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The ability to understand and control the electronic properties of individual molecules in a device environment is crucial for developing future technologies at the nanometre scale and below. Achieving this, however, requires the creation of three-terminal devices that allow single molecules to be both gated and imaged at the atomic scale. We have accomplished this by integrating a graphene field effect transistor with a scanning tunnelling microscope, thus allowing gate-controlled charging and spectroscopic interrogation of individual tetrafluoro-tetracyanoquinodimethane molecules. We observe a non-rigid shift in the molecule’s lowest unoccupied molecular orbital energy (relative to the Dirac point) as a function of gate voltage due to graphene polarization effects. Our results show that electron–electron interactions play an important role in how molecular energy levels align to the graphene Dirac point, and may significantly influence charge transport through individual molecules incorporated in graphene-based nanodevices. The development of single-molecule electronics calls for precise tuning of the electronic properties of individual molecules that go beyond two-terminal control. Here, Wickenburg et al . show gate-tunable switch of charge states of an isolated molecule using a graphene-based field-effect transistor.

To be able to control the properties of a system that has strong electron–electron interactions using only an external electric field would be ideal, but the material must be thin enough to avoid shielding of the electric field in the bulk material; here pure electric-field control of the charge-density wave and superconductivity transition temperatures is achieved by electrolyte gating through an electric-field double layer transistor in the two-dimensional material 1T-TiSe 2 . Electronic behavior in 1T-TiSe 2 The properties of a system with strong electron–electron interactions are ideally studied using only an external electric field, but this is only effective if the material is thin enough to avoid the shielding effect of the bulk material. Various fabrication techniques have been developed in recent years to produce ultrathin, two-dimensional forms of electronic materials. Antonoi Castro-Neto and colleagues use one such method to study the layered transition-metal dichalcogenide 1T-TiSe 2 in the form of a flake less than 10 nanometres thick and encapsulated between hexagonal boron nitride. By varying the electric field, magnetic field and temperature, they reveal details about the transition between different electronic phases, such as a correlation between the existence of superconductivity and appearance of spatially modulated electronic states. To understand the complex physics of a system with strong electron–electron interactions, the ideal is to control and monitor its properties while tuning an external electric field applied to the system (the electric-field effect). Indeed, complete electric-field control of many-body states in strongly correlated electron systems is fundamental to the next generation of condensed matter research and devices 1 , 2 , 3 . However, the material must be thin enough to avoid shielding of the electric field in the bulk material. Two-dimensional materials do not experience electrical screening, and their charge-carrier density can be controlled by gating. Octahedral titanium diselenide (1T-TiSe 2 ) is a prototypical two-dimensional material that reveals a charge-density wave (CDW) and superconductivity in its phase diagram 4 , presenting several similarities with other layered systems such as copper oxides 5 , iron pnictides 6 , and crystals of rare-earth elements and actinide atoms 7 . By studying 1T-TiSe 2 single crystals with thicknesses of 10 nanometres or less, encapsulated in two-dimensional layers of hexagonal boron nitride, we achieve unprecedented control over the CDW transition temperature (tuned from 170 kelvin to 40 kelvin), and over the superconductivity transition temperature (tuned from a quantum critical point at 0 kelvin up to 3 kelvin). Electrically driving TiSe 2 over different ordered electronic phases allows us to study the details of the phase transitions between many-body states. Observations of periodic oscillations of magnetoresistance induced by the Little–Parks effect show that the appearance of superconductivity is directly correlated with the spatial texturing of the amplitude and phase of the superconductivity order parameter, corresponding to a two-dimensional matrix of superconductivity. We infer that this superconductivity matrix is supported by a matrix of incommensurate CDW states embedded in the commensurate CDW states. Our results show that spatially modulated electronic states are fundamental to the appearance of two-dimensional superconductivity.

Two-dimensional superconductor (2DSC) monolayers with non-centrosymmetry exhibit unconventional Ising pair superconductivity and an enhanced upper critical field beyond the Pauli paramagnetic limit, driving intense research interest. However, they are often susceptible to structural disorder and environmental oxidation, which destroy electronic coherence and provide technical challenges in the creation of artificial van der Waals heterostructures (vdWHs) for devices. Herein, we report a general and scalable synthesis of highly crystalline 2DSC monolayers via a mild electrochemical exfoliation method using flexible organic ammonium cations solvated with neutral solvent molecules as co-intercalants. Using NbSe 2 as a model system, we achieved a high yield (>75%) of large-sized single-crystal monolayers up to 300 µm. The as-fabricated, twisted NbSe 2 vdWHs demonstrate high stability, good interfacial properties and a critical current that is modulated by magnetic field when one flux quantum fits to an integer number of moiré cells. Additionally, formulated 2DSC inks can be exploited to fabricate wafer-scale 2D superconducting wire arrays and three-dimensional superconducting composites with desirable morphologies. A mild electrochemical exfoliation method has been developed to obtain large-size two-dimensional superconductor monolayers with high crystallinity and production yield, which enables the easy fabrication of twisted van der Waals heterostructures and printed films.

