title: Probing Chemical Bonding and Electronic Structures in ThO-by Anion Photoelectron Imaging and Theoretical Calculations.
abstract: Because of renewed research on thorium-based molten salt reactors, there is growing demand and interest in enhancing the knowledge of thorium chemistry both experimentally and theoretically. Compared with uranium, thorium has few chemical studies reported up to the present. Here we report the vibrationally resolved photoelectron imaging of the thorium monoxide anion. The electron affinity of ThO is first reported to be 0.707 ± 0.020 eV. Vibrational frequencies of the ThO molecule and its anion are determined from Franck-Condon simulation. Spectroscopic evidence is obtained for the two-electron transition in ThO-, indicating the strong electron correlation among the (7sσ)2(6dδ)1electrons in ThO-and the (7sσ)2electrons in ThO. These findings are explained by using quantum-chemical calculations including spin-orbit coupling, and the chemical bonding of gaseous ThO molecules is analyzed. The present work will enrich our understanding of bonding capacities with the 6d valence shell.
authors.affiliation: Shanghai Institute of Applied Physics, Chinese Academy of Sciences , Shanghai 201800, China.
authors.forename: Yanli
authors.initials: Y
authors.lastname: Li
authors.affiliation: State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian 116023, China.
authors.forename: Jinghan
authors.initials: J
authors.lastname: Zou
authors.affiliation: Shanghai Institute of Applied Physics, Chinese Academy of Sciences , Shanghai 201800, China.
authors.forename: Xiao-Gen
authors.initials: XG
authors.lastname: Xiong
authors.affiliation: Shanghai Institute of Applied Physics, Chinese Academy of Sciences , Shanghai 201800, China.
authors.forename: Jing
authors.initials: J
authors.lastname: Su
authors.affiliation: State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian 116023, China.
authors.forename: Hua
authors.initials: H
authors.lastname: Xie
authors.affiliation: Shanghai Institute of Applied Physics, Chinese Academy of Sciences , Shanghai 201800, China.
authors.forename: Zejie
authors.initials: Z
authors.lastname: Fei
authors.affiliation: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University , Xiamen 361005, China.
authors.forename: Zichao
authors.initials: Z
authors.lastname: Tang
authors.affiliation: Shanghai Institute of Applied Physics, Chinese Academy of Sciences , Shanghai 201800, China.
authors.forename: Hongtao
authors.identifier: http://orcid.org/0000-0001-6450-2585
authors.initials: H
authors.lastname: Liu