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1.
Nature ; 632(8026): 782-787, 2024 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-39143208

RESUMO

Hot-carrier transistors are a class of devices that leverage the excess kinetic energy of carriers. Unlike regular transistors, which rely on steady-state carrier transport, hot-carrier transistors modulate carriers to high-energy states, resulting in enhanced device speed and functionality. These characteristics are essential for applications that demand rapid switching and high-frequency operations, such as advanced telecommunications and cutting-edge computing technologies1-5. However, the traditional mechanisms of hot-carrier generation are either carrier injection6-11 or acceleration12,13, which limit device performance in terms of power consumption and negative differential resistance14-17. Mixed-dimensional devices, which combine bulk and low-dimensional materials, can offer different mechanisms for hot-carrier generation by leveraging the diverse potential barriers formed by energy-band combinations18-21. Here we report a hot-emitter transistor based on double mixed-dimensional graphene/germanium Schottky junctions that uses stimulated emission of heated carriers to achieve a subthreshold swing lower than 1 millivolt per decade beyond the Boltzmann limit and a negative differential resistance with a peak-to-valley current ratio greater than 100 at room temperature. Multi-valued logic with a high inverter gain and reconfigurable logic states are further demonstrated. This work reports a multifunctional hot-emitter transistor with significant potential for low-power and negative-differential-resistance applications, marking a promising advancement for the post-Moore era.

2.
Small ; 19(35): e2300338, 2023 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-37186166

RESUMO

It is crucial to control the ion transport in membranes for various technological applications such as energy storage and conversion. The emerging functional two-dimensional (2D) nanosheets such as graphene oxide and MXenes show great potential for constructing ordered nanochannels, but the assembled membranes suffer from low ion selectivity and stability. Here a class of robust charge-selective membranes with superhigh cation/anion selectivity, which are assembled with monolayer nanosheets of cationic/anionic clays that inherently have permanent and uniform charges on each layer is reported. The transport number of cations/anions of cationic vermiculite nanosheet membranes (VNMs)/anionic Co-Al layered double hydroxide (CoAl-LDH) nanosheet membranes is over 0.90 in different NaCl concentration gradients, outperforming all the reported ion-selective membranes. Importantly, this excellent ion selectivity can persist at high-concentration salt solutions, under acidic and alkaline conditions, and for a wide range of ions of different sizes and charges. By coupling a pair of cation-selective vermiculite membrane and anion-selective CoAl-LDH membrane, a reverse electrodialysis device which shows an output power density of 0.7 W m-2 and energy conversion efficiency of 45.5% is constructed. This work provides a new strategy to rationally design high-performance ion-selective membranes by using 2D nanosheets with inherent surface charges for controllable ion-transport applications.

3.
Small ; 19(40): e2302920, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-37267934

RESUMO

Integrating a graphene transparent electrode (TE) matrix with driving circuits is essential for the practical use of graphene in optoelectronics such as active-matrix organic light-emitting diode (OLED) display, however it is disabled by the transport of carriers between graphene pixels after deposition of a semiconductor functional layer caused by the atomic thickness of graphene. Here, the carrier transport regulation of a graphene TE matrix by using an insulating polyethyleneimine (PEIE) layer is reported. The PEIE forms an ultrathin uniform film (≤10 nm) to fill the gap of the graphene matrix, blocking horizontal electron transport between graphene pixels. Meanwhile, it can reduce the work function of graphene, improving the vertical electron injection through electron tunneling. This enables the fabrication of inverted OLED pixels with record high current and power efficiencies of 90.7 cd A-1 and 89.1 lm W-1 , respectively. By integrating these inverted OLED pixels with a carbon nanotube-based thin-film transistor (CNT-TFT)-driven circuit, an inch-size flexible active-matrix OLED display is demonstrated, in which all OLED pixels are independently controlled by CNT-TFTs. This research paves a way for the application of graphene-like atomically thin TE pixels in flexible optoelectronics such as displays, smart wearables, and free-form surface lighting.

