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Highly luminescent scintillating hetero-ligand MOF nanocrystals with engineered Stokes shift for photonic applications.

ABSTRACT: Large Stokes shift fast emitters show a negligible reabsorption of their luminescence, a feature highly desirable for several applications such as fluorescence imaging, solar-light managing, and fabricating sensitive scintillating detectors for medical imaging and high-rate high-energy physics experiments. Here we obtain high efficiency luminescence with significant Stokes shift by exploiting fluorescent conjugated acene building blocks arranged in nanocrystals. Two ligands of equal molecular length and connectivity, yet complementary electronic properties, are co-assembled by zirconium oxy-hydroxy clusters, generating crystalline hetero-ligand metal-organic framework (MOF) nanocrystals. The diffusion of singlet excitons within the MOF and the matching of ligands absorption and emission properties enables an ultrafast activation of the low energy emission in the 100 ps time scale. The hybrid nanocrystals show a fluorescence quantum efficiency of ~60% and a Stokes shift as large as 750 meV (~6000 cm^-1), which suppresses the emission reabsorption also in bulk devices. The fabricated prototypal nanocomposite fast scintillator shows benchmark performances which compete with those of some inorganic and organic commercial systems.

SUBMITTER: Perego J

PROVIDER: S-EPMC9205964 | biostudies-literature | 2022 Jun

REPOSITORIES: biostudies-literature

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Highly luminescent scintillating hetero-ligand MOF nanocrystals with engineered Stokes shift for photonic applications.

Perego J J Bezuidenhout Charl X CX Villa I I Cova F F Crapanzano R R Frank I I Pagano F F Kratochwill N N Auffray E E Bracco S S Vedda A A Dujardin C C Sozzani P E PE Meinardi F F Comotti A A Monguzzi A A

Nature communications 20220617 1

Large Stokes shift fast emitters show a negligible reabsorption of their luminescence, a feature highly desirable for several applications such as fluorescence imaging, solar-light managing, and fabricating sensitive scintillating detectors for medical imaging and high-rate high-energy physics experiments. Here we obtain high efficiency luminescence with significant Stokes shift by exploiting fluorescent conjugated acene building blocks arranged in nanocrystals. Two ligands of equal molecular le ...[more]

PMID: 35715391

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Project description:Glass and ceramic materials doped with rare earth (RE) ions have gained wide interest in photonics as active materials for lasers, optical amplifiers, and luminescent sensors. The emission properties of RE-doped glasses depend on their chemical composition, but they can also be tailored by modifying the surrounding active ions. Typically, this is achieved through heat treatment (including continuous-wave and pulsed lasers) after establishing the ordering mechanisms in the particular glass-RE system. Within the known systems, silicate glasses predominate, while much less work relates to materials with lower energy phonons, which allow more efficient radiation sources to be constructed for photonic applications. In the present work, the luminescent and structural properties of germanate glasses modified with phosphate oxide doped with Eu3+ ions were investigated. Europium dopant was used as a "spectroscopic probe" in order to analyze the luminescence spectra, which characterizes the changes in the local site symmetries of Eu3+ ions. Based on the spectroscopic results, a strong influence of P2O5 content was observed on the excitation and luminescence spectra. The luminescence study of the most intense 5D0→7F2 (electric dipole) transition revealed that the increase in the P2O5 content leads to the linewidth reduction (from 15 nm to 10 nm) and the blue shift (~2 nm) of the emission peak. According to the crystal field theory, the introduction of P2O5 into the glass structure changes the splitting number of sublevels of the 5D0→7F1 (magnetic dipole) transition, confirming the higher polymerization of fabricated glass. The slightly different local environment of Eu3+ centers the results in a number of sites and causes inhomogeneous broadening of spectral lines. It was found that the local asymmetry ratio estimated by the relation of (5D0→7F2)/(5D0→7F1) transitions also confirms greater changes in local symmetry around Eu3+ ions. Our results indicate that modification of germanate glass by P2O5 allows control of their structural properties in order to functionalize the emissions for application as luminescent light sources and sensors.

Dataset Information

Highly luminescent scintillating hetero-ligand MOF nanocrystals with engineered Stokes shift for photonic applications.

Publications

Highly luminescent scintillating hetero-ligand MOF nanocrystals with engineered Stokes shift for photonic applications.

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