论文标题

通过多体平面波辅助场量子蒙特卡罗计算的固体中的电子密度

Ab initio electronic density in solids by many-body plane-wave auxiliary-field quantum Monte Carlo calculations

论文作者

Chen, Siyuan, Motta, Mario, Ma, Fengjie, Zhang, Shiwei

论文摘要

我们介绍了几种固体材料(包括SI,NACL和CU)中电子密度的精确多体结果。这些结果是使用从头算辅助场量子Carlo(AFQMC)方法以平面波和规范性的多个项目伪电势来获得的。 AFQMC已被证明是一种极好的多体总能量方法。本文讨论了基础能量以外的可观察力和相关函数的计算,还需要反向传播,在本文中讨论了其在平面波基础基础AFQMC框架中的适应和实现。这种发展使我们能够计算相关函数,电子密度和原子质力,从而为固体中热力学特性的几何优化和计算铺平了道路。在多体框架中,有限的超级细胞尺寸效应比在独立电子计算中更为微妙。我们分析电子密度的收敛性,并获得热力学极限的最佳估计。与我们的近乎杰出的结果相对于几个典型密度功能的密度进行了基准测试。我们获得的电子密度也可用于帮助构建改进的密度功能。

We present accurate many-body results of the electronic densities in several solid materials, including Si, NaCl, and Cu. These results are obtained using the ab initio auxiliary-field quantum Monte Carlo (AFQMC) method working in a plane-wave basis with norm-conserving, multiple-projector pseudopotentials. AFQMC has been shown to be an excellent many-body total energy method. Computation of observables and correlation functions other than the ground-state energy requires back-propagation, whose adaption and implementation in the plane-wave basis AFQMC framework are discussed in the present paper. This development allows us to compute correlation functions, electronic densities and interatomic forces, paving the way for geometry optimizations and calculations of thermodynamic properties in solids. Finite supercell size effects are considerably more subtle in the many-body framework than in independent-electron calculations. We analyze the convergence of the electronic density, and obtain best estimates for the thermodynamic limit. The densities from several typical density functionals are benchmarked against our near-exact results. The electronic densities we have obtained can also be used to help construct improved density functionals.

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