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Two-dimensional (2D) magnetic materials provide an ideal platform for spintronics, magnetoelectrics, and numerous intriguing physical phenomena in 2D limits. Moiré superlattices based on 2D magnets offer an avenue for controlling the spin degree of freedom and engineering magnetic properties. However, the synthesis of high-quality, large-grain, and stable 2D magnets, much less obtaining a magnetic moiré superlattice, is still challenging. We synthesize 2D ferromagnets (trigonal Cr

Niobium diselenide (NbSe2) is a layered transition metal dichalcogenide with novel quantum phases at low temperatures (T) such as superconductivity and charge density wave order. While its electronic correlations and the interaction between electrons and other collective modes have been explored extensively, a detailed study of the transport behavior of photo-excited charge carriers still remains elusive. Here, we report a systematic investigation of the photoresponse generated in homogenous NbSe2 nano-flakes near the superconducting critical temperature (Tc). By combining scanning photocurrent microscopy and classic photoconductivity measurements, three distinctive mechanisms of the photoresponse are established, including the band bending at the NbSe2–metal junction, the perturbation of the superconducting state, and the photo-bolometric effect. Among them, the photo-induced phase transition from the superconducting to normal state results in an extremely large photocurrent, which is tunable by the bias voltage and is consistent with the observation via the electrical transport characterization. The photoresponsivity of our device reaches 42.3 A/W, and the response time is less than 2 μs at T = 3.8 K for an excitation in the visible wavelength, whose performance could be further improved by optimizing the device design and the experimental condition. Our result sheds light on ultrasensitive broadband photodetection with atomically thin NbSe2 and points to a potential means of probing the correlated electronic phases by exploring light–matter interactions.

The recent discovery of magnetism in atomically thin layers of van der Waals (vdW) crystals has created new opportunities for exploring magnetic phenomena in the two-dimensional (2D) limit. In most 2D magnets studied to date, the c-axis is an easy axis, so that at zero applied field the polarization of each layer is perpendicular to the plane. Here, we demonstrate that atomically thin CrCl

The recent discovery of magnetism in atomically thin layers of van der Waals (vdW) crystals has created new opportunities for exploring magnetic phenomena in the two-dimensional (2D) limit. In most 2D magnets studied to date, the c-axis is an easy axis, so that at zero applied field the polarization of each layer is perpendicular to the plane. Here, we demonstrate that atomically thin CrCl3 is a layered antiferromagnetic insulator with an easy-plane normal to the c-axis, that is, the polarization is in the plane of each layer and has no preferred direction within it. Ligand-field photoluminescence at 870 nm is observed down to the monolayer limit, demonstrating its insulating properties. We investigate the in-plane magnetic order using tunneling magnetoresistance in graphene/CrCl3/graphene tunnel junctions, establishing that the interlayer coupling is antiferromagnetic down to the bilayer. From the temperature dependence of the magnetoresistance, we obtain an effective magnetic phase diagram for the bilayer. Our result shows that CrCl3 should be useful for studying the physics of 2D phase transitions and for making new kinds of vdW spintronic devices.

A two-dimensional (2D) topological insulator (TI) exhibits the quantum spin Hall (QSH) effect, in which topologically protected spin-polarized conducting channels exist at the sample edges. Experimental signatures of the QSH effect have recently been reported for the first time in an atomically thin material, monolayer WTe2. Electrical transport measurements on exfoliated samples and scanning tunneling spectroscopy on epitaxially grown monolayer islands signal the existence of edge modes with conductance approaching the quantized value. Here, we directly image the local conductivity of monolayer WTe2 devices using microwave impedance microscopy, establishing beyond doubt that conduction is indeed strongly localized to the physical edges at temperatures up to 77 K and above. The edge conductivity shows no gap as a function of gate voltage, ruling out trivial conduction due to band bending or in-gap states, and is suppressed by magnetic field as expected. Interestingly, we observe additional conducting lines and rings within most samples which can be explained by edge states following boundaries between topologically trivial and non-trivial regions. These observations will be critical for interpreting and improving the properties of devices incorporating WTe2 or other air-sensitive 2D materials. At the same time, they reveal the robustness of the QSH channels and the potential to engineer and pattern them by chemical or mechanical means in the monolayer material platform., 9 pages, 4 figures

Atomically thin chromium triiodide (CrI3) has recently been identified as a layered antiferromagnetic insulator, in which adjacent ferromagnetic monolayers are antiferromagnetically coupled. This unusual magnetic structure naturally comprises a series of anti-aligned spin filters which can be utilized to make spin-filter magnetic tunnel junctions with very large tunneling magnetoresistance (TMR). Here we report voltage control of TMR formed by four-layer CrI3 sandwiched by monolayer graphene contacts in a dual-gated structure. By varying the gate voltages at fixed magnetic field, the device can be switched reversibly between bistable magnetic states with the same net magnetization but drastically different resistance (by a factor of ten or more). In addition, without switching the state, the TMR can be continuously modulated between 17,000% and 57,000%, due to the combination of spin-dependent tunnel barrier with changing carrier distributions in the graphene contacts. Our work demonstrates new kinds of magnetically moderated transistor action and opens up possibilities for voltage-controlled van der Waals spintronic devices.

