Electric double-layer capacitance between an ionic liquid and few-layer graphene

PubMed Central

Uesugi, Eri; Goto, Hidenori; Eguchi, Ritsuko; Fujiwara, Akihiko; Kubozono, Yoshihiro

2013-01-01

Ionic-liquid gates have a high carrier density due to their atomically thin electric double layer (EDL) and extremely large geometrical capacitance Cg. However, a high carrier density in graphene has not been achieved even with ionic-liquid gates because the EDL capacitance CEDL between the ionic liquid and graphene involves the series connection of Cg and the quantum capacitance Cq, which is proportional to the density of states. We investigated the variables that determine CEDL at the molecular level by varying the number of graphene layers n and thereby optimising Cq. The CEDL value is governed by Cq at n < 4, and by Cg at n > 4. This transition with n indicates a composite nature for CEDL. Our finding clarifies a universal principle that determines capacitance on a microscopic scale, and provides nanotechnological perspectives on charge accumulation and energy storage using an ultimately thin capacitor. PMID:23549208

Ultrathin Graphene Membranes as Flexible Electrodes for Electrochemical Double Layer Capacitors

NASA Astrophysics Data System (ADS)

Talapatra, Saikat; Kar, Swastik; Shah, Rakesh; Ghosh, Sujoy; An, Xiaohong; Simmons, Trevor; Washington, Morris; Nayak, Saroj

2010-03-01

We will present the results of our investigations of electrochemical double layer capacitors (EDLCs) or supercapacitors (SC) fabricated using graphene based ultra thin membranes. These EDLC's show far superior performance compared to other carbon nanomaterials based EDLC's devices. We found that the graphene based devices possess specific capacitance values as high as 120 F/g, with impressive power densities (˜105 kW/kg) and energy densities (˜9.2 Wh/kg). Further, these devices indicated rapid charge transfer response even without the use of any binders or specially prepared current collectors. Our ultracapacitors reflect a significant improvement over previously reported graphene-based ultracapacitors and are substantially better than those obtained with carbon nanotubes.

Role of electron back action on photons in hybridizing double-layer graphene plasmons with localized photons.

PubMed

Huang, Danhong; Iurov, Andrii; Gumbs, Godfrey

2018-05-23

In this paper, we deal with the electromagnetic coupling between an incident surface-plasmon-polariton wave and relativistic electrons in two graphene layers. Our previous investigation was limited to single-layer graphene (Iurov et al 2017 Phys. Rev. B 96 081408). However, the present work, is both an expanded and extended version of this previous Phys. Rev. B paper after having included very detailed theoretical formalisms and extensive comparisons of results from either one or two graphene layers embedded in a dielectric medium. The additional retarded Coulomb interaction between two graphene layers will compete with the coupling between the single graphene layer and the surface of a conductor. Consequently, some distinctive features, such as triply-hybridized absorption peaks and a new acoustic-like graphene plasmon mode within the anticrossing region, have been found for the double-layer graphene system. Physically, our theory is self-consistent, in comparison with a commonly adopted perturbative theory, for studying hybrid light-plasmon modes and the electron back action on photons. Instead of usual radiation or grating-deflection field coupling, a surface-plasmon-polariton localized field coupling is introduced with completely different dispersion relations for radiative (small wave numbers) and evanescent (large wave numbers) field modes. Technically, the exactly calculated effective scattering matrix for this theory can be employed to construct an effective-medium theory in order to improve the accuracy of the well-known finite-difference time-domain method for solving Maxwell's equations numerically. Practically, the predicted triply-hybridized absorption peaks can excite polaritons only, giving rise to a possible polariton-condensation based laser.

Role of electron back action on photons in hybridizing double-layer graphene plasmons with localized photons

NASA Astrophysics Data System (ADS)

Huang, Danhong; Iurov, Andrii; Gumbs, Godfrey

2018-05-01

In this paper, we deal with the electromagnetic coupling between an incident surface-plasmon-polariton wave and relativistic electrons in two graphene layers. Our previous investigation was limited to single-layer graphene (Iurov et al 2017 Phys. Rev. B 96 081408). However, the present work, is both an expanded and extended version of this previous Phys. Rev. B paper after having included very detailed theoretical formalisms and extensive comparisons of results from either one or two graphene layers embedded in a dielectric medium. The additional retarded Coulomb interaction between two graphene layers will compete with the coupling between the single graphene layer and the surface of a conductor. Consequently, some distinctive features, such as triply-hybridized absorption peaks and a new acoustic-like graphene plasmon mode within the anticrossing region, have been found for the double-layer graphene system. Physically, our theory is self-consistent, in comparison with a commonly adopted perturbative theory, for studying hybrid light-plasmon modes and the electron back action on photons. Instead of usual radiation or grating-deflection field coupling, a surface-plasmon-polariton localized field coupling is introduced with completely different dispersion relations for radiative (small wave numbers) and evanescent (large wave numbers) field modes. Technically, the exactly calculated effective scattering matrix for this theory can be employed to construct an effective-medium theory in order to improve the accuracy of the well-known finite-difference time-domain method for solving Maxwell’s equations numerically. Practically, the predicted triply-hybridized absorption peaks can excite polaritons only, giving rise to a possible polariton-condensation based laser.

Contribution of Dielectric Screening to the Total Capacitance of Few-Layer Graphene Electrodes.

PubMed

Zhan, Cheng; Jiang, De-en

2016-03-03

We apply joint density functional theory (JDFT), which treats the electrode/electrolyte interface self-consistently, to an electric double-layer capacitor (EDLC) based on few-layer graphene electrodes. The JDFT approach allows us to quantify a third contribution to the total capacitance beyond quantum capacitance (CQ) and EDL capacitance (CEDL). This contribution arises from the dielectric screening of the electric field by the surface of the few-layer graphene electrode, and we therefore term it the dielectric capacitance (CDielec). We find that CDielec becomes significant in affecting the total capacitance when the number of graphene layers in the electrode is more than three. Our investigation sheds new light on the significance of the electrode dielectric screening on the capacitance of few-layer graphene electrodes.

Synthesis of layer-tunable graphene: A combined kinetic implantation and thermal ejection approach

DOE PAGES

Wang, Gang; Zhang, Miao; Liu, Su; ...

2015-05-04

Layer-tunable graphene has attracted broad interest for its potentials in nanoelectronics applications. However, synthesis of layer-tunable graphene by using traditional chemical vapor deposition (CVD) method still remains a great challenge due to the complex experimental parameters and the carbon precipitation process. Herein, by performing ion implantation into a Ni/Cu bilayer substrate, the number of graphene layers, especially single or double layer, can be controlled precisely by adjusting the carbon ion implant fluence. The growth mechanism of the layer-tunable graphene is revealed by monitoring the growth process is observed that the entire implanted carbon atoms can be expelled towards the substratemore » surface and thus graphene with designed layer number can be obtained. Such a growth mechanism is further confirmed by theoretical calculations. The proposed approach for the synthesis of layer-tunable graphene offers more flexibility in the experimental conditions. Being a core technology in microelectronics processing, ion implantation can be readily implemented in production lines and is expected to expedite the application of graphene to nanoelectronics.« less

Plasmons in spatially separated double-layer graphene nanoribbons

NASA Astrophysics Data System (ADS)

Bagheri, Mehran; Bahrami, Mousa

2014-05-01

Motivated by innovative progresses in designing multi-layer graphene nanostructured materials in the laboratory, we theoretically investigate the Dirac plasmon modes of a spatially separated double-layer graphene nanoribbon system, made up of a vertically offset armchair and metallic graphene nanoribbon pair. We find striking features of the collective excitations in this novel Coulomb correlated system, where both nanoribbons are supposed to be either intrinsic (undoped/ungated) or extrinsic (doped/gated). In the former, it is shown the low-energy acoustical and the high-energy optical plasmon modes are tunable only by the inter-ribbon charge separation. In the later, the aforementioned plasmon branches are modified by the added doping factor. As a result, our model could be useful to examine the existence of a linear Landau-undamped low-energy acoustical plasmon mode tuned via the inter-ribbon charge separation as well as doping. This study might also be utilized for devising novel quantum optical waveguides based on the Coulomb coupled graphene nanoribbons.

Development of a 3D Graphene Electrode Dielectrophoretic Device

PubMed Central

Xie, Hongyu; Tewari, Radheshyam; Fukushima, Hiroyuki; Narendra, Jeffri; Heldt, Caryn; King, Julia; Minerick, Adrienne R.

2014-01-01

The design and fabrication of a novel 3D electrode microdevice using 50 µm thick graphene paper and 100 µm double sided tape is described. The protocol details the procedures to construct a versatile, reusable, multiple layer, laminated dielectrophoresis chamber. Specifically, six layers of 50 µm x 0.7 cm x 2 cm graphene paper and five layers of double sided tape were alternately stacked together, then clamped to a glass slide. Then a 700 μm diameter micro-well was drilled through the laminated structure using a computer-controlled micro drilling machine. Insulating properties of the tape layer between adjacent graphene layers were assured by resistance tests. Silver conductive epoxy connected alternate layers of graphene paper and formed stable connections between the graphene paper and external copper wire electrodes. The finished device was then clamped and sealed to a glass slide. The electric field gradient was modeled within the multi-layer device. Dielectrophoretic behaviors of 6 μm polystyrene beads were demonstrated in the 1 mm deep micro-well, with medium conductivities ranging from 0.0001 S/m to 1.3 S/m, and applied signal frequencies from 100 Hz to 10 MHz. Negative dielectrophoretic responses were observed in three dimensions over most of the conductivity-frequency space and cross-over frequency values are consistent with previously reported literature values. The device did not prevent AC electroosmosis and electrothermal flows, which occurred in the low and high frequency regions, respectively. The graphene paper utilized in this device is versatile and could subsequently function as a biosensor after dielectrophoretic characterizations are complete. PMID:24998694

Development of a 3D graphene electrode dielectrophoretic device.

PubMed

Xie, Hongyu; Tewari, Radheshyam; Fukushima, Hiroyuki; Narendra, Jeffri; Heldt, Caryn; King, Julia; Minerick, Adrienne R

2014-06-22

The design and fabrication of a novel 3D electrode microdevice using 50 µm thick graphene paper and 100 µm double sided tape is described. The protocol details the procedures to construct a versatile, reusable, multiple layer, laminated dielectrophoresis chamber. Specifically, six layers of 50 µm x 0.7 cm x 2 cm graphene paper and five layers of double sided tape were alternately stacked together, then clamped to a glass slide. Then a 700 μm diameter micro-well was drilled through the laminated structure using a computer-controlled micro drilling machine. Insulating properties of the tape layer between adjacent graphene layers were assured by resistance tests. Silver conductive epoxy connected alternate layers of graphene paper and formed stable connections between the graphene paper and external copper wire electrodes. The finished device was then clamped and sealed to a glass slide. The electric field gradient was modeled within the multi-layer device. Dielectrophoretic behaviors of 6 μm polystyrene beads were demonstrated in the 1 mm deep micro-well, with medium conductivities ranging from 0.0001 S/m to 1.3 S/m, and applied signal frequencies from 100 Hz to 10 MHz. Negative dielectrophoretic responses were observed in three dimensions over most of the conductivity-frequency space and cross-over frequency values are consistent with previously reported literature values. The device did not prevent AC electroosmosis and electrothermal flows, which occurred in the low and high frequency regions, respectively. The graphene paper utilized in this device is versatile and could subsequently function as a biosensor after dielectrophoretic characterizations are complete.

Contribution of dielectric screening to the total capacitance of few-layer graphene electrodes

DOE PAGES

Zhan, Cheng; Jiang, De-en

2016-02-17

We apply joint density functional theory (JDFT), which treats the electrode/electrolyte interface self-consistently, to an electric double-layer capacitor (EDLC) based on few-layer graphene electrodes. The JDFT approach allows us to quantify a third contribution to the total capacitance beyond quantum capacitance (C Q) and EDL capacitance (C EDL). This contribution arises from the dielectric screening of the electric field by the surface of the few-layer graphene electrode, and we therefore term it the dielectric capacitance (C Dielec). We find that C Dielec becomes significant in affecting the total capacitance when the number of graphene layers in the electrode is moremore » than three. In conclusion, our investigation sheds new light on the significance of the electrode dielectric screening on the capacitance of few-layer graphene electrodes.« less

Electric double layer capacitors employing nitrogen and sulfur co-doped, hierarchically porous graphene electrodes with synergistically enhanced performance

NASA Astrophysics Data System (ADS)

Kannan, Aravindaraj G.; Samuthirapandian, Amaresh; Kim, Dong-Won

2017-01-01

Hierarchically porous graphene nanosheets co-doped with nitrogen and sulfur are synthesized via a simple hydrothermal method, followed by a pore activation step. Pore architectures are controlled by varying the ratio of chemical activation agents to graphene, and its influence on the capacitive performance is evaluated. The electric double layer capacitor (EDLC) assembled with optimized dual-doped graphene delivers a high specific capacitance of 146.6 F g-1 at a current density of 0.8 A g-1, which is higher than that of cells with un-doped and single-heteroatom doped graphene. The EDLC with dual-doped graphene electrodes exhibits stable cycling performance with a capacitance retention of 94.5% after 25,000 cycles at a current density of 3.2 A g-1. Such a good performance can be attributed to synergistic effects due to co-doping of the graphene nanosheets and the presence of hierarchical porous structures.

