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Inverted perovskite solar cells (IPSCs) have attracted unprecedented attention due to their negligible hysteresis, long‐term operational stability, low temperature, and cost‐effective fabrication process, as well as wide applications. The power conversion efficiency (PCE) of IPSCs has skyrocketed from 3.9% in 2013 to certified 26.1% in 2023, which is over the certified 25.8% of regular counterpart, benefiting from the emergence of a great number of organic hole‐transporting materials (HTM). This review provides an overview of the recent development of organic hole‐transporting materials in the efficiency and stability of IPSCs, including organic small molecules and conjugated conductive polymers. The effective strategies for the charge‐transport layer and perovskite films of IPSCs are also discussed. Finally, the prospective for further development of IPSCs is outlined, including developing novel hole‐transporting materials and fabricating techniques to meet the requirements of commercial application. [ABSTRACT FROM AUTHOR]

As simple and versatile tools, additives have been widely used to refine active layer morphology and have played a crucial role in boosting the power conversion efficiency (PCE) of organic solar cells (OSCs). Herein, three novel solvent additives named Th‐FSi, Th‐ClSi, and Th‐BrSi with the same backbone of 2,5‐bis(trimethylsilyl)thiophene are designed and synthesized by substituting different halogens of fluorine, chlorine, and bromine, respectively. Notably, Th‐ClSi exhibits the more significant dipole moment and engages in non‐covalent interactions with a small‐molecule acceptor (SMA) L8‐BO, which slight adjustments in intermolecular interaction, crystallinity, and molecular packing in the PM6:L8‐BO active layer. Consequently, the OSCs incorporating Th‐ClSi outperform their Th‐FSi and Th‐BrSi counterparts in photo‐capturing, reduced energy loss, superior exciton dissociation, and charge transfer properties, out‐coming yields in an enhanced PCE of 18.29%. Moreover, by integrating a near‐infrared absorbing SMA (BTP‐eC9) guest into the PM6:L8‐BO matrix, the absorption spectrum to span 880–930 nm, and the resultant ternary OSCs achieve a commendable PCE of 19.17%, ranking among the highest efficiencies reported to date is expanded. These findings underscore the promise of halogenated thiophene‐based solvent additives as a potent avenue for morphological fine‐tuning and consequent PCE enhancement in OSCs. [ABSTRACT FROM AUTHOR]

To simultaneously stabilize cesium lead triiodide (CsPbI3) precursor solution and passivate the defects in CsPbI3 film is greatly significant for achieving highly stable and efficient CsPbI3 perovskite solar cells (PSCs). Herein, an effective redox 4‐fluorobenzothiohydrazide (FBTH) is developed to stabilize the precursor solution and passivate iodine/lead‐related defects for high‐quality CsPbI3 film. The comprehensive research confirms that 1) a new compound FBTH‐I is obtained from an effective redox interaction between FBTH and molecular iodine (I2) in perovskite precursor solution, which can effectively impede the formation of I2 molecule and restrain I− migration in perovskite film by forming N–H···I bond; 2) FBTH‐I can also passivate Pb‐related defects via forming S···Pb interaction. Consequently, the CsPbI3 PSC based on FBTH‐treated precursor solution exhibits a fascinating power conversion efficiency (PCE) of 21.41%, which is one of the highest PCE values among the reported pure CsPbI3 PSCs so far, and an outstanding stability against the harsh conditions, such as thermal annealing and continuous light‐illumination. [ABSTRACT FROM AUTHOR]

Employing volatile solid additives have emerged as a promising method to optimize the morphology and improve the performance of organic solar cells (OSCs). However, principles governing the efficient design of solid additives remain elusive. Herein, the programmed fluorination and/or bromination on benzene core to develop efficient additives for OSCs is reported. The programmed fluorination and/or bromination endow the five halogen benzene derivatives, 1,3,5‐trifluorobenzene, hexafluorobenzene, 1,3,5‐tribromo‐2,4,6‐trifluorobenzene (TFTB), 1,3,5‐tribromobenzene, and hexabromobenzene, with different melting and boiling points, volatility, as well as interactions with the host blend. Studies indicate that the additives with extremely high and low volatility are almost powerless and even detrimental to the morphology evolution. Among them, the combination of fluorine and bromine atoms on TFTB not only enables the more appropriate m.p./b.p. and volatility, but also exerts stronger molecular interactions with the host blend, giving rise to higher ordered molecular packing and more favorable morphology. Importantly, TFTB exhibits good universality to optimize the performances of OSCs with high power conversion efficiencies (PCEs; over 18%) in a group of binary blend systems, and an impressive PCE of 19.43% in the ternary PBTz‐F:PM6:L8‐BO system. [ABSTRACT FROM AUTHOR]

