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The Role of Delocalization and Excess Energy in the Quantum Efficiency of Organic Solar Cells and the Validity of Optical Reciprocity Relations
Linköping University, Department of Physics, Chemistry and Biology, Complex Materials and Devices. Linköping University, Faculty of Science & Engineering.
Stanford Univ, CA 94305 USA.
Linköping University, Department of Physics, Chemistry and Biology, Biomolecular and Organic Electronics. Linköping University, Faculty of Science & Engineering. Heidelberg Univ, Germany.ORCID iD: 0000-0002-7104-7127
2020 (English)In: Journal of Physical Chemistry Letters, ISSN 1948-7185, E-ISSN 1948-7185, Vol. 11, no 9, p. 3563-3570Article in journal (Refereed) Published
Abstract [en]

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 similar to 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.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC , 2020. Vol. 11, no 9, p. 3563-3570
National Category
Theoretical Chemistry
Identifiers
URN: urn:nbn:se:liu:diva-166487DOI: 10.1021/acs.jpclett.0c00945ISI: 000535177500056PubMedID: 32301322OAI: oai:DiVA.org:liu-166487DiVA, id: diva2:1444126
Note

Funding Agencies|Knut and Alice Wallenberg FoundationKnut & Alice Wallenberg Foundation [KAW 2016.0494]

Available from: 2020-06-20 Created: 2020-06-20 Last updated: 2020-06-20

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Felekidis, NikolaosKemerink, Martijn
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