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The role of spin in the degradation of organic photovoltaics

Abstract:
Stability is now a critical factor in the commercialization of organic photovoltaic (OPV) devices. Both extrinsic stability to oxygen and water and intrinsic stability to light and heat in inert conditions must be achieved. Triplet states are known to be problematic in both cases, leading to singlet oxygen production or fullerene dimerization. The latter is thought to proceed from unquenched singlet excitons that have undergone intersystem crossing (ISC). Instead, we show that in bulk heterojunction (BHJ) solar cells the photo-degradation of C<sub>60</sub> via photo-oligomerization occurs primarily via back-hole transfer (BHT) from a charge-transfer state to a C<sub>60</sub> excited triplet state. We demonstrate this to be the principal pathway from a combination of steady-state optoelectronic measurements, time-resolved electron paramagnetic resonance, and temperature-dependent transient absorption spectroscopy on model systems. BHT is a much more serious concern than ISC because it cannot be mitigated by improved exciton quenching, obtained for example by a finer BHJ morphology. As BHT is not specific to fullerenes, our results suggest that the role of electron and hole back transfer in the degradation of BHJs should also be carefully considered when designing stable OPV devices.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1038/s41467-020-20601-6

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Role:
Author
ORCID:
0000-0002-7062-8077
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Role:
Author
ORCID:
0000-0001-7568-2825
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Role:
Author
ORCID:
0000-0001-5683-9495


Publisher:
Springer Nature
Journal:
Nature Communications More from this journal
Volume:
12
Issue:
1
Article number:
471
Publication date:
2021-01-20
Acceptance date:
2020-12-07
DOI:
EISSN:
2041-1723
ISSN:
2041-1723
Pmid:
33473110


Language:
English
Keywords:
Pubs id:
1158522
Local pid:
pubs:1158522
Deposit date:
2021-02-10

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