Directed Electron Transfer
Lead Research Organisation:
Newcastle University
Department Name: School of Chemistry
Abstract
Electron-transfer processes play key roles in chemical reactions, energy-storage systems and contemporary devices for information transfer. Such reactions are driven by thermodynamics and, given the choice between several partners, electron transfer will generate a thermodynamically stable distribution of products. Selectivity is acquired only by way of proximity and reduction potential. Here, we set out to devise rational ways to direct an electron along one particular pathway when several seemingly identical routes are available. In this case, selectivity is obtained by the choice of excitation wavelength. Low energy excitation of the main chromophore causes electron transfer to a proximal acceptor. Higher energy excitation into the same chromophore causes energy transfer to a secondary chromophore, which subsequently transfers an electron to a distal acceptor. The redox products differ in terms of spin and/or chemical identity. The ultimate achievement within this programme refers to directed electron transfer around a ring. Thus, low energy excitation causes clockwise electron flow but higher energy illumination causes electrons to move around the ring in an anti-clockwise direction.
Organisations
Publications
Benniston A
(2008)
Redox-Controlled Fluorescence Modulation in a BODIPY-Quinone Dyad
in European Journal of Organic Chemistry
Benniston A
(2011)
Thermoresponsive fluorescent polymers based on a quaterthiophene-containing boron dipyrromethene (Bodipy) dyad dispersed in silicone rubber
in Journal of Materials Chemistry
BENNISTON A
(2008)
Controlling electron exchange in molecular assemblies
in Coordination Chemistry Reviews
Benniston AC
(2007)
Competition between energy transfer and interligand electron transfer in porphyrin-osmium(II) bis(2,2':6',2' '-terpyridine) dyads.
in The journal of physical chemistry. A
Benniston AC
(2010)
Bidirectional electron transfer in molecular tetrads.
in Journal of the American Chemical Society
Benniston AC
(2008)
A donor-acceptor molecular dyad showing multiple electronic energy-transfer processes in crystalline and amorphous states.
in Journal of the American Chemical Society
Harriman A
(2009)
Length dependence for intramolecular energy transfer in three- and four-color donor-spacer-acceptor arrays.
in Journal of the American Chemical Society
Ziessel R
(2009)
Boron dipyrrin dyes exhibiting "push-pull-pull" electronic signatures.
in Chemistry (Weinheim an der Bergstrasse, Germany)
Ziessel R
(2009)
Selective triplet-state formation during charge recombination in a fullerene/Bodipy molecular dyad (Bodipy=borondipyrromethene).
in Chemistry (Weinheim an der Bergstrasse, Germany)