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Measurement of the Phonon Density of States of PuO2(+2%Ga)

Published online by Cambridge University Press:  28 May 2012

M. E. Manley ,
J. R. Jeffries ,
A. H. Said ,
C. A. Marianetti ,
H. Cynn ,
B. M. Leu  and
M. Wall
M. E. Manley
Affiliation:
Lawrence Livermore National Laboratory, Livermore, California 94550, USA
J. R. Jeffries
Affiliation:
Lawrence Livermore National Laboratory, Livermore, California 94550, USA
A. H. Said
Affiliation:
Argonne National Laboratory, Argonne, Illinois 60439, USA
C. A. Marianetti
Affiliation:
Department of Applied Physics, Columbia University, New York, New York 10027, USA
H. Cynn
Affiliation:
Lawrence Livermore National Laboratory, Livermore, California 94550, USA
B. M. Leu
Affiliation:
Argonne National Laboratory, Argonne, Illinois 60439, USA
M. Wall
Affiliation:
Lawrence Livermore National Laboratory, Livermore, California 94550, USA
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Abstract

Inelastic x-ray scattering measurements of the phonon density of states (DOS) of PuO2(+2%Ga) were made and compared to recent predictions from the literature made using three leading theoretical approaches; Density Functional Theory (DFT), DFT plus the Hubbard U (DFT+U), and Dynamical Mean-Field Theory (DMFT). The DFT prediction, which does not account for strong electronic correlations, underestimates the measured energies of most features. The DFT+U and DMFT predictions, which include approximations to strong correlation effects, more accurately reflect the low energy features but exaggerate splitting in the highest energy optic oxygen modes. The exaggeration of the splitting is worse for DFT+U than for DMFT. The transverse acoustic mode shows the least sensitivity to calculation type, and is well reproduced by all three theories. The longitudinal acoustic mode, which is thought to control the thermal conductivity, is more sensitive to calculation type, suggesting an important role for electronic correlations in making application-critical predictions.

Type
Articles
Information
MRS Online Proceedings Library (OPL) , Volume 1444: Symposium S/Y – Actinides and Nuclear Energy Materials , 2012 , mrss12-1444-y05-02
Copyright
Copyright © Materials Research Society 2012

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References

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