Density-functional study of plutonium monoxide monohydride

TL;DR

This study uses density-functional theory to predict the structure, electronic, mechanical, optical, and thermodynamic properties of plutonium monoxide monohydride, providing comprehensive insights into its stability and bonding characteristics.

Contribution

It offers the first detailed theoretical analysis of PuOH's properties, predicting its crystal structure, magnetic state, and stability using advanced DFT methods.

Findings

F-43m is the lowest-energy crystal structure of PuOH

PuOH is an antiferromagnetic charge-transfer insulator

The predicted formation and oxidation energies agree with experimental data

Abstract

The structural, electronic, mechanical, optical, thermodynamic properties of plutonium monoxide monohydride (PuOH) are studied by density-functional calculations within the framework of LDA/GGA and LDA/GGA+U.From the total energy calculation, the lowest-energy crystal structure of PuOH is predicted to have space group F-43m (No. 216). Within the LDA+U framework, the calculated lattice parameter of F-43m-PuOH is in good agreement with the experimental value and the corresponding ground state is predicted to be an antiferromagnetic charge-transfer insulator. Furthermore, we investigate the bonding character of PuOH by analyzing the electron structure and find that there are a stronger Pu-O bond and a weaker Pu-H bond.The mechanical properties including the elastic constants, elastic moduli and Debye's temperature, and the optical properties including the reflectivity and absorption coefficient are also calculated. We then compute the phonon spectrum which verified the dynamical stability of F-43m-PuOH. Some thermodynamic quantities such as the specific heat are evaluated. Finally we calculate the formation energy of PuOH, and the reaction energies for the oxidation of PuOH and PuOH-coated Pu, which are in reasonable agreement with the experimental values.