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J Am Chem Soc. 2012 Dec 5;134(48):19828-38. doi: 10.1021/ja308949m. Epub 2012 Nov 19.

Photoinduced charge generation in a molecular bulk heterojunction material.

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Center for Polymers and Organic Solids, University of California-Santa Barbara, Santa Barbara, California 93106, United States.


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 15 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, λ/4π > 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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