精确的氦-苯烯势能面：从CCSD(T)到高斯过程回归
Accurate Helium-Benzene Potential: from CCSD(T) to Gaussian Process Regression
AI总结：
本文通过多级方法构建了精确的氦-苯烯势能面，结合高斯过程回归与密度泛函理论结果，实现了亚厘米-1精度的连续三维势能面，用于研究低温下氦原子在苯上的溶剂化行为。
摘要：
准确建模氦与石墨材料之间的非共价相互作用对于理解二维量子现象至关重要，氦-苯烯复合作为基本原型。然而，为这种弱束缚系统创建量上可靠势能面（PES）仍是一个重大计算挑战。本文通过高阶耦合簇单双激发（CCSD(T)）方法外推到完全基组极限，结合对称适应微扰理论（SAPT）验证了相互作用由色散和交换排斥的平衡主导。通过多保真度高斯过程回归构建了连续三维PES，结合密度泛函理论结果与稀疏耦合簇能量。结果是一个亚厘米-1精度的PES，符合物理定律。该新PES用于路径积分蒙特卡罗（PIMC）模拟研究低温下氦原子在苯上的溶剂化行为。PIMC结果揭示了与常用经验Lennard-Jones势模拟相比，溶剂化行为有显著差异，特别是吸附层填充行为。本文提供了用于更准确模拟氦在更大多环芳烃向石墨方向的多体模拟的基准PES。
英文摘要：
The accurate modeling of non-covalent interactions between helium and graphitic materials is important for understanding quantum phenomena in reduced dimensions, with the helium-benzene complex serving as the fundamental prototype. However, creating a quantitatively reliable potential energy surface (PES) for this weakly bound system remains a significant computational challenge. In this work, we present a comprehensive, multi-level investigation of the He-Bz interaction, establishing benchmark energies using high-level coupled-cluster singles-and-doubles with perturbative triples (CCSD(T)) methods extrapolated to the complete basis set limit and assessing higher-order (CCSDT(Q)) contributions. We use symmetry-adapted perturbation theory (SAPT) to benchmark it against CCSD(T) and to decompose the interaction into its physical components-confirming it is dominated by a balance between dispersion and exchange-repulsion. A continuous, three-dimensional PES is constructed from discrete ab initio points using multifidelity Gaussian process regression that combines density functional theory results with sparse coupled-cluster energies. The result is a highly accurate PES with sub-cm-1 accuracy that obeys physical laws. This new PES is applied to path integral Monte Carlo (PIMC) simulations to study the solvation of 4He atoms on benzene at low temperatures. Our PIMC results reveal qualitatively different solvation behavior, particularly in the filling of adsorption layers, when compared to simulations using commonly employed empirical Lennard-Jones potentials. This work provides a benchmark PES essential for accurate many-body simulations of helium on larger polycyclic aromatic hydrocarbons towards graphene.
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