Cao Lin-Li, Wang Yun-Jiang
State Key Laboratory of Nonlinear Mechanics, Institute of Mechanics Chinese Academy of Sciences, Beijing 100190, China.
School of Engineering Science, University of Chinese Academy of Sciences, Beijing 100049, China.
J Phys Chem Lett. 2024 Jan 25;15(3):811-816. doi: 10.1021/acs.jpclett.3c03530. Epub 2024 Jan 17.
Establishing a robust quantitative correlation between thermodynamics and dynamics in amorphous matter remains a significant challenge in condensed matter physics. Although the classical Adam-Gibbs relationship represents a pivotal step in this direction and the correlation between relaxation time and configurational entropy has been partially verified in simple liquids, this quantitative link has yet to be tested in realistic glass-forming systems where complex many-body interactions are present. Here we conduct free energy samplings and lattice dynamics analysis to distinguish vibrational entropy from configurational entropy in a realistic Cu-Zr model of a metallic glass. Our calculations unveil a power-law relationship (with a substantial exponent of ∼3) between the logarithmic relaxation time and configurational entropy, surpassing the linear prediction of the original Adam-Gibbs relationship. This nonlinear entropy driven relaxation time variation likely originates from anisotropic nature of atomic many-body interactions, suggesting that factors beyond thermodynamics contribute to the glass transition phenomenon.
在凝聚态物理中，在无定形物质中建立热力学与动力学之间稳健的定量关联仍然是一项重大挑战。尽管经典的亚当 - 吉布斯关系代表了朝这个方向迈出的关键一步，并且弛豫时间与构型熵之间的关联已在简单液体中得到部分验证，但这种定量联系尚未在存在复杂多体相互作用的实际玻璃形成系统中得到检验。在此，我们进行自由能抽样和晶格动力学分析，以在金属玻璃的实际铜 - 锆模型中区分振动熵和构型熵。我们的计算揭示了对数弛豫时间与构型熵之间的幂律关系（指数约为3），超越了原始亚当 - 吉布斯关系的线性预测。这种非线性的熵驱动弛豫时间变化可能源于原子多体相互作用的各向异性性质，这表明除了热力学之外的因素也对玻璃转变现象有贡献。
