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Rodney S. Ruoff

Publications and source records attributed to Rodney S. Ruoff.

33 records · Page 2Linked to original sources

Integration of the Ferromagnetic Insulator EuO onto Graphene

We have demonstrated the deposition of EuO films on graphene by reactive molecular beam epitaxy in a special adsorption-controlled and oxygen-limited regime, which is a critical advance toward the realization of the exchange proximity interaction (EPI). It has been predicted that when the ferromagnetic insulator (FMI) EuO is brought into contact with graphene, an overlap of electronic wavefunctions at the FMI/graphene interface can induce a large spin splitting inside the graphene. Experimental realization of this effect could lead to new routes for spin manipulation, which is a necessary requirement for a functional spin transistor. Furthermore, EPI could lead to novel spintronic behavior such as controllable magnetoresistance, gate tunable exchange bias, and quantized anomalous Hall effect. However, experimentally, EuO has not yet been integrated onto graphene. Here we report the successful growth of high quality crystalline EuO on highly-oriented pyrolytic graphite (HOPG) and single-layer graphene. The epitaxial EuO layers have (001) orientation and do not induce an observable D peak (defect) in the Raman spectra. Magneto-optic measurements indicate ferromagnetism with Curie temperature of 69 K, which is the value for bulk EuO. Transport measurements on exfoliated graphene before and after EuO deposition indicate only a slight decrease in mobility.

cond-mat.mtrl-sci↗

Uniform wafer-scale synthesis of graphene on evaporated Cu (111) film with quality comparable to exfoliated monolayer

Monolayer graphene has been grown on crystallized Cu (111) films on standard oxidized Si 100 mm wafers. The monolayer graphene demonstrates high uniformity (>97% coverage), with immeasurable defects (>95% defect-negligible) across the entire wafer. Key to these results is the phase transition of evaporated copper films from amorphous to crystalline at the growth temperature as corroborated by X-ray diffraction and electron backscatter diffraction. Noticeably, phase transition of copper film is observed on technologically ubiquitous oxidized Si wafer where the oxide is a standard amorphous thermal oxide. Ion mass spectroscopy indicates that the copper films can be purposely hydrogen-enriched during a hydrogen anneal which subsequently affords graphene growth with a sole carbonaceous precursor for low defect densities. Owing to the strong hexagonal lattice match, the graphene domains align to the Cu (111) domains, suggesting a pathway for increasing the graphene grains by maximizing the copper grain sizes. Fabricated graphene transistors on a flexible polyimide film yield a peak carrier mobility ~4,930 cm2/Vs.

cond-mat.mtrl-sci↗

Thermal Properties of Isotopically Engineered Graphene

In addition to its exotic electronic properties graphene exhibits unusually high intrinsic thermal conductivity. The physics of phonons - the main heat carriers in graphene - was shown to be substantially different in two-dimensional (2D) crystals, such as graphene, than in three-dimensional (3D) graphite. Here, we report our experimental study of the isotope effects on the thermal properties of graphene. Isotopically modified graphene containing various percentages of 13C were synthesized by chemical vapor deposition (CVD). The regions of different isotopic composition were parts of the same graphene sheet to ensure uniformity in material parameters. The thermal conductivity, K, of isotopically pure 12C (0.01% 13C) graphene determined by the optothermal Raman technique, was higher than 4000 W/mK at the measured temperature Tm~320 K, and more than a factor of two higher than the value of K in a graphene sheets composed of a 50%-50% mixture of 12C and 13C. The experimental data agree well with our molecular dynamics (MD) simulations, corrected for the long-wavelength phonon contributions via the Klemens model. The experimental results are expected to stimulate further studies aimed at better understanding of thermal phenomena in 2D crystals.

cond-mat.mes-hall↗

Oxidation resistance of graphene-coated Cu and Cu/Ni alloy

The ability to protect refined metals from reactive environments is vital to many industrial and academic applications. Current solutions, however, typically introduce several negative effects, including increased thickness and changes in the metal physical properties. In this paper, we demonstrate for the first time the ability of graphene films grown by chemical vapor deposition to protect the surface of the metallic growth substrates of Cu and Cu/Ni alloy from air oxidation. SEM, Raman spectroscopy, and XPS studies show that the metal surface is well protected from oxidation even after heating at 200 \degree C in air for up to 4 hours. Our work further shows that graphene provides effective resistance against hydrogen peroxide. This protection method offers significant advantages and can be used on any metal that catalyzes graphene growth.

