First-principles study of structural, elastic, electronic, vibrational and thermodynamic properties of UN

Abstract

Abstract The structural, elastic, electronic, phonon and thermodynamic properties of UN are studied by density functional theory (DFT) within local-density approximation (LDA) and generalized gradient approximation (GGA), and GGA + U . The GGA calculations of the ground state structural and elastic properties of UN show an overall better agreement with experimental data compared to LDA or GGA + U . The melting temperature of UN ( T m ) is estimated from the calculated elastic constant, with GGA predicting T m = 2944 ± 300 K, in excellent agreement with experimental data. The calculated phonon dispersions of UN agree well with the low temperature measurements. Furthermore, the thermodynamic properties of UN are studied using quasiharmonic approximation by including both lattice vibrational and thermal electronic contributions. The predicted thermodynamic properties, such as enthalpy, entropy, Gibbs energy, heat capacity and thermal expansion coefficient, agree well with experimental data. The derived thermodynamic functions of UN are useful to the thermodynamic modeling of phase stabilities in UN-based materials. This study shows that the thermal electronic energy and entropy due to U 5 f electrons are important to describe the free energy of UN, due to the metallic character of UN. The calculated thermodynamic properties also suggest that the anharmonic effects are less important in UN even at high-temperature.