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Toward effective and reliable fluorescence energies in solution by a new state specific polarizable continuum model time dependent density functional theory approach (80 visite)

Improta R, Scalmani G, Frisch MJ, Barone V

J Chem Phys (ISSN: 0021-9606, 0897-690online), 2007 Sep 21; 127(7): N/D-N/D.

Tipo di articolo: Journal Article, Abstract, Conference, Research Support, Non-U. S. Gov'T,

Impact factor: 3.044

Impact factor a 5 anni: 3.043


Parole chiave: Density Functional Theory, Fluorescence, Ground State, Optimization, Phosphorescence, Relaxation Time, Solvents, Continuum Models, Dynamical Solvents, Linear Response (lr) Models, Solutions, Alcohol, Coumarin Derivative, Formaldehyde, Water, Article, Chemical Model, Chemistry, Luminescence, Spectrofluorometry, Statistical Model, Theoretical Model, Ethanol, Luminescent Measurements, Spectrometry, Time Factors, Coumarins Chemistry, Ethanol Chemistry, Formaldehyde Chemistry, Solvents Chemistry, Water Chemistry,

Url: http://www.scopus.com/inward/record.url?eid=2-s2.0-34548058138&partnerID=40&md5=b53226a2fcedc7a67a2bb646b25492a1

A state specific (SS) model for the inclusion of solvent effects in time dependent density functional theory (TD-DFT) computations of emission energies has been developed and coded in the framework of the so called polarizable continuum model (PCM). The new model allows for a rigorous and effective treatment of dynamical solvent effects in the computation of fluorescence and phosphorescence spectra in solution, and it can be used for studying different relaxation time regimes. SS and conventional linear response (LR) models have been compared by computing the emission energies for different benchmark systems (formaldehyde in water and three coumarin derivatives in ethanol). Special attention is given to the influence of dynamical solvation effects on LR geometry optimizations in solution. The results on formaldehyde point out the complementarity of LR and SS approaches and the advantages of the latter model especially for polar solvents and/or weak transitions. The computed emission energies for coumarin derivatives are very close to their experimental counterparts, pointing out the importance of a proper treatment of nonequilibrium solvent effects on both the excited and the ground state energies. The availability of SS-PCM/TD-DFT models for the study of absorption and emission processes allows for a consistent treatment of a number of different spectroscopic properties in solution. © 2007 American Institute of Physics.
*** IBB - CNR ***

Dipartimento di Chimica, Universit̀ Federico II, Complesso Monte S. Angelo, via Cintia, I-80126 Napoli, Italy

Istituto di Biostrutture e Bioimmagini-CNR, via Mezzocannone 16, 80134 Napoli, Italy

Gaussian, Inc., Wallingford, CT 06492, United States
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28 Records (24 escludendo Abstract e Conferenze).
Impact factor totale: 91.088 (87.027 escludendo Abstract e Conferenze).
Impact factor a 5 anni totale: 96.262 (91.847 escludendo Abstract e Conferenze).







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