Nickel–cobalt layered double hydroxide ultrathin nanoflakes decorated on graphene sheets with a 3D nanonetwork structure as supercapacitive materials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yan, Tao; Li, Ruiyi; Li, Zaijun, E-mail: zaijunli@263.net

2014-03-01

Graphical abstract: The microwave heating reflux approach was developed for the fabrication of nickel–cobalt layered double hydroxide ultrathin nanoflakes decorated on graphene sheets, in which ammonia and ethanol were used as the precipitator and medium for the synthesis. The obtained composite shows a 3D flowerclusters morphology with nanonetwork structure and largely enhanced supercapacitive performance. - Highlights: • The paper reported the microwave synthesis of nickel–cobalt layered double hydroxide/graphene composite. • The novel synthesis method is rapid, green, efficient and can be well used to the mass production. • The as-synthesized composite offers a 3D flowerclusters morphology with nanonetwork structure. •more » The composite offers excellent supercapacitive performance. • This study provides a promising route to design and synthesis of advanced graphene-based materials with the superiorities of time-saving and cost-effective characteristics. - Abstract: The study reported a novel microwave heating reflux method for the fabrication of nickel–cobalt layered double hydroxide ultrathin nanoflakes decorated on graphene sheets (GS/NiCo-LDH). Ammonia and ethanol were employed as precipitant and reaction medium for the synthesis, respectively. The resulting GS/NiCo-LDH offers a 3D flowerclusters morphology with nanonetwork structure. Due to the greatly enhanced rate of electron transfer and mass transport, the GS/NiCo-LDH electrode exhibits excellent supercapacitive performances. The maximum specific capacitance was found to be 1980.7 F g{sup −1} at the current density of 1 A g{sup −1}. The specific capacitance can remain 1274.7 F g{sup −1} at the current density of 15 A g{sup −1} and it has an increase of about 2.9% after 1500 cycles. Moreover, the study also provides a promising approach for the design and synthesis of metallic double hydroxides/graphene hybrid materials with time-saving and cost-effective characteristics, which can be potentially applied in the energy storage/conversion devices.« less

Frictional Magneto-Coulomb Drag in Graphene Double-Layer Heterostructures.

PubMed

Liu, Xiaomeng; Wang, Lei; Fong, Kin Chung; Gao, Yuanda; Maher, Patrick; Watanabe, Kenji; Taniguchi, Takashi; Hone, James; Dean, Cory; Kim, Philip

2017-08-04

Coulomb interaction between two closely spaced parallel layers of conductors can generate the frictional drag effect by interlayer Coulomb scattering. Employing graphene double layers separated by few-layer hexagonal boron nitride, we investigate density tunable magneto- and Hall drag under strong magnetic fields. The observed large magnetodrag and Hall-drag signals can be related with Laudau level filling status of the drive and drag layers. We find that the sign and magnitude of the drag resistivity tensor can be quantitatively correlated to the variation of magnetoresistivity tensors in the drive and drag layers, confirming a theoretical formula for magnetodrag in the quantum Hall regime. The observed weak temperature dependence and ∼B^{2} dependence of the magnetodrag are qualitatively explained by Coulomb scattering phase-space argument.

Van Der Waals heterogeneous layer-layer carbon nanostructures involving π···H-C-C-H···π···H-C-C-H stacking based on graphene and graphane sheets.

PubMed

Yuan, Kun; Zhao, Rui-Sheng; Zheng, Jia-Jia; Zheng, Hong; Nagase, Shigeru; Zhao, Sheng-Dun; Liu, Yan-Zhi; Zhao, Xiang

2017-04-15

Noncovalent interactions involving aromatic rings, such as π···π stacking, CH···π are very essential for supramolecular carbon nanostructures. Graphite is a typical homogenous carbon matter based on π···π stacking of graphene sheets. Even in systems not involving aromatic groups, the stability of diamondoid dimer and layer-layer graphane dimer originates from C - H···H - C noncovalent interaction. In this article, the structures and properties of novel heterogeneous layer-layer carbon-nanostructures involving π···H-C-C-H···π···H-C-C-H stacking based on [n]-graphane and [n]-graphene and their derivatives are theoretically investigated for n = 16-54 using dispersion corrected density functional theory B3LYP-D3 method. Energy decomposition analysis shows that dispersion interaction is the most important for the stabilization of both double- and multi-layer-layer [n]-graphane@graphene. Binding energy between graphane and graphene sheets shows that there is a distinct additive nature of CH···π interaction. For comparison and simplicity, the concept of H-H bond energy equivalent number of carbon atoms (noted as NHEQ), is used to describe the strength of these noncovalent interactions. The NHEQ of the graphene dimers, graphane dimers, and double-layered graphane@graphene are 103, 143, and 110, indicating that the strength of C-H···π interaction is close to that of π···π and much stronger than that of C-H···H-C in large size systems. Additionally, frontier molecular orbital, electron density difference and visualized noncovalent interaction regions are discussed for deeply understanding the nature of the C-H···π stacking interaction in construction of heterogeneous layer-layer graphane@graphene structures. We hope that the present study would be helpful for creations of new functional supramolecular materials based on graphane and graphene carbon nano-structures. © 2017 Wiley Periodicals, Inc. © 2017 Wiley Periodicals, Inc.

Electrochemical double-layer capacitors based on functionalized graphene

NASA Astrophysics Data System (ADS)

Pope, Michael Allan

Graphene is a promising electrode material for electrochemical double-layer capacitors (EDLCs) used for energy storage due to its high electrical conductivity and theoretical specific surface area. However, the intrinsic capacitance of graphene is known to be low and governed by the electronic side of the interface. Furthermore, graphene tends to aggregate and stack together when processed into thick electrode films. This significantly lowers the ion-accessible specific surface area (SSA). Maximizing both the SSA and the intrinsic capacitance are the main problems addressed in this thesis in an effort to improve the specific capacitance and energy density of EDLCs. In contrast to pristine graphene, functionalized graphene produced by the thermal exfoliation of graphite oxide contains residual functional groups and lattice defects. To study how these properties affect the double-layer capacitance, a model electrode system capable of measuring the intrinsic electrochemical properties of functionalized graphene was developed. To prevent artifacts and uncertainties related to measurements on porous electrodes, the functionalized graphene sheets (FGSs) were assembled as densely tiled monolayers using a Langmuir-Blodgett technique. In this way, charging can be studied in a well-defined 2D geometry. The possibility of measuring and isolating the intrinsic electrochemical properties of FGS monolayers was first demonstrated by comparing capacitance and redox probe measurements carried out on coatings deposited on passivated gold and single crystal graphite substrates. This monolayer system was then used to follow the double-layer capacitance of the FGS/electrolyte interface as the structure and chemistry of graphene was varied by thermal treatments ranging from 300 °C to 2100 °C. Elemental analysis and Raman spectroscopy were used to determine the resulting chemical and structural transformation upon heat treatment. It was demonstrated that intrinsically defective graphene monolayers can exhibit four-fold higher double-layer capacitance than pristine graphene. High temperature annealing lowered the capacitance until it approached that of pristine graphene. An optimal level of functionalization and lattice disorder is found necessary to retain high double-layer capacitance suggesting that graphene-based materials can be chemically tailored to engineer higher capacitance electrodes. The second half of this thesis focuses on understanding the factors that control the SSA of FGS aggregates when processed into dense electrodes and the development of a new electrode fabrications strategy to improve the ion-accessible surface area of FGS-based electrodes. Using various processing conditions, it was demonstrated that aggregates can exhibit a wide range of SSAs (1 m 2/g to 1750 m2/g) accessible to the adsorption of nitrogen or methylene blue. The effects of capillary forces, van der Waals interactions and aggregation kinetics on the SSA were explored and an aggregation model was proposed to account for these effects. In order to minimize aggregation, a new strategy for preparing graphene-based electrodes for EDLCs was developed. Colloidal gels of graphene oxide in a water-ethanol-ionic liquid solution were assembled into graphene-ionic liquid laminated structures. Our process involves evaporating the solvents water and ethanol yielding a graphene oxide/ionic liquid composite, followed by thermal reduction of the graphene oxide to electrically conducting functionalized graphene. This yields an electrode in which the ionic liquid serves not only as the working electrolyte but also as a spacer to separate the graphene sheets and to increase their electrolyte-accessible surface area. Using this approach, we achieve an outstanding energy density of 17.5 Wh/kg at a gravimetric capacitance of 156 F/g and 3 V operating voltage, due to a high effective density of the active electrode material of 0.46 g/cm2. By increasing the ionic liquid content and degree of thermal reduction, we obtain electrodes that retain >90% of their capacity at a scan rate of 500 mV/s, illustrating that we can tailor the electrodes towards higher power density if energy density is not the primary goal. The ease of manufacturing, achieved by combining the steps of electrode assembly and electrolyte infiltration, makes this bottom-up assembly approach scalable and well suited for combinations of potentially any graphene material with ionic liquid electrolytes.

Low Temperature Graphene Synthesis from Poly(methyl methacrylate) Using Microwave Plasma Treatment

NASA Astrophysics Data System (ADS)

Yamada, Takatoshi; Ishihara, Masatou; Hasegawa, Masataka

2013-11-01

A graphene film having low sheet resistance (600 Ω/sq.) was synthesized at low temperatures of 280 °C. Utilizing microwave plasma treatment, graphene films were synthesized from a solid phase on a copper surface. The full width at half maximum of the 2D-band in the Raman spectrum indicated that a high quality graphene film was formed. Cross-sectional transmission electron microscopy observation revealed that the deposited graphene films consisted of single- or double-layer graphene flakes of nanometer order on the Cu surface, which agrees with the estimated number of layers from an average optical transmittance of 96%.

Quantum Effects on the Capacitance of Graphene-Based Electrodes

DOE PAGES

Zhan, Cheng; Neal, Justin; Wu, Jianzhong; ...

2015-09-08

We recently measured quantum capacitance for electric double layers (EDL) at electrolyte/graphene interfaces. However, the importance of quantum capacitance in realistic carbon electrodes is not clear. Toward understanding that from a theoretical perspective, here we studied the quantum capacitance and total capacitance of graphene electrodes as a function of the number of graphene layers. The quantum capacitance was obtained from electronic density functional theory based on fixed band approximation with an implicit solvation model, while the EDL capacitances were from classical density functional theory. We found that quantum capacitance plays a dominant role in total capacitance of the single-layer graphenemore » both in aqueous and ionic-liquid electrolytes but the contribution decreases as the number of graphene layers increases. Moreover, the total integral capacitance roughly levels off and is dominated by the EDL capacitance beyond about four graphene layers. Finally, because many porous carbons have nanopores with stacked graphene layers at the surface, this research provides a good estimate of the effect of quantum capacitance on their electrochemical performance.« less

Graphene electrode modified with electrochemically reduced graphene oxide for label-free DNA detection.

PubMed

Li, Bing; Pan, Genhua; Avent, Neil D; Lowry, Roy B; Madgett, Tracey E; Waines, Paul L

2015-10-15

A novel printed graphene electrode modified with electrochemically reduced graphene oxide was developed for the detection of a specific oligonucleotide sequence. The graphene oxide was immobilized onto the surface of a graphene electrode via π-π bonds and electrochemical reduction of graphene oxide was achieved by cyclic voltammetry. A much higher redox current was observed from the reduced graphene oxide-graphene double-layer electrode, a 42% and 36.7% increase, respectively, in comparison with that of a bare printed graphene or reduced graphene oxide electrode. The good electron transfer activity is attributed to a combination of the large number of electroactive sites in reduced graphene oxide and the high conductivity nature of graphene. The probe ssDNA was further immobilized onto the surface of the reduced graphene oxide-graphene double-layer electrode via π-π bonds and then hybridized with its target cDNA. The change of peak current due to the hybridized dsDNA could be used for quantitative sensing of DNA concentration. It has been demonstrated that a linear range from 10(-7)M to 10(-12)M is achievable for the detection of human immunodeficiency virus 1 gene with a detection limit of 1.58 × 10(-13)M as determined by three times standard deviation of zero DNA concentration. Copyright © 2015 Elsevier B.V. All rights reserved.

Carrier mobility and scattering lifetime in electric double-layer gated few-layer graphene

NASA Astrophysics Data System (ADS)

Piatti, E.; Galasso, S.; Tortello, M.; Nair, J. R.; Gerbaldi, C.; Bruna, M.; Borini, S.; Daghero, D.; Gonnelli, R. S.

2017-02-01

We fabricate electric double-layer field-effect transistor (EDL-FET) devices on mechanically exfoliated few-layer graphene. We exploit the large capacitance of a polymeric electrolyte to study the transport properties of three, four and five-layer samples under a large induced surface charge density both above and below the glass transition temperature of the polymer. We find that the carrier mobility shows a strong asymmetry between the hole and electron doping regime. We then employ ab initio density functional theory (DFT) calculations to determine the average scattering lifetime from the experimental data. We explain its peculiar dependence on the carrier density in terms of the specific properties of the electrolyte we used in our experiments.

Graphene-based stretchable and transparent moisture barrier

NASA Astrophysics Data System (ADS)

Won, Sejeong; Van Lam, Do; Lee, Jin Young; Jung, Hyun-June; Hur, Min; Kim, Kwang-Seop; Lee, Hak-Joo; Kim, Jae-Hyun

2018-03-01

We propose an alumina-deposited double-layer graphene (2LG) as a transparent, scalable, and stretchable barrier against moisture; this barrier is indispensable for foldable or stretchable organic displays and electronics. Both the barrier property and stretchability were significantly enhanced through the introduction of 2LG between alumina and a polymeric substrate. 2LG with negligible polymeric residues was coated on the polymeric substrate via a scalable dry transfer method in a roll-to-roll manner; an alumina layer was deposited on the graphene via atomic layer deposition. The effect of the graphene layer on crack generation in the alumina layer was systematically studied under external strain using an in situ micro-tensile tester, and correlations between the deformation-induced defects and water vapor transmission rate were quantitatively analyzed. The enhanced stretchability of alumina-deposited 2LG originated from the interlayer sliding between the graphene layers, which resulted in the crack density of the alumina layer being reduced under external strain.

