AI 中文总结
研究多组分固溶体相稳定性，通过炼金术插值等方法扩展非平衡热力学积分，应用于Au-Cu二元合金构建相图，显式构型采样降低转变温度、拓宽固溶体稳定性范围，强调需显式采样非理想构型熵并选好泛函。
AI 中文摘要
多组分固溶体中的相稳定性取决于理想混合极限之外的构型熵，但在同一原子框架内同时捕捉振动熵仍具有挑战性。本文通过相互作用的炼金术插值将非平衡热力学积分扩展到成分依赖的转变，结合蒙特卡罗恒等交换移动和分子动力学，沿积分路径对振动和非理想构型熵进行采样。将该框架应用于Au-Cu二元合金，使用基于密度泛函理论数据训练的原子团簇展开势构建成分-温度相图。结果表明，显式构型采样降低了基于LDA数据训练的ACE势预测的AuCu有序-无序转变温度，更接近实验值，拓宽了固溶体的稳定性范围。同时，对交换关联泛函的更大敏感性表明，这种程度的一致性不应被视为一般预测准确性。因此，为了可靠地描述二元相图，必须显式采样非理想构型熵并仔细选择泛函。
英文摘要
Phase stability in multicomponent solid solutions depends on configurational entropy beyond the ideal mixing limit, but capturing it together with vibrational entropy within the same atomistic framework remains challenging. Here, we extend non-equilibrium thermodynamic integration to composition-dependent transformations through an alchemical interpolation of the interactions, combined with Monte Carlo identity exchange moves and molecular dynamics that sample the vibrational and non-ideal configurational entropy along the integration path. We apply the framework to the Au-Cu binary alloy using Atomic Cluster Expansion potentials trained on density functional theory data using the LDA, PBE, and r2SCAN functionals, and construct composition-temperature phase diagrams directly from atomistic free energies. We find that explicit configurational sampling lowers the AuCu order-disorder transition temperature predicted by the ACE potential trained on LDA data from approximately 810 K to 710 K, closer to the experimental value of 683 K, and substantially widens the stability range of the solid solution. At the same time, the much larger sensitivity to the exchange-correlation functional shows that this level of agreement should not be interpreted as general predictive accuracy. Non-ideal configurational entropy must therefore be sampled explicitly, alongside a careful choice of functional, for a reliable atomistic description of binary phase diagrams.
