van der Waals Epitaxial Growth of One-Unit-Cell-Thick Ferroelectric CuCrS2 Nanosheets.

Ferroelectric two-dimensional (2D) materials with a high transition temperature are highly desirable for new physics and next-generation memory electronics. However, the long-range polar order of ferroelectrics will barely persist when the thickness reaches the nanoscale. In this work, we synthesized 2D CuCrS2 nanosheets with thicknesses down to one unit cell via van der Waals epitaxy in a chemical vapor deposition system. A combination of transmission electron microscopy, second-harmonic generation, and Raman spectroscopy measurements confirms the R3m space group and noncentrosymmetric structure. Switchable ferroelectric domains and obvious ferroelectric hysteresis loops were created and visualized by piezoresponse force microscopy. Theoretical calculation helps us understand the mechanism of ferroelectric switching in CuCrS2 nanosheets. Finally, we fabricated a ferroelectric memory device that achieves an on/off ratio of ∼102 and remains stable after 2000 s, indicating its applicability in novel nanoelectronics. Overall, 2D CuCrS2 nanosheets exhibit excellent ferroelectric properties at the nanoscale, showing great promise for next-generation devices.

Growth of single-crystal black phosphorus and its alloy films through sustained feedstock release.

Black phosphorus (BP), a fascinating semiconductor with high mobility and a tunable direct bandgap, has emerged as a candidate beyond traditional silicon-based devices for next-generation electronics and optoelectronics. The ability to grow large-scale, high-quality BP films is a prerequisite for scalable integrated applications but has thus far remained a challenge due to unmanageable nucleation events. Here we develop a sustained feedstock release strategy to achieve subcentimetre-size single-crystal BP films by facilitating the lateral growth mode under a low nucleation rate. The as-grown single-crystal BP films exhibit high crystal quality, which brings excellent field-effect electrical properties and observation of pronounced Shubnikov-de Haas oscillations, with high mobilities up to ~6,500 cm2 V-1 s-1 at low temperatures. We further extend this approach to the growth of single-crystal BP alloy films, which broaden the infrared emission regime of BP from 3.7 µm to 6.9 µm at room temperature. This work will greatly facilitate the development of high-performance electronics and optoelectronics based on BP family materials.

A mutated glycosaminoglycan-binding domain functions as a novel probe to selectively target heparin-like epitopes on tumor cells.

The high heterogeneity and mutation rate of cancer cells often lead to the failure of targeted therapy, and therefore, new targets for multitarget therapy of tumors are urgently needed. Aberrantly expressed glycosaminoglycans (GAGs) have been shown to be involved in tumorigenesis and are promising new targets. Recently, the GAG-binding domain rVAR2 of the Plasmodium falciparum VAR2CSA protein was identified as a probe targeting cancer-associated chondroitin sulfate A-like epitopes. In this study, we found that rVAR2 could also bind to heparin (Hep) and chondroitin sulfate E. Therefore, we used rVAR2 as a model to establish a method based on random mutagenesis of the GAG-binding protein and phage display to identify and optimize probes targeting tumor GAGs. We identified a new probe, VAR2HP, which selectively recognized Hep by interacting with unique epitopes consisting of a decasaccharide structure that contains at least three HexA2S(1-4)GlcNS6S disaccharides. Moreover, we found that these Hep-like epitopes were overexpressed in various cancer cells. Most importantly, our in vivo experiments showed that VAR2HP had good biocompatibility and preferentially localizes to tumors, which indicates that VAR2HP has great application potential in tumor diagnosis and targeted therapy. In conclusion, this study provides a strategy for the discovery of novel tumor-associated GAG epitopes and their specific probes.

Two-Dimensional Unipolar Memristors with Logic and Memory Functions.

