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Two-dimensional (2D) materials offer unique opportunities in engineering the ultrafast spatiotemporal response of composite nanomechanical structures. In this work, we report on high frequency, high quality factor ( Q ) 2D acoustic cavities operating in the 50–600 GHz frequency ( f ) range with f × Q up to 1 × 10 14 . Monolayer steps and material interfaces expand cavity functionality, as demonstrated by building adjacent cavities that are isolated or strongly-coupled, as well as a frequency comb generator in MoS 2 /h-BN systems. Energy dissipation measurements in 2D cavities are compared with attenuation derived from phonon-phonon scattering rates calculated using a fully microscopic ab initio approach. Phonon lifetime calculations extended to low frequencies (<1 THz) and combined with sound propagation analysis in ultrathin plates provide a framework for designing acoustic cavities that approach their fundamental performance limit. These results provide a pathway for developing platforms employing phonon-based signal processing and for exploring the quantum nature of phonons. Here, authors report on acoustic cavities in 2D materials operating in the 50–600 GHz range and show that quality factors approach the limit set by lattice anharmonicity. Functionality expanded by heterogeneities (steps and interfaces) is demonstrated through coupled cavities and frequency comb generation.

Harnessing electronic excitations involving coherent coupling to bosonic modes is essential for the design and control of emergent phenomena in quantum materials. In situations where charge carriers induce a lattice distortion due to the electron-phonon interaction, the conducting states get “dressed\", which leads to the formation of polaronic quasiparticles. The exploration of polaronic effects on low-energy excitations is in its infancy in two-dimensional materials. Here, we present the discovery of an interlayer plasmon polaron in heterostructures composed of graphene on top of single-layer WS 2 . By using micro-focused angle-resolved photoemission spectroscopy during in situ doping of the top graphene layer, we observe a strong quasiparticle peak accompanied by several carrier density-dependent shake-off replicas around the single-layer WS 2 conduction band minimum. Our results are explained by an effective many-body model in terms of a coupling between single-layer WS 2 conduction electrons and an interlayer plasmon mode. It is important to take into account the presence of such interlayer collective modes, as they have profound consequences for the electronic and optical properties of heterostructures that are routinely explored in many device architectures involving 2D transition metal dichalcogenides. Here, the authors report the observation of an interlayer plasmon polaron in heterostructures composed of graphene and monolayer WS 2 . This is manifested in the ARPES spectra as a strong quasiparticle peak accompanied by several carrier density-dependent shake-off replicas around the WS 2 conduction band minimum.

Mechanical stress can drive chemical reactions and is unique in that the reaction product can depend on both the magnitude and the direction of the applied force. Indeed, this directionality can drive chemical reactions impossible through conventional means. However, unlike heat- or pressure-driven reactions, mechanical stress is rarely applied isometrically, obscuring how mechanical inputs relate to the force applied to the bond. Here we report an atomic force microscope technique that can measure mechanically induced bond scission on graphene in real time with sensitivity to atomic-scale interactions. Quantitative measurements of the stress-driven reaction dynamics show that the reaction rate depends both on the bond being broken and on the tip material. Oxygen cleaves from graphene more readily than fluorine, which in turn cleaves more readily than hydrogen. The technique may be extended to study the mechanochemistry of any arbitrary combination of tip material, chemical group and substrate. Breaking chemical bonds with mechanical force can be a useful route to modify chemical species, but studying the process in detail can be challenging. Here, the authors use atomic force microscopy to apply pressure and monitor bond cleavage on chemically modified graphene.

By combining optical imaging, Raman spectroscopy, kelvin probe force microscopy (KFPM), and photoemission electron microscopy (PEEM), we show that graphene’s layer orientation, as well as layer thickness, measurably changes the surface potential (Φ). Detailed mapping of variable-thickness, rotationally-faulted graphene films allows us to correlate Φ with specific morphological features. Using KPFM and PEEM we measure ΔΦ up to 39 mV for layers with different twist angles, while ΔΦ ranges from 36–129 mV for different layer thicknesses. The surface potential between different twist angles or layer thicknesses is measured at the KPFM instrument resolution of ≤ 200 nm. The PEEM measured work function of 4.4 eV for graphene is consistent with doping levels on the order of 10 12 cm −2 . We find that Φ scales linearly with Raman G-peak wavenumber shift (slope = 22.2 mV/cm −1 ) for all layers and twist angles, which is consistent with doping-dependent changes to graphene’s Fermi energy in the ‘high’ doping limit. Our results here emphasize that layer orientation is equally important as layer thickness when designing multilayer two-dimensional systems where surface potential is considered.

Here we report how two-dimensional crystal (2DC) overlayers influence the recrystallization of relatively thick metal films and the subsequent synergetic benefits this provides for coupling surface plasmon-polaritons (SPPs) to photon emission in 2D semiconductors. We show that annealing 2DC/Au films on SiO 2 results in a reverse epitaxial process where initially nanocrystalline Au films gain texture, crystallographically orient with the 2D crystal overlayer, and form an oriented porous metallic network (OPEN) structure in which the 2DC can suspend above or coat the inside of the metal pores. Both laser excitation and exciton recombination in the 2DC semiconductor launch propagating SPPs in the OPEN film. Energy in-/out- coupling occurs at metal pore sites, alleviating the need for dielectric spacers between the metal and 2DC layer. At low temperatures, single-photon emitters (SPEs) are present across an OPEN-WSe 2 film, and we demonstrate remote SPP-mediated excitation of SPEs at a distance of 17 μm. Here, the authors develop a reverse epitaxial process whereby a nanocrystalline Au film becomes highly textured and support a suspended 2D WSe 2 overlayer. Surface plasmon polaritons are launched in nanostructured Au by laser excitation and couple remotely to single photon emitters present in WSe 2 .

