Search and design of nonmagnetic centrosymmetric layered crystals with large local spin polarization

TL;DR

This paper develops design principles for nonmagnetic, centrosymmetric layered crystals with large local spin polarization, expanding potential materials for spintronic applications by identifying specific structures and compounds with hidden R-2 spin polarization effects.

Contribution

It introduces material-specific design criteria and uses first-principles calculations to identify promising R-2 spin polarization materials within layered crystal families.

Findings

Predicted large spin splittings up to ~200 meV.

Identified stable and synthesizable LaOBiS2-type compounds with R-2 effects.

Predicted surface Rashba states in candidate materials.

Abstract

Until recently, spin-polarization in nonmagnetic materials was the exclusive territory of non- centrosymmetric structures. It was recently shown that a form of hidden spin polarization (named the Rashba-2 or R-2 effect) could exist in globally centrosymmetric crystals provided the individual layers belong to polar point group symmetries. This realization could considerably broaden the range of materials that might be considered for spin-polarization spintronic applications to include the hitherto forbidden spintronic compound that belong to centrosymetric symmetries. Here we take the necessary steps to transition from such general, material-agnostic condensed matter theory arguments to material-specific design principles that could aid future laboratory search of R-2 materials. Specifically, we (i) classify different prototype layered structures that have been broadly studied in the literature in terms of their expected R-2 behavior, including the Bi2Se3-structure type (a prototype topological insulator), MoS2-structure type (a prototype valleytronic compound) and LaBiOS2-structure type (a host of superconductivity upon doping); (ii) formulate the properties that ideal R-2 compounds should have in terms of combination of their global unit cell symmetries with specific point group symmetries of their constituent sectors; (iii) use first-principles band theory to search for compounds from the prototype family of LaOBiS2-type structures that satisfy these R-2 design metrics. We initially consider both stable and hypothetical compounds to establish an understanding of trends of R-2 with composition, and then indicate the predictions that are expected to be stable and synthesizable. We predict large spin splittings (up to ~ 200 meV for holes in LaOBiTe2) as well as surface Rashba states. Experimental testing of such predictions is called for.