Dataset Information

Up-Conversion Luminescence Properties of Lanthanide-Gold Hybrid Nanoparticles as Analyzed with Discrete Dipole Approximation.

ABSTRACT: Up-conversion nanoparticles (UCNP) under near-infrared (NIR) light irradiation have been well investigated in the field of bio-imaging. However, the low up-conversion luminescence (UCL) intensity limits applications. Plasmonic modulation has been proposed as an effective tool to adjust the luminescence intensity and lifetime. In this study discrete dipole approximation (DDA) was explored concerning guiding the design of UCNP@mSiO?-Au structures with enhanced UCL intensity. The extinction effects of gold shells could be changed by adjusting the distance between the UCNPs and the Au NPs by synthesized tunable mesoporous silica (mSiO?) spacers. Enhanced UCL was obtained under 808 nm irradiation. The original theoretical predictions could not be demonstrated to full extend by experimental data, indicating that better models for simulation need to take into account in homogeneities in particle morphologies. Yet, one very certain conclusion resulting from the DDA calculations and experiments is that the absorbance can blue-shift with more Au NPs added and the absorbance can-red shift for samples with enhanced silica sizes in the UCNP@mSiO?-Au structures. Furthermore, when the DDA model is more consistent with the practical structure (dispersed Au NPs instead of Au shell), the theoretical absorbance occurs almost the same as the practical absorbance. All in all, the DDA could fit the extinction effect of Au perfectly and be suitable for guiding how to design the UCNP and Au.

SUBMITTER: Lv R

PROVIDER: S-EPMC6315549 | biostudies-literature | 2018 Nov

REPOSITORIES: biostudies-literature

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Up-Conversion Luminescence Properties of Lanthanide-Gold Hybrid Nanoparticles as Analyzed with Discrete Dipole Approximation.

Lv Ruichan R Feng Miao M Parak Wolfgang J WJ

Nanomaterials (Basel, Switzerland) 20181129 12

Up-conversion nanoparticles (UCNP) under near-infrared (NIR) light irradiation have been well investigated in the field of bio-imaging. However, the low up-conversion luminescence (UCL) intensity limits applications. Plasmonic modulation has been proposed as an effective tool to adjust the luminescence intensity and lifetime. In this study discrete dipole approximation (DDA) was explored concerning guiding the design of UCNP@mSiO₂-Au structures with enhanced UCL intensity. The extinction effects ...[more]

PMID: 30501026

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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

Up-Conversion Luminescence Properties of Lanthanide-Gold Hybrid Nanoparticles as Analyzed with Discrete Dipole Approximation.

Publications

Up-Conversion Luminescence Properties of Lanthanide-Gold Hybrid Nanoparticles as Analyzed with Discrete Dipole Approximation.

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