Abstract
GGA+U has been used as a framework for computational study of UH2, and alpha- and ,B-UH3, exploring specific features of the polar U-H bonding and its influence on magnetic and cohesion properties, including elastic parameters and vibrational properties. The description of the U-5 f states with direct Coulomb U = 0.5 eV and equal exchange J = 0.5 eV not only reproduce equilibrium volumes but provides a realistic description of total magnetic moments, consisting of smaller spin and larger antiparallel orbital components.
For UH(2 )and alpha-UH3, the spin-axis is aligned along the [111] direction. For ,B-UH3, there is a significant difference between both size and orientation U moments of atoms at the 2 a and 6 c Wyckoff positions.
The former has U moments aligned along [111], while in the latter, not fixed to any specific direction by symmetry, they deviate by 10. The method corroborates previous bonding analyses, indicating a prominent hybridization and charge transfer, affecting the 6 d and 7 s states of U, being partly transferred to the H-1 s states, revealed by the Bader analysis.
Analyzing individual effective inter-site magnetic coupling parameters it was possible to identify sources of relatively high Curie temperatures of 170 K for both UH(3 )variants and 120 K for UH2. Our results give predictions of elastic coefficients (consistent with the known bulk modulus in the case of ,B-UH3) and phonon densities of states, yielding expected infrared, Raman, and Hyper Raman active modes. (C) 2022 Elsevier B.V.
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