Role of di-interstitial clusters in oxygen transport in UO2+x from first principles

被引：51

作者：

Andersson, D. A. ^{[1
]}

Watanabe, T. ^{[2
]}

Deo, C. ^{[3
]}

Uberuaga, B. P. ^{[1
]}

机构：

[1] Los Alamos Natl Lab, Div Mat Sci & Technol, Los Alamos, NM 87545 USA

[2] Georgia Inst Technol, Sch Chem & Biomol Engn, Atlanta, GA 30332 USA

[3] Georgia Inst Technol, George W Woodruff Sch Mech Engn, Nucl & Radiol Engn Program, Atlanta, GA 30332 USA

来源：

PHYSICAL REVIEW B | 2009年 / 80卷 / 06期

关键词：

density functional theory; diffusion; interstitials; Monte Carlo methods; uranium compounds; GENERALIZED GRADIENT APPROXIMATION; TEMPERATURE-ACCELERATED DYNAMICS; TOTAL-ENERGY CALCULATIONS; FINDING SADDLE-POINTS; AUGMENTED-WAVE METHOD; URANIUM-DIOXIDE; ELECTRONIC-STRUCTURE; SELF-DIFFUSION; BASIS-SET; DEFECTS;

D O I：

10.1103/PhysRevB.80.060101

中图分类号：

T [工业技术];

学科分类号：

08 ;

摘要：

Using density functional theory, we examine a recently discovered structure for di-interstitial oxygen clusters in UO2+x in which three oxygen ions share one lattice site. This di-interstitial cluster exhibits a fast diffusion pathway; the migration barrier for these clusters is approximately half of that for mono-interstitials. Using kinetic Monte Carlo, we calculate the diffusivity of oxygen with and without the di-interstitial mechanism as a function of x and find that oxygen transport is significantly increased for higher values of x when the di-interstitial mechanism is included, agreeing much more closely with experimental data. These results emphasize the importance of clustering phenomena in UO2+x and have implications for the evolution of UO2+x.

引用

页数：4

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