TY - JOUR A1 - Alqahtani, Obaid A1 - Babics, Maxime A1 - Gorenflot, Julien A1 - Savikhin, Victoria A1 - Ferron, Thomas A1 - Balawi, Ahmed H. A1 - Paulke, Andreas A1 - Kan, Zhipeng A1 - Pope, Michael A1 - Clulow, Andrew J. A1 - Wolf, Jannic A1 - Burn, Paul L. A1 - Gentle, Ian R. A1 - Neher, Dieter A1 - Toney, Michael F. A1 - Laquai, Frederic A1 - Beaujuge, Pierre M. A1 - Collins, Brian A. T1 - Mixed Domains Enhance Charge Generation and Extraction in Bulk-Heterojunction Solar Cells with Small-Molecule Donors JF - Advanced energy materials N2 - The interplay between nanomorphology and efficiency of polymer-fullerene bulk-heterojunction (BHJ) solar cells has been the subject of intense research, but the generality of these concepts for small-molecule (SM) BHJs remains unclear. Here, the relation between performance; charge generation, recombination, and extraction dynamics; and nanomorphology achievable with two SM donors benzo[1,2-b:4,5-b]dithiophene-pyrido[3,4-b]-pyrazine BDT(PPTh2)(2), namely SM1 and SM2, differing by their side-chains, are examined as a function of solution additive composition. The results show that the additive 1,8-diiodooctane acts as a plasticizer in the blends, increases domain size, and promotes ordering/crystallinity. Surprisingly, the system with high domain purity (SM1) exhibits both poor exciton harvesting and severe charge trapping, alleviated only slightly with increased crystallinity. In contrast, the system consisting of mixed domains and lower crystallinity (SM2) shows both excellent exciton harvesting and low charge recombination losses. Importantly, the onset of large, pure crystallites in the latter (SM2) system reduces efficiency, pointing to possible differences in the ideal morphologies for SM-based BHJ solar cells compared with polymer-fullerene devices. In polymer-based systems, tie chains between pure polymer crystals establish a continuous charge transport network, whereas SM-based active layers may in some cases require mixed domains that enable both aggregation and charge percolation to the electrodes. KW - charge transport KW - domain purity KW - microscopy KW - mixed domains KW - organic solar cells KW - photovoltaic devices KW - resonant X-ray scattering KW - small molecules KW - transient spectroscopy Y1 - 2018 U6 - https://doi.org/10.1002/aenm.201702941 SN - 1614-6832 SN - 1614-6840 VL - 8 IS - 19 PB - Wiley-VCH CY - Weinheim ER - TY - JOUR A1 - Perdigón-Toro, Lorena A1 - Le Quang Phuong, A1 - Eller, Fabian A1 - Freychet, Guillaume A1 - Saglamkaya, Elifnaz A1 - Khan, Jafar A1 - Wei, Qingya A1 - Zeiske, Stefan A1 - Kroh, Daniel A1 - Wedler, Stefan A1 - Koehler, Anna A1 - Armin, Ardalan A1 - Laquai, Frederic A1 - Herzig, Eva M. A1 - Zou, Yingping A1 - Shoaee, Safa A1 - Neher, Dieter T1 - Understanding the role of order in Y-series non-fullerene solar cells to realize high open-circuit voltages JF - Advanced energy materials N2 - Non-fullerene acceptors (NFAs) as used in state-of-the-art organic solar cells feature highly crystalline layers that go along with low energetic disorder. Here, the crucial role of energetic disorder in blends of the donor polymer PM6 with two Y-series NFAs, Y6, and N4 is studied. By performing temperature-dependent charge transport and recombination studies, a consistent picture of the shape of the density of state distributions for free charges in the two blends is developed, allowing an analytical description of the dependence of the open-circuit voltage V-OC on temperature and illumination intensity. Disorder is found to influence the value of the V-OC at room temperature, but also its progression with temperature. Here, the PM6:Y6 blend benefits substantially from its narrower state distributions. The analysis also shows that the energy of the equilibrated free charge population is well below the energy of the NFA singlet excitons for both blends and possibly below the energy of the populated charge transfer manifold, indicating a down-hill driving force for free charge formation. It is concluded that energetic disorder of charge-separated states has to be considered in the analysis of the photovoltaic properties, even for the more ordered PM6:Y6 blend. KW - energetic disorder KW - non-fullerene acceptors KW - open-circuit voltage KW - organic solar cells Y1 - 2022 U6 - https://doi.org/10.1002/aenm.202103422 SN - 1614-6832 SN - 1614-6840 VL - 12 IS - 12 PB - Wiley-VCH CY - Weinheim ER -