Spin density stabilization of local distortions induced by a monovacancy in -Pu
Abstract
Density functional theory calculations elucidate crystallographic and electronic structural responses of the fcc delta phase of plutonium (δ-Pu) to point defects. Discussed are responses that vary from a defect exhibiting a local structural instability common in fcc metals to an unusual defect structure that mimics properties similar to the monoclinic α phase. In the prior case, the existence of a self-vacancy when ionic relaxation is allowed induces in the fcc lattice a local tetragonal instability in nearest-neighbor atoms, slight electronic charge increase, and a spin-density decrease. However, in the latter case, after ionic relaxation, the defect is not recognizable as the structure of a vacant site common to many simple fcc metals, but is a complex extended defect involving neighboring atoms to collectively exhibit loss of lattice symmetry through formation of short Pu-Pu bonds and associated narrow bands at the Fermi energy. Partial density of states (PDOS) indicates that these narrow bands form as spectral weighting from the less energetic 6d electronic states is shifted to the 5f electronic states by means of the spin density, which occupies states at the Fermi energy. Finally, the PDOS of a 5f system exhibiting narrow bands at the Fermi energy is associated withmore »
- Authors:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE; LANL Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 1483534
- Alternate Identifier(s):
- OSTI ID: 1465607
- Report Number(s):
- LA-UR-18-23844
Journal ID: ISSN 2475-9953
- Grant/Contract Number:
- 89233218CNA000001
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Materials
- Additional Journal Information:
- Journal Volume: 2; Journal Issue: 8; Journal ID: ISSN 2475-9953
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; distortions & defects; electronic structure; point defects
Citation Formats
Hernandez, Sarah C., Freibert, Franz J., Hoagland, Richard G., Uberuaga, Blas P., and Wills, John M.. Spin density stabilization of local distortions induced by a monovacancy in δ -Pu. United States: N. p., 2018.
Web. doi:10.1103/PhysRevMaterials.2.085005.
Hernandez, Sarah C., Freibert, Franz J., Hoagland, Richard G., Uberuaga, Blas P., & Wills, John M.. Spin density stabilization of local distortions induced by a monovacancy in δ -Pu. United States. https://doi.org/10.1103/PhysRevMaterials.2.085005
Hernandez, Sarah C., Freibert, Franz J., Hoagland, Richard G., Uberuaga, Blas P., and Wills, John M.. Tue .
"Spin density stabilization of local distortions induced by a monovacancy in δ -Pu". United States. https://doi.org/10.1103/PhysRevMaterials.2.085005. https://www.osti.gov/servlets/purl/1483534.
@article{osti_1483534,
title = {Spin density stabilization of local distortions induced by a monovacancy in δ -Pu},
author = {Hernandez, Sarah C. and Freibert, Franz J. and Hoagland, Richard G. and Uberuaga, Blas P. and Wills, John M.},
abstractNote = {Density functional theory calculations elucidate crystallographic and electronic structural responses of the fcc delta phase of plutonium (δ-Pu) to point defects. Discussed are responses that vary from a defect exhibiting a local structural instability common in fcc metals to an unusual defect structure that mimics properties similar to the monoclinic α phase. In the prior case, the existence of a self-vacancy when ionic relaxation is allowed induces in the fcc lattice a local tetragonal instability in nearest-neighbor atoms, slight electronic charge increase, and a spin-density decrease. However, in the latter case, after ionic relaxation, the defect is not recognizable as the structure of a vacant site common to many simple fcc metals, but is a complex extended defect involving neighboring atoms to collectively exhibit loss of lattice symmetry through formation of short Pu-Pu bonds and associated narrow bands at the Fermi energy. Partial density of states (PDOS) indicates that these narrow bands form as spectral weighting from the less energetic 6d electronic states is shifted to the 5f electronic states by means of the spin density, which occupies states at the Fermi energy. Finally, the PDOS of a 5f system exhibiting narrow bands at the Fermi energy is associated with the formation of an unusual defect structure in the lattice.},
doi = {10.1103/PhysRevMaterials.2.085005},
journal = {Physical Review Materials},
number = 8,
volume = 2,
place = {United States},
year = {2018},
month = {8}
}
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