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Two‐step sequential deposition is a widespread technique for the fabrication of perovskite films, renowned for its better control of the crystallization process. However, achieving a well‐controlled and complete reaction of PbI2 by organic ammonium salts remains a key challenge. Previous studies have predominantly focused on regulating the properties of the PbI2 layer while paying less attention to the high reactivity of organic ammonium salts. In this study, the natural molecule anethole is first explored to control perovskite crystallization during two‐step sequential deposition, focusing on the reactivity modulation of organic formamidine ion (FA+). It is demonstrated that FA+ exhibits strong hydrogen bond interactions with anethole, inhibiting the high reactivity of FA+ and effectively delaying the rapid reaction between FAI and PbI2. This decelerates the crystallization kinetics of perovskite films, facilitating the orderly and complete reaction of PbI2 by FAI while suppressing detrimental δ‐phase formation. Consequently, FA‐based perovskite films with high crystallinity, preferred orientation, and low defect state density are obtained. The fabricated planar hole transport layer‐free carbon electrode perovskite solar cells deliver an efficiency of 20.41% (certified efficiency of 20.0%), which is a new record for this kind of solar cell. [ABSTRACT FROM AUTHOR]

The high‐quality perovskite film is a prerequisite for high‐performance optoelectronic devices. Herein, CdSe colloidal quantum dots (QDs) serve as crystallization seeds for the first time to modulate the nucleation and crystal growth processes simultaneously of the CsPbI2Br film in the ambient environment. As additives, CdSe QDs help promote the nucleation process in the initial stage of perovskite formation. In addition, it is revealed that the surface ligands of QDs also have an essential influence on the subsequent crystal growth of the perovskite film. The bifunctional ligands on the surface of QDs are beneficial in delaying the growth process of perovskite due to the free functional groups at the ends. The CsPbI2Br film prepared with bifunctional organic ligand‐capped CdSe QD additives shows better crystallinity than that of the inorganic ligand‐based one due to the dual function of these kinds of QDs in not only promoting nucleation but also retarding crystal growth of CsPbI2Br crystals. As a result, the high‐quality CsPbI2Br film with a low defect state density is prepared in the ambient environment. The optimized efficiency of the assembled hole‐conductor‐free carbon‐based perovskite solar cells (C‐PSCs) is increased from 12.73% to 14.49%, which is one of the best results for all‐inorganic C‐PSCs. [ABSTRACT FROM AUTHOR]

All‐inorganic CsPbI3 quantum dots (QDs) have shown great potential in photovoltaic applications. However, their performance has been limited by defects and phase stability. Herein, an anion/cation synergy strategy to improve the structural stability of CsPbI3 QDs and reduce the pivotal iodine vacancy (VI) defect states is proposed. The Zn‐doped CsPbI3 (Zn:CsPbI3) QDs have been successfully synthesized employing ZnI2 as the dopant to provide Zn2+ and extra I−. Theoretical calculations and experimental results demonstrate that the Zn:CsPbI3 QDs show better thermodynamic stability and higher photoluminescence quantum yield (PLQY) compared to the pristine CsPbI3 QDs. The doping of Zn in CsPbI3 QDs increases the formation energy and Goldschmidt tolerance factor, thereby improving the thermodynamic stability. The additional I− helps to reduce the VI defects during the synthesis of CsPbI3 QDs, resulting in the higher PLQY. More importantly, the synergistic effect of Zn2+ and I− in CsPbI3 QDs can prevent the iodine loss during the fabrication of CsPbI3 QD film, inhibiting the formation of new VI defect states in the construction of solar cells. Consequently, the anion/cation synergy strategy affords the CsPbI3 quantum dot solar cells (QDSC) a power conversion efficiency over 16%, which is among the best efficiencies for perovskite QDSCs. [ABSTRACT FROM AUTHOR]

Lead‐free CsSnX3 perovskite NCs are becoming a promising alternative to CsPbX3 (X=Cl, Br, I), but suffer from extremely poor stability. Herein, we highlight the significant effect of SnII precursors used in the synthesis on the stability of the resultant CsSnX3 NCs. A method is proposed for synthesizing CsSnX3 NCs using Cs2CO3, SnC2O4, and NH4X as corresponding constituent precursors, wherein the ratio of reactants can be easily adjusted. Stable CsSnX3 NCs can be obtained with the use of antioxidative SnC2O4 as the SnII precursor. Experimental results show that the improvement of NCs stability is mainly ascribed to the role of oxalate in the SnC2O4 precursor. Oxalate ion has a strong antioxidative ability and can effectively inhibit the oxidation of SnII during the synthesis. Besides, oxalate as a bidentate capping ligand is shown to be coordinated on the surface of formed NCs. This can not only passivate the uncoordinated Sn on the surface but also prevent the oxidation of the NCs. [ABSTRACT FROM AUTHOR]

Lead-free CsSnX 3 perovskite NCs are becoming a promising alternative to CsPbX 3 (X=Cl, Br, I), but suffer from extremely poor stability. Herein, we highlight the significant effect of Sn II precursors used in the synthesis on the stability of the resultant CsSnX 3 NCs. A method is proposed for synthesizing CsSnX 3 NCs using Cs 2 CO 3 , SnC 2 O 4 , and NH 4 X as corresponding constituent precursors, wherein the ratio of reactants can be easily adjusted. Stable CsSnX 3 NCs can be obtained with the use of antioxidative SnC 2 O 4 as the Sn II precursor. Experimental results show that the improvement of NCs stability is mainly ascribed to the role of oxalate in the SnC 2 O 4 precursor. Oxalate ion has a strong antioxidative ability and can effectively inhibit the oxidation of Sn II during the synthesis. Besides, oxalate as a bidentate capping ligand is shown to be coordinated on the surface of formed NCs. This can not only passivate the uncoordinated Sn on the surface but also prevent the oxidation of the NCs., (© 2020 Wiley-VCH GmbH.)