Ionic Liquid Gating Control of Spin Reorientation Transition and Switching of Perpendicular Magnetic Anisotropy

Electric field (E‐field) modulation of perpendicular magnetic anisotropy (PMA) switching, in an energy‐efficient manner, is of great potential to realize magnetoelectric (ME) memories and other ME devices. Voltage control of the spin‐reorientation transition (SRT) that allows the magnetic moment rotating between the out‐of‐plane and the in‐plane direction is thereby crucial. In this work, a remarkable magnetic anisotropy field change up to 1572 Oe is achieved under a small operation voltage of 4 V through ionic liquid (IL) gating control of SRT in Au/[DEME]⁺[TFSI]^?/Pt/(Co/Pt)₂/Ta capacitor heterostructures at room temperature, corresponding to a large ME coefficient of 378 Oe V^?1. As revealed by both ferromagnetic resonance measurements and magnetic domain evolution observation, the magnetization can be switched stably and reversibly between the out‐of‐plane and in‐plane directions via IL gating. The key mechanism, revealed by the first‐principles calculation, is that the IL gating process influences the interfacial spin–orbital coupling as well as net Rashba magnetic field between the Co and Pt layers, resulting in the modulation of the SRT and in‐plane/out‐of‐plane magnetization switching. This work demonstrates a unique IL‐gated PMA with large ME tunability and paves a way toward IL gating spintronic/electronic devices such as voltage tunable PMA memories.     

Spin‐Orbit Torque Switching of a Nearly Compensated Ferrimagnet by Topological Surface States

Utilizing spin‐orbit torque (SOT) to switch a magnetic moment provides a promising route for low‐power‐dissipation spintronic devices. Here, the SOT switching of a nearly compensated ferrimagnet Gd_x(FeCo)_1?x by the topological insulator [Bi₂Se₃ and (BiSb)₂Te₃] is investigated at room temperature. The switching current density of (BiSb)₂Te₃ (1.20 × 10⁵ A cm^?2) is more than one order of magnitude smaller than that in conventional heavy‐metal‐based structures, which indicates the ultrahigh efficiency of charge‐spin conversion (>1) in topological surface states. By tuning the net magnetic moment of Gd_x(FeCo)_1?x via changing the composition, the SOT efficiency has a significant enhancement (6.5 times) near the magnetic compensation point, and at the same time the switching speed can be as fast as several picoseconds. Combining the topological surface states and the nearly compensated ferrimagnets provides a promising route for practical energy‐efficient and high‐speed spintronic devices.     

Structural Phase Transition Effect on Resistive Switching Behavior of MoS2‐Polyvinylpyrrolidone Nanocomposites Films for Flexible Memory Devices

The 2H phase and 1T phase coexisting in the same molybdenum disulfide (MoS₂) nanosheets can influence the electronic properties of the materials. The 1T phase of MoS₂ is introduced into the 2H‐MoS₂ nanosheets by two‐step hydrothermal synthetic methods. Two types of nonvolatile memory effects, namely write‐once read‐many times memory and rewritable memory effect, are observed in the flexible memory devices with the configuration of Al/1T@2H‐MoS₂‐polyvinylpyrrolidone (PVP)/indium tin oxide (ITO)/polyethylene terephthalate (PET) and Al/2H‐MoS₂‐PVP/ITO/PET, respectively. It is observed that structural phase transition in MoS₂ nanosheets plays an important role on the resistive switching behaviors of the MoS₂‐based device. It is hoped that our results can offer a general route for the preparation of various promising nanocomposites based on 2D nanosheets of layered transition metal dichalcogenides for fabricating the high performance and flexible nonvolatile memory devices through regulating the phase structure in the 2D nanosheets.     

