Intramolecular sensitization of americium luminescence in solution: shining light on short-lived forbidden 5f transitions

Sturzbecher-Hoehne, M.; Yang, P.; D'Aleo, A.; Abergel, R. J.

doi:10.1039/c6dt00328a

Title: Intramolecular sensitization of americium luminescence in solution: shining light on short-lived forbidden 5f transitions

Journal Article · Thu Mar 10 00:00:00 EST 2016 · Dalton Transactions

DOI:https://doi.org/10.1039/c6dt00328a· OSTI ID:1454447

Sturzbecher-Hoehne, M. ^[1]; Yang, P. ^[2]; D'Aleo, A. ^[3]; Abergel, R. J. ^[1]

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Aix-Marseille Univ., CNRS, CINaM UMR, Marseille (France)

In this study, the photophysical properties and solution thermodynamics of water soluble trivalent americium (Am^III) complexes formed with multidentate chromophore-bearing ligands, 3,4,3-LI(1,2-HOPO), Enterobactin, and 5-LIO(Me-3,2-HOPO), were investigated. The three chelators were shown to act as antenna chromophores for AmIII, generating sensitized luminescence emission from the metal upon complexation, with very short lifetimes ranging from 33 to 42 ns and low luminescence quantum yields (10^–3 to 10^–2%), characteristic of Near Infra-Red emitters in similar systems. The specific emission peak of Am^III assigned to the ⁵D₁ → ⁷F₁ f–f transition was exploited to characterize the high proton-independent stability of the complex formed with the most efficient sensitizer 3,4,3-LI(1,2-HOPO), with a log β₁₁₀ = 20.4 ± 0.2 value. In addition, the optical and solution thermodynamic features of these Am^III complexes, combined with density functional theory calculations, were used to probe the influence of electronic structure on coordination properties across the f-element series and to gain insight into ligand field effects.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC02-05CH11231; AC52-06NA25396

OSTI ID:: 1454447

Alternate ID(s):: OSTI ID: 1246892

Report Number(s):: LA-UR-16-20418; ICHBD9; ark:/13030/qt2xf4r3h7

Journal Information:: Dalton Transactions, Vol. 45, Issue 24; Related Information: © 2016 The Royal Society of Chemistry.; ISSN 1477-9226

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 19 works

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