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1.
Since discovered in 2011, transition metal carbides or nitrides (MXenes) have attracted enormous attention due to their unique properties. Morphology regulation strategies assembling 2D MXene sheets into 3D architecture have endowed the as-formed porous MXene with a better performance in various fields. However, the direct patterning strategy for the porous MXene into integration with multifunctional and multichannel electronic devices still needs to be investigated. The metal-assisted electro-gelation method the authors propose can directly generate porous-structured MXene hydrogel with a tunable feature. By electrolyzing the sacrificial metal, the released metal cations initiate the electro-gelation process during which electrostatic interactions occur between cations and the MXene sheets. A high spatial resolution down to micro-meter level is achieved utilizing the method, enabling high-performance hydrogels with more complex architectures. Electronics prepared through this metal-assisted electro-gelation process have shown promising applications of the porous MXene in energy and biochemical sensing fields. Energy storage devices with a capacitance at 33.3 mF cm−2 and biochemical sensors show prominent current responses towards metabolites (sensitivity of H2O2: 165.6  µ A mm −1 cm−2; sensitivity of DA: 212 nA  µ m −1 cm−2), suggesting that the metal-assisted electro-gelation method will become a prospective technique for advanced fabrication of MXene-based devices.  相似文献   

2.
Recent advances in 2D magnetism have heightened interest in layered magnetic materials due to their potential for spintronics. In particular, layered semiconducting antiferromagnets exhibit intriguing low-dimensional semiconducting behavior with both charge and spin as carrier controls. However, synthesis of these compounds is challenging and remains rare. Here, first-principles based high-throughput search is conducted to screen potentially stable mixed metal phosphorous trichalcogenides (MMP2X6, where M and M are transition metals and X is a chalcogenide) that have a wide range of tunable bandgaps and interesting magnetic properties. Among the potential candidates, a stable semiconducting layered magnetic material, CdFeP2Se6, that exhibits a short-range antiferromagnetic order at TN = 21 K with an indirect bandgap of 2.23 eV is successfully synthesized . This work suggests that high-throughput screening assisted synthesis can be an effective method for layered magnetic materials discovery.  相似文献   

3.
Antiferroelectrics, characterized by electrically controlled antipolar-polar phase transformation, have attracted tremendous attention as a class of promising electroactive materials for assembling electronic devices. The emerging two-dimensional (2D) halide perovskites with superior compositional diversity offer an ideal platform for exploring electroactive materials, whereas lead-free antiferroelectric counterparts are still scarcely reported. Herein, for the first time, a new lead-free 2D germanium iodide perovskite antiferroelectric (i-BA)2CsGe2I7 ( 1 , i-BA is iso-butylammonium) has been presented, which exhibits a high Curie temperature (Tc) up to 403 K. Remarkably, benefiting from the lone pair stereochemical activity in Ge2+ induced large structural distortion and Cs+ ion off-center displacement, 1 shows well-defined double P–E hysteresis loops in a wide temperature range with a giant maximum polarization up to 18.8 µC cm−2, which achieves a new high record among molecular antiferroelectrics. Moreover, under a low external electric field of 22.5 kV cm−1, the antipolar-polar phase transformation in 1 affords a recoverable energy storage density Wrec of 0.27 J cm−3 and high storage efficiency up to 79.76%. Such lead-free halide perovskite antiferroelectric with intriguing antiferroelectric behaviors, including high Tc, large polarization and remarkable energy storage properties, is exciting, which provides an alternative candidate for high-performance antiferroelectrics for environmentally friendly electronic devices.  相似文献   

