jz0c00058_si_001.pdf (2.13 MB)
Efficient Charge Generation via Hole Transfer in Dilute Organic Donor–Fullerene Blends
journal contribution
posted on 2020-03-05, 13:10 authored by Yin Song, Alexander Schubert, Xiao Liu, Srijana Bhandari, Stephen R. Forrest, Barry D. Dunietz, Eitan Geva, Jennifer P. OgilvieEfficient
organic photovoltaics (OPVs) require broadband charge photogeneration
with near-unity quantum yield. This can only be achieved by exploiting
all pathways that generate charge. Electron transfer from organic
donors to acceptors has been well-studied and is considered the primary
path to charge photogeneration in OPVs. In contrast, much less is
known about the hole transfer pathway. Here we study charge photogeneration
in an archetypal system comprising tetraphenyldibenzoperiflanthene:C70 blends using our recently developed multispectral two-dimensional
electronic spectroscopy (M-2DES), supported by time-dependent density
functional theory and fully quantum-mechanical Fermi’s golden
rule rate calculations. Our approach identifies in real time two rapid
charge transfer pathways that are confirmed through computational
analysis. Surprisingly, we find that both electron and hole transfer
occur with comparable rates and efficiencies, facilitated by donor–acceptor
electronic interactions. Our results highlight the importance of the
hole transfer pathway for optimizing the efficiency of OPV devices
employing small-molecule heterojunctions.
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study charge photogenerationtime-dependent densitycharge photogenerationOPV devicesdonorM -2DESnear-unity quantumEfficient Charge Generationsmall-molecule heterojunctionsefficiencyarchetypal systemcharge transfer pathwayselectron transferhole transferbroadband charge photogenerationhole transfer pathwayrule rate calculationsHole Transfer
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