Polaron pair mediated triplet generation in polymer/fullerene blends

Stoichko D. Dimitrov (), Scot Wheeler, Dorota Niedzialek, Bob C. Schroeder, Hendrik Utzat, Jarvist M. Frost, Jizhong Yao, Alexander Gillett, Pabitra S. Tuladhar, Iain McCulloch, Jenny Nelson and James R. Durrant ()
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Stoichko D. Dimitrov: Centre for Plastic Electronics, Imperial College London
Scot Wheeler: Centre for Plastic Electronics, Imperial College London
Dorota Niedzialek: Centre for Plastic Electronics, Imperial College London
Bob C. Schroeder: Centre for Plastic Electronics, Imperial College London
Hendrik Utzat: Centre for Plastic Electronics, Imperial College London
Jarvist M. Frost: Centre for Plastic Electronics, Imperial College London
Jizhong Yao: Centre for Plastic Electronics, Imperial College London
Alexander Gillett: Centre for Plastic Electronics, Imperial College London
Pabitra S. Tuladhar: Centre for Plastic Electronics, Imperial College London
Iain McCulloch: Centre for Plastic Electronics, Imperial College London
Jenny Nelson: Centre for Plastic Electronics, Imperial College London
James R. Durrant: Centre for Plastic Electronics, Imperial College London

Nature Communications, 2015, vol. 6, issue 1, 1-8

Abstract: Abstract Electron spin is a key consideration for the function of organic semiconductors in light-emitting diodes and solar cells, as well as spintronic applications relying on organic magnetoresistance. A mechanism for triplet excited state generation in such systems is by recombination of electron-hole pairs. However, the exact charge recombination mechanism, whether geminate or nongeminate and whether it involves spin-state mixing is not well understood. In this work, the dynamics of free charge separation competing with recombination to polymer triplet states is studied in two closely related polymer-fullerene blends with differing polymer fluorination and photovoltaic performance. Using time-resolved laser spectroscopic techniques and quantum chemical calculations, we show that lower charge separation in the fluorinated system is associated with the formation of bound electron-hole pairs, which undergo spin-state mixing on the nanosecond timescale and subsequent geminate recombination to triplet excitons. We find that these bound electron-hole pairs can be dissociated by electric fields.

Date: 2015
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DOI: 10.1038/ncomms7501

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