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Effect of Multiple Adduct Fullerenes on Microstructure and Phase Behavior of P3HT:Fullerene Blend Films for Organic Solar Cells

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    Effect of Multiple Adduct Fullerenes on Microstructure and Phase Behavior of P3HT:Fullerene Blend Films for Organic Solar Cells
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    † Centre for Plastic Electronics and Department of Physics, Blackett Laboratory, Imperial College London, London SW7 2AZ, United Kingdom
    ‡ Centre for Plastic Electronics and Department of Chemistry, Imperial College London, London SW7 2AZ, United Kingdom
    § School of Physics and Astronomy, Cardiff University, Queens buildings, The Parade, Cardiff CF24 3AA, United Kingdom
    ⊥ Centre for Plastic Electronics and Department of Materials, Royal School of Mines, Imperial College London, London SW7 2AZ, United Kingdom
    *Address correspondence to [email protected], [email protected]
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    ACS Nano

    Cite this: ACS Nano 2012, 6, 5, 3868–3875
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    https://doi.org/10.1021/nn204996w
    Published April 25, 2012
    Copyright © 2012 American Chemical Society
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    Abstract

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    The bis and tris adducts of [6,6]phenyl-C61-butyric acid methyl ester (PCBM) offer lower reduction potentials than PCBM and are therefore expected to offer larger open-circuit voltages and more efficient energy conversion when blended with conjugated polymers in photovoltaic devices in place of PCBM. However, poor photovoltaic device performances are commonly observed when PCBM is replaced with higher-adduct fullerenes. In this work, we use transmission electron microscopy (TEM), steady-state and ultrafast time-resolved photoluminescence spectroscopy (PL), and differential scanning calorimetry (DSC) to probe the microstructural properties of blend films of poly(3-hexylthiophene-2,5-diyl) (P3HT) with the bis and tris adducts of PCBM. TEM and PL indicate that, in as-spun blend films, fullerenes become less soluble in P3HT as the number of adducts increases. PL indicates that upon annealing crystallization leads to phase separation in P3HT:PCBM samples only. DSC studies indicate that the interactions between P3HT and the fullerene become weaker with higher-adduct fullerenes and that all systems exhibit eutectic phase behavior with a eutectic composition being shifted to higher molar fullerene content for higher-adduct fullerenes. We propose two different mechanisms of microstructure development for PCBM and higher-adduct fullerenes. P3HT:PCBM blends, phase segregation is the result of crystallization of either one or both components and is facilitated by thermal treatments. In contrast, for blends containing higher adducts, the phase separation is due to a partial demixing of the amorphous phases. We rationalize the lower photocurrent generation by the higher-adduct fullerene blends in terms of film microstructure.

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    Supporting Information

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    Additional figures contain UV–vis absorption spectra, steady-state PL spectra, ultrafast PL initial fluorescence intensity, GIXRD data and analysis of P3HT:PCBM, P3HT:bis-PCBM, and P3HT:tris-PCBM blends, DSC scans of blends of P3HT:bis-PCBM and P3HT:tris-PCBM at different compositions, and device characteristics for P3HT:bis-PCBM blends at different compositions. This material is available free of charge via the Internet at http://pubs.acs.org.

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    ACS Nano

    Cite this: ACS Nano 2012, 6, 5, 3868–3875
    Click to copy citationCitation copied!
    https://doi.org/10.1021/nn204996w
    Published April 25, 2012
    Copyright © 2012 American Chemical Society
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