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1.
Adv Mater ; : e2402435, 2024 May 09.
Artigo em Inglês | MEDLINE | ID: mdl-38723286

RESUMO

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.

2.
ACS Nano ; 18(11): 7739-7768, 2024 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-38456396

RESUMO

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.

3.
ACS Nano ; 18(11): 8475-8483, 2024 Mar 19.
Artigo em Inglês | MEDLINE | ID: mdl-38456704

RESUMO

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.

5.
Nano Lett ; 24(6): 2118-2124, 2024 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-38305203

RESUMO

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.

6.
Adv Mater ; 36(2): e2304708, 2024 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-37452605

RESUMO

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.

7.
ACS Nano ; 17(24): 24423-24430, 2023 Dec 26.
Artigo em Inglês | MEDLINE | ID: mdl-38095315

RESUMO

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.

8.
Adv Mater ; 35(51): e2306850, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37688530

RESUMO

The ultrathin thickness of 2D layered materials affords the control of their properties through defects, surface modification, and electrostatic fields more efficiently compared with bulk architecture. In particular, patterning design, such as moiré superlattice patterns and spatially periodic dielectric structures, are demonstrated to possess the ability to precisely control the local atomic and electronic environment at large scale, thus providing extra degrees of freedom to realize tailored material properties and device functionality. Here, the scalable atomic-scale patterning in superionic cuprous telluride by using the bonding difference at nonequivalent copper sites is reported. Moreover, benefitting from the natural coupling of ordered and disordered sublattices, controllable piezoelectricity-like multilevel switching and bipolar switching with the designed crystal structure and electrical contact is realized, and their application in image enhancement is demonstrated. This work extends the known classes of patternable crystals and atomic switching devices, and ushers in a frontier for image processing with memristors.

9.
Adv Mater ; 35(42): e2304118, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37437137

RESUMO

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.

10.
Adv Mater ; : e2305044, 2023 Jul 24.
Artigo em Inglês | MEDLINE | ID: mdl-37486859

RESUMO

The emerging nonvolatile memory technologies based on ferroic materials are promising for producing high-speed, low-power, and high-density memory in the field of integrated circuits. Long-range ferroic orders observed in 2D materials have triggered extensive research interest in 2D magnets, 2D ferroelectrics, 2D multiferroics, and their device applications. Devices based on 2D ferroic materials and heterostructures with an atomically smooth interface and ultrathin thickness have exhibited impressive properties and significant potential for developing advanced nonvolatile memory. In this context, a systematic review of emergent 2D ferroic materials is conducted here, emphasizing their recent research on nonvolatile memory applications, with a view to proposing brighter prospects for 2D magnetic materials, 2D ferroelectric materials, 2D multiferroic materials, and their relevant devices.

11.
12.
Adv Mater ; 35(22): e2301668, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-37015006

RESUMO

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.

13.
Adv Mater ; 35(19): e2209346, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36862987

RESUMO

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.

14.
Nat Mater ; 22(6): 717-724, 2023 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-36959500

RESUMO

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.

15.
Adv Mater ; 35(18): e2211388, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36780341

RESUMO

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.

16.
Adv Mater ; 35(19): e2211701, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36807945

RESUMO

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.

17.
Sci Bull (Beijing) ; 67(16): 1659-1668, 2022 Aug 31.
Artigo em Inglês | MEDLINE | ID: mdl-36546045

RESUMO

Inspired by the great success of ultrathin two-dimensional (2D) layered crystals, more and more attention is being paid to preparing 2D nanostructures from non-layered materials. They can significantly enrich the 2D materials and 2D heterostructures family, extend their application prospects, and bring us distinct properties from their bulk counterparts due to the strong 2D confinement effect. However, the realization of 2D non-layered semiconductors with strong light-harvesting capability and the ability to construct high-performance 2D heterostructures is still a critical challenge. Herein, we successfully synthesized 2D PbSe semiconductors with a large lateral dimension and ultrathin thickness via van der Waals epitaxy. The fabricated 2D PbSe device exhibits good electrical conductivity and superior multi-wavelength photoresponse performance with high responsivity (∼103 A/W) and impressive detectivity (∼2 × 1011 Jones). Furthermore, we demonstrate that 2D PbSe nanosheets can serve as component units for constructing high-performance heterostructure devices. With our strategy, ultrahigh current on/off ratio (∼108) and rectification ratio (∼106), as well as high responsivity (∼3 × 103 A/W) and detectivity (∼7 × 1012 Jones), can be achieved in PbSe/MoS2 back-gated transistors. These results indicate that 2D PbSe nanosheets and their heterostructures have tremendous applications potential in electrical and optoelectronic devices.

18.
J Biol Chem ; 298(12): 102609, 2022 12.
Artigo em Inglês | MEDLINE | ID: mdl-36265583

RESUMO

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.


Assuntos
Heparina , Neoplasias , Humanos , Heparina/metabolismo , Epitopos/química , Glicosaminoglicanos/metabolismo , Sulfatos de Condroitina/genética , Sulfatos de Condroitina/metabolismo , Neoplasias/genética
19.
Nat Commun ; 13(1): 5241, 2022 Sep 06.
Artigo em Inglês | MEDLINE | ID: mdl-36068242

RESUMO

The discovery of magnetism in ultrathin crystals opens up opportunities to explore new physics and to develop next-generation spintronic devices. Nevertheless, two-dimensional magnetic semiconductors with Curie temperatures higher than room temperature have rarely been reported. Ferrites with strongly correlated d-orbital electrons may be alternative candidates offering two-dimensional high-temperature magnetic ordering. This prospect is, however, hindered by their inherent three-dimensional bonded nature. Here, we develop a confined-van der Waals epitaxial approach to synthesizing air-stable semiconducting cobalt ferrite nanosheets with thickness down to one unit cell using a facile chemical vapor deposition process. The hard magnetic behavior and magnetic domain evolution are demonstrated by means of vibrating sample magnetometry, magnetic force microscopy and magneto-optical Kerr effect measurements, which shows high Curie temperature above 390 K and strong dimensionality effect. The addition of room-temperature magnetic semiconductors to two-dimensional material family provides possibilities for numerous novel applications in computing, sensing and information storage.

20.
Adv Mater ; 34(9): e2108313, 2022 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-34989444

RESUMO

Copper chalcogenides represent a class of materials with unique crystal structures, high electrical conductivity, and earth abundance, and are recognized as promising candidates for next-generation green electronics. However, their 2D structures and the corresponding electronic properties have rarely been touched. Herein, a series of ultrathin copper chalcogenide nanosheets with thicknesses down to two unit cells are successfully synthesized, including layered Cu2 Te, as well as nonlayered CuSe and Cu9 S5 , via van der Waals epitaxy, and their nonvolatile memristive behavior is investigated for the first time. Benefiting from the highly active Cu ions with low migration barriers, the memristors based on ultrathin 2D copper chalcogenide crystals exhibit relatively small switching voltage (≈0.4 V), fast switching speed, high switching uniformity, and wide operating temperature range (from 80 to 420 K), as well as stable retention and good cyclic endurance. These results demonstrate their tangible applications in future low-power, cryogenic, and high temperature harsh electronics.

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