Large and tunable spin-orbit effect of 6p orbitals through structural cavities in crystals

TL;DR

This study demonstrates how structural cavities in ferroelectric Pb5Ge3O11 crystals enable large, tunable spin-orbit effects originating from 6p orbitals, with implications for spintronic applications.

Contribution

It reveals a novel mechanism where structural cavities and specific Pb sites induce significant, tunable spin-orbit effects via 6p orbitals in a ferroelectric crystal.

Findings

Cavities deepen the ferroelectric double well.

Cavity states exhibit sizeable spin splitting with Rashba-Weyl character.

SOC effects are robust against n-doping.

Abstract

We explore from first-principles calculations the ferroelectric material Pb5Ge3O11 as a model for controlling the spin-orbit interaction (SOC) in crystalline solids. The SOC has a surprisingly strong effect on the structural energy landscape by deepening the ferroelectric double well. We observe that this effect comes from a specific Pb Wyckoff site that lies on the verge of a natural cavity channel of the crystal. We also find that a unique cavity state is formed by the empty 6p states of another Pb site at the edge of the cavity channel. This cavity state exhibits a sizeable spin splitting with a mixed Rashba-Weyl character and a topologically protected crossing of the related bands. We also show that the ferroelectric properties and the significant SOC effects are exceptionally robust against n-doping up to several electrons per unit cell. We trace the provenance of these original effects to the unique combination of the structural cavity channel and the chemistry of the Pb atoms with 6p orbitals localizing inside the channel.