We report a large area terahertz detector utilizing a tunable plasmonic resonance in subwavelength graphene microribbons on SiC(0001) to increase the absorption efficiency. By tailoring the orientation of the graphene ribbons with respect to an array of subwavelength bimetallic electrodes, we achieve a condition in which the plasmonic mode can be efficiently excited by an incident wave polarized perpendicular to the electrode array, while the resulting photothermal voltage can be observed between the outermost electrodes.

Magnetic multilayer devices that exploit magnetoresistance are the backbone of magnetic sensing and data storage technologies. Here we report novel multiple-spin-filter magnetic tunnel junctions (sf-MTJs) based on van der Waals (vdW) heterostructures in which atomically thin chromium triiodide (CrI3) acts as a spin-filter tunnel barrier sandwiched between graphene contacts. We demonstrate tunneling magnetoresistance which is drastically enhanced with increasing CrI3 layer thickness, reaching a record 19,000% for magnetic multilayer structures using four-layer sf-MTJs at low temperatures. These devices also show multiple resistance states as a function of magnetic field, suggesting the potential for multi-bit functionalities using an individual vdW sf-MTJ. Using magnetic circular dichroism measurements, we attribute these effects to the intrinsic layer-by-layer antiferromagnetic ordering of the atomically thin CrI3. Our work reveals the possibility to push magnetic information storage to the atomically thin limit, and highlights CrI3 as a superlative magnetic tunnel barrier for vdW heterostructure spintronic devices., Comment: Submitted

A two-dimensional topological insulator (2DTI) is guaranteed to have a helical 1D edge mode in which spin is locked to momentum, producing the quantum spin Hall effect and prohibiting elastic backscattering at zero magnetic field. No monolayer material has yet been shown to be a 2DTI, but recently the Weyl semimetal WTe2 was predicted to become a 2DTI in monolayer form if a bulk gap opens. Here, we report that at temperatures below about 100 K monolayer WTe2 does become insulating in its interior, while the edges still conduct. The edge conduction is strongly suppressed by in-plane magnetic field and is independent of gate voltage, save for mesoscopic fluctuations that grow on cooling due to a zero-bias anomaly which reduces the linear-response conductance. Bilayer WTe2 also becomes insulating at low temperatures but does not show edge conduction. Many of these observations are consistent with monolayer WTe2 being a 2DTI. However, the low temperature edge conductance, for contacts spacings down to 150 nm, is below the quantized value, 10 pages of main text plus 8 pages of supplementary materials

Hot electron effects in graphene are significant because of graphene's small electronic heat capacity and weak electron-phonon coupling, yet the dynamics and cooling mechanisms of hot electrons in graphene are not completely understood. We describe a novel photocurrent spectroscopy method that uses the mixing of continuous-wave lasers in a graphene photothermal detector to measure the frequency dependence and nonlinearity of hot-electron cooling in graphene as a function of the carrier concentration and temperature. The method offers unparalleled sensitivity to the nonlinearity, and probes the ultrafast cooling of hot carriers with an optical fluence that is orders of magnitude smaller than in conventional time-domain methods, allowing for accurate characterization of electron-phonon cooling near charge neutrality. Our measurements reveal that near the charge neutral-point the nonlinear power dependence of the electron cooling is dominated by disorder-assisted collisions, while at higher carrier concentrations conventional momentum-conserving cooling prevails in the nonlinear dependence. The relative contribution of these competing mechanisms can be electrostatically tuned through the application of a gate voltage -- an effect that is unique to graphene.

A nonlocal Hall bar geometry is used to detect neutral-current Hall effects in graphene on silicon dioxide. Disorder is tuned by the addition of $\mathrm{Au}$ or $\mathrm{Ir}$ adatoms in ultrahigh vacuum. A reproducible neutral-current Hall effect is found in both as-fabricated and adatom-decorated graphene. The Hall angle exhibits a complex but reproducible dependence on gate voltage and disorder, and notably breaks electron-hole symmetry. An exponential dependence on length between Hall and inverse Hall probes indicates a neutral-current relaxation length of approximately $300\phantom{\rule{0.16em}{0ex}}\mathrm{nm}$. The short relaxation length and lack of precession in a parallel magnetic field suggest that the neutral currents are valley currents. No signature of the spin-orbit coupling induced spin Hall effect is observed in the $\mathrm{Au}$- or $\mathrm{Ir}$-decorated graphene. The near lack of temperature dependence from 7 to 300 K is unprecedented among reports of valley Hall effect in graphene, and promising for using controlled disorder for room temperature neutral-current electronics.

