Novel luminescent silicone hybrids (LSHs) containing lanthanide ions were prepared via different sol-gel processes. The precursor, dimethyl ester-functionalized silane, was synthesized via a facile amino-ene reaction. The coordinated assembly of the ester ligands and lanthanide ions (Eu(3+), Tb(3+) and Dy(3+)) occurred. The ester ligands were immobilized onto the Si-O network backbone during the preparation of the silicone hybrid materials. The particle size can be controlled to ca 50 nm by adjusting the solvent ratio. The obtained materials were characterized by Fourier transform infrared, (1)H nuclear magnetic resonance spectroscopy (NMR), (13)C NMR, (28)Si NMR, X-ray diffraction, X-ray photoelectron spectroscopy, thermogravimetric analysis, high-resolution scanning electronic microscopy and luminescent (excitation and emission) spectroscopy. The coordination state and photophysical performance of the compounds were studied in detail. The terbium- and europium-containing materials show sharp green and red emissions, respectively, which indicate that efficient intramolecular energy transfer took place in these LSHs.
A series of theoretical calculations were performed on thienyl-functionalized polysilanes in order to understand their geometries, excited state spectra, energy band structures, and adsorption stability onto Au (111) surfaces. The thienyl functionalization causes a significant red-shift of the electronic spectra of the oligosilanes, which is due to the maximum absorption energy resulting from r ? p* transition in oligo(methylthienylsilane) much lower than that from r ? r* transition, and a great decrease of the r ? r* transition energy in thienyl endfunctionalized oligo(dimethylsilane). The thienyl substitution exerts a small effect on the band gap of the polysilane, and yet disturbs slightly the r electronic delocalization. There exists a stable adsorption between thienyl-functionalized polysilanes and Au (111) surfaces through nonbonding interaction of thiophenes with Au.
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