发表机构
Center for Advanced Systems Understanding (CASUS); Helmholtz-Zentrum Dresden-Rossendorf (HZDR); Microsoft Research AI for Science; Department of Chemistry, University of Zurich; Institute of Artificial Intelligence, Technische Universität Dresden（高级系统理解中心; 德累斯顿-罗斯多夫亥姆霍兹中心; 微软研究院科学人工智能; 苏黎世大学化学系; 德累斯顿工业大学人工智能研究所）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究通过GauXC在CP2K中实现了机器学习的Skala交换-关联泛函的分子级应用，经dietGMTKN55基准验证，其总平均绝对偏差与参考值偏差极小，实现了可靠的泛函计算接口。
AI 中文摘要
机器学习的交换-关联（XC）泛函为改进Kohn-Sham密度泛函理论提供了途径，且不会产生显式关联电子结构方法的成本。然而，将其应用于生产模拟代码需要在学习模型与宿主代码的密度表示之间建立明确定义的映射。我们通过外部GauXC库在CP2K中构建并实现了Skala-1.1接口。CP2K提供几何结构、高斯基组、自旋分辨的原子轨道密度矩阵以及通信器，而GauXC则计算XC能量、原子轨道势矩阵和可用的核导数。该接口接受全电子和仅价电子两种密度矩阵，后者可源自可分离双空间赝势或分子有效芯势。通过比较经GauXC评估的Perdew-Burke-Ernzerhof（PBE）泛函与原生CP2K的PBE，可将实现误差与泛函差异隔离开。该接口针对代表性分子案例给出了一致的能量、经有限差分总能检查验证的力，以及基于力的分子-维里诊断结果。我们使用dietGMTKN55基准套件进行评估，其中对溴及之前的元素采用全电子高斯增广平面波处理，对更重元素采用def2有效芯势，得到的总平均绝对偏差为1.255 kcal/mol，与对应的Skala参考值1.235 kcal/mol的偏差在0.020 kcal/mol以内。本研究在CP2K中通过GauXC建立了经验证的Skala泛函分子级实现。
英文摘要
Machine-learned exchange--correlation (XC) functionals offer a route to improve Kohn--Sham density-functional theory without incurring the cost of explicitly correlated electronic-structure methods. Their use in production simulation codes, however, requires a well-defined mapping between the learned model and the host-code density representation. We formulate and implement a Skala-1.1 interface in CP2K through the external GauXC library. CP2K supplies the geometry, Gaussian basis, spin-resolved atomic-orbital density matrix, and communicator, while GauXC evaluates the XC energy, atomic-orbital potential matrix, and available nuclear derivatives. The interface accepts both all-electron and valence-only density matrices. The latter may arise from separable dual-space pseudopotentials or molecular effective-core potentials. Implementation errors are isolated from functional differences by comparing the Perdew--Burke--Ernzerhof (PBE) functional evaluated through GauXC with native CP2K PBE. The resulting interface gives consistent energies, forces validated against finite-difference total-energy checks, and force-based molecular-virial diagnostics for representative molecular cases. The dietGMTKN55 benchmark suite is evaluated with an all-electron Gaussian augmented plane-wave treatment for elements up to bromine and def2 effective-core potentials for the heavier elements. The resulting aggregate mean absolute deviation of 1.255 kcal/mol is within 0.012 kcal/mol of the corresponding Skala reference value of 1.243 kcal/mol. This work establishes a validated molecular implementation of Skala in CP2K through GauXC.
Comments16 pages including Supplementary Information. Revised benchmark comparison and AI-assistance declaration
