Realization of Quantum Hall Effect in Chemically Synthesized InSe

Recently, 2D electron gases have been observed in atomically thin semiconducting crystals, enabling the observation of rich physical phenomena at the quantum level within the ultimate thickness limit. However, the observation of 2D electron gases and subsequent quantum Hall effect require exceptionally high crystalline quality, rendering mechanical exfoliation as the only method to produce high‐quality 2D semiconductors of black phosphorus and indium selenide (InSe), which hinder large‐scale device applications. Here, the controlled one‐step synthesis of high‐quality 2D InSe thin films via chemical vapor transport method is reported. The carrier Hall mobility of hexagonal boron nitride (hBN) encapsulated InSe flakes can be up to 5000 cm² V^?1 s^?1 at 1.5 K, enabling to observe the quantum Hall effect in a synthesized van der Waals semiconductor. The existence of the quantum Hall effect in directly synthesized 2D semiconductors indicates a high quality of the chemically synthesized 2D semiconductors, which hold promise in quantum devices and applications with high mobility.     

Electrical‐Polarization‐Induced Ultrahigh Responsivity Photodetectors Based on Graphene and Graphene Quantum Dots

Hybrid quantum dot–graphene photodetectors have recently attracted substantial interest because of their remarkable performance and low power consumption. However, the performance of the device greatly depends on the interfacial states and photogenerated screening field. As a consequence, the sensitivity is limited and the response time is relatively slow. In order to circumvent these challenges, herein, a composite graphene and graphene quantum dot (GQD) photodetector on lead zirconate titanate (Pb(Zr_0.2Ti_0.8)O₃) (PZT) substrates has been designed to form an ultrasensitive photodetector over a wide range of illumination power. Under 325 nm UV light illumination, the device shows sensitivity as high as 4.06 × 10⁹ A W^?1, which is 120 times higher than reported sensitivity of the same class of devices. Plant derived GQD has a broad range of absorptivity and is an excellent candidate for harvesting photons generating electron–hole pairs. Intrinsic electric field from PZT substrate separates photogenerated electron–hole pairs as well as provides the built‐in electric field that causes the holes to transfer to the underlying graphene channel. The composite structure of graphene and GQD on PZT substrate therefore produces a simple, stable, and highly sensitive photodetector over a wide range of power with short response time, which shows a way to obtain high‐performance optoelectronic devices.     

Label‐Free Electrical Detection of DNA Hybridization on Graphene using Hall Effect Measurements: Revisiting the Sensing Mechanism

There is broad interest in using graphene or graphene oxide sheets as a transducer for label‐free and selective electrical detection of biomolecules such as DNA. However, it is still not well explored how the DNA molecules interact with and influence the properties of graphene during the detection. Here, Hall effect measurements based on the Van der Pauw method are used to perform single‐base sequence selective detection of DNA on graphene sheets, which are prepared by chemical vapor deposition. The sheet resistance increases and the mobility decreases with the addition of either complementary or one‐base mismatched DNA to the graphene device. The hole carrier concentration of the graphene devices increases significantly with the addition of complementary DNA but it is less affected by the one‐base mismatched DNA. It is concluded that the increase in hole carrier density, indicating p‐doping to graphene, is better correlated with the DNA hybridization compared to the commonly used parameters such as conductivity change. The different electrical observations of p‐doping from Hall effect measurements and n‐doping from electrolyte‐gated transistors can be explained by the characteristic morphology of partially hybridized DNA on graphene and the mismatch between DNA chain length and Debye length in electrolytes.     

Interlayer Band‐to‐Band Tunneling and Negative Differential Resistance in van der Waals BP/InSe Field‐Effect Transistors

Atomically thin layers of van der Waals (vdW) crystals offer an ideal material platform to realize tunnel field‐effect transistors (TFETs) that exploit the tunneling of charge carriers across the forbidden gap of a vdW heterojunction. This type of device requires a precise energy band alignment of the different layers of the junction to optimize the tunnel current. Among 2D vdW materials, black phosphorus (BP) and indium selenide (InSe) have a Brillouin zone‐centered conduction and valence bands, and a type II band offset, both ideally suited for band‐to‐band tunneling. TFETs based on BP/InSe heterojunctions with diverse electrical transport characteristics are demonstrated: forward rectifying, Zener tunneling, and backward rectifying characteristics are realized in BP/InSe junctions with different thickness of the BP layer or by electrostatic gating of the junction. Electrostatic gating yields a large on/off current ratio of up to 10⁸ and negative differential resistance at low applied voltages (V ≈ 0.2 V). These findings illustrate versatile functionalities of TFETs based on BP and InSe, offering opportunities for applications of these 2D materials beyond the device architectures reported in the current literature.     

