All-optical switching of magnetization in atomically thin CrI3.

Control of magnetism has attracted interest in achieving low-power and high-speed applications such as magnetic data storage and spintronic devices. Two-dimensional magnets allow for control of magnetic properties using the electric field, electrostatic doping and strain. In two-dimensional atomically thin magnets, a non-volatile all-optical method would offer the distinct advantage of switching magnetic states without application of an external field. Here, we demonstrate such all-optical magnetization switching in the atomically thin ferromagnetic semiconductor, CrI3, triggered by circularly polarized light pulses. The magnetization switching behaviour strongly depends on the exciting photon energy and polarization, in correspondence with excitonic transitions in CrI3, indicating that the switching process is related to spin angular momentum transfer from photoexcited carriers to local magnetic moments. Such an all-optical magnetization switching should allow for further exploration of magneto-optical interactions and open up applications in high-speed and low-power spintronic devices.

Enhanced Graphene Photodetector with Fractal Metasurface.

Graphene has been demonstrated to be a promising photodetection material because of its ultrabroadband optical absorption, compatibility with CMOS technology, and dynamic tunability in optical and electrical properties. However, being a single atomic layer thick, graphene has intrinsically small optical absorption, which hinders its incorporation with modern photodetecting systems. In this work, we propose a gold snowflake-like fractal metasurface design to realize broadband and polarization-insensitive plasmonic enhancement in graphene photodetector. We experimentally obtain an enhanced photovoltage from the fractal metasurface that is an order of magnitude greater than that generated at a plain gold-graphene edge and such an enhancement in the photovoltage sustains over the entire visible spectrum. We also observed a relatively constant photoresponse with respect to polarization angles of incident light, as a result of the combination of two orthogonally oriented concentric hexagonal fractal geometries in one metasurface.

Optical phonons in twisted bilayer graphene with gate-induced asymmetric doping.

Twisted bilayer graphene (tBLG) devices with ion gel gate dielectrics are studied using Raman spectroscopy in the twist angle regime where a resonantly enhanced G band can be observed. We observe prominent splitting and intensity quenching on the G Raman band when the carrier density is tuned away from charge neutrality. This G peak splitting is attributed to asymmetric charge doping in the two graphene layers, which reveals individual phonon self-energy renormalization of the two weakly coupled layers of graphene. We estimate the effective interlayer capacitance at low doping density of tBLG using an interlayer screening model. The anomalous intensity quenching of both G peaks is ascribed to the suppression of resonant interband transitions between the two saddle points (van Hove singularities) that are displaced in the momentum space by gate-tuning. In addition, we observe a softening (hardening) of the R Raman band, a superlattice-induced phonon mode in tBLG, in electron (hole) doping. Our results demonstrate that gate modulation can be used to control the optoelectronic and vibrational properties in tBLG devices.

Electrical modulation of fano resonance in plasmonic nanostructures using graphene.

Pauli blocking of interband transistions gives rise to tunable optical properties in single layer graphene (SLG). This effect is exploited in a graphene-nanoantenna hybrid device where Fano resonant plasmonic nanostructures are fabricated on top of a graphene sheet. The use of Fano resonant elements enhances the interaction of incident radiation with the graphene sheet and enables efficient electrical modulation of the plasmonic resonance. We observe electrically controlled damping in the Fano resonances occurring at approximately 2 µm, and the results are verified by full-wave 3D finite-element simulations. Our approach can be used for development of next generation of tunable plasmonic and hybrid nanophotonic devices.

Observation of low energy Raman modes in twisted bilayer graphene.

Two new Raman modes below 100 cm(-1) are observed in twisted bilayer graphene grown by chemical vapor deposition. The two modes are observed in a small range of twisting angle at which the intensity of the G Raman peak is strongly enhanced, indicating that these low energy modes and the G Raman mode share the same resonance enhancement mechanism, as a function of twisting angle. The ~94 cm(-1) mode (measured with a 532 nm laser excitation) is assigned to the fundamental layer breathing vibration (ZO' mode) mediated by the twisted bilayer graphene lattice, which lacks long-range translational symmetry. The dependence of this mode's frequency and line width on the rotational angle can be explained by the double resonance Raman process that is different from the previously identified Raman processes activated by twisted bilayer graphene superlattice. The dependence also reveals the strong impact of electronic-band overlaps of the two graphene layers. Another new mode at ~52 cm(-1), not observed previously in the bilayer graphene system, is tentatively attributed to a torsion mode in which the bottom and top graphene layers rotate out-of-phase in the plane.

Nanoscale strainability of graphene by laser shock-induced three-dimensional shaping.

