Quantum mechanical study of the solvent-dependence of electronic energy transfer rates in a Bodipy closely-spaced dyad

Title	Quantum mechanical study of the solvent-dependence of electronic energy transfer rates in a Bodipy closely-spaced dyad
Publication Type	Journal Article
Year of Publication	2011
Authors	Caprasecca, S, Curutchet C, Mennucci B
Journal	Photochemical & Photobiological Sciences
Volume	10
Issue	10
Pagination	1602 - 1609
Date Published	2011
ISBN Number	1474-905X
Keywords	anisotropic dielectrics, exchange, field, forster theory, model dyad, molecules
Abstract	The ability of Forster theory to describe electronic energy transfer rates, and their solvent-dependence, have been studied theoretically in a series of 15 solvents of varying degrees of polarity for a rigid closely-spaced dyad, constituted by two boron dipyrromethene dyes, which was recently studied experimentally by Harriman & Ziessel, Photochem. Photobiol. Sci., 2010, 9, 960. We use time-dependent density functional theory calculations coupled to the polarizable continuum model to analyse the solvent-dependence of the spectroscopic and energy transfer properties of the system. This methodology allows us to examine the impact of the solvent on both electronic (solvent screening) and structural (dipole separation and orientation) factors by consistently incorporating solvent effects in the determination of molecular geometries, transition densities, and electronic couplings. In addition, we analyse the impact of bridge-mediated contributions to the electronic interaction between the dyes. We are therefore able to assess whether a Forster-type point-dipole approximation is valid for the molecular system studied.

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