All‐inorganic perovskite solar cells (PSCs) have been the research focus due to their high thermal stability and proper band gap for tandem solar cells. However, their power conversion efficiency (PCE) is still lower than that of organic‐inorganic hybrid PSCs. Herein, a sacrificing dye (Rhodamine B isothiocyanate, RBITC) is developed to regulate the growth of perovskite film by in situ release of ethylammonium cations, isothiocyanate anions and benzoic acid molecules upon annealing and illumination. The ethylammonium cations can efficiently passivate surface defects. The isothiocyanate anions incorporate with uncoordinated Pb to regulate the crystallization process. The benzoic acid molecules facilitate the nucleation of the perovskite crystals. Especially, the illumination can accelerate the release of these beneficial ions/molecules to improve the quality of perovskite films further. After optimization with RBITC, a high open circuit voltage (VOC) of 1.24 V and a champion PCE of 20.95% are obtained, which are among the highest Voc and PCE values of CsPbI3 PSCs. Accordingly, the operational stability of the PSC devices is significantly improved. The results provide an efficient chemical strategy to regulate the formation of perovskite films in whole crystallization process for high performance all‐inorganic PSCs. [ABSTRACT FROM AUTHOR]

The poor interface quality between cesium lead triiodide (CsPbI3) perovskite and the electron transport layer limits the stability and efficiency of CsPbI3 perovskite solar cells (PSCs). Herein, a 4‐amino‐2,3,5,6‐tetrafluorobenzoate cesium (ATFC) is designed as a bifacial defect passivator to tailor the perovskite/TiO2 interface. The comprehensive experiments demonstrate that ATFC can not only optimize the conductivity, electron mobility, and energy band structure of the TiO2 layer by passivation of the undercoordinated Ti4+, oxygen vacancy (VO), and free OH defects but also promote the yield of high‐quality CsPbI3 film by synergistic passivation of undercoordinated Pb2+ defects with the CO group and F atom, and limiting I− migration via F···I interaction. Benefiting from the above interactions, the ATFC‐modified CsPbI3 device yields a champion power conversion efficiency (PCE) of 21.11% and an excellent open‐circuit voltage (VOC) of 1.24 V. Meanwhile, the optimized CsPbI3 PSC maintains 92.74% of its initial efficiency after aging 800 h in air atmosphere, and has almost no efficiency attenuation after tracking at maximum power point for 350 h. [ABSTRACT FROM AUTHOR]

High density of defects at interface severely affects the performance of perovskite solar cells (PSCs). Herein, cobalt (II) hexafluoro‐2,4‐pentanedionat (CoFAc), a hinge‐type fluorine‐rich complex, is introduced onto the surface of formamidinium cesium lead iodide (FACsPbI3) film to address the issues of perovskite/Spiro‐OMeTAD interface. The existence of CoFAc passivates both organic cation and halide anion vacancies by establishing powerful hydrogen bonds with HC(NH2)2+ (FA+) and strong ionic bonds with Pb2+ in perovskite films. In addition, CoFAc serves as a connecting link to enhance interfacial hole‐transport kinetics via interacting with Spiro‐OMeTAD. Consequently, FACsPbI3 PSCs with CoFAc modification display a champion power conversion efficiency (PCE) of 24.64% with a charming open‐circuit voltage (VOC) of 1.191 V, which is the record VOC among all the reported organic‐inorganic hybrid PSCs with TiO2 as electron transport layer. Furthermore, CoFAc‐modified devices exhibit an outstanding long‐term stability, which can maintain 95% of their initial PCEs after exposure to ambient atmosphere for 1500 h without any encapsulation. [ABSTRACT FROM AUTHOR]

The ternary copolymerization strategy has emerged as a promising strategy for developing high‐efficiency donor polymers in polymer solar cells (PSCs). Terpolymers based on the star polymer PM6 have already realized good photovoltaic performance. However, challenges such as the intricate synthesis of fluorine‐substituted benzodithiophene (F‐BDT) unit of PM6 and entropy increase induced by backbone disorder have hindered the construction of high‐performance donor terpolymers. In this work, these challenges are addressed by opting for the cost‐effective chlorinated‐substituted benzodithiophene unit (Cl‐BDT) as an alternative to F‐BDT and incorporating the large dipole moment and electron‐deficient TPD group as the third component into the high‐performance donor polymer of PM7. As expected, this approach effectively suppresses terpolymer backbone disorder while enhancing crystallinity, thereby optimizing morphology and improving charge generation and transport. Remarkably, the PM7‐TPD‐10‐based device with 10% TPD replacement achieves a champion power conversion efficiency (PCE) of 18.26%. After introducing PM7‐TPD‐10 as the third component into D18:L8‐BO blend, a dual mechanism for improving the efficiency to 19.40% is realized. This work demonstrates that the high dipole moiety as the third component to construct terpolymers is an important strategy to suppress the backbone disorder and increase the crystallinity, facilitating the optimization of morphology and device performance. [ABSTRACT FROM AUTHOR]