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Abstract Antimony selenide (Sb₂Se₃) has excellent directional optical and electronic behaviors due to its quasi‐1D nanoribbons structure. The photovoltaic performance of Sb₂Se₃solar cells largely depends on the orientation of the nanoribbons. It is desired to grow these Sb₂Se₃ribbons normal to the substrate to enhance photoexcited carrier transport. Therefore, it is necessary to develop a strategy for the vertical growth of Sb₂Se₃nanoribbons to achieve high‐efficiency solar cells. Since antimony sulfide (Sb₂S₃) and Sb₂Se₃are from the same space group (Pbnm) and have the same crystal structure, herein an ultrathin layer (≈20 nm) of Sb₂S₃has been used to assist the vertical growth of Sb₂Se₃nanoribbons to improve the overall efficiency of Sb₂Se₃solar cell. The Sb₂S₃thin layer deposited by the hydrothermal process helps the Sb₂Se₃ribbons grow normal to the substrate and increases the efficiency from 5.65% to 7.44% through the improvement of all solar cell parameters. This work is expected to open a new direction to tailor the Sb₂Se₃grain growth and further develop the Sb₂Se₃solar cell in the future. 

Antimony selenide (Sb₂Se₃) emerges as a promising sunlight absorber in thin film photovoltaic applications due to its excellent light absorption properties and carrier transport behavior, attributed to the quasi‐one‐dimensional Sb₄Se₆‐nanoribbon crystal structure. Overcoming the challenge of aligning Sb₂Se₃‐nanoribbons normal to substrates for efficient photogenerated carrier extraction, a solution‐processed nanocrystalline Sb₂(S,Se)₃‐seeds are employed on the CdS buffer layer. These seeds facilitate superstrated Sb₂Se₃thin film solar cell growth through a close‐space sublimation approach. The Sb₂(S,Se)₃‐seeds guided the Sb₂Se₃absorber growth along a [002]‐preferred crystal orientation, ensuring a smoother interface with the CdS window layer. Remarkably, Sb₂(S,Se)₃‐seeds improve carrier transport, reduce series resistance, and increase charge recombination resistance, resulting in an enhanced power conversion efficiency of 7.52%. This cost‐effective solution‐processed seeds planting approach holds promise for advancing chalcogenide‐based thin film solar cells in large‐scale manufacturing. 

Antimony selenide (Sb2Se3) is a promising light absorber material for solar cells because of its superior photovoltaic properties. However, the current performance of the Sb2Se3 solar cell is much lower than its theoretical value (∼32%) due to its low open-circuit voltage (VOC). In this paper, we have demonstrated inorganic vanadium oxides (VOx) as a hole transport layer (HTL) for Sb2Se3 solar cells to enhance efficiency through the VOC improvement. Here, a solution-processed VOx through the decomposition of the triisopropoxyvanadium (V) oxide is deposited on the Sb2Se3 absorber layer prepared by close-spaced sublimation (CSS). With VOx HTL, the built-in voltage (Vbi) is significantly increased, leading to improved VOC for the Sb2Se3 solar cell devices. As a result, the efficiency of the device increases from an average efficiency of 5.5% to 6.3% with the VOx.