Tailoring MoS2 Valley‐Polarized Photoluminescence with Super Chiral Near‐Field

Transition metal dichalcogenides with intrinsic spin–valley degrees of freedom hold great potentials for applications in spintronic and valleytronic devices. MoS₂ monolayer possesses two inequivalent valleys in the Brillouin zone, with each valley coupling selectively with circularly polarized photons. The degree of valley polarization (DVP) is a parameter to characterize the purity of valley‐polarized photoluminescence (PL) of MoS₂ monolayer. Usually, the detected values of DVP in MoS₂ monolayer show achiral property under optical excitation of opposite helicities due to reciprocal phonon‐assisted intervalley scattering process. Here, it is reported that valley‐polarized PL of MoS₂ can be tailored through near‐field interaction with plasmonic chiral metasurface. The resonant field of the chiral metasurface couples with valley‐polarized excitons, and tailors the measured PL spectra in the far‐field, resulting in observation of chiral DVP of MoS₂‐metasurface under opposite helicities excitations. Valley‐contrast PL in the chiral heterostructure is also observed when illuminated by linearly polarized light. The manipulation of valley‐polarized PL in 2D materials using chiral metasurface represents a viable route toward valley‐polaritonic devices.     

Direct Growth of High Mobility and Low‐Noise Lateral MoS2–Graphene Heterostructure Electronics

Reliable fabrication of lateral interfaces between conducting and semiconducting 2D materials is considered a major technological advancement for the next generation of highly packed all‐2D electronic circuitry. This study employs seed‐free consecutive chemical vapor deposition processes to synthesize high‐quality lateral MoS₂–graphene heterostructures and comprehensively investigated their electronic properties through a combination of various experimental techniques and theoretical modeling. These results show that the MoS₂–graphene devices exhibit an order of magnitude higher mobility and lower noise metrics compared to conventional MoS₂–metal devices as a result of energy band rearrangement and smaller Schottky barrier height at the contacts. These findings suggest that MoS₂–graphene in‐plane heterostructures are promising materials for the scale‐up of all‐2D circuitry with superlative electrical performance.     

Synthesis of Co-Doped MoS2 Monolayers with Enhanced Valley Splitting

Internal magnetic moments induced by magnetic dopants in MoS₂ monolayers are shown to serve as a new means to engineer valley Zeeman splitting (VZS). Specifically, successful synthesis of monolayer MoS₂ doped with the magnetic element Co is reported, and the magnitude of the valley splitting is engineered by manipulating the dopant concentration. Valley splittings of 3.9, 5.2, and 6.15 meV at 7 T in Co-doped MoS₂ with Co concentrations of 0.8%, 1.7%, and 2.5%, respectively, are achieved as revealed by polarization-resolved photoluminescence (PL) spectroscopy. Atomic-resolution electron microscopy studies clearly identify the magnetic sites of Co substitution in the MoS₂ lattice, forming two distinct types of configurations, namely isolated single dopants and tridopant clusters. Density functional theory (DFT) and model calculations reveal that the observed enhanced VZS arises from an internal magnetic field induced by the tridopant clusters, which couples to the spin, atomic orbital, and valley magnetic moment of carriers from the conduction and valence bands. The present study demonstrates a new method to control the valley pseudospin via magnetic dopants in layered semiconducting materials, paving the way toward magneto-optical and spintronic devices.     

Magnetic Proximity Effect in Graphene/CrBr3 van der Waals Heterostructures

2D van der Waals heterostructures serve as a promising platform to exploit various physical phenomena in a diverse range of novel spintronic device applications. Efficient spin injection is the prerequisite for these devices. The recent discovery of magnetic 2D materials leads to the possibility of fully 2D van der Waals spintronics devices by implementing spin injection through the magnetic proximity effect (MPE). Here, the investigation of MPE in 2D graphene/CrBr₃ van der Waals heterostructures is reported, which is probed by the Zeeman spin Hall effect through non-local measurements. Quantitative estimation of the Zeeman splitting field demonstrates a significant MPE field even in a low magnetic field. Furthermore, the observed anomalous longitudinal resistance changes at the Dirac point R_XX,D with increasing magnetic field near ν = 0 may be attributed to the MPE-induced new ground state phases. This MPE revealed in the graphene/CrBr₃ van der Waals heterostructures therefore provides a solid physics basis and key functionality for next-generation 2D spin logic and memory devices.     

