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Manipulation of grain boundaries in polycrystalline perovskite is an essential consideration for both the optoelectronic properties and environmental stability of solar cells as the solution-processing of perovskite films inevitably introduces many defects at grain boundaries. Though small molecule-based additives have proven to be effective defect passivating agents, their high volatility and diffusivity cannot render perovskite films robust enough against harsh environments. Here we suggest design rules for effective molecules by considering their molecular structure. From these, we introduce a strategy to form macromolecular intermediate phases using long chain polymers, which leads to the formation of a polymer-perovskite composite cross-linker. The cross-linker functions to bridge the perovskite grains, minimizing grain-to-grain electrical decoupling and yielding excellent environmental stability against moisture, light, and heat, which has not been attainable with small molecule defect passivating agents. Consequently, all photovoltaic parameters are significantly enhanced in the solar cells and the devices also show excellent stability. Defective grain boundaries of polycrystalline perovskite films are one of the major causes of the instability of the solar cell devices. Here Han et al. choose a polymer with proper molecular structure to crosslink the perovskite grains to greatly improve the device stability.

Hybrid heterostructures are essential for functional device systems. The advent of 2D materials has broadened the material set beyond conventional 3D material-based heterostructures. It has triggered the fundamental investigation and use in applications of new coupling phenomena between 3D bulk materials and 2D atomic layers that have unique van der Waals features. Here we review the state-of-the-art fabrication of 2D and 3D heterostructures, present a critical survey of unique phenomena arising from forming 3D/2D interfaces, and introduce their applications. We also discuss potential directions for research based on these new coupled architectures.Integrating 3D bulk materials with 2D layered materials can harness promising properties and unique functions. This Review discusses the progress in the fabrication, physical coupling and potential applications of 3D/2D hybrid heterostructures.

The ground-breaking demonstration of the electric field effect in graphene reported more than a decade ago prompted the strong push towards the commercialization of graphene as evidenced by a wealth of graphene research, patents and applications. Graphene flake production capability has reached thousands of tonnes per year, while continuous graphene sheets of tens of metres in length have become available. Various graphene technologies developed in laboratories have now transformed into commercial products, with the very first demonstrations in sports goods, automotive coatings, conductive inks and touch screens, to name a few. Although challenges related to quality control in graphene materials remain to be addressed, the advancement in the understandings of graphene will propel the commercial success of graphene as a compelling technology. This Review discusses the progress towards commercialization of graphene for the past decade and future perspectives.

Using adhesive tape to pull off monolayers of two-dimensional (2D) materials is now a well-established approach. However, the flakes tend to be micrometer scale, and the creation of multilayer stacks for device application can be challenging and time consuming. Shim et al. show that monolayers of a variety of 2D materials, including molybdenum disulfide and hexagonal boron nitride, can be cleaved from multilayers grown as 5-centimeter-diameter wafers. The multilayer is capped with a nickel layer, which can be used to pull off the entire grown stack. The bottom of the stack is again capped with nickel, and a second round of cleaving leaves the monolayer on the bottom nickel layer. The monolayers could be transferred to other surfaces, which allowed the authors to make field-effect transistors with high charge-carrier mobilities. Science , this issue p. 665 Nickel overlayers transfer stress and enable cleavage of two-dimensional materials as monolayers at the wafer scale. Although flakes of two-dimensional (2D) heterostructures at the micrometer scale can be formed with adhesive-tape exfoliation methods, isolation of 2D flakes into monolayers is extremely time consuming because it is a trial-and-error process. Controlling the number of 2D layers through direct growth also presents difficulty because of the high nucleation barrier on 2D materials. We demonstrate a layer-resolved 2D material splitting technique that permits high-throughput production of multiple monolayers of wafer-scale (5-centimeter diameter) 2D materials by splitting single stacks of thick 2D materials grown on a single wafer. Wafer-scale uniformity of hexagonal boron nitride, tungsten disulfide, tungsten diselenide, molybdenum disulfide, and molybdenum diselenide monolayers was verified by photoluminescence response and by substantial retention of electronic conductivity. We fabricated wafer-scale van der Waals heterostructures, including field-effect transistors, with single-atom thickness resolution.

Perovskite/CIGS tandem cellsTandem solar cells can boost efficiency by using more of the available solar spectrum. Han et al. fabricated a two-terminal tandem cell with an inorganicorganic hybrid perovskite top layer and a Cu(In,Ga)Se2 (CIGS) bottom layer. Control of the roughness of the CIGS surface and the use of a heavily doped organic hole transport layer were crucial to achieve a 22.4% power conversion efficiency. The unencapsulated tandem cells maintained almost 90% of their efficiency after 500 hours of operation under ambient conditions.Science, this issue p. 904The combination of hybrid perovskite and Cu(In,Ga)Se2 (CIGS) has the potential for realizing high-efficiency thin-film tandem solar cells because of the complementary tunable bandgaps and excellent photovoltaic properties of these materials. In tandem solar device architectures, the interconnecting layer plays a critical role in determining the overall cell performance, requiring both an effective electrical connection and high optical transparency. We used nanoscale interface engineering of the CIGS surface and a heavily doped poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) hole transport layer between the subcells that preserves open-circuit voltage and enhances both the fill factor and short-circuit current. A monolithic perovskite/CIGS tandem solar cell achieved a 22.43% efficiency, and unencapsulated devices under ambient conditions maintained 88% of their initial efficiency after 500 hours of aging under continuous 1-sun illumination.