Two-dimensional materials have been widely used in electronics due to their electrical properties that are not accessible in traditional materials. Here, we present the first demonstration of logic functions of unipolar memristors made of functionalized HfSe2-xOx flakes and memtransistors made of MoS2/graphene/HfSe2-xOx van der Waals heterostructures. The two-terminal memristors exhibit stable unipolar switching behavior with high switching ratio (>106), high operating temperature (106 °C), long-term endurance (>104 s), and multibit data storage and can operate as memory latches and logic gates. Benefiting from these superior memristive properties, the three-terminal heterostructure memtransistors show wide tunability in electrical switching behaviors, which can simultaneously implement logic operation and data storage. Finally, we investigate their application prospect in logical units with memory capability, such as D-type flip-flop. These results demonstrate the potential of two-dimensional materials for resistive switching applications and open up an avenue for future in-memory computing.

Tunable Room-Temperature Ferromagnetism in Two-Dimensional Cr2Te3.

The manipulation of magnetism provides a unique opportunity for the development of data storage and spintronic applications. Until now, electrical control, pressure tuning, stacking structure dependence, and nanoscale engineering have been realized. However, as the dimensions are decreased, the decrease of the ferromagnetism phase transition temperature (Tc) is a universal trend in ferromagnets. Here, we make a breakthrough to realize the synthesis of 1 and 2 unit cell (UC) Cr2Te3 and discover a room-temperature ferromagnetism in two-dimensional Cr2Te3. The newly observed Tc increases strongly from 160 K in the thick flake (40.3 nm) to 280 K in 6 UC Cr2Te3 (7.1 nm). The magnetization and anomalous Hall effect measurements provided unambiguous evidence for the existence of spontaneous magnetization at room temperature. The theoretical model revealed that the reconstruction of Cr2Te3 could result in anomalous thickness-dependent Tc. This dimension tuning method opens up a new avenue for manipulation of ferromagnetism.

Sub-millimeter-Scale Growth of One-Unit-Cell-Thick Ferrimagnetic Cr2S3 Nanosheets.

Two-dimensional (2D) magnetic materials provide an ideal platform for the application in spintronic devices due to their unique spin states in nanometer scale. However, recent research on the exfoliated monolayer magnetic materials suffers from the instability in ambient atmosphere, which needs extraordinary protection. Hence the controllable synthesis of 2D magnetic materials with good quality and stability should be addressed. Here we report for the first time the van der Waals (vdW) epitaxial growth of one-unit-cell-thick air-stable ferrimagnet Cr2S3 semiconductor via a facile chemical vapor deposition method. Single crystal Cr2S3 with the domain size reaching to 200 µm is achieved. Most importantly, we observe the as grown Cr2S3 with a Néel temperature ( TN) of up to 120 K and a maximum saturation magnetic momentum of up to 65 µemu. As the temperature decreases, the samples show a transition from soft magnet to hard magnet with the highest coercivity of 1000 Oe. The one-unit-cell-thick Cr2S3 devices show a p-type transfer behavior with an on/off ratio over 103. Our work highlights Cr2S3 monolayer as an ideal magnetic semiconductor for 2D spintronic devices. The vdW epitaxy of nonlayered magnets introduces a new route for realizing magnetism in 2D limit and provides more application potential in the 2D spintronics.

2D library beyond graphene and transition metal dichalcogenides: a focus on photodetection.

Two-dimensional layered materials (2DLMs) have attracted a tremendous amount of attention as photodetectors due to their fascinating features, including high potentials in new-generation electronic devices, wide coverage of bandgaps, ability to construct van der Waals heterostructures, extraordinary light-mass interaction, strong mechanical flexibility, and the capability of enabling synthesis of 2D nonlayered materials. Until now, most attention has been focused on the well-known graphene and transition metal dichalcogenides (TMDs). However, a growing number of functional materials (more than 5619) with novel optoelectronic and electronic properties are being re-discovered, thereby widening the horizon of 2D libraries. In addition to showing common features of 2DLMs, these new 2D members may bring new opportunities to their well-known analogues, like wider bandgap coverage, direct bandgaps independence with thickness, higher mechanical flexibility, and new photoresponse phenomena. The impressive results communicated so far testify that they have shown high potentials with photodetections covering THz, IR, visible, and UV ranges with comparable or even higher performances than well-known TMDs. Here, we give a comprehensive review on the state-of-the-art photodetections of two-dimensional materials beyond graphene and TMDs. The review is organized as follows: fundamentals of photoresponse first are discussed, followed by detailed photodetections of new 2D members including both layered and non-layered ones. After that, photodiodes and hybrid structures based on these new 2D materials are summarized. Then, the integration of these 2D materials with flexible substrates is reviewed. Finally, we conclude with the current research status of this area and offer our perspectives on future developments. We hope that, through reading this manuscript, readers will quickly have a comprehensive view on this research area.