Graphene has many promising physical properties. It has been discovered that local strain in a graphene sheet can alter its conducting properties and transport gaps. It is of great importance to develop scalable strain engineering techniques to control the local strains in graphene and understand the limit of the strains. Here, we present a scalable manufacturing process to generate three-dimensional (3D) nanostructures and thus induce local strains in the graphene sheet. This process utilizes laser-induced shock pressure to generate 3D tunable straining in the graphene sheet. The size dependent straining limit of the graphene and the critical breaking pressure are both studied. It is found that the graphene film can be formed to a circular mold (∼50 nm in diameter) with an aspect ratio of 0.25 and strain of 12%, and the critical breaking pressure is 1.77 GPa. These values were found to be decreasing with the increase of mold size. The local straining and breaking of graphene film are verified by Raman spectra. Large scale processing of the graphene sheet into nanoscale patterns is presented. The process could be scaled up to roll-to-roll process by changing laser beam size and scanning speed. The presented laser shock straining approach is a fast, tunable, and low-cost technique to realize strain engineering of graphene for its applications in nanoelectrical devices.

Electrically tunable damping of plasmonic resonances with graphene.

Dynamic switching of a plasmonic resonance may find numerous applications in subwavelength optoelectronics, spectroscopy, and sensing. Graphene shows a highly tunable carrier concentration under electrostatic gating, and this could provide an effective route to achieving electrical control of the plasmonic resonance. In this Letter, we demonstrate electrical control of a plasmonic resonance at infrared frequencies using large-area graphene. Plasmonic structures fabricated on graphene enhance the interaction of the incident optical field with the graphene sheet, and the impact of graphene is much stronger at mid-infrared wavelengths. Full-wave simulations, where graphene is modeled as a 1 nm thick effective medium, show excellent agreement with experimental results.

Control and characterization of individual grains and grain boundaries in graphene grown by chemical vapour deposition.

The strong interest in graphene has motivated the scalable production of high-quality graphene and graphene devices. As the large-scale graphene films synthesized so far are typically polycrystalline, it is important to characterize and control grain boundaries, generally believed to degrade graphene quality. Here we study single-crystal graphene grains synthesized by ambient chemical vapour deposition on polycrystalline Cu, and show how individual boundaries between coalescing grains affect graphene's electronic properties. The graphene grains show no definite epitaxial relationship with the Cu substrate, and can cross Cu grain boundaries. The edges of these grains are found to be predominantly parallel to zigzag directions. We show that grain boundaries give a significant Raman 'D' peak, impede electrical transport, and induce prominent weak localization indicative of intervalley scattering in graphene. Finally, we demonstrate an approach using pre-patterned growth seeds to control graphene nucleation, opening a route towards scalable fabrication of single-crystal graphene devices without grain boundaries.

Enhancing the graphene photocurrent using surface plasmons and a p-n junction.

The recently proposed concept of graphene photodetectors offers remarkable properties such as unprecedented compactness, ultrabroadband detection, and an ultrafast response speed. However, owing to the low optical absorption of pristine monolayer graphene, the intrinsically low responsivity of graphene photodetectors significantly hinders the development of practical devices. To address this issue, numerous efforts have thus far been made to enhance the light-graphene interaction using plasmonic structures. These approaches, however, can be significantly advanced by leveraging the other critical aspect of graphene photoresponsivity enhancement-electrical junction control. It has been reported that the dominant photocarrier generation mechanism in graphene is the photothermoelectric (PTE) effect. Thus, the two energy conversion mechanisms involved in the graphene photodetection process are light-to-heat and heat-to-electricity conversions. In this work, we propose a meticulously designed device architecture to simultaneously enhance the two conversion efficiencies. Specifically, a gap plasmon structure is used to absorb a major portion of the incident light to induce localized heating, and a pair of split gates is used to produce a p-n junction in graphene to augment the PTE current generation. The gap plasmon structure and the split gates are designed to share common key components so that the proposed device architecture concurrently realizes both optical and electrical enhancements. We experimentally demonstrate the dominance of the PTE effect in graphene photocurrent generation and observe a 25-fold increase in the generated photocurrent compared to the un-enhanced cases. While further photocurrent enhancement can be achieved by applying a DC bias, the proposed device concept shows vast potential for practical applications.

Strain-stress study of AlxGa1-xN/AlN heterostructures on c-plane sapphire and related optical properties.

This work presents a systematic study of stress and strain of AlxGa1-xN/AlN with composition ranging from GaN to AlN, grown on a c-plane sapphire by metal-organic chemical vapor deposition, using synchrotron radiation high-resolution X-ray diffraction and reciprocal space mapping. The c-plane of the AlxGa1-xN epitaxial layers exhibits compressive strain, while the a-plane exhibits tensile strain. The biaxial stress and strain are found to increase with increasing Al composition, although the lattice mismatch between the AlxGa1-xN and the buffer layer AlN gets smaller. A reduction in the lateral coherence lengths and an increase in the edge and screw dislocations are seen as the AlxGa1-xN composition is varied from GaN to AlN, exhibiting a clear dependence of the crystal properties of AlxGa1-xN on the Al content. The bandgap of the epitaxial layers is slightly lower than predicted value due to a larger tensile strain effect on the a-axis compared to the compressive strain on the c-axis. Raman characteristics of the AlxGa1-xN samples exhibit a shift in the phonon peaks with the Al composition. The effect of strain on the optical phonon energies of the epitaxial layers is also discussed.

