Quantitative relationships between film morphology, charge carrier dynamics, and photovoltaic performance in bulk-heterojunction binary vs. ternary acceptor blends

Zhu, Weigang; Li, Guoping; Mukherjee, Subhrangsu; Powers-Riggs, Natalia E.; Jones, Leighton O.; Gann, Eliot; Kline, R. Joseph; Herzing, Andrew; Logsdon, Jenna L.; Flagg, Lucas; Stern, Charlotte L.; Young, Ryan M.; Kohlstedt, Kevin L.; Schatz, George C.; DeLongchamp, Dean M.; Wasielewski, Michael R.; Melkonyan, Ferdinand S.; Facchetti, Antonio; Marks, Tobin J.

doi:10.1039/d2ee03883h

Quantitative relationships between film morphology, charge carrier dynamics, and photovoltaic performance in bulk-heterojunction binary vs. ternary acceptor blends

Journal Article · Tue Feb 07 00:00:00 EST 2023 · Energy & Environmental Science

DOI:https://doi.org/10.1039/d2ee03883h· OSTI ID:2419588

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Northwestern Univ., Evanston, IL (United States); Tianjin Univ. (China); OSTI
Northwestern Univ., Evanston, IL (United States)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Northwestern Univ., Evanston, IL (United States); Flexterra Corporation, Skokie, IL (United States)

Addressing pertinent and perplexing questions regarding why nonfullerene acceptors (NFAs) promote higher power conversion efficiencies (PCEs) than traditional fullerenes and how photoactive bulk heterojunction (BHJ) film morphology, charge photogeneration, and recombination dynamics dictate solar cell performance have stimulated many studies of polymer solar cells (PSCs), yet quantitative relationships remain limited. Better understanding in these areas offers the potential to advance materials design and device engineering, afford higher PCEs, and ultimate commercialization. Here we probe quantitative relationships between BHJ film morphology, charge carrier dynamics, and photovoltaic performance in model binary and ternary blend systems having a wide bandgap donor polymer, a fullerene, and a promising NFA. We show that optimal PC₇₁BM incorporation in a PBDB-TF:ITIC-Th binary system matrix retains the original π-face-on orientation, ITIC-Th crystallinity and BHJ film crystallite dimensions, and reduces film upper surface ITIC-Th segregation. Such morphology changes together simultaneously increase hole (μ_h) and electron (μ_e) mobilities, facilitate light-activated ITIC-Th to PC₇₁BM domain electron delocalization, reduce free charge carrier (FC) bimolecular recombination (BR) within PBDB-TF:ITIC-Th mixed regions, and increase FC extraction pathways viaPBDB-TF:PC₇₁BM pairs. The interplay of these effects yields significantly enhanced inverted cell short-circuit current density (J_SC), fill factor (FF), and PCE. Unexpectedly, we also find that excessive PC₇₁BM in the PBDB-TF:ITIC-Th binary system alters the PBDB-TF orientation to π-edge-on, increases large scale PC₇₁BM-rich aggregations and BHJ upper surface PC₇₁BM composition. Further, these morphology changes increase parasitic decay processes such as intersystem crossing from photoexcited PC₇₁BM, compromising the J_SC, FF, and PCE metrics. ITIC-Th X-ray diffraction reveals a unique sidechain-dominated molecular network with previously unknown sidechain-end group stacking, rationalizing the STEM and GIWAXS results, photophysics, and the high μ_e. DFT computation reveals charge transfer networks within ITIC-Th crystallites, supporting excited-state electron delocalization from ITIC-Th to PC₇₁BM. This structure–property understanding leads to a newly reported NFA blend with PCE near 17%.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); Energy Frontier Research Centers (EFRC) (United States). Center for Light Energy Activated Redox Processes (LEAP); Northwestern Univ., Evanston, IL (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL); Stanford Univ., CA (United States); Univ. of California, Oakland, CA (United States)

Sponsoring Organization:: Qatar National Research Foundation; US Department of the Navy, Office of Naval Research (ONR); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC02-76SF00515; SC0001059; SC0012704

OSTI ID:: 2419588

Alternate ID(s):: OSTI ID: 1957848

Journal Information:: Energy & Environmental Science, Journal Name: Energy & Environmental Science Journal Issue: 3 Vol. 16; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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