Sub-10 nm Nanopattern Architecture for 2D Material Field-Effect Transistors.

Two-dimensional materials (2DMs) are competitive candidates in replacing or supplementing conventional semiconductors owing to their atomically uniform thickness. However, current conventional micro/nanofabrication technologies realize hardly ultrashort channel and integration, especially for sub-10 nm. Meanwhile, experimental device performance associated with the scaling of dimension needs to be investigated, due to the short channel effects. Here, we show a novel and universal technological method to fabricate sub-10 nm gaps with sharp edges and steep sidewalls. The realization of sub-10 nm gaps derives from a corrosion crack along the cleavage plane of Bi2O3. By this method, ultrathin body field-effect transistors (FETs), consisting of 8.2 nm channel length, 6 nm high-k dielectric, and 0.7 nm monolayer MoS2, exhibit no obvious short channel effects. The corresponding current on/off ratio and subthreshold swing reaches to 106 and 140 mV/dec, respectively. Moreover, integrated circuits with sub-10 nm channel are capable of operating as digital inverters with high voltage gain. The results suggest our technological method can be used to fabricate the ultrashort channel nanopatterns, build the experimental groundwork for 2DMs FETs with sub-10 nm channel length and 2DMs integrated circuits, and offer new potential opportunities for large-scale device constructions and applications.

Progress on Electronic and Optoelectronic Devices of 2D Layered Semiconducting Materials.

2D layered semiconducting materials (2DLSMs) represent the thinnest semiconductors, holding many novel properties, such as the absence of surface dangling bonds, sizable band gaps, high flexibility, and ability of artificial assembly. With the prospect of bringing revolutionary opportunities for electronic and optoelectronic applications, 2DLSMs have prospered over the past twelve years. From materials preparation and property exploration to device applications, 2DLSMs have been extensively investigated and have achieved great progress. However, there are still great challenges for high-performance devices. In this review, we provide a brief overview on the recent breakthroughs in device optimization based on 2DLSMs, particularly focussing on three aspects: device configurations, basic properties of channel materials, and heterostructures. The effects from device configurations, i.e., electrical contacts, dielectric layers, channel length, and substrates, are discussed. After that, the affect of the basic properties of 2DLSMs on device performance is summarized, including crystal defects, crystal symmetry, doping, and thickness. Finally, we focus on heterostructures based on 2DLSMs. Through this review, we try to provide a guide to improve electronic and optoelectronic devices of 2DLSMs for achieving practical device applications in the future.

Two-Dimensional Oxide Crystals for Device Applications: Challenges and Opportunities.

Atomically thin two-dimensional (2D) oxide crystals have garnered considerable attention because of their remarkable physical properties and potential for versatile applications. In recent years, significant advancements have been made in the design, preparation, and application of ultrathin 2D oxides, providing many opportunities for new-generation advanced technologies. This review focuses on the controllable preparation of 2D oxide crystals and their applications in electronic and optoelectronic devices. Based on their bonding nature, the various types of 2D oxide crystals are first summarized, including both layered and nonlayered crystals, as well as their current top-down and bottom-up synthetic approaches. Subsequently, in terms of the unique physical and electrical properties of 2D oxides, recent advances in device applications are emphasized, including photodetectors, field-effect transistors, dielectric layers, magnetic and ferroelectric devices, memories, and gas sensors. Finally, conclusions and future prospects of 2D oxide crystals are presented. It is hoped that this review will provide comprehensive and insightful guidance for the development of 2D oxide crystals and their device applications.

Van der Waals Epitaxial Growth of Ultrathin Indium Antimonide on Arbitrary Substrates through Low-Thermal Budget.

