Chiral Transport of Hot Carriers in Graphene in the Quantum Hall Regime.

Photocurrent (PC) measurements can reveal the relaxation dynamics of photoexcited hot carriers beyond the linear response of conventional transport experiments, a regime important for carrier multiplication. Here, we study the relaxation of carriers in graphene in the quantum Hall regime by accurately measuring the PC signal and modeling the data using optical Bloch equations. Our results lead to a unified understanding of the relaxation processes in graphene over different magnetic field strength regimes, which is governed by the interplay of Coulomb interactions and interactions with acoustic and optical phonons. Our data provide clear indications of a sizable carrier multiplication. Moreover, the oscillation pattern and the saturation behavior of PC are manifestations of not only the chiral transport properties of carriers in the quantum Hall regime but also the chirality change at the Dirac point, a characteristic feature of a relativistic quantum Hall effect.

Thermoelectric transport in coupled double layers with interlayer excitons and exciton condensation.

Quantum Boltzmann formalism is employed to study the transport properties of strongly-coupled double layer systems that enable the formation of interlayer excitons and exciton condensation. The importance of exciton formation, dissociation, and condensation is highlighted in the context of thermoelectric power generation, and this mathematical inquiry provides an alternative methodology to calculate the thermoelectric efficiency given the conditions of exciton formation. The Onsager relation for the Coulomb drag resistivity is shown to be valid even when exciton condensation is present. In addition, it is found that the traditional thermoelectric figure of merit is no longer sufficient to predict the efficiency of thermoelectric power generation in the presented situations. This inquiry offers insights for designing double layer systems, including their interlayer interactions, with enhanced thermoelectric energy conversion efficiency.

Atypical Quantized Resistances in Millimeter-Scale Epitaxial Graphene p-n Junctions.

We have demonstrated the millimeter-scale fabrication of monolayer epitaxial graphene p-n junction devices using simple ultraviolet photolithography, thereby significantly reducing device processing time compared to that of electron beam lithography typically used for obtaining sharp junctions. This work presents measurements yielding nonconventional, fractional multiples of the typical quantized Hall resistance at ν = 2 (R H ≈ 12906 Ω) that take the form: a b R H . Here, a and b have been observed to take on values such 1, 2, 3, and 5 to form various coefficients of R H. Additionally, we provide a framework for exploring future device configurations using the LTspice circuit simulator as a guide to understand the abundance of available fractions one may be able to measure. These results support the potential for drastically simplifying device processing time and may be used for many other two-dimensional materials.

Towards epitaxial graphene p-n junctions as electrically programmable quantum resistance standards.

We report the fabrication and measurement of top gated epitaxial graphene p-n junctions where exfoliated hexagonal boron nitride (h-BN) is used as the gate dielectric. The four-terminal longitudinal resistance across a single junction is well quantized at the von Klitzing constant [Formula: see text] with a relative uncertainty of 10-7. After the exploration of numerous parameter spaces, we summarize the conditions upon which these devices could function as potential resistance standards. Furthermore, we offer designs of programmable electrical resistance standards over six orders of magnitude by using external gating.

Quantum Hall device data monitoring following encapsulating polymer deposition.

The information provided in this data article will cover the growth parameters for monolayer, epitaxial graphene, as well as how to verify the layer homogeneity by confocal laser scanning and optical microscopy. The characterization of the subsequently fabricated quantum Hall device is shown for example cases during a series of environmental exposures. Quantum Hall data acquired from a CYTOP encapsulation is also provided. Data from Raman spectroscopy, atomic force microscopy, and other electrical property trends are shown. Lastly, quantum Hall effect data are presented from devices with deposited Parylene C films measuring 10.7 µm and 720 nm. All data are relevant for Rigosi et al. [1].

Examining epitaxial graphene surface conductivity and quantum Hall device stability with Parylene passivation.

Homogeneous, single-crystal, monolayer epitaxial graphene (EG) is the one of most promising candidates for the advancement of quantized Hall resistance (QHR) standards. A remaining challenge for the electrical characterization of EG-based quantum Hall devices as a useful tool for metrology is that they are electrically unstable when exposed to air due to the adsorption of and interaction with atmospheric molecular dopants. The resulting changes in the charge carrier density become apparent by variations in the surface conductivity, the charge carrier mobility, and may result in a transition from n-type to p-type conductivity. This work evaluates the use of Parylene C and Parylene N as passivation layers for EG. Electronic transport of EG quantum Hall devices and non-contact microwave perturbation measurements of millimeter-sized areas of EG are both performed on bare and Parylene coated samples to test the efficacy of the passivation layers. The reported results, showing a significant improvement in passivation due to Parylene deposition, suggest a method for the mass production of millimeter-scale graphene devices with stable electrical properties.

Measuring the dielectric and optical response of millimeter-scale amorphous and hexagonal boron nitride films grown on epitaxial graphene.