Overcoming the Cut‐Off Charge Transfer Bandgaps at the PbS Quantum Dot Interface

Light harvesting from large size of semiconductor PbS quantum dots (QDs) with a bandgap of less than 1 eV is one of the greatest challenges precluding the development of PbS QD‐based solar cells because the interfacial charge transfer (CT) from such QDs to the most commonly used electron acceptor materials is very inefficient, if it occurs at all. Thus, an alternative electron‐accepting unit with a new driving force for CT is urgently needed to harvest the light from large‐sized PbS QDs. Here, a cationic porphyrin is utilized as a new electron acceptor unit with unique features that bring the donor–acceptor components into close molecular proximity, allowing ultrafast and efficient electron transfer for QDs of all sizes, as inferred from the drastic photoluminescence quenching and the ultrafast formation of the porphyrin anionic species. The time‐resolved results clearly demonstrate the possibility of modulating the electron transfer process between PbS QDs and porphyrin moieties not only by the size quantization effect but also by the interfacial electrostatic interaction between the positively charged porphyrin and the negatively charged QDs. This approach provides a new pathway for engineering QD‐based solar cells that make the best use of the diverse photons making up the Sun's broad irradiance spectrum.     

Top‐Emission Organic Light‐Emitting Diode with a Novel Copper/Graphene Composite Anode

The relatively high sheet resistance of graphene compared with indium tin oxide (ITO) blocks the applications of graphene as transparent electrodes in organic light‐emitting diodes. A novel copper (Cu)/graphene composite electrode is presented and employed as the anode of a top‐emission organic light‐emitting diode with the structure of Cu/graphene/V₂O₅/NPB/Alq₃/Alq₃: C545T/Bphen: Cs₂CO₃/Sm/Au. The Cu/graphene composite electrodes are fabricated by growing graphene directly on Cu substrates via the chemical vapor deposition method without any transfer process. The maxima of current efficiency and power efficiency of a typical Cu/graphene composite anode device reach 6.1 cd/A and 7.6 lm/W, respectively, which are markedly higher than those of the control devices with a graphene anode, a Cu anode or an ITO anode. The low sheet resistance of the composite electrode, the high quality of graphene without any transfer process and the avoidance of wave guiding loss in glass or polyethylene terephthalate substrates result in the improvements of light emission efficiencies.     

Graphene Liquid Cells Assembled through Loop‐Assisted Transfer Method and Located with Correlated Light‐Electron Microscopy

Graphene liquid cells (GLCs) for transmission electron microscopy (TEM) enable high‐resolution, real‐time imaging of dynamic processes in water. Large‐scale implementation, however, is prevented by major difficulties in reproducing GLC fabrication. Here, a high‐yield method is presented to fabricate GLCs under millimeter areas of continuous graphene, facilitating efficient GLC formation on a TEM grid. Additionally, GLCs are located on the grid using correlated light‐electron microscopy (CLEM), which reduces beam damage by limiting electron exposure time. CLEM allows the acquisition of reliable statistics and the investigation of the most common shapes of GLCs. In particular, a novel type of liquid cell is found, formed from only a single graphene sheet, greatly simplifying the fabrication process. The methods presented in this work—particularly the reproducibility and simplicity of fabrication—will enable future application of GLCs for high‐resolution dynamic imaging of biomolecular systems.     

