Extremely thin absorber (ETA) solar cells integrating ZnO nanowires have been receiving increasing interest owing to efficient light-trapping phenomena and charge-carrier management, but the chemical instability of ZnO in acidic conditions limits its combination with a variety of absorbing semiconducting shells grown by chemical deposition techniques. By covering the ZnO nanowires grown by chemical bath deposition with a protective, passivating, conformal, thin, anatase-TiO2 layer by atomic layer deposition, we show that a uniform Sb2S3 absorbing shell is formed by chemical spray pyrolysis without structural degradation of the ZnO. The Sb2S3 absorbing shell consists of a very thin, conformal layer together with homogeneously distributed small clusters from the bottom to the top of the ZnO/TiO2 core–shell nanowire arrays. The resulting ETA solar cells integrating these ZnO/TiO2/Sb2S3 core–shell nanowire heterostructures with an Sb2S3 absorbing shell less than 10 nm-thick and P3HT as the hole-transporting material have a photoconversion efficiency of 2.3% with a promising short-circuit current density of 7.5 mA/cm2 and a high open-circuit voltage of 656 mV as one of the largest reported values in ZnO nanowire-based ETA solar cells. The present findings thus reveal the great potential of Sb2S3 as an absorbing, semiconducting shell when coupled with ZnO/TiO2 core–shell nanowire heterostructures, opening the way for new strategies to improve the performance of ZnO nanowire-based ETA solar cells fabricated by low-cost, surface-scalable, easily implemented chemical deposition techniques.

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Antimony sulfide (Sb2S3), an environmentally benign material, has been prepared by various deposition methods for use as a solar absorber due to its direct band gap of ≈1.7 eV and high absorption coefficient in the visible light spectrum (1.8 × 105 cm−1 at 450 nm). Rapid, scalable, economically viable and controllable in-air growth of continuous, uniform, polycrystalline Sb2S3 absorber layers has not yet been accomplished. This could be achieved with chemical spray pyrolysis, a robust chemical method for deposition of thin films. We applied a two-stage process to produce continuous Sb2S3 optical coatings with uniform thickness. First, amorphous Sb2S3 layers, likely forming by 3D Volmer–Weber island growth through a molten phase reaction between SbCl3 and SC(NH2)2, were deposited in air on a glass/ITO/TiO2 substrate by ultrasonic spraying of methanolic Sb/S 1:3 molar ratio solution at 200–210 °C. Second, we produced polycrystalline uniform films of Sb2S3 (E g 1.8 eV) with a post-deposition thermal treatment of amorphous Sb2S3 layers in vacuum at 170 °C, <4 × 10−6 Torr for 5 minutes. The effects of the deposition temperature, the precursor molar ratio and the thermal treatment temperature on the Sb2S3 layers were investigated using Raman spectroscopy, X-ray diffraction, scanning electron microscopy, energy dispersive X-ray spectroscopy and UV–vis–NIR spectroscopy. We demonstrated that Sb2S3 optical coatings with controllable structure, morphology and optical properties can be deposited by ultrasonic spray pyrolysis in air by tuning of the deposition temperature, the Sb/S precursor molar ratio in the spray solution, and the post-deposition treatment temperature.

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