Rashba engineering at van der Waals interfaces

TL;DR

This paper demonstrates how stacking different TMD monolayers can control Rashba spin splitting, leading to enhanced THz spintronic emission and tunable spin-to-charge conversion at interfaces.

Contribution

It reveals that TMD heterobilayers can be engineered to manipulate Rashba spin splitting and improve spintronic device performance.

Findings

Enhanced THz emission in optimized heterobilayers like HfSe2/PtSe2.

Electronic hybridization causes strong Rashba spin-orbit coupling.

Layer choice enables tuning of spin-to-charge conversion.

Abstract

Two-dimensional transition metal dichalcogenide (TMD) interfaces offer a versatile platform for studying emergent quantum phenomena and enabling novel device functionalities. When distinct TMD monolayers are stacked vertically or laterally stitched, their interfaces can exhibit unique electronic band alignments, giving rise to long-lived interlayer excitons, charge transfer effects, and moir\'e superlattices with correlated states. Here, we demonstrate that the interface between a large variety of two different epitaxially grown TMD monolayers controls the intensity and sign of the Rashba spin splitting, which is probed using THz spintronic emission. Optimized TMD heterobilayers, such as HfSe$_2$/PtSe$_2$, show enhanced THz emission that surpass the spin-to-charge conversion efficiency of bulk TMDs, confirming the presence of Rashba states with large spin splitting at the interface. By combining spin- and angle-resolved photoemission spectroscopy with density functional theory, we reveal that the electronic hybridization between the two different TMD monolayers gives rise to extended in-gap states with strong Rashba spin-orbit coupling. The choice of TMD layers enables to engineer the sign and strength of spin-to-charge conversion in van der Waals heterobilayers opening up perspectives to build efficient and tunable THz spintronic emitters.