Challenges and opportunities in proximity-driven exciton-spin engineering in van der Waals heterostructures
Abstract
van der Waals heterostructures consisting of transition metal dichalcogenides (TMDs) and two-dimensional (2D) magnets offer a versatile platform to study the coexistence and transformation of different excitons. By focusing on TMD WSe2 and 2D magnetic CrI3, as a bilayer WSe2/CrI3 and a trilayer CrI3/WSe2/CrI3, we provide their description using a parameter-free, high-fidelity many-body perturbation theory. This ab initio approach allows us to elucidate the character of magnetic Frenkel excitons in CrI3 and how the nonmagnetic Wannier-Mott excitons in WSe2 are modified by the proximity of CrI3. We reveal novel proximity-induced interlayer excitons in these heterostructures. In contrast to the sensitivity of proximity-induced modifications of excitons in WSe2, which depend on the interfacial details, the interlayer magnetic excitons are remarkably robust and are present across the different stacking configurations between WSe2 and CrI3, simplifying their experimental demonstration. These findings suggest unexplored opportunities for information transduction using magnetic excitons and integrating photonics, electronics, and spintronics in proximitized materials.
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