Structural, electronic and thermodynamic properties of cubic Zn3N2 under high pressure from first-principles calculations

Abstract: The structural, electronic and thermodynamic properties of cubic Zn3N2 under hydrostatic pressure up to 80GPa are investigated using the local density approximation method with pseudopotentials of the ab initio norm-conserving full separable Troullier–Martin scheme in the frame of density functional theory. The structural parameters obtained at ambient pressure are in agreement with experimental data and other theoretical results. The change of bond lengths of two different types of Zn–N bond with pressure suggests that the tetrahedral Zn–N bond is slightly less compressible than the octahedral bond. By fitting the calculated band gap, the first and second order pressure coefficients for the direct band gap ofthe Zn3N2 were determined to be 1.18×10−2 eV/GPa and −2.4×10−4 eV/(GPa)2, respectively. Based on the Mulliken population analysis, Zn3N2 was found to have a higher covalent character with increasing pressure. As temperature increases, heat capacity, enthalpy, product of temperature and entropy increase, whereas the Debye temperature and free energy decrease. The present study leads to a better understanding of how Zn3N2 materials respond to compression. [Copyright &y& Elsevier]