Microwave‐Assisted Preparation of White Fluorescent Graphene Quantum Dots as a Novel Phosphor for Enhanced White‐Light‐Emitting Diodes

Graphene quantum dots (GQDs) with white fluorescence are synthesized by a microwave‐assisted hydrothermal method using graphite as the precursor. A solution‐processed white‐light‐emitting diode (WLED) is fabricated using the as‐prepared white fluorescent GQDs (white‐light‐emitting graphene quantum dots, WGQDs) doped 4,4‐bis(carbazol‐9‐yl)biphenyl as the emissive layer. White‐light emission is obtained from the WLED with 10 wt% doping concentration of WGQDs, which shows a luminance of 200 cd m^?2 at the applied voltage of 11–14 V. Importantly, an external quantum efficiency of 0.2% is achieved, which is the highest among all the reported WLED based on GQDs or carbon dots. The results demonstrate that WGQDs as a novel phosphor may open up a new avenue to develop the environmentally friendly WLEDs for practical application in solid‐state lighting.     

Gate‐Controlled Energy Barrier at a Graphene/Molecular Semiconductor Junction

The formation of an energy‐barrier at a metal/molecular semiconductor junction is a universal phenomenon which limits the performance of many molecular semiconductor‐based electronic devices, from field‐effect transistors to light‐emitting diodes. In general, a specific metal/molecular semiconductor combination of materials leads to a fixed energy‐barrier. However, in this work, a graphene/C₆₀ vertical field‐effect transistor is presented in which control of the interfacial energy‐barrier is demonstrated, such that the junction switches from a highly rectifying diode at negative gate voltages to a highly conductive nonrectifying behavior at positive gate voltages and at room temperature. From the experimental data, an energy‐barrier modulation of up to 660 meV, a transconductance of up to five orders of magnitude, and a gate‐modulated photocurrent are extracted. The ability to tune the graphene/molecular semiconductor energy‐barrier provides a promising route toward novel, high performance molecular devices.     

Transparent and Stretchable Interactive Human Machine Interface Based on Patterned Graphene Heterostructures

An interactive human‐machine interface (iHMI) enables humans to control hardware and collect feedback information. In particular, wearable iHMI systems have attracted tremendous attention owing to their potential for use in personal mobile electronics and the Internet of Things. Although significant progress has been made in the development of iHMI systems, those based on rigid electronics have constraints in terms of wearability, comfortability, signal‐to‐noise ratio (SNR), and aesthetics. Herein the fabrication of a transparent and stretchable iHMI system composed of wearable mechanical sensors and stimulators is reported. The ultrathin and lightweight design of the system allows superior wearability and high SNR. The use of conductive/piezoelectric graphene heterostructures, which consist of poly(l ‐lactic acid), single‐walled carbon nanotubes, and silver nanowires, results in high transparency, excellent performance, and low power consumption as well as mechanical deformability. The control of a robot arm for various motions and the feedback stimulation upon successful executions of commands are demonstrated using the wearable iHMI system.     

Doping‐Induced Charge Trapping in Organic Light‐Emitting Devices

By using pyran‐containing donor–acceptor dyes as doping molecules in organic light‐emitting devices (OLEDs), we scrutinize the effects of charge trapping and polarization induced by the guest molecules in the electro‐active host material. Laser dyes 4‐(dicyanomethylene)‐2‐methyl‐6‐[2‐(julolidin‐9‐yl)phenyl]ethenyl]‐4H‐pyran (DCM2) and the novel 4‐(dicyanomethylene)‐2‐methyl‐6‐{2‐[(4‐diphenylamino)phenyl]ethenyl}‐4H‐pyran (DCM‐TPA) are used as model compounds. The emission color of these polar dyes depends strongly on doping concentration, which we have attributed to polarization effects induced by the doping molecules themselves. Their frontier orbital energy levels are situated within the bandgap of the tris(8‐hydroxyquinoline)aluminum (Alq₃) host matrix and allow the investigation of either electron trapping or both electron and hole trapping. In the case of DCM‐TPA doping, we were able to show that electron trapping leads to a partial shift of the recombination zone out of the doped Alq₃ region. To impede charge‐recombination processes taking place in the undoped host matrix, a charge‐blocking layer efficiently confines the recombination zone inside the doped zone and gives rise to increased luminous efficiency. For a doping concentration of 1 wt.‐% we obtain a maximum luminous efficiency of 10.4 cd A^–1. At this doping concentration, the yellow emission spectrum shows excellent color saturation with CIE chromaticity coordinates x, y of 0.49 and 0.50, respectively. In the case of DCM2 the recombination zone is much less affected for the same doping concentrations, which is ascribed to the fact that both electrons and holes are being trapped. The experimental findings are corroborated with a numerical simulation of the doped multilayer devices.     

