Anisotropic ferromagnetism in carbon-doped zinc oxide from first-principles studies

Abstract

A density functional theory study of substitutional carbon impurities in ZnO has been performed, using both the generalized gradient approximation (GGA) and a hybrid functional (HSE06) as exchange-correlation functional. It is found that the non-spinpolarized C$_\mathrm{Zn}$ impurity is under almost all conditions thermodynamically more stable than the C$_\mathrm{O}$ impurity which has a magnetic moment of $2\mu_{\mathrm{B}}$, with the exception of very O-poor and C-rich conditions. This explains the experimental difficulties in sample preparation in order to realize $d^{0}$-ferromagnetism in C-doped ZnO. From GGA calculations with large 96-atom supercells, we conclude that two C$_\mathrm{O}$-C$_\mathrm{O}$ impurities in ZnO interact ferromagnetically, but the interaction is found to be short-ranged and anisotropic, much stronger within the hexagonal $ab$-plane of wurtzite ZnO than along the c-axis. This layered ferromagnetism is attributed to the anisotropy of the dispersion of carbon impurity bands near the Fermi level for C$_{\mathrm{O}}$ impurities in ZnO. From the calculated results, we derive that a C$_{\mathrm{O}}$ concentration between 2% and 6% should be optimal to achieve $d^{0}$-ferromagnetism in C-doped ZnO.