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.

Soft X-ray Exposure Promotes Na Intercalation in Graphene Grown on Si-Face SiC.

An investigation of how electron/photon beam exposures affect the intercalation rate of Na deposited on graphene prepared on Si-face SiC is presented. Focused radiation from a storage ring is used for soft X-ray exposures while the electron beam in a low energy electron microscope is utilized for electron exposures. The microscopy and core level spectroscopy data presented clearly show that the effect of soft X-ray exposure is significantly greater than of electron exposure, i.e., it produces a greater increase in the intercalation rate of Na. Heat transfer from the photoelectrons generated during soft X-ray exposure and by the electrons penetrating the sample during electron beam exposure is suggested to increase the local surface temperature and thus the intercalation rate. The estimated electron flux density is 50 times greater for soft X-ray exposure compared to electron exposure, which explains the larger increase in the intercalation rate from soft X-ray exposure. Effects occurring with time only at room temperature are found to be fairly slow, but detectable. The graphene quality, i.e., domain/grain size and homogeneity, was also observed to be an important factor since exposure-induced effects occurred more rapidly on a graphene sample prepared in situ compared to on a furnace grown sample.

A versatile photoelectron spectrometer for pressures up to 30 mbar.

High-pressure photoelectron spectroscopy is a rapidly developing technique with applications in a wide range of fields ranging from fundamental surface science and catalysis to energy materials, environmental science, and biology. At present the majority of the high-pressure photoelectron spectrometers are situated at synchrotron end stations, but recently a small number of laboratory-based setups have also emerged. In this paper we discuss the design and performance of a new laboratory based high pressure photoelectron spectrometer equipped with an Al Kα X-ray anode and a hemispherical electron energy analyzer combined with a differentially pumped electrostatic lens. The instrument is demonstrated to be capable of measuring core level spectra at pressures up to 30 mbar. Moreover, valence band spectra of a silver sample as well as a carbon-coated surface (graphene) recorded under a 2 mbar nitrogen atmosphere are presented, demonstrating the versatility of this laboratory-based spectrometer.

Visualisation of edge effects in side-gated graphene nanodevices.

Using local scanning electrical techniques we study edge effects in side-gated Hall bar nanodevices made of epitaxial graphene. We demonstrate that lithographically defined edges of the graphene channel exhibit hole conduction within the narrow band of ~60-125 nm width, whereas the bulk of the material is electron doped. The effect is the most pronounced when the influence of atmospheric contamination is minimal. We also show that the electronic properties at the edges can be precisely tuned from hole to electron conduction by using moderate strength electrical fields created by side-gates. However, the central part of the channel remains relatively unaffected by the side-gates and retains the bulk properties of graphene.

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.

Broadband antireflection and light extraction enhancement in fluorescent SiC with nanodome structures.

We demonstrate a time-efficient and low-cost approach to fabricate Si3N4 coated nanodome structures in fluorescent SiC. Nanosphere lithography is used as the nanopatterning method and SiC nanodome structures with Si3N4 coating are formed via dry etching and thin film deposition process. By using this method, a significant broadband surface antireflection and a considerable omnidirectional luminescence enhancement are obtained. The experimental observations are then supported by numerical simulations. It is believed that our fabrication method will be well suitable for large-scale production in the future.

Approaching magnetic ordering in graphene materials by FeCl3 intercalation.

We show the successful intercalation of large area (1 cm(2)) epitaxial few-layer graphene grown on 4H-SiC with FeCl3. Upon intercalation the resistivity of this system drops from an average value of ∼200 Ω/sq to ∼16 Ω/sq at room temperature. The magneto-conductance shows a weak localization feature with a temperature dependence typical of graphene Dirac fermions demonstrating the decoupling into parallel hole gases of each carbon layer composing the FeCl3 intercalated structure. The phase coherence length (∼1.2 µm at 280 mK) decreases rapidly only for temperatures higher than the 2D magnetic ordering in the intercalant layer while it tends to saturate for temperatures lower than the antiferromagnetic ordering between the planes of FeCl3 molecules providing the first evidence for magnetic ordering in the extreme two-dimensional limit of graphene.

Kinks in the σ band of graphene induced by electron-phonon coupling.

