Organic solar cells (OSCs) based on non-fullerene acceptors (NFAs) have developed very fast in recent years. A proper balance among power conversion efficiency (PCE), stability, and production cost needs further elaboration. Here we investigate the industrial viability of highly efficient OSCs based on several representative NFAs. The most stable OSCs exhibit PCE of $8% along with extrapolated T 80 lifetime (80% of the initial PCE) of over 11,000 hr under equivalent 1 sun illumination, which would lead to a very impressive operational lifetime approaching 10 years. Photo-stability is strongly dependent on the end-group and side-chain engineering of the NFAs. Breaking of conjugation during photo-aging leads to increased energetic traps. Fluorination of the end-group stabilizes molecules against light soaking, while adding methyl groups shows an opposite trend. Side-chain modification can significantly influence the morphological stability. Reducing synthetic complexity of this class of NFAs will ultimately push the organic photovoltaics technology into real-life applications.

The performance of organic solar cells is determined by the delicate, meticulously optimized bulk-heterojunction microstructure, which consists of finely mixed and relatively separated donor/acceptor regions. Here we demonstrate an abnormal strong burn-in degradation in highly efficient polymer solar cells caused by spinodal demixing of the donor and acceptor phases, which dramatically reduces charge generation and can be attributed to the inherently low miscibility of both materials. Even though the microstructure can be kinetically tuned for achieving high-performance, the inherently low miscibility of donor and acceptor leads to spontaneous phase separation in the solid state, even at room temperature and in the dark. A theoretical calculation of the molecular parameters and construction of the spinodal phase diagrams highlight molecular incompatibilities between the donor and acceptor as a dominant mechanism for burn-in degradation, which is to date the major short-time loss reducing the performance and stability of organic solar cells.

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The performance of organic photovoltaic (OPV) material systems are hypothesized to depend strongly on the intermolecular arrangements at the donor:fullerene interfaces. A review of some of the most efficient polymers utilized in polymer:fullerene PV devices, combined with an analysis of reported polymer donor materials wherein the same conjugated backbone was used with varying alkyl substituents, supports this hypothesis. Specifically, the literature shows that higher-performing donor-acceptor type polymers generally have acceptor moieties that are sterically accessible for interactions with the fullerene derivative, whereas the corresponding donor moieties tend to have branched alkyl substituents that sterically hinder interactions with the fullerene. To further explore the idea that the most beneficial polymer:fullerene arrangement involves the fullerene docking with the acceptor moiety, a family of benzo[1,2-b:4,5-b']dithiophene-thieno[3,4-c]pyrrole-4,6-dione polymers (PBDTTPD derivatives) was synthesized and tested in a variety of PV device types with vastly different aggregation states of the polymer. In agreement with our hypothesis, the PBDTTPD derivative with a more sterically accessible acceptor moiety and a more sterically hindered donor moiety shows the highest performance in bulk-heterojunction, bilayer, and low-polymer concentration PV devices where fullerene derivatives serve as the electron-accepting materials. Furthermore, external quantum efficiency measurements of the charge-transfer state and solid-state two-dimensional (2D) (13)C{(1)H} heteronuclear correlation (HETCOR) NMR analyses support that a specific polymer:fullerene arrangement is present for the highest performing PBDTTPD derivative, in which the fullerene is in closer proximity to the acceptor moiety of the polymer. This work demonstrates that the polymer:fullerene arrangement and resulting intermolecular interactions may be key factors in determining the performance of OPV material systems.

The charge carrier lifetime in small molecule: C60 photovoltaic devices is increased by reducing the physical interface area availabe for recombination. For donor contents below 10%, the gain in open‐circuit voltage (Voc) depends logarithmically on the interface area while the energy of the interfacial charge‐transfer state ECT remains invariant.