Measuring the complex optical conductivity of graphene by Fabry-Pérot reflectance spectroscopy [Determination of the optical index for few-layer graphene by reflectivity spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ghamsari, Behnood G.; Tosado, Jacob; Yamamoto, Mahito

Here, we have experimentally studied the optical refractive index of few-layer graphene through reflection spectroscopy at visible wavelengths. A laser scanning microscope (LSM) with a coherent supercontinuum laser source measured the reflectivity of an exfoliated graphene flake on a Si/SiO 2 substrate, containing monolayer, bilayer and trilayer areas, as the wavelength of the laser was varied from 545nm to 710nm. The complex refractive index of few-layer graphene, n-ik, was extracted from the reflectivity contrast to the bare substrate and the Fresnel reflection theory. Since the SiO 2 thickness enters to the modeling as a parameter, it was precisely measured atmore » the location of the sample. It was found that a common constant optical index cannot explain the wavelength-dependent reflectivity data for single-, double- and three-layer graphene simultaneously, but rather each individual few-layer graphene possesses a unique optical index whose complex values were precisely and accurately determined from the experimental data.« less

Measuring the complex optical conductivity of graphene by Fabry-Pérot reflectance spectroscopy [Determination of the optical index for few-layer graphene by reflectivity spectroscopy

DOE PAGES

Ghamsari, Behnood G.; Tosado, Jacob; Yamamoto, Mahito; ...

2016-09-29

Here, we have experimentally studied the optical refractive index of few-layer graphene through reflection spectroscopy at visible wavelengths. A laser scanning microscope (LSM) with a coherent supercontinuum laser source measured the reflectivity of an exfoliated graphene flake on a Si/SiO 2 substrate, containing monolayer, bilayer and trilayer areas, as the wavelength of the laser was varied from 545nm to 710nm. The complex refractive index of few-layer graphene, n-ik, was extracted from the reflectivity contrast to the bare substrate and the Fresnel reflection theory. Since the SiO 2 thickness enters to the modeling as a parameter, it was precisely measured atmore » the location of the sample. It was found that a common constant optical index cannot explain the wavelength-dependent reflectivity data for single-, double- and three-layer graphene simultaneously, but rather each individual few-layer graphene possesses a unique optical index whose complex values were precisely and accurately determined from the experimental data.« less

Local, global, and nonlinear screening in twisted double-layer graphene

DOE PAGES

Lu, Chih -Pin; Rodriguez-Vega, Martin; Li, Guohong; ...

2016-06-02

One-atom-thick crystalline layers and their vertical heterostructures carry the promise of designer electronic materials that are unattainable by standard growth techniques. To realize their potential it is necessary to isolate them from environmental disturbances, in particular those introduced by the substrate. However, finding and characterizing suitable substrates, and minimizing the random potential fluctuations they introduce, has been a persistent challenge in this emerging field. In this paper, we show that Landau-level (LL) spectroscopy offers the unique capability to quantify both the reduction of the quasiparticles’ lifetime and the long-range inhomogeneity due to random potential fluctuations. Harnessing this technique together withmore » direct scanning tunneling microscopy and numerical simulations we demonstrate that the insertion of a graphene buffer layer with a large twist angle is a very effective method to shield a 2D system from substrate interference that has the additional desirable property of preserving the electronic structure of the system under study. Finally, we further show that owing to its remarkable nonlinear screening capability a single graphene buffer layer provides better shielding than either increasing the distance to the substrate or doubling the carrier density and reduces the amplitude of the potential fluctuations in graphene to values even lower than the ones in AB-stacked bilayer graphene.« less

Local, global, and nonlinear screening in twisted double-layer graphene

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lu, Chih -Pin; Rodriguez-Vega, Martin; Li, Guohong

One-atom-thick crystalline layers and their vertical heterostructures carry the promise of designer electronic materials that are unattainable by standard growth techniques. To realize their potential it is necessary to isolate them from environmental disturbances, in particular those introduced by the substrate. However, finding and characterizing suitable substrates, and minimizing the random potential fluctuations they introduce, has been a persistent challenge in this emerging field. In this paper, we show that Landau-level (LL) spectroscopy offers the unique capability to quantify both the reduction of the quasiparticles’ lifetime and the long-range inhomogeneity due to random potential fluctuations. Harnessing this technique together withmore » direct scanning tunneling microscopy and numerical simulations we demonstrate that the insertion of a graphene buffer layer with a large twist angle is a very effective method to shield a 2D system from substrate interference that has the additional desirable property of preserving the electronic structure of the system under study. Finally, we further show that owing to its remarkable nonlinear screening capability a single graphene buffer layer provides better shielding than either increasing the distance to the substrate or doubling the carrier density and reduces the amplitude of the potential fluctuations in graphene to values even lower than the ones in AB-stacked bilayer graphene.« less

Bimodal behaviour of charge carriers in graphene induced by electric double layer

PubMed Central

Tsai, Sing-Jyun; Yang, Ruey-Jen

2016-01-01

A theoretical investigation is performed into the electronic properties of graphene in the presence of liquid as a function of the contact area ratio. It is shown that the electric double layer (EDL) formed at the interface of the graphene and the liquid causes an overlap of the conduction bands and valance bands and increases the density of state (DOS) at the Fermi energy (EF). In other words, a greater number of charge carriers are induced for transport and the graphene changes from a semiconductor to a semimetal. In addition, it is shown that the dependence of the DOS at EF on the contact area ratio has a bimodal distribution which responses to the experimental observation, a pinnacle curve. The maximum number of induced carriers is expected to occur at contact area ratios of 40% and 60%. In general, the present results indicate that modulating the EDL provides an effective means of tuning the electronic properties of graphene in the presence of liquid. PMID:27464986

Computational insight into the capacitive performance of graphene edge planes

DOE PAGES

Zhan, Cheng; Zhang, Yu; Cummings, Peter T.; ...

2017-02-01

Recent experiments have shown that electric double-layer capacitors utilizing electrodes consisting of graphene edge plane exhibit higher capacitance than graphene basal plane. However, theoretical understanding of this capacitance enhancement is still limited. Here we applied a self-consistent joint density functional theory calculation on the electrode/electrolyte interface and found that the capacitance of graphene edge plane depends on the edge type: zigzag edge has higher capacitance than armchair edge due to the difference in their electronic structures. We further examined the quantum, dielectric, and electric double-layer (EDL) contributions to the total capacitance of the edge-plane electrodes. Classical molecular dynamics simulation foundmore » that the edge planes have higher EDL capacitance than the basal plane due to better adsorption of counter-ions and higher solvent accessible surface area. Finally, our work therefore has elucidated the capacitive energy storage in graphene edge planes that take into account both the electrode's electronic structure and the EDL structure.« less

Resonant and nondissipative tunneling in independently contacted graphene structures

NASA Astrophysics Data System (ADS)

Vasko, F. T.

2013-02-01

The tunneling processes between independently contacted graphene sheets separated by thin insulator are restricted by the momentum and energy conservation laws. Because of this, both dissipative tunneling transitions, with momentum transfer due to disorder scattering, and nondissipative regime of tunneling, which appears due to intersection of electron and hole branches of energy spectrum, must be taken into account. The tunneling current density is calculated for the graphene-boron nitride-graphene layers, which is described by the tight-binding approach, and for the predominant momentum scattering by static disorder. Dependencies of current on concentrations in top and bottom graphene layers, which are governed by the voltages applied through independent contacts and gates, are considered for the back- and double-gated structures. The current-voltage characteristics of the back-gated structure are in agreement with the recent experiment [ScienceSCIEAS0036-807510.1126/science.1218461 335, 947 (2012)]. For the double-gated structures, the resonant dissipative tunneling causes a 10-fold enhancement of response which is important for transistor applications.

High-efficiency and multi-frequency polarization converters based on graphene metasurface with twisting double L-shaped unit structure array

NASA Astrophysics Data System (ADS)

Chen, Ming; Xiao, Xiaofei; Chang, Linzi; Wang, Congyun; Zhao, Deping

2017-07-01

In this work, a high-efficiency and tunable dual-frequency reflective polarization converter composed of graphene metasurface with twisting double L-shaped unit is firstly realized. Numerical results demonstrate that the device can convert a linearly polarized wave to its cross-polarized wave, and meantime it can also convert to a circularly polarized wave. Subsequently, one thickness of 500 nm SiO2 layer sandwiched by two graphene metasurfaces with similar pattern is stacked on the top of the two-layered structure, a four-frequency efficient reflective polarization converters is realized. Above all, those working frequencies can also be dynamically tuned within a large frequency range by adjusting the Fermi energy of the graphene, without reoptimizing and refabricating the nanostructures, which paves a novel way toward developing a controllable polarization converter for mid-infrared applications.

Enhanced performance of photonic crystal GaN light-emitting diodes with graphene transparent electrodes

NASA Astrophysics Data System (ADS)

Ge, Hai-Liang; Xu, Chen; Xu, Kun; Xun, Meng; Wang, Jun; Liu, Jie

2015-03-01

The two-dimensional (2D) triangle lattice air hole photonic crystal (PC) GaN-based light-emitting diodes (LED) with double-layer graphene transparent electrodes (DGTE) have been produced. The current spreading effect of the double-layer graphene (GR) on the surface of the PC structure of the LED has been researched. Specially, we found that the part of the graphene suspending over the air hole of the PC structure was of much higher conductivity, which reduced the average sheet resistance of the graphene transparent conducting electrode and improved the current spreading of the PC LED. Therefore, the work voltage of the DGTE-PC LED was obviously decreased, and the output power was greatly enhanced. The COMSOL software was used to simulate the current density distribution of the samples. The results show that the etching of PC structure results in the degradation of the current spreading and that the graphene transparent conducting electrode can offer an uniform current spreading in the DGTE-PC LED. PACS: 85.60.Jb; 68.65.Pq; 42.70.Qs

How the Number of Layers and Relative Position Modulate the Interlayer Electron Transfer in π-Stacked 2D Materials.

PubMed

Biancardi, Alessandro; Caraiani, Claudiu; Chan, Wai-Lun; Caricato, Marco

2017-04-06

Understanding the interfacial electron transfer (IET) between 2D layers is central to technological applications. We present a first-principles study of the IET between a zinc phthalocyanine film and few-layer graphene by using our recent method for the calculation of electronic coupling in periodic systems. The ultimate goal is the development of a predictive in silico approach for designing new 2D materials. We find IET to be critically dependent on the number of layers and their stacking orientation. In agreement with experiment, IET to single-layer graphene is shown to be faster than that to double-layer graphene due to interference effects between layers. We predict that additional graphene layers increase the number of IET pathways, eventually leading to a faster rate. These results shed new light on the subtle interplay between structure and IET, which may lead to more effective "bottom up" design strategies for these materials.

Graphene Double-Layer Capacitor with ac Line-Filtering Performance

NASA Astrophysics Data System (ADS)

Miller, John R.; Outlaw, R. A.; Holloway, B. C.

2010-09-01

Electric double-layer capacitors (DLCs) can have high storage capacity, but their porous electrodes cause them to perform like resistors in filter circuits that remove ripple from rectified direct current. We have demonstrated efficient filtering of 120-hertz current with DLCs with electrodes made from vertically oriented graphene nanosheets grown directly on metal current collectors. This design minimized electronic and ionic resistances and produced capacitors with RC time constants of less than 200 microseconds, in contrast with ~1 second for typical DLCs. Graphene nanosheets have a preponderance of exposed edge planes that greatly increases charge storage as compared with that of designs that rely on basal plane surfaces. Capacitors constructed with these electrodes could be smaller than the low-voltage aluminum electrolyte capacitors that are typically used in electronic devices.

Graphene double-layer capacitor with ac line-filtering performance.

PubMed

Miller, John R; Outlaw, R A; Holloway, B C

2010-09-24

Electric double-layer capacitors (DLCs) can have high storage capacity, but their porous electrodes cause them to perform like resistors in filter circuits that remove ripple from rectified direct current. We have demonstrated efficient filtering of 120-hertz current with DLCs with electrodes made from vertically oriented graphene nanosheets grown directly on metal current collectors. This design minimized electronic and ionic resistances and produced capacitors with RC time constants of less than 200 microseconds, in contrast with ~1 second for typical DLCs. Graphene nanosheets have a preponderance of exposed edge planes that greatly increases charge storage as compared with that of designs that rely on basal plane surfaces. Capacitors constructed with these electrodes could be smaller than the low-voltage aluminum electrolyte capacitors that are typically used in electronic devices.

Adsorption and Formation of Small Na Clusters on Pristine and Double-Vacancy Graphene for Anodes of Na-Ion Batteries.

PubMed

Liang, Zhicong; Fan, Xiaofeng; Zheng, Weitao; Singh, David J

2017-05-24

Layered carbon is a likely anode material for Na-ion batteries (NIBs). Graphitic carbon has a low capacity of approximately 35 (mA h)/g due to the formation of NaC 64 . Using first-principles methods including van der Waals interactions, we analyze the adsorption of Na ions and clusters on graphene in the context of anodes. The interaction between Na ions and graphene is found to be weak. Small Na clusters are not stable on the surface of pristine graphene in the electrochemical environment of NIBs. However, we find that Na ions and clusters can be stored effectively on defected graphene that has double vacancies. In addition, the adsorption energy of small Na clusters near a double vacancy is found to decrease with increasing cluster size. With high concentrations of vacancies the capacity of Na on defective graphene is found to be as much as 10-30 times higher than that of graphitic carbon.

Postbuckling analysis of multi-layered graphene sheets under non-uniform biaxial compression

NASA Astrophysics Data System (ADS)

Farajpour, Ali; Arab Solghar, Alireza; Shahidi, Alireza

2013-01-01

In this article, the nonlinear buckling characteristics of multi-layered graphene sheets are investigated. The graphene sheet is modeled as an orthotropic nanoplate with size-dependent material properties. The graphene film is subjected by non-uniformly distributed in-plane load through its thickness. To include the small scale and the geometrical nonlinearity effects, the governing differential equations are derived based on the nonlocal elasticity theory in conjunction with the von Karman geometrical model. Explicit expressions for the postbuckling loads of single- and double-layered graphene sheets with simply supported edges under biaxial compression are obtained. For numerical results, six types of armchair and zigzag graphene sheets with different aspect ratio are considered. The present formulation and method of solution are validated by comparing the results, in the limit cases, with those available in the open literature. Excellent agreement between the obtained and available results is observed. Finally, the effects of nonlocal parameter, buckling mode number, compression ratio and non-uniform parameter on the postbuckling behavior of multi-layered graphene sheets are studied.

Renewing functionalized graphene as electrodes for high-performance supercapacitors.