Recent theoretical proposals suggest that strain can be used to engineer graphene electronic states through the creation of a pseudo-magnetic field. This effect is unique to graphene because of its massless Dirac fermion-like band structure and particular lattice symmetry (C₃v). Here, we present experimental spectroscopic measurements by scanning tunneling microscopy of highly strained nanobubbles that form when graphene is grown on a platinum (111) surface. The nanobubbles exhibit Landau levels that form in the presence of strain-induced pseudo-magnetic fields greater than 300 tesla. This demonstration of enormous pseudo-magnetic fields opens the door to both the study of charge carriers in previously inaccessible high magnetic field regimes and deliberate mechanical control over electronic structure in graphene or so-called \"strain engineering.\"

Strain engineering has been proposed as an alternative method for manipulating the electronic properties of graphene. However, the bottleneck for strain engineering in graphene has been the ability to control such strain patterns at the nanoscale. Here we show that high level of control can be accomplished by chemically modifying the adherence of graphene on metal. Using scanning tunnelling microscopy, the shape evolution of graphene Moiré blisters towards geometrically well-defined graphene bubbles was studied during the controlled, sub-layer oxidation of the ruthenium substrate. Understanding the dynamics of the oxidation process and defects generation on the Ru substrate allows us to control the size, shape and the density of the bubbles and its associated pseudo-magnetism. We also show that a modification of the same procedure can be used to create antidots in graphene by catalytic reaction of the same nanobubbles. Strain engineering has been proposed as a promising strategy for manipulating the electronic properties of graphene. This scanning tunnelling microscopy study demonstrates the feasibility of controlling strain patterns in graphene down to the nanoscale.

Plasmons are directly launched in graphene, and their key parameters — propagation and attenuation — are studied with near-field infrared nano-imaging. Voltage-controlled graphene plasmonics Plasmonic devices, which exploit surface plasmons (electromagnetic waves that propagate along the surface of metals) offer the possibility of controlling and guiding light at subwavelength scales. All eyes are on graphene — atom-thick layers of carbon — as a promising platform for plasmonic applications because it can strongly interact with light and host surface plasmons in the infrared range. Two independent groups reporting in this issue of Nature show that plasmons can be directly launched in graphene, and observed with near-field optical microscopy. Moreover, the wavelengths and amplitudes of the plasmons can be tuned by a gate voltage, a promising capability for the development of on-chip graphene photonics for use in applications including telecommunications and information processing. Surface plasmons are collective oscillations of electrons in metals or semiconductors that enable confinement and control of electromagnetic energy at subwavelength scales 1 , 2 , 3 , 4 , 5 . Rapid progress in plasmonics has largely relied on advances in device nano-fabrication 5 , 6 , 7 , whereas less attention has been paid to the tunable properties of plasmonic media. One such medium—graphene—is amenable to convenient tuning of its electronic and optical properties by varying the applied voltage 8 , 9 , 10 , 11 . Here, using infrared nano-imaging, we show that common graphene/SiO 2 /Si back-gated structures support propagating surface plasmons. The wavelength of graphene plasmons is of the order of 200 nanometres at technologically relevant infrared frequencies, and they can propagate several times this distance. We have succeeded in altering both the amplitude and the wavelength of these plasmons by varying the gate voltage. Using plasmon interferometry, we investigated losses in graphene by exploring real-space profiles of plasmon standing waves formed between the tip of our nano-probe and the edges of the samples. Plasmon dissipation quantified through this analysis is linked to the exotic electrodynamics of graphene 10 . Standard plasmonic figures of merit of our tunable graphene devices surpass those of common metal-based structures.

Control of magnetism by applied voltage is desirable for spintronics applications. Finding a suitable material remains an elusive goal, with only a few candidates found so far. Graphene is one of them and attracts interest because of its weak spin–orbit interaction, the ability to control electronic properties by the electric field effect and the possibility to introduce paramagnetic centres such as vacancies and adatoms. Here we show that the magnetism of adatoms in graphene is itinerant and can be controlled by doping, so that magnetic moments are switched on and off. The much-discussed vacancy magnetism is found to have a dual origin, with two approximately equal contributions; one from itinerant magnetism and the other from dangling bonds. Our work suggests that graphene’s spin transport can be controlled by the field effect, similar to its electronic and optical properties, and that spin diffusion can be significantly enhanced above a certain carrier density. Local magnetic properties that can be controlled by an applied electric field are desirable for spintronics applications. Nair et al. show that tuning carrier concentration by molecular doping or electric field can be used to control adatoms magnetism on graphene, enabling magnetic moments to be switched on and off.