4.
Proc Natl Acad Sci U S A ; 117(42): 25991-25998, 2020 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-33020292

RESUMO

Graphene has emerged as an attractive candidate for flexible transparent electrode (FTE) for a new generation of flexible optoelectronics. Despite tremendous potential and broad earlier interest, the promise of graphene FTE has been plagued by the intrinsic trade-off between electrical conductance and transparency with a figure of merit (σDC/σOp) considerably lower than that of the state-of-the-art ITO electrodes (σDC/σOp <123 for graphene vs. ∼240 for ITO). Here we report a synergistic electrical/optical modulation strategy to simultaneously boost the conductance and transparency. We show that a tetrakis(pentafluorophenyl)boric acid (HTB) coating can function as highly effective hole doping layer to increase the conductance of monolayer graphene by sevenfold and at the same time as an anti-reflective layer to boost the visible transmittance to 98.8%. Such simultaneous improvement in conductance and transparency breaks previous limit in graphene FTEs and yields an unprecedented figure of merit (σDC/σOp ∼323) that rivals the best commercial ITO electrode. Using the tailored monolayer graphene as the flexible anode, we further demonstrate high-performance green organic light-emitting diodes (OLEDs) with the maximum current, power and external quantum efficiencies (111.4 cd A-1, 124.9 lm W-1 and 29.7%) outperforming all comparable flexible OLEDs and surpassing that with standard rigid ITO by 43%. This study defines a straightforward pathway to tailor optoelectronic properties of monolayer graphene and to fully capture their potential as a generational FTE for flexible optoelectronics.

5.
Nano Lett ; 22(23): 9380-9388, 2022 12 14.
Artigo em Inglês | MEDLINE | ID: mdl-36455614

RESUMO

Graphene has been considered a promising platform for molecular detection due to the graphene-enhanced Raman scattering (GERS) effect. However, the GERS performance of pristine graphene is limited by a low chemically active surface and insufficient density of states (DOS). Although diverse defects have been introduced, it remains a great challenge to improve the enhancement performance. Here, we show that graphene grain boundaries (GBs) possess stronger adsorption capacity and more abundant DOS. Thus, GERS performance increases with the atomic percentage of GBs, which makes nanocrystalline graphene (NG) film a superior GERS substrate. For R6G as a probe molecule, a low detection limit of 3 × 10-10 M was achieved. Utilizing the high chemical activity of GBs, we also fabricated NG film decorated with Au particles using a one-step quenching strategy, and this hybrid film exhibits an extremely low limit of detection down to 5 × 10-11 M, outperforming all the reported graphene-based systems.


Assuntos
Grafite , Grafite/química , Análise Espectral Raman
6.
Angew Chem Int Ed Engl ; 61(13): e202115389, 2022 Mar 21.
Artigo em Inglês | MEDLINE | ID: mdl-34931418

RESUMO

Electrochemical deposition has emerged as an efficient technique for preparing conjugated polymer films on electrodes. However, this method encounters difficulties in synthesizing crystalline products and controlling their orientation on electrodes. Here we report electrochemical film deposition of a large polycyclic aromatic hydrocarbon. The film is composed of single-crystalline nanorods, in which the molecules adopt a cofacial stacking arrangement along the π-π direction. Film thickness and crystal size can be controlled by electrochemical conditions such as scan rate and electrolyte species, while the choice of anode material determines crystal orientation. The film supports exceptionally efficient migration of both free carriers and excitons: the free carrier mobility reaches over 30 cm2 V-1 s-1 , whereas the excitons are delocalized with a low binding energy of 118.5 meV and a remarkable exciton diffusion length of 45 nm.

