Prediction of giant and ideal Rashba-type splitting in ordered alloy monolayers grown on a polar surface

A large and ideal Rashba-type spin-orbit splitting is desired for the applications of materials in spintronic devices and the detection of Majorana fermions in solids. Here, we propose an approach to achieve giant and ideal spin-orbit splittings through a combination of ordered surface alloying and interface engineering, that is, growing alloy monolayers on an insulating polar surface. We illustrate this unique strategy by means of first-principle calculations of buckled hexagonal monolayers of SbBi and PbBi supported on Al₂O₃(0001). Both systems display ideal Rashba-type states with giant spin-orbit splittings, characterized with energy offsets over 600 meV and momentum offsets over 0.3 Å^-1, respectively. Our study thus points to an effective way of tuning spin-orbit splitting in low-dimensional materials to draw immediate experimental interest.