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Title: Possible Bose-condensated Behavior in a Quantum Phase Originating in a Collective Excitation in the Chemically and Optically Doped Mott-Hubbard System UO2+x

The pinned charge defects in U4O9, and U3O7 that are the single phase fluoritestructured derivatives of UO2 have been characterized by U L3 EXAFS at 30, 100, and 200 K, xray and neutron pair distribution function analysis, O K edge XAS and non-resonant inelastic xray scattering, and Raman spectroscopy, while mobile charge defects were investigated by femtosecond time-resolved pump-probe laser spectroscopy on single crystal UO2 between 7 and 300 K. The results from all of these measurements show highly complex and anomalous behaviors, which we attribute to a charge-lattice instability in UO2 that most likely originates in the intersection of the ground U(IV) and a proximate uranyl-like excited state in a conic section, causing a breakdown of the Born-Oppenheimer approximation. Furthermore, the photoinduced quasiparticles undergo a gap-opening condensation between 50 and 60 K. Doped UO2 may therefore exhibit novel correlated electron physics that extends beyond that of the cuprate-manganite-pnictide family of compounds.
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Publication Date:
OSTI Identifier:
Report Number(s):
28693; KP1704020
DOE Contract Number:
Resource Type:
Journal Article
Resource Relation:
Journal Name: Physical Review. B, Condensed Matter, 88(11):Article No. 115135
Research Org:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org:
Country of Publication:
United States
Environmental Molecular Sciences Laboratory