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Title: An Octadentate Luminescent Eu(III) 1,2-HOPO Chelate with PotentAqueous Stability

Authors:
; ; ; ;
Publication Date:
Research Org.:
Ernest Orlando Lawrence Berkeley NationalLaboratory, Berkeley, CA (US)
Sponsoring Org.:
USDOE Director, Office of Science; National Institutes ofHealth
OSTI Identifier:
927030
Report Number(s):
LBNL-62517
R&D Project: 403015; BnR: KC0302030
DOE Contract Number:
DE-AC02-05CH11231; NIHHL69832
Resource Type:
Journal Article
Resource Relation:
Journal Name: Inorganic Chemistry; Journal Volume: 46; Journal Issue: 14; Related Information: Journal Publication Date: 06/13/2007
Country of Publication:
United States
Language:
English
Subject:
37

Citation Formats

Moore, Evan G., Jocher, Christoph J., Xu, Jide, Werner, Eric J., and Raymond,Kenneth N. An Octadentate Luminescent Eu(III) 1,2-HOPO Chelate with PotentAqueous Stability. United States: N. p., 2007. Web. doi:10.1021/ic700364t.
Moore, Evan G., Jocher, Christoph J., Xu, Jide, Werner, Eric J., & Raymond,Kenneth N. An Octadentate Luminescent Eu(III) 1,2-HOPO Chelate with PotentAqueous Stability. United States. doi:10.1021/ic700364t.
Moore, Evan G., Jocher, Christoph J., Xu, Jide, Werner, Eric J., and Raymond,Kenneth N. Mon . "An Octadentate Luminescent Eu(III) 1,2-HOPO Chelate with PotentAqueous Stability". United States. doi:10.1021/ic700364t. https://www.osti.gov/servlets/purl/927030.
@article{osti_927030,
title = {An Octadentate Luminescent Eu(III) 1,2-HOPO Chelate with PotentAqueous Stability},
author = {Moore, Evan G. and Jocher, Christoph J. and Xu, Jide and Werner, Eric J. and Raymond,Kenneth N.},
abstractNote = {},
doi = {10.1021/ic700364t},
journal = {Inorganic Chemistry},
number = 14,
volume = 46,
place = {United States},
year = {Mon Feb 26 00:00:00 EST 2007},
month = {Mon Feb 26 00:00:00 EST 2007}
}
  • We report the preparation and new insight into photophysical properties of luminescent hydroxypyridonate complexes [M IIIL] - (M = Eu or Sm) of the versatile 3,4,3-LI(1,2-HOPO) ligand (L). We report the crystal structure of this ligand with EuIII as well as insights into the coordination behavior and geometry in solution by using magnetic circular dichroism. In addition TD-DFT calculations were used to examine the excited states of the two different chromophores present in the 3,4,3-LI(1,2-HOPO) ligand. We find that the Eu III and Sm III complexes of this ligand undergo a transformation after in situ preparation to yield complexes withmore » higher quantum yield (QY) over time. We propose that the lower QY in the in situ complexes is not only due to water quenching but could also be due to a lower degree of f-orbital overlap (in a kinetic isomer) as indicated by magnetic circular dichroism measurements.« less
    Cited by 24
  • We report the preparation and new insight into photophysical properties of luminescent hydroxypyridonate complexes [M IIIL] - (M = Eu or Sm) of the versatile 3,4,3-LI(1,2-HOPO) ligand (L). We report the crystal structure of this ligand with EuIII as well as insights into the coordination behavior and geometry in solution by using magnetic circular dichroism. In addition TD-DFT calculations were used to examine the excited states of the two different chromophores present in the 3,4,3-LI(1,2-HOPO) ligand. We find that the Eu III and Sm III complexes of this ligand undergo a transformation after in situ preparation to yield complexes withmore » higher quantum yield (QY) over time. We propose that the lower QY in the in situ complexes is not only due to water quenching but could also be due to a lower degree of f-orbital overlap (in a kinetic isomer) as indicated by magnetic circular dichroism measurements.« less
  • The luminescence properties of lanthanoid ions can be dramatically enhanced by coupling them to antenna ligands that absorb light in the UV-visible and then efficiently transfer the energy to the lanthanoid centre. The synthesis and the complexation of Ln{sup III} cations (Ln = Eu, Gd) for a ligand based on four 1-hydroxy-2-pyridinone (1,2-HOPO) chelators appended to a ligand backbone derived by linking two L-lysine units (3LI-bis-LYS) is described. This octadentate Eu{sup III} complex ([Eu(3LI-bis-LYS-1,2-HOPO)]{sup -}) has been evaluated in terms of its thermodynamic stability, UV-visible absorption and luminescence properties. For this complex, the conditional stability constant (pM) is 19.9, whichmore » is an order of magnitude higher than diethylenetriaminepentacetic acid at pH = 7.4. This Eu{sup III} complex also shows an almost two-fold increase in its luminescence quantum yield in aqueous solution (pH = 7.4) when compared with other octadentate ligands. Hence, despite a slight decrease of the molar absorption coefficient, a much higher brightness is obtained for [Eu(3LI-bis-LYS-1,2-HOPO)]{sup -}. This overall improvement was achieved by saturating the coordination sphere of the Eu{sup III} cation, yielding an increased metal-centred efficiency by excluding solvent water molecules from the metal's inner sphere.« less