7.
Phys Chem Chem Phys ; 23(40): 23024-23031, 2021 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-34612268

RESUMO

Photodetectors based on intrinsic graphene can operate over a broad wavelength range with ultrafast response, but their responsivity is much lower than commercial silicon photodiodes. The combination of graphene with two-dimensional (2D) semiconductors may enhance the light absorption, but there is still a cutoff wavelength originating from the bandgap of semiconductors. Here, we report a highly responsive broadband photodetector based on the heterostructure of graphene and transition metal carbides (TMCs, more specifically Mo2C). The graphene-Mo2C heterostructure enhanced light absorption over a broad wavelength range from ultraviolet to infrared. In addition, there is very small resistance for photoexcited carriers in both graphene and Mo2C. Consequently, photodetectors based on the graphene-Mo2C heterostructure deliver a very high responsivity from visible to infrared telecommunication wavelengths.

8.
Nano Lett ; 19(2): 857-865, 2019 02 13.
Artigo em Inglês | MEDLINE | ID: mdl-30645133

RESUMO

The grain boundaries (GBs) of graphene and molybdenum disulfide have been extensively demonstrated to have a strong influence on electronic, thermal, optical, and mechanical properties. 2D transition-metal carbides (TMCs), known as MXenes, are a rapidly growing new family of 2D materials with many fascinating properties and promising applications. However, the GB structure of 2D TMCs and the influence of GB on their properties remain unknown. Here, we used aberration-corrected scanning transmission electron microscopy combined with electrical measurements to study the GB characteristic of highly crystalline 2D Mo2C superconductor, a newly emerging member of the 2D TMC family. The 2D Mo2C superconductor shows a unique tilt-angle-dependent GB structure and electronic transport properties. Different from the reported 2D materials, the GB of 2D Mo2C shows a peculiar dislocation configuration or sawtooth pattern depending on the tilt angle. More importantly, we found two new periodic GBs with different periodic structures and crystallographic orientations. Electrical measurements on individual GBs show that GB structure strongly affects the transport properties. In the normal state, an increasingly stronger electron localization behavior is observed at the GB region with increasing tilt angle. In the superconducting state, the magnitude of the critical current across the GBs is dramatically reduced, associated with local suppression of superconductivity at GBs. These findings provide new understandings on the GB structure of 2D TMCs and the influence of GB on 2D superconductivity, which would be helpful for tailoring the properties of 2D TMCs through GB engineering.

9.
Nano Lett ; 19(5): 3327-3335, 2019 05 08.
Artigo em Inglês | MEDLINE | ID: mdl-30995413

RESUMO

Materials can exhibit exotic properties when they approach the two-dimensional (2D) limit. Because of promising applications in catalysis and energy storage, 2D transition-metal carbides (TMCs) have attracted considerable attention in recent years. Among these TMCs, ultrathin crystalline α-Mo2C flakes have been fabricated by chemical vapor deposition on Cu/Mo bilayer foils, and their 2D superconducting property was revealed by transport measurements. Herein, we studied the ultrathin α-Mo2C flakes by atomic-resolved scanning tunneling microscopy/spectroscopy (STM/S). Strain-related structural modulation and the coexistence of different layer-stacking modes are observed on the Mo-terminated surface of α-Mo2C flakes as well as various lattice defects. Furthermore, an enhanced superconductivity with shorter correlation length was observed by STS technique, and such superconductivity is very robust despite the appearance of the defects. A mechanism of superconducting enhancement is proposed based on the strain-induced strong coupling and the increased disordering originated from lattice defects. Our results provide a comprehensive understanding of the correlations between atomic structure, defects, and enhanced superconductivity of this emerging 2D material.

