Recent studies have unveiled the similar nature of solvent (screening) effects and bridge-mediated contributions to electronic energy transfer, both related to the bridge/solvent polarizability properties. Here, we exploit the similarity of such contributions to develop a fully polarizable mixed QM/discrete/continuum model aimed at studying electronic energy transfer processes in supramolecular systems. In the model, the definition of the three regions is completely flexible and allows us to explore the possibility to describe bridge mediated contributions by using a polarizable MM description of the linker. In addition, we show that the classical MMPol description of the bridge can be complemented either with an analogous atomistic or with a continuum description of the solvent. Advantages and drawbacks of the model are finally presented and discussed with respect to the system under study.

Toward a Unified Modeling of Environment and Bridge-Mediated Contributions to Electronic Energy Transfer: A Fully Polarizable QM/MM/PCM Approach

CAPRASECCA, STEFANO;CURUTCHET BARAT, CARLES EDUARD;MENNUCCI, BENEDETTA
2012-01-01

Abstract

Recent studies have unveiled the similar nature of solvent (screening) effects and bridge-mediated contributions to electronic energy transfer, both related to the bridge/solvent polarizability properties. Here, we exploit the similarity of such contributions to develop a fully polarizable mixed QM/discrete/continuum model aimed at studying electronic energy transfer processes in supramolecular systems. In the model, the definition of the three regions is completely flexible and allows us to explore the possibility to describe bridge mediated contributions by using a polarizable MM description of the linker. In addition, we show that the classical MMPol description of the bridge can be complemented either with an analogous atomistic or with a continuum description of the solvent. Advantages and drawbacks of the model are finally presented and discussed with respect to the system under study.
2012
Caprasecca, Stefano; CURUTCHET BARAT, CARLES EDUARD; Mennucci, Benedetta
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11568/156196
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