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Tytuł pozycji:

Probing the electronic structures of low oxidation-state uranium fluoride molecules UFx- (x = 2-4).

Tytuł :
Probing the electronic structures of low oxidation-state uranium fluoride molecules UFx- (x = 2-4).
Autorzy :
Li, Wei-Li
Hu, Han-Shi
Jian, Tian
Lopez, Gary V.
Su, Jing
Li, Jun
Wang, Lai-Sheng
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Temat :
ELECTRONIC structure
OXIDATION states
URANIUM fluorides
ANIONS
PHOTOELECTRON spectroscopy
ELECTRON affinity
CHEMICAL bonds
QUANTUM chemistry
Źródło :
Journal of Chemical Physics; Dec2013, Vol. 139 Issue 24, p244303, 8p, 1 Diagram, 3 Charts, 3 Graphs
Czasopismo naukowe
We report the experimental observation of gaseous UFx- (x = 2-4) anions, which are investigated using photoelectron spectroscopy and relativistic quantum chemistry. Vibrationally resolved photoelectron spectra are obtained for all three species and the electron affinities of UFx (x = 2-4) are measured to be 1.16(3), 1.09(3), and 1.58(3) eV, respectively. Significant multi-electron transitions are observed in the photoelectron spectra of U(5f37s2)F2-, as a result of strong electron correlation effects of the two 7s electrons. The U-F symmetric stretching vibrational modes are resolved for the ground states of all UFx (x = 2-4) neutrals. Theoretical calculations are performed to qualitatively understand the photoelectron spectra. The entire UFx- and UFx (x = 1-6) series are considered theoretically to examine the trends of U-F bonding and the electron affinities as a function of fluorine coordination. The increased U-F bond lengths and decreased bond orders from UF2- to UF4- indicate that the U-F bonding becomes weaker as the oxidation state of U increases from I to III. [ABSTRACT FROM AUTHOR]
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