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. © 2022, The Author(s).

We have demonstrated quantum Hall resistance measurements with metrological accuracy in a relatively easy to use and compact cryogen-free system operating at a temperature of around 3.8 K and magnetic field below 5 T. This advance in technology is due to the unique properties of epitaxial graphene on silicon carbide (SiC) which lifts the stringent requirements for quantum hall effect seen in conventional semiconductors. This paper presents the processes involved in fabrication and characterization of metrologically viable epitaxial graphene samples.

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. 

Here we demonstrate a stable and tunable method to alter the carrier concentration of epitaxial graphene grown on silicon carbide. This technique relies on chemical doping by an acceptor molecule. Through careful tuning one can produce chemically doped graphene quantum resistance devices which show long-term stability in ambient conditions and have performance comparable to that of GaAs quantum resistance standards. This development paves the way for controlled device fabrication of graphene quantum hall resistance standards, which can be reliably tailored to operate below 5 T and above 4 K out-of-the-box, without further adjustments from the end-user.

One of the aspirations of quantum metrology is to deliver primary standards directly to end-users thereby significantly shortening the traceability chains and enabling more accurate products. Epitaxial graphene grown on silicon carbide (epigraphene) is known to be a viable candidate for a primary realisation of a quantum Hall resistance standard, surpassing conventional semiconductor two-dimensional electron gases, such as those based on GaAs, in terms of performance at higher temperatures and lower magnetic fields. The bottleneck in the realisation of a turn-key quantum resistance standard requiring minimum user intervention has so far been the need to fine-tune the carrier density in this material to fit the constraints imposed by a simple cryo-magnetic system. Previously demonstrated methods, such as via photo-chemistry or corona discharge, require application prior to every cool-down as well as specialist knowledge and equipment. To this end we perform metrological evaluation of epigraphene with carrier density tuned by a recently reported permanent molecular doping technique. Measurements at two National Metrology Institutes confirm accurate resistance quantisation below 5n-1. Furthermore, samples show no significant drift in carrier concentration and performance on multiple thermal cycles over three years. This development paves the way for dissemination of primary resistance standards based on epigraphene

We show that epitaxial graphene on silicon carbide (epigraphene) grown at high temperatures (T >1850 °C) readily acts as material for implementing solar-blind ultraviolet (UV) detectors with outstanding performance. We present centimeter-sized epigraphene metal-semiconductor-metal (MSM) detectors with a peak external quantum efficiency of η ∼85% for wavelengths λ = 250-280 nm, corresponding to nearly 100% internal quantum efficiency when accounting for reflection losses. Zero bias operation is possible in asymmetric devices, with the responsivity to UV remaining as high as R = 134 mA/W, making this a self-powered detector. The low dark currents Io ∼50 fA translate into an estimated record high specific detectivity D = 3.5 × 1015 Jones. The performance that we demonstrate, together with material reproducibility, renders epigraphene technologically attractive to implement high-performance planar MSM devices with a low processing effort, including multi-pixel UV sensor arrays, suitable for a number of practical applications. © 2022 Author(s).

Wedemonstrate quantum Hall resistance measurements with metrological accuracy in a small cryogen-free system operating at a temperature of around 3.8Kand magnetic fields below 5 T. Operating this system requires little experimental knowledge or laboratory infrastructure, thereby greatly advancing the proliferation of primary quantum standards for precision electrical metrology. This significant advance in technology has come about as a result of the unique properties of epitaxial graphene on SiC.

We demonstrate quantum Hall resistance measurements with metrological accuracy in a small cryogen-free system operating at a temperature of around 3.8 K and magnetic fields below 5 T. We use this system to investigate the optimisation of graphene/SiC devices for maximum breakdown current. In addition we report the first characterisation of a cryogen-free cryogenic current comparator which enables entirely cryogen-free primary resistance metrology.

We present a study of quasi-free-standing monolayer graphene obtained by intercalation of Au atoms at the interface between the carbon buffer layer (Bu-L) and the silicon-terminated face (0001) of 4H-silicon carbide. Au intercalation is achieved by deposition of an atomically thin Au layer on the Bu-L followed by annealing at 850 °C in an argon atmosphere. We explore the intercalation of Au and decoupling of the Bu-L into quasi-free-standing monolayer graphene by surface science characterization and electron transport in top-gated electronic devices. By gate-dependent magnetotransport we find that the Au-intercalated buffer layer displays all properties of monolayer graphene, namely gate-tunable ambipolar transport across the Dirac point, but we find no observable enhancement of spin-orbit effects in the graphene layer, despite its proximity to the intercalated Au layer. 

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. 

We used large area, monolayer graphene epitaxially grown on SiC (0001) as contact electrodes for polymer nanofiber devices. Our fabrication process, which avoids polymer resist residues on the graphene surface, results in graphene-polyaniline nanofiber devices with Ohmic contacts and electrical conductivity comparable to that of Au-nanofiber devices. We further checked the thermal stability of the graphene contacts to polyaniline devices by annealing up to T = 800 °C, the temperature at which polyaniline nanofibers are carbonized but the graphene electrode remains intact. The thermal stability and Ohmic contact of polymer nanofibers are demonstrated here, which together with the chemical stability and atomic flatness of graphene, make epitaxial graphene on SiC an attractive contact material for future all-carbon electronic devices.

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. 

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The paper reports an interlaboratory comparison of low impedance measurements at frequencies relevant for electrochemical impedance spectroscopy (EIS) of commercial lithium-ion cells. The comparisons cover an impedance range from 50 ΌΩ to 100 mΩ across the full complex plane in a frequency range 0.01 Hz up to 5 kHz. A first comparison covered calibration of low impedance standards by reference digital sampling impedance setups in 4-terminal and 4 terminal-pair connections. A second comparison used commercial 4-terminal EIS meters to measure the low impedance standards characterised in the first comparison. 