cond-mat.mtrl-sci↗

Adsorption/desorption and electrically controlled flipping of ammonia molecules on graphene

In this paper, we evaluate of the adsorption/ desorption of ammonia molecules on a graphene surface by studying the Fermi level shift. Based on a physically plausible model, the adsorption and desorption rates of ammonia molecules on graphene have been extracted from the measured Fermi level shift as a function of exposure time. An electric field-induced flipping behavior of ammonia molecules on graphene is suggested, based on field effect transistor (FET) measurements.

cond-mat.mes-hall↗

Graphene films with large domain size by a two-step chemical vapor deposition process

The fundamental properties of graphene are making it an attractive material for a wide variety of applications. Various techniques have been developed to produce graphene and recently we discovered the synthesis of large area graphene by chemical vapor deposition (CVD) of methane on Cu foils. We also showed that graphene growth on Cu is a surface-mediated process and the films were polycrystalline with domains having an area of tens of square microns. In this paper we report on the effect of growth parameters such as temperature, and methane flow rate and partial pressure on the growth rate, domain size, and surface coverage of graphene as determined by Raman spectroscopy, and transmission and scanning electron microscopy. Based on the results, we developed a two-step CVD process to synthesize graphene films with domains having an area of hundreds of square microns. Scanning electron microscopy and Raman spectroscopy clearly show an increase in domain size by changing the growth parameters. Transmission electron microscopy further shows that the domains are crystallographically rotated with respect to each other with a range of angles from about 13 degrees to nearly 30 degrees. Electrical transport measurements performed on back-gated FETs show that overall films with larger domains tend to have higher carrier mobility, up to about 16,000 cm2 V-1 s-1 at room temperature.

cond-mat.mtrl-sci↗

Large domain graphene

Graphene growth by chemical vapor deposition has received a lot of attention recently owing to the ease with which large area films can be grown, but growth of large domain or equivalently large grain size has not been reported yet. In this brevia, we report on a CVD process that yields graphene with domains of hundreds of micrometers, by very low pressure CVD, less than 50 mTorr, and very low precursor flow rates using methane as the source of carbon on the inside of copper foil enclosures at high temperature, around 1000 oC. The carrier mobility for the large-domain graphene films is up to 21,000 cm2/Vs.

cond-mat.mtrl-sci↗

Domain (Grain) Boundaries and Evidence of Twin Like Structures in CVD Grown Graphene

Understanding and engineering the domain boundaries in chemically vapor deposited (CVD) monolayer graphene will be critical for improving its properties. In this study, a combination of transmission electron microscopy (TEM) techniques including selected area electron diffraction (SAED), high resolution transmission electron microscopy (HRTEM), and dark field (DF) TEM was used to study the boundary orientation angle distribution and the nature of the carbon bonds at the domain boundaries. This report provides an important first step towards a fundamental understanding of these domain boundaries. The results show that, for the graphene grown in this study, the 46 measured misorientation angles are all between 11-30 degrees (with the exception of one at 7 degrees). HRTEM images show the presence of adsorbates in almost all of the boundary areas. When a boundary was imaged, defects were seen (dangling bonds) at the boundaries that likely contribute to adsorbates binding at these boundaries. DFTEM images also showed the presence of a 'twin like' boundary.

cond-mat.mtrl-sci↗

Anomalous Strength Characteristics of Tilt Grain Boundaries in Graphene

Using molecular dynamics simulations and first principles calculations, we have studied the structure and mechanical strength of tilt grain boundaries in graphene sheets that arise during CVD growth of graphene on metal substrates. Surprisingly, we find that for tilt boundaries in the vicinity of both the zig-zag and arm-chair orientations, large angle boundaries with a higher density of 5-7 defect pairs are stronger than the low-angle boundaries which are comprised of fewer defects per unit length. Interestingly, the trends in our results cannot be explained by a continuum Griffith-type fracture mechanics criterion, which predicts the opposite trend due to that fact that it does not account for the critical bonds that are responsible for the failure mechanism. We have identified the highly-strained bonds in the 7-member rings that lead to the failure of the sheets, and we have found that large angle boundaries are able to better accommodate the strained 7-rings. Our results provide guidelines for designing growth methods to obtain grain boundary structures that can have strengths close to that of pristine graphene.

