论文标题
从头算全细胞GW+DMFT，用于相关材料
Ab Initio Full Cell GW+DMFT for Correlated Materials
论文作者
论文摘要
相关材料中电子特性的定量预测需要模拟，而无需经验截断和参数。我们提出了一种方法，通过对动态平均场理论（DMFT）的新概念提出来实现这一目标。我们描述了一个完整的细胞$ GW $+DMFT方法，而不是使用低能子空间中定义的小型杂质，而这些杂质通常构成了一个完整的细胞$ GW $+DMFT方法，其中杂质包含晶体的所有原子或晶体的超级细胞中的所有原子。我们的配方会导致巨大的杂质问题，我们在此处使用有效的量子化学杂质求解器来处理，这些杂质杂质求解器可在实际频率轴上使用，并结合了一次性$ G_0W_0 $处理长期相互作用的处理。我们将完整的单元方法应用于散装SI，两个抗铁磁相关的绝缘子NiO和$α$ -FE $ _2 $ o $ $ _3 $以及promagnetic相关的金属srmoo $ _3 $，其中杂质最多包含10个原子和124个Orbitals。我们发现光谱特性，磁矩和两粒子自旋相关功能与实验良好相吻合。此外，在金属氧化物绝缘子中，涉及细胞中所有轨道的相关性的平衡处理可带来对绝缘间隙周围轨道特征的新见解。
Quantitative prediction of electronic properties in correlated materials requires simulations without empirical truncations and parameters. We present a method to achieve this goal through a new ab initio formulation of dynamical mean-field theory (DMFT). Instead of using small impurities defined in a low-energy subspace, which require complicated downfolded interactions which are often approximated, we describe a full cell $GW$+DMFT approach, where the impurities comprise all atoms in a unit cell or supercell of the crystal. Our formulation results in large impurity problems, which we treat here with efficient quantum chemistry impurity solvers that work on the real-frequency axis, combined with a one-shot $G_0W_0$ treatment of long-range interactions. We apply our full cell approach to bulk Si, two antiferromagnetic correlated insulators NiO and $α$-Fe$_2$O$_3$, and the paramagnetic correlated metal SrMoO$_3$, with impurities containing up to 10 atoms and 124 orbitals. We find that spectral properties, magnetic moments, and two-particle spin correlation functions are obtained in good agreement with experiments. In addition, in the metal oxide insulators, the balanced treatment of correlations involving all orbitals in the cell leads to new insights into the orbital character around the insulating gap.
