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Atomic layer deposition of amorphous antimony sulfide (a-Sb <sub/>2</sub> S <sub/>3</sub> ) as semiconductor sensitizer in extremely thin absorber solar cell
摘要： Atomic layer deposition of amorphous antimony sulfide (a-Sb2S3) is demonstrated with an alternating exposure of tris(dimethylamino) antimony (TDMASb) and hydrogen sulfide (H2S) at 150 °C in a custom-built viscous flow reactor. Growth mechanism and deposition chemistry are investigated by in situ quartz crystal microbalance and in situ Fourier Transform Infrared spectroscopy. Reaction hypothesis facilitating the binary reaction is established by quantum mechanical density functional theory calculations that essentially support the experimental findings. The developed material is used as a photon harvester in solar cells under extremely thin absorber configuration, with TiO2 and Spiro-OMeTAD as electron and hole transporting layers, respectively. Investigation of charge injection properties with surface photovoltage spectroscopy reveals low but non-negligible density of interfacial (sensitizer/TiO2) electronic defects. The conventional viscous flow reactor configuration is modified to showerhead-type reactor configuration to achieve better uniformity and conformality of a-Sb2S3 on highly porous TiO2 scaffolds. a-Sb2S3 device performance is optimized to achieve the highest power conversion efficiencies of 0.5% while annealed crystalline c-Sb2S3 device reaches power conversion efficiencies of 1.9% under 1 sun illumination.
关键词： surface photovoltage spectroscopy,extremely thin absorber solar cell,quantum mechanical density functional theory,amorphous antimony sulfide,Atomic layer deposition
更新于2025-09-19 17:13:59
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Adjusting Interfacial Chemistry and Electronic Properties of Photovoltaics Based on a Highly Pure Sb <sub/>2</sub> S <sub/>3</sub> Absorber by Atomic Layer Deposition
摘要： The combination of oxide and heavier chalcogenide layers in thin film photovoltaics suffers limitations associated with oxygen incorporation and sulfur deficiency in the chalcogenide layer or with a chemical incompatibility which results in dewetting issues and defect states at the interface. Here, we establish atomic layer deposition (ALD) as a tool to overcome these limitations. ALD allows one to obtain highly pure Sb2S3 light absorber layers, and we exploit this technique to generate an additional interfacial layer consisting of 1.5 nm ZnS. This ultrathin layer simultaneously resolves dewetting and passivates defect states at the interface. We demonstrate via transient absorption spectroscopy that interfacial electron recombination is one order of magnitude slower at the ZnS-engineered interface than hole recombination at the Sb2S3/P3HT interface. The comparison of solar cells with and without oxide incorporation in Sb2S3, with and without the ultrathin ZnS interlayer, and with systematically varied Sb2S3 thickness provides a complete picture of the physical processes at work in the devices.
关键词： interfacial layer,extremely thin absorber,transient absorption,atomic layer deposition,antimony sulfide,ultrathin layer
更新于2025-09-12 10:27:22