III-V semiconductors possess high mobility, high frequency response, and detection sensitivity, making them potentially attractive for beyond-silicon electronics applications. However, the traditional heteroepitaxy of III-V semiconductors is impeded by a significant lattice mismatch and the necessity for extreme vacuum and high temperature conditions, thereby impeding their in situ compatibility with flexible substrates and silicon-based circuits. In this study, a novel approach is presented for fabricating ultrathin InSb single-crystal nanosheets on arbitrary substrates with a thickness as thin as 2.4 nm using low-thermal-budget van der Waals (vdW) epitaxy through chemical vapor deposition (CVD). In particular, in situ growth has been successfully achieved on both silicon-based substrates and flexible polyimide (PI) substrates. Notably, the growth temperature required for InSb nanosheets (240 °C) is significantly lower than that employed in back-end-of-line processes (400 °C). The field effect transistor devices based on fabricated ultrathin InSb nanosheets exhibit ultra-high on-off ratio exceeding 108 and demonstrate minimal gate leakage currents. Furthermore, these ultrathin InSb nanosheets display p-type characteristics with hole mobilities reaching up to 203 cm2 V-1 s-1 at room temperatures. This study paves the way for achieving heterogeneous integration of III-V semiconductors and facilitating their application in flexible electronics.

Two-Dimensional Semiconductors and Transistors for Future Integrated Circuits.

Silicon transistors are approaching their physical limit, calling for the emergence of a technological revolution. As the acknowledged ultimate version of transistor channels, 2D semiconductors are of interest for the development of post-Moore electronics due to their useful properties and all-in-one potentials. Here, the promise and current status of 2D semiconductors and transistors are reviewed, from materials and devices to integrated applications. First, we outline the evolution and challenges of silicon-based integrated circuits, followed by a detailed discussion on the properties and preparation strategies of 2D semiconductors and van der Waals heterostructures. Subsequently, the significant progress of 2D transistors, including device optimization, large-scale integration, and unconventional devices, are presented. We also examine 2D semiconductors for advanced heterogeneous and multifunctional integration beyond CMOS. Finally, the key technical challenges and potential strategies for 2D transistors and integrated circuits are also discussed. We envision that the field of 2D semiconductors and transistors could yield substantial progress in the upcoming years and hope this review will trigger the interest of scientists planning their next experiment.

Revealing Enhanced Optical Nonlinearity and Robust Ferromagnetism in Atomically Sharp Stacking Binary-Ternary Magnetic Heterostructures.

Two-dimensional (2D) materials provide a versatile platform for the integration of diverse crystals, enabling the formation of heterostructures with intriguing functionalities. Coherently growing 2D heterostructures are highly desirable for property manipulation due to their strong interfacial interaction. In this work, we propose a general synthesis approach and provide insight into well-designed 2D binary-ternary magnetic heterostructures. Atomically sharp interfaces were achieved in typical lateral and vertical Cr1+mSe2(001)/CuCr2Se4(111) heterostructures owing to their similar lattice arrangement, with the observation of a significant enhancement of optical second-harmonic generation. Further magnetism measurements revealed a Curie temperature up to 360 K and thickness- and temperature-dependent magnetism in this heterostructure. Additionally, we synthesized three analogous 2D magnetic heterostructures in Fe-Cr-S, Co-Cr-S, and Cu-Cr-S systems, demonstrating the ubiquitous nature of the coherent heteroepitaxy. Our work involves the development of an innovative platform for investigating the underlying physics and potential applications of 2D binary-ternary heterostructures as well as the fabrication of associated functional devices.

Spontaneous Skyrmion Bubbles in an Iron-Silicon Alloy with Uniaxial Magnetic Anisotropy.