To pinpoint the electronic and structural mechanisms that affect intrinsic and extrinsic performance limits of 2D material devices, it is of critical importance to resolve the electronic properties on the mesoscopic length scale of such devices under operating conditions. Herein, angle‐resolved photoemission spectroscopy with nanoscale spatial resolution (nanoARPES) is used to map the quasiparticle electronic structure of a twisted bilayer graphene device. The dispersion and linewidth of the Dirac cones associated with top and bottom graphene layers are determined as a function of spatial position on the device under both static and operating conditions. The analysis reveals that microscopic rotational domains in the two graphene layers establish a range of twist angles from 9.8° to 12.7°. Application of current and electrostatic gating lead to strong electric fields with peak strengths of 0.75 V/μm at the rotational domain boundaries in the device. These proof‐of‐principle results demonstrate the potential of nanoARPES to link mesoscale structural variations with electronic states in operating device conditions and to disentangle such extrinsic factors from the intrinsic quasiparticle dispersion. Nanoscale angle‐resolved photoemission spectroscopy is applied to map the electronic structure of a twisted bilayer graphene device during the application of current and an electrostatic gate voltage. Rotational domains are found to strongly affect the measured linewidth of the top and bottom Dirac cones and lead to a spatially inhomogeneous electric field during operation of the device.

We report a novel and easily accessible method to chemically reduce graphene fluoride （GF） sheets with nanoscopic precision using high electrostatic fields generated between an atomic force microscope （AFM） tip and the GF substrate. Reduction of fluorine by the electric field produces graphene nanoribbons （GNR） with a width of 105-1,800 nm with sheet resistivity drastically decreased from 〉1 TΩ.sq.^-1 （GF） down to 46 kΩ.sq.^-1 （GNR）. Fluorine reduction also changes the topography, friction, and work function of the GF. Kelvin probe force microscopy measurements indicate that the work function of GF is 180-280 meV greater than that of graphene. The reduction process was optimized by varying the AFM probe velocity between 1.2 μm.s^-1 and 12 μm.s^-1 and the bias voltage applied to the sample between -8 and -12 V. The electrostatic field required to remove fluorine from carbon is -1.6 V.nm-1. Reduction of the fluorine may be due to the softening of the C-F bond in this intense field or to the accumulation and hydrolysis of adventitious water into a meniscus.

The coupled imperatives for reduced heat dissipation and power consumption in high-density electronics have rekindled interest in devices based on tunnelling. Such devices require mating dissimilar materials, raising issues of heteroepitaxy, layer uniformity, interface stability and electronic states that severely complicate fabrication and compromise performance. Two-dimensional materials such as graphene obviate these issues and offer a new paradigm for tunnel barriers. Here we demonstrate a homoepitaxial tunnel barrier structure in which graphene serves as both the tunnel barrier and the high-mobility transport channel. We fluorinate the top layer of a graphene bilayer to decouple it from the bottom layer, so that it serves as a single-monolayer tunnel barrier for both charge and spin injection into the lower graphene channel. We demonstrate high spin injection efficiency with a tunnelling spin polarization >60%, lateral transport of spin currents in non-local spin-valve structures and determine spin lifetimes with the Hanle effect. The long spin diffusion lengths in graphene make it attractive for spintronic applications but achieving efficient spin injection is proving challenging. Here, the authors show that functionalized graphene can act as a tunnel barrier, demonstrating non-local homoepitaxial spin valves.

We experimentally investigate the effects of Co-60 irradiation on the electrical properties of single-walled carbon nanotube and graphene field-effect transistors. We observe significant differences in the radiation response of devices depending on their irradiation environment, and confirm that, under controlled conditions, standard dielectric hardening approaches are applicable to carbon nanoelectronics devices.

We describe a method for phase separating and transferring block copolymer (BCP) nanoscale patterns to arbitrary substrates for surface-independent nanolithography. The enabling technology is a hydrogenated or oxidized graphene thin film that only weakly adheres to its substrate. BCPs are applied to these graphene-based materials and solvent annealed to effect nanoscale phase separation. Then, taking advantage of the weak interaction of the graphene film and its substrate, the BCP/graphene stack is delaminated easily in water. A target substrate is then used to retrieve the stack, which can then serve as a lithographic mask. The use of water as a lift-off agent allows for chemically mild retrieval of the phase-separated BCP, extending the BCP lithography technique to essentially arbitrary substrates. We demonstrate this graphene-enabled BCP lithography on silicon nitride and polyethylene. We also show that using reduced graphene oxide (RGO) as a thin film enables the transfer of wafer-scale BCP films and lithography on SiO x and Si. We use an RGO support to produce phase-separated BCP solvent-annealed patterns on polystyrene, a result which is not possible using standard BCP solvent annealing and which shows the utility of this technique. Finally, we demonstrate the ability to create nanopatterns of higher complexity by stacking multiple BCP masks, a capability that is not possible using conventional BCP lithography. This technique may have applications in fabricating nanoporous membranes and photonically active coatings.