用于溶液中从头算自由能计算的炼金术热力学积分
Alchemical thermodynamic integration for ab initio free-energy calculations in solutions
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中文总结 AI 辅助
开发用于溶液中从头算自由能计算的炼金术热力学积分方案，通过耦合从头算力计算器，经验证后得出高压铁镍和常压锂钠液体溶液的自由能，与先前计算相符，效率与标准方法相当，确立为实用积分框架。
中文摘要 AI 辅助
我们开发了一种炼金术热力学积分方案，该方案在蒙特卡罗和分子动力学模拟过程中即时耦合从头算力计算器。该实现与现有的混合哈密顿方法进行了验证。该方案得出的高压铁镍和常压锂钠液体溶液的从头算自由能与先前计算结果一致，并再现了实验观察到的锂钠混溶间隙。该代码的效率与标准从头算分子动力学相当。这些结果将该方案确立为溶液中第一性原理自由能计算的实用炼金术积分框架。
英文摘要
We develop an alchemical thermodynamic integration scheme that couples ab initio force calculators on the fly during Monte Carlo and molecular dynamics simulations. The implementation is validated against existing hybrid-Hamiltonian approaches. The scheme yields ab initio free energies of high-pressure Fe-Ni and ambient Li-Na liquid solutions that agree with previous calculations and reproduce the experimentally observed Li-Na miscibility gap. The code has an efficiency comparable to standard ab initio molecular dynamics. These results establish this scheme as a practical alchemical-integration framework for first-principles free-energy calculations in solutions.
