Toward tunable band gap and tunable dirac point in bilayer graphene with molecular doping

The bilayer graphene has attracted considerable attention for potential applications in future electronics and optoelectronics because of the feasibility to tune its band gap with a vertical displacement field to break the inversion symmetry. Surface chemical doping in bilayer graphene can induce an additional offset voltage to fundamentally affect the vertical displacement field and the band gap opening in bilayer graphene. In this study, we investigate the effect of chemical molecular doping on band gap opening in bilayer graphene devices with single or dual gate modulation. Chemical doping with benzyl viologen molecules modulates the displacement field to allow the opening of a transport band gap and the increase of the on/off ratio in the bilayer graphene transistors. Additionally, Fermi energy level in the opened gap can be rationally controlled by the amount of molecular doping to obtain bilayer graphene transistors with tunable Dirac points, which can be readily configured into functional devices, such as complementary inverters.     

Giant two-photon absorption in bilayer graphene

We present a quantum perturbation theory on two-photon absorption (2PA) in monolayer and bilayer graphene which is Bernal-stacked. The theory shows that 2PA is significantly greater in bilayer graphene than monolayer graphene in the visible and infrared spectrum (up to 3 μm) with a resonant 2PA coefficient of up to ～0.2 cm/W located at half of the bandgap energy, γ(1) = 0.4 eV. In the visible and terahertz region, 2PA exhibits a light frequency dependence of ω(-3) in bilayer graphene, while it is proportional to ω(-4) for monolayer graphene at all photon energies. Within the same order of magnitude, the 2PA theory is in agreement with our Z-scan measurements on high-quality epitaxial bilayer graphene deposited on SiC substrate at light wavelength of 780 and 1100 nm.     

Wafer scale homogeneous bilayer graphene films by chemical vapor deposition

The discovery of electric field induced band gap opening in bilayer graphene opens a new door for making semiconducting graphene without aggressive size scaling or using expensive substrates. However, bilayer graphene samples have been limited to μm(2) size scale thus far, and synthesis of wafer scale bilayer graphene poses a tremendous challenge. Here we report homogeneous bilayer graphene films over at least a 2 in. × 2 in. area, synthesized by chemical vapor deposition on copper foil and subsequently transferred to arbitrary substrates. The bilayer nature of graphene film is verified by Raman spectroscopy, atomic force microscopy, and transmission electron microscopy. Importantly, spatially resolved Raman spectroscopy confirms a bilayer coverage of over 99%. The homogeneity of the film is further supported by electrical transport measurements on dual-gate bilayer graphene transistors, in which a band gap opening is observed in 98% of the devices.     

High on/off ratios in bilayer graphene field effect transistors realized by surface dopants

The unique property of bilayer graphene to show a band gap tunable by external electrical fields enables a variety of different device concepts with novel functionalities for electronic, optoelectronic, and sensor applications. So far the operation of bilayer graphene-based field effect transistors requires two individual gates to vary the channel's conductance and to create a band gap. In this paper, we report on a method to increase the on/off ratio in single gated bilayer graphene field effect transistors by adsorbate doping. The adsorbate dopants on the upper side of the graphene establish a displacement field perpendicular to the graphene surface breaking the inversion symmetry of the two graphene layers. Low-temperature measurements indicate that the increased on/off ratio is caused by the opening of a mobility gap.     

Phonon and structural changes in deformed Bernal stacked bilayer graphene

We present the first Raman spectroscopic study of Bernal bilayer graphene flakes under uniaxial tension. Apart from a purely mechanical behavior in flake regions where both layers are strained evenly, certain effects stem from inhomogeneous stress distribution across the layers. These phenomena such as the removal of inversion symmetry in bilayer graphene may have important implications in the band gap engineering, providing an alternative route to induce the formation of a band gap.     