4.
Quasi-2D perovskites have shown great potential in achieving solution-processed electrically pumped laser diodes due to their multiple-quantum-well structure, which induces a carrier cascade process that can significantly enhance population inversion. However, continuous-wave (CW) optically pumped lasing has yet to be achieved with near-infrared (NIR) quasi-2D perovskites due to the challenges in obtaining high-quality quasi-2D films with suitable phase distribution and morphology. This study regulates the crystallization of a NIR quasi-2D perovskite ((NMA)2FAn−1PbnI3n+1) using an 18-crown-6 additive, resulting in a compact and smooth film with a largely improved carrier cascade efficiency. The amplified spontaneous emission threshold of the film is reduced from 47.2 to 35.9 µJ cm−2. Furthermore, by combining the film with a high-quality distributed feedback grating, this study successfully realizes a CW NIR laser of 809 nm at 110 K, with a high Q-factor of 4794 and a low threshold of 911.6 W cm−2. These findings provide an important foundation for achieving electrically pumped laser diodes based on the unique quasi-2D perovskites.  相似文献   

5.
Two-dimensional (2D) photodetecting materials have shown superior performances over traditional materials (e.g., silicon, perylenes), which demonstrate low responsivity (R) ( < 1 AW−1), external quantum efficiency (EQE) ( < 100%), and limited detection bandwidth. Recently, 2D indium selenide (InSe) emerged as high-performance active material in field-effect transistors and photodetectors, whose fabrication required expensive and complex techniques. Here, it is shown for the first time how molecular functionalization with a common surfactant molecule (didodecyldimethylammonium bromide) (DDAB) represents a powerful strategy to boost the (opto)electronic performances of InSe yielding major performance enhancements in phototransistors, Schottky junctions, and van der Waals heterostructures via a lithography-compatible fabrication route. The functionalization can controllably dope and heal vacancies in InSe, resulting in ultrahigh field-effect mobility (103 cm2 V−1 s−1) and photoresponsivity (106 A W−1), breaking the record of non-graphene-contacted 2D photodetectors. The strategy towards the molecular doping of 2D photodetecting materials is efficient, practical, up-scalable, and operable with ultra-low power input, ultimately paving the way to next-generation 2D opto-electronics.  相似文献   

6.
Energy conversion and storage devices are highly desirable for the sustainable development of human society. Hybrid organic–inorganic perovskites have shown great potential in energy conversion devices including solar cells and photodetectors. However, its potential in energy storage has seldom been explored. Here the crystal structure and electrical properties of the 2D hybrid perovskite (benzylammonium)2PbBr4 (PVK-Br) are investigated, and the consecutive ferroelectric-I (FE1) to ferroelectric-II (FE2) then to antiferroelectric (AFE) transitions that are driven by the orderly alignment of benzylamine and the distortion of [PbBr6] octahedra are found. Furthermore, accompanied by field-induced AFE to FE transition near room temperature, a large energy storage density of ≈1.7 J cm−3 and a wide working temperature span of ≈70 K are obtained; both of which are among the best in hybrid AFEs. This good energy storage performance is attributed to the large polarization of ≈7.6 µC cm−2 and the high maximum electric field of over 1000 kV cm−1, which, as revealed by theoretical calculations, originate from the cooperative coupling between the [PbBr6] octahedral framework and the benzylamine molecules. The research clarifies the discrepancy in the phase transition character of PVK-Br and shed light on developing high-performance energy storage devices based on 2D hybrid perovskite.  相似文献   

7.
2D semiconductors are promising for fabricating miniaturized and flexible electronic devices. The manipulation of polarities in 2D semiconductors is key to fabricate functional devices and circuits. However, the switchable and reversible control of polarity in 2D semiconductors is challenging due to their ultrathin body. Herein, a reversible and non-destructive method is developed to dope 2D semiconductors by using ionic 2D minerals as the electrostatic gating. The 2D semiconductor channel can be reversibly transformed between n+ and p+ types with carrier concentrations of 1.59 × 1013 and 6.82 × 1012 cm−2, respectively. With the ability to in situ control carrier type and concentration in 2D semiconductors by ionic gating, a reversible PN/NP junction and programmable logic gate are demonstrated in such devices. This 2D mineral materials-based ionic doping approach provides an alternative method for achieving multi-functional and complex circuits in an all-2D material flatform.  相似文献   

