Tight-binding modeling of interstitial ordering processes in metals: Application to zirconium hydrides

[摘要] We present here a theoretical study of ordering processes in metal-hydrogen compounds based on a generalized perturbation method and on tight-binding coherent potential approximation. This approach is illustrated for zirconium hydrides, in which case we demonstrate that a cluster expansion of the ordering energy can be limited to effective pair interactions, the leading one being between hydrogen atoms in third-neighbor positions. These results are quantitatively confirmed by comparison to density functional theory calculations and qualitatively interpreted through orbital symmetry analysis. The method is then applied first to draw a preliminary Zr-H phase diagram and then to characterize the effect of lattice deformation on the ordering processes in zirconium hydrides.

[关键词] GENERALIZED PERTURBATION-THEORY;INITIO MOLECULAR-DYNAMICS;TOTAL-ENERGY CALCULATIONS;AB-INITIO;ELECTRONIC-STRUCTURE;ZIRCALOY-4 PLATE;H-ZR;TRANSITION;ALLOYS;EMBRITTLEMENT