Gap‐Mode Surface‐Plasmon‐Enhanced Photoluminescence and Photoresponse of MoS2

2D materials hold great potential for designing novel electronic and optoelectronic devices. However, 2D material can only absorb limited incident light. As a representative 2D semiconductor, monolayer MoS₂ can only absorb up to 10% of the incident light in the visible, which is not sufficient to achieve a high optical‐to‐electrical conversion efficiency. To overcome this shortcoming, a “gap‐mode” plasmon‐enhanced monolayer MoS₂ fluorescent emitter and photodetector is designed by squeezing the light‐field into Ag shell‐isolated nanoparticles–Au film gap, where the confined electromagnetic field can interact with monolayer MoS₂. With this gap‐mode plasmon‐enhanced configuration, a 110‐fold enhancement of photoluminescence intensity is achieved, exceeding values reached by other plasmon‐enhanced MoS₂ fluorescent emitters. In addition, a gap‐mode plasmon‐enhanced monolayer MoS₂ photodetector with an 880% enhancement in photocurrent and a responsivity of 287.5 A W^?1 is demonstrated, exceeding previously reported plasmon‐enhanced monolayer MoS₂ photodetectors.     

Engineering Chemically Active Defects in Monolayer MoS2 Transistors via Ion‐Beam Irradiation and Their Healing via Vapor Deposition of Alkanethiols

Irradiation of 2D sheets of transition metal dichalcogenides with ion beams has emerged as an effective approach to engineer chemically active defects in 2D materials. In this context, argon‐ion bombardment has been utilized to introduce sulfur vacancies in monolayer molybdenum disulfide (MoS₂). However, a detailed understanding of the effects of generated defects on the functional properties of 2D MoS₂ is still lacking. In this work, the correlation between critical electronic device parameters and the density of sulfur vacancies is systematically investigated through the fabrication and characterization of back‐gated monolayer MoS₂ field‐effect transistors (FETs) exposed to a variable fluence of low‐energy argon ions. The electrical properties of pristine and ion‐irradiated FETs can be largely improved/recovered by exposing the devices to vapors of short linear thiolated molecules. Such a solvent‐free chemical treatment—carried out strictly under inert atmosphere—rules out secondary healing effects induced by oxygen or oxygen‐containing molecules. The results provide a guideline to design monolayer MoS₂ optoelectronic devices with a controlled density of sulfur vacancies, which can be further exploited to introduce ad hoc molecular functionalities by means of thiol chemistry approaches.     

Ultrathin Magnetic 2D Single‐Crystal CrSe

2D magnetic materials have generated an enormous amount of attention due to their unique 2D‐limited magnetism and their potential applications in spintronic devices. Recently, most of this research has focused on 2D van der Waals layered magnetic materials exfoliated from the bulk with random size and thicknesses. Controllable growth of these materials is still a great challenge. In contrast, 2D nonlayered magnetic materials have rarely been investigated, not especially regarding their preparation. Cr_nX (X = S, Se and Te; 0 < n < 1), a class of nonlayered transition metal dichalcogenides, has rapidly attracted extensive attention due to its abundance of structural compounds and unique magnetic properties. Herein, the controlled synthesis of ultrathin CrSe crystals, with grain size reaching the sub‐millimeter scale, on mica substrates via an ambient pressure chemical vapor deposition (CVD) method is demonstrated. A continuous CrSe film can also be achieved via precise control of the key growth parameters. Importantly, the CVD‐grown 2D CrSe crystals possess obvious ferromagnetic properties at temperatures below 280 K, which has not been observed experimentally before. This work broadens the scope of the CVD growth of 2D magnetic materials and highlights their significant application possibilities in spintronics.     

