Controlling magnetism at nanometer length scales is essential for realizing high-performance spintronic, magneto-electric and topological devices and creating on-demand spin Hamiltonians probing fundamental concepts in physics. Van der Waals (vdW)-bonded layered magnets offer exceptional opportunities for such spin texture engineering. Here, we demonstrate nanoscale structural control in the layered magnet CrSBr with the potential to create spin patterns without the environmental sensitivity that has hindered such manipulations in other vdW magnets. We drive a local phase transformation using an electron beam that moves atoms and exchanges bond directions, effectively creating regions that have vertical vdW layers embedded within the initial horizontally vdW bonded exfoliated flakes. We calculate that the newly formed two-dimensional structure is ferromagnetically ordered in-plane with an energy gap in the visible spectrum, and weak antiferromagnetism between the planes, suggesting possibilities for creating spin textures and quantum magnetic phases.

Department of Chemistry Columbia University New York 10027 NY USA

Department of Electrical Engineering and Computer Science University of Michigan Ann Arbor MI USA

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

Department of Materials Science and Engineering Massachusetts Institute of Technology Cambridge MA 02139 USA

Department of Physics Harvard University Cambridge MA USA

Ernst Ruska Centre for Microscopy and Spectroscopy with Electrons and Peter Grünberg Institute Forschungszentrum Jülich 52425 Jülich Germany

Institut für Theoretische Physik Universität Bremen P O Box 330 440 28334 Bremen Germany

John A Paulson School of Engineering and Applied Sciences Harvard University Cambridge MA USA

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