First-principles calculation of the electronic and optical properties of Gd${}_2$FeCrO${}_6$ double perovskite: Effect of Hubbard U parameter

Abstract

We have synthesized Gd${}_2$FeCrO${}_6$ (GFCO) double perovskite which is crystallized in a monoclinic structure with P2${}_1/$n space group. The UV-visible and photoluminescence spectroscopic analyses confirmed its direct bandgap semiconducting nature. Employing experimentally obtained structural parameters in first-principles calculation, we report the spin-polarized electronic band structure, charge carrier effective mass, density of states, electronic charge density distribution and optical absorption property of the GFCO double perovskite. The effects of on-site d-d Coulomb interaction energy (U${}_{eff}$) on the electronic and optical properties were investigated by applying a range of Hubbard U${}_{eff}$ parameters from 0 to 6 eV to the Fe-3d and Cr-3d orbitals within the generalized gradient approximation (GGA) and GGA+U methods. When we applied U${}_{eff}$ in the range of 1 to 5 eV, both the up-spin and down-spin band structures were observed to be direct. The charge carrier effective masses were also found to enhance gradually from U${}_{eff}=$ 1 eV to 5 eV, but, these values were anomalous for U${}_{eff}=$ 0 and 6 eV. These results suggest that U${}_{eff}$ should be limited within the range of 1 to 5 eV to calculate the structural, electronic and optical properties of GFCO double perovskite. We observed that considering U${}_{eff}=$ 3 eV, the theoretically calculated optical band gap 1.99 eV matched well with the experimentally obtained value 2.0 eV. The outcomes of our finding imply that the U${}_{eff}$ value of 3 eV most accurately localized the Fe-3d and Cr-3d orbitals of GFCO keeping the effect of self-interaction error from the other orbitals almost negligible. Therefore, we may recommend U${}_{eff}=$ 3 eV for first-principles calculation of the electronic and optical properties of GFCO double perovskite that might have potential in photocatalytic and related solar energy applications.

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• First-principles study of spontaneous polarization in multiferroic BiFeO${}_3$
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