arXiv:2603.04523physics.chem-phcs.AI2026-03被引 3

用随机投影加速训练,让机器学习势能模型更准地捕捉能量曲率。

Projected Hessian Learning: Fast Curvature Supervision for Accurate Machine-Learning Interatomic Potentials

  • 通过随机方向的海森向量积,间接获取曲率信息
  • 相比完整海森矩阵,训练速度提升24倍以上
  • 适合大分子系统,尤其在非平衡构型下表现更优

海森矩阵(二阶导数)比能量和力蕴含更丰富的势能面局部曲率信息。然而,显式构建和存储海森矩阵会带来二次方量级的计算与内存开销,通常不切实际。本文提出投影海森学习(PHL),一种可扩展的二阶训练框架,仅通过海森向量积(HVP)注入曲率信息。PHL不构造海森矩阵,而是沿随机探测方向投影曲率,并采用无偏的随机迹损失,具有优异的系统规模缩放性,实现无需二次内存增长的曲率感知训练。我们在涵盖反应物、产物、过渡态、内禀反应坐标及正常模采样几何的化学多样性数据集上进行基准测试,使用omegaB97XD/6-31G(d)方法生成。对比了能量-力训练(E-F)、两种基于HVP的方案(单列或随机探测),以及完整能量-力-海森训练(E-F-H)。在每批随机探测的设置下,两种HVP方案在能量、力和海森精度上均达到全海森训练水平,且对小分子系统实现超过24倍的单周期加速。固定探测模式下(每分子一个HVP),随机投影始终优于单列探测,尤其在远离平衡构型时表现更佳。总体而言,PHL以力复杂度的代价替代显式海森监督,保留大部分二阶精度优势,同时可扩展至更大更复杂的分子体系。

原文摘要 · Abstract (English)

The Hessian matrix (second derivatives) encodes far richer local curvature of the potential energy surface than energies and forces alone. However, training machine-learning interatomic potentials (MLIPs) with full Hessians is often impractical because explicitly forming and storing Hessian matrices scales quadratically in cost and memory. We introduce Projected Hessian Learning (PHL), a scalable second-order training framework that injects curvature information using only Hessian-vector products (HVPs). Rather than constructing the Hessian, PHL projects curvature along stochastic probe directions and uses an unbiased stochastic trace-based loss with favorable system-size scaling, enabling curvature-informed training without quadratic memory growth. We benchmark PHL on a chemically diverse dataset of reactants, products, transition states, intrinsic reaction coordinates, and normal-mode sampled geometries computed at omegaB97XD/6-31G(d). We compare energy-force training (E-F), two HVP-based schemes (E-F-HVP with one-hot or randomized probes), and full energy-force-Hessian training (E-F-H). With randomized probes per minibatch, both HVP schemes match full-Hessian training in energy, force, and Hessian accuracy while delivering >24x epoch speedups for the small molecular systems studied. In a fixed-probe regime with one HVP per molecule, randomized projections consistently outperform one-column probing, especially for far-from-equilibrium geometries. Overall, PHL replaces explicit Hessian supervision with force-complexity curvature training, retaining most second-order accuracy gains while scaling to larger, more complex molecular systems.

机器学习势能曲率学习高效训练分子模拟

Thank you to arXiv for use of its open access interoperability. PaperDance 不是 arXiv 官方产品;中文卡片由大模型生成,请以原文为准。