Monolayer epitaxial graphene (EG), grown on the Si face of SiC, is an advantageous material for a variety of electronic and optical applications. EG forms as a single crystal over millimeter-scale areas and consequently, the large scale single crystal can be utilized as a template for growth of other materials. In this work, we present the use of EG as a template to form millimeter-scale amorphous and hexagonal boron nitride (a-BN and h-BN) films. The a-BN is formed with pulsed laser deposition and the h-BN is grown with triethylboron (TEB) and NH3 precursors, making it the first metal organic chemical vapor deposition (MOCVD) process of this growth type performed on epitaxial graphene. A variety of optical and non-optical characterization methods are used to determine the optical absorption and dielectric functions of the EG, a-BN, and h-BN within the energy range of 1 eV to 8.5 eV. Furthermore, we report the first ellipsometric observation of high-energy resonant excitons in EG from the 4H polytype of SiC and an analysis on the interactions within the EG and h-BN heterostructure.

Confocal laser scanning microscopy for rapid optical characterization of graphene.

Two-dimensional (2D) materials such as graphene have become the focus of extensive research efforts in condensed matter physics. They provide opportunities for both fundamental research and applications across a wide range of industries. Ideally, characterization of graphene requires non-invasive techniques with single-atomic-layer thickness resolution and nanometer lateral resolution. Moreover, commercial application of graphene requires fast and large-area scanning capability. We demonstrate the optimized balance of image resolution and acquisition time of non-invasive confocal laser scanning microscopy (CLSM), rendering it an indispensable tool for rapid analysis of mass-produced graphene. It is powerful for analysis of 1-5 layers of exfoliated graphene on Si/SiO2, and allows us to distinguish the interfacial layer and 1-3 layers of epitaxial graphene on SiC substrates. Furthermore, CLSM shows excellent correlation with conventional optical microscopy, atomic force microscopy, Kelvin probe force microscopy, conductive atomic force microscopy, scanning electron microscopy and Raman mapping.

Graphene Devices for Tabletop and High-Current Quantized Hall Resistance Standards.

We report the performance of a quantum Hall resistance standard based on epitaxial graphene maintained in a 5-T tabletop cryocooler system. This quantum resistance standard requires no liquid helium and can operate continuously, allowing year-round accessibility to quantized Hall resistance measurements. The ν = 2 plateau, with a value of R K/2, also seen as R H, is used to scale to 1 kΩ using a binary cryogenic current comparator (BCCC) bridge and a direct current comparator (DCC) bridge. The uncertainties achieved with the BCCC are such as those obtained in the state-of-the-art measurements using GaAs-based devices. BCCC scaling methods can achieve large resistance ratios of 100 or more, and while room temperature DCC bridges have smaller ratios and lower current sensitivity, they can still provide alternate resistance scaling paths without the need for cryogens and superconducting electronics. Estimates of the relative uncertainties of the possible scaling methods are provided in this report, along with a discussion of the advantages of several scaling paths. The tabletop system limits are addressed as are potential solutions for using graphene standards at higher currents.

Quantum transport in graphene p-n junctions with moiré superlattice modulation.

We present simulations of quantum transport in graphene p-n junctions (pnJs) in which moiré superlattice potentials are incorporated to demonstrate the interplay between pnJs and moiré superlattice potentials. It is shown that the longitudinal and Hall resistivity maps can be strongly modulated by the pnJ profile, junction height, and moiré potentials. Device resistance measurements are subsequently performed on graphene/hexagonal- boron-nitride heterostructure samples with accurate alignment of crystallographic orientations to complement and support the simulation results.

Electrical Stabilization of Surface Resistivity in Epitaxial Graphene Systems by Amorphous Boron Nitride Encapsulation.

Homogeneous monolayer epitaxial graphene (EG) is an ideal candidate for the development of millimeter-sized devices with single-crystal domains. A clean fabrication process was used to produce EG-based devices, with n-type doping level of the order of 1012 cm-2. Generally, electrical properties of EG, such as longitudinal resistivity, remain unstable when devices are exposed to air due to adsorption of molecular dopants, whose presence shifts the carrier density close to the Dirac point (<1010 cm-2) or into the p-type regime. Here, we report experimental results on the use of amorphous boron nitride (a-BN) as an encapsulation layer, whereby EG can maintain its longitudinal resistivity and have its carrier density modulated. Furthermore, we exposed 12 devices to controlled temperatures of up to 85 °C and relative humidity of up to 85% and reported that an approximately 20 nm a-BN encapsulation thickness is sufficient to preserve their longitudinal resistivity to within 10% of the previously measured value. We monitored the electronic properties of our encapsulated and nonencapsulated EG samples by magnetotransport measurements, using a neodymium iron boron magnet. Our results have essential importance in the mass production of millimeter-scale graphene devices, with stable electrical properties.

Preservation of Surface Conductivity and Dielectric Loss Tangent in Large-Scale, Encapsulated Epitaxial Graphene Measured by Noncontact Microwave Cavity Perturbations.

