An Integrated Deposition and Passivation Strategy for Controlled Crystallization of 2D/3D Halide Perovskite Films.

This work introduces a simplified deposition procedure for multidimensional (2D/3D) perovskite thin films, integrating a phenethylammonium chloride (PEACl)-treatment into the antisolvent step when forming the 3D perovskite. This simultaneous deposition and passivation strategy reduces the number of synthesis steps while simultaneously stabilizing the halide perovskite film and improving the photovoltaic performance of resulting solar cell devices to 20.8%. Using a combination of multimodal in situ and additional ex situ characterizations, it is demonstrated that the introduction of PEACl during the perovskite film formation slows down the crystal growth process, which leads to a larger average grain size and narrower grain size distribution, thus reducing carrier recombination at grain boundaries and improving the device's performance and stability. The data suggests that during annealing of the wet film, the PEACl diffuses to the surface of the film, forming hydrophobic (quasi-)2D structures that protect the bulk of the perovskite film from humidity-induced degradation.

Coordination Chemistry as a Universal Strategy for a Controlled Perovskite Crystallization.

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.

Highly efficient p-i-n perovskite solar cells that endure temperature variations.

Daily temperature variations induce phase transitions and lattice strains in halide perovskites, challenging their stability in solar cells. We stabilized the perovskite black phase and improved solar cell performance using the ordered dipolar structure of ß-poly(1,1-difluoroethylene) to control perovskite film crystallization and energy alignment. We demonstrated p-i-n perovskite solar cells with a record power conversion efficiency of 24.6% over 18 square millimeters and 23.1% over 1 square centimeter, which retained 96 and 88% of the efficiency after 1000 hours of 1-sun maximum power point tracking at 25° and 75°C, respectively. Devices under rapid thermal cycling between -60° and +80°C showed no sign of fatigue, demonstrating the impact of the ordered dipolar structure on the operational stability of perovskite solar cells.

Lamination methods for the fabrication of perovskite and organic photovoltaics.

Perovskite solar cells (PSCs) have shown rapid progress in a decade of extensive research and development, aiming now towards commercialization. However, the development of more facile, reliable, and reproducible manufacturing techniques will be essential for industrial production. Many lamination methods have been initially designed for organic photovoltaics (OPVs), which are conceptually similar to PSCs. Lamination could provide a low-cost and adaptable technique for the roll-to-roll production of solar cells. This review presents an overview of lamination methods for the fabrication of PSCs and OPVs. The lamination of different electrodes consisting of various materials such as metal back contacts, photoactive layers, hole transport layers (HTLs), and electron transport layers (ETLs) is discussed. The efficiency and stability of the laminated devices are also presented. Finally, the challenges and opportunities of laminated solar cells are discussed.

Tin-based halide perovskite materials: properties and applications.

Organic-inorganic hybrid halide perovskite materials have attracted considerable research interest, especially for photovoltaics. In addition, their scope has been extended towards light-emitting devices, photodetectors, or detectors. However, the toxicity of lead (Pb) element in perovskite compositions limits their applications. Therefore, a tremendous research effort on replacing is underway. More specifically, tin-based perovskites have shown the highest potential for this purpose. However, many challenges remain before these materials reach the goals of stability, safety, and eventually commercial application. This perspective considers many aspects and the critical development possibilities of tin-based perovskites, including drawbacks and challenges based on their physical properties. Additionally, it provides insights for future device applications that go beyond solar cells. Finally, the existing challenges and opportunities in tin-based perovskites are discussed.

One-Step Thermal Gradient- and Antisolvent-Free Crystallization of All-Inorganic Perovskites for Highly Efficient and Thermally Stable Solar Cells.

All-inorganic perovskites have emerged as promising photovoltaic materials due to their superior thermal stability compared to their heat-sensitive hybrid organic-inorganic counterparts. In particular, CsPbI2 Br shows the highest potential for developing thermally-stable perovskite solar cells (PSCs) among all-inorganic compositions. However, controlling the crystallinity and morphology of all-inorganic compositions is a significant challenge. Here, a simple, thermal gradient- and antisolvent-free method is reported to control the crystallization of CsPbI2 Br films. Optical in situ characterization is used to investigate the dynamic film formation during spin-coating and annealing to understand and optimize the evolving film properties. This leads to high-quality perovskite films with micrometer-scale grain sizes with a noteworthy performance of 17% (≈16% stabilized), fill factor (FF) of 80.5%, and open-circuit voltage (VOC ) of 1.27 V. Moreover, excellent phase and thermal stability are demonstrated even after extreme thermal stressing at 300 °C.

Defect Passivation in Lead-Halide Perovskite Nanocrystals and Thin Films: Toward Efficient LEDs and Solar Cells.

Lead-halide perovskites (LHPs), in the form of both colloidal nanocrystals (NCs) and thin films, have emerged over the past decade as leading candidates for next-generation, efficient light-emitting diodes (LEDs) and solar cells. Owing to their high photoluminescence quantum yields (PLQYs), LHPs efficiently convert injected charge carriers into light and vice versa. However, despite the defect-tolerance of LHPs, defects at the surface of colloidal NCs and grain boundaries in thin films play a critical role in charge-carrier transport and nonradiative recombination, which lowers the PLQYs, device efficiency, and stability. Therefore, understanding the defects that play a key role in limiting performance, and developing effective passivation routes are critical for achieving advances in performance. This Review presents the current understanding of defects in halide perovskites and their influence on the optical and charge-carrier transport properties. Passivation strategies toward improving the efficiencies of perovskite-based LEDs and solar cells are also discussed.

Self-Assembled Monolayer of Wavelength-Scale Core-Shell Particles for Low-Loss Plasmonic and Broadband Light Trapping in Solar Cells.

Scattering particles constitute a key light trapping solution for thin film photovoltaics where either the particles are embedded in the light absorbing layer or a thick layer of them is used as a reflector. Here we introduce a monolayer of wavelength-scale core-shell silica@Ag particles as a novel light trapping strategy for thin film photovoltaics. These particles show hybrid photonic-plasmonic resonance modes that scatter light strongly and with small parasitic absorption losses in Ag (<1.5%). In addition, their scattering efficiency does not vary significantly with the refractive index of the surrounding medium. A monolayer of these particles is applied as the top-scattering layers in a dye-sensitized solar cells and it improves the short-circuit current density of a cell with 7 µm-thick dye-sensitized layer by 38%. Optical measurements of the scattering properties of these particles confirm that the strong scattering and low-parasitic absorption losses constitute the main reason for this efficient light trapping.