Energy Transfer from Antenna Ligand to Europium(III) Followed Using Ultrafast Optical and X-ray Spectroscopy

Mara, Michael W.; Tatum, David S.; March, Anne-Marie; Doumy, Gilles; Moore, Evan G.; Raymond, Kenneth N.

doi:10.1021/jacs.9b02792

Title: Energy Transfer from Antenna Ligand to Europium(III) Followed Using Ultrafast Optical and X-ray Spectroscopy

Journal Article · 23 June 2019 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.9b02792 · OSTI ID:1559459

^[1]; Tatum, David S. ^[2];

^[3]; Doumy, Gilles ^[3];

^[4];

^[2]

Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Univ. of Queensland, Brisbane (Australia)

A series of highly luminescent europium(III) complexes which exhibit photoluminescence from the Eu(III) center following energy transfer from the UV absorbing organic sensitizer have been investigated using a combination of ultrafast optical transient absorption and Eu L3 X-ray transient absorption techniques. We have previously demon- strated that the latter can be used as a signature of 4f–4f excitation responsible for the photoluminescence in these Eu(III) coordination complexes, but the long time scale of the earlier measurements did not allow direct observation of the ligand-to-metal energy transfer step, preventing a determi- nation of the sensitization mechanism. Here, we provide the first direct experimental verification that Dexter electron exchange from the ligand triplet state is the dominant energy transfer mechanism in these photoluminescent systems. Moreover, the optical transient absorption results obtained herein imply that energy transfer for all three compounds has near unity yield, regardless of differences in the sensitization efficiencies, suggesting that the variations in the sensitization efficiencies are determined almost entirely by differences in the ligand-centered intersystem crossing rates. As a result, the implications for the rational design of more effective photoluminescent lanthanide complexes are discussed.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

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

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1559459

Journal Information:: Journal of the American Chemical Society, Vol. 141, Issue 28; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 53 works

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