Absorption and emission spectra of fluorescent silica nanoparticles from TD-DFT/MM/PCM calculations.

TitleAbsorption and emission spectra of fluorescent silica nanoparticles from TD-DFT/MM/PCM calculations.
Publication TypeJournal Article
Year of Publication2011
AuthorsPedone, A, Prampolini, G, Monti, S, Barone, V
JournalPhysical Chemistry Chemical Physics
Volume13
Pagination16689–97
ISSN1463-9084
Abstract

A multi-scale computational protocol, which combines Quantum Mechanics and Molecular Mechanics (QM/MM) calculations with the polarisable continuum model (PCM), has been used to study the tetramethylrhodamine isothiocyanate (TRITC) fluorophore, embedded in three different environments, namely in water, on an amorphous silica surface and covalently encapsulated in a silica nanoparticle (C dot). Absorption and emission spectra have been simulated by using TD-B3LYP/PCM calculations, performed on the TRITC ground and excited state geometries, optimized at the QM/MM level. The results are in good agreement with experimental data confirming the caging effect played by the silica shell on the mobility of the TRITC molecule when covalently encapsulated in silica nanoparticles. This could result in a decrease of the nonradiative decay rate and thus an increase of the quantum yield of the molecule.

DOI10.1039/c1cp21475f