Modelling the luminescence of extended solids: an example of a highly luminescent MCM-41 impregnated with a Eu3+ beta-diketonate complex
authors Felicio, MR; Nunes, TG; Vaz, PM; Botas, AMP; Ribeiro-Claro, P; Ferreira, RAS; Freire, RO; Vaz, PD; Carlos, LD; Nunes, CD; Nolasco, MM
nationality International
journal JOURNAL OF MATERIALS CHEMISTRY C
keywords ORGANIC-INORGANIC HYBRIDS; INTRAMOLECULAR ENERGY-TRANSFER; EMISSION QUANTUM YIELD; RARE-EARTH COMPLEX; MESOPOROUS SILICA; COORDINATION-COMPOUNDS; SPECTROSCOPIC PROPERTIES; PHOTOPHYSICAL PROPERTIES; LANTHANIDE LUMINESCENCE; DIFFERENTIAL-OVERLAP
abstract A regular MCM-41 type mesostructured silica was used as a support for the incorporation of the highly luminescent tris(beta-diketonate) complex Eu(tta)(3)ephen yielding the hybrid MCM-Eu material. Suitable characterization by powder X-ray diffraction (XRD), thermogravimetric analyses (TGA), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), C-13 and Si-21 solid state NMR spectroscopy and photoluminescence was accomplished. The combination of ultraviolet-visible spectroscopy (UV-Vis) and photoluminescence techniques shows that the complex incorporation seems to modify essentially the second Eu3+ coordination shell. For a material that has a simply impregnated lanthanide complex, the herein reported maximum D-5(0) quantum yield value of 0.31 is a significantly high value, being almost in the same scale of the values obtained for the materials with covalently bonded complexes. A detailed theoretical photoluminescence study of the MCM-Eu with the recently developed Luminescence Package - LUMPAC is presented. The high accuracy of the theoretical calculations is achieved through the comparison with the experimental values. Aiming at a deeper understanding of the photoluminescence process, the ligand-to-Eu3+ intramolecular energy transfer and back-transfer rates were also predicted. The dominant pathway involves the energy transfer between the lowest energy ligand triplet and the D-5(0) level (9.70 x 10(7) s(-1)).
publisher ROYAL SOC CHEMISTRY
issn 2050-7526
year published 2014
volume 2
issue 45
beginning page 9701
ending page 9711
digital object identifier (doi) 10.1039/c4tc01072h
web of science category Materials Science, Multidisciplinary; Physics, Applied
subject category Materials Science; Physics
unique article identifier WOS:000344470400019
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journal impact factor 5.976
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