8.
Near infrared (NIR) photodetectors based on 2D materials are widely studied for their potential application in next generation sensing, thermal imaging, and optical communication. Construction of van der Waals (vdWs) heterostructure provides a tremendous degree of freedom to combine and extend the features of 2D materials, opening up new functionalities on photonic and optoelectronic devices. Herein, a type-II InSe/PdSe2 vdWs heterostructure with strong interlayer transition for NIR photodetection is demonstrated. Strong interlayer transition between InSe and PdSe2 is predicted via density functional theory calculation and confirmed by photoluminance spectroscopy and Kelvin probe force microscopy. The heterostructure exhibits highly sensitive photodetection in NIR region up to 1650 nm. The photoresponsivity, detectivity, and external quantum efficiency at this wavelength respectively reaches up to 58.8 A W−1, 1 × 1010 Jones, and 4660%. The results suggest that the construction of vdWs heterostructure with strong interlayer transition is a promising strategy for infrared photodetection, and this work paves the way to developing high-performance optoelectronic devices based on 2D vdWs heterostructures.  相似文献   

9.
The Dirac semimetal cadmium arsenide (Cd3As2), a 3D electronic analog of graphene, has sparked renewed research interests for its novel topological phases and excellent optoelectronic properties. The gapless nature of its 3D electronic band facilitates strong optical nonlinearity and supports Dirac plasmons that are of particular interest to realize high-performance electronic and photonic devices at terahertz (1 THz = 4.1 meV) frequencies, where the performance of most dynamic materials are limited by the tradeoff between power-efficiency and switching speed. Here, all-optical, low-power, ultrafast broadband modulation of terahertz waves using an ultrathin film (100 nm, λ/3000) of Cd3As2 are experimentally demonstrated through active tailoring of the photoconductivity. The measurements reveal the photosensitive metallic behavior of Cd3As2 with high terahertz electron mobility of 7200 cm2 (Vs)−1. In addition, optical fluence dependent ultrafast charge carrier relaxation (15.5 ps), terahertz mobility, and long momentum scattering time (157 fs) comparable to superconductors that invoke kinetic inductance at terahertz frequencies are demonstrated. These remarkable properties of 3D Dirac topological semimetal envision a new class of power-efficient, high speed, compact, tunable electronic, and photonic devices.  相似文献   

10.
Herein, a novel D4 symmetrical redox-active ligand tetrathia[8]circulene-2,3,5,6,8,9,11,12-octaol (8OH-TTC) is designed and synthesized, which coordinates with Ni2+ ions to construct a 2D conductive metal-organic framework (2D c-MOF) named Ni-TTC. Ni-TTC exhibits typical semiconducting properties with electrical conductivity up to ≈1.0 S m−1 at 298 K. Furthermore, magnetism measurements show the paramagnetic property of Ni-TTC with strong antiferromagnetic coupling due to the presence of semiquinone ligand radicals and Ni2+ sites. In virtue of its decent electrical conductivity and good redox activity, the gravimetric capacitance of Ni-TTC is up to 249 F g−1 at a discharge rate of 0.2 A g−1, which demonstrates the potential of tetrathia[8]circulene-based redox-active 2D c-MOFs in energy storage applications.  相似文献   

11.
As the fresh blood of 2D family, non-layered 2D materials (2DNLMs) have demonstrated great potential in the application of next-generation optoelectronic devices. However, stemming from the weak light absorption brought by atomically thin thickness and the interfacial recombination brought by surface dangling bonds, traditional 2DNLM photodetectors are always accompanied by limited performance. Herein, a structure that integrates Si nanopillar array and non-layered 2D In2S3 to construct an ultrasensitive photodetector is designed. In particular, periodically Si nanopillars can act as Fabry–Pérot-enhanced Mie resonators that can effectively control and enhance the light absorption of 2D In2S3. On the other hand, a vertical built-in electric field is introduced in the In2S3 channel to capture photogenerated holes and leave electrons recycling in In2S3, obtaining a high photogain. Benefiting from these two mechanisms, this proposed photodetector presents a high responsivity of 4812 A W−1 and short rise/decay time of 5.2/4.0 ms at the wavelength of 405 nm. Especially, a high light on–off ratio greater than 106 and a record-high detectivity of 5.4 × 1015 Jones are achieved, representing one of the most sensitive photodetectors based on 2D materials. This deliberate device design concept suggests an effective scheme to construct high-performance 2DNLM optoelectronic devices.  相似文献   

