Studies of vibrational properties in Ga stabilized delta-Pu by extended X-ray absorption fine structure

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Temperature dependent extended x-ray absorption fine structure (EXAFS) spectra were measured for a 3.3 at. % Ga stabilized Pu alloy over the range T= 20 - 300 K. EXAFS data were acquired at both the Ga K-edge and the Pu L{sub III} edge. Curve-fits were performed to the first shell interactions to obtain pair-distance distribution widths, {sigma}, as a function of temperature. The temperature dependence of {sigma}(T) was accurately modeled using a correlated-Debye model for the lattice vibrational properties, suggesting Debye-like behavior in this material. Using this formalism, we obtain pair-specific correlated-Debye temperatures, {Theta}{sub cD}, of 110.7 {+-} 1.7 K ... continued below

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Allen, P.G.; Henderson, A.L.; Sylwester, E.R.; Turchi, P.E.A.; Shen, T.H.; Gallegos, G.F. et al. February 14, 2002.

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Temperature dependent extended x-ray absorption fine structure (EXAFS) spectra were measured for a 3.3 at. % Ga stabilized Pu alloy over the range T= 20 - 300 K. EXAFS data were acquired at both the Ga K-edge and the Pu L{sub III} edge. Curve-fits were performed to the first shell interactions to obtain pair-distance distribution widths, {sigma}, as a function of temperature. The temperature dependence of {sigma}(T) was accurately modeled using a correlated-Debye model for the lattice vibrational properties, suggesting Debye-like behavior in this material. Using this formalism, we obtain pair-specific correlated-Debye temperatures, {Theta}{sub cD}, of 110.7 {+-} 1.7 K and 202.6 {+-} 3.7 K, for the Pu-Pu and Ga-Pu pairs, respectively. The result for the Pu-{Theta}{sub cD} value compares well with previous vibrational studies on {delta}-Pu. In addition, our results represent the first unambiguous determination of Ga-specific vibrational properties in Pu-Ga alloys, i.e, {Theta}{sub cD} for the Ga-Pu pair. Because the Debye temperature can be related to a measure of the lattice stiffness, these results indicate the Ga-Pu bonds are significantly stronger than the Pu-Pu bonds. This effect has important implications for lattice stabilization mechanisms in these alloys.

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  • Journal Name: Physical Review B; Journal Volume: 65; Journal Issue: 21; Other Information: Journal Publication Date: June 1, 2002

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  • Report No.: LBNL--49403
  • Report No.: UCRL-JC-146442 (LLNL)
  • Grant Number: AC03-76SF00098
  • DOI: 10.1103/PhysRevB.65.214107 | External Link
  • Office of Scientific & Technical Information Report Number: 797841
  • Archival Resource Key: ark:/67531/metadc734163

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  • February 14, 2002

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  • Oct. 19, 2015, 7:39 p.m.

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  • April 4, 2016, 6:29 p.m.

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Allen, P.G.; Henderson, A.L.; Sylwester, E.R.; Turchi, P.E.A.; Shen, T.H.; Gallegos, G.F. et al. Studies of vibrational properties in Ga stabilized delta-Pu by extended X-ray absorption fine structure, article, February 14, 2002; Berkeley, California. (digital.library.unt.edu/ark:/67531/metadc734163/: accessed October 19, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.