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Title: Effect of Spin-Orbit Coupling on the Actinide Dioxides AnO2 (An=Th, Pa, U, Np, Pu, and Am): A Screened Hybrid Density Functional Study

Abstract

We present a systematic comparison of the lattice structures, electronic density of states, and band gaps of actinide dioxides, AnO₂ (An=Th, Pa, U, Np, Pu, and Am) predicted by the Heyd-Scuseria-Ernzerhof screened hybrid density functional (HSE) with the self-consistent inclusion of spin-orbit coupling(SOC). The computed HSE lattice constants and band gaps of AnO₂ are in consistently good agreement with the available experimental data across the series, and differ little from earlier HSE results without SOC. ThO₂ is a simple band insulator (f⁰), while PaO₂, UO₂, and NpO₂ are predicted to be Mott insulators. The remainders (PuO₂ and AmO₂) show considerable O2p/An5f mixing and are classified as charge-transfer insulators. We also compare our results for UO₂, NpO₂, and PuO₂with the PBE+U, self interaction correction (SIC), and dynamic mean-field theory (DMFT) many-body approximations.

Authors:
; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1222162
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics, 137(15):154707
Additional Journal Information:
Journal Name: Journal of Chemical Physics, 137(15):154707
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Wen, Xiaodong, Martin, Richard L., Roy, Lindsay E., Scuseria, Gustavo E., Rudin, Sven P., Batista, Enrique R., McCleskey, Thomas M., Scott, Brian L., Bauer, Eve, Joyce, John J., and Durakiewicz, Tomasz. Effect of Spin-Orbit Coupling on the Actinide Dioxides AnO2 (An=Th, Pa, U, Np, Pu, and Am): A Screened Hybrid Density Functional Study. United States: N. p., 2012. Web. doi:10.1063/1.4757615.
Wen, Xiaodong, Martin, Richard L., Roy, Lindsay E., Scuseria, Gustavo E., Rudin, Sven P., Batista, Enrique R., McCleskey, Thomas M., Scott, Brian L., Bauer, Eve, Joyce, John J., & Durakiewicz, Tomasz. Effect of Spin-Orbit Coupling on the Actinide Dioxides AnO2 (An=Th, Pa, U, Np, Pu, and Am): A Screened Hybrid Density Functional Study. United States. doi:10.1063/1.4757615.
Wen, Xiaodong, Martin, Richard L., Roy, Lindsay E., Scuseria, Gustavo E., Rudin, Sven P., Batista, Enrique R., McCleskey, Thomas M., Scott, Brian L., Bauer, Eve, Joyce, John J., and Durakiewicz, Tomasz. Sun . "Effect of Spin-Orbit Coupling on the Actinide Dioxides AnO2 (An=Th, Pa, U, Np, Pu, and Am): A Screened Hybrid Density Functional Study". United States. doi:10.1063/1.4757615.
@article{osti_1222162,
title = {Effect of Spin-Orbit Coupling on the Actinide Dioxides AnO2 (An=Th, Pa, U, Np, Pu, and Am): A Screened Hybrid Density Functional Study},
author = {Wen, Xiaodong and Martin, Richard L. and Roy, Lindsay E. and Scuseria, Gustavo E. and Rudin, Sven P. and Batista, Enrique R. and McCleskey, Thomas M. and Scott, Brian L. and Bauer, Eve and Joyce, John J. and Durakiewicz, Tomasz},
abstractNote = {We present a systematic comparison of the lattice structures, electronic density of states, and band gaps of actinide dioxides, AnO₂ (An=Th, Pa, U, Np, Pu, and Am) predicted by the Heyd-Scuseria-Ernzerhof screened hybrid density functional (HSE) with the self-consistent inclusion of spin-orbit coupling(SOC). The computed HSE lattice constants and band gaps of AnO₂ are in consistently good agreement with the available experimental data across the series, and differ little from earlier HSE results without SOC. ThO₂ is a simple band insulator (f⁰), while PaO₂, UO₂, and NpO₂ are predicted to be Mott insulators. The remainders (PuO₂ and AmO₂) show considerable O2p/An5f mixing and are classified as charge-transfer insulators. We also compare our results for UO₂, NpO₂, and PuO₂with the PBE+U, self interaction correction (SIC), and dynamic mean-field theory (DMFT) many-body approximations.},
doi = {10.1063/1.4757615},
journal = {Journal of Chemical Physics, 137(15):154707},
number = ,
volume = ,
place = {United States},
year = {2012},
month = {10}
}