Observation of Electrically Tunable van Hove Singularities in Twisted Bilayer Graphene from NanoARPES

The possibility of triggering correlated phenomena by placing a singularity of the density of states near the Fermi energy remains an intriguing avenue toward engineering the properties of quantum materials. Twisted bilayer graphene is a key material in this regard because the superlattice produced by the rotated graphene layers introduces a van Hove singularity and flat bands near the Fermi energy that cause the emergence of numerous correlated phases, including superconductivity. Direct demonstration of electrostatic control of the superlattice bands over a wide energy range has, so far, been critically missing. This work examines the effect of electrical doping on the electronic band structure of twisted bilayer graphene using a back-gated device architecture for angle-resolved photoemission measurements with a nano-focused light spot. A twist angle of 12.2° is selected such that the superlattice Brillouin zone is sufficiently large to enable identification of van Hove singularities and flat band segments in momentum space. The doping dependence of these features is extracted over an energy range of 0.4 eV, expanding the combinations of twist angle and doping where they can be placed at the Fermi energy and thereby induce new correlated electronic phases in twisted bilayer graphene.     

Tunable band gaps in bilayer graphene-BN heterostructures

We investigate band gap tuning of bilayer graphene between hexagonal boron nitride sheets, by external electric fields. Using density functional theory, we show that the gap is continuously tunable from 0 to 0.2 eV and is robust to stacking disorder. Moreover, boron nitride sheets do not alter the fundamental response from that of free-standing bilayer graphene, apart from additional screening. The calculations suggest that graphene-boron nitride heterostructures could provide a viable route to graphene-based electronic devices.     

A Density Functional Theory study of the chemical surface modification of β-SiC nanopores

The dependence of the electronic band structure and density of states on the chemical surface passivation of cubic porous silicon carbide (PSiC) is investigated by means of the ab-initio Density Functional Theory and the supercell method in which pores with different sizes and morphologies were created. The porous structures were modeled by removing atoms in the [0 0 1] direction producing two different surface chemistries; one with both Silicon (Si) and Carbon (C) atoms and the other with only Si or C atoms. The changes in the electronic band gap due to a Si-rich and C-rich phase in the porous surfaces are studied with two kind of surface passivation, one with hydrogen atoms and other with a combination between hydrogen and oxygen atoms. The calculations show that for the hydrogenated case, the band gap is larger for the C-rich than for the Si-rich case. For the partial oxygenation the tendency is contrary, by decreasing and increasing the band gap for the C-rich and Si-rich configuration, respectively, according to the percentage of oxygen in the pore surface.     

The effects of impurity doping on the optical properties of biased bilayer graphene

We address the optical conductivity of doped AA-stacked bilayer graphene in the presence of a finite bias voltage at finite temperature. The effect of scattering by dilute charged impurities is discussed in terms of the self-consistent Born approximation. Green's function approach has been implemented to find the behavior of optical conductivity of bilayer graphene within linear response theory. We have found the frequency dependence of optical conductivity for different values of concentration and scattering strength of dopant impurity. Also the dependence of optical conductivity on the impurity concentration and bias voltage has been investigated in details. A peak appears in the plot of optical conductivity versus impurity concentration for different values of chemical potential. Furthermore we find optical conductivity reduces with frequency for any impurity concentration and scattering strength.     

Using the G' Raman cross-section to understand the phonon dynamics in bilayer graphene systems

The G' (or 2D) Raman band of AB stacked bilayer graphene comes from a double resonance Raman (DRR) process and is composed of four peaks (P(11), P(12), P(21), and P(22)). In this work, the integrated areas (IA) of these four peaks are analyzed as a function of the laser power for different laser lines. We show that the dependence of the IA of each peak on temperature is different for each distinct laser excitation energy. This special dependence is explained in terms of the electron-phonon coupling and the relaxation of the photon-excited electron. In this DRR process, the electron is scattered by an iTO phonon from a K to an inequivalent K' point of the Brillouin zone. Here, we show that this electron relaxes while in the conduction band before being scattered by an iTO phonon due to the short relaxation time of the excited electron, and the carrier relaxation occurs predominantly by emitting a low-energy acoustic phonon. The different combinations of relaxation processes determine the relative intensities of the four peaks that give rise to the G' band. Some peaks show an increase of their IA at the expense of others, thereby making the IA of the peaks both different from each other and dependent on laser excitation energy and on power level. Also, we report that the IA of the G' mode excited at 532 nm, shows a resonance regime involving ZO' phonons (related to the interlayer breathing mode in bilayer graphene systems) in which a saturation of what we call the P(12) process occurs. This effect gives important information about the electron and phonon dynamics and needs to be taken into account for certain applications of bilayer graphene in the field of nanotechnology.     

