Abstract

As poly[4,8-bis(5-(2-ethylhexyl)thiophen-2-yl)benzo[1,2-b; 4,5-b′]dithiophene-2,6-diyl-alt-(4-(2-ethylhexyl)-3-fluorothieno[3,4-b]thiophene-)-2-carboxylate-2-6-diyl)] has good potential as a low-band gap donor polymer for organic photovoltaic cells (OPVs), we investigated the optimized electrospray deposition condition for realizing suitable polymer ordering and/or crystallite size by controlling the solvent evaporation time. Previous studies on the electrospray process have mainly focused on novel device structure owing to its unique characteristic of small droplet size, which is less than 1 μm. However, in this research, we investigated the spontaneous formation of interpenetrating continuous networks of the donor- and acceptor-rich domains of solvent evaporation during the electrospray process. By evaluating the ultraviolet–visible absorption spectrum, Raman spectroscopy, and direction of polymer ordering, it was shown that the polymer-stacking condition was not influenced by solvent evaporation time, even though poly(3-hexylthiophene-2,5-diyl) along the face-on direction was well stacked under the slow solvent evaporation condition. In contrast, the crystallite size, which was estimated from the full width at half maximum X-ray diffraction pattern, increased as the solvent evaporation time increased. This means that the crystalline grain spontaneously grew in the droplet and that the large crystalline grain was formed during the slow evaporation condition. Furthermore, the photovoltaic performance trend was the same as the performance trend of the crystallite size and were increased with increasing solvent evaporation time for both polymers. Therefore, the crystalline grain size was a dominant factor in determining the photovoltaic performance. Additionally, the crystalline grain size could be controlled by the solvent evaporation time. Finally, by optimizing the active-layer thickness, the highest photoconversion efficiency of 8.6% was achieved. This is the highest value of an electrospray-based device. These results indicate that the solvent evaporation time is an important factor in determining the crystallite size of an organic thin film, which directly affects the photoconversion efficiency of OPVs.

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