12.
Facing the future development trend of miniaturization and intelligence of electronic devices, solar-blind photodetectors based on ultrawide-bandgap 2D semiconductors have the advantages of low dark current, and high signal-to-noise ratio, as well as the features of micro-nanometer miniaturization and multi-functionalization of 2D material devices, which have potential applications in the photoelectric sensor part of high-performance machine vision systems. This study reports a 2D oxide semiconductor, AsSbO3, with an ultrawide bandgap (4.997 eV for monolayer and 4.4 eV for multilayer) to be used to fabricate highly selective solar-blind UV photodetectors, of which the dark current as low as 100 fA and rejection ratio of UV-C and UV-A reaches 7.6 × 103. Under 239 nm incident light, the responsivity is 105 mA W−1 and the detectivity is 7.58 × 1012 Jones. Owing to the remarkable anisotropic crystal structure, AsSbO3 also shows significant linear dichroism and nonlinear optical properties. Finally, a simple machine vision system is simulated by combining the real-time imaging function in solar-blind UV with a convolutional neural network. This study enriches the material system of ultrawide-bandgap 2D semiconductors and provides insight into the future development of high-performance solar-blind UV optoelectronic devices.  相似文献   

13.
This research demonstrates a state-of-the-art vertical-transport photodetector with an n-type 3D MAPbI3/p-type quasi-2D (Q-2D) BA2MA2Pb3I10 perovskite heterojunction. This structure introduces a ≈0.6 V built-in electric field at the n-p junction that greatly improves the characteristics of the perovskite photodetector, and the presence of Q-2D perovskite on the surface improves the life. The electrical polarities of the 3D and the Q-2D perovskite layers are simply controlled by self-constituent doping, making clearly defined n-p characteristics. Doctor-blade coating is used to fabricate the photodetector with a large area. The Q-2D materials with highly oriented (040) Q-2D (n = 2,3) planes are near the surface, and the (111) preferred planes mixed with high index Q-2D materials (n = 4,5) are found near the 3D/Q-2D interface. The stacking and interface are beneficial for carrier extraction and transport, yielding an external quantum efficiency of 77.9%, a carrier lifetime long as 295.7 ns, and a responsibility of 0.41 A W−1. A low dark current density of 6.2 × 10−7 mA cm−2 and a high detectivity of 2.82 × 1013 Jones are obtained. Rise time and fall time are fast as 1.33 and 10.1 µs, respectively. The results show the application potential of 3D/Q-2D n-p junction perovskite photodetectors.  相似文献   

14.
2D magnetic materials with dimerized honeycomb lattices can be treated as mixed-spin square lattices, in which a quantum phase transition may occur to realize the Bose–Einstein condensation of magnons under reachable experimental conditions. However, this has never been successfully realized with integer spin centers. Herein, a spin integer (S = 2) dimerized honeycomb lattice in an iron(II)-azido compound [Fe(4-etpy)2(N3)2]n (FEN, 4-etpy = 4-ethylpyridine) is realized. Morphology characterization by transmission electron microscopy, scanning electron microscopy, and atomic force microscopy spectroscopies show that the thinnest place of the sample is ≈13 nm, which is equal to ten layers of the compound. In contrast to the common magnetic properties of long-range magnetic ordering, Mössbauer and polarized neutron scattering studies reveal that FEN exhibits a reentrant spin glass behavior owing to competing ferro- and antiferromagnetic exchange-coupling interactions within the lattice. Two spin glass phases with disparate canting angles are characterized at 39 and 28 K, respectively. By using Curély's model, two exchange-coupling constants (J1 = +35.8 cm−1 and J2 = −3.7 cm−1) can be simulated. Moreover, a very large coercive field of ≈1.9 Tesla is observed at 2 K, making FEN a “very hard” van der Waals 2D magnetic material.  相似文献   

