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High-quality perovskite films are essential for achieving high performance of optoelectronic devices; However, solution-processed perovskite films are known to suffer from compositional and structural inhomogeneity due to lack of systematic control over the kinetics during the formation. Here, the microscopic homogeneity of perovskite films is successfully enhanced by modulating the conversion reaction kinetics using a catalyst-like system generated by a foaming agent. The chemical and structural evolution during this catalytic conversion is revealed by a multimodal synchrotron toolkit with spatial resolutions spanning many length scales. Combining these insights with computational investigations, a cyclic conversion pathway model is developed that yields exceptional perovskite homogeneity due to enhanced conversion, having a power conversion efficiency of 24.51% for photovoltaic devices. This work establishes a systematic link between processing of precursor and homogeneity of the perovskite films.

The most efficient and stable perovskite solar cells (PSCs) are made from a complex mixture of precursors. Typically, to then form a thin film, an extreme oversaturation of the perovskite precursor is initiated to trigger nucleation sites, e.g., by vacuum, an airstream, or a so-called antisolvent. Unfortunately, most oversaturation triggers do not expel the lingering (and highly coordinating) dimethyl sulfoxide (DMSO), which is used as a precursor solvent, from the thin films; this detrimentally affects long-term stability. In this work, (the green) dimethyl sulfide (DMS) is introduced as a novel nucleation trigger for perovskite films combining, uniquely, high coordination and high vapor pressure. This gives DMS a universal scope: DMS replaces other solvents by coordinating more strongly and removes itself once the film formation is finished. To demonstrate this novel coordination chemistry approach, MAPbI3 PSCs are processed, typically dissolved in hard-to-remove (and green) DMSO achieving 21.6% efficiency, among the highest reported efficiencies for this system. To confirm the universality of the strategy, DMS is tested for FAPbI3 as another composition, which shows higher efficiency of 23.5% compared to 20.9% for a device fabricated with chlorobenzene. This work provides a universal strategy to control perovskite crystallization using coordination chemistry, heralding the revival of perovskite compositions with pure DMSO.

Weak bonding between the perovskite and charge transport layers can lead to interfacial defects, hindering charge transfer and limiting the efficiency and stability of perovskite solar cells (PSCs). To address this issue, two halogenated spiro[fluorene‐9,9′‐xanthene]‐based molecules (SFX‐DM‐F and SFX‐DM‐Cl) are designed as an interfacial layer between perovskite and hole transport materials (HTMs). Both first‐principles simulations and experimental results are used to demonstrate that these halogenated interfacial layers improve the contact stability between perovskite's Pb(II) and HTMs, increasing the efficiency of charge transfer. The similar structure of interlayer to HTM also enhances the interfacial hole transfer integral, favoring effective hole transport. The PSCs based on SFX‐DM‐Cl achieve power conversion efficiencies of 24.8% (0.0625 cm2) and 23.1% (1 cm2). Even after 2000 h at a relative humidity of 15–20%, the unencapsulated PSC retains 94% of its initial efficiency. This work proposes the halogenated homologous HTMs as interfacial molecular bridges to optimize weak chemical bonds and hole transfer, thereby enabling efficient and stable PSCs. [ABSTRACT FROM AUTHOR]

The efficient functioning of perovskite solar cells largely depends on the interaction between perovskite halide materials and the hole‐transport layer poly(3‐hexylthiophene) (P3HT). However, a high rate of nonradiative recombination often hampers this interaction, leading to poor performance of the solar cells. We have developed a technique to modify the interface using a long‐chain alkyl halide molecule called n‐hexyl trimethylammonium bromide to address this issue. This modification technique significantly improves hole extraction, leading to an impressive open‐circuit voltage of 1.14 V and a power conversion efficiency of 15.8% for inorganic perovskite CsPbI3 with P3HT as a dopant‐free hole‐transport layer. This breakthrough can pave the way for developing more efficient and sustainable solar cells. [ABSTRACT FROM AUTHOR]

Developing efficient wide‐bandgap perovskites is critical to exploit the benefits of a multi‐absorber solar cell and engineering commercially attractive tandem solar cells. Here, a robust, additive‐free, methylammonium‐free triple halide composition for the fabrication of close‐to‐ideal wide‐bandgap perovskites (1.64 eV) is reported. The introduction of low percentages of chloride into the perovskite layer avoided photoinduced halide segregation and lead to an evident improvement in the crystallization process, reaching enhanced open‐circuit voltages as high as 1.23 V. A perovskite of these characteristics is introduced for the first time in a p‐i‐n single‐junction configuration using a self‐assembled monolayer, with devices achieving photoconversion efficiencies of up to 22.6% with ultra‐high stability, retaining ≈80% of their initial efficiency after >1000 h of continuous operation unencapsulated in a nitrogen atmosphere at 85 °C. This result paves the way toward highly efficient multi‐junction tandem solar cells, bringing perovskite technology closer to commercialization. [ABSTRACT FROM AUTHOR]

Nickel oxide (NiO1+δ) is a versatile material used in various fields such as optoelectronics, spintronics, electrochemistry, and catalysis which is prepared with a wide range of deposition methods. Herein, for the deposition of NiO1+δ films, the reactive gas flow sputtering (GFS) process using a metallic Ni hollow cathode is developed. This technique is distinct and has numerous advantages compared to conventional sputtering methods. The NiO1+δ films are sputtered at low temperatures (100 ºC) for various oxygen partial pressures during the GFS process. Additionally, Cu‐incorporated NiO1+δ (CuxNi1−xO1+δ) films are obtained with 5 and 8 at% Cu. The thin films of NiO1+δ are characterized and evaluated as a hole‐transporting layer (HTL) in perovskite solar cells (PSCs). The NiO1+δ devices are benchmarked against state‐of‐the‐art self‐assembled monolayers (SAM) ([2‐(3,6‐dimethoxy‐9H‐carbazol‐9‐yl)ethyl]phosphonic acid (also known as MeO2PACz)‐based PSCs. The best‐performing NiO1+δ PSC achieves an efficiency (η) of ≈16% without a passivation layer at the HTL interface and demonstrates better operational stability compared to the SAM device. The findings suggest that further optimization of GFS NiO1+δ devices can lead to higher‐performing and more stable PSCs. [ABSTRACT FROM AUTHOR]

In recent years, SnO2 quantum dots (QDs) have been widely used for preparing the electron‐transport layer within perovskite solar cells (PSCs). However, the fabricated devices exhibit an evident hysteresis unless interlayer materials are introduced to passivate or prevent the formation of trap states at the SnO2–perovskite interface. Herein, the use of the zwitterion 3‐(1‐pyridinio)‐1‐propanesulfonate (PPS) as additive inside the SnO2 QDs solution is proposed. The results highlight that the PPS plays a multifunctional role by accelerating the synthesis of the QDs, enhancing the electron transfer and passivating defects at the SnO2–perovskite interface. The resulting PSCs with SnO2 QDs incorporating PPS exhibit a remarkable reduction in hysteresis index (HI) compared to those prepared with thiourea or without any additives. This reduction in HI suggests that PPS serves as a cost‐effective alternative additive for SnO2 QDs preparation, eliminating the need for additional interlayers or expensive additives. [ABSTRACT FROM AUTHOR]