PubMed

Fang, Yan; Luo, Bin; Jia, Yuying; Li, Xianglong; Wang, Bin; Song, Qi; Kang, Feiyu; Zhi, Linjie

2012-12-11

An acid-assisted ultrarapid thermal strategy is developed for constructing specifically functionalized graphene. The electrochemical performance of functionalized graphene can be boosted via elaborate coupling between the pseudocapacitance and the electronic double layer capacitance through rationally tailoring the structure of graphene sheets. This presents an opportunity for developing further high-performance graphene-based electrodes to bridge the performance gap between traditional capacitors and batteries. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Graphene-Based Electrode for a Supercapacitor

NASA Technical Reports Server (NTRS)

Chen, Bin (Inventor); Meyyappan, Meyya (Inventor)

2015-01-01

A supercapacitor electrode mechanism comprising an electrically conductive, porous substrate, having one or more metallic oxides deposited on a first surface and a chemically reduced graphene oxide deposited on a second surface, to thereby provide an electrical double layer associated with the substrate. The substrate may be carbon paper or a similar substance. The layers of the supercapacitor are optionally rolled into an approximately cylindrical structure.

Band structure of one-dimensional photonic crystal with graphene layers using the Fresnel coefficients method

NASA Astrophysics Data System (ADS)

Jafari, A.; Rahmat, A.

2018-04-01

In this paper, we have calculated the band structure of an instance of one-dimensional photonic crystal (1DPC) composed of double-layered dielectrics via the Fresnel coefficients method. Then, we supposed the addition of a thin layer of graphene to each dielectric layer and the given photonic crystal (PC) composed of dielectric-graphene composites. The effects of graphene layers on the PC band structure were evaluated. We found out that according to the effective medium theory unlike the TE polarization, the electric permittivity of the dielectric layers changed at TM polarization. As such, the band structure of PC for TM polarization changed, too. Moreover, instead of bandgap related to “zero averaged refractive index” an approximately omnidirectional bandgap appeared and a related bandgap to “𝜀 = 0” disappeared. In addition, a new angular gap branch appeared at a new frequency at TM polarization in which the width of gap increased as the angle increased.

Investigation of the graphene-electrolyte interface in Li-air batteries: A molecular dynamics study

NASA Astrophysics Data System (ADS)

Pavlov, S. V.; Kislenko, S. A.

2018-01-01

In this work the behavior of the main reactants (Li+, O2) of the oxygen reduction reaction (ORR) in acetonitrile solvent near the multi-layer graphene edge has been studied. It was observed by molecular dynamics simulations that the concentration distributions of the Li+ and O2 represent a “chessboard” structure. It was ascertained that the concentrations of the lithium ions and oxygen molecules reach their maximum values near the graphene edges pushed out from the surface, which may act as nucleation centers for the formation of crystalline products of the ORR. The maps of the free energy were estimated for the Li+ and O2. Energy optimal trajectories for the adsorption of oxygen molecules and lithium ions were found. Moreover, the distributions of the electric potential were obtained near the following carbon surfaces: single- and multi-layer graphene edge, graphene plane, which shows the qualitative differences in the double-layer structure.

Dual functional passivating layer of graphene/TiO2 for improved performance of dye-sensitized solar cells

NASA Astrophysics Data System (ADS)

Shahid, Muhammad Umair; Mohamed, Norani Muti; Muhsan, Ali Samer; Khatani, Mehboob; Bashiri, Robabeh; Zaine, Siti Nur Azella; Shamsudin, Adel Eskandar

2018-02-01

The FTO/TiO2 interface plays a crucial role in the performance of dye-sensitized solar cells (DSSCs). The uneven microstructure morphology of FTO (fluorine-doped tin oxide) glass surface and high porosity of TiO2 layer produce tiny gaps and voids at the FTO/TiO2 interface that breaks the connectivity, leading to an increase in the recombination process. In the current work, a dual functional passivating layer is introduced by the combination of the graphene/TiO2 compact layer. The excellent mobility and flexibility of graphene is capitalized using its layer to fill the voids in the FTO surface, which can consequently reduce the charge transfer resistance at the interface, while the added TiO2 compact layer avoids direct contact with the electrolyte thus reducing the recombination. Graphene was synthesized by the facile solvent exfoliation method with the assistance of the probe sonication process. The parameters of sonication were optimized to achieve high-quality concentrated graphene inks (0.177-0.51 mg/ml). Raman spectroscopy and transmission electron microscopy (TEM) revealed that the graphene obtained is of a few-layer type. Electrochemical impedance spectroscopy (EIS) analysis indicated that the incorporated compact layer of graphene/TiO2 was capable of accelerating the charge transfer and reducing the recombination process at the FTO/TiO2 interface. Consequently, the photoconversion efficiency (PCE) for the device (1 cm2 active area) with double-coated graphene layer under one sun irradiation (AM 1.5) was found to be 49.49% higher than the conventional one.

Hybridization-induced broadband terahertz wave absorption with graphene metasurfaces.

PubMed

Mou, Nanli; Sun, Shulin; Dong, Hongxing; Dong, Shaohua; He, Qiong; Zhou, Lei; Zhang, Long

2018-04-30

Electromagnetic (EM) wave absorption plays a vital role in photonics. While metasurfaces are proposed to absorb EM waves efficiently, most of them exhibit limited bandwidth and fixed functionalities. Here, we propose a broadband and tunable terahertz (THz) absorber based on a graphene-based metasurface, which is constructed by a single layer of closely patterned graphene concentric double rings and a metallic mirror separated by an ultrathin SiO 2 layer. Plasmonic hybridization between two graphene rings significantly enlarges the absorption bandwidth, which can be further tuned by gating the graphene. Moreover, the specific design also makes our device insensitive to the incident angle and polarization state of impinging EM waves. Our results may inspire certain wave-modulation-related applications, such as THz imaging, smart absorber, tunable sensor, etc.

Superparamagnetic magnetite nanocrystals-graphene oxide nanocomposites: facile synthesis and their enhanced electric double-layer capacitor performance.

PubMed

Wang, Qihua; Wang, Dewei; Li, Yuqi; Wang, Tingmei

2012-06-01

Superparamagnetic magnetite nanocrystals-graphene oxide (FGO) nanocomposites were successfully synthesized through a simple yet versatile one-step solution-processed approach at ambient conditions. Magnetite (Fe3O4) nanocrystals (NCs) with a size of 10-50 nm were uniformly deposited on the surfaces of graphene oxide (GO) sheets, which were confirmed by transmission electron microscopy (TEM) and high-angle annular dark field scanning transmission election microscopy (HAADF-STEM) studies. FGO with different Fe3O4 loadings could be controlled by simply manipulating the initial weight ratio of the precursors. The M-H measurements suggested that the as-prepared FGO nanocomposites have a large saturation magnetizations that made them can move regularly under an external magnetic field. Significantly, FGO nanocomposites also exhibit enhanced electric double-layer capacitor (EDLC) activity compared with pure Fe3O4 NCs and GO in terms of specific capacitance and high-rate charge-discharge.

Performance of Liquid Phase Exfoliated Graphene As Electrochemical Double Layer Capacitors Electrodes

NASA Astrophysics Data System (ADS)

Huffstutler, Jacob; Wasala, Milinda; Richie, Julianna; Winchester, Andrew; Ghosh, Sujoy; Kar, Swastik; Talapatra, Saikat

2014-03-01

We will present the results of our investigations of electrochemical double layer capacitors (EDLCs) or supercapacitors (SC) fabricated using liquid-phase exfoliated graphene. Several electrolytes, such as aqueous potassium hydroxide KOH (6M), ionic 1-Butyl-3-methylimidazolium hexafluorophosphate [BMIM][PF6], and ionic 1-butyl-1-methylpyrrolidinium tris(pentafluoroethyl)trifluorophosphate[BMP][FAP] were used. These EDLC's show good performance compared to other carbon nanomaterials based EDLC's devices. We found that the liquid phase exfoliated graphene based devices possess specific capacitance values as high as 262 F/g, when used with ionic liquid electrolyte[BMP][FAP], with power densities (~ 454 W/kg) and energy densities (~ 0.38Wh/kg). Further, these devices indicated rapid charge transfer response even without the use of any binders or specially prepared current collectors. A detailed electrochemical impedance spectroscopy analysis in order to understand the phenomenon of charge storage in these materials will be presented.

Excitation of hybridized Dirac plasmon polaritons and transition radiation in multi-layer graphene traversed by a fast charged particle.

PubMed

Akbari, Kamran; Mišković, Zoran L; Segui, Silvina; Gervasoni, Juana L; Arista, Néstor R

2018-06-01

We analyze the energy loss channels for a fast charged particle traversing a multi-layer graphene (MLG) structure with N layers under normal incidence. Focusing on a terahertz (THz) range of frequencies, and assuming equally doped graphene layers with a large enough separation d between them to neglect interlayer electron hopping, we use the Drude model for two-dimensional conductivity of each layer to describe hybridization of graphene's Dirac plasmon polaritons (DPPs). Performing a layer decomposition of ohmic energy losses, which include excitation of hybridized DPPs (HDPPs), we have found for N = 3 that the middle HDPP eigenfrequency is not excited in the middle layer due to symmetry constraint, whereas the excitation of the lowest HDPP eigenfrequency produces a Fano resonance in the graphene layer that is first traversed by the charged particle. While the angular distribution of transition radiation emitted in the far field region also shows asymmetry with respect to the traversal order by the incident charged particle at supra-THz frequencies, the integrated radiative energy loss is surprisingly independent of both d and N for N ≤ 5, which is explained by a dominant role of the outer graphene layers in transition radiation. We have further found that the integrated ohmic energy loss in optically thin MLG scales as ∝1/N at sub-THz frequencies, which is explained by exposing the role of dissipative processes in graphene at low frequencies. Finally, prominent peaks are observed at supra-THz frequencies in the integrated ohmic energy loss for MLG structures that are not optically thin. The magnitude of those peaks is found to scale with N for N ≥ 2, while their shape and position replicate the peak in a double-layer graphene (N = 2), which is explained by arguing that plasmon hybridization in such MLG structures is dominated by electromagnetic interaction between the nearest-neighbor graphene layers.

Electrochemical immunosensor with NiAl-layered double hydroxide/graphene nanocomposites and hollow gold nanospheres double-assisted signal amplification.

PubMed

Qiao, Lu; Guo, Yemin; Sun, Xia; Jiao, Yancui; Wang, Xiangyou

2015-08-01

A sensitive electrochemical immunosensor based on NiAl-layered double hydroxide/graphene nanocomposites (NiAl-LDH/G) and hollow gold nanospheres (HGNs) was proposed for chlorpyrifos detection. The NiAl-LDH/G was prepared using a conventional coprecipitation process and reduction of the supporting graphene oxide. Subsequently, the nanocomposites were dispersed with chitosan (CS). The NiAl-LDH/G possessed good electrochemical behavior and high binding affinity to the electrode. The high surface areas of HGNs and the vast aminos and hydroxyls of CS provided a platform for the covalently crosslinking of antibody. Under optimal conditions, the immunosensor exhibited a wide linear range from 5 to 150 μg/mL and from 150 to 2 μg/mL, with a detection limit of 0.052 ng/mL. The detection results showed good agreement with standard gas chromatography method. The constructed immunosensor exhibited good reproducibility, high specificity, acceptable stability and regeneration performance, which provided a new promising tool for chlorpyrifos detection in real samples.

Design and numerical analysis of highly sensitive Au-MoS2-graphene based hybrid surface plasmon resonance biosensor

NASA Astrophysics Data System (ADS)

Rahman, M. Saifur; Anower, Md. Shamim; Hasan, Md. Rabiul; Hossain, Md. Biplob; Haque, Md. Ismail

2017-08-01

We demonstrate a highly sensitive Au-MoS2-Graphene based hybrid surface plasmon resonance (SPR) biosensor for the detection of DNA hybridization. The performance parameters of the proposed sensor are investigated in terms of sensitivity, detection accuracy and quality factor at operating wavelength of 633 nm. We observed in the numerical study that sensitivity can be greatly increased by adding MoS2 layer in the middle of a Graphene-on-Au layer. It is shown that by using single layer of MoS2 in between gold and graphene layer, the proposed biosensor exhibits simultaneously high sensitivity of 87.8 deg/RIU, high detection accuracy of 1.28 and quality factor of 17.56 with gold layer thickness of 50 nm. This increased performance is due to the absorption ability and optical characteristics of graphene biomolecules and high fluorescence quenching ability of MoS2. On the basis of changing in SPR angle and minimum reflectance, the proposed sensor can sense nucleotides bonding happened between double-stranded DNA (dsDNA) helix structures. Therefore, this sensor can successfully detect the hybridization of target DNAs to the probe DNAs pre-immobilized on the Au-MoS2-Graphene hybrid with capability of distinguishing single-base mismatch.

Two-band induced superconductivity in single-layer graphene and topological insulator bismuth selenide

NASA Astrophysics Data System (ADS)

Talantsev, E. F.; Crump, W. P.; Tallon, J. L.

2018-01-01

Proximity-induced superconductivity in single-layer graphene (SLG) and in topological insulators represent almost ideal examples of superconductivity in two dimensions. Fundamental mechanisms governing superconductivity in the 2D limit are of central interest for modern condensed-matter physics. To deduce fundamental parameters of superconductor/graphene/superconductor and superconductor/bismuth selenide/superconductor junctions we investigate the self-field critical currents in these devices using the formalism of the Ambegaokar-Baratoff model. Our central finding is that the induced superconducting state in SLG and bismuth selenide each exhibits gapping on two superconducting bands. Based on recent results obtained on ultra-thin films of natural superconductors, including single-atomic layer of iron selenide, double and triple atomic layers of gallium, and several atomic layer tantalum disulphide, we conclude that a two-band induced superconducting state in SLG and bismuth selenide is part of a wider, more general multiple-band phenomenology of currently unknown origin.

