基于Mori-Zwanzig记忆核的非谐液体熵泛函
An anharmonic liquid-entropy functional from the Mori-Zwanzig memory kernel
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中文总结 AI 辅助
该研究利用Mori-Zwanzig记忆核提出3PT方法，将液体态密度分解为三类组分并自洽计算笼熵，其可准确重现液态金属熵并适配水模型基准，建立了记忆与液体熵的轨迹级映射。
中文摘要 AI 辅助
我们利用Mori-Zwanzig记忆核将液体的态密度分解为气体、笼和谐晶三个组分。笼熵自洽计算为全速度响应相对于其马尔可夫对应物的非马尔可夫过剩，且被赋予排除体积熵参考而非谐熵参考。采用基于物理的约束，所得的三相显式非谐热力学（3PT）方法重现了液态金属的热力学积分熵，并使两个水模型与独立的自由能微扰基准对齐。对于单原子伦纳德-琼斯液体，3PT的精度遵循由记忆核非马尔可夫性决定的通用效率曲线。我们因此建立了记忆、瞬态笼动力学与液体熵之间直接的轨迹级映射关系。
英文摘要
We utilize the Mori-Zwanzig memory kernel to separate the density of states of a liquid into gas, cage, and harmonic-solid components. The cage entropy is computed self-consistently as the non-Markovian excess of the full velocity response over its Markovian counterpart, and is assigned an excluded-volume entropy reference rather than a harmonic one. Employing physically motivated constraints, the resulting Three-Phase Explicit Anharmonic Thermodynamics (3PT) method reproduces thermodynamic-integration entropies of liquid metals and aligns two water models with independent free-energy perturbation benchmarks. For monoatomic Lennard-Jones liquids, 3PT's accuracy follows a universal efficiency curve governed by the kernel's non-Markovianity. We thus establish a direct, trajectory-level mapping between memory, transient cage dynamics, and liquid entropy.
发表机构
- University of California San Diego（加州大学圣地亚哥分校）
- ATLAS Materials Physics Laboratory, Aiiso Yufeng Li Family Department of Nano and Chemical Engineering, University of California San Diego（加州大学圣地亚哥分校艾索·于峰李家族纳米与化学工程实验室）
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