cond-mat.mtrl-sci↗

Review of Best Practice Methods for Determining an Electrode Material's Performance for Ultracapacitors

Ultracapacitors are rapidly being adopted for use for a wide range of electrical energy storage applications. While ultracapacitors are able to deliver high rates of charge and discharge, they are limited in the amount of energy stored. The capacity of ultracapacitors is largely determined by the electrode material and as a result, research to improve the performance of electrode materials has dramatically increased. While test methods for packaged ultracapacitors are well developed, it is often not feasible for the materials scientist to assemble full sized, packaged cells to test electrode materials. Methodology to reliably measure a material's performance for ultracapacitor electrode use is not well standardized with the different techniques currently being used yielding widely varying results. In this manuscript, we review the best practice test methods that accurately predict a materials performance, yet are flexible and quick enough to accommodate a wide range of material sample types and amounts.

cond-mat.mtrl-sci↗

Evolution of graphene growth on Cu and Ni studied by carbon isotope labeling

Large-area graphene is a new material with properties that make it desirable for advanced scaled electronic devices1. Recently, chemical vapor deposition (CVD) of graphene and few-layer graphene using hydrocarbons on metal substrates such as Ni and Cu has shown to be a promising technique2-5. It has been proposed in recent publications that graphene growth on Ni occurs by C segregation2 or precipitation3, while that on Cu is by surface adsorption5. In this letter, we used a carbon isotope labeling technique to elucidate the growth kinetics and unambiguously demonstrate that graphene growth on Cu is by surface adsorption whereas on Ni is by segregation-precipitation. An understanding of the evolution of graphene growth and thus growth mechanism(s) is desired to obtain uniform graphene films. The results presented in this letter clearly demonstrate that surface adsorption is preferred over precipitation to grow graphene because it is a self-limiting process and thus manufacturable.

cond-mat.mtrl-sci↗

Large-Area Synthesis of High-Quality and Uniform Graphene Films on Copper Foils

Graphene has been attracting great interest because of its distinctive band structure and physical properties. Today, graphene is limited to small sizes because it is produced mostly by exfoliating graphite. We grew large-area graphene films of the order of centimeters on copper substrates by chemical vapor deposition using methane. The films are predominantly single layer graphene with a small percentage (less than 5%) of the area having few layers, and are continuous across copper surface steps and grain boundaries. The low solubility of carbon in copper appears to help make this growth process self-limiting. We also developed graphene film transfer processes to arbitrary substrates, and dual-gated field-effect transistors fabricated on Si/SiO2 substrates showed electron mobilities as high as 4050 cm2V-1s-1 at room temperature.

cond-mat.mtrl-sci↗

Simple approach for high-contrast optical imaging and characterization of graphene-based sheets

A simple optical method is presented for identifying and measuring the effective optical properties of nanometer-thick, graphene-based materials, based on the use of substrates consisting of a thin dielectric layer on silicon. High contrast between the graphene-based materials and the substrate is obtained by choosing appropriate optical properties and thickness of the dielectric layer. The effective refractive index and optical absorption coefficient of graphene oxide, thermally reduced graphene oxide, and graphene are obtained by comparing the predicted and measured contrasts.

cond-mat.mes-hall↗

Conduction in Carbon Nanotubes Through Metastable Resonant States

We report here on electrical measurements on individual multi-walled carbon nanotubes (MWNTs) that show that the presence or movement of impurities or defects in the carbon nanotube can radically change its low temperature transport characteristics. The low temperature conductance can either decrease monotonically with decreasing temperature, or show a sudden increase at very low temperatures, sometimes in the same sample at different times. This unusual behavior of the temperature dependence of the conductance is correlated with large variations in the differential conductance as a function of the dc voltage across the wire. The effect is well described as arising from quantum interference of conduction channels corresponding to direct transmission through the nanotube and resonant transmission through a discrete electron state, the so-called Fano resonance.

cond-mat.mes-hall↗

Length distribution of single walled carbon nanotubes determined by ac atomic force microscopy

A simple method to disperse individual single walled carbon nanotubes (SWCNT ) on an atomically flat substrate is presented. Proper tuning of ac modes of atomic force microscopes(AFM) is discussed. This is needed to discriminate between individual nanotubes and very small bundles. The distribution of lengths of the nanotubes measured by these methods is reported.

cond-mat.mtrl-sci↗