中文

Equivariant learning of a transferable three-dimensional classical density functional

统计力学 2026-08-13 v1 软凝聚态物质 机器学习 化学物理 计算物理

摘要

Liquids exhibit collective behavior that depends sensitively on thermodynamic conditions, interfaces and confinement, yet predicting each new state commonly requires a separate atomistic simulation. Classical density functional theory offers a reusable variational description, but its central excess free-energy functional is generally unknown, and learned approximations have largely remained restricted to planar or lower-dimensional settings. Here we show that this functional can be learned directly from fully three-dimensional equilibrium density fields while preserving spatial symmetry and variational consistency, without free-energy or chemical-potential labels. A single learned functional transfers across temperatures, system sizes and statistical ensembles, and recovers structure factors, the equation of state, liquid--vapor coexistence and interfacial broadening, none of which are used as training targets. Applied to complex three-dimensional geometries, it predicts the non-monotonic force associated with formation and rupture of a solvent-depleted bridge between colloids and adsorption in an interconnected gyroid pore. These results demonstrate that equilibrium density data can be converted into a transferable thermodynamic generator connecting microscopic liquid structure to response, phase behavior and collective phenomena.

引用

@article{arxiv.2608.13506,
  title  = {Equivariant learning of a transferable three-dimensional classical density functional},
  author = {Bingqing Cheng},
  journal= {arXiv preprint arXiv:2608.13506},
  year   = {2026}
}