The role of delocalization and excess energy in the quantum efficiency of organic solar cells and the validity of optical reciprocity relations

The photon energy dependence of long-range charge separation is studied for two prototypical polymer:fullerene systems. The internal quantum efficiency (IQE) of PCDTBT:PC61BM is experimentally shown to be independent of the excitation energy. In contrast, for TQ1:PC71BM the IQE is strongly energy-de...

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Main Authors: Felekidis, Nikolaos (Author) , Melianas, Armantas (Author) , Kemerink, Martijn (Author)
Format: Article (Journal)
Language:English
Published: April 17, 2020
In: The journal of physical chemistry letters
Year: 2020, Volume: 11, Issue: 9, Pages: 3563-3570
ISSN:1948-7185
DOI:10.1021/acs.jpclett.0c00945
Online Access:Verlag, lizenzpflichtig, Volltext: https://dx.doi.org/10.1021/acs.jpclett.0c00945
Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1021/acs.jpclett.0c00945
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Author Notes:N. Felekidis, A. Melianas, and M. Kemerink
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Summary:The photon energy dependence of long-range charge separation is studied for two prototypical polymer:fullerene systems. The internal quantum efficiency (IQE) of PCDTBT:PC61BM is experimentally shown to be independent of the excitation energy. In contrast, for TQ1:PC71BM the IQE is strongly energy-dependent for excitation energies close to charge transfer (CT) electroluminescence peak maximum while it becomes energy-independent at higher excitation energies. Kinetic Monte Carlo simulations reproduce the experimental IQE and reveal that the photon energy-dependence of the IQE is governed by charge delocalization. Efficient long-range separation at excitation energies corresponding to the CT electroluminescence peak maximum or lower requires an initial separation of the hole-electron pair by ∼4-5 nm, whereas delocalization is less important for charge separation at higher photon energies. Our modeling results suggest that a phenomenological reciprocity between CT electroluminescence and external quantum efficiency does not necessarily prove that commonly employed reciprocity relations between these spectra are valid from a fundamental perspective.
Item Description:Gesehen am 23.06.2020
Physical Description:Online Resource
ISSN:1948-7185
DOI:10.1021/acs.jpclett.0c00945