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An Integrated Experimental and Theoretical Study of Actinide Clusters


EMSL Project ID
47888

Abstract

Understanding the chemistry of the actinide elements, in particular uranium, is of critical importance to the mission of the U.S. Department of Energy. With the challenges to develop renewable energy sources, nuclear energy is a viable option to reduce our dependence on fossil fuels. Since UO2 is currently the most common nuclear fuel, a deep understanding of the electronic structures of uranium oxide clusters is warranted; furthermore, related species should be studied to gain further insight into uranium chemistry and form comparisons between alternative nuclear fuels. In addition, uranium carbide and nitrides are also actively investigated as more advanced nuclear fuels. We will study the geometric and electronic structures of gas-phase clusters of the forms UxBy-, UxCy-, UxNy-, and UxOy-, where x=1-2 and y=1-5 through a joint relativistic quantum chemistry and photoelectron spectroscopy technique that will allow us to elucidate the fundamental bonding, structural, and spectroscopic properties of these important species. This work involved two grand computing challenges suitable for use of EMSL supercomputing resources: 1) large global minimum search of the theoretical potential energy surface to determine the structure of each cluster studied and 2) state-specific photoelectron spectroscopy simulations which require calculations using the expensive but accurate CASSCF/CCSD(T)/SO method. Data obtained from this research will provide invaluable information for a fundamental understanding of uranium species which are directly related to the chemistry of nuclear energy and the geochemistry/biogeochemistry and subsurface science area of EMSL.

Project Details

Project type
Large-Scale EMSL Research
Start Date
2013-10-01
End Date
2014-09-30
Status
Closed

Team

Principal Investigator

Lai-Sheng Wang
Institution
Brown University

Team Members

Zachary Piazza
Institution
Brown University

Related Publications

Sergeeva AP, IA Popov, ZA Piazza, WL Li, C Romanescu, LS Wang, and AI Boldyrev. 2014. "Understanding Boron through Size-Selected Clusters: Structure, Chemical Bonding, and Fluxionality." Accounts of Chemical Research 47(4):1349-1358. doi:10.1021/ar400310g