Mapping Rashba-spin-valley coalescence in two-dimensional monolayers via high-throughput first-principles calculations

This study delves into the interplay of symmetry and structure in 2D systems to identify monolayers hosting valley physics together with the Rashba effect. Through high-throughput density functional theory calculations, 57 monolayers are identified exhibiting the Rashba effect, with the Rashba parameter αR spanning from 0 < αR < 2.0. The robustness of the Rashba parameters (αR) in these monolayers is primarily influenced by the physical parameters, highlighting the anti-crossing of Rashba-split bands and the Born effective charge (Z*). Among the 57 monolayers exhibiting the Rashba effect, the study identifies a subset of 23 monolayers presenting valley physics, demonstrating both in-plane and out-of-plane spin polarizations. The pronounced coupling of the valley and Rashba spin splitting is influenced by the in-plane and out-of-plane orbital contributions at the relevant K-points in the band spectra. In particular, the AB-type buckled structures feature these dual properties due to the presence of the broken inversion and mirror symmetries in them. Overall, the study eases the identification of monolayers with significant spin splitting and spin polarization, aiding in the design of high-performance 2D materials.