Electric Field and Strain Tuning of 2D Semiconductor van der Waals Heterostructures for Tunnel Field-Effect Transistors.

Heterostacks consisting of low-dimensional materials are attractive candidates for future electronic nanodevices in the post-silicon era. In this paper, using first-principles calculations based on density functional theory (DFT), we explore the structural and electronic properties of MoTe2/ZrS2 heterostructures with various stacking patterns and thicknesses. Our simulations show that the valence band (VB) edge of MoTe2 is almost aligned with the conduction band (CB) edge of ZrS2, and (MoTe2)m/(ZrS2)m (m = 1, 2) heterostructures exhibit the long-sought broken gap band alignment, which is pivotal for realizing tunneling transistors. Electrons are found to spontaneously flow from MoTe2 to ZrS2, and the system resembles an ultrascaled parallel plate capacitor with an intrinsic electric field pointed from MoTe2 to ZrS2. The effects of strain and external electric fields on the electronic properties are also investigated. For vertical compressive strains, the charge transfer increases due to the decreased coupling between the layers, whereas tensile strains lead to the opposite behavior. For negative electric fields a transition from the type-III to the type-II band alignment is induced. In contrast, by increasing the positive electric fields, a larger overlap between the valence and conduction bands is observed, leading to a larger band-to-band tunneling (BTBT) current. Low-strained heterostructures with various rotation angles between the constituent layers are also considered. We find only small variations in the energies of the VB and CB edges with respect to the Fermi level, for different rotation angles up to 30°. Overall, our simulations offer insights into the fundamental properties of low-dimensional heterostructures and pave the way for their future application in energy-efficient electronic nanodevices.

Accurate graphene quantum Hall arrays for the new International System of Units.

Graphene quantum Hall effect (QHE) resistance standards have the potential to provide superior realizations of three key units in the new International System of Units (SI): the ohm, the ampere, and the kilogram (Kibble Balance). However, these prospects require different resistance values than practically achievable in single graphene devices (~12.9 kΩ), and they need bias currents two orders of magnitude higher than typical breakdown currents IC ~ 100 µA. Here we present experiments on quantization accuracy of a 236-element quantum Hall array (QHA), demonstrating RK/236 ≈ 109 Ω with 0.2 part-per-billion (nΩ/Ω) accuracy with IC ≥ 5 mA (~1 nΩ/Ω accuracy for IC = 8.5 mA), using epitaxial graphene on silicon carbide (epigraphene). The array accuracy, comparable to the most precise universality tests of QHE, together with the scalability and reliability of this approach, pave the road for wider use of graphene in the new SI and beyond.

On the nature of decoherence in quantum circuits: Revealing the structural motif of the surface radicals in α-Al2O3.

Quantum information technology puts stringent demands on the quality of materials and interfaces in the pursuit of increased device coherence. Yet, little is known about the chemical structure and origins of paramagnetic impurities that produce flux/charge noise that causes decoherence of fragile quantum states and impedes the progress toward large-scale quantum computing. Here, we perform high magnetic field electron paramagnetic resonance (HFEPR) and hyperfine multispin spectroscopy on α-Al2O3, a common substrate for quantum devices. In its amorphous form, α-Al2O3 is also unavoidably present in aluminum-based superconducting circuits and qubits. The detected paramagnetic centers are immanent to the surface and have a well-defined but highly complex structure that extends over multiple hydrogen, aluminum, and oxygen atoms. Modeling reveals that the radicals likely originate from well-known reactive oxygen chemistry common to many metal oxides. We discuss how EPR spectroscopy might benefit the search for surface passivation and decoherence mitigation strategies.

Pulsed electron spin resonance of an organic microcrystal by dispersive readout.

We establish a testbed system for the development of high-sensitivity Electron Spin Resonance (ESR) techniques for small samples at cryogenic temperatures. Our system consists of a NbN thin-film planar superconducting microresonator designed to have a concentrated mode volume to couple to a small amount of paramagnetic material, and to be resilient to magnetic fields of up to 400mT. At 65mK we measure high-cooperativity coupling (C≈19) to an organic radical microcrystal containing 1012 spins in a pico-litre volume. We detect the spin-lattice decoherence rate via the dispersive frequency shift of the resonator. Techniques such as these could be suitable for applications in quantum information as well as for pulsed ESR interrogation of very few spins to provide insights into the surface chemistry of, for example, the material defects in superconducting quantum processors.

Author Correction: Apparent Power Law Scaling of Variable Range Hopping Conduction in Carbonized Polymer Nanofibers.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Effect of graphene substrate type on formation of Bi2Se3 nanoplates.

