通过自适应稀疏性提升哈密顿量预测效率,实现更快更准的分子计算。
Efficient and Scalable Density Functional Theory Hamiltonian Prediction through Adaptive Sparsity
- 引入自适应稀疏门,动态裁剪非关键相互作用,减少张量运算量。
- 在QH9和PubchemQH数据集上达到顶尖精度,速度提升最高达7倍。
- 适用于大分子系统与大规模基组,适合需要高效量子化学建模的研究者。
哈密顿量矩阵预测在计算化学中至关重要,是解析分子性质的基础。尽管SE(3)等变图神经网络在此领域表现优异,但其高阶张量积运算带来的巨大计算开销限制了其在大型分子系统和大基组下的可扩展性。为此,我们提出SPHNet,一种高效且可扩展的等变网络,将自适应稀疏性融入哈密顿量预测。SPHNet设计两种创新稀疏门,有选择地约束非关键相互作用组合,显著降低张量积计算量同时保持精度。为优化稀疏表示,我们开发三阶段稀疏调度器,确保稳定收敛,并在高达70%的稀疏率下实现高性能。在QH9和PubchemQH数据集上的广泛评估表明,SPHNet在保持最先进精度的同时,相较现有模型提速最高达7倍。该稀疏化技术亦可推广至其他SE(3)等变网络,进一步拓展其应用潜力。代码已开源:https://github.com/microsoft/SPHNet。
原文摘要 · Abstract (English)
Hamiltonian matrix prediction is pivotal in computational chemistry, serving as the foundation for determining a wide range of molecular properties. While SE(3) equivariant graph neural networks have achieved remarkable success in this domain, their substantial computational cost--driven by high-order tensor product (TP) operations--restricts their scalability to large molecular systems with extensive basis sets. To address this challenge, we introduce SPHNet, an efficient and scalable equivariant network, that incorporates adaptive SParsity into Hamiltonian prediction. SPHNet employs two innovative sparse gates to selectively constrain non-critical interaction combinations, significantly reducing tensor product computations while maintaining accuracy. To optimize the sparse representation, we develop a Three-phase Sparsity Scheduler, ensuring stable convergence and achieving high performance at sparsity rates of up to 70%. Extensive evaluations on QH9 and PubchemQH datasets demonstrate that SPHNet achieves state-of-the-art accuracy while providing up to a 7x speedup over existing models. Beyond Hamiltonian prediction, the proposed sparsification techniques also hold significant potential for improving the efficiency and scalability of other SE(3) equivariant networks, further broadening their applicability and impact. Our code can be found at https://github.com/microsoft/SPHNet.
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