10.
Nano Lett ; 16(7): 4243-50, 2016 07 13.
Artigo em Inglês | MEDLINE | ID: mdl-27323935

RESUMO

The properties of two-dimensional (2D) materials such as graphene and monolayer transition metal dichalcogenides are strongly influenced by domain boundaries. Ultrathin transition metal carbides are a class of newly emerging 2D materials that are superconducting and have many potential applications such as in electrochemical energy storage, catalysis, and thermoelectric energy conversion. However, little is known about their domain structure and the influence of domain boundaries on their properties. Here we use atomic-resolution scanning transmission electron microscopy combined with large-scale diffraction-filtered imaging to study the microstructure of chemical vapor deposited high-quality 2D α-Mo2C superconducting crystals of different regular shapes including triangles, rectangles, hexagons, octagons, nonagons, and dodecagons. The Mo atom sublattice in all these crystals has a uniform hexagonal closely packed arrangement without any boundaries. However, except for rectangular and octagonal crystals, the C atom sublattices are composed of three or six domains with rotational-symmetry and well-defined line-shaped domain boundaries because of the presence of three equivalent off-center directions of interstitial carbon atoms in Mo octahedra. We found that there is very small lattice shear strain across the domain boundary. In contrast to the single sharp transition observed in single-domain crystals, transport studies across domain boundaries show a broad resistive superconducting transition with two distinct transition processes due to the formation of localized phase slip events within the boundaries, indicating a significant influence of the boundary on 2D superconductivity. These findings provide new understandings on not only the microstructure of 2D transition metal carbides but also the intrinsic influence of domain boundaries on 2D superconductivity.

11.
Nat Mater ; 14(11): 1135-41, 2015 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-26280223

RESUMO

Transition metal carbides (TMCs) are a large family of materials with many intriguing properties and applications, and high-quality 2D TMCs are essential for investigating new physics and properties in the 2D limit. However, the 2D TMCs obtained so far are chemically functionalized, defective nanosheets having maximum lateral dimensions of ∼10 µm. Here we report the fabrication of large-area high-quality 2D ultrathin α-Mo2C crystals by chemical vapour deposition (CVD). The crystals are a few nanometres thick, over 100 µm in size, and very stable under ambient conditions. They show 2D characteristics of superconducting transitions that are consistent with Berezinskii-Kosterlitz-Thouless behaviour and show strong anisotropy with magnetic field orientation; moreover, the superconductivity is also strongly dependent on the crystal thickness. Our versatile CVD process allows the fabrication of other high-quality 2D TMC crystals, such as ultrathin WC and TaC crystals, which further expand the large family of 2D materials.

12.
Proc Natl Acad Sci U S A ; 110(51): 20386-91, 2013 Dec 17.
Artigo em Inglês | MEDLINE | ID: mdl-24297886

RESUMO

The controlled growth of large-area, high-quality, single-crystal graphene is highly desired for applications in electronics and optoelectronics; however, the production of this material remains challenging because the atomistic mechanism that governs graphene growth is not well understood. The edges of graphene, which are the sites at which carbon accumulates in the two-dimensional honeycomb lattice, influence many properties, including the electronic properties and chemical reactivity of graphene, and they are expected to significantly influence its growth. We demonstrate the growth of single-crystal graphene domains with controlled edges that range from zigzag to armchair orientations via growth-etching-regrowth in a chemical vapor deposition process. We have observed that both the growth and the etching rates of a single-crystal graphene domain increase linearly with the slanted angle of its edges from 0° to ∼19° and that the rates for an armchair edge are faster than those for a zigzag edge. Such edge-structure-dependent growth/etching kinetics of graphene can be well explained at the atomic level based on the concentrations of the kinks on various edges and allow the evolution and control of the edge and morphology in single-crystal graphene following the classical kinetic Wulff construction theory. Using these findings, we propose several strategies for the fabrication of wafer-sized, high-quality, single-crystal graphene.

13.
Nano Lett ; 15(10): 6677-82, 2015 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-26378374

RESUMO

A monolithic double-balanced graphene mixer integrated circuit (IC) has been successfully designed and fabricated. The IC adopted the cross-coupled resistive mixer topology, integrating four 500 nm-gate-length graphene field-effect transistors (GFETs), four on-chip inductors, and four on-chip capacitors. Passive-first-active-last fabrication flow was developed on 200 mm CMOS wafers. CMOS back-end-of-line processes were utilized to realize most fabrication steps followed by GFET-customized processes. Test results show excellent output spectrum purity with suppressed radio frequency (RF) and local oscillation (LO) signals feedthroughs, and third-order input intercept (IIP3) reaches as high as 21 dBm. The results are compared with a fabricated single-GEFT mixer, which generates IIP3 of 16.5 dBm. Stand-alone 500 nm-gate-length GFETs feature cutoff frequency 22 GHz and maximum oscillation frequency 20.7 GHz RF performance. The double-balanced mixer IC operated with off-chip baluns realizing a print-circuit-board level electronic system. It demonstrates graphene's potential to compete with other semiconductor technologies in RF front-end applications.

