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Quasi‐2D perovskites have attracted significant attention because of their environmental robustness and superior long‐term stability compared with their 3D counterparts. However, they typically consist of a mixture of multiple quantum wells with different optoelectrical properties, which degrades the electronic properties and hinders further electronic applications. Here, to challenge this issue, a surface p‐doping strategy involving the introduction of a thiophene‐containing polymer onto the surface of quasi‐2D tin perovskites is reported. The tin ions in the perovskites effectively interact with the sulfur atoms in the thiophene moieties, thereby generating hole carriers and inducing p‐doping. The resulting doped quasi‐2D perovskites exhibit excellent surface crystallinity, lower trap density, and enhanced charge carrier transport capability along the perovskite semiconductor channels. Consequently, the doped quasi‐2D tin perovskite‐based transistors exhibit a high field‐effect mobility of 53 cm2V−1s−1 (7 cm2V−1s−1 for the control device) and an outstanding on/off ratio (>107), together with superior operational stability. [ABSTRACT FROM AUTHOR]

The utilization of wide bandgap (WBG) tin halide perovskites (Sn‐HPs) offers an environmentally friendly alternative for multi‐junction Sn‐HP photovoltaics. Nonetheless, rapid crystallization leads to suboptimal film morphology and substantial creation of defect states, which undermine device efficiency. This study introduces 4‐Phenylthiosemicarbazide (4PTSC) as an additive to achieve a densely packed Sn‐HP film with fewer imperfections. The strong chemical coordination between SnI2 and the functional groups S═C─N (Sn···S═C─N), NH2, and phenyl conjugation enhances solution stability and supports the delay of perovskite crystallization through adduct formation. This process yields pinhole‐free films with preferred grain growth. 4PTSC acts as a strong coordination complex and a reducing agent to passivate uncoordinated Sn2+ and halide ions and reduce the formation of SnI4, thereby reducing defect formation. The π‐conjugated phenyl ring in the 4PTSC facilitates the preferred crystal growth orientation of perovskite grains. Furthermore, the hydrophobic nature of 4PTSC mitigates Sn2+ oxidation by repelling moisture, enhancing stability. The open circuit voltage significantly increased from 0.78 to 0.94 V, resulting in achieving the champion efficiency of 12.22% (certified 11.70%), surpassing all previously reported efficiencies for WBG Sn halide perovskite solar cells. Additionally, the unencapsulated 4PTSC‐1.0 device maintained outstanding stability over 1200 h under ambient atmospheric conditions. [ABSTRACT FROM AUTHOR]

Photoinduced intermolecular charge transfer (PICT) determines the voltage loss in bulk heterojunction (BHJ) organic photovoltaics (OPVs), and this voltage loss can be minimized by inducing efficient PICT, which requires energy‐state matching between the donor and acceptor at the BHJ interfaces. Thus, both geometrically and energetically accessible delocalized state matching at the hot energy level is crucial for achieving efficient PICT. In this study, an effective method for quantifying the hot state matching of OPVs was developed. The degree of energy‐state matching between the electron donor and acceptor at BHJ interfaces was quantified using a mismatching factor (MF) calculated from the modified optical density of the BHJ. Furthermore, the correlation between the open‐circuit voltage (Voc) of the OPV device and energy‐state matching at the BHJ interface was investigated using the calculated MF. The OPVs with small absolute MF values exhibited high Voc values. This result clearly indicates that the energy‐state matching between the donor and acceptor is crucial for achieving a high Voc in OPVs. Because the MF indicates the degree of energy‐state matching, which is a critical factor for suppressing energy loss, it can be used to estimate the Voc loss in OPVs. [ABSTRACT FROM AUTHOR]

Because of its high conductivity, wide bandgap, and excellent photostability, tin oxide (SnO2) has long been recognized as an electron‐transport layer (ETL) in organic solar cells (OSCs). However, the energy‐level mismatch between the work function (WF) of SnO2 and the lowest unoccupied molecular orbital level of Y‐series nonfullerene acceptors (NFAs), along with the abundance of surface defects on SnO2, have limited its widespread application as ETLs in OSCs. Herein, a novel approach utilizing urea‐functionalized polyethyleneimine (PEI) materials called u‐PEIs for modifying SnO2 is introduced. This modification, which serves dual purposes of WF modulation and surface‐defect passivation, can mitigate the energy barriers of SnO2/Y‐series NFA and increase the conductivity of the SnO2 film. PM6:Y6‐based OSCs with u‐PEI‐modified SnO2 (SnO2:u‐PEI) ETLs exhibit a remarkable efficiency of 16%, which significantly exceeds that (13.5%) achieved with bare SnO2‐based OSCs, along with outstanding photo‐ and thermal stability. This study confirms the efficacy of urea‐functionalized PEI for efficient and stable OCSs, paving the way for SnO2 applications. [ABSTRACT FROM AUTHOR]

