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Correlation between the Covalency and the Thermometric Properties of Yb³⁺/Er³⁺ Codoped Nanocrystalline Orthophosphates.

ABSTRACT: Lanthanide-doped NaYF₄ nanoparticles are most frequently studied host materials for numerous biomedical applications. Although efficient upconversion can be obtained in fluoride nanomaterials and good homogeneity of size and morphology is achieved, they are not very predestined for extensive material optimization toward enhanced features and functions. Here, we study the impact of rare-earth metals RE = Y, Lu, La, and Gd ions within Yb³⁺/Er³⁺ codoped nanocrystalline REPO₄ orthophosphates. The enhanced luminescent thermometry features were found to be in relation to the covalency of RE³⁺-O^2- bonds being modulated by these optically inactive rare-earth ion substitutes. Up to 30% relative sensitivity enhancement was found (from ca. 3.0 to ca. 3.8%/K at -150 °C) by purposefully increasing the covalence of the RE³⁺-O^2- bond. These studies form the basis for intentional optimization thermal couple-based luminescent thermometers such as Yb³⁺-Er³⁺ upconverting ratiometric thermometer.

SUBMITTER: Maciejewska K

PROVIDER: S-EPMC7876742 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature

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Correlation between the Covalency and the Thermometric Properties of Yb3+/Er3+ Codoped Nanocrystalline Orthophosphates.

Maciejewska K K Bednarkiewicz A A Meijerink A A Marciniak L L

The journal of physical chemistry. C, Nanomaterials and interfaces 20210121 4

Lanthanide-doped NaYF4 nanoparticles are most frequently studied host materials for numerous biomedical applications. Although efficient upconversion can be obtained in fluoride nanomaterials and good homogeneity of size and morphology is achieved, they are not very predestined for extensive material optimization toward enhanced features and functions. Here, we study the impact of rare-earth metals RE = Y, Lu, La, and Gd ions within Yb3+/Er3+ codoped nanocrystall ...[more]

PMID: 33584938

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Project description:A family of homodinuclear Ln3+ (Ln3+ = Gd3+, Eu3+) luminescent complexes with the general formula [Ln2(β-diketonato)6(N-oxide)y] has been developed to study the effect of the β-diketonato and N-oxide ligands on their thermometric properties. The investigated complexes are [Ln2(tta)6(pyrzMO)2] (Ln = Eu (1·C7H8), Gd (5)), [Ln2(dbm)6(pyrzMO)2] (Ln = Eu (2), Gd (6)), [Ln2(bta)6(pyrzMO)2] (Ln = Eu (3), Gd (7)), [Ln2(hfac)6(pyrzMO)3] (Ln = Eu (4), Gd (8)) (pyrzMO = pyrazine N-oxide, Htta = thenoyltrifluoroacetone, Hdbm = dibenzoylmethane, Hbta = benzoyltrifluoroacetone, Hhfac = hexafluoroacetylacetone, C7H8 = toluene), and their 4,4'-bipyridine N-oxide (bipyMO) analogues. Europium complexes emit a bright red light under UV radiation at room temperature, whose intensity displays a strong temperature (T) dependence between 223 and 373 K. This remarkable variation is exploited to develop a series of luminescent thermometers by using the integrated intensity of the 5D0 → 7F2 europium transition as the thermometric parameter (Δ). The effect of different β-diketonato and N-oxide ligands is investigated with particular regard to the shape of thermometer calibration (Δ vs T) and relative thermal sensitivity curves: i.e.. the change in Δ per degree of temperature variation usually indicated as Sr (% K-1). The thermometric properties are determined by the presence of two nonradiative deactivation channels, back energy transfer (BEnT) from Eu3+ to the ligand triplet levels and ligand to metal charge transfer (LMCT). In the complexes bearing tta and dbm ligands, whose triplet energy is ca. 20000 cm-1, both deactivation channels are active in the same temperature range, and both contribute to determine the thermometric properties. Conversely, with bta and hfac ligands the response of the europium luminescence to temperature variation is ruled by LMCT channels since the high triplet energy (>21400 cm-1) makes BEnT ineffective in the investigated temperature range.

Dataset Information

Correlation between the Covalency and the Thermometric Properties of Yb³⁺/Er³⁺ Codoped Nanocrystalline Orthophosphates.

Publications

Correlation between the Covalency and the Thermometric Properties of Yb<sup>3+</sup>/Er<sup>3+</sup> Codoped Nanocrystalline Orthophosphates.

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