An ionic electro-active actuator made with graphene film electrode, chitosan and ionic liquid

NASA Astrophysics Data System (ADS)

He, Qingsong; Yu, Min; Yang, Xu; Kim, Kwang Jin; Dai, Zhendong

2015-06-01

A newly developed ionic electro-active actuator composed of an ionic electrolyte layer sandwiched between two graphene film layers was investigated. Scanning electronic microscopy observation and x-ray diffraction analysis showed that the graphene sheets in the film stacked in a nearly face-to-face fashion but did not restack back to graphite, and the resulting graphene film with low sheet resistance (10 Ω sq-1) adheres well to the electrolyte membrane. Contact angle measurement showed the surface energy (37.98 mJ m-2) of the ionic electrolyte polymer is 2.67 times higher than that (14.2 mJ m-2) of the Nafion membrane, contributing to the good adhesion between the graphene film electrode and the electrolyte membrane. An electric double-layer is formed at the interface between the graphene film electrode and the ionic electrolyte membrane under the input potential, resulting in a higher capacitance of 27.6 mF cm-2. We report that this ionic actuator exhibits adequate bending strain, ranging from 0.032 to 0.1% (305 to 945 μm) as functions of voltage.

Excitation of hybridized Dirac plasmon polaritons and transition radiation in multi-layer graphene traversed by a fast charged particle

NASA Astrophysics Data System (ADS)

Akbari, Kamran; Mišković, Zoran L.; Segui, Silvina; Gervasoni, Juana L.; Arista, Néstor R.

2018-06-01

We analyze the energy loss channels for a fast charged particle traversing a multi-layer graphene (MLG) structure with N layers under normal incidence. Focusing on a terahertz (THz) range of frequencies, and assuming equally doped graphene layers with a large enough separation d between them to neglect interlayer electron hopping, we use the Drude model for two-dimensional conductivity of each layer to describe hybridization of graphene’s Dirac plasmon polaritons (DPPs). Performing a layer decomposition of ohmic energy losses, which include excitation of hybridized DPPs (HDPPs), we have found for N = 3 that the middle HDPP eigenfrequency is not excited in the middle layer due to symmetry constraint, whereas the excitation of the lowest HDPP eigenfrequency produces a Fano resonance in the graphene layer that is first traversed by the charged particle. While the angular distribution of transition radiation emitted in the far field region also shows asymmetry with respect to the traversal order by the incident charged particle at supra-THz frequencies, the integrated radiative energy loss is surprisingly independent of both d and N for N ≤ 5, which is explained by a dominant role of the outer graphene layers in transition radiation. We have further found that the integrated ohmic energy loss in optically thin MLG scales as ∝1/N at sub-THz frequencies, which is explained by exposing the role of dissipative processes in graphene at low frequencies. Finally, prominent peaks are observed at supra-THz frequencies in the integrated ohmic energy loss for MLG structures that are not optically thin. The magnitude of those peaks is found to scale with N for N ≥ 2, while their shape and position replicate the peak in a double-layer graphene (N = 2), which is explained by arguing that plasmon hybridization in such MLG structures is dominated by electromagnetic interaction between the nearest-neighbor graphene layers.

Contamination-free Ge-based graphene as revealed by graphene enhanced secondary ion mass spectrometry (GESIMS)

NASA Astrophysics Data System (ADS)

Michałowski, P. P.; Pasternak, I.; Strupiński, W.

2018-01-01

In this study, we demonstrate that graphene grown on Ge does not contain any copper contamination, and identify some of the errors affecting the accuracy of commonly used measurement methods. Indeed, one of these, the secondary ion mass spectrometry (SIMS) technique, reveals copper contamination in Ge-based graphene but does not take into account the effect of the presence of the graphene layer. We have shown that this layer increases negative ionization significantly, and thus yields false results, but also that the graphene enhances, by an order of two, the magnitude of the intensity of SIMS signals when compared with a similar graphene-free sample, enabling much better detection limits. This forms the basis of a new measurement procedure, graphene enhanced SIMS (GESIMS) (pending European patent application no. EP 16461554.4), which allows for the precise estimation of the realistic distribution of dopants and contamination in graphene. In addition, we present evidence that the GESIMS effect leads to unexpected mass interferences with double-ionized species, and that these interferences are negligible in samples without graphene. The GESIMS method also shows that graphene transferred from Cu results in increased copper contamination.

Graphene, microscale metallic mesh, and transparent dielectric hybrid structure for excellent transparent electromagnetic interference shielding and absorbing

NASA Astrophysics Data System (ADS)

Lu, Zhengang; Ma, Limin; Tan, Jiubin; Wang, Heyan; Ding, Xuemei

2017-06-01

A high-performance transparent electromagnetic interference (EMI) shielding material based on a graphene/metallic mesh/transparent dielectric (GMTD) hybrid structure is designed and characterized. It consists of stacked graphene and metallic mesh layers, with neighboring layers separated by a quartz-glass substrsate. The GMTD hybrid structure combines the microwave-reflecting characteristics of the metallic mesh and the microwave-absorbing characteristics of graphene to achieve simultaneously high visible transmittance, strong microwave shielding effectiveness (SE), and low microwave reflection. Experiments show that a double-graphene and double-metallic mesh GMTD hybrid structure with a mesh periodicity of 160 µm provides microwave SE exceeding 47.79 dB in the K u-band, and an SE exceeding 32.12 dB in the K a-band, with a maximum value of 37.78 dB at 26.5 GHz. SE by absorption exceeds 30.78 dB in the K a-band, with a maximum value of 34.55 dB at 26.5 GHz, while maintaining a normalized visible transmittance of ~85% at 700 nm. This remarkable performance favors the application of the proposed structure as a transparent microwave shield and absorber, and offers a new strategy for transparent EMI shielding.

Hierarchical Ni-Co layered double hydroxide nanosheets on functionalized 3D-RGO films for high energy density asymmetric supercapacitor

NASA Astrophysics Data System (ADS)

Jiang, Liyang; Sui, Yanwei; Qi, Jiqiu; Chang, Yuan; He, Yezeng; Meng, Qingkun; Wei, Fuxiang; Sun, Zhi; Jin, Yunxue

2017-12-01

In this paper, ultrathin reduced graphene oxide films on nickel foam were fabricated via a facile dip-coating method combined with thermal reduction. Hierarchical Ni-Co layered double hydroxide nanosheets with network structure were electrodeposited on the ultrathin reduced graphene oxide films in a simple three-electrode system. The thickness of Ni-Co layered double hydroxide nanosheets can be controlled through adjusting the deposition temperature. The as-prepared electrode exhibited excellent electrochemical performance with specific capacitance of 1454.2 F g-1 at a current density of 1 A g-1. An asymmetric supercapacitor device was designed with the as-prepared composites as positive electrode material and Nitrogen-doped reduced graphene oxide as negative electrode material. This device could be operated in a working voltage range of 0-1.8 V in 1 M KOH aqueous electrolyte, delivering a high energy density of 56.4 W h kg-1 at a power density of 882.5 W kg-1. One supercapacitor can power two LEDs with rated voltage of 1.8-2.0 V. After 10,000 consecutive charge-discharge tests at 10 A g-1, this asymmetric supercapacitor revealed an excellent cycle life with 98.3% specific capacitance retention. These excellent electrochemical performances make it become one of most promising candidates for high energy supercapacitor device.

Graphene hydrogels deposited in nickel foams for high-rate electrochemical capacitors.

PubMed

Chen, Ji; Sheng, Kaixuan; Luo, Peihui; Li, Chun; Shi, Gaoquan

2012-08-28

Graphene hydrogel/nickel foam composite electrodes for high-rate electrochemical capacitors are produced by reduction of an aqueous dispersion of graphene oxide in a nickel foam (upper half of figure). The micropores of the hydrogel are exposed to the electrolyte so that ions can enter and form electrochemical double-layers. The nickel framework shortens the distances of charge transfer. Therefore, the electrochemical capacitor exhibits highrate performance (see plots). Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Mechanical and Electrochemical Performance of Graphene-Based Flexible Supercapacitors

DTIC Science & Technology

2014-08-01

Charge/ discharge testing of a packaged, flexible, graphene-based supercapacitor using 0.5 M K2SO4 electrolyte...the use of electrochemical double-layer capacitors (commonly referred to as “supercapacitors”) for high power charging/ discharging and long cyclic...exhibit rapid charging/ discharging and good performance over a wide temperature range. 1 Supercapacitors may prove useful as a standalone power

Facile preparation of magnetic graphene double-sided mesoporous composites for the selective enrichment and analysis of endogenous peptides.

PubMed

Yin, Peng; Sun, Nianrong; Deng, Chunhui; Li, Yan; Zhang, Xiangmin; Yang, Pengyuan

2013-08-01

In this work, magnetic graphene double-sided mesoporous nanocomposites (mag-graphene@mSiO₂) were synthesized by coating a layer of mesoporous silica materials on each side of magnetic grapheme. The surfactant (CTAB) mediated sol-gel coating was performed using tetraethyl orthosilicate as the silica source. The as-made magnetic graphene double-sided mesoporous silica composites were treated with high-temperature calcination to remove the hydroxyl on the surface. The novel double-sided materials possess high surface area (167.8 cm²/g) and large pore volume (0.2 cm³/g). The highly open pore structure presents uniform pore size (3.2 nm) and structural stability. The hydrophobic interior pore walls could ensure an efficient adsorption of target molecules through hydrophobic-hydrophobic interaction. At the same time, the magnetic Fe₃O₄ particles on both sides of the materials could simplify the process of enrichment, which plays an important role in the treatment of complex biological samples. The magnetic graphene double-sided nanocomposites were successfully applied to size-selective and specific enrichment of peptides in standard peptide mixtures, protein digest solutions, and human urine samples. Finally, the novel material was applied to selective enrichment of endogenous peptides in mouse brain tissue. The enriched endogenous peptides were then analyzed by LC-MS/MS, and 409 endogenous peptides were detected and identified. The results demonstrate that the as-made mag-graphene@mSiO₂ have powerful potential for peptidome research. © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Applications of Nanostructured Graphene in Optoelectronics as Transparent Conductors and Photodetectors

NASA Astrophysics Data System (ADS)

Xu, Guowei

Graphene, a single layer of carbon atoms arranged in a hexagonal lattice, has unique properties of high carrier mobility, high optical transmittance, chemical inertness and flexibility, making it attractive for electronic and optoelectronic applications, such as graphene transistors, ultrahigh capacitors, transparent conductors (TCs), photodetectors. This work explores novel schemes of nanostructured graphene for optoelectronic applications including advanced TCs and photodetectors. In nanophotonic graphene nanohole arrays patterned using nanoimprinting lithography (NIL), highly efficient chemical doping was achieved on the hole edges. This provides a unique scheme for improving both optical transmittance and electrical conductivity of graphene-based TCs. In plasmonic graphene, Ag nanoparticles were decorated on graphene using thermally assisted self-assembly and NIL. Much enhanced conductivity by a factor of 2-4 was achieved through electron doping in graphene from Ag nanoparticles. More importantly, surface plasmonic effect has been incorporated into plasmonic graphene as advanced TCs with light trapping, which is critical to ultrathin-film optoelectronics such as photovoltaics and photodetectors. Based on plasmonic graphene electric double-layer (EDL) transistor, a novel scheme of photodetection has been demonstrated using plasmonic enhanced local field gating. The resulting tuning of interfacial capacitance as well as the quantum capacitance of graphene manifested as extraordinary photoconductivity and hence photoresponse.

A broadband metamaterial absorber based on multi-layer graphene in the terahertz region

NASA Astrophysics Data System (ADS)

Fu, Pan; Liu, Fei; Ren, Guang Jun; Su, Fei; Li, Dong; Yao, Jian Quan

2018-06-01

A broadband metamaterial absorber, composed of the periodic graphene pattern on SiO2 dielectric with the double layer graphene films inserted in it and all of them backed by metal plan, is proposed and investigated. The simulation results reveal that the wide absorption band can be flexibly tuned between the low-frequency band and the high-frequency band by adjusting graphene's Fermi level. The absorption can achieve 90% in 5.50-7.10 THz, with Fermi level of graphene is 0.3 eV, while in 6.98-9.10 THz with Fermi level 0.6 eV. Furthermore, the proposed structure can be switched from reflection (>81%) to absorption (>90%) over the whole operation band, when the Fermi level of graphene varies from 0 to 0.6 eV. Besides, the proposed absorber is insensitive to the polarization and can work over a wide range of incident angle. Compared with the previous broadband absorber, our graphene based wideband terahertz absorber can enable a wide application of high performance terahertz devices, including sensors, imaging devices and electro-optic switches.

Scalable Synthesis of Freestanding Sandwich-structured Graphene/Polyaniline/Graphene Nanocomposite Paper for Flexible All-Solid-State Supercapacitor

NASA Astrophysics Data System (ADS)

Xiao, Fei; Yang, Shengxiong; Zhang, Zheye; Liu, Hongfang; Xiao, Junwu; Wan, Lian; Luo, Jun; Wang, Shuai; Liu, Yunqi

2015-03-01

We reported a scalable and modular method to prepare a new type of sandwich-structured graphene-based nanohybrid paper and explore its practical application as high-performance electrode in flexible supercapacitor. The freestanding and flexible graphene paper was firstly fabricated by highly reproducible printing technique and bubbling delamination method, by which the area and thickness of the graphene paper can be freely adjusted in a wide range. The as-prepared graphene paper possesses a collection of unique properties of highly electrical conductivity (340 S cm-1), light weight (1 mg cm-2) and excellent mechanical properties. In order to improve its supercapacitive properties, we have prepared a unique sandwich-structured graphene/polyaniline/graphene paper by in situ electropolymerization of porous polyaniline nanomaterials on graphene paper, followed by wrapping an ultrathin graphene layer on its surface. This unique design strategy not only circumvents the low energy storage capacity resulting from the double-layer capacitor of graphene paper, but also enhances the rate performance and cycling stability of porous polyaniline. The as-obtained all-solid-state symmetric supercapacitor exhibits high energy density, high power density, excellent cycling stability and exceptional mechanical flexibility, demonstrative of its extensive potential applications for flexible energy-related devices and wearable electronics.