The magnetic skyrmions exhibit intriguing topological behaviors, holding promise for future applications in the realm of spintronic devices. Despite recent advancements, achieving spontaneous magnetic skyrmions and topological transitions in magnets featuring uniaxial magnetic anisotropy, particularly at elevated temperatures (>100 K), remains a challenging endeavor. Here, single-crystal Fe5Si3 nanorods with the central symmetry and uniaxial magnetic anisotropy were successfully synthesized on a mica substrate through chemical vapor deposition, which exhibit a high Curie temperature (TC) of about 372 K. The real-time observation, facilitated by Lorentz transmission electron microscopy, revealed the spontaneous formation of magnetic skyrmions and evolution of domains in focused ion beam-prepared Fe5Si3 thin foils. Moreover, Fe5Si3 device transport measurements expose notable magnetoresistance (MR) effects, enabling the interchange between positive and negative MR across specific temperature settings. These results offer various potential avenues for exploring diverse topological spin textures and their formation mechanisms, indicating inventive applications for iron-silicon alloy in the realm of spintronics.

Tuning 2D Magnetism in Cobalt Monoxide Nanosheets Via In Situ Nickel-Doping.

Element doping has become an effective strategy to engineer the magnetic properties of two-dimensional (2D) materials and is widely explored in van der Waals layered transition metal dichalcogenides. However, the high-concentration substitution doping of 2D nonlayered metal oxides, which can preserve the original crystal texture and guarantee the homogeneity of doping distribution, is still a critical challenge due to the isotropic bonding of closed-packed structures. In this work, the synthesis of high-quality 2D nonlayered nickel-doped cobalt monoxide nanosheets via in situ atmospheric pressure chemical vapor deposition method is reported. High-resolution transmission electron microscopy confirmed that nickel atoms are doped at the intrinsic cobalt atom sites. The nickel doping concentration is stable at ≈15%, superior to most magnetic dopants doping in 2D materials and metal oxides. Magnetic measurements showed that pristine cobalt monoxide is nonferromagnetic, whereas nickel-doped cobalt monoxide exhibits robust ferromagnetic behavior with a Curie temperature of ≈180 K. Density functional theory calculations reveal that nickel atoms can improve the internal ferromagnetic correlation, giving rise to significant ferromagnetic performance of cobalt monoxide nanosheets. These results provide a valuable case for tuning the competing correlated states and magnetic ordering by substitution doping in 2D nonlayered oxide semiconductors.

Heteroepitaxy of 2D CuCr2 Te4 with Robust Room-temperature Ferromagnetism.

Magnetic materials in 2D have attracted widespread attention for their intriguing magnetic properties. 2D magnetic heterostructures can provide unprecedented opportunities for exploring fundamental physics and novel spintronic devices. Here, the heteroepitaxial growth of ferromagnetic CuCr2 Te4 nanosheets is reported on Cr2 Te3 and mica by chemical vapor deposition. Magneto-optical Kerr effect measurements reveal the thickness-dependent ferromagnetism of CuCr2 Te4 nanosheets on mica, where a decrease of Curie temperature (TC ) from 320 to 260 K and an enhancement of perpendicular magnetic anisotropy with reducing thickness are observed. Moreover, lattice-matched heteroepitaxial ultrathin CuCr2 Te4 on Cr2 Te3 exhibits an enhanced robust ferromagnetism with TC up to 340 K due to the interfacial charge transfer. Stripe-type magnetic domains and single magnetic domain are discovered in this heterostructure with different thicknesses. The work provides a way to construct robust room-temperature 2D magnetic heterostructures for functional spintronic devices.

Cutting-Edge Research in Nanoscience and Nanotechnology: Celebrating the 130th Anniversary of Wuhan University.

Thanks to the fast-paced progress of microscopic theories and nanotechnologies, a tremendous world of fundamental science and applications has opened up at the nanoscale. Ranging from quantum physics to chemical and biological mechanisms and from device functionality to materials engineering, nanoresearch has become an essential part of various fields. As one of the top universities in China, Wuhan University (WHU) aims to promote cutting-edge nanoresearch in multiple disciplines by leveraging comprehensive academic programs established throughout 130 years of history. As visible in prestigious scientific journals such as ACS Nano, WHU has made impactful advancements in various frontiers, including nanophotonics, functional nanomaterials and devices, biomedical nanomaterials, nanochemistry, and environmental science. In light of these contributions, WHU will be committed to serving talents and scientists wholeheartedly, fully supporting international collaborations and continuously driving innovative research.

