For organic solar cells (OSCs) based on nonplanar phthalocyanines, it has previously been reported that a thin film composed of triclinic crystals with face-on (or flat-lying)-oriented molecules, typically obtained with a CuI template layer, is desired for optical absorption in the near-infrared (NIR) spectral region. However, this work demonstrates that for a PbPc-C donor-acceptor pair, less face-on orientation with a broader orientation distribution obtained with a new template layer consisting of a ZnPc/CuI bilayer is more desirable in terms of solar cell efficiency than the face-on orientation. A NIR-sensitive PbPc-C OSC employing this bilayer-templated PbPc film is found to increase the internal quantum efficiency (IQE) by 36% on average in the NIR spectral region compared to a device using a CuI-templated PbPc film. Analyses of the change in IQE using the exciton diffusion model and the entropy- and disorder-driven charge-separation model suggest that the improved IQE is attributed to the facilitated dissociation of charge-transfer excitons as well as the reduction in exciton quenching near the indium tin oxide surface.
When a perovskite precursor solution is electrosprayed using the conventional method where the nebulization of the solution is primarily governed by electrostatics, its high electrical conductivity tends to cause electrospray instabilities and thus makes high-quality perovskite films very difficult to obtain. Here, we report high-throughput fabrication of efficient perovskite solar cells (PSCs) whose CHNHPbICl films are deposited using a sheath-gas-assisted electrospray system. Our system, based on strong pneumatic nebulization as well as high-voltage electrostatic charging of droplets, enables very stable high-flow electrospray of small charged droplets, even for the highly conductive perovskite precursor solution. Consequently, with the control of the drying rate of the droplets deposited on substrates by adjusting the substrate temperature during deposition, crystalline, void-free CHNHPbICl films with nearly 100% surface coverage and high thickness uniformity are obtained. Inverted planar-heterojunction PSCs employing these films have a maximum power conversion efficiency of 14.2% with a small standard deviation of 0.9%, comparable to that of the spin-coated device.
Interconnection layers (ICLs) for polymer tandem solar cells reported so far are limited in materials' choice and layer structure, because of a requirement that the ICLs must prevent the penetration of solvents used for the top cells. In this research, it is demonstrated that depositing the active layer of the top subcell using a dry thin-film transfer technique allows for incorporation of an ICL composed of vacuum deposited materials in a polymer tandem cell, providing a large degree of freedom in ICL design. Specifically, a polymer tandem solar cell was fabricated using an ICL composed of bathocuproine:silver/silver islands/1,4,5,8,9,11-hexaazatriphenylene hexacarbonitrile (BCP:Ag/Ag islands/HAT-CN), where the thicknesses of the BCP:Ag and Ag island layers are precisely controlled at the nanoscale to facilitate the transport of electrons generated in the bottom subcell and to ensure their efficient recombination with holes generated in the top subcell. Consequently, the tandem device featuring the optimized ICL, whose active layers are composed of poly(3-hexylthiophene):[6,6]-phenyl-C61-butyric acid methyl ester (P3HT:PC61BM) and poly[2,6-(4,4-bis-(2-ethylhexyl)-4H-cyclopenta[2,1-b;3,4-b']dithiophene)-alt-4,7-(2,1,3-benzothiadiazole)]:[6,6]-phenyl-C71-butyric acid methyl ester (PCPDTBT:PC71BM), exhibits an open-circuit voltage of 1.20 V, which is equal to the sum of the open-circuit voltages of the two subcells, with a fill factor (FF) of 0.60 almost identical to the FFs of the subcells.
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