Layered magnetic materials are becoming a major platform for future spin-based applications. Particularly, the air-stable van der Waals compound CrSBr is attracting considerable interest due to its prominent magneto-transport and magneto-optical properties. In this work, we observe a transition from antiferromagnetic to ferromagnetic behavior in CrSBr crystals exposed to high-energy, non-magnetic ions. Already at moderate fluences, ion irradiation induces a remanent magnetization with hysteresis adapting to the easy-axis anisotropy of the pristine magnetic order up to a critical temperature of 110 K. Structure analysis of the irradiated crystals in conjunction with density functional theory calculations suggests that the displacement of constituent atoms due to collisions with ions and the formation of interstitials favors ferromagnetic order between the layers.

Condensed Matter Physics Center and Departamento de Física Teórica de la Materia Condensada Universidad Autónoma de Madrid Ciudad Universitaria de Cantoblanco 28049 Madrid Spain

Department of Inorganic Chemistry University of Chemistry and Technology Prague Technická 5 166 28 Prague 6 Czech Republic

Helmholtz Zentrum Dresden Rossendorf Institute of Ion Beam Physics and Materials Research Bautzner Landstrasse 400 01328 Dresden Germany

Institute of Applied Physics and Würzburg Dresden Cluster of Excellence ct qmat Technische Universität Dresden 01069 Dresden Germany

TU Dresden 01062 Dresden Germany

University of Michigan Shanghai Jiao Tong University Joint Institute Shanghai Jiao Tong University Shanghai 200240 China

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