• Accepted Paper

Magnetic proximity beyond the interface: Layer-sequence-dependent exchange in WSe2/CrI3 heterostructures

Natalie Kuhn, Marc Schütte, Joachim Emming, Felix Hellenkamp, Leo Dreyer, Frank Volmer, Kenji Watanabe, Takashi Taniguchi, Lutz Waldecker, Christoph Stampfer, and Bernd Beschoten

Phys. Rev. Materials - Accepted 21 October, 2026

DOI: https://doi.org/10.1103/3sgj-pdxr

Abstract

Magnetic proximity effects in transition metal dichalcogenide (TMD)/2D-magnet heterostructures are often described in terms of the magnetization of the interfacial magnetic layer. Here, we show that this picture is sufficient to describe the neutral-exciton valley splitting of the TMD, but incomplete for its hole-doped electronic structure. We study a gate-tunable van der Waals heterostructure composed of monolayer WSe2 in direct contact with trilayer CrI3. By combining spatially and helicity-resolved reflection-contrast spectroscopy with magnetic circular dichroism, we identify two distinct magnetic domains in the trilayer CrI3: one with purely antiferromagnetic interlayer coupling and one with a mixed antiferromagnetic (AFM)/ferromagnetic (FM) coupling. In both domains, the sign of the neutral-exciton valley splitting of WSe2 switches with the magnetization reversal of the adjacent CrI3 layer. In contrast, helicity-resolved positive-trion spectroscopy of WSe2 reveals a qualitatively different response. While the AFM domain shows a strongly helicity-selective trion resonance, the mixed AFM/FM domain exhibits trion resonances in both helicities. This behavior disappears when all CrI3 layers are aligned in a parallel magnetization direction. Our results demonstrate that the positive-trion response is sensitive to the magnetic configuration of CrI3 beyond the directly adjacent layer, revealing a magnetic proximity response that cannot be described solely by the interfacial magnetization.

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