The recent rapid development in perovskite solar cells (PSCs) has led to significant research interest due to their notable photovoltaic performance, currently exceeding 25% power conversion efficiency for small-area PSCs. The materials used to fabricate PSCs dominate the current photovoltaic market, especially with the rapid increase in efficiency and performance. The present work reviews recent developments in PSCs’ preparation and fabrication methods, the associated advantages and disadvantages, and methods for improving the efficiency of large-area perovskite films for commercial application. The work is structured in three parts. First is a brief overview of large-area PSCs, followed by a discussion of the preparation methods and methods to improve PSC efficiency, quality, and stability. Envisioned future perspectives on the synthesis and commercialization of large-area PSCs are discussed last. Most of the growth in commercial PSC applications is likely to be in building integrated photovoltaics and electric vehicle battery charging solutions. This review concludes that blade coating, slot-die coating, and ink-jet printing carry the highest potential for the scalable manufacture of large-area PSCs with moderate-to-high PCEs. More research and development are key to improving PSC stability and, in the long-term, closing the chasm in lifespan between PSCs and conventional photovoltaic cells.

When layered transition-metal dichalcogenides (TMDs) are scaled down from a three-to a 2D geometry, electronic and structural transitions occur, leading to the emergence of properties not usually found in the bulk. Here, we report a systematic Raman study of exfoliated semi-metallic WTe 2 flakes with thickness ranging from few layers down to a single layer. A dramatic change in the Raman spectra occurs between the monolayer and few-layer WTe 2 as a vibrational mode centered at ~86.9 cm −1 in the monolayer splits into two active modes at 82.9 and 89.6 cm −1 in the bilayer. Davydov splitting of these two modes is found in the bilayer, as further evidenced by polarized Raman measurements. Strong angular dependence of Raman modes on the WTe 2 film thickness reflects that the existence of directional interlayer interaction, rather than isotropic van der Waals (vdw) coupling, is playing an essential role affecting the phonon modes, especially in anisotropic 2D WTe 2 material. Therefore, the strong evolution of Raman modes with thickness and polarization direction, can not only be a reliable fingerprint for the determination of the thickness and the crystallographic orientation, but can also be an ideal probe for such strong and directional interlayer interaction.

It is known that an isolated single‐molecule magnet tends to become super‐paramagnetic even at an ultralow temperature of a few Kelvin due to the low spin switching barrier. Herein, single‐molecule ferroelectrics/multiferroics is proposed, as the ultimate size limit of memory, such that every molecule can store 1 bit data. The primary strategy is to identify polar molecules that possess bistable states, moderate switching barriers, and polarizations fixed along the vertical direction for high‐density perpendicular recording. First‐principles computation shows that several selected magnetic metal porphyrin molecules possess buckled structures with switchable vertical polarizations that are robust at ambient conditions. When intercalated within a bilayer of 2D materials such as bilayer MoS2 or CrI3, the magnetization can alter the spin distribution or can be even switched by 180° upon ferroelectric switching, rendering efficient electric writing and magnetic reading. It is found that the upper limit of areal storage density can be enhanced by four orders of magnitude, from the previous super‐paramagnetic limit of ≈40 to ≈106 GB in.−2, on the basis of the design of cross‐point multiferroic tunneling junction array and multiferroic hard drive.

Multiferroics are rare in nature due to the mutual exclusive origins of magnetism and ferroelectricity. The simultaneous coexistence of robust magnetism/ferroelectricity and strong magnetoelectric coupling in single multiferroics is hitherto unreported, which may also be attributed to their potential conflictions. In this paper, we show the first-principles evidence of such desired coexistence in ultrathin-layer CuCrS2 and CuCrSe2. The vertical ferroelectricity is neither induced by an empty d shell nor spin-driven, giving rise to an alternative possibility of resolving those intrinsic exclusions and contradictions. Compared with their bulk phases, the ferromagnetism in the thin-layer structures (two–six layers) can be greatly stabilized due to the enhanced carrier density and orbital shifting by vertical polarization, and the Curie temperatures of both ferromagnetism and ferroelectricity can be above room temperature. Moreover, a considerable net magnetization can be reversed upon ferroelectric switching, where the change in spin-resolved band structure also renders efficient ‘magnetic reading + electrical writing’. The thickness-different layers may even exhibit diversified types of magnetoelectric coupling, which both enriches the physics of multiferroics and facilitates their practical applications.