High Coercivity and Magnetization in WSe2 by Codoping Co and Nb

Introducing ferromagnetism in transition metal dichalcogenides has attracted lots of attention due to the possible applications in spintronics devices. Generally, single magnetic element doping is used to introduce magnetism. However, mostly, weak ferromagnetism is observed. In this work, codoping of two kinds of transition metals (Nb and Co) into WSe₂ is used to study its magnetic properties. In detail, single crystal WSe₂ is codoped with 4 at% Co and various concentrations of Nb by employing the physical ion implantation method. Raman, X‐ray diffraction and X‐ray photoelectron spectroscopy results reveal the effective substitutional doping of implanted elements (Co and Nb). Magnetic measurements illustrate that both un‐doped and 4 at% Co doped WSe₂ show weak ferromagnetism whereas magnetization is strongly enhanced when Co and Nb are codoped into WSe₂. The magnetization is comparable with a ferromagnet, which may be attributed to Co, Nb doping and defects. In addition, a large coercivity of ≈1.2 kOe is observed in the 1 at% Nb–4 at% Co codoped WSe₂ sample, which may be ascribed to the combined effect of doping‐induced stress, defect‐dictated pinning and anisotropy of Nb? Se bond owing to the charge transfer between Nb and Se ions.     

Enhanced Photocarrier Generation with Selectable Wavelengths by M‐Decorated‐CuInS2 Nanocrystals (M = Au and Pt) Synthesized in a Single Surfactant Process on MoS2 Bilayers

A facile approach for the synthesis of Au‐ and Pt‐decorated CuInS₂ nanocrystals (CIS NCs) as sensitizer materials on the top of MoS₂ bilayers is demonstrated. A single surfactant (oleylamine) is used to prepare such heterostructured noble metal decorated CIS NCs from the pristine CIS. Such a feasible way to synthesize heterostructured noble metal decorated CIS NCs from the single surfactant can stimulate the development of the functionalized heterostructured NCs in large scale for practical applications such as solar cells and photodetectors. Photodetectors based on MoS₂ bilayers with the synthesized nanocrystals display enhanced photocurrent, almost 20–40 times higher responsivity and the On/Off ratio is enlarged one order of magnitude compared with the pristine MoS₂ bilayers‐based photodetectors. Remarkably, by using Pt‐ or Au‐decorated CIS NCs, the photocurrent enhancement of MoS₂ photodetectors can be tuned between blue (405 nm) to green (532 nm). The strategy described here acts as a perspective to significantly improve the performance of MoS₂‐based photodetectors with the controllable absorption wavelengths in the visible light range, showing the feasibility of the possible color detection.     

Ultrathin Transition Metal Dichalcogenide/3d Metal Hydroxide Hybridized Nanosheets to Enhance Hydrogen Evolution Activity

The vast majority of the reported hydrogen evolution reaction (HER) electrocatalysts perform poorly under alkaline conditions due to the sluggish water dissociation kinetics. Herein, a hybridization catalyst construction concept is presented to dramatically enhance the alkaline HER activities of catalysts based on 2D transition metal dichalcogenides (TMDs) (MoS₂ and WS₂). A series of ultrathin 2D‐hybrids are synthesized via facile controllable growth of 3d metal (Ni, Co, Fe, Mn) hydroxides on the monolayer 2D‐TMD nanosheets. The resultant Ni(OH)₂ and Co(OH)₂ hybridized ultrathin MoS₂ and WS₂ nanosheet catalysts exhibit significantly enhanced alkaline HER activity and stability compared to their bare counterparts. The 2D‐MoS₂/Co(OH)₂ hybrid achieves an extremely low overpotential of ≈128 mV at 10 mA cm^?2 in 1 m KOH. The combined theoretical and experimental studies confirm that the formation of the heterostructured boundaries by suitable hybridization of the TMD and 3d metal hydroxides is responsible for the improved alkaline HER activities because of the enhanced water dissociation step and lowers the corresponding kinetic energy barrier by the hybridized 3d metal hydroxides.     

MoS2/Rubrene van der Waals Heterostructure: Toward Ambipolar Field‐Effect Transistors and Inverter Circuits

2D transition metal dichalcogenides are promising channel materials for the next‐generation electronic device. Here, vertically 2D heterostructures, so called van der Waals solids, are constructed using inorganic molybdenum sulfide (MoS₂) few layers and organic crystal – 5,6,11,12‐tetraphenylnaphthacene (rubrene). In this work, ambipolar field‐effect transistors are successfully achieved based on MoS₂ and rubrene crystals with the well balanced electron and hole mobilities of 1.27 and 0.36 cm² V^?1 s^?1, respectively. The ambipolar behavior is explained based on the band alignment of MoS₂ and rubrene. Furthermore, being a building block, the MoS₂/rubrene ambipolar transistors are used to fabricate CMOS (complementary metal oxide semiconductor) inverters that show good performance with a gain of 2.3 at a switching threshold voltage of ?26 V. This work paves a way to the novel organic/inorganic ultrathin heterostructure based flexible electronics and optoelectronic devices.     