Knowledge of nucleation and further growth of Bi2Se3 nanoplates on different substrates is crucial for obtaining ultrathin nanostructures and films of this material by physical vapour deposition technique. In this work, Bi2Se3 nanoplates were deposited under the same experimental conditions on different types of graphene substrates (as-transferred and post-annealed chemical vapour deposition grown monolayer graphene, monolayer graphene grown on silicon carbide substrate). Dimensions of the nanoplates deposited on graphene substrates were compared with the dimensions of the nanoplates deposited on mechanically exfoliated mica and highly ordered pyrolytic graphite flakes used as reference substrates. The influence of different graphene substrates on nucleation and further lateral and vertical growth of the Bi2Se3 nanoplates is analysed. Possibility to obtain ultrathin Bi2Se3 thin films on these substrates is evaluated. Between the substrates considered in this work, graphene grown on silicon carbide is found to be the most promising substrate for obtaining of 1-5 nm thick Bi2Se3 films.

Uniform doping of graphene close to the Dirac point by polymer-assisted assembly of molecular dopants.

Tuning the charge carrier density of two-dimensional (2D) materials by incorporating dopants into the crystal lattice is a challenging task. An attractive alternative is the surface transfer doping by adsorption of molecules on 2D crystals, which can lead to ordered molecular arrays. However, such systems, demonstrated in ultra-high vacuum conditions (UHV), are often unstable in ambient conditions. Here we show that air-stable doping of epitaxial graphene on SiC-achieved by spin-coating deposition of 2,3,5,6-tetrafluoro-tetracyano-quino-dimethane (F4TCNQ) incorporated in poly(methyl-methacrylate)-proceeds via the spontaneous accumulation of dopants at the graphene-polymer interface and by the formation of a charge-transfer complex that yields low-disorder, charge-neutral, large-area graphene with carrier mobilities ~70 000 cm2 V-1 s-1 at cryogenic temperatures. The assembly of dopants on 2D materials assisted by a polymer matrix, demonstrated by spin-coating wafer-scale substrates in ambient conditions, opens up a scalable technological route toward expanding the functionality of 2D materials.

Probing variable range hopping lengths by magneto conductance in carbonized polymer nanofibers.

Using magneto transport, we probe hopping length scales in the variable range hopping conduction of carbonized polyacetylene and polyaniline nanofibers. In contrast to pristine polyacetylene nanofibers that show vanishing magneto conductance at large electric fields, carbonized polymer nanofibers display a negative magneto conductance that decreases in magnitude but remains finite with respect to the electric field. We show that this behavior of magneto conductance is an indicator of the electric field and temperature dependence of hopping length in the gradual transition from the thermally activated to the activation-less electric field driven variable range hopping transport. This reveals magneto transport as a useful tool to probe hopping lengths in the non-linear hopping regime.

Apparent Power Law Scaling of Variable Range Hopping Conduction in Carbonized Polymer Nanofibers.

We induce dramatic changes in the structure of conducting polymer nanofibers by carbonization at 800 °C and compare charge transport properties between carbonized and pristine nanofibers. Despite the profound structural differences, both types of systems display power law dependence of current with voltage and temperature, and all measurements can be scaled into a single universal curve. We analyze our experimental data in the framework of variable range hopping and argue that this mechanism can explain transport properties of pristine polymer nanofibers as well.

Influence of Impurity Spin Dynamics on Quantum Transport in Epitaxial Graphene.

Experimental evidence from both spin-valve and quantum transport measurements points towards unexpectedly fast spin relaxation in graphene. We report magnetotransport studies of epitaxial graphene on SiC in a vector magnetic field showing that spin relaxation, detected using weak-localization analysis, is suppressed by an in-plane magnetic field B(∥), and thereby proving that it is caused at least in part by spinful scatterers. A nonmonotonic dependence of the effective decoherence rate on B(∥) reveals the intricate role of the scatterers' spin dynamics in forming the interference correction to the conductivity, an effect that has gone unnoticed in earlier weak localization studies.

Nanopatterning of mobile lipid monolayers on electron-beam-sculpted Teflon AF surfaces.

Direct electron-beam lithography is used to fabricate nanostructured Teflon AF surfaces, which are utilized to pattern surface-supported monolayer phospholipid films with 50 nm lateral feature size. In comparison with unexposed Teflon AF coatings, e-beam-irradiated areas show reduced surface tension and surface potential. For phospholipid monolayer spreading experiments, these areas can be designed to function as barriers that enclose unexposed areas of nanometer dimensions and confine the lipid film within. We show that the effectiveness of the barrier is defined by pattern geometry and radiation dose. This surface preparation technique represents an efficient, yet simple, nanopatterning strategy supporting studies of lipid monolayer behavior in ultraconfined spaces. The generated structures are useful for imaging studies of biomimetic membranes and other specialized surface applications requiring spatially controlled formation of self-assembled, molecularly thin films on optically transparent patterned polymer surfaces with very low autofluorescence.

