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The Importance of Entanglements in Optimizing the Mechanical and Electrical Performance of All-Polymer Solar Cells

  • Nrup Balar
    Nrup Balar
    Department of Mechanical and Aerospace Engineering, North Carolina State University, Raleigh, North Carolina 27695, United States
    More by Nrup Balar
  • , 
  • Jeromy James Rech
    Jeromy James Rech
    Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States
    More by Jeromy James Rech
    Orcidhttp://orcid.org/0000-0001-7963-9357
  • , 
  • Reece Henry
    Reece Henry
    Department of Physics, North Carolina State University, Raleigh, North Carolina 27695, United States
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  • , 
  • Long Ye
    Long Ye
    Department of Physics, North Carolina State University, Raleigh, North Carolina 27695, United States
    More by Long Ye
    Orcidhttp://orcid.org/0000-0002-5884-0083
  • , 
  • Harald Ade
    Harald Ade
    Department of Physics, North Carolina State University, Raleigh, North Carolina 27695, United States
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  • , 
  • Wei You
    Wei You
    Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States
    More by Wei You
    Orcidhttp://orcid.org/0000-0003-0354-1948
  • , and 
  • Brendan T. O’Connor*
    Brendan T. O’Connor
    Department of Mechanical and Aerospace Engineering, North Carolina State University, Raleigh, North Carolina 27695, United States
    *E-mail: [email protected]
    More by Brendan T. O’Connor
    Orcidhttp://orcid.org/0000-0002-8999-5184
Cite this: Chem. Mater. 2019, 31, 14, 5124–5132
Publication Date (Web):June 27, 2019
https://doi.org/10.1021/acs.chemmater.9b01011
Copyright © 2019 American Chemical Society
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    Abstract

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    Organic solar cells that have all-polymer active layers may have several advantages compared with polymer–small molecule systems including improved mechanical and thermodynamic stability; however, an all-polymer active layer does not guarantee robust mechanical behavior. Here, we consider key parameters that may influence the mechanical behavior and power conversion efficiency of all-polymer solar cells (all-PSCs). Considerations include the thermal transition temperature of the polymers, the molecular weight (MW) of the polymers, and film morphology. The impact these features have on mechanical behavior is probed by measuring the cohesive fracture energy (Gc), crack onset strain, and elastic modulus. We find that the selection of ductile polymers with high MW enhances interchain interactions that improve the mechanical resilience of the films. High-MW polymers are also found to maximize the power conversion efficiency (PCE). Using this strategy, BHJ films with the best reported combination of Gc (7.96 J m–2) and PCE (6.94%) are demonstrated. Finally, it is found that increasing the film thickness increases the fracture energy of the films but at the cost of PCE. These findings provide a fundamental perspective on the design strategy to achieve high performance and mechanically robust organic solar cells.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.chemmater.9b01011.

    • GPC traces, recipes of film processing, X-ray based morphology analysis, DMA plots of the blend films, AFM scans of the neat and the blend fractured films, relationship between COS and Gc for the neat and the blend films, recipes to achieve different thicknesses of 100k:PNDI(2OD)2T blend films, photovoltaic characteristics of OPV devices at different thicknesses, and AFM scans of fractured films of different thicknesses (PDF)

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