Tuning Photoinduced Electron Transfer in POM‐bodipy Hybrids by Controlling the Environment, Experiment and Theory. - Archive ouverte HAL Access content directly
Journal Articles Angewandte Chemie International Edition Year : 2021

Tuning Photoinduced Electron Transfer in POM‐bodipy Hybrids by Controlling the Environment, Experiment and Theory.

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Albert Masip-Sánchez
  • Function : Author
Xavier López
  • Function : Author
Pavel Chabera
  • Function : Author
Ian P Clark
  • Function : Author
  • PersonId : 1088319
Tönu Pullerits
  • Function : Author
  • PersonId : 1088320
Josep M Poblet
  • Function : Author
  • PersonId : 1088321
Elizabeth A Gibson
  • Function : Author
  • PersonId : 980677
Guillaume Izzet

Abstract

The optical and electrochemical properties of a series of polyoxometalates (POMs) oxoclusters decorated with two bodipy (boron-dipyrromethene) light harvesting units were examined. We evaluated in this polyanionic donor-acceptor system the effect of the solvent and associated counterions on the intramolecular photoinduced electron transfer. Our results show that both solvents and counterions have a major impact upon the energy of the charge transfer state by modifying the solvation shell around the POM. This leads to a significantly shorter charge separation time in case of smaller counterion and slower charge recombination in a less polar solvent. We rationalize these results in terms of Marcus theory and show that solvent and counterion both affect the driving force for photoinduced electron transfer and the reorganization energy. This was corroborated with theoretical investigations combining DFT and molecular dynamics simulations.
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Dates and versions

hal-03107704 , version 1 (12-01-2021)

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Georgios Toupalas, Joshua Karlsson, Fiona A Black, Albert Masip-Sánchez, Xavier López, et al.. Tuning Photoinduced Electron Transfer in POM‐bodipy Hybrids by Controlling the Environment, Experiment and Theory.. Angewandte Chemie International Edition, In press, ⟨10.1002/anie.202014677⟩. ⟨hal-03107704⟩
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