Two-dimensional (2D) ferroelectrics have attracted intensive attention. However, the 2D ferroelectrics remain rare, and especially few of them represent high ferroelectric transition temperature (T C), which is important for the usability of ferroelectrics. Herein, CuCrS2 nanoflakes are synthesized by salt-assisted chemical vapor deposition and exhibit switchable ferroelectric polarization even when the thickness is downscaled to 6 nm. On the contrary, a CuCrS2 nanoflake shows a T C as high as ∼700 K, which can be attributed to the robust tetrahedral bonding configurations of Cu cations. Such robustness can be further clarified by a theoretically predicted high order–disorder transition barrier and structure evolution from 600 to 800 K. Additionally, the interlocked out-of-plane (OOP) and in-plane (IP) ferroelectric domains are observed and two kinds of devices based on OOP and IP polarizations are demonstrated.

Light-modulated lead-free perovskites-based memristors, combining photoresponse and memory, are promising as multifunctional devices. In this work, lead-free double perovskite Cs2AgBiBr6 films with dense surfaces and uniform grains were prepared by the low-temperature sol-gel method on indium tin oxide (ITO) substrates. A memory device based on a lead-free double perovskite Cs2AgBiBr6 film, Pt/Cs2AgBiBr6/ITO/glass, presents obvious bipolar resistive switching behavior. The ROFF/RON ratio under 445 nm wavelength light illumination is ~100 times greater than that in darkness. A long retention capability (>2400 s) and cycle-to-cycle consistency (>500 times) were observed in this device under light illumination. The resistive switching behavior is primarily attributed to the trap-controlled space-charge-limited current mechanism caused by bromine vacancies in the Cs2AgBiBr6 medium layer. Light modulates resistive states by regulating the condition of photo-generated carriers and changing the Schottky-like barrier of the Pt/Cs2AgBiBr6 interface under bias voltage sweeping.

According to the model of sliding ferroelectricity we proposed in 2017, a type of vertical polarizations switchable via interlayer sliding may exist in a series of two-dimensional van der Waals...

Lead-free, bismuth-based perovskite solar cells (PSCs) are promising, non-toxic, and stable alternatives to lead-based PSCs, which are environmentally harmful and highly unstable under deprived air conditions. However, bismuth-based PSCs still suffer from low-power-conversion efficiency (PCE) due to their large bandgap and poor film morphology. Their poor film-forming ability is the greatest obstacle to Cs₃Bi₂I₉ progress in thin-film solar cell technology. This study synthesizes novel, lead-free perovskites with a small bandgap, excellent stability, and highly improved photovoltaic performance by integrating different amounts of potassium iodide (KI) into a perovskite precursor solution. KI incorporation improves the crystallinity of the perovskite, increases the grain size, and decreases the potential contact distribution, which is demonstrated by X-ray diffraction, electronic scanning microscopy, atomic force microscopy, and ultraviolet-visible spectroscopy. The Cs₃Bi₂I₉ PSC device with 2 vol. % incorporation of KI shows the highest PCE of 2.81% and Voc of 1.01 V as far as all the Bi-based cells fabricated for this study are concerned. The study demonstrates that incorporating KI in the Cs₃Bi₂I₉ perovskite layer highly stabilizes the resultant PSC device against humidity to the extent that it maintains 98% of the initial PCE after 90 days, which is suitable for solar cell applications. The devices also demonstrate greater resistance to airborne contaminants and high temperatures without encapsulation, opening up new possibilities for lead-free Cs₃Bi₂I₉ PSCs in future commercialization.