Photoinduced charge generation in a molecular bulk heterojunction material

Loren G Kaake, Jacek Jaroslaw Jasieniak, Ronald C Bakus II, Gregory C Welch, Daniel Moses, Guillermo C Bazan, Alan J Heeger

Research output: Contribution to journalArticleResearchpeer-review

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Abstract

Understanding the charge generation dynamics in organic photovoltaic bulk heterojunction (BHJ) blends is important for providing the necessary guidelines to improve overall device efficiency. Despite more than IS years of experimental and theoretical studies, a universal picture describing the generation and recombination processes operating in organic photovoltaic devices is still being forged. We report here the results of ultrafast transient absorption spectroscopy measurements of charge photogeneration and recombination processes in a high-performing solution-processed molecular BHJ. For comparison, we also studied a high-performing polymer-based BHJ material. We find that the majority of charge carriers in both systems are generated on <100 fs time scales and posit that excited state delocalization is responsible for the ultrafast charge transfer. This initial delocalization is consistent with the fundamental uncertainty associated with the photon absorption process (in the visible, lambda/4 pi > 30 nm) and is comparable with the phase-separated domain size. In addition, exciton diffusion to charge-separating heterojunctions is observed at longer times (1-500 ps). Finally, charge generation in pure films of the solution processed molecule was studied. Polarization anisotropy measurements clearly demonstrate that the optical properties are dominated by molecular (Frenkel) exictons and delocalized charges are promptly produced (t <100 fs).
Original languageEnglish
Pages (from-to)19828 - 19838
Number of pages11
JournalJournal of the American Chemical Society
Volume134
Issue number48
DOIs
Publication statusPublished - 2012

Cite this

Kaake, L. G., Jasieniak, J. J., Bakus II, R. C., Welch, G. C., Moses, D., Bazan, G. C., & Heeger, A. J. (2012). Photoinduced charge generation in a molecular bulk heterojunction material. Journal of the American Chemical Society, 134(48), 19828 - 19838. https://doi.org/10.1021/ja308949m
Kaake, Loren G ; Jasieniak, Jacek Jaroslaw ; Bakus II, Ronald C ; Welch, Gregory C ; Moses, Daniel ; Bazan, Guillermo C ; Heeger, Alan J. / Photoinduced charge generation in a molecular bulk heterojunction material. In: Journal of the American Chemical Society. 2012 ; Vol. 134, No. 48. pp. 19828 - 19838.
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Kaake, LG, Jasieniak, JJ, Bakus II, RC, Welch, GC, Moses, D, Bazan, GC & Heeger, AJ 2012, 'Photoinduced charge generation in a molecular bulk heterojunction material', Journal of the American Chemical Society, vol. 134, no. 48, pp. 19828 - 19838. https://doi.org/10.1021/ja308949m

Photoinduced charge generation in a molecular bulk heterojunction material. / Kaake, Loren G; Jasieniak, Jacek Jaroslaw; Bakus II, Ronald C; Welch, Gregory C; Moses, Daniel; Bazan, Guillermo C; Heeger, Alan J.

In: Journal of the American Chemical Society, Vol. 134, No. 48, 2012, p. 19828 - 19838.

Research output: Contribution to journalArticleResearchpeer-review

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AU - Bazan, Guillermo C

AU - Heeger, Alan J

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AB - Understanding the charge generation dynamics in organic photovoltaic bulk heterojunction (BHJ) blends is important for providing the necessary guidelines to improve overall device efficiency. Despite more than IS years of experimental and theoretical studies, a universal picture describing the generation and recombination processes operating in organic photovoltaic devices is still being forged. We report here the results of ultrafast transient absorption spectroscopy measurements of charge photogeneration and recombination processes in a high-performing solution-processed molecular BHJ. For comparison, we also studied a high-performing polymer-based BHJ material. We find that the majority of charge carriers in both systems are generated on <100 fs time scales and posit that excited state delocalization is responsible for the ultrafast charge transfer. This initial delocalization is consistent with the fundamental uncertainty associated with the photon absorption process (in the visible, lambda/4 pi > 30 nm) and is comparable with the phase-separated domain size. In addition, exciton diffusion to charge-separating heterojunctions is observed at longer times (1-500 ps). Finally, charge generation in pure films of the solution processed molecule was studied. Polarization anisotropy measurements clearly demonstrate that the optical properties are dominated by molecular (Frenkel) exictons and delocalized charges are promptly produced (t <100 fs).

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