论文标题
固有过程的动力学抵消了超冷的美色液体中结晶的动力学
Kinetics of inherent processes counteracting crystallization in supercooled monatomic liquid
论文作者
论文摘要
超冷液体的结晶主要取决于与颗粒（原子）从液相转变为结晶的两个竞争过程，反之亦然，颗粒从结晶相返回到液相。这些过程的定量特征是所谓的附件率$ g^{+} $和分离率$ g^{ - } $，它们决定了粒子如何将其属性从一个相变为另一个阶段。在本研究中，第一次定义了$ g^{+} $和$ g^{ - } $之间的{\ IT对应规则}作为首次定义生长晶核的大小$ n $的函数。 In contrast to the well-known detailed balance condition, which relates $g^{+}(N)$ and $g^{-}(N)$ at $N=n_c$ (where $n_c$ is the critical nucleus size) and is satisfied only at the beginning of the nucleation regime, the found {\it correspondence rule} is fulfilled at all the main stages of crystallization kinetics (crystal nucleation, growth and结合）。以结晶过冷的Lennard-Jones液体结晶的例子，第一次以不同的超冷级别和较大范围的核大小$ n \ in [n_c; \，40 \ \，n_c] $计算了$ g^{ - } $。已经发现，在整个核大小范围内，分离率$ g^{ - } $仅比附件$ g^{+} $小于$ \ oft2 $ \％。这是直接的证据表明，在结晶的所有阶段，应对结晶的过程的作用仍然很重要。基于获得的结果，为核大小的时间依赖性分布函数制定了动力学方程，这是众所周知的动力学Becker-Döring-Zeldovich-frenkel方程的替代方法。
Crystallization of supercooled liquids is mainly determined by two competing processes associated with the transition of particles (atoms) from liquid phase to crystalline one and, vice versa, with the return of particles from crystalline phase to liquid one. The quantitative characteristics of these processes are the so-called attachment rate $g^{+}$ and the detachment rate $g^{-}$, which determine how particles change their belonging from one phase to another. In the present study, a {\it correspondence rule} between the rates $g^{+}$ and $g^{-}$ as functions of the size $N$ of growing crystalline nuclei is defined for the first time. In contrast to the well-known detailed balance condition, which relates $g^{+}(N)$ and $g^{-}(N)$ at $N=n_c$ (where $n_c$ is the critical nucleus size) and is satisfied only at the beginning of the nucleation regime, the found {\it correspondence rule} is fulfilled at all the main stages of crystallization kinetics (crystal nucleation, growth and coalescence). On the example of crystallizing supercooled Lennard-Jones liquid, the rate $g^{-}$ was calculated for the first time at different supercooling levels and for the wide range of nucleus sizes $N\in[n_c;\,40\,n_c]$. It was found that for the whole range of nucleus sizes, the detachment rate $g^{-}$ is only $\approx2$\% less than the attachment rate $g^{+}$. This is direct evidence that the role of the processes that counteract crystallization remains significant at all the stages of crystallization. Based on the obtained results, a kinetic equation was formulated for the time-dependent distribution function of the nucleus sizes, that is an alternative to the well-known kinetic Becker-Döring-Zeldovich-Frenkel equation.
