A variety of measurement techniques including photothermal deflection spectroscopy (PDS), auger electron spectroscopy (AES), (sub–bandgap) external quantum efficiency (EQE), and impedance spectroscopy are applied to poly[N‐900‐hepta‐decanyl‐2,7‐carbazole‐alt‐5,5‐(40,70‐di‐2‐thienyl‐20,10,30‐benzothiadiazole (PCDTBT)/[6,6]‐phenyl C71 butyric acid methyl ester (PC71BM) films and devices to probe the stability under thermal annealing. Upon annealing, solar cell performance is drastically decreased for temperatures higher than 140 °C. Detailed investigation indicate changes in polymer:fullerene interactions resulting in the formation of a polymer wetting layer upon annealing at temperatures higher than 140 °C. Upon device completion this wetting layer is located close to the metal electrode and therefore leads to an increase in recombination and a decrease in charge carrier extraction, providing an explanation for the reduced fill factor (FF) and power conversion efficiency (PCE).
In this work, we demonstrate the successful replacement of a chlorinated solvent system based on a 1 : 1 mixture of chlorobenzene and ortho-dichlorobenzene with the chlorine-free solvent xylene, resulting in chlorine-free processing with a small amount of diiodooctane additive. In fact, the overall power conversion efficiency is improved from 6.71% for the chlorinated solvents to 7.15% for the chlorine-free solvent m-xylene.
The influence of various polar solvent additives with different dipole moments has been investigated since the performance of a photovoltaic device comprising a donor-acceptor copolymer (benzothiadiazole-fluorene-diketopyrrolopyrrole (BTD-F-DKPP)) and phenyl-C60-butyric acid methyl ester (PCBM) was notably increased. A common approach for controlling bulk heterojunction morphology and thereby improving the solar cell performance involves the use of solvent additives exhibiting boiling points higher than that of the surrounding solvent in order to allow the fullerene to aggregate during the host solvent evaporation and film solidification. In contrast to that, we report the application of polar solvent additives with widely varied dipole moments, where intentionally no dependence on their boiling points was applied. We found that an appropriate amount of the additive can improve all solar cell parameters. This beneficial effect could be largely attributed to a modification of the poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)-active layer interface within the device layer stack, which was successfully reproduced for polymer solar cells based on the commonly used PCDTBT (poly[N-900-hepta-decanyl-2,7-carbazole-alt-5,5-(40,70-di-2-thienyl-20,10,30-benzothiadiazole)]) copolymer.
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