Tuning Electronic and Magnetic Properties of Wurtzite ZnO Nanosheets by Surface Hydrogenation

Through density functional theory computations, we systematically investigated the structural, electronic, and magnetic properties as well as the relative stabilities of fully and partially hydrogenated ZnO nanosheets. Unlike bare ZnO nanosheets terminating with polar {0001} surfaces, their hydrogenated counterparts preserve the initial wurtzite configuration. Full hydrogenation is more favorable energetically for thinner ZnO nanosheets, whereas semihydrogenation at O sites is preferred for thicker ones. Moreover, semiconductor --> half-metal --> metal transition occurs with nonmagnetic --> magnetic transfer upon adopting surface hydrogenation and increasing sheet thickness. The predicted diverse and tunable electronic and magnetic properties endow ZnO nanosheets potential applications in electronics and spintronics.