Polaron pair mediated triplet generation in polymer/fullerene blends

Nature Communications
Stoichko D DimitrovJames R Durrant

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.

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Citations

Oct 7, 2015·Journal of the American Chemical Society·Ajith R MalliaMahesh Hariharan
Jul 23, 2015·Journal of the American Chemical Society·Rolf AndernachHugo Bronstein
Oct 11, 2016·Chemical Reviews·Oksana Ostroverkhova
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Aug 15, 2020·Chemical Society Reviews·Devika SasikumarMahesh Hariharan
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Jan 13, 2016·Polymers·Stoichko D DimitrovJames R Durrant
Jan 22, 2021·Nature Communications·Ivan RamirezMoritz Riede
Mar 16, 2021·Journal of the American Chemical Society·Rui WangMin Xiao
May 22, 2021·The Journal of Physical Chemistry Letters·Philip C Y ChowKam Sing Wong
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Nov 14, 2021·Advanced Materials·Jiaying WuJames R Durrant

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Methods Mentioned

BETA
X-ray
transmission electron microscopy

Software Mentioned

Matlab
origin
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