15.
2D piezoelectric materials such as transition metal dichalcogenides are attracting significant attention because they offer various benefits over bulk piezoelectrics. In this work, the fabrication of layered biomolecular crystals of diphenylalanine (FF) obtained via a co-assembly of l,l - and d,d - enantiomers of FF monomers is reported. Their crystal structure, thermal and chemical stabilities, and piezoelectric properties are investigated. Single crystal X-ray diffraction results show that FF enantiomers are arranged in the form of bilayers consisting of monomers with alternating chirality packed into a tape-like monoclinic structure belonging to a polar space group P21. Each bilayer ( ≈ 1.5 nm thick) demonstrates strong out-of-plane piezoelectricity (d33  ≈  20 pm V−1) that is almost an order of magnitude higher than in the archetypical piezoelectric material quartz. The grown crystals demonstrate better thermal and chemical stabilities than self-assembled hexagonal FF nanotubes studied in the past. Piezoelectric bilayers, being held via weak aromatic interaction in the bulk crystals, can be exfoliated by mechanical or chemical methods, thus resulting in a 2D piezoelectric material, which can find various applications in biocompatible and ecologically friendly electromechanical microdevices, such as sensors, actuators, and energy harvesting elements used in implantable and wearable electronics.  相似文献   

16.
Even though atomically thin 2D semiconductors have shown great potential for next-generation electronics, the low carrier mobility caused by poor metal–semiconductor contacts and the inherently high density of impurity scatterings remains a critical issue. Herein, high-mobility field-effect transistors (FETs) by introducing few-layer PdSe2 flakes as channels is achieved, via directly depositing semimetal antimony (Sb) as drain–source electrodes. The formation of clean and defect-free van der Waals (vdW) stackings at the Sb–PdSe2 heterointerfaces boosts the room temperature transport characteristics, including low contact resistance down to 0.55 kΩ µm, high on-current density reaching 96 µA µm−1, and high electron mobility of 383 cm2 V−1 s−1. Furthermore, metal–insulator transition (MIT) is observed in the PdSe2 FETs with and without hexagonal boron nitride (h–BN) as buffer layers. However, the layered h–BN/PdSe2 vdW stacking eliminates the interference of interfacial disorders, and thus the corresponding device exhibits a lower MIT crossing point, larger mobility exponent of γ ∼ 1.73, significantly decreased hopping parameter of T0, and ultrahigh electron mobility of 2,184 cm2 V−1 s−1 at 10 K. These findings are expected to be significant for developing high mobility 2D-based quantum devices.  相似文献   

17.
Ferroelectricity and X-ray detection property have been recently implemented for the first time in hybrid bromide double perovskites. It sheds a light on achieving photosensitive and ferroelectric multifunctional materials based on 2D lead-free hybrid halide double perovskites. However, the low Tc, small Ps, and relatively low X-ray sensitivity in the reported bromide double perovskites hinder practical applications. Herein, the authors demonstrate a novel 2D lead-free iodide double perovskite (4,4-difluoropiperidinium)4AgBiI8 (1) for high-performance X-ray sensitive ferroelectric devices. Centimeter-sized single crystal of 1 is obtained and exhibits an excellent ferroelectricity including a high Tc up to 422 K and a large Ps of 10.5 μC cm−2. Moreover, due to a large X-ray attenuation and efficient charge carrier mobility (μ)–charge carrier lifetime (τ) product, the crystal 1 also exhibits promising X-ray response with a high sensitivity up to 188 μC·Gyair−1 cm−2 and a detection limit below 3.13 μGyair·s−1. Therefore, this finding is a step further toward practical applications of lead-free halide perovskite in high-performance photoelectronic devices. It will afford a promising platform for exploring novel photosensitive ferroelectric multifunctional materials based on lead-free double perovskites.  相似文献   

