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.

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.

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.

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.