Two-dimensional transition metal dichalcogenide nanoribbons are touted as the future extreme device downscaling for advanced logic and memory devices but remain a formidable synthetic challenge. Here, we demonstrate a ledge-directed epitaxy (LDE) of dense arrays of continuous, self-aligned, monolayer and single-crystalline MoS 2 nanoribbons on β-gallium ( iii ) oxide (β-Ga 2 O 3 ) (100) substrates. LDE MoS 2 nanoribbons have spatial uniformity over a long range and transport characteristics on par with those seen in exfoliated benchmarks. Prototype MoS 2 -nanoribbon-based field-effect transistors exhibit high on/off ratios of 10 8 and an averaged room temperature electron mobility of 65 cm 2  V −1  s −1 . The MoS 2 nanoribbons can be readily transferred to arbitrary substrates while the underlying β-Ga 2 O 3 can be reused after mechanical exfoliation. We further demonstrate LDE as a versatile epitaxy platform for the growth of p-type WSe 2 nanoribbons and lateral heterostructures made of p-WSe 2 and n-MoS 2 nanoribbons for futuristic electronics applications. Aligned arrays of single-crystalline monolayer TMD nanoribbons with high aspect ratios, as well as their lateral heterostructures, are realized, with the growth directed by the ledges on the β-Ga 2 O 3 substrate. This approach provides an epitaxy platform for advanced electronics applications of TMD nanoribbons.

The transparency of two-dimensional (2D) materials to intermolecular interactions of crystalline materials has been an unresolved topic. Here we report that remote atomic interaction through 2D materials is governed by the binding nature, that is, the polarity of atomic bonds, both in the underlying substrates and in 2D material interlayers. Although the potential field from covalent-bonded materials is screened by a monolayer of graphene, that from ionic-bonded materials is strong enough to penetrate through a few layers of graphene. Such field penetration is substantially attenuated by 2D hexagonal boron nitride, which itself has polarization in its atomic bonds. Based on the control of transparency, modulated by the nature of materials as well as interlayer thickness, various types of single-crystalline materials across the periodic table can be epitaxially grown on 2D material-coated substrates. The epitaxial films can subsequently be released as free-standing membranes, which provides unique opportunities for the heterointegration of arbitrary single-crystalline thin films in functional applications.

Although conventional homoepitaxy forms high-quality epitaxial layers1–5, the limited set of material systems for commercially available wafers restricts the range of materials that can be grown homoepitaxially. At the same time, conventional heteroepitaxy of lattice-mismatched systems produces dislocations above a critical strain energy to release the accumulated strain energy as the film thickness increases. The formation of dislocations, which severely degrade electronic/photonic device performances6–8, is fundamentally unavoidable in highly lattice-mismatched epitaxy9–11. Here, we introduce a unique mechanism of relaxing misfit strain in heteroepitaxial films that can enable effective lattice engineering. We have observed that heteroepitaxy on graphene-coated substrates allows for spontaneous relaxation of misfit strain owing to the slippery graphene surface while achieving single-crystalline films by reading the atomic potential from the substrate. This spontaneous relaxation technique could transform the monolithic integration of largely lattice-mismatched systems by covering a wide range of the misfit spectrum to enhance and broaden the functionality of semiconductor devices for advanced electronics and photonics.The spontaneous relaxation of misfit strain achieved on graphene-coated substrates enables the growth of heteroepitaxial single-crystalline films with reduced dislocation density.

The demand for improved electronic and optoelectronic devices has fuelled the development of epitaxial growth techniques for single-crystalline semiconductors. However, lattice and thermal expansion coefficient mismatch problems limit the options for growth and integration of high-efficiency electronic and photonic devices on dissimilar materials. Accordingly, advanced epitaxial growth and layer lift-off techniques have been developed to address issues relating to lattice mismatch. Here, we review epitaxial growth and layer-transfer techniques for monolithic integration of dissimilar single-crystalline materials for application in advanced electronic and photonic devices. We also examine emerging epitaxial growth techniques that involve two-dimensional materials as an epitaxial release layer and explore future integrated computing systems that could harness both advanced epitaxial growth and lift-off approaches. This Review Article examines the development of epitaxial growth and layer transfer techniques for monolithic integration of dissimilar single-crystalline materials for application in advanced electronic and photonic devices.

Although conventional p-type doping using small molecules on graphene decreases its sheet resistance ( R sh ), it increases after exposure to ambient conditions, and this problem has been considered as the biggest impediment to practical application of graphene electrodes. Here, we report an extremely stable graphene electrode doped with macromolecular acid (perfluorinated polymeric sulfonic acid (PFSA)) as a p-type dopant. The PFSA doping on graphene provides not only ultra-high ambient stability for a very long time (> 64 days) but also high chemical/thermal stability, which have been unattainable by doping with conventional small-molecules. PFSA doping also greatly increases the surface potential (~0.8 eV) of graphene, and reduces its R sh by ~56%, which is very important for practical applications. High-efficiency phosphorescent organic light-emitting diodes are fabricated with the PFSA-doped graphene anode (~98.5 cd A −1 without out-coupling structures). This work lays a solid platform for practical application of thermally-/chemically-/air-stable graphene electrodes in various optoelectronic devices. Chemical doping is a viable strategy to tune the electrical properties of pristine graphene, but suffers from stability issues. Here, the authors develop a macromolecular chemical doping approach that makes use of polymeric acid and provides high stability.