Linking the electronic structure of solids to their thermodynamic and kinetic properties
Linking the electronic structure of solids to their thermodynamic and kinetic properties
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DOI：
10.1016/j.matcom.2009.08.008
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发表时间：
2010-03
期刊：
影响因子：
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通讯作者：
Anton Van der Ven;J. Thomas;Q. Xu;J. Bhattacharya
中科院分区：
文献类型：
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作者：
Anton Van der Ven;J. Thomas;Q. Xu;J. Bhattacharya
从第一性原理预测固体的可测量的热力学和动力学性质需要使用统计力学。对于具有重要技术意义的材料来说，一个主要的挑战来自于这样一个事实，即基本激发态的第一性原理电子结构计算在计算上要求非常高。因此，在激发态谱上的统计力学平均必须依赖于有效哈密顿量的使用，这些哈密顿量是由有限数量的第一性原理电子结构计算参数化的，但仍然可以高精度地预测激发态的能量。在这里，我们回顾了重要的有效哈密顿量，它解释了多组分结晶固体中的振动和构型自由度，并展示了如何使用它们来预测相稳定性作为组成和温度的函数，以及非稀释结晶固体中的动力学传输常数，如扩散系数。
Predicting measurable thermodynamic and kinetic properties of solids from first-principles requires the use of statistical mechanics. A major challenge for materials of technological importance arises from the fact that first-principles electronic structure calculations of elementary excited states are computationally very demanding. Hence statistical mechanical averaging over the spectrum of excited states must rely on the use of effective Hamiltonians that are parameterized by a limited number of first-principles electronic structure calculations, but nevertheless predict energies of excited states with a high level accuracy. Here we review important effective Hamiltonians that account for vibrational and configurational degrees of freedom in multi-component crystalline solids and show how they can be used to predict phase stability as a function of composition and temperature as well as kinetic transport constants such as diffusion coefficients in non-dilute crystalline solids.