Regarding the improvement of current quantized Hall resistance (QHR) standards, one promising avenue is the growth of homogeneous monolayer epitaxial graphene (EG). A clean and simple process is used to produce large, precise areas of EG. Properties like the surface conductivity and dielectric loss tangent remain unstable when EG is exposed to air due to doping from molecular adsorption. Experimental results are reported on the extraction of the surface conductivity and dielectric loss tangent from data taken with a noncontact resonance microwave cavity, assembled with an air-filled, standard R100 rectangular waveguide configuration. By using amorphous boron nitride (a-BN) as an encapsulation layer, stability of EG's electrical properties under ambient laboratory conditions is greatly improved. Moreover, samples are exposed to a variety of environmental and chemical conditions. Both thicknesses of a-BN encapsulation are sufficient to preserve surface conductivity and dielectric loss tangent to within 10% of its previously measured value, a result which has essential importance in the mass production of millimeter-scale graphene devices demonstrating electrical stability.

Phonon lateral confinement enables thermal rectification in asymmetric single-material nanostructures.

We show that thermal rectification (TR) in asymmetric graphene nanoribbons (GNRs) is originated from phonon confinement in the lateral dimension, which is a fundamentally new mechanism different from that in macroscopic heterojunctions. Our molecular dynamics simulations reveal that, though TR is significant in nanosized asymmetric GNRs, it diminishes at larger width. By solving the heat diffusion equation, we prove that TR is indeed absent in both the total heat transfer rate and local heat flux for bulk-size asymmetric single materials, regardless of the device geometry or the anisotropy of the thermal conductivity. For a deeper understanding of why lateral confinement is needed, we have performed phonon spectra analysis and shown that phonon lateral confinement can enable three possible mechanisms for TR: phonon spectra overlap, inseparable dependence of thermal conductivity on temperature and space, and phonon edge localization, which are essentially related to each other in a complicated manner. Under such guidance, we demonstrate that other asymmetric nanostructures, such as asymmetric nanowires, thin films, and quantum dots, of a single material are potentially high-performance thermal rectifiers.

Existence of negative differential thermal conductance in one-dimensional diffusive thermal transport.

We show that in a finite one-dimensional (1D) system with diffusive thermal transport described by the Fourier's law, negative differential thermal conductance (NDTC) cannot occur when the temperature at one end is fixed and there are no abrupt junctions. We demonstrate that NDTC in this case requires the presence of junction(s) with temperature-dependent thermal contact resistance (TCR). We derive a necessary and sufficient condition for the existence of NDTC in terms of the properties of the TCR for systems with a single junction. We show that under certain circumstances we even could have infinite (negative or positive) differential thermal conductance in the presence of the TCR. Our predictions provide theoretical basis for constructing NDTC-based devices, such as thermal amplifiers, oscillators, and logic devices.

Quantized Hall effect and Shubnikov-de Haas oscillations in highly doped Bi2Se3: evidence for layered transport of bulk carriers.

Bi2Se3 is an important semiconductor thermoelectric material and a prototype topological insulator. Here we report observation of Shubnikov-de Hass oscillations accompanied by quantized Hall resistances (R(xy)) in highly doped n-type Bi2Se3 with bulk carrier concentrations of few 10(19) cm(-3). Measurements under tilted magnetic fields show that the magnetotransport is 2D-like, where only the c-axis component of the magnetic field controls the Landau level formation. The quantized step size in 1/R(xy) is found to scale with the sample thickness, and average ~e(2)/h per quintuple layer. We show that the observed magnetotransport features do not come from the sample surface, but arise from the bulk of the sample acting as many parallel 2D electron systems to give a multilayered quantum Hall effect. In addition to revealing a new electronic property of Bi2Se3, our finding also has important implications for electronic transport studies of topological insulator materials.

Thermal conductivity and thermal rectification in graphene nanoribbons: a molecular dynamics study.

We have used molecular dynamics to calculate the thermal conductivity of symmetric and asymmetric graphene nanoribbons (GNRs) of several nanometers in size (up to approximately 4 nm wide and approximately 10 nm long). For symmetric nanoribbons, the calculated thermal conductivity (e.g., approximately 2000 W/m-K at 400 K for a 1.5 nm x 5.7 nm zigzag GNR) is on the similar order of magnitude of the experimentally measured value for graphene. We have investigated the effects of edge chirality and found that nanoribbons with zigzag edges have appreciably larger thermal conductivity than nanoribbons with armchair edges. For asymmetric nanoribbons, we have found significant thermal rectification. Among various triangularly shaped GNRs we investigated, the GNR with armchair bottom edge and a vertex angle of 30 degrees gives the maximal thermal rectification. We also studied the effect of defects and found that vacancies and edge roughness in the nanoribbons can significantly decrease the thermal conductivity. However, substantial thermal rectification is observed even in the presence of edge roughness.