Babak Fallahazad

The Role of Surface Oxygen in the Growth of Large Single-Crystal Graphene on Copper

Oxygen Control of Graphene Growth The growth of graphene on copper surfaces through the decomposition of hydrocarbons such as methane can result in a wide variety of crystal domain sizes and morphologies. Hao et al. (p. 720, published online 24 October; see the cover) found that the presence of surface oxygen could limit the number of nucleation sites and allowed centimeter-scale domains to grow through a diffusion-limited mechanism. The electrical conductivity of the graphene was comparable to that of exfoliated graphene. Oxygen treatment of a copper surface promoted the faster growth of compact, centimeter-scale graphene domains. The growth of high-quality single crystals of graphene by chemical vapor deposition on copper (Cu) has not always achieved control over domain size and morphology, and the results vary from lab to lab under presumably similar growth conditions. We discovered that oxygen (O) on the Cu surface substantially decreased the graphene nucleation density by passivating Cu surface active sites. Control of surface O enabled repeatable growth of centimeter-scale single-crystal graphene domains. Oxygen also accelerated graphene domain growth and shifted the growth kinetics from edge-attachment–limited to diffusion-limited. Correspondingly, the compact graphene domain shapes became dendritic. The electrical quality of the graphene films was equivalent to that of mechanically exfoliated graphene, in spite of being grown in the presence of O.

Field-effect transistors and intrinsic mobility in ultra-thin MoSe2 layers

We report the fabrication of back-gated field-effect transistors (FETs) using ultra-thin, mechanically exfoliated MoSe2 flakes. The MoSe2 FETs are n-type and possess a high gate modulation, with On/Off ratios larger than 106. The devices show asymmetric characteristics upon swapping the source and drain, a finding explained by the presence of Schottky barriers at the metal contact/MoSe2 interface. Using four-point, back-gated devices, we measure the intrinsic conductivity and mobility of MoSe2 as a function of gate bias, and temperature. Samples with a room temperature mobility of ∼ 50 cm2/V·s show a strong temperature dependence, suggesting phonons are a dominant scattering mechanism.

Dielectric thickness dependence of carrier mobility in graphene with HfO2 top dielectric

We investigate the carrier mobility in monolayer and bilayer graphene with a top HfO2 dielectric, as a function of the HfO2 film thickness and temperature. The results show that the carrier mobility decreases during the deposition of the first 2–4 nm of top dielectric and remains constant for thicker layers. The carrier mobility shows a relatively weak dependence on temperature indicating that phonon scattering does not play a dominant role in controlling the carrier mobility. The data strongly suggest that fixed charged impurities located in close proximity to the graphene are responsible for the mobility degradation.

Gate-tunable resonant tunneling in double bilayer graphene heterostructures.

We demonstrate gate-tunable resonant tunneling and negative differential resistance in the interlayer current-voltage characteristics of rotationally aligned double bilayer graphene heterostructures separated by hexagonal boron nitride (hBN) dielectric. An analysis of the heterostructure band alignment using individual layer densities, along with experimentally determined layer chemical potentials indicates that the resonance occurs when the energy bands of the two bilayer graphene are aligned. We discuss the tunneling resistance dependence on the interlayer hBN thickness, as well as the resonance width dependence on mobility and rotational alignment.

Scaling of Al2O3 dielectric for graphene field-effect transistors

We investigate the scaling of Al2O3 dielectric on graphene by atomic layer deposition (ALD) using ultra-thin, oxidized Ti and Al films as nucleation layers. We show that the nucleation layer significantly impacts the dielectric constant (k) and morphology of the ALD Al2O3, yielding k = 5.5 and k = 12.7 for Al and Ti nucleation layers, respectively. Transmission electron microscopy shows that Al2O3 grown using the Ti interface is partially crystalline, while Al2O3 grown on Al is amorphous. Using a spatially uniform 0.6 nm-thick Ti nucleation layer, we demonstrate graphene field-effect transistors with top dielectric stacks as thin as 2.6 nm.

Band offset and negative compressibility in graphene-MoS2 heterostructures.

