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Gelation and luminescence of lanthanide hydrogels formed with deuterium oxide.

ABSTRACT: Gel formations and efficient lanthanide luminescence appeared in deuterium oxide (D₂O) medium instead of light water (H₂O), and their solvation possibilities by using luminescence lifetimes were discussed. The lanthanide ions in the hydrogel of 1 obtained by H₂O (abbreviated as H₂O-Ln1; Ln = Eu, Tb, and Gd) in our previous report act as the coupling part between neighbor molecules for the bundle structure. Here, D₂O also acts as a medium to form the lanthanide-hydrogel of 1, and increases intensities of luminescence for Tb, because a soft crystalline state reducing resonance thermal relaxation is realized. The gel-formation and luminescence band positions of Ln1 in D₂O corresponded to those in H₂O. From the observation of luminescence lifetimes in H₂O and D₂O, the number of coordinating water molecules on Eu and Tb were estimated to be around 3 or 4 for both. The luminescence intensity of Eu1 did not increase even in D₂O, due to a blue shift of the excited triplet state of 1, as compared to that in H₂O.

SUBMITTER: Zama Y

PROVIDER: S-EPMC9059775 | biostudies-literature | 2019 Jan

REPOSITORIES: biostudies-literature

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Gelation and luminescence of lanthanide hydrogels formed with deuterium oxide.

Zama Yusuke Y Yanai Kazushige K Takeshita Juri J Ishii Ayumi A Yamanaka Masamichi M Hasegawa Miki M

RSC advances 20190115 4

Gel formations and efficient lanthanide luminescence appeared in deuterium oxide (D2O) medium instead of light water (H2O), and their solvation possibilities by using luminescence lifetimes were discussed. The lanthanide ions in the hydrogel of 1 obtained by H2O (abbreviated as H2O-Ln1; Ln = Eu, Tb, and Gd) in our previous report act as the coupling part between neighbor molecules for the bundle structure. Here, D2O also acts as a medium to ...[more]

PMID: 35516109

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Project description:Ligand-sensitized, luminescent lanthanide(III) complexes are of considerable importance because their unique photophysical properties (microsecond to millisecond lifetimes, characteristic and narrow emission bands, and large Stokes shifts) make them well suited as labels in fluorescence-based bioassays. The long-lived emission of lanthanide(III) cations can be temporally resolved from scattered light and background fluorescence to vastly enhance measurement sensitivity. One challenge in this field is the design of sensitizing ligands that provide highly emissive complexes with sufficient stability and aqueous solubility for practical applications. In this Account, we give an overview of some of the general properties of the trivalent lanthanides and follow with a summary of advances made in our laboratory in the development of highly luminescent Tb(III) and Eu(III) complexes for applications in biotechnology. A focus of our research has been the optimization of these compounds as potential commercial agents for use in homogeneous time-resolved fluorescence (HTRF) technology. Our approach involves developing high-stability octadentate Tb(III) and Eu(III) complexes that rely on all-oxygen donor atoms and using multichromophore chelates to increase molar absorptivity; earlier examples utilized a single pendant chromophore (that is, a single "antenna"). Ligands based on 2-hydroxyisophthalamide (IAM) provide exceptionally emissive Tb(III) complexes with quantum yield values up to approximately 60% that are stable at the nanomolar concentrations required for commercial assays. Through synthetic modification of the IAM chromophore and time-dependent density functional theory (TD-DFT) calculations, we have developed a method to predict absorption and emission properties of these chromophores as a tool to guide ligand design. Additionally, we have investigated chiral IAM ligands that yield Tb(III) complexes possessing both high quantum yield values and strong circularly polarized luminescence (CPL) activity. To efficiently sensitize Eu(III) emission, we have used the 1-hydroxypyridin-2-one (1,2-HOPO) chelate to create remarkable ligands that combine excellent photophysical properties and exceptional aqueous stabilities. A more complete understanding of this chromophore has been achieved by combining low-temperature phosphorescence measurements with the same TD-DFT approach used with the IAM system. Eu(III) complexes with strong CPL activity have also been obtained with chiral 1,2-HOPO ligands. We have also undertaken kinetic analysis of radiative and nonradiative decay pathways for a series of Eu(III) complexes; the importance of the metal ion symmetry on the ensuing photophysical properties is clear. Lastly, we describe a Tb(III)-IAM compound--now carried through to commercial availability--that offers improved performance in the common HTRF platform and has the potential to vastly improve sensitivity.

Dataset Information

Gelation and luminescence of lanthanide hydrogels formed with deuterium oxide.

Publications

Gelation and luminescence of lanthanide hydrogels formed with deuterium oxide.

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