14.
Proc Natl Acad Sci U S A ; 109(43): 17360-5, 2012 Oct 23.
Artigo em Inglês | MEDLINE | ID: mdl-23045691

RESUMO

There is growing interest in thin, lightweight, and flexible energy storage devices to meet the special needs for next-generation, high-performance, flexible electronics. Here we report a thin, lightweight, and flexible lithium ion battery made from graphene foam, a three-dimensional, flexible, and conductive interconnected network, as a current collector, loaded with Li(4)Ti(5)O(12) and LiFePO(4), for use as anode and cathode, respectively. No metal current collectors, conducting additives, or binders are used. The excellent electrical conductivity and pore structure of the hybrid electrodes enable rapid electron and ion transport. For example, the Li(4)Ti(5)O(12)/graphene foam electrode shows a high rate up to 200 C, equivalent to a full discharge in 18 s. Using them, we demonstrate a thin, lightweight, and flexible full lithium ion battery with a high-rate performance and energy density that can be repeatedly bent to a radius of 5 mm without structural failure and performance loss.

15.
Nature ; 497(7450): 448-9, 2013 May 23.
Artigo em Inglês | MEDLINE | ID: mdl-23698442
16.
Angew Chem Int Ed Engl ; 53(34): 8908-12, 2014 Aug 18.
Artigo em Inglês | MEDLINE | ID: mdl-24981312

RESUMO

Chemical decoration of defects is an effective way to functionalize graphene and to study mechanisms of their interaction with environment. We monitored dynamic atomic processes during the formation of a rotary Si trimer in monolayer graphene using an aberration-corrected scanning-transmission electron microscope. An incoming Si atom competed with and replaced a metastable C dimer next to a pair of Si substitutional atoms at a topological defect in graphene, producing a Si trimer. Other atomic events including removal of single C atoms, incorporation and relocation of a C dimer, reversible C-C bond rotation, and vibration of Si atoms occurred before the final formation of the Si trimer. Theoretical calculations indicate that it requires 2.0 eV to rotate the Si trimer. Our real-time results provide insight with atomic precision for reaction dynamics during chemical doping at defects in graphene, which have implications for defect nanoengineering of graphene.

17.
Nat Commun ; 15(1): 2706, 2024 Mar 27.
Artigo em Inglês | MEDLINE | ID: mdl-38538584

RESUMO

Proton transport in nanofluidic channels is not only fundamentally important but also essential for energy applications. Although various strategies have been developed to improve the concentration of active protons in the nanochannels, it remains challenging to achieve a proton conductivity higher than that of Nafion, the benchmark for proton conductors. Here, taking H3Sb3P2O14 and HSbP2O8 as examples, we show that the interactions between protons and the layer frameworks in layered solid acid HnMnZ2O3n+5 are substantially reduced at the monolayer limit, which significantly increases the number of active protons and consequently improves the proton conductivities by ∼8 ‒ 66 times depending on the humidity. The membranes assembled by monolayer H3Sb3P2O14 and HSbP2O8 nanosheets exhibit in-plane proton conductivities of ~ 1.02 and 1.18 S cm-1 at 100% relative humidity and 90 °C, respectively, which are over 5 times higher than the conductivity of Nafion. This work provides a general strategy for facilitating proton transport, which will have broad implications in advancing both nanofluidic research and device applications from energy storage and conversion to neuromorphic computing.

