Interlayer Interaction of Excitons and Magnons in Graphene/WS2/Néel‐Type Manganese Phosphorus Trichalcogenide Heterostructures.

2D materials, particularly 2D semiconductors, and layered antiferromagnetic (AFM) compounds, exhibit rich light‐matter coupling phenomena in low‐dimensional systems. In this work, the occurrence of interlayer exciton–magnon coupling (EMC) is observed in Néel‐type AFM of MnPX3 (X = S or Se) and monolayer (1L) WS2 heterostructures. The energy of neutral exciton in 1L WS2 can be tuned by the adjacent AFM order, resulting in an additional energy shift of 10–14 meV. Furthermore, by filtering the photoluminescence spectrum with graphene and conducting magnetic measurements, the correlation is elucidated between the interlayer EMC and AFM transition process. In MnPS3, this coupling behavior exhibits sensitivity to the changes of magnetic structures, manifesting with a correlated length ξ of 8.34 Å at temperatures higher than Néel temperature (TN). The decoupling process in WS2/MnPS3 heterostructure below 50 K is originated from a weak out‐of‐plane ferromagnetic order, confirming the presence of an XY‐type magnetic phase transition in MnPS3 at sub‐TN temperature. This study provides a fundamental understanding of EMC and its potential applications in the integration of optical and magnetic devices. [ABSTRACT FROM AUTHOR]