Organic solar cells (OSCs) have been studied widely as renewable energy resources for a few decades owing to their technological advantages, including low cost, light weight, flexibility, and the potential of large area printing. To upgrade the active layers of OSCs into an optimized form, a simple and straightforward strategy is demonstrated by introducing two types of size‐controlled chevron (V)‐shaped blades to delicately control PM6:Y6‐based bulk heterojunction (BHJ) films under ambient conditions. A power conversion efficiency of 15.97% is achieved from the blade‐coating methods using a small‐sized V‐shaped blade (V1), compared with 14.31% using a conventional flat blade (F). Using blade coating based on V1 improves the phase separation and molecular crystallinity in the active layer, which lead to decreased trap‐assisted recombination and leakage current, finally increasing the short circuit current and fill factor. In addition, following these morphological changes in the optimal BHJ structure, the devices printed with V1 exhibit higher stability in the long‐term shelf‐life test (320 h storage in ambient conditions). Notably, strategy is a facile layer fabrication method that adopts V‐shaped blades to achieve high device performance and stability for the practical use of large‐area OSCs. [ABSTRACT FROM AUTHOR]

The introduction of molecular doping process is necessary to enhance the optic and electronic properties of organic semiconductors for facilitating charge transport. In particular, since the doping process has a positive influence on the charge transfer interaction between host semiconductor and dopant, improved mobility has been efficiently achieved. Despite its advantages, doping technologies in organic solar cells (OSCs) are emphasized to the development of n‐type dopants used for balancing the electron and hole. In addition, since the bulk‐heterojunction microstructure in OSCs has randomly blended phases of the donor and acceptor, it is important to optimize charge extraction without loss by controlling the morphology. Herein, OSCs by p‐type doping with formic acid (FA) into a photoactive layer is reported. The champion device yields a significantly improved power conversion efficiency from 14.3% to 15.3% with a high fill factor of 71.7%. It is found that the p‐doped photoactive layer exhibits enhanced conductivity, improved carrier mobilities, suppressed charge recombination, and lowered leakage current. The FA simultaneously acts as a film morphology controller of the photoactive layer with enhanced phase separation to transport the charge efficiently. Thus, the doping process with FA can maintain the device performance in stability tests (95.6% remaining). [ABSTRACT FROM AUTHOR]

Bulk heterojunction (BHJ) composites show improved power conversion efficiencies when optimized in terms of morphology using various film processing methods. A reduced carrier recombination loss in an optimized BHJ was characterized previously. However, the driving force that leads to this reduction was not clearly understood. In this study, we focus on the decreased carrier recombination loss and its driving force in optimized nonfullerene acceptor‐based PTB7‐Th:IEICO‐4F BHJ composites. We demonstrate that the optimized BHJ shows deactivation in the sub‐nanosecond nongeminate carrier recombination process. The driving force for this deactivation was determined to be the improved interchain hole delocalization between the polymers. An enhanced interchain hole delocalization was observed using steady‐state photoinduced absorption (PIA) spectroscopy. In particular, increased splitting between the polaron PIA bands was noted. Moreover, improved interchain hole delocalization was observed for other state‐of‐the‐art BHJ materials, including D18:Y6 with optimized morphologies. [ABSTRACT FROM AUTHOR]

Solution‐processed transition metal oxides (TMOs) prepared from complex ion precursors are developed as promising scalable interfacial layers for non‐fullerene organic photovoltaics (OPVs); however, challenges remain in achieving defect‐free and highly oriented metal‐oxygen networks without post‐deposition treatments due to the presence of residual organic metal‐binding ligands in films. Herein, the novel strategy that the problematic organic metal‐binding ligands in TMO precursors can be successfully eliminated by an anion‐induced catalytic reaction (ACR) at room temperature is demonstrated, in which the low‐level anions induce electron redistribution and instability of TMO precursors, expediting binding ligand removal during the hydrolysis reaction. The subsequent condensation process facilitates a dimensionally confined and continuous metal‐oxygen network with a 20‐fold increase in electrical conductivity (from 8.4 × 10−4 to 1.8 × 10−2 S m−1) and superior work function tunability (from 5.1 to 5.3 eV) compared to the pristine film. The ACR‐derived TMO thin film on top of a ternary PBDB‐TF:Y6:PC71BM photoactive layer enables an inverted device configuration with improved efficiency of 17.6%, as well as enhanced stability over 70% of the initial efficiency for up to 100 h AM 1.5G illumination. [ABSTRACT FROM AUTHOR]