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Poly[bis(4‐phenyl)(2,4,6‐trimethylphenyl)amine (PTAA) is one of the most efficient hole transport materials for p–i–n structured perovskite solar cells (PSCs). However, the hydrophobicity of PTAA causes wettability problems and is thereby associated with low yield and poor reproducibility. Herein, a new strategy for improving the perovskite precursor wettability on PTAA is developed. A Cu2(Thiourea)Br2 complex interfacial layer is introduced on the PTAA, improving the coverage of perovskite precursors and thereby the perovskite film. Partially dissolved Cu2(Thiourea)Br2 in the perovskite absorber further enhances band alignment and carrier extraction between layers. With the addition of Cu2(Thiourea)Br2 layer on nondoped PTAA, PSCs in p–i–n structure with a bandgap of 1.63 eV have achieved over 21% efficiency both on 0.1 and 1.0 cm2 sized devices with a significantly improved yield and reproducibility. Unencapsulated devices retain 100% of their initial efficiency after 2000 h at 65 °C. [ABSTRACT FROM AUTHOR]

Effectively incorporating alkali metals or alternative isovalent cations into Cu2ZnSnS4 (CZTS) is considered one of the most promising strategies for realizing a step‐change improvement in the photovoltaic device performance. Herein, the local distribution of Na and Cd by a moisture‐assisted postdeposition annealing (MAPDA) treatment combined with a subsequent heterojunction heat treatment is manipulated. The MAPDA treatment facilitates the controllable reduction of the Na concentration, thus promoting the spontaneous diffusion of Cd into the heterojunction region. A subsequent 150 °C low‐temperature heterojunction heat treatment after MAPDA treatment enables further modification of Cd and Na distributions, leading to significantly enhanced optoelectronic properties at the CZTS/CdS heterojunction and greatly improved device performance with a peak conversion efficiency of 9.40%. The modified heterojunction significantly improves quasi‐Fermi‐level splitting under low‐photon injection, making CZTS solar cells more feasible in low‐light applications. This work provides an effective approach to simultaneously manipulate the distribution of Na and Cd, enabling pronounced modification of the heterojunction quality of CZTS solar cells and boost of conversion efficiencies. Insights gleaned herein may also be applicable to manipulating other critical trace elements in chalcogenide materials in general. [ABSTRACT FROM AUTHOR]

Antimony sulfide (Sb2S3) is a promising wide‐bandgap photovoltaic material, and a potential top‐cell candidate for next‐generation Si‐based tandem solar cells. The most widely used electron transport layers in Sb2S3 solar cells are TiO2 and CdS, which present an obvious performance variation in open‐circuit voltage (VOC) and short current (Jsc). However, the mechanisms behind the performance disparity because of the electron transport layer (ETL) have not been disclosed. Herein, a comprehensive comparative study of using TiO2 and CdS as the electron transport layers in Sb2S3 solar cells is presented, which covers their influence on preferential crystal orientation, band alignment, interface, and bulk defects. It is found that the CdS ETL results in less interfacial defects and more favorable band alignment, enabling a higher VOC, while the high resistance of the CdS film and parasitic light absorption restricts the JSC. The findings provide a substantial guidance on device optimization for Sb2S3 solar cells. [ABSTRACT FROM AUTHOR]

Antimony sulfide is an emerging 1D nontoxic Earth‐abundant photovoltaic material with favorable wide bandgap as a suitable top‐cell candidate for multijunction tandem solar cells. However, the current fabrication technology for Sb2S3 solar cells relies heavily on a high‐purity Sb2S3 source, which limits its large‐scale deployment. Therefore, it is attractive to fabricate the Sb2S3 solar cells directly from the raw stibnite source, which can be cost effective by avoiding the complicated, costly purification and refinement process of the stibnite ore, while reducing process‐emitted pollution. Herein, high‐quality Sb2S3 films (thickness: ≈1 μm) by the vapor transport deposition of raw stibnite ore powder are obtained, followed by a sulfurization process to remove the surface oxides and facilitate alkali element redistribution. In this way, the particle size is increased from ≈500 nm to ≈1.5 μm, the carrier concentration of the Sb2S3 film is increased from ≈1015 to ≈1016 cm−3, and the power conversion efficiency of Sb2S3 solar cell is increased by more than two times. Through the elemental distribution analysis, it is found that it is the redistribution of alkali elements introduced from the natural stibnite ore that induces the grain growth, contributes toward defect suppression, and leads toward enhanced device performance. [ABSTRACT FROM AUTHOR]

Kesterite Cu2ZnSnS4 (CZTS) solar cell has emerged as one of the most promising thin‐film photovoltaic technologies that allows for cheap, clean, and efficient renewable power in the future. Nevertheless, limited by the large photovoltage deficit caused by severe interface recombination, the potential of CZTS solar cells is far from being fully tapped. Herein, it is demonstrated that the carrier density of the CZTS absorber and the acceptor‐like interface defects are two critical factors governing the interface recombination in addition to the unfavorable conduction band alignment. Results of device simulation suggest that passivating the acceptor‐like interface defects combined with appropriate absorber carrier density is the essential way to promote the photovoltage and efficiency of CZTS solar cells to a more competitive level. It is believed that these results could be generally applicable to the interface recombination of other heterojunction solar cells. [ABSTRACT FROM AUTHOR]

The anomalous optoelectronic properties of a quasi‐vertical orientated Chalcostibite CuSbS2 thin film synthesized on glass substrate are studied in detail. Two well‐separated absorption edges of CuSbS2 are identified by photothermal‐deflection spectroscopy (PDS) at 1.48 and 0.90 eV. The formation mechanism of the 0.9 eV infrared edge is found to be crystal orientation related. The properties of the 0.9 eV absorption edge are subject to detailed investigation using temperature‐dependent photoluminescence (TDPL) characterization, which attribute the origin of this phenomenon to a deep‐level defect state near the mid‐bandgap of CuSbS2. [ABSTRACT FROM AUTHOR]

While interfacial and grain‐boundary passivation presently attract enormous research interest for perovskite solar cells (PSCs), the improvement of Cs‐(FAPbI3)X(MAPbBr3)Y bulk quality still lacks systematical study, especially for constructing polycrystalline layers in planar configurations. Here, a DMSO‐molecule‐process for improving the quality of Cs‐(FAPbI3)0.85(MAPbBr3)0.15 is developed, where the molar ratio of precursors, the kind of anti‐solvents, and speed‐time profiles are found critical. The optimized treatment significantly enhanced the crystal orientation, grain size, surface roughness, photo‐response, carrier lifetime, and contact potential difference of absorbers. Cs‐(FAPbI3)0.85(MAPbBr3)0.15 absorbers also present superior charge transport, as well as reduced carrier recombination and decreased trap densities via DMSO‐molecule‐control, enabling performance improvement on both long‐term stability and photovoltaic parameters of 1 cm2 PSCs. Champion planar cells demonstrated a power conversion efficiency (PCE) of 21.07% (0.159 cm2) and PCE of 19.4% (1 cm2) with negligible hysteresis. Moreover, 1 cm2 devices retained 90% of initial PCE after aging 50 days in ambient air. DMSO‐molecule‐control is demonstrated to enhance the morphological and electronic qualities of Cs‐(FAPbI3)0.85(MAPbBr3)0.15 absorbers, thus increasing the efficiency (reaching 19.4%) and boosting the long‐term stability (retaining 90% of the initial efficiency after 50 days in ambient air) of 1 cm2 sized planar perovskite solar cells. [ABSTRACT FROM AUTHOR]