Quantum Hall effect and quantum point contact in bilayer-patched epitaxial graphene.

We study an epitaxial graphene monolayer with bilayer inclusions via magnetotransport measurements and scanning gate microscopy at low temperatures. We find that bilayer inclusions can be metallic or insulating depending on the initial and gated carrier density. The metallic bilayers act as equipotential shorts for edge currents, while closely spaced insulating bilayers guide the flow of electrons in the monolayer constriction, which was locally gated using a scanning gate probe.

Express optical analysis of epitaxial graphene on SiC: impact of morphology on quantum transport.

We show that inspection with an optical microscope allows surprisingly simple and accurate identification of single and multilayer graphene domains in epitaxial graphene on silicon carbide (SiC/G) and is informative about nanoscopic details of the SiC topography, making it ideal for rapid and noninvasive quality control of as-grown SiC/G. As an illustration of the power of the method, we apply it to demonstrate the correlations between graphene morphology and its electronic properties by quantum magneto-transport.

Aligned growth of gold nanorods in PMMA channels: parallel preparation of nanogaps.

We demonstrate alignment and positional control of gold nanorods grown in situ on substrates using a seed-mediated synthetic approach. Alignment control is obtained by directing the growth of spherical nanoparticle seeds into nanorods in well-defined poly(methyl methacrylate) nanochannels. Substrates with prepatterned metallic electrodes provide an additional handle for the position of the gold nanorods and yield nanometer-sized gaps between the electrode and nanorod. The presented approach is a novel demonstration of bottom-up device fabrication of multiple nanogap junctions on a single chip mediated viain situ growth of gold nanorods acting as nanoelectrodes.

Disordered Fermi liquid in epitaxial graphene from quantum transport measurements.

We have performed magnetotransport measurements on monolayer epitaxial graphene and analyzed them in the framework of the disordered Fermi liquid theory. We have separated the electron-electron and weak-localization contributions to resistivity and demonstrated the phase coherence over a micrometer length scale, setting the limit of at least 50 ps on the spin relaxation time in this material.

Towards a quantum resistance standard based on epitaxial graphene.

The quantum Hall effect allows the international standard for resistance to be defined in terms of the electron charge and Planck's constant alone. The effect comprises the quantization of the Hall resistance in two-dimensional electron systems in rational fractions of R(K) = h/e(2) = 25,812.807557(18) Omega, the resistance quantum. Despite 30 years of research into the quantum Hall effect, the level of precision necessary for metrology--a few parts per billion--has been achieved only in silicon and iii-v heterostructure devices. Graphene should, in principle, be an ideal material for a quantum resistance standard, because it is inherently two-dimensional and its discrete electron energy levels in a magnetic field (the Landau levels) are widely spaced. However, the precisions demonstrated so far have been lower than one part per million. Here, we report a quantum Hall resistance quantization accuracy of three parts per billion in monolayer epitaxial graphene at 300 mK, four orders of magnitude better than previously reported. Moreover, by demonstrating the structural integrity and uniformity of graphene over hundreds of micrometres, as well as reproducible mobility and carrier concentrations across a half-centimetre wafer, these results boost the prospects of using epitaxial graphene in applications beyond quantum metrology.

Nanoelectromechanical switch operating by tunneling of an entire C60 molecule.

We present a solid state single molecule electronic device where switching between two states with different conductance happens predominantly by tunneling of an entire C60 molecule. This conclusion is based on a novel statistical analysis of approximately 10(5) switching events. The analysis yields (i) the relative contribution of tunneling, current induced heating and thermal fluctuations to the switching mechanism, (ii) the voltage dependent energy barrier (approximately 100-200 meV) separating the two states of the switch and (iii) the switching attempt frequency, omega0, corresponding to a 2.8 meV mode, which is most likely rotational.

Electronic transport in single molecule junctions: control of the molecule-electrode coupling through intramolecular tunneling barriers.

We report on single molecule electron transport measurements of two oligophenylenevinylene (OPV3) derivatives placed in a nanogap between gold (Au) or lead (Pb) electrodes in a field effect transistor device. Both derivatives contain thiol end groups that allow chemical binding to the electrodes. One derivative has additional methylene groups separating the thiols from the delocalized pi-electron system. The insertion of methylene groups changes the open state conductance by 3-4 orders of magnitude and changes the transport mechanism from a coherent regime with finite zero-bias conductance to sequential tunneling and Coulomb blockade behavior.