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Controlling the magnetic state of two-dimensional (2D) materials is crucialfor spintronic applications. By employing data-mining and autonomous densityfunctional theory calculations, we demonstrate the switching of magneticproperties of 2D non-van der Waals materials upon hydrogen passivation. Themagnetic configurations are tuned to states with flipped and enhanced moments.For 2D CdTiO$_3$ - a nonmagnetic compound in the pristine case - we observe anonset of ferromagnetism upon hydrogenation. Further investigation of themagnetization density of the pristine and passivated systems provides adetailed analysis of modified local spin symmetries and the emergence offerromagnetism. Our results indicate that selective surface passivation is apowerful tool for tailoring magnetic properties of nanomaterials such asnon-vdW 2D compounds.

Magnetic State Control of Non-van der Waals 2D Materials by Hydrogenation