The impact of donor-acceptor phase separation on the charge carrier dynamics in pBTTT:PCBM photovoltaic blends
Dominik Gehrig a, Ian Howard a, Frédéric Laquai a, Sean Sweetnam b, Michael McGehee b
a Max Planck Institute for Polymer Research, Mainz, Ackermannweg, 10, Mainz, Germany
b Materials Science and Engineering, Standford University, 476 Lomita Mall, Stanford, California, 94305-4045
International Conference on Hybrid and Organic Photovoltaics
Proceedings of International Conference on Hybrid and Organic Photovoltaics 2015 (HOPV15)
Roma, Italy, 2015 May 11th - 13th
Organizer: Filippo De Angelis
Oral, Dominik Gehrig, presentation 088
Publication date: 5th February 2015

We study the effect of phase separation and domain formation, controlled by the donor-acceptor mixing ratio, on the charge generation and recombination in pBTTT-C14:PC60BM bulk heterojunction (BHJ) photovoltaic blends by transient absorption (TA) spectroscopy. Changing the donor-acceptor mixing ratio is an effective strategy to control the morphology in pBTTT-C14:PC60BM blends. A 1:1 blending ratio results in a fully-intercalated cocrystal structure, while higher fullerene loads lead to pure PCBM domains in addition to the cocrystal phase. We show that in a 1:1 blend electron transfer is exclusively ultrafast, however, the majority of charges create bound interfacial charge-transfer (CT) states, which decay on the sub-nanosecond timescale. On the contrary, a mixing ratio of 1:4 polymer:fullerene facilitates free charge generation, while only a small fraction of  CT state formation is observed. This clearly illustrates that extended PCBM domains play an essential role in the generation and spatial separation of free charges on an ultrafast timescale (<100 fs), indicating that they are not only relevant as percolation paths for efficient extraction of free carriers, but also critically influence the initial stages of free carrier formation.



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