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Title: Highly Luminescent Lanthanide Complexes of 1 Hydroxy-2-pyridinones

The synthesis, X-ray structure, stability, and photophysical properties of several trivalent lanthanide complexes formed from two differing bis-bidentate ligands incorporating either alkyl or alkyl ether linkages and featuring the 1-hydroxy-2-pyridinone (1,2-HOPO) chelate group in complex with Eu(III), Sm(III) and Gd(III) are reported. The Eu(III) complexes are among some of the best examples, pairing highly efficient emission ({Phi}{sub tot}{sup Eu} {approx} 21.5%) with high stability (pEu {approx} 18.6) in aqueous solution, and are excellent candidates for use in biological assays. A comparison of the observed behavior of the complexes with differing backbone linkages shows remarkable similarities, both in stability and photophysical properties. Low temperature photophysical measurements for a Gd(III) complex were also used to gain insight into the electronic structure, and were found to agree with corresponding TD-DFT calculations for a model complex. A comparison of the high resolution Eu(III) emission spectra in solution and from single crystals also revealed a more symmetric coordination geometry about the metal ion in solution due to dynamic rotation of the observed solid state structure.
Authors:
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Publication Date:
OSTI Identifier:
927871
Report Number(s):
LBNL-192E
Journal ID: ISSN 0020-1669; INOCAJ; TRN: US200816%%1104
DOE Contract Number:
DE-AC02-05CH11231
Resource Type:
Journal Article
Resource Relation:
Journal Name: Inorganic Chemistry
Research Org:
Ernest Orlando Lawrence Berkeley National Laboratory, Berkeley, CA (US)
Sponsoring Org:
Chemical Sciences Division
Country of Publication:
United States
Language:
English
Subject:
37; AQUEOUS SOLUTIONS; CHELATES; ELECTRONIC STRUCTURE; EMISSION SPECTRA; ETHERS; GEOMETRY; MONOCRYSTALS; RARE EARTHS; RESOLUTION; ROTATION; STABILITY; SYNTHESIS DELFIA(R) DNA