Photocatalyst Interface Engineering: Spatially Confined Growth of ZnFe2O4 within Graphene Networks as Excellent Visible‐Light‐Driven Photocatalysts

High‐performance photocatalysts should have highly crystallized nanocrystals (NCs) with small sizes, high separation efficiency of photogenerated electron–hole pairs, fast transport and consumption of photon‐excited electrons from the surface of catalyst, high adsorption of organic pollutant, and suitable band gap for maximally utilizing sunlight energy. However, the design and synthesis of these versatile structures still remain a big challenge. Here, we report a novel strategy for the synthesis of ultrasmall and highly crystallized graphene–ZnFe₂O₄ photocatalyst through interface engineering by using interconnected graphene network as barrier for spatially confined growth of ZnFe₂O₄, as transport channels for photon‐excited electron from the surface of catalyst, as well as the electron reservoir for suppressing the recombination of photogenerated electron–hole pairs. As a result, about 20 nm ZnFe₂O₄ NCs with highly crystallized (311) plane confined in the graphene network exhibit an excellent visible‐light‐driven photocatalytic activity with an ultrafast degradation rate of 1.924 × 10^?7 mol g^?1 s^?1 for methylene blue, much higher than those of previously reported photocatalysts such as spinel‐based photocatalysts (20 times), TiO₂‐based photocatalysts (4 times), and other photocatalysts (4 times). Our strategy can be further extended to fabricate other catalysts and electrode materials for supercapacitors and Li‐ion batteries.     

Highly Polarized and Fast Photoresponse of Black Phosphorus‐InSe Vertical p–n Heterojunctions

The van der Waals heterojunctions of 2D materials offer tremendous opportunities in designing and investigating multifunctional and high‐performance electronic and optoelectronic devices. In this study, a vertical p–n diode is constructed by vertically stacking p‐type few‐layer black phosphorus (BP) on n‐type few‐layer indium selenide (InSe). The photodetector based on the heterojunction displays a broadband and gate‐modulated photoresponse under illumination. More importantly, by taking advantage of the strong linear dichroism of BP, the device demonstrates a highly polarization‐sensitive photocurrent with an anisotropy ratio as high as 0.83. Additionally, the device can function in a zero‐bias photovoltaic mode, enabling a fast photoresponse and low dark current. The external quantum efficiency can reach ≈3%, which is impressive for BP‐based devices. The results pave the way for the implementation of p‐BP/n‐InSe heterostructure as a promising candidate for future multifunctional optoelectronics and, especially, polarization‐sensitive applications.     

Graphene Solution‐Gated Field‐Effect Transistor Array for Sensing Applications

Graphene, with its unique combination of physical and electronic properties, holds great promise for biosensor and bioelectronic applications. In this respect, the development of graphene solution‐gated field‐effect transistor (SGFET) arrays capable of operation in aqueous environments will establish the real potential of graphene in this rapidly emerging field. Here, we report on a facile route for the scalable fabrication of such graphene transistor arrays and provide a comprehensive characterization of their operation in aqueous electrolytes. An on‐chip structure for Hall‐effect measurements allows the direct determination of charge carrier concentrations and mobilities under electrolyte gate control. The effect of the solution‐gate potential on the electronic properties of graphene is explained using a model that considers the microscopic structure of water at the graphene/electrolyte interface. The graphene SGFETs exhibit a high transconductance and correspondingly high sensitivity, together with an effective gate noise as low as tens of μV. Our study demonstrates that graphene SGFETs, with their facile technology, high transconductance, and low noise promise to far outperform state‐of‐the‐art Si‐based devices for biosensor and bioelectronic applications.     