We use electron transport to characterize monolayer graphene-multilayer MoS2 heterostructures. Our samples show ambipolar characteristics and conductivity saturation on the electron branch that signals the onset of MoS2 conduction band population. Surprisingly, the carrier density in graphene decreases with gate bias once MoS2 is populated, demonstrating negative compressibility in MoS2. We are able to interpret our measurements quantitatively by accounting for disorder and using the random phase approximation (RPA) for the exchange and correlation energies of both Dirac and parabolic-band two-dimensional electron gases. This interpretation allows us to extract the energetic offset between the conduction band edge of MoS2 and the Dirac point of graphene.

High-Mobility Holes in Dual-Gated WSe2 Field-Effect Transistors

We demonstrate dual-gated p-type field-effect transistors (FETs) based on few-layer tungsten diselenide (WSe2) using high work-function platinum source/drain contacts and a hexagonal boron nitride top-gate dielectric. A device topology with contacts underneath the WSe2 results in p-FETs with ION/IOFF ratios exceeding 10(7) and contacts that remain ohmic down to cryogenic temperatures. The output characteristics show current saturation and gate tunable negative differential resistance. The devices show intrinsic hole mobilities around 140 cm(2)/(V s) at room temperature and approaching 4000 cm(2)/(V s) at 2 K. Temperature-dependent transport measurements show a metal-insulator transition, with an insulating phase at low densities and a metallic phase at high densities. The mobility shows a strong temperature dependence consistent with phonon scattering, and saturates at low temperatures, possibly limited by Coulomb scattering or defects.

Chemical Potential and Quantum Hall Ferromagnetism in Bilayer Graphene

Breaking down graphene degeneracy Bilayer graphene has two layers of hexagonally arranged carbon atoms stacked on top of each other in a staggered configuration. This spatial arrangement results in degenerate electronic states: distinct states that have the same energy. Interaction between electrons can cause the states to separate in energy, and so can external fields (see the Perspective by LeRoy and Yankowitz). Kou et al., Lee et al., and Maher et al. used three distinct experimental setups that clarify different parameter regimes of bilayer graphene. Science, this issue p. 55, p. 58, p. 61; see also p. 31 One graphene bilayer is used to tune and study the electronic properties of another. [Also see Perspective by LeRoy and Yankowitz] Bilayer graphene has a distinctive electronic structure influenced by a complex interplay between various degrees of freedom. We probed its chemical potential using double bilayer graphene heterostructures, separated by a hexagonal boron nitride dielectric. The chemical potential has a nonlinear carrier density dependence and bears signatures of electron-electron interactions. The data allowed a direct measurement of the electric field–induced bandgap at zero magnetic field, the orbital Landau level (LL) energies, and the broken-symmetry quantum Hall state gaps at high magnetic fields. We observe spin-to-valley polarized transitions for all half-filled LLs, as well as emerging phases at filling factors ν = 0 and ν = ±2. Furthermore, the data reveal interaction-driven negative compressibility and electron-hole asymmetry in N = 0, 1 LLs.

Direct measurement of the fermi energy in graphene using a double-layer heterostructure

We describe a technique which allows a direct measurement of the relative Fermi energy in an electron system by employing a double-layer heterostructure. We illustrate this method by using a graphene double layer to probe the Fermi energy as a function of carrier density in monolayer graphene, at zero and in high magnetic fields. This technique allows us to determine the Fermi velocity, Landau level spacing, and Landau level broadening. We find that the N=0 Landau level broadening is larger by comparison to the broadening of upper and lower Landau levels.

van der Waals Heterostructures with High Accuracy Rotational Alignment

We describe the realization of van der Waals (vdW) heterostructures with accurate rotational alignment of individual layer crystal axes. We illustrate the approach by demonstrating a Bernal-stacked bilayer graphene formed using successive transfers of monolayer graphene flakes. The Raman spectra of this artificial bilayer graphene possess a wide 2D band, which is best fit by four Lorentzians, consistent with Bernal stacking. Scanning tunneling microscopy reveals no moiré pattern on the artificial bilayer graphene, and tunneling spectroscopy as a function of gate voltage reveals a constant density of states, also in agreement with Bernal stacking. In addition, electron transport probed in dual-gated samples reveals a band gap opening as a function of transverse electric field. To illustrate the applicability of this technique to realize vdW heterostructuctures in which the functionality is critically dependent on rotational alignment, we demonstrate resonant tunneling double bilayer graphene heterostructures separated by hexagonal boron-nitride dielectric.