The paper reports a results of series of interlaboratory comparisons of low impedance measurements at frequencies relevant for electrochemical impedance spectroscopy (EIS) of commercial lithium-ion cells. Two comparisons are presented. The first, bilateral comparison has focused on low impedance standards calibration in a full complex plane using digital sampling setups. The second comparison has focused on calibration and use of commercial 4-terminal battery EIS meters. Both comparisons have covered the impedance range from 50μ℧ to 100m℧ across the full complex plane in a frequency range from 0.01Hz up to 5kHz. Finally, the paper summarizes practices identified as critical for achieving measurement compatibility among various labs. © 2023 The Authors

The paper reports an interlaboratory comparison of low impedance measurements at frequencies relevant for electrochemical impedance spectroscopy (EIS) of commercial lithium-ion cells. The comparisons cover an impedance range from 50 μΩ to 100 mΩ across the full complex plane in a frequency range 0.01 Hz up to 5 kHz. A first comparison covered calibration of low impedance standards by reference digital sampling impedance setups in 4-terminal and 4 terminal-pair connections. A second comparison used commercial 4-terminal EIS meters to measure the low impedance standards characterised in the first comparison.

We report the lowest recorded levels of 1/ f noise for graphene-based devices, at the level of S V / V 2 = S I / I 2 = 4.4 × 10 − 16 (1/Hz), measured at f = 10 Hz ( S V / V 2 = S I / I 2 < 10 − 16 1/Hz for f > 100 Hz) in large-area epitaxial graphene on silicon carbide (epigraphene) Hall sensors. This performance is made possible through the combination of high material quality, low contact resistance achieved by edge contact fabrication process, homogeneous doping, and stable passivation of the graphene layer. Our study explores the nature of 1/ f noise as a function of carrier density and device geometry and includes data from Hall sensors with device area range spanning over six orders of magnitude, with characteristic device length ranging from L = 1 μm to 1 mm. In optimized graphene Hall sensors, we demonstrate arrays to be a viable route to improve further the magnetic field detection: a simple parallel connection of two devices displays record-high magnetic field sensitivity at room temperature, with minimum detectable magnetic field levels down to B min = 9.5 nT/√Hz. The remarkable low levels of 1/ f noise observed in epigraphene devices hold immense capacity for the design and fabrication of scalable epigraphene-based sensors with exceptional performance. © 2024 Author(s).

In this work we investigate the long-term stability of epitaxial graphene (epigraphene) quantum Hall resistance standards, including single devices and an array device composed of 236 elements providing (R K/236 ≈ 109 Ω) , with R K the von Klitzing constant. All devices utilize the established technique of chemical doping via molecular dopants to achieve homogenous doping and control over carrier density. However, optimal storage conditions and the long-term stability of molecular dopants for metrological applications have not been widely studied. In this work we aim to identify simple storage techniques that use readily available and cost-effective materials which provide long-term stability for devices without the need for advanced laboratory equipment. The devices are stored in glass bottles with four different environments: ambient, oxygen absorber, silica gel desiccant, and oxygen absorber/desiccant mixture. We have tracked the carrier densities, mobilities, and quantization accuracies of eight different epigraphene quantum Hall chips for over two years. We observe the highest stability (i.e. lowest change in carrier density) for samples stored in oxygen absorber/desiccant mixture, with a relative change in carrier density below 0.01% per day and no discernable degradation of quantization accuracy at the part-per-billion level. This storage technique yields a comparable stability to the currently established best storage method of inert nitrogen atmosphere, but it is much easier to realize in practice. It is possible to further optimize the mixture of oxygen absorber/desiccant for even greater stability performance in the future. We foresee that this technique can allow for simple and stable long-term storage of polymer-encapsulated molecular doped epigraphene quantum Hall standards, removing another barrier for their wide-spread use in practical metrology. 

We report a reliable and scalable fabrication method for producing electrical contacts to two-dimensional (2D) materials based on the tri-layer resist system. We demonstrate the applicability of this method in devices fabricated on epitaxial graphene on silicon carbide (epigraphene) used as a scalable 2D material platform. For epigraphene, data on nearly 70 contacts result in median values of the one-dimensional (1D) specific contact resistances ρc ∼ 67 Ω·μm and follow the Landauer quantum limit ρc ∼ n-1/2, consistently reaching values ρc &lt; 50 Ω·μm at high carrier densityn. As a proof of concept, we apply the same fabrication method to the transition metal dichalcogenide (TMDC) molybdenum disulfide (MoS2). Our edge contacts enable MoS2 field-effect transistor (FET) behavior with an ON/OFF ratio of &gt;106 at room temperature (&gt;109 at cryogenic temperatures). The fabrication route demonstrated here allows for contact metallization using thermal evaporation and also by sputtering, giving an additional flexibility when designing electrical interfaces, which is key in practical devices and when exploring the electrical properties of emerging materials. © 2023 The Authors. 

We present the first steps taken towards a graphene quantum Hall effect ac resistance standard at RISE. A new measurement setup has been developed including a graphene quantum Hall effect device suitable for the kilohertz range and a coaxial cryoprobe to be used together with a coaxial impedance bridge based on inductive voltage dividers. 1:1 ratio resistance measurements of the graphene device against a 12.9 kΩ ac resistance standard resulted in a linear frequency dependent (≈ 0.2(μΩ/Ω)/kHz) deviation from the quantized dc value.