Phase Engineering of 2D Spinel-Type Manganese Oxides.

2D magnetic materials have been of interest due to their unique long-range magnetic ordering in the low-dimensional regime and potential applications in spintronics. Currently, most studies are focused on strippable van der Waals magnetic materials with layered structures, which typically suffer from a poor stability and scarce species. Spinel oxides have a good environmental stability and rich magnetic properties. However, the isotropic bonding and close-packed nonlayered crystal structure make their 2D growth challenging, let alone the phase engineering. Herein, a phase-controllable synthesis of 2D single-crystalline spinel-type oxides is reported. Using the van der Waals epitaxy strategy, the thicknesses of the obtained tetragonal and hexagonal manganese oxide (Mn3 O4 ) nanosheets can be tuned down to 7.1 nm and one unit cell (0.7 nm), respectively. The magnetic properties of these two phases are evaluated using vibrating-sample magnetometry and first-principle calculations. Both structures exhibit a Curie temperature of 48 K. Owing to its ultrathin geometry, the Mn3 O4 nanosheet exhibits a superior ultraviolet detection performance with an ultralow noise power density of 0.126 pA Hz-1/2 . This study broadens the range of 2D magnetic semiconductors and highlights their potential applications in future information devices.

Van der Waals Epitaxy Growth of 2D Single-Element Room-Temperature Ferromagnet.

2D single-element materials, which are pure and intrinsically homogeneous on the nanometer scale, can cut the time-consuming material-optimization process and circumvent the impure phase, bringing about opportunities to explore new physics and applications. Herein, for the first time, the synthesis of ultrathin cobalt single-crystalline nanosheets with a sub-millimeter scale via van der Waals epitaxy is demonstrated. The thickness can be as low as ≈6 nm. Theoretical calculations reveal their intrinsic ferromagnetic nature and epitaxial mechanism: that is, the synergistic effect between van der Waals interactions and surface energy minimization dominates the growth process. Cobalt nanosheets exhibit ultrahigh blocking temperatures above 710 K and in-plane magnetic anisotropy. Electrical transport measurements further reveal that cobalt nanosheets have significant magnetoresistance (MR) effect, and can realize a unique coexistence of positive MR and negative MR under different magnetic field configurations, which can be attributed to the competition and cooperation effect among ferromagnetic interaction, orbital scattering, and electronic correlation. These results provide a valuable case for synthesizing 2D elementary metal crystals with pure phase and room-temperature ferromagnetism and pave the way for investigating new physics and related applications in spintronics.

Room-Temperature Intrinsic Ferromagnetic Chromium Tellurium Compounds with Thickness-Tunable Magnetic Texture.

2D ferromagnetic chromium tellurides exhibit intriguing spin configurations and high-temperature intrinsic ferromagnetism, providing unprecedented opportunities to explore the fundamental spin physics and build spintronic devices. Here, a generic van der Waals epitaxial approach is developed to synthesize the 2D ternary chromium tellurium compounds with thicknesses down to mono-, bi-, tri-, and few-unit cells (UC). The Mn0.14 Cr0.86 Te evolves from intrinsic ferromagnetic behavior in bi-UC, tri-UC, and few-UC to temperature-induced ferrimagnetic behavior as the thickness increases, resulting in a sign reversal of the anomalous Hall resistance. Temperature- and thickness-tunable labyrinthine-domain ferromagnetic behaviors are derived from the dipolar interactions in Fe0.26 Cr0.74 Te and Co0.40 Cr0.60 Te. Furthermore, the dipolar-interaction-induced stripe domain and field-induced domain wall (DW) motion velocity are studied, and multibit data storage is realized through an abundant DW state. The magnetic storage can function in neuromorphic computing tasks, and the pattern recognition accuracy can reach up to 97.93%, which is similar to the recognition accuracy of ideal software-based training (98.28%). Room-temperature ferromagnetic chromium tellurium compounds with intriguing spin configurations can significantly promote the exploration of the processing, sensing, and storage based on 2D magnetic systems.