We use an ultra-fast near-infrared pulse coincidence technique to study the time, temperature and power dependence of the photoresponse of a bi-metal contacted graphene photodetector. We observe two components of the photovoltage signal. One component is gate-voltage dependent, linear in power at room temperature and sub-linear at low temperature-consistent with the hot-electron photothermoelectric effect due to absorption in the graphene. The power dependence is consistent with supercollision-dominated cooling in graphene. The other component is gate-voltage independent and linear in temperature and power, which we interpret as due to thermoelectricity of the metal electrodes due to differential light absorption.

Graphene decorated with 5d transitional metal atoms is predicted to exhibit many intriguing properties; for example iridium adatoms are proposed to induce a substantial topological gap in graphene. We extensively investigated the conductivity of single-layer graphene decorated with iridium deposited in ultra-high vacuum at low temperature (7 K) as a function of Ir concentration, carrier density, temperature and annealing conditions. Our results are consistent with the formation of Ir clusters of ~100 atoms at low temperature, with each cluster donating a single electronic charge to graphene. Annealing graphene increases the cluster size, reducing the doping and increasing the mobility. We do not observe any sign of an energy gap induced by spin-orbit coupling, possibly due to the clustering of Ir.

We study the response of a graphene photothermoelectric-based detector illuminated by two continuous-wave optical beams. The power and frequency dependence of the photoresponse are used to probe the graphene hot-electron cooling rates and mechanisms.

The temporal response of a broadband, monolayer graphene photodetector based on the photothermoelectric effect is characterized. Pulse-coincidence and impulse response measurements indicate fast photodetection on the timescale of 10 ps.

Various bandstructure engineering methods have been studied to improve the performance of graphitic transparent conductors; however none demonstrated an increase of optical transmittance in the visible range. Here we measure in situ optical transmittance spectra and electrical transport properties of ultrathin-graphite (3-60 graphene layers) simultaneously via electrochemical lithiation/delithiation. Upon intercalation we observe an increase of both optical transmittance (up to twofold) and electrical conductivity (up to two orders of magnitude), strikingly different from other materials. Transmission as high as 91.7% with a sheet resistance of 3.0 {\Omega} per square is achieved for 19-layer LiC6, which corresponds to a figure of merit {\sigma}_dc/{\sigma}_opt = 1400, significantly higher than any other continuous transparent electrodes. The unconventional modification of ultrathin-graphite optoelectronic properties is explained by the suppression of interband optical transitions and a small intraband Drude conductivity near the interband edge. Our techniques enable the investigation of other aspects of intercalation in nanostructures., Comment: Published 01 July 2014 in Nature Communications

Terahertz (THz) radiation has uses from security to medicine; however, sensitive room-temperature detection of THz is notoriously difficult. The hot-electron photothermoelectric effect in graphene is a promising detection mechanism: photoexcited carriers rapidly thermalize due to strong electron-electron interactions, but lose energy to the lattice more slowly. The electron temperature gradient drives electron diffusion, and asymmetry due to local gating or dissimilar contact metals produces a net current via the thermoelectric effect. Here we demonstrate a graphene thermoelectric THz photodetector with sensitivity exceeding 10 V/W (700 V/W) at room temperature and noise equivalent power less than 1100 pW/Hz^1/2 (20 pW/Hz^1/2), referenced to the incident (absorbed) power. This implies a performance which is competitive with the best room-temperature THz detectors for an optimally coupled device, while time-resolved measurements indicate that our graphene detector is eight to nine orders of magnitude faster than those. A simple model of the response, including contact asymmetries (resistance, work function and Fermi-energy pinning) reproduces the qualitative features of the data, and indicates that orders-of-magnitude sensitivity improvements are possible., Comment: Published 07 September 2014 in Nature Nanotechnology

The responsivity of a monolayer graphene photodetector based on the photo-thermoelectric effect was measured at room temperature for dc, terahertz, and optical frequencies and found to be approximately 81, 188, and 18 V/W respectively.

We fabricate MoS2 field effect transistors on both SiO2 and polymethyl methacrylate (PMMA) dielectrics and measure charge carrier mobility in a four-probe configuration. For multilayer MoS2 on SiO2, the mobility is 30-60 cm2/Vs, relatively independent of thickness (15-90 nm), and most devices exhibit unipolar n-type behavior. In contrast, multilayer MoS2 on PMMA shows mobility increasing with thickness, up to 470 cm2/Vs (electrons) and 480 cm2/Vs (holes) at thickness ~50 nm. The dependence of the mobility on thickness points to a long-range dielectric effect of the bulk MoS2 in increasing mobility., 3 figures