Spin selective charge recombination in chiral donor-bridge-acceptor triads

Kavli Affiliate: David T. Limmer

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| Summary:

In this paper we outline a physically motivated framework for describing
spin-selective recombination processes in chiral systems, from which we derive
spin-selective reaction operators for recombination reactions of
donor-bridge-acceptor molecules, where the electron transfer is mediated by
chirality and spin-orbit coupling. In general the recombination process is
selective only for spin-coherence between singlet and triplet states, and it is
not in general selective for spin polarisation. We find that spin polarisation
selectivity only arises in hopping mediated electron transfer. We describe how
this effective spin-polarisation selectivity is a consequence of
spin-polarisation generated transiently in the intermediate state. The
recombination process also augments the coherent spin dynamics of the charge
separated state, which is found to have a significant effect on recombination
dynamics and to destroy any long-lived spin polarisation. Although we only
consider a simple donor-bridge-acceptor system, the framework we present here
can be straightforwardly extended to describe spin-selective recombination
processes in more complex systems.

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