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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]

A double‐fibril network of the photoactive layer morphology is recognized as an ideal structure facilitating exciton diffusion and charge carrier transport for high‐performance organic solar cells (OSCs). However, in the layer‐by‐layer processed OSCs (LbL‐OSCs), polymer donors and small molecule acceptors (SMAs) are separately deposited, and it is challenging to realize a fibril network of pure SMAs with the absence of tight interchain entanglement as polymers. In this work, crystalline small molecule donors (SMDs), named TDZ‐3TR and SeDZ‐3TR, were designed and introduced into the L8‐BO acceptor solution, forcing the phase separation and molecular fibrilization. SeDZ‐3TR showed higher crystallinity and lower miscibility with L8‐BO acceptor than TDZ‐3TR, enabling more driving force to favor the phase separation and better molecular fibrilization of L8‐BO. On the other hand, two donor polymers of PM6 and D18 with different fibril widths and lengths were put together to optimize the fibril network of the donor layer. The simultaneously optimization of the acceptor and donor layers resulted in a more ideal double‐fibril network of the photoactive layer and an impressive power conversion efficiency (PCE) of 19.38 % in LbL‐OSCs. [ABSTRACT FROM AUTHOR]

The improvement of power conversion efficiency (PCE) and stability of the perovskite solar cell (PSC) is hindered by carrier recombination originating from the defects at the buried interface of the PSC. It is crucial to suppress the nonradiative recombination and facilitate carrier transfer in PSC via interface engineering. Herein, P‐biguanylbenzoic acid hydrochloride (PBGH) is developed to modify the tin oxide (SnO2)/perovskite interface. The effects of PBGH on carrier transportation, perovskite growth, defect passivation, and PSC performance are systematically investigated. On the one hand, the PBGH can effectively passivate the trap states of Sn dangling bonds and O vacancies on the SnO2 surface via Lewis acid/base coordination, which is conducive to improving the conductivity of SnO2 film and accelerating the electron extraction. On the other hand, PBGH modification assists the formation of high‐quality perovskite film with low defect density due to its strong interaction with PbI2. Consequently, the PBGH‐modified PSC exhibits a champion power conversion efficiency (PCE) of 24.79%, which is one of the highest PCEs among all the FACsPbI3‐based PSCs reported to date. In addition, the stabilities of perovskite films and devices under high temperature/humidity and light illumination conditions are also systematically studied. [ABSTRACT FROM AUTHOR]

A desired morphology is essential for achieving efficient polymer solar cells. Donors and acceptors with appropriate crystallization can lead to a suitable phase-separated morphology for effective photocurrent generation process. Inspired by the success of Y6 acceptors and the 2D side chain engineering on popular polymer donors and small molecule acceptors, the usage of unique 2D 3,4-ethylene dioxythiophene (EDOT) side chains on Y6 to regulate its crystallinity, compatibility, and thus the related blend morphology is explored. In this study, two molecules of BTP-EDOT-4F and BTP-EDOT-4Cl with such unique 2D EDOT side chains are designed and synthesized. Due to the advantage of EDOT side chain, when these molecules are blended with PM6, the decent power conversion efficiencies (PCEs) of 16.78% and 15.87% are obtained. Furthermore, BTP-EDOT-4F is selected as the third component and added into PM6:L8-BO binary system to form ternary blends. The optimized crystallinity, compatibility, and morphology of such ternary blend are discovered in the presence of BTP-EDOT-4F, which enables efficient exciton dissociation and charge transport as well as decreased recombination, resulting in higher short circuit current density Jsc) and fill factor. Finally, the outstanding PCE of 18.56% is achieved in ternary blends containing PM6, L8-BO, and BTP-EDOT-4F. [ABSTRACT FROM AUTHOR]

The molecular planarity of a small molecule donor is one of the key factors affecting its molecular packing behavior, the morphology of the related active blend and thus the photovoltaic properties of all small molecule organic solar cells (ASM-OSCs). In this contribution, a series of new benzodithiophene (BDT)-based A-π-D-π-A type small molecules were developed, namely SD1, SD2 and SD3, by combining the chemical modification of side chain (sulfuration), π-bridge (alkoxy groups introducing) and end group (different type or different alkyl chain). The sulfuration of the BDT side chains and introducing alkoxy group to the π-bridge could induce intermolecular S⋯S and intramolecular S⋯O non-covalent interactions for higher planarity of these small molecules. The rhodanine and cyanoacetate end groups showed less effect on the optical and electronic properties but significantly affected the molecular packing behavior and blend morphology. From SD1:Y6-T to SD2:Y6-T and SD3:Y6-T, the face-to-face packing was gradually reduced, while the face-to-edge packing was increased, which resulted in lowered exciton dissociation efficiency, further decreased the device performance. SD1:Y6-T blend exhibited more favorable face-to-face packing and ideal morphology for efficient charge dissociation and transport, contributing to a champion PCE of 10.12%. This work provided a deep insight of the donor and acceptor packing behavior effect on the photovoltaic property by molecular design. [Display omitted] [ABSTRACT FROM AUTHOR]