Angle-resolved photoemission spectroscopy reveals pronounced kinks in the dispersion of the σ band of graphene. Such kinks are usually caused by the combination of a strong electron-boson interaction and the cutoff in the Fermi-Dirac distribution. They are therefore not expected for the σ band of graphene that has a binding energy of more than ≈3.5 eV. We argue that the observed kinks are indeed caused by the electron-phonon interaction, but the role of the Fermi-Dirac distribution cutoff is assumed by a cutoff in the density of σ states. The existence of the effect suggests a very weak coupling of holes in the σ band not only to the π electrons of graphene but also to the substrate electronic states. This is confirmed by the presence of such kinks for graphene on several different substrates that all show a strong coupling constant of λ≈1.

Standardization of surface potential measurements of graphene domains.

We compare the three most commonly used scanning probe techniques to obtain a reliable value of the work function in graphene domains of different thickness. The surface potential (SP) of graphene is directly measured in Hall bar geometry via a combination of electrical functional microscopy and spectroscopy techniques, which enables calibrated work function measurements of graphene domains in ambient conditions with values Φ1LG ~4.55 ± 0.02 eV and Φ2LG ~ 4.44 ± 0.02 eV for single- and bi-layer, respectively. We demonstrate that frequency-modulated Kelvin probe force microscopy (FM-KPFM) provides more accurate measurement of the SP than amplitude-modulated (AM)-KPFM. The discrepancy between experimental results obtained by different techniques is discussed. In addition, we use FM-KPFM for contactless measurements of the specific components of the device resistance. We show a strong non-Ohmic behavior of the electrode-graphene contact resistance and extract the graphene channel resistivity.

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.

On the differing sensitivity to chemical gating of single and double layer epitaxial graphene explored using scanning Kelvin probe microscopy.

Using environmental scanning Kelvin probe microscopy, we show that the position of the Fermi level of single layer graphene is more sensitive to chemical gating than that of double layer graphene. We calculate that the difference in sensitivity to chemical gating is not entirely due to the difference in band structure of 1 and 2 layer graphene. The findings are important for gas sensing where the sensitivity of the electronic properties to gas adsorption is monitored and suggest that single layer graphene could make a more sensitive gas sensor than double layer graphene. We propose that the difference in surface potential between adsorbate-free single and double layer graphene, measured using scanning kelvin probe microscopy, can be used as a noninvasive method of estimating substrate-induced doping in epitaxial graphene.

Omnidirectional luminescence enhancement of fluorescent SiC via pseudoperiodic antireflective subwavelength structures.

In the present work, an approach of fabricating pseudoperiodic antireflective subwavelength structures (ARS) on fluorescent SiC by using self-assembled etch mask is demonstrated. By applying the pseudoperiodic (ARS), the average surface reflectance at 6° incidence over the spectral range of 390-785 nm is dramatically suppressed from 20.5% to 1.62%, and the hydrophobic surface with a large contact angle of 98° is also achieved. The angle-resolved photoluminescence study presents a considerable omnidirectional luminescence enhancement with an integral intensity enhancement of 66.3% and a fairly preserved spatial emission pattern.

Broadband and omnidirectional light harvesting enhancement of fluorescent SiC.

In the present work, antireflective sub-wavelength structures have been fabricated on fluorescent 6H-SiC to enhance the white light extraction efficiency by using the reactive-ion etching method. Broadband and omnidirectional antireflection characteristics show that 6H-SiC with antireflective sub-wavelength structures suppress the average surface reflection significantly from 20.5 % to 1.01 % over a wide spectral range of 390-784 nm. The luminescence intensity of the fluorescent 6H-SiC could be enhanced in the whole emission angle range. It maintains an enhancement larger than 91 % up to the incident angle of 70 degrees, while the largest enhancement of 115.4 % could be obtained at 16 degrees. The antireflective sub-wavelength structures on fluorescent 6H-SiC could also preserve the luminescence spectral profile at a large emission angle by eliminating the Fabry-Pérot microcavity interference effect.

Long spin relaxation times in wafer scale epitaxial graphene on SiC(0001).

