基于相图的李-杨理论引导力场优化
Lee-Yang Theory Guided Force Field Refinement Based on Phase Diagrams
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中文总结 AI 辅助
该研究提出基于李-杨相变理论的力场优化通用框架，将配分函数模作为优化目标，在伦纳德-琼斯势和铜的嵌入原子法势上验证，优化后力场的相图再现性显著提升。
中文摘要 AI 辅助
我们提出了一种以李-杨相变理论为基础、由相图引导的自动力场优化通用框架。核心思路是直接将配分函数模作为相图引导的优化目标。在靠近实轴的点上评估该模，而李-杨零点大多与相变相关，这种做法更具物理意义，且避免了显式求解零点的数值困难。该方法无需针对特定系统的序参量或响应性质来表征相变点，因此适用于各类不连续相变和材料体系。我们在两种场景下验证了该方法：一是优化覆盖气-液和固-液转变的伦纳德-琼斯势参数，二是基于实验熔化曲线优化铜的嵌入原子法势参数。优化后的力场在所有体系中均显著提升了目标相图的再现性。对于铜体系，优化同时改善了焓和热容的预测，而这两者是超出优化目标的可观测物理量。这些结果确立了李-杨理论作为现代力场开发实用工具的地位。
英文摘要
We propose a general framework for automatic force field refinement guided by phase diagrams, grounded in Lee-Yang phase transition theory. The central idea is to directly use the partition function modulus as a phase-diagram-guided optimization target. Evaluating the modulus at points close to the real axis, where the Lee-Yang zeros are mostly associated with the phase transition, is more physically meaningful and avoids the numerical difficulty of explicitly solving for the zeros. This approach requires no system-specific order parameters or response properties for characterizing phase transition points, making it universal across various discontinuous phase transitions and material systems. We validate the method on refining parameters of a Lennard-Jones potential covering both gas-liquid and solid-liquid transitions, and a Cu embedded-atom method potential based on experimental melting curves. The refined force fields reproduce the target phase diagrams with significant improvement across all systems. For Cu, the refinement simultaneously improves predictions of enthalpy and heat capacity, which are observables beyond the optimization target. These results establish Lee-Yang theory as a practical tool for contemporary force field development.