热光源和稳恒磁场对石墨烯阻值的影响

研究了热光源和稳恒磁场对石墨烯阻值的影响。首先分析了光致吸附作用,利用Drude形式,建立了温度与阻值之间的关系。然后利用哈伯德模型和微扰理论,找到稳恒磁场中石墨烯从金属态到绝缘态的临界相变条件。实验结果表明,热光源的光功率从0增加到0.88 mW时,石墨烯的阻值从38.44Ω减小到33.48Ω。稳恒磁场从0增加到122.70 mT时,石墨烯阻值从38.44Ω增加到44.24Ω。实验结果证明了磁场强度与石墨烯阻值之间有着良好的线性关系。这对于石墨烯在导电涂层、抗腐蚀涂层和锂离子电池领域的应用具有一定的指导意义。     

Electrochemical Control of Charge Current Flow in Nanoporous Graphene

During the last decade, on-surface fabricated graphene nanoribbons (GNRs) have gathered enormous attention due to their semiconducting π-conjugated nature and atomically precise structure. A significant breakthrough is the recent fabrication of nanoporous graphene (NPG) as a 2D array of laterally bonded GNRs. This covalent integration of GNRs could enable complex electronic functionality at the nanoscale; however, for that, it is crucial to externally control the electronic coupling between GNRs within NPGs, which, to date, has not been possible. Using quantum chemical calculations and large-scale transport simulations, this study demonstrates that such control is enabled in a newly designed quinone-NPG (q-NPG) thanks to its GNRs inter-connections based on electroactive para-benzoquinone units. As a result, the spatial distribution of injected currents in q-NPG may be tuned, with sub-nanometer precision, via the application of external electrostatic gates and electrochemical means. These results thus provide a fundamental strategy to design organic nanodevices with built-in externally tunable electronics and spintronics, which is key for future applications such as bio-chemical nanosensing and carbon nanoelectronics.     

High Sensitivity Graphene Field Effect Transistor‐Based Detection of DNA Amplification

Enzymatic DNA amplification‐based approaches involving intercalating DNA‐binding fluorescent dyes and expensive optical detectors are the gold standard for nucleic acid detection. As components of a simplified and miniaturized system, conventional silicon‐based ion sensitive field effect transistors (ISFETs) that measure a decrease in pH due to the generation of pyrophosphates during DNA amplification have been previously reported. In this article, Bst polymerase in a loop‐mediated isothermal amplification (LAMP) reaction combined with target‐specific primers and crumpled graphene field effect transistors (gFETs) to electrically detect amplification by sensing the reduction in primers is used. Graphene is known to adsorb single‐stranded DNA due to noncovalent π–π bonds, but not double‐stranded DNA. This approach does not require any surface functionalization and allows the detection of primer concentrations at the endpoint of reactions. As recently demonstrated, the crumpled gFET over the conventional flat gFET sensors due to their superior sensitivity is chosen. The endpoint of amplification reaction with starting concentrations down to 8 × 10^?21 m in 90 min including the time of amplification and detection is detected. With its high sensitivity and small footprint, this platform will help bring complex lab‐based diagnostic and genotyping amplification assays to the point‐of‐care.     

An Ultralight Graphene Honeycomb Sandwich for Stretchable Light‐Emitting Displays

Materials that can simultaneously achieve excellent electrical conductivity and stretchability are essential components for the next‐generation stretchable electronics. Herein, a highly conductive and stretchable graphene honeycomb (GHC) sandwich consisting of a porous GHC/polydimethylsiloxane (PDMS) composite core and ultrahigh‐density graphene foam/PDMS composite face sheets is rationally assembled. The GHCs prepared by a 3D printing technique possess a long‐range ordered hexagonal porous structure with an ultralow density of 3.25 mg cm^?3 and deliver an excellent electrical conductivity of 72 S m^?1. To the best of authors' knowledge, they are the lightest honeycomb structure reported in open literature. The highly porous GHC core endows the sandwich with an ultralow resistance change over large external strains of 60% with excellent structural durability. A stretchable light‐emitting display is demonstrated using the sandwich as the electric circuit and light‐emitting diodes as the pixels, which exhibits reliable lighting performance under different loading conditions.