Photocarrier generation from interlayer charge-transfer transitions in WS2-graphene heterostructures.

Efficient interfacial carrier generation in van der Waals heterostructures is critical for their electronic and optoelectronic applications. We demonstrate broadband photocarrier generation in WS2-graphene heterostructures by imaging interlayer coupling-dependent charge generation using ultrafast transient absorption microscopy. Interlayer charge-transfer (CT) transitions and hot carrier injection from graphene allow carrier generation by excitation as low as 0.8 eV below the WS2 bandgap. The experimentally determined interlayer CT transition energies are consistent with those predicted from the first-principles band structure calculation. CT interactions also lead to additional carrier generation in the visible spectral range in the heterostructures compared to that in the single-layer WS2 alone. The lifetime of the charge-separated states is measured to be ~1 ps. These results suggest that interlayer interactions make graphene-two-dimensional semiconductor heterostructures very attractive for photovoltaic and photodetector applications because of the combined benefits of high carrier mobility and enhanced broadband photocarrier generation.

Position-dependent and millimetre-range photodetection in phototransistors with micrometre-scale graphene on SiC.

The extraordinary optical and electronic properties of graphene make it a promising component of high-performance photodetectors. However, in typical graphene-based photodetectors demonstrated to date, the photoresponse only comes from specific locations near graphene over an area much smaller than the device size. For many optoelectronic device applications, it is desirable to obtain the photoresponse and positional sensitivity over a much larger area. Here, we report the spatial dependence of the photoresponse in backgated graphene field-effect transistors (GFET) on silicon carbide (SiC) substrates by scanning a focused laser beam across the GFET. The GFET shows a nonlocal photoresponse even when the SiC substrate is illuminated at distances greater than 500 µm from the graphene. The photoresponsivity and photocurrent can be varied by more than one order of magnitude depending on the illumination position. Our observations are explained with a numerical model based on charge transport of photoexcited carriers in the substrate.

Substrate Doping Effect and Unusually Large Angle van Hove Singularity Evolution in Twisted Bi- and Multilayer Graphene.

Graphene has demonstrated great potential in new-generation electronic applications due to its unique electronic properties such as large carrier Fermi velocity, ultrahigh carrier mobility, and high material stability. Interestingly, the electronic structures can be further engineered in multilayer graphene by the introduction of a twist angle between different layers to create van Hove singularities (vHSs) at adjustable binding energy. In this work, using angle-resolved photoemission spectroscopy with sub-micrometer spatial resolution, the band structures and their evolution are systematically studied with twist angle in bilayer and trilayer graphene sheets. A doping effect is directly observed in graphene multilayer system as well as vHSs in bilayer graphene over a wide range of twist angles (from 5° to 31°) with wide tunable energy range over 2 eV. In addition, the formation of multiple vHSs (at different binding energies) is also observed in trilayer graphene. The large tuning range of vHS binding energy in twisted multilayer graphene provides a promising material base for optoelectrical applications with broadband wavelength selectivity from the infrared to the ultraviolet regime, as demonstrated by an example application of wavelength selective photodetector.

Highly sensitive transient absorption imaging of graphene and graphene oxide in living cells and circulating blood.

We report a transient absorption (TA) imaging method for fast visualization and quantitative layer analysis of graphene and GO. Forward and backward imaging of graphene on various substrates under ambient condition was imaged with a speed of 2 µs per pixel. The TA intensity linearly increased with the layer number of graphene. Real-time TA imaging of GO in vitro with capability of quantitative analysis of intracellular concentration and ex vivo in circulating blood were demonstrated. These results suggest that TA microscopy is a valid tool for the study of graphene based materials.

Use of graphene as protection film in biological environments.

Corrosion of metal in biomedical devices could cause serious health problems to patients. Currently ceramics coating materials used in metal implants can reduce corrosion to some extent with limitations. Here we proposed graphene as a biocompatible protective film for metal potentially for biomedical application. We confirmed graphene effectively inhibits Cu surface from corrosion in different biological aqueous environments. Results from cell viability tests suggested that graphene greatly eliminates the toxicity of Cu by inhibiting corrosion and reducing the concentration of Cu(2+) ions produced. We demonstrated that additional thiol derivatives assembled on graphene coated Cu surface can prominently enhance durability of sole graphene protection limited by the defects in graphene film. We also demonstrated that graphene coating reduced the immune response to metal in a clinical setting for the first time through the lymphocyte transformation test. Finally, an animal experiment showed the effective protection of graphene to Cu under in vivo condition. Our results open up the potential for using graphene coating to protect metal surface in biomedical application.