Tuning terahertz magnons in a mixed van der Waals antiferromagnet

Alloying stands out as a pivotal technological method employed across various compounds, be they metallic, magnetic, or semiconducting, serving to fine-tune their properties to meet specific requirements. Ternary semiconductors represent a prominent example of such alloys. They offer fine-tuning of electronic bands, the band gap in particular, thus granting the technology of semiconductor heterostructures devices, key elements in current electronics and optoelectronics. In the realm of magnetically ordered systems, akin to electronic bands in solids, spin waves exhibit characteristic dispersion relations, featuring sizable magnon gaps in many antiferromagnets. The engineering of the magnon gap constitutes a relevant direction in current research on antiferromagnets, aiming to leverage their distinct properties for terahertz technologies, spintronics, or magnonics. In this study, we showcase the tunability of the magnon gap across the terahertz spectral range within an alloy comprising representative semiconducting van der Waals antiferromagnets FePS3 and NiPS3. These constituents share identical in-plane crystal structures, magnetic unit cells, and the direction of the magnetic anisotropy, but differ in the amplitude and sign of the latter. Altogether these attributes result in the wide tunability of the magnon gap in the Fe1−𝑥⁢Ni𝑥⁢PS3 alloy in which the magnetic order is imposed by the stronger, perpendicular anisotropy of iron.