We developed an easy, upscalable process to prepare lateral spin-valve devices on epitaxially grown monolayer graphene on SiC(0001) and perform nonlocal spin transport measurements. We observe the longest spin relaxation times τ(S) in monolayer graphene, while the spin diffusion coefficient D(S) is strongly reduced compared to typical results on exfoliated graphene. The increase of τ(S) is probably related to the changed substrate, while the cause for the small value of D(S) remains an open question.

Direct graphene growth on Co3O4(111) by molecular beam epitaxy.

Direct growth of graphene on Co(3)O(4)(111) at 1000 K was achieved by molecular beam epitaxy from a graphite source. Auger spectroscopy shows a characteristic sp(2) carbon lineshape, at average carbon coverages from 0.4 to 3 ML. Low energy electron diffraction (LEED) indicates (111) ordering of the sp(2) carbon film with a lattice constant of 2.5(±0.1) Å characteristic of graphene. Sixfold symmetry of the graphene diffraction spots is observed at 0.4, 1 and 3 ML. The LEED data also indicate an average domain size of ~1800 Å, and show an incommensurate interface with the Co(3)O(4)(111) substrate, where the latter exhibits a lattice constant of 2.8(±0.1) Å. Core level photoemission shows a characteristically asymmetric C(1s) feature, with the expected π to π* satellite feature, but with a binding energy for the 3 ML film of 284.9(±0.1) eV, indicative of substantial graphene-to-oxide charge transfer. Spectroscopic ellipsometry data demonstrate broad similarity with graphene samples physically transferred to SiO(2) or grown on SiC substrates, but with the π to π* absorption blue-shifted, consistent with charge transfer to the substrate. The ability to grow graphene directly on magnetically and electrically polarizable substrates opens new opportunities for industrial scale development of charge- and spin-based devices.

ZnO materials and surface tailoring for biosensing.

ZnO nanostructured materials, such as films and nanoparticles, could provide a suitable platform for development of high performance biosensors due to their unique fundamental material properties. This paper reviews different preparation techniques of ZnO nanocrystals and material issues like wettability, biocompatibility and toxicity, which have an important relevance to biosensor functionality. Efforts are made to summarize and analyze existing results regarding surface modification and molecular attachments for successful biofunctionalization and understanding of the mechanisms involved. A section is devoted to implementations of tailored surfaces in biosensors. We end with conclusions on the feasibility of using ZnO nanocrystals for biosensing.

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.

Nanoscale structural characterization of epitaxial graphene grown on off-axis 4H-SiC (0001).

In this work, we present a nanometer resolution structural characterization of epitaxial graphene (EG) layers grown on 4H-SiC (0001) 8° off-axis, by annealing in inert gas ambient (Ar) in a wide temperature range (Tgr from 1600 to 2000°C). For all the considered growth temperatures, few layers of graphene (FLG) conformally covering the 100 to 200-nm wide terraces of the SiC surface have been observed by high-resolution cross-sectional transmission electron microscopy (HR-XTEM). Tapping mode atomic force microscopy (t-AFM) showed the formation of wrinkles with approx. 1 to 2 nm height and 10 to 20 nm width in the FLG film, as a result of the release of the compressive strain, which builds up in FLG during the sample cooling due to the thermal expansion coefficients mismatch between graphene and SiC. While for EG grown on on-axis 4H-SiC an isotropic mesh-like network of wrinkles interconnected into nodes is commonly reported, in the present case of a vicinal SiC surface, wrinkles are preferentially oriented in the direction perpendicular to the step edges of the SiC terraces. For each Tgr, the number of graphene layers was determined on very small sample areas by HR-XTEM and, with high statistics and on several sample positions, by measuring the depth of selectively etched trenches in FLG by t-AFM. Both the density of wrinkles and the number of graphene layers are found to increase almost linearly as a function of the growth temperature in the considered temperature range.

Mapping of local electrical properties in epitaxial graphene using electrostatic force microscopy.

Local electrical characterization of epitaxial graphene grown on 4H-SiC(0001) using electrostatic force microscopy (EFM) in ambient conditions and at elevated temperatures is presented. EFM provides a straightforward identification of graphene with different numbers of layers on the substrate where topographical determination is hindered by adsorbates. Novel EFM spectroscopy has been developed measuring the EFM phase as a function of the electrical DC bias, establishing a rigorous way to distinguish graphene domains and facilitating optimization of EFM imaging.