Atomic‐Level Customization of 4 in. Transition Metal Dichalcogenide Multilayer Alloys for Industrial Applications

Despite many encouraging properties of transition metal dichalcogenides (TMDs), a central challenge in the realm of industrial applications based on TMD materials is to connect the large‐scale synthesis and reproducible production of highly crystalline TMD materials. Here, the primary aim is to resolve simultaneously the two inversely related issues through the synthesis of MoS_{2(1?x )}Se_2x ternary alloys with customizable bichalcogen atomic (S and Se) ratio via atomic‐level substitution combined with a solution‐based large‐area compatible approach. The relative concentration of bichalcogen atoms in the 2D alloy can be effectively modulated by altering the selenization temperature, resulting in 4 in. scale production of MoS_1.62Se_0.38, MoS_1.37Se_0.63, MoS_1.15Se_0.85, and MoS_0.46Se_1.54 alloys, as well as MoS₂ and MoSe₂. Comprehensive spectroscopic evaluations for vertical and lateral homogeneity in terms of heteroatom distribution in the large‐scale 2D TMD alloys are implemented. Se‐stimulated strain effects and a detailed mechanism for the Se substitution in the MoS₂ crystal are further explored. Finally, the capability of the 2D alloy for industrial application in nanophotonic devices and hydrogen evolution reaction (HER) catalysts is validated. Substantial enhancements in the optoelectronic and HER performances of the 2D ternary alloy compared with those of its binary counterparts, including pure‐phase MoS₂ and MoSe₂, are unambiguously achieved.     

Molybdenum Disulfide Nanosheet/Quantum Dot Dynamic Memristive Structure Driven by Photoinduced Phase Transition

MoS₂ 2D nanosheets (NS) with intercalated 0D quantum dots (QDs) represent promising structures for creating low‐dimensional (LD) resistive memory devices. Nonvolatile memristors based 2D materials demonstrate low power consumption and ultrahigh density. Here, the observation of a photoinduced phase transition in the 2D NS/0D QDs MoS₂ structure providing dynamic resistive memory is reported. The resistive switching of the MoS₂ NS/QD structure is observed in an electric field and can be controlled through local QD excitations. Photoexcitation of the LD structure at different laser power densities leads to a reversible MoS₂ 2H‐1T phase transition and demonstrates the potential of the LD structure for implementing a new dynamic ultrafast photoresistive memory. The dynamic LD photomemristive structure is attractive for real‐time pattern recognition and photoconfiguration of artificial neural networks in a wide spectral range of sensitivity provided by QDs.     

Lowering the Schottky Barrier Height by Graphene/Ag Electrodes for High‐Mobility MoS2 Field‐Effect Transistors

2D transition metal dichalcogenides (TMDCs) have emerged as promising candidates for post‐silicon nanoelectronics owing to their unique and outstanding semiconducting properties. However, contact engineering for these materials to create high‐performance devices while adapting for large‐area fabrication is still in its nascent stages. In this study, graphene/Ag contacts are introduced into MoS₂ devices, for which a graphene film synthesized by chemical vapor deposition (CVD) is inserted between a CVD‐grown MoS₂ film and a Ag electrode as an interfacial layer. The MoS₂ field‐effect transistors with graphene/Ag contacts show improved electrical and photoelectrical properties, achieving a field‐effect mobility of 35 cm² V^?1 s^?1, an on/off current ratio of 4 × 10⁸, and a photoresponsivity of 2160 A W^?1, compared to those of devices with conventional Ti/Au contacts. These improvements are attributed to the low work function of Ag and the tunability of graphene Fermi level; the n‐doping of Ag in graphene decreases its Fermi level, thereby reducing the Schottky barrier height and contact resistance between the MoS₂ and electrodes. This demonstration of contact interface engineering with CVD‐grown MoS₂ and graphene is a key step toward the practical application of atomically thin TMDC‐based devices with low‐resistance contacts for high‐performance large‐area electronics and optoelectronics.     