18.
Optoelectronic performance of 2D transition metal dichalcogenides (TMDs)-based solar cells and self-powered photodetectors remain limited due to fabrication challenges, such as difficulty in doping TMDs to form p–n junctions. Herein, MoS2 diodes based on geometrically asymmetric contact areas are shown to achieve a high current rectification ratio of ≈105, facilitating efficient photovoltaic charge collection. Under solar illumination, the device demonstrates a high open-circuit voltage (Voc) of 430 mV and a short-circuit current density (Jsc) of −13.42 mA cm−2, resulting in a high photovoltaic power conversion efficiency (PCE) of 3.16%, the highest reported for a lateral 2D solar cell. The diodes also show a high photoresponsivity of 490.3 mA W−1, and a large photo detectivity of 4.05 × 1010 Jones, along with a fast response time of 0.8 ms under 450 nm wavelength at zero bias for self-powered photodetection applications. The device transferred on a flexible substrate shows a high photocurrent and PCE retentions of 94.4%, and 88.2% after 5000 bending cycles at a bending radius of 1.5 cm, respectively, demonstrating robustness for flexible optoelectronic applications. The simple fabrication process, superior photovoltaic properties, and high flexibility suggests that the geometrically asymmetric MoS2 device architecture is an excellent candidate for flexible photovoltaic and optoelectronic applications.  相似文献   

19.
Electronic devices based on 2D materials have exhibited outstanding figures of merit. However, the fabrication of 2D diodes still relies on manual or semi-automated handling processing. To unleash their commercial potential, the integration of 2D materials into a fully-automated fabrication line is a critical step. Here, the focused ion-beam writing as an automated approach to construct lateral diodes on a 2D heterostructure (MoSe2/G) consisting of graphene and MoSe2 is elucidated. Se-defects generated by focused ion writing endow the 2D heterostructure with unique electronic properties, which allows for the construction of the barrier at the boundary of the writing and non-writing region. Benefiting from this feature, the ion-beam-written heterostructure is used to realize rectifying and current regulating diodes. Exhibiting comparable performance to traditional diodes, the rectifying diode has a rectification ratio of ≈104, while the current regulative diode has a dynamic resistance larger than 4.5 MΩ. Furthermore, to illustrate practical applications of these diodes in digital logic electronics, AND and OR logic gates are directly inscribed on the heterostructure by ion beams. This work demonstrates focused ion-beam writing as an additional strategy for direct-writing of 2D diodes on graphene-based heterostructures.  相似文献   

20.
2D perovskite is an organic–inorganic hybrid material with good photoelectric properties, generally prepared by using organic groups as isolation molecules. In this study, using manganese chloride and potassium halide as raw materials, all-inorganic 2D lead-free perovskites are prepared by the Bridgeman melting and cooling method. Different from the 2D perovskites synthesized by organic spacer molecules, the prepared all-inorganic 2D perovskites have smaller layer spacings and good crystallization performance due to the use of potassium halide as spacer molecules. They are direct bandgap semiconductors and their energy bandgaps are tuned by the different types of potassium halides. High degree orientation crystal thin films with (001) lattice plane parallel to silicon wafer substrate are prepared by double-source evaporation. The physical morphology of the films is characterized by grazing angle X-ray diffraction, transmission electron microscopy, and electron diffraction. The field effect transistors prepared from these 2D films show excellent electronic characteristics. The mobility of the optimized device is ≈24 cm2 v−1 s−1 and the on/off ratio reaches 105. This study reveals the potential of lead-free manganese 2D perovskite as a high-performance perovskite field effect transistor.  相似文献   

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