Spin-exciton coupling modified by interfacial magnetic interactions in a van der Waals heterostructure

Abstract Excitons are primary elementary excitations in solids that present both fundamental interest and technological importance, showing great potential for photospintronic and quantum transduction applications. The emerging coherent collective excitations in two-dimensional antiferromagnetic semiconductors raise prospects for spin-exciton interactions and multifield control schemes. However, realizing the arbitrary manipulation of excitonic quantum states, while preserving the inherent dynamic and response advantages of antiferromagnetic nature remains challenging. Here we achieve bidirectional modulation of the CrSBr exciton energy via interfacial interaction-modified spin-exciton coupling in a CrSBr/Fe 3 GaTe 2 heterostructure. Compared with pristine CrSBr, the photoluminescence peaks in the heterostructure can exhibit blueshift and redshift corresponding to 6.1% and 8.6% of the total bandwidth, respectively. We reveal that the interfacial charge-transfer-driven magnetic coupling in the heterostructure effectively enhances the magnetic anisotropy and the exchange interaction of CrSBr, thereby stabilizing its antiferromagnetic spin configuration, suppressing interlayer electron-hole recombination, and ultimately leading to an anomalous blueshift of the exciton emission. Our findings demonstrate an approach for bidirectionally modulating exciton energy in two-dimensional antiferromagnetic semiconductors, which provides substantial flexibility in device design and offers an avenue for potential wavelength control in quantum information and optoelectronic technologies.