Large Electrically and Chemically Tunable Rashba–Dresselhaus Effects in Ferroelectric CsGeX₃ (X = Cl, Br, I) Perovskites

Abstract

Rashba–Dresselhaus effects, which originate from spin–orbit coupling and allow for spin manipulations, are actively explored in materials, following the pursuit of spintronics and quantum computing. However, materials that possess practically significant Rashba–Dresselhaus effects often contain toxic elements and offer little opportunity for the tunability of the effects. We used first-principles simulations to reveal that the recently discovered halide ferroelectrics in the CsGeX3 (X = Cl, Br, I) family possess large and tunable Rashba-Dresselhaus effects. In particular, they give origin to the spin splitting of up to 171 meV in the valence band of CsGeI3. The value is chemically tunable and can decrease by 25% and 70% for CsGeBr3 and CsGeCl3, respectively. Such chemical tunability could result in the engineering of desired values through a solid solution technique. Application of an electric field was found to result in structural changes that could decrease and increase spin splitting, leading to electrical tunability of the effect. In the vicinity of conduction and valence band extrema, the spin textures are mostly of the Rashba type, which is promising for spin-to-charge conversion applications. The spin directions are coupled with the polarization direction, leading to Rashba-ferroelectricity cofunctionality. Our work identifies lead-free perovskite halides as excellent candidates for spin-based applications and is likely to stimulate further research in this direction.