Scalable Synthesis of Freestanding Sandwich-structured Graphene/Polyaniline/Graphene Nanocomposite Paper for Flexible All-Solid-State Supercapacitor

PubMed Central

Xiao, Fei; Yang, Shengxiong; Zhang, Zheye; Liu, Hongfang; Xiao, Junwu; Wan, Lian; Luo, Jun; Wang, Shuai; Liu, Yunqi

2015-01-01

We reported a scalable and modular method to prepare a new type of sandwich-structured graphene-based nanohybrid paper and explore its practical application as high-performance electrode in flexible supercapacitor. The freestanding and flexible graphene paper was firstly fabricated by highly reproducible printing technique and bubbling delamination method, by which the area and thickness of the graphene paper can be freely adjusted in a wide range. The as-prepared graphene paper possesses a collection of unique properties of highly electrical conductivity (340 S cm−1), light weight (1 mg cm−2) and excellent mechanical properties. In order to improve its supercapacitive properties, we have prepared a unique sandwich-structured graphene/polyaniline/graphene paper by in situ electropolymerization of porous polyaniline nanomaterials on graphene paper, followed by wrapping an ultrathin graphene layer on its surface. This unique design strategy not only circumvents the low energy storage capacity resulting from the double-layer capacitor of graphene paper, but also enhances the rate performance and cycling stability of porous polyaniline. The as-obtained all-solid-state symmetric supercapacitor exhibits high energy density, high power density, excellent cycling stability and exceptional mechanical flexibility, demonstrative of its extensive potential applications for flexible energy-related devices and wearable electronics. PMID:25797022

Scalable synthesis of freestanding sandwich-structured graphene/polyaniline/graphene nanocomposite paper for flexible all-solid-state supercapacitor.

PubMed

Xiao, Fei; Yang, Shengxiong; Zhang, Zheye; Liu, Hongfang; Xiao, Junwu; Wan, Lian; Luo, Jun; Wang, Shuai; Liu, Yunqi

2015-03-23

We reported a scalable and modular method to prepare a new type of sandwich-structured graphene-based nanohybrid paper and explore its practical application as high-performance electrode in flexible supercapacitor. The freestanding and flexible graphene paper was firstly fabricated by highly reproducible printing technique and bubbling delamination method, by which the area and thickness of the graphene paper can be freely adjusted in a wide range. The as-prepared graphene paper possesses a collection of unique properties of highly electrical conductivity (340 S cm(-1)), light weight (1 mg cm(-2)) and excellent mechanical properties. In order to improve its supercapacitive properties, we have prepared a unique sandwich-structured graphene/polyaniline/graphene paper by in situ electropolymerization of porous polyaniline nanomaterials on graphene paper, followed by wrapping an ultrathin graphene layer on its surface. This unique design strategy not only circumvents the low energy storage capacity resulting from the double-layer capacitor of graphene paper, but also enhances the rate performance and cycling stability of porous polyaniline. The as-obtained all-solid-state symmetric supercapacitor exhibits high energy density, high power density, excellent cycling stability and exceptional mechanical flexibility, demonstrative of its extensive potential applications for flexible energy-related devices and wearable electronics.

Tunable Electrical and Optical Characteristics in Monolayer Graphene and Few-Layer MoS2 Heterostructure Devices.

PubMed

Rathi, Servin; Lee, Inyeal; Lim, Dongsuk; Wang, Jianwei; Ochiai, Yuichi; Aoki, Nobuyuki; Watanabe, Kenji; Taniguchi, Takashi; Lee, Gwan-Hyoung; Yu, Young-Jun; Kim, Philip; Kim, Gil-Ho

2015-08-12

Lateral and vertical two-dimensional heterostructure devices, in particular graphene-MoS2, have attracted profound interest as they offer additional functionalities over normal two-dimensional devices. Here, we have carried out electrical and optical characterization of graphene-MoS2 heterostructure. The few-layer MoS2 devices with metal electrode at one end and monolayer graphene electrode at the other end show nonlinearity in drain current with drain voltage sweep due to asymmetrical Schottky barrier height at the contacts and can be modulated with an external gate field. The doping effect of MoS2 on graphene was observed as double Dirac points in the transfer characteristics of the graphene field-effect transistor (FET) with a few-layer MoS2 overlapping the middle part of the channel, whereas the underlapping of graphene have negligible effect on MoS2 FET characteristics, which showed typical n-type behavior. The heterostructure also exhibits a strongest optical response for 520 nm wavelength, which decreases with higher wavelengths. Another distinct feature observed in the heterostructure is the peak in the photocurrent around zero gate voltage. This peak is distinguished from conventional MoS2 FETs, which show a continuous increase in photocurrent with back-gate voltage. These results offer significant insight and further enhance the understanding of the graphene-MoS2 heterostructure.

Model of large volumetric capacitance in graphene supercapacitors based on ion clustering

NASA Astrophysics Data System (ADS)

Skinner, Brian; Fogler, M. M.; Shklovskii, B. I.

2011-12-01

Electric double-layer supercapacitors (SCs) are promising devices for high-power energy storage based on the reversible absorption of ions into porous conducting electrodes. Graphene is a particularly good candidate for the electrode material in SCs due to its high conductivity and large surface area. In this paper, we consider SC electrodes made from a stack of graphene sheets with randomly inserted spacer molecules. We show that the large volumetric capacitances C≳100F/cm3 observed experimentally can be understood as a result of collective intercalation of ions into the graphene stack and the accompanying nonlinear screening by graphene electrons that renormalizes the charge of the ion clusters.

A model of large volumetric capacitance in graphene supercapacitors based on ion clustering

NASA Astrophysics Data System (ADS)

Skinner, Brian; Fogler, Michael; Shklovskii, Boris

2012-02-01

Electric double layer supercapacitors are promising devices for high-power energy storage based on the reversible absorption of ions into porous, conducting electrodes. Graphene is a particularly good candidate for the electrode material in supercapacitors due to its high conductivity and large surface area. In this paper we consider supercapacitor electrodes made from a stack of graphene sheets with randomly-inserted ``spacer" molecules. We show that the large volumetric capacitances C > 100 F/cm^3 observed experimentally can be understood as a result of collective intercalation of ions into the graphene stack and the accompanying nonlinear screening by graphene electrons that renormalizes the charge of the ion clusters.

Synthesis of Fluorinated Graphene/CoAl-Layered Double Hydroxide Composites as Electrode Materials for Supercapacitors.

PubMed

Peng, Weijun; Li, Hongqiang; Song, Shaoxian

2017-02-15

CoAl-layered double hydroxide/fluorinated graphene (CoAl-LDH/FGN) composites were fabricated via a two-step hydrothermal method. The synthesized CoAl-LDH/FGN composites have been characterized by powder X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), field-emission scanning electron microscopy (FESEM), energy dispersive X-ray spectroscopy (EDS), and electrochemical measurements. The results indicated that the fluorinated carbon with various configuration forms were grafted onto the framework of graphene, and the C-F bond configuration and fluorine content could be tuned by the fluorination time. Most of semi-ionic C-F bonds were formed at an appropriate fluorination time and, then, converted into fluorine rich surface groups (such as CF 2 , CF 3 , etc.) which were electrochemically inactive as the fluorination time prolonged. Moreover, the CoAl-LDH/FGN composites prepared at the optimal fluorination time exhibited the highest specific capacitance (1222 F/g at 1 A/g), the best rate capability, and the most stable capacitance retention, which offered great promise as electrode materials for supercapacitors.

Self-propagated combustion synthesis of few-layered graphene: an optical properties perspective.

PubMed

Mohandoss, Manonmani; Sen Gupta, Soujit; Kumar, Ramesh; Islam, Md Rabiul; Som, Anirban; Mohd, Azhardin Ganayee; Pradeep, T; Maliyekkal, Shihabudheen M

2018-04-26

This paper describes a labour efficient and cost-effective strategy to prepare few-layered of reduced graphene oxide like (RGOL) sheets from graphite. The self-propagated combustion route enables the bulk production of RGOL sheets. Microscopic and spectroscopic analyses confirmed the formation of few-layer graphene sheets of an average thickness of ∼3 nm and the presence of some oxygen functional groups with a C/O ratio of 8.74. A possible mechanistic pathway for the formation of RGOL sheets is proposed. The optical properties of the RGOL sample were studied in detail by means of Spectroscopic Ellipsometry (SE). The experimental abilities of SE in relating the optical properties with the number of oxygen functionalities present in the samples are explored. The data were analysed by a double-layered optical model along with the Drude-Lorentz oscillatory dispersion relation. The refractive index (n = 2.24), extinction coefficient (k = 2.03), and dielectric functions are obtained using point-by-point analysis and are also checked for Kramers-Kronig (KK) consistency.

Colorimetry Technique for Scalable Characterization of Suspended Graphene.

PubMed

Cartamil-Bueno, Santiago J; Steeneken, Peter G; Centeno, Alba; Zurutuza, Amaia; van der Zant, Herre S J; Houri, Samer

2016-11-09

Previous statistical studies on the mechanical properties of chemical-vapor-deposited (CVD) suspended graphene membranes have been performed by means of measuring individual devices or with techniques that affect the material. Here, we present a colorimetry technique as a parallel, noninvasive, and affordable way of characterizing suspended graphene devices. We exploit Newton's rings interference patterns to study the deformation of a double-layer graphene drum 13.2 μm in diameter when a pressure step is applied. By studying the time evolution of the deformation, we find that filling the drum cavity with air is 2-5 times slower than when it is purged.

Surfactant-treated graphene covered polyaniline nanowires for supercapacitor electrode

NASA Astrophysics Data System (ADS)

Rajagopalan, Balasubramaniyan; Hur, Seung Hyun; Chung, Jin Suk

2015-04-01

Surfactant-treated graphene/polyaniline (G/PANI) nanocomposites were prepared by the MnO2 template-aided oxidative polymerization of aniline (ANI) on the surfactant-treated graphene sheets. The electrochemical performances of the G/PANI nanocomposites in a three-electrode system using an aqueous sulfuric acid as an electrolyte exhibited a specific capacitance of 436 F g-1 at 1 A g-1, which is much higher than the specific capacitance of pure PANI (367 F g-1). Such a higher specific capacitance of the G/PANI nanocomposite inferred an excellent synergistic effect of respective pseudocapacitance and electrical double-layer capacitance of PANI and graphene.

Study of storage capacity in various carbon/graphene-based solid-state supercapacitors

NASA Astrophysics Data System (ADS)

Subramaniam, C. K.; Boopalan, G.

2014-09-01

Solid-state electrochemical double-layer capacitor (SEDLC) forms excellent energy storage device for high-power applications. They are highly reliable, with no electrolyte leaks, and can be packaged to suit various applications. The electrode material can be activated carbon to graphene. These can have a range of particle size, surface area, pore size and pore distribution for charge storage. The emphasis will be to optimize the graphene to carbon blend in the electrodes which would provide appreciable storage density of the SEDLC. We can use perfluorosulfonic acid polymer as the solid electrolyte in the SEDLC assembly. They have high ionic conductivity, good thermal stability, and mechanical strength. They also have excellent long-term chemical stability. Carbon is widely used for many practical applications, especially for the adsorption of ions and molecules, as it is possible to synthesize one-, two- or three-dimensional (1-, 2-, or 3-D) carbons. Some of the problems in activated carbon like varying micro or mesopores, poor ion mobility due to varying pore distribution, low electrical conductivity, can be overcome using graphene and blends of graphene with carbon of the right pore dimension and distribution. Graphene in various structural nomenclatures have been used by various groups for charge storage. Graphene nanoplates (GNP), with narrow mesopore distributions have been effectively used for SEDLCs. SEDLCs assembled with GNP and blends of GNP with Vulcan XC and solid polymer electrolyte like Nafion show exceptional performance. The cyclic voltammetric studies show that they support high scan rates with substantial smaller capacitance drop as we increase scan rates. Optimization of the electrode structure in terms of blend percentage, binder content and interface character in the frequency and time domain provides excellent insight into the double-layer interface.

3D graphene nanomaterials for binder-free supercapacitors: scientific design for enhanced performance.

PubMed

He, Shuijian; Chen, Wei

2015-04-28

Because of the excellent intrinsic properties, especially the strong mechanical strength, extraordinarily high surface area and extremely high conductivity, graphene is deemed as a versatile building block for fabricating functional materials for energy production and storage applications. In this article, the recent progress in the assembly of binder-free and self-standing graphene-based materials, as well as their application in supercapacitors are reviewed, including electrical double layer capacitors, pseudocapacitors, and asymmetric supercapacitors. Various fabrication strategies and the influence of structures on the capacitance performance of 3D graphene-based materials are discussed. We finally give concluding remarks and an outlook on the scientific design of binder-free and self-standing graphene materials for achieving better capacitance performance.

3D graphene nanomaterials for binder-free supercapacitors: scientific design for enhanced performance

NASA Astrophysics Data System (ADS)

He, Shuijian; Chen, Wei

2015-04-01

Because of the excellent intrinsic properties, especially the strong mechanical strength, extraordinarily high surface area and extremely high conductivity, graphene is deemed as a versatile building block for fabricating functional materials for energy production and storage applications. In this article, the recent progress in the assembly of binder-free and self-standing graphene-based materials, as well as their application in supercapacitors are reviewed, including electrical double layer capacitors, pseudocapacitors, and asymmetric supercapacitors. Various fabrication strategies and the influence of structures on the capacitance performance of 3D graphene-based materials are discussed. We finally give concluding remarks and an outlook on the scientific design of binder-free and self-standing graphene materials for achieving better capacitance performance.

