Abstract

Understanding the mechanisms underlying the emergence of giant spin splitting (GSS) is fundamental in the pursuit of more robust strategies for designing materials with desired spin splitting. This drive for material innovation continues to captivate a burgeoning community of early-career researchers with backgrounds in chemistry and material science. However, new to the field, they are often equipped only with the insight provided by the original Bychkov-Rashba model. Furthermore, daunted by the tight-binding perspective on the non-vanishing orbital angular momentum (OAM), they struggle to accurately account for the atomic spin-orbit interaction (SOI) in the formation of GSS. To address these challenges and equip young chemists with better-suited tools, this review aims to provide a more intuitive perspective on atomic interactions (orbital hybridization), structure symmetry, and atomic SOI in the formation of GSS. In pursuit of this goal, the review explores the Bychkov-Rashba model, its advantages, and limitations. Subsequently, it introduces the orbital framework, wherein GSS is modulated by atomic SOI and the interplay of OAM with the surface electrostatic field. Given the explicit dependence of both these factors on OAM, the review examines why OAM is typically quenched in crystal structures and how chemical bonds involving different orbital types can lead to its non-zero values in the presence of inversion symmetry breaking. Finally, with this chemistry-focused perspective, the review examines the rise of GSS in selected examples.

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