Electronic properties of GaxIn1−xP from pseudopotential calculations

Based on a pseudopotential scheme within the virtual crystal approximation, we present a theoretical investigation of the electronic properties of Ga_xIn_1−xP. The effect of alloy disorder on energy band-gaps has been examined and found to be not negligible. The composition dependence of energy band-gaps and electron effective mass is shown to be non-linear. In agreement with experiment, a direct-to-indirect band-gap crossover is found to occur close to x = 0.7. Besides, the electron valence and conduction charge densities for Ga_0.50In_0.50P derived from pseudopotential band-structure calculations are reported and trends in bonding and ionicity are discussed.     

Transport spectroscopy of symmetry-broken insulating states in bilayer graphene

Bilayer graphene is an attractive platform for studying new two-dimensional electron physics, because its flat energy bands are sensitive to out-of-plane electric fields and these bands magnify electron-electron interaction effects. Theory predicts a variety of interesting broken symmetry states when the electron density is at the carrier neutrality point, and some of these states are characterized by spontaneous mass gaps, which lead to insulating behaviour. These proposed gaps are analogous to the masses generated by broken symmetries in particle physics, and they give rise to large Berry phase effects accompanied by spontaneous quantum Hall effects. Although recent experiments have provided evidence for strong electronic correlations near the charge neutrality point, the presence of gaps remains controversial. Here, we report transport measurements in ultraclean double-gated bilayer graphene and use source-drain bias as a spectroscopic tool to resolve a gap of ～2 meV at the charge neutrality point. The gap can be closed by a perpendicular electric field of strength ～15 mV nm(-1), but it increases monotonically with magnetic field, with an apparent particle-hole asymmetry above the gap. These data represent the first spectroscopic mapping of the ground states in bilayer graphene in the presence of both electric and magnetic fields.     

Study of the indirect interaction in the quantum dots of the graphene bilayer in the framework of the <Emphasis Type="Italic">s-d</Emphasis> model

Specific features of the RKKY interaction in triangular quantum dots of the graphene bilayer have been studied according to the s-d exchange model. Theoretical model calculations showed that, with allowance for an electron spectrum limited by the Dirac approximation, the dependence of the exchange interaction energy on the distance between spins ceases to possess a periodic (oscillatory) character.     

Irradiated bilayer graphene

We describe the gated bilayer graphene system when it is subjected to intense terahertz frequency electromagnetic radiation. We examine the electron band structure and density of states via exact diagonalization methods within Floquet theory. We find that dynamical states are induced which lead to modification of the band structure. We first examine the situation where there is no external magnetic field. In the unbiased case, dynamical gaps appear in the spectrum which manifest as dips in the density of states. For finite inter-layer bias (where a static gap is present in the band structure of unirradiated bilayer graphene), dynamical states may be induced in the static gap. These states can show a high degree of valley polarization. When the system is placed in a strong magnetic field, the radiation induces coupling between the Landau levels which allows dynamical levels to exist. For strong fields, this means the Landau levels are smeared to form a near-continuum of states.     

Magnetotransport properties of quasi-free-standing epitaxial graphene bilayer on SiC: evidence for Bernal stacking

We investigate the magnetotransport properties of quasi-free-standing epitaxial graphene bilayer on SiC, grown by atmospheric pressure graphitization in Ar, followed by H(2) intercalation. At the charge neutrality point, the longitudinal resistance shows an insulating behavior, which follows a temperature dependence consistent with variable range hopping transport in a gapped state. In a perpendicular magnetic field, we observe quantum Hall states (QHSs) both at filling factors (ν) multiples of four (ν = 4, 8, 12), as well as broken valley symmetry QHSs at ν = 0 and ν = 6. These results unambiguously show that the quasi-free-standing graphene bilayer grown on the Si-face of SiC exhibits Bernal stacking.     

Graphene-metal interface: two-terminal resistance of low-mobility graphene in high magnetic fields

The two-terminal magnetotransport of a single graphene layer was investigated up to a field of 55 T. The dependence of the electron transmission probability at the organo-metallic interface between the graphene and the metal electrodes was studied as a function of filling factor and electron density. A resistance-plateau spanning several tens of tesla width was observed. We argue that this plateau originates from an augmented sublattice spin-splitting due to the high surface-impurity concentration of the graphene layer. At electron densities close to the Dirac point, fingerprints of a thermally activated energy gap were observed.     

