Structural and Spectroscopic Comparison of Soft‐Se vs. Hard‐O Donor Bonding in Trivalent Americium/Neodymium Molecules

Goodwin, Conrad A. P.; Schlimgen, Anthony W.; Albrecht‐Schönzart, Thomas E.; Batista, Enrique R.; Gaunt, Andrew J.; Janicke, Michael T.; Kozimor, Stosh A.; Scott, Brian L.; Stevens, Lauren M.; White, Frankie D.; Yang, Ping

doi:10.1002/ange.202017186

Title: Structural and Spectroscopic Comparison of Soft‐Se vs. Hard‐O Donor Bonding in Trivalent Americium/Neodymium Molecules

Journal Article · Wed Mar 10 00:00:00 EST 2021 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202017186· OSTI ID:1786144

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Chemistry Division Los Alamos National Laboratory Los Alamos NM 87545 USA
Theoretical Division Los Alamos National Laboratory Los Alamos NM 87545 USA
Department of Chemistry and Biochemistry Florida State University 95 Chieftain Way Tallahassee FL 32306 USA
Materials Physics and Applications Division Los Alamos National Laboratory Los Alamos NM 87545 USA

Abstract Covalency is often considered to be an influential factor in driving An ³⁺ vs. Ln ³⁺ selectivity invoked by soft donor ligands. This is intensely debated, particularly the extent to which An ³⁺ /Ln ³⁺ covalency differences prevail and manifest as the f‐block is traversed, and the effects of periodic breaks beyond Pu. Herein, two Am complexes, [Am{N(E=PPh ₂ ) ₂ } ₃ ] ( 1‐Am , E=Se; 2‐Am , E=O) are compared to isoradial [Nd{N(E=PPh ₂ ) ₂ } ₃ ] ( 1‐Nd , 2‐Nd ) complexes. Covalent contributions are assessed and compared to U/La and Pu/Ce analogues. Through ab initio calculations grounded in UV‐vis‐NIR spectroscopy and single‐crystal X‐ray structures, we observe differences in f orbital involvement between Am–Se and Nd–Se bonds, which are not present in O‐donor congeners.

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Sponsoring Organization:: USDOE

OSTI ID:: 1786144

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Vol. 133 Journal Issue: 17; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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