Electronic correlation strength of inorganic electrides from first principles

TL;DR

This study systematically analyzes the electronic correlation in inorganic electrides from first principles, revealing a strong dependence on dimensionality and cation species, and highlighting potential for strongly correlated electron systems.

Contribution

First-principles calculations of correlation strength in electrides show its dependence on dimensionality and cation type, providing insights into their electronic properties.

Findings

Correlation strength varies with dimensionality: 0D > 1D > 2D ≈ 3D.

Correlation exceeds 10 in all 0D and some 1D electrides.

Cation species influence the electronic correlation in 1D electrides.

Abstract

We present a systematic study clarifying an electronic correlation trend of electrides from first principles. By using the maximally localized Wannier function and the constrained random phase approximation, we calculated the electronic correlation strength $(U-U_{nn})/|t|$ of 19 inorganic electrides, where $U$, $U_{nn}$, and $t$ are the effective onsite Coulomb repulsion, nearest-neighbor Coulomb repulsion, and the nearest-neighbor transfer integrals, respectively. The electronic correlation was found to be highly correlated with the dimensionality of the Wannier-function network of anionic electrons in electrides; the correlation strength varies in the order 0D $>>$ 1D $>$ 2D $\sim$ 3D, showing good correspondence with experimental trends, and exceeds 10 (a measure for the emergence of exotic properties) in all the 0D systems and some of the 1D materials. We also found that the electronic correlation depends on the cation species surrounding the anionic electrons; in the 1D electrides, the electronic correlation becomes stronger for cationic walls consisting of $\mathrm{Ca^{2+}}$, $\mathrm{Sr^{2+}}$, and $\mathrm{Ba^{2+}}$ in this order, and the correlation strength exceeds 10 for $\mathrm{Ba_5As_3}$. The theoretical results indicate that 0- and 1-dimensional electrides will be new research targets for studies on strongly correlated electron systems.