Potential 2D Materials with Phase Transitions: Structure,Synthesis, and Device Applications

Layered materials with phase transitions, such as charge density wave (CDW) and magnetic and dipole ordering, have potential to be exfoliated into monolayers and few‐layers and then become a large and important subfamily of two‐dimensional (2D) materials. Benefitting from enriched physical properties from the collective interactions, long‐range ordering, and related phase transitions, as well as the atomic thickness yet having nondangling bonds on the surface, 2D phase‐transition materials have vast potential for use in new‐concept and functional devices. Here, potential 2D phase‐transition materials with CDWs and magnetic and dipole ordering, including transition metal dichalcogenides, transition metal halides, metal thio/selenophosphates, chromium silicon/germanium tellurides, and more, are introduced. The structures and experimental phase‐transition properties are summarized for the bulk materials and some of the obtained monolayers. In addition, recent experimental progress on the synthesis and measurement of monolayers, such as 1T‐TaS₂, CrI₃, and Cr₂Ge₂Te₆, is reviewed.     

Threshold Voltage Control of Multilayered MoS2 Field‐Effect Transistors via Octadecyltrichlorosilane and their Applications to Active Matrixed Quantum Dot Displays Driven by Enhancement‐Mode Logic Gates

In recent past, for next‐generation device opportunities such as sub‐10 nm channel field‐effect transistors (FETs), tunneling FETs, and high‐end display backplanes, tremendous research on multilayered molybdenum disulfide (MoS₂) among transition metal dichalcogenides has been actively performed. However, nonavailability on a matured threshold voltage control scheme, like a substitutional doping in Si technology, has been plagued for the prosperity of 2D materials in electronics. Herein, an adjustment scheme for threshold voltage of MoS₂ FETs by using self‐assembled monolayer treatment via octadecyltrichlorosilane is proposed and demonstrated to show MoS₂ FETs in an enhancement mode with preservation of electrical parameters such as field‐effect mobility, subthreshold swing, and current on–off ratio. Furthermore, the mechanisms for threshold voltage adjustment are systematically studied by using atomic force microscopy, Raman, temperature‐dependent electrical characterization, etc. For validation of effects of threshold voltage engineering on MoS₂ FETs, full swing inverters, comprising enhancement mode drivers and depletion mode loads are perfectly demonstrated with a maximum gain of 18.2 and a noise margin of ≈45% of 1/2 V_DD. More impressively, quantum dot light‐emitting diodes, driven by enhancement mode MoS₂ FETs, stably demonstrate 120 cd m^?2 at the gate‐to‐source voltage of 5 V, exhibiting promising opportunities for future display application.     

Synthesis of Ultrahigh‐Quality Monolayer Molybdenum Disulfide through In Situ Defect Healing with Thiol Molecules

Monolayer transition metal dichalcogenides are 2D materials with many potential applications. Chemical vapor deposition (CVD) is a promising method to synthesize these materials. However, CVD‐grown materials generally have poorer quality than mechanically exfoliated ones and contain more defects due to the difficulties in controlling precursors' distribution and concentration during growth where solid precursors are used. Here, thiol is proposed to be used as a liquid precursor for CVD growth of high quality and uniform 2D MoS₂. Atomic‐resolved structure characterizations indicate that the concentration of sulfur vacancies in the MoS₂ grown from thiol is the lowest among all reported CVD samples. Low temperature spectroscopic characterization further reveals the ultrahigh optical quality of the grown MoS₂. Density functional theory simulations indicate that thiol molecules could interact with sulfur vacancies in MoS₂ and repair these defects during the growth of MoS₂, resulting in high‐quality MoS₂. This work provides a facile and controllable method for the growth of high‐quality 2D materials with ultralow sulfur vacancies and high optical quality, which will benefit their optoelectronic applications.