Rationalizing the influence of tunable energy levels on quantum efficiency to design optimal non-fullerene acceptor-based ternary organic solar cells

Non-fullerene acceptor (NFA)-based ternary bulk heterojunction solar cells (TSC) are the most efficient organic solar cells (OSCs) today due to their broader absorption and quantum efficiencies (QE) often surpassing those of corresponding binary blends. We study how the energetics driving charge transfer at the electron donor:electron acceptor (D/A) interfaces impact the QE in blends of PBDB-T-2F donor with several pairs of lower bandgap NFAs. As in binary blends, the ionization energy offset between donor and acceptor ({\Delta}IE) controls the QE and maximizes for {\Delta}IE > 0.5 eV. However, {\Delta}IE is not controlled by the individual NFAs IEs but by their average, weighted for their blending ratio. Using this property, we improved the QE of a PBDB-T-2F:IEICO binary blend that had an insufficient {\Delta}IE for charge generation by adding a deep IE third component: IT-4F. Combining two NFAs enables to optimize the D/A energy alignment and cells' QE without molecular engineering.
Comment: S Karuthedath and S H K Paleti contributed equally. MS: 35 pages, 9 figures. SI: 21 pages, 23 figures - updates: added a model scheme as Fig1, updated T1 EQE and blends PL in Fig 2 (former 1). Added Figure (5): charge generation upon acceptor excitation. Corrected {\Delta}IEs in fig7 and 9 (a few tens of meV off). Added more blends to show generality (2 groups, 10 blends compositions)