N-doped structures and surface functional groups of reduced graphene oxide and their effect on the electrochemical performance of supercapacitor with organic electrolyte

NASA Astrophysics Data System (ADS)

Li, Shin-Ming; Yang, Shin-Yi; Wang, Yu-Sheng; Tsai, Hsiu-Ping; Tien, Hsi-Wen; Hsiao, Sheng-Tsung; Liao, Wei-Hao; Chang, Chien-Liang; Ma, Chen-Chi M.; Hu, Chi-Chang

2015-03-01

Nitrogen-doped reduced graphene oxide (N-rGO) has been synthesized using a simple, efficient method combining instant thermal exfoliation and covalent bond transformation from a melamine-graphene oxide mixture. The capacitive performance of N-rGO has been tested in both aqueous (0.5 M H2SO4) and organic (1 M tetraethyl-ammonium tetrafluoroborate (TEABF4) in propylene carbonate (PC)) electrolytes, which are compared with those obtained from thermal-reduced graphene oxide (T-rGO) and chemical-reduced graphene oxide (C-rGO). The contributions of scan-rate-independent (double-layer-like) and scan-rate-dependent (pseudo-capacitance-like) capacitance of all reduced graphene oxides in both aqueous and organic electrolytes were evaluated and compared. The results show that relatively rich oxygen-containing functional groups on C-rGO form significant ion-diffusion barrier, resulting in worse electrochemical responses in organic electrolyte. By contrast, the N-doped structures, large surface area, and lower density of oxygen-containing groups make N-rGO become a promising electrode material for organic electric double-layer capacitors (EDLCs). The capacitance rate-retention of N-rGO reaches 71.1% in 1 M TEABF4/PC electrolyte when the scan rate is elevated to 200 mVs-1, demonstrating that N-rGO improves the relatively low-power drawback of EDLCs in organic electrolytes. The specific energy and power of a symmetric N-rGO cell in the organic electrolyte reach 25 Wh kg-1 and 10 kW kg-1, respectively.

Molecular Simulations of Graphene-Based Electric Double-Layer Capacitors

NASA Astrophysics Data System (ADS)

Kalluri, Raja K.; Konatham, Deepthi; Striolo, Alberto

2011-03-01

Towards deploying renewable energy sources it is crucial to develop efficient and cost-effective technologies to store electricity. Traditional batteries are plagued by a number of practical problems that at present limit their widespread applicability. One possible solution is represented by electric double-layer capacitors (EDLCs). To deploy EDLCs at the large scale it is necessary to better understand how electrolytes pack and diffuse within narrow charged pores. We present here simulation results for the concentrated aqueous solutions of NaCl, CsCl, and NaI confined within charged graphene-based porous materials. We discuss how the structure of confined water, the salt concentration, the ions size, and the surface charge density determine the accumulation of electrolytes within the porous network. Our results, compared to data available for bulk systems, are critical for relating macroscopic observations to molecular-level properties of the confined working fluids. Research supported by the Department of Energy.

Nanostructured pseudocapacitive materials decorated 3D graphene foam electrodes for next generation supercapacitors.

PubMed

Patil, Umakant; Lee, Su Chan; Kulkarni, Sachin; Sohn, Ji Soo; Nam, Min Sik; Han, Suhyun; Jun, Seong Chan

2015-04-28

Nowadays, advancement in performance of proficient multifarious electrode materials lies conclusively at the core of research concerning energy storage devices. To accomplish superior capacitance performance the requirements of high capacity, better cyclic stability and good rate capability can be expected from integration of electrochemical double layer capacitor based carbonaceous materials (high power density) and pseudocapacitive based metal hydroxides/oxides or conducting polymers (high energy density). The envisioned three dimensional (3D) graphene foams are predominantly advantageous to extend potential applicability by offering a large active surface area and a highly conductive continuous porous network for fast charge transfer with decoration of nanosized pseudocapacitive materials. In this article, we review the latest methodologies and performance evaluation for several 3D graphene based metal oxides/hydroxides and conducting polymer electrodes with improved electrochemical properties for next-generation supercapacitors. The most recent research advancements of our and other groups in the field of 3D graphene based electrode materials for supercapacitors are discussed. To assess the studied materials fully, a careful interpretation and rigorous scrutiny of their electrochemical characteristics is essential. Auspiciously, both nano-structuration as well as confinement of metal hydroxides/oxides and conducting polymers onto a conducting porous 3D graphene matrix play a great role in improving the performance of electrodes mainly due to: (i) active material access over large surface area with fast charge transportation; (ii) synergetic effect of electric double layer and pseudocapacitive based charge storing.

Nanoarchitectured graphene-based supercapacitors for next-generation energy-storage applications.

PubMed

Salunkhe, Rahul R; Lee, Ying-Hui; Chang, Kuo-Hsin; Li, Jing-Mei; Simon, Patrice; Tang, Jing; Torad, Nagy L; Hu, Chi-Chang; Yamauchi, Yusuke

2014-10-20

Tremendous development in the field of portable electronics and hybrid electric vehicles has led to urgent and increasing demand in the field of high-energy storage devices. In recent years, many research efforts have been made for the development of more efficient energy-storage devices such as supercapacitors, batteries, and fuel cells. In particular, supercapacitors have great potential to meet the demands of both high energy density and power density in many advanced technologies. For the last half decade, graphene has attracted intense research interest for electrical double-layer capacitor (EDLC) applications. The unique electronic, thermal, mechanical, and chemical characteristics of graphene, along with the intrinsic benefits of a carbon material, make it a promising candidate for supercapacitor applications. This Review focuses on recent research developments in graphene-based supercapacitors, including doped graphene, activated graphene, graphene/metal oxide composites, graphene/polymer composites, and graphene-based asymmetric supercapacitors. The challenges and prospects of graphene-based supercapacitors are also discussed. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Few layer graphene wrapped mixed phase TiO2 nanofiber as a potential electrode material for high performance supercapacitor applications

NASA Astrophysics Data System (ADS)

Thirugnanam, Lavanya; Sundara, Ramaprabhu

2018-06-01

A combination of favorable composition and optimized anatase/rutile mixed-phase TiO2 (MPTNF)/Hydrogen exfoliated graphene (HEG) composite nanofibers (MPTNF/HEG) and anatase/rutile mixed-phase TiO2/reduced graphene oxide (rGO) composite nanofibers (MPTNF/rGO) have been reported to enhance the electrochemical properties for supercapacitor applications. These composite nanofibers have been synthesized by an efficient route of electrospinning together with the help of easy chemical methods. Both the composites exhibit good charge storage capability with enhanced pseudocapacitance and electric double-layer capacitance (EDLC) as confirmed by cyclic voltammetry studies. MPTNF/HEG composite showed maximum specific capacitance of 210.5 F/g at the current density of 1 A/g, which was mainly due to its availability of the more active sites for ions adsorption on a few layers of graphene wrapped TiO2 nanofiber surface. The synergistic effect of anatase/rutile mixed phase with one dimensional nanostructure and the electronic interaction between TiO2 and few layer graphene provided the subsequent improvement of ion adsorption capacity. Also exhibit excellent electrochemical performance to improve the capacitive properties of TiO2 electrode materials which is required for the development of flexible electrodes in energy storage devices and open up new opportunities for high performance supercapacitors.

Analytical solution for static and dynamic analysis of magnetically affected viscoelastic orthotropic double-layered graphene sheets resting on viscoelastic foundation

NASA Astrophysics Data System (ADS)

Jalaei, M. H.; Arani, A. Ghorbanpour

2018-02-01

By considering the small scale effect based on the nonlocal Eringen's theory, the static and dynamic analysis of viscoelastic orthotropic double-layered graphene sheets subjected to longitudinal magnetic field and mechanical load is investigated analytically. For this objective, first order shear deformation theory (FSDT) is proposed. The surrounding medium is simulated by visco-Pasternak foundation model in which damping, normal and transverse shear loads are taken into account. The governing equations of motion are obtained via energy method and Hamilton's principle which are then solved analytically by means of Navier's approach and Laplace inversion technique in the space and time domains, respectively. Through various parametric studies, the influences of the nonlocal parameter, structural damping, van der Waals (vdW) interaction, stiffness and damping coefficient of the foundation, magnetic parameter, aspect ratio and length to thickness ratio on the static and dynamic response of the nanoplates are examined. The results depict that when the vdW interaction is considered to be zero, the upper layer deflection reaches a maximum point whereas the lower layer deflection becomes zero. In addition, it is observed that with growing the vdW interaction, the effect of magnetic field on the deflection of the lower layer increases while this effect reduces for the upper layer deflection.

A manufacturable process integration approach for graphene devices

NASA Astrophysics Data System (ADS)

Vaziri, Sam; Lupina, Grzegorz; Paussa, Alan; Smith, Anderson D.; Henkel, Christoph; Lippert, Gunther; Dabrowski, Jarek; Mehr, Wolfgang; Östling, Mikael; Lemme, Max C.

2013-06-01

In this work, we propose an integration approach for double gate graphene field effect transistors. The approach includes a number of process steps that are key for future integration of graphene in microelectronics: bottom gates with ultra-thin (2 nm) high-quality thermally grown SiO2 dielectrics, shallow trench isolation between devices and atomic layer deposited Al2O3 top gate dielectrics. The complete process flow is demonstrated with fully functional GFET transistors and can be extended to wafer scale processing. We assess, through simulation, the effects of the quantum capacitance and band bending in the silicon substrate on the effective electric fields in the top and bottom gate oxide. The proposed process technology is suitable for other graphene-based devices such as graphene-based hot electron transistors and photodetectors.

An Ideal Electrode Material, 3D Surface-Microporous Graphene for Supercapacitors with Ultrahigh Areal Capacitance

DOE PAGES

Chang, Liang; Stacchiola, Dario J.; Hu, Yun Hang

2017-07-03

The efficient charge accumulation of an ideal supercapacitor electrode requires abundant micropores and its fast electrolyte-ions transport prefers meso/macropores. But, current electrode materials cannot meet both requirements, resulting in poor performance. We creatively constructed three-dimensional cabbage-coral-like graphene as an ideal electrode material, in which meso/macro channels are formed by graphene walls and rich micropores are incorporated in the surface layer of the graphene walls. The unique 3D graphene material can achieve a high gravimetric capacitance of 200 F/g with aqueous electrolyte, 3 times larger than that of commercially used activated carbon (70.8 F/g). Furthermore, it can reach an ultrahigh arealmore » capacitance of 1.28 F/cm 2 and excellent rate capability (83.5% from 0.5 to 10 A/g) as well as high cycling stability (86.2% retention after 5000 cycles). The excellent electric double-layer performance of the 3D graphene electrode can be attributed to the fast electrolyte ion transport in the meso/macro channels and the rapid and reversible charge adsorption with negligible transport distance in the surface micropores.« less

An Ideal Electrode Material, 3D Surface-Microporous Graphene for Supercapacitors with Ultrahigh Areal Capacitance

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chang, Liang; Stacchiola, Dario J.; Hu, Yun Hang

The efficient charge accumulation of an ideal supercapacitor electrode requires abundant micropores and its fast electrolyte-ions transport prefers meso/macropores. But, current electrode materials cannot meet both requirements, resulting in poor performance. We creatively constructed three-dimensional cabbage-coral-like graphene as an ideal electrode material, in which meso/macro channels are formed by graphene walls and rich micropores are incorporated in the surface layer of the graphene walls. The unique 3D graphene material can achieve a high gravimetric capacitance of 200 F/g with aqueous electrolyte, 3 times larger than that of commercially used activated carbon (70.8 F/g). Furthermore, it can reach an ultrahigh arealmore » capacitance of 1.28 F/cm 2 and excellent rate capability (83.5% from 0.5 to 10 A/g) as well as high cycling stability (86.2% retention after 5000 cycles). The excellent electric double-layer performance of the 3D graphene electrode can be attributed to the fast electrolyte ion transport in the meso/macro channels and the rapid and reversible charge adsorption with negligible transport distance in the surface micropores.« less

An acetylcholinesterase biosensor based on graphene-gold nanocomposite and calcined layered double hydroxide.

PubMed

Zhai, Chen; Guo, Yemin; Sun, Xia; Zheng, Yuhe; Wang, Xiangyou

2014-05-10

In this study, a novel acetylcholinesterase-based biosensor was fabricated. Acetylcholinesterase (AChE) was immobilized onto a glassy carbon electrode (GCE) with the aid of Cu-Mg-Al calcined layered double hydroxide (CLDH). CLDH can provide a bigger effective surface area for AChE loading, which could improve the precision and stability of AChE biosensor. However, the poor electroconductibility of CLDHs could lead to the low sensitivity of AChE biosensor. In order to effectively compensate the disadvantages of CLDHs, graphene-gold nanocomposites were used for improving the electron transfer rate. Thus, the graphene-gold nanocomposite (GN-AuNPs) was firstly modified onto the GCE, and then the prepared CLDH-AChE composite was immobilized onto the modified GCE to construct a sensitive AChE biosensor for pesticides detection. Relevant parameters were studied in detail and optimized, including the pH of the acetylthiocholine chloride (ATCl) solution, the amount of AChE immobilized on the biosensor and the inhibition time governing the analytical performance of the biosensor. The biosensor detected chlorpyrifos at concentrations ranging from 0.05 to 150μg/L. The detection limit for chlorpyrifos was 0.05μg/L. Copyright © 2014 Elsevier Inc. All rights reserved.

Thermal treatment effects on charge storage performance of graphene-based materials for supercapacitors.

PubMed

Zhang, Hongxin; Bhat, Vinay V; Gallego, Nidia C; Contescu, Cristian I

2012-06-27

Graphene materials were synthesized by reduction of exfoliated graphite oxide and then thermally treated in nitrogen to improve the surface area and their electrochemical performance as electrical double-layer capacitor electrodes. The structural and surface properties of the prepared reduced graphite oxide (RGO) were investigated using atomic force microscopy, scanning electron microscopy, Raman spectra, X-ray diffraction pattern analysis, and nitrogen adsorption/desorption studies. RGO forms a continuous network of crumpled sheets, which consist of large amounts of few-layer and single-layer graphenes. Electrochemical studies were conducted by cyclic voltammetry, impedance spectroscopy, and galvanostatic charge-discharge measurements. The modified RGO materials showed enhanced electrochemical performance, with maximum specific capacitance of 96 F/g, energy density of 12.8 Wh/kg, and power density of 160 kW/kg. These results demonstrate that thermal treatment of RGO at selected conditions is a convenient and efficient method for improving its specific capacitance, energy, and power density.

