Near-infrared C-term MCD spectroscopy of octahedral uranium (V) complexes

Curran, Daniel J.; Ganguly, Gaurab; Heit, Yonaton N.; Wolford, Nikki J.; Minasian, Stefan G.; Löble, Matthias W.; Cary, Samantha K.; Kozimor, Stosh A.; Autschbach, Jochen; Neidig, Michael L.

doi:10.1039/d1dt00513h

Title: Near-infrared C-term MCD spectroscopy of octahedral uranium (V) complexes

Journal Article · Thu Apr 01 00:00:00 EDT 2021 · Dalton Transactions

DOI:https://doi.org/10.1039/d1dt00513h· OSTI ID:1874921

Curran, Daniel J. ^[1];

^[2]; Heit, Yonaton N. ^[2];

^[1];

^[3]; Löble, Matthias W. ^[2]; Cary, Samantha K. ^[2];

^[4];

^[2];

^[1]

Univ. of Rochester, NY (United States)
State Univ. of New York at Buffalo, NY (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

C-term magnetic circular dichroism (MCD) spectroscopy is a powerful method for probing d–d and f–f transitions in paramagnetic metal complexes. However, this technique remains underdeveloped both experimentally and theoretically for studies of U(V) complexes of Oh symmetry, which have been of longstanding interest for probing electronic structure, bonding, and covalency in 5f systems. In this study, C-term NIR MCD of the Laporte forbidden f–f transitions of [UCl₆]^- and [UF₆]^- are reported, demonstrating the significant fine structure resolution possible with this technique including for the low energy Γ₇ → Γ₈ transitions in [UF₆]^-. The experimental NIR MCD studies were further extended to [U(OC₆F₅)₆]^-, [U(CH₂SiMe₃)₆]^-, and [U(NC(tBu)(Ph))₆]^- to evaluate the effects of ligand-type on the f–f MCD fine structure features. Theoretical calculations were conducted to determine the Laporte forbidden f–f transitions and their MCD intensity experimentally observed in the NIR spectra of the U(V) hexahalide complexes, via the inclusion of vibronic coupling, to better understand the underlying spectral fine structure features for these complexes. These spectra and simulations provide an important platform for the application of MCD spectroscopy to this widely studied class of U(V) complexes and identify areas for continued theoretical development.

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

Sponsoring Organization:: USDOE Office of Science (SC). Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: 89233218CNA000001; SC0016002; SC0001136; AC02-05CH11231; 2020LANLE372

OSTI ID:: 1874921

Alternate ID(s):: OSTI ID: 1773551

Report Number(s):: LA-UR-21-21245; TRN: US2307158

Journal Information:: Dalton Transactions, Vol. 50, Issue 16; ISSN 1477-9226

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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