Fully relativistic density functional calculations on hydroxylated actinide oxide surfaces

被引:73
作者
Boettger, JC
Ray, AK
机构
[1] Los Alamos Natl Lab, Div Appl Phys, Los Alamos, NM 87545 USA
[2] Univ Texas, Dept Phys, Arlington, TX 76019 USA
关键词
actinide oxides; LCGTO-FF method; DFT calculations; scalar- and fully relativistic levels of approximation;
D O I
10.1002/qua.10350
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The linear combinations of Gaussian-type orbitals-fitting function (LCGTO-FF) method has been used to investigate the cohesive properties of three fluorite structure actinide oxides (ThO2, UO2, and PuO2), and their clean and hydroxylated (111) surfaces, within the generalized gradient approximation (GGA) to density functional theory (DFT). Relativistic effects have been considered at both the scalar-relativistic and the fully relativistic (spin-orbit coupling included) levels of approximation. It is found here that the 5f states have only a minimal effect on the cohesive properties of these systems, despite the fact that the two heavier actinide oxides (both Mott-Hubbard-type insulators) are incorrectly predicted to be good metals. The cause of this insensitivity to the spurious metallic nature of the 5f states, is elucidated. (C) 2002 Wiley Periodicals, Inc.
引用
收藏
页码:1470 / 1477
页数:8
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