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Intercalated vs Nonintercalated Morphologies in Donor–Acceptor Bulk Heterojunction Solar Cells: PBTTT:Fullerene Charge Generation and Recombination Revisited

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Department of Physics and Astronomy, University of Potsdam, Karl-Liebknecht-Straße 24−25, 14476 Potsdam-Golm, Germany
Centre for Engineered Quantum Systems, School of Mathematics and Physics, The University of Queensland, Brisbane, Queensland 4072, Australia
§ Materials Research Institute and School of Biological and Chemical Sciences, Queen Mary University of London, Mile End Road, London E1 4NS, United Kingdom
Centre for Plastic Electronics, Department of Chemistry, Imperial College London, Exhibition Road, London SW7 2AZ, United Kingdom
KSC, King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia
# Centre for Engineered Quantum Systems, Australian Institute for Nanoscale Science and Technology, and School of Chemistry, The University of Sydney, Sydney, New South Wales 2006, Australia
SPECIFIC IKC, College of Engineering, Swansea University, Swansea SA12 7AX, United Kingdom
*E-mail: [email protected] (D.N.).
*E-mail: [email protected] (J.R.D.).
Cite this: J. Phys. Chem. Lett. 2017, 8, 17, 4061–4068
Publication Date (Web):August 4, 2017
https://doi.org/10.1021/acs.jpclett.7b01571
Copyright © 2017 American Chemical Society

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    Abstract

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    In this Letter, we study the role of the donor:acceptor interface nanostructure upon charge separation and recombination in organic photovoltaic devices and blend films, using mixtures of PBTTT and two different fullerene derivatives (PC70BM and ICTA) as models for intercalated and nonintercalated morphologies, respectively. Thermodynamic simulations show that while the completely intercalated system exhibits a large free-energy barrier for charge separation, this barrier is significantly lower in the nonintercalated system and almost vanishes when energetic disorder is included in the model. Despite these differences, both femtosecond-resolved transient absorption spectroscopy (TAS) and time-delayed collection field (TDCF) exhibit extensive first-order losses in both systems, suggesting that geminate pairs are the primary product of photoexcitation. In contrast, the system that comprises a combination of fully intercalated polymer:fullerene areas and fullerene-aggregated domains (1:4 PBTTT:PC70BM) is the only one that shows slow, second-order recombination of free charges, resulting in devices with an overall higher short-circuit current and fill factor. This study therefore provides a novel consideration of the role of the interfacial nanostructure and the nature of bound charges and their impact upon charge generation and recombination.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpclett.7b01571.

    • Structures of the donor polymer and fullerene acceptors as well as UV–vis steady-state absorption of the respective neat and blend films, details of the thermodynamic simulations and optical spectroscopy (TAS and PL) complementary data, EQE and device efficiency figures, and TDCF transient of devices (PDF)

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