arXiv:2410.11391physics.chem-phcs.LG2024-10

提出新型多保真度Δ-机器学习模型,显著降低量子化学预测的数据成本。

Benchmarking Data Efficiency in $Δ$-ML and Multifidelity Models for Quantum Chemistry

  • 融合多保真度数据与Δ-机器学习思想,构建新模型MFΔML
  • 在大量预测任务中,比传统Δ-ML和多保真度方法更省数据
  • 适合需要高精度且数据昂贵的量子化学计算场景

机器学习方法降低了量子化学计算的算力需求,但训练数据生成成本上升。为此发展出Δ-机器学习(Δ-ML)和多保真度机器学习(MFML)方法,利用不同精度级别的数据。本文在多保真度基准数据集QeMFi上,对比了Δ-ML、MFML、优化版MFML(o-MFML)与新提出的多保真度Δ-机器学习(MFΔML)方法在基态能量、垂直激发能及电子偶极矩贡献量预测上的数据成本。评估基于各模型的训练数据生成开销,并与单保真度核岭回归(KRR)对比。结果表明,在大量预测任务中,多保真度方法优于标准Δ-ML;而在少量评估场景下,MFΔML展现出更高效率。

原文摘要 · Abstract (English)

The development of machine learning (ML) methods has made quantum chemistry (QC) calculations more accessible by reducing the compute cost incurred in conventional QC methods. This has since been translated into the overhead cost of generating training data. Increased work in reducing the cost of generating training data resulted in the development of $Δ$-ML and multifidelity machine learning methods which use data at more than one QC level of accuracy, or fidelity. This work compares the data costs associated with $Δ$-ML, multifidelity machine learning (MFML), and optimized MFML (o-MFML) in contrast with a newly introduced Multifidelity$Δ$-Machine Learning (MF$Δ$ML) method for the prediction of ground state energies, vertical excitation energies, and the magnitude of electronic contribution of molecular dipole moments from the multifidelity benchmark dataset QeMFi. This assessment is made on the basis of training data generation cost associated with each model and is compared with the single fidelity kernel ridge regression (KRR) case. The results indicate that the use of multifidelity methods surpasses the standard $Δ$-ML approaches in cases of a large number of predictions. For applications which require only a few evaluations to be made using ML models, while the $Δ$-ML method might be favored, the MF$Δ$ML method is shown to be more efficient.

量子化学多保真度数据效率机器学习

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