题。 Deepks采用计算高效的基于神经网络的功能模型来构建在廉价DFT模型上添加的校正项。在训练后,DeepKs提供了与高级QM方法相比,具有紧密匹配的能量和力,但是所需的训练数据的数量是比训练可靠的ML潜力所需的数量级要小。因此,DeepKs可以用作昂贵的QM型号和ML电位之间的桥梁:一个人可以生成大量的高准确性QM数据来训练DeepKs模型,然后使用DeepKs型号来标记大量的配置来训练ML电位。该周期系统方案是在DFT软件包算盘中实现的,该计划是开源的,可以在各种应用程序中使用。

Recently, the development of machine learning (ML) potentials has made it possible to perform large-scale and long-time molecular simulations with the accuracy of quantum mechanical (QM) models. However, for high-level QM methods, such as density functional theory (DFT) at the meta-GGA level and/or with exact exchange, quantum Monte Carlo, etc., generating a sufficient amount of data for training a ML potential has remained computationally challenging due to their high cost. In this work, we demonstrate that this issue can be largely alleviated with Deep Kohn-Sham (DeePKS), a ML-based DFT model. DeePKS employs a computationally efficient neural network-based functional model to construct a correction term added upon a cheap DFT model. Upon training, DeePKS offers closely-matched energies and forces compared with high-level QM method, but the number of training data required is orders of magnitude less than that required for training a reliable ML potential. As such, DeePKS can serve as a bridge between expensive QM models and ML potentials: one can generate a decent amount of high-accuracy QM data to train a DeePKS model, and then use the DeePKS model to label a much larger amount of configurations to train a ML potential. This scheme for periodic systems is implemented in a DFT package ABACUS, which is open-source and ready for use in various applications.

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