Electronic excited states in bilayer graphene double quantum dots

We report tunneling spectroscopy experiments on a bilayer graphene double quantum dot device that can be tuned by all-graphene lateral gates. The diameter of the two quantum dots are around 50 nm and the constrictions acting as tunneling barriers are 30 nm in width. The double quantum dot features additional energies on the order of 20 meV. Charge stability diagrams allow us to study the tunable interdot coupling energy as well as the spectrum of the electronic excited states on a number of individual triple points over a large energy range. The obtained constant level spacing of 1.75 meV over a wide energy range is in good agreement with the expected single-particle energy spacing in bilayer graphene quantum dots. Finally, we investigate the evolution of the electronic excited states in a parallel magnetic field.     

Strong suppression of electrical noise in bilayer graphene nanodevices

Low-frequency 1/f noise is ubiquitous and dominates the signal-to-noise performance in nanodevices. Here we investigate the noise characteristics of single-layer and bilayer graphene nanodevices and uncover an unexpected 1/f noise behavior for bilayer devices. Graphene is a single layer of graphite, where carbon atoms form a two-dimensional (2D) honeycomb lattice. Despite the similar composition, bilayer graphene (two graphene monolayers stacked in the natural graphite order) is a distinct 2D system with a different band structure and electrical properties. 1,2In graphene monolayers, the 1/f noise is found to follow Hooge's empirical relation with a noise parameter comparable to that of bulk semiconductors. However, this 1/f noise is strongly suppressed in bilayer graphene devices and exhibits an unusual dependence on the carrier density, different from most other materials. The unexpected noise behavior in graphene bilayers is associated with its unique band structure that varies with the charge distribution among the two layers, resulting in an effective screening of potential fluctuations due to external impurity charges. The findings here point to exciting opportunities for graphene bilayers in low-noise applications.     

Temperature dependence of the Raman spectra of graphene and graphene multilayers

We investigated the temperature dependence of the frequency of G peak in the Raman spectra of graphene on Si/SiO2 substrates. The micro-Raman spectroscopy was carried out under the 488 nm laser excitation over the temperature range from -190 to +100 degrees C. The extracted value of the temperature coefficient of G mode of graphene is chi = -0.016 cm-1/ degrees C for the single layer and chi = -0.015 cm-1/ degrees C for the bilayer. The obtained results shed light on the anharmonic properties of graphene.     

Enhancement of mechanical and tribological properties in AISI D3 steel substrates by using a non-isostructural CrN/AlN multilayer coating

Enhancement of mechanical and tribological properties on AISI D3 steel surfaces coated with CrN/AlN multilayer systems deposited in various bilayer periods (Λ) via magnetron sputtering has been studied in this work exhaustively. The coatings were characterized in terms of structural, chemical, morphological, mechanical and tribological properties by X-ray diffraction (XRD), electron dispersive spectrograph, atomic force microscopy, scanning and transmission electron microscopy, nanoindentation, pin-on-disc and scratch tests. The failure mode mechanisms were observed via optical microscopy. Results from X-ray diffraction analysis revealed that the crystal structure of CrN/AlN multilayer coatings has a NaCl-type lattice structure and hexagonal structure (wurtzite-type) for CrN and AlN, respectively, i.e., made was non-isostructural multilayers. An enhancement of both hardness and elastic modulus up to 28 GPa and 280 GPa, respectively, was observed as the bilayer periods (Λ) in the coatings were decreased. The sample with a bilayer period (Λ) of 60 nm and bilayer number n  =  50 showed the lowest friction coefficient (∼0.18) and the highest critical load (43 N), corresponding to 2.2 and 1.6 times better than those values for the coating deposited with n = 1, respectively. The best behavior was obtained when the bilayer period (Λ) is 60 nm (n = 50), giving the highest hardness 28 GPa and elastic modulus of 280 GPa, the lowest friction coefficient (∼0.18) and the highest critical load of 43 N. These results indicate an enhancement of mechanical, tribological and adhesion properties, comparing to the CrN/AlN multilayer systems with 1 bilayer at 28%, 21%, 40%, and 30%, respectively. This enhancement in hardness and toughness for multilayer coatings could be attributed to the different mechanisms for layer formation with nanometric thickness such as the Hall–Petch effect and the number of interfaces that act as obstacles for the crack deflection and dissipation of crack energy.