18.
Gene ; 893: 147912, 2024 Jan 30.
Artigo em Inglês | MEDLINE | ID: mdl-37863300

RESUMO

Heat shock proteins (HSPs) are essential for plant growth, development, and stress adaptation. However, their roles in Jerusalem artichoke are largely unexplored. Using bioinformatics, we classified 143 HSP genes into distinct families: HSP40 (82 genes), HSP60 (22 genes), HSP70 (29 genes), HSP90 (6 genes), and HSP100 (4 genes). Our analysis covered their traits, evolution, and structures. Using RNA-seq data, we uncovered unique expression patterns of these HSP genes across growth stages and tissues. Notably, HSP40, HSP60, HSP70, HSP90, and HSP100 families each had specific roles. We also studied how these gene families responded to various stresses, from extreme temperatures to drought and salinity, revealing intricate expression dynamics. Remarkably, HSP40 showed remarkable flexibility, while HSP60, HSP70, HSP90, and HSP100 responded specifically to stress types. Moreover, our analysis unveiled significant correlations between gene pairs under stress, implying cooperative interactions. qRT-PCR validation underscored the significance of particular genes such as HtHSP60-7, HtHSP90-5, HtHSP100-2, and HtHSP100-3 in responding to stress. In summary, our study advances the understanding of how HSP gene families collectively manage stresses in Jerusalem artichoke. This provides insights into specific gene functions and broader plant stress responses.


Assuntos
Helianthus , Helianthus/genética , Helianthus/metabolismo , Proteínas de Choque Térmico/metabolismo , Estresse Fisiológico/genética , Proteínas de Choque Térmico HSP70/genética , Proteínas de Choque Térmico HSP90/genética
19.
ACS Nano ; 18(34): 23468-23476, 2024 Aug 27.
Artigo em Inglês | MEDLINE | ID: mdl-39149802

RESUMO

Highly thermally conductive and flexible thermal interface materials (TIMs) are desirable for heat dissipation in modern electronic devices. Here, we fabricated a high-crystalline aligned graphene lamella framework (AGLF) with precisely controlled lamella thickness, pore structure, and excellent intergraphene contact by manipulating the thermal expansion behavior of scanning centrifugal casted graphene oxide films. The rational design of the AGLF balances the trade-off between the thermal conductivity and flexibility of TIMs. The AGLF-based TIM (AGLF-TIM) shows a record thermal conductivity of 196.3 W m-1 K-1 with a graphene loading of only 9.4 vol %, which is about 4 times higher than those of reported TIMs at a similar graphene loading. Meanwhile, good flexibility remains comparable to that of commercial TIMs. As a result, an LED device achieves an additional temperature decrease of ∼8 °C with the use of AGLF-TIM compared to high-performance commercial TIMs. This work offers a strategy for the controlled fabrication of graphene macrostructures, showing the potential use of graphene as filler frameworks in thermal management.

20.
Sci Bull (Beijing) ; 69(10): 1427-1436, 2024 May 30.
Artigo em Inglês | MEDLINE | ID: mdl-38531717

RESUMO

Developing low-power FETs holds significant importance in advancing logic circuits, especially as the feature size of MOSFETs approaches sub-10 nanometers. However, this has been restricted by the thermionic limitation of SS, which is limited to 60 mV per decade at room temperature. Herein, we proposed a strategy that utilizes 2D semiconductors with an isolated-band feature as channels to realize sub-thermionic SS in MOSFETs. Through high-throughput calculations, we established a guiding principle that combines the atomic structure and orbital interaction to identify their sub-thermionic transport potential. This guides us to screen 192 candidates from the 2D material database comprising 1608 systems. Additionally, the physical relationship between the sub-thermionic transport performances and electronic structures is further revealed, which enables us to predict 15 systems with promising device performances for low-power applications with supply voltage below 0.5 V. This work opens a new way for the low-power electronics based on 2D materials and would inspire extensive interests in the experimental exploration of intrinsic steep-slope MOSFETs.

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