Covalency in Americium(III) Hexachloride

Cross, Justin Neil; Su, Jing; Batista, Enrigue R.; Schrell, Samantha K.; Evans, William J; Kozimor, Stosh A.; Mocko, Veronika; Scott, Brian L.; Stein, Benjamin A.; Windorff, Cory J.; Yang, Ping

doi:10.1021/jacs.7b03755

Title: Covalency in Americium(III) Hexachloride

Journal Article · Wed Jun 14 00:00:00 EDT 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b03755· OSTI ID:1371672

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^[1]; Evans, William J ^[2];

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^[1]; Windorff, Cory J. ^[3];

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Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Univ. of California, Irvine, CA (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of California, Irvine, CA (United States)

Developing a better understanding of covalency (or orbital mixing) is of fundamental importance. Covalency occupies a central role in directing chemical and physical properties for almost any given compound or material. Hence, the concept of covalency has potential to generate broad and substantial scientific advances, ranging from biological applications to condensed matter physics. Given the importance orbital mixing combined with the difficultly in measuring covalency, estimating or inferring covalency often leads to fiery debate. Consider the 60-year controversy sparked by SEABORG and COWORKERS (1954) when it was proposed that covalency from 5f-orbitals contributed to the unique behavior of americium in chloride matrixes. Herein, we describe the use of ligand K-edge X-ray absorption spectroscopy (XAS) and electronic structure calculations to quantify the extent of covalent bonding in – arguably – one of the most difficult systems to study, the Am–Cl interaction within AmCl₆^3-. We observed both 5fand 6d-orbital mixing with the Cl-3p orbitals; however, contributions from the 6d-orbitals were more substantial. Comparisons with the isoelectronic EuCl₆^3- indicated similar bonding for the Am^III 6d- and Eu^III 5d-orbitals. Meanwhile, the results confirmed SEABORG’S 1954 hypothesis that Am^III 5f-orbital covalency was more substantial than 4forbital mixing for Eu^III.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC). Nuclear Physics (NP) (SC-26); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC52-06NA25396; AC05-06OR23100; SC0004739; AC02-76SF00515

OSTI ID:: 1371672

Report Number(s):: LA-UR-17-22510; TRN: US1702332

Journal Information:: Journal of the American Chemical Society, Vol. 139, Issue 25; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 58 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Americium · Covalency · X-ray Absorption · Crystallography · Bonding · UV-Vis-NIR · Density Functional Theory · Spin-Orbit Coupling
Americium
Covalency
X-ray Absorption
Crystallography
Bonding
UV-Vis-NIR
Density Functional Theory
Spin-Orbit Coupling

Title: Covalency in Americium(III) Hexachloride

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