Graphene oxide-MnO2 nanocomposite for supercapacitor application

NASA Astrophysics Data System (ADS)

Muhammed Shafi, P.; Vishal, Jose K.; Chandra Bose, A.

2016-09-01

Increased depletion of fossil fuels along with global warming and climate change made the society to think about alternate green and sustainable energy sources and better energy storage devices. Extensive research has been performed on the development of solar cells, fuel cells, Lithium- ion battery and supercapacitors to combat the green house effect and its consequences, and to meet the increased energy crisis. Supercapacitors, also known as electrochemical capacitors are gained a great attention because of their pulse power supply, long cycle life (>100,000), simple principle and high dynamic of charge propagation. Its greater power density than lithium- ion battery and much larger energy density than conventional capacitors brought super capacitors to a promising energy storage device to meet the increased energy demands. Here we demonstrate supercapacitor electrode materials with graphene oxide (electric double layer capacitor) and α-MnO2 nanomaterial (pseudo-capacitor), as well as composite of these materials, which means that the bulk of the material undergoes a fast redox reaction to provide the capacitive response and they exhibit superior specific energies in addition to the carbon-based supercapacitors (double-layer capacitors). A simple soft chemical route is utilized to synthesize graphene oxide, α-MnO2 and graphene oxide-MnO2 composite. The phase and the structure of the synthesized materials are studied using X-ray diffractometry (XRD). The functional group and the presence of impurities are understood from Fourier transform infrared (FTIR) spectra. The capacitive properties of the graphene oxide, graphene oxide - MnO2 nanocomposite and α-MnO2 are tested with the help of cyclic voltammetry (CV) and galvanostatic charge - discharge techniques using 1 M Na2SO4 in aqueous solution as electrolyte. It was found that graphene oxide - MnO2 nanocomposite shows better electrochemical behaviour compared to individual graphene oxide and α-MnO2 nanomaterial.

Synthesis and Characterization of 2-D Materials

NASA Astrophysics Data System (ADS)

Pazos, S.; Sahoo, P.; Afaneh, T.; Rodriguez Gutierrez, H.

Atomically thin transition-metal dichacogenides (TMD), graphene, and boron nitride (BN) are two-dimensional materials where the charge carriers (electrons and holes) are confined to move in a plane. They exhibit distinctive optoelectronic properties compared to their bulk layered counterparts. When combined into heterostructures, these materials open more possibilities in terms of new properties and device functionality. In this work, WSe2 and graphene were grown using Chemical Vapor Deposition (CVD) and Physical Vapor Deposition (PVD) techniques. The quality and morphology of each material was checked using Raman, Photoluminescence Spectroscopy, and Scanning Electron Microscopy. Graphene had been successfully grown homogenously, characterized, and transferred from copper to silicon dioxide substrates; these films will be used in future studies to build 2-D devices. Different morphologies of WSe2 2-D islands were successfully grown on SiO2 substrates. Depending on the synthesis conditions, the material on each sample had single layer, double layer, and multi-layer areas. A variety of 2-D morphologies were also observed in the 2-D islands. This project is supported by the NSF REU Grant #1560090 and NSF Grant #DMR-1557434.

The Origin of Improved Electrical Double-Layer Capacitance by Inclusion of Topological Defects and Dopants in Graphene for Supercapacitors.

PubMed

Chen, Jiafeng; Han, Yulei; Kong, Xianghua; Deng, Xinzhou; Park, Hyo Ju; Guo, Yali; Jin, Song; Qi, Zhikai; Lee, Zonghoon; Qiao, Zhenhua; Ruoff, Rodney S; Ji, Hengxing

2016-10-24

Low-energy density has long been the major limitation to the application of supercapacitors. Introducing topological defects and dopants in carbon-based electrodes in a supercapacitor improves the performance by maximizing the gravimetric capacitance per mass of the electrode. However, the main mechanisms governing this capacitance improvement are still unclear. We fabricated planar electrodes from CVD-derived single-layer graphene with deliberately introduced topological defects and nitrogen dopants in controlled concentrations and of known configurations, to estimate the influence of these defects on the electrical double-layer (EDL) capacitance. Our experimental study and theoretical calculations show that the increase in EDL capacitance due to either the topological defects or the nitrogen dopants has the same origin, yet these two factors improve the EDL capacitance in different ways. Our work provides a better understanding of the correlation between the atomic-scale structure and the EDL capacitance and presents a new strategy for the development of experimental and theoretical models for understanding the EDL capacitance of carbon electrodes. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

An overview of the applications of graphene-based materials in supercapacitors.

PubMed

Huang, Yi; Liang, Jiajie; Chen, Yongsheng

2012-06-25

Due to their unique 2D structure and outstanding intrinsic physical properties, such as extraordinarily high electrical conductivity and large surface area, graphene-based materials exhibit great potential for application in supercapacitors. In this review, the progress made so far for their applications in supercapacitors is reviewed, including electrochemical double-layer capacitors, pseudo-capacitors, and asymmetric supercapacitors. Compared with traditional electrode materials, graphene-based materials show some novel characteristics and mechanisms in the process of energy storage and release. Several key issues for improving the structure of graphene-based materials and for achieving better capacitor performance, along with the current outlook for the field, are also discussed. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Synthesis of graphene nanoribbons from amyloid templates by gallium vapor-assisted solid-phase graphitization

DOE Office of Scientific and Technical Information (OSTI.GOV)

Murakami, Katsuhisa, E-mail: k.murakami@bk.tsukuba.ac.jp; Dong, Tianchen; Kajiwara, Yuya

2014-06-16

Single- and double-layer graphene nanoribbons (GNRs) with widths of around 10 nm were synthesized directly onto an insulating substrate by solid-phase graphitization using a gallium vapor catalyst and carbon templates made of amyloid fibrils. Subsequent investigation revealed that the crystallinity, conductivity, and carrier mobility were all improved by increasing the temperature of synthesis. The carrier mobility of the GNR synthesized at 1050 °C was 0.83 cm{sup 2}/V s, which is lower than that of mechanically exfoliated graphene. This is considered to be most likely due to electron scattering by the defects and edges of the GNRs.

Tunneling magnetoresistance tuned by a vertical electric field in an AA-stacked graphene bilayer with double magnetic barriers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Dali, E-mail: wangdali@mail.ahnu.edu.cn; National Laboratory of Solid State Microstructures and Department of Physics, Nanjing University, Nanjing 210093; Jin, Guojun, E-mail: gjin@nju.edu.cn

2013-12-21

We investigate the effect of a vertical electric field on the electron tunneling and magnetoresistance in an AA-stacked graphene bilayer modulated by the double magnetic barriers with parallel or antiparallel configuration. The results show that the electronic transmission properties in the system are sensitive to the magnetic-barrier configuration and the bias voltage between the graphene layers. In particular, it is found that for the antiparallel configuration, within the low energy region, the blocking effect is more obvious compared with the case for the parallel configuration, and even there may exist a transmission spectrum gap which can be arbitrarily tuned bymore » the field-induced interlayer bias voltage. We also demonstrate that the significant discrepancy between the conductance for both parallel and antiparallel configurations would result in a giant tunneling magnetoresistance ratio, and further the maximal magnetoresistance ratio can be strongly modified by the interlayer bias voltage. This leads to the possible realization of high-quality magnetic sensors controlled by a vertical electric field in the AA-stacked graphene bilayer.« less

Bilayer insulator tunnel barriers for graphene-based vertical hot-electron transistors

NASA Astrophysics Data System (ADS)

Vaziri, S.; Belete, M.; Dentoni Litta, E.; Smith, A. D.; Lupina, G.; Lemme, M. C.; Östling, M.

2015-07-01

Vertical graphene-based device concepts that rely on quantum mechanical tunneling are intensely being discussed in the literature for applications in electronics and optoelectronics. In this work, the carrier transport mechanisms in semiconductor-insulator-graphene (SIG) capacitors are investigated with respect to their suitability as electron emitters in vertical graphene base transistors (GBTs). Several dielectric materials as tunnel barriers are compared, including dielectric double layers. Using bilayer dielectrics, we experimentally demonstrate significant improvements in the electron injection current by promoting Fowler-Nordheim tunneling (FNT) and step tunneling (ST) while suppressing defect mediated carrier transport. High injected tunneling current densities approaching 103 A cm-2 (limited by series resistance), and excellent current-voltage nonlinearity and asymmetry are achieved using a 1 nm thick high quality dielectric, thulium silicate (TmSiO), as the first insulator layer, and titanium dioxide (TiO2) as a high electron affinity second layer insulator. We also confirm the feasibility and effectiveness of our approach in a full GBT structure which shows dramatic improvement in the collector on-state current density with respect to the previously reported GBTs. The device design and the fabrication scheme have been selected with future CMOS process compatibility in mind. This work proposes a bilayer tunnel barrier approach as a promising candidate to be used in high performance vertical graphene-based tunneling devices.

Boosting Photon Harvesting in Organic Solar Cells with Highly Oriented Molecular Crystals via Graphene-Organic Heterointerface.

PubMed

Jo, Sae Byeok; Kim, Hyun Ho; Lee, Hansol; Kang, Boseok; Lee, Seongkyu; Sim, Myungsun; Kim, Min; Lee, Wi Hyoung; Cho, Kilwon

2015-08-25

Photon harvesting in organic solar cells is highly dependent on the anisotropic nature of the optoelectronic properties of photoactive materials. Here, we demonstrate an efficient approach to dramatically enhance photon harvesting in planar heterojunction solar cells by using a graphene-organic heterointerface. A large area, residue-free monolayer graphene is inserted at anode interface to serve as an atomically thin epitaxial template for growing highly orientated pentacene crystals with lying-down orientation. This anisotropic orientation enhances the overall optoelectronic properties, including light absorption, charge carrier lifetime, interfacial energetics, and especially the exciton diffusion length. Spectroscopic and crystallographic analysis reveal that the lying-down orientation persists until a thickness of 110 nm, which, along with increased exciton diffusion length up to nearly 100 nm, allows the device optimum thickness to be doubled to yield significantly enhanced light absorption within the photoactive layers. The resultant photovoltaic performance shows simultaneous increment in Voc, Jsc, and FF, and consequently a 5 times increment in the maximum power conversion efficiency than the equivalent devices without a graphene layer. The present findings indicate that controlling organic-graphene heterointerface could provide a design strategy of organic solar cell architecture for boosting photon harvesting.

Active pore space utilization in nanoporous carbon-based supercapacitors: Effects of conductivity and pore accessibility

NASA Astrophysics Data System (ADS)

Seredych, Mykola; Koscinski, Mikolaj; Sliwinska-Bartkowiak, Malgorzata; Bandosz, Teresa J.

2012-12-01

Composites of commercial graphene and nanoporous sodium-salt-polymer-derived carbons were prepared with 5 or 20 weight% graphene. The materials were characterized using the adsorption of nitrogen, SEM/EDX, thermal analysis, Raman spectroscopy and potentiometric titration. The samples' conductivity was also measured. The performance of the carbon composites in energy storage was linked to their porosity and electronic conductivity. The small pores (<0.7) were found as very active for double layer capacitance. It was demonstrated that when double layer capacitance is a predominant mechanism of charge storage, the degree of the pore space utilization for that storage can be increased by increasing the conductivity of the carbons. That active pore space utilization is defined as gravimetric capacitance per unit pore volume in pores smaller than 0.7 nm. Its magnitude is affected by conductivity of the carbon materials. The functional groups, besides pseudocapacitive contribution, increased the wettability and thus the degree of the pore space utilization. Graphene phase, owing to its conductivity, also took part in an insitu increase of the small pore accessibility and thus the capacitance of the composites via enhancing an electron transfer to small pores and thus imposing the reduction of groups blocking the pores for electrolyte ions.

Sandwich-like graphene/polypyrrole/layered double hydroxide nanowires for high-performance supercapacitors

NASA Astrophysics Data System (ADS)

Li, Xuejin; Zhang, Yu; Xing, Wei; Li, Li; Xue, Qingzhong; Yan, Zifeng

2016-11-01

Electrode design in nanoscale is considered to be ultra-important to construct a superb capacitor. Herein, a sandwich-like composite was made by combining graphene/polypyrrole (GPPY) with nickel-aluminum layered double hydroxide nanowires (NiAl-NWs) via a facile hydrothermal method. This sandwich-like architecture is promising in energy storage applications due to three unique features: (1) the conductive GPPY substrate not only effectively prevents the layered double hydroxides species from aggregating, but also considerably facilitates the electron transmission; (2) the ultrathin NiAl-NWs ensure a maximum exposure of active Ni2+, which can improve the efficiency of rapid redox reactions even at high current densities; (3) the sufficient space between anisotropic NiAl-NWs can accommodate a large volume change of the nanowires to avoid their collapse or distortion during the reduplicative redox reactions. Keeping all these unique features in mind, when the as-prepared composite was applied to supercapacitors, it presented an enhanced capacitive performance in terms of high specific capacitance (845 F g-1), excellent rate performance (67% retained at 30 A g-1), remarkable cyclic stability (92% maintained after 5000 cycles) and large energy density (40.1 Wh·Kg-1). This accomplishment in the present work inspires an innovative strategy of nanoscale electrode design for high-rate performance supercapacitor electrodes containing pseuducapacitive metal oxide.

Mogul-Patterned Elastomeric Substrate for Stretchable Electronics.

PubMed

Lee, Han-Byeol; Bae, Chan-Wool; Duy, Le Thai; Sohn, Il-Yung; Kim, Do-Il; Song, You-Joon; Kim, Youn-Jea; Lee, Nae-Eung

2016-04-01

A mogul-patterned stretchable substrate with multidirectional stretchability and minimal fracture of layers under high stretching is fabricated by double photolithography and soft lithography. Au layers and a reduced graphene oxide chemiresistor on a mogul-patterned poly(dimethylsiloxane) substrate are stable and durable under various stretching conditions. The newly designed mogul-patterned stretchable substrate shows great promise for stretchable electronics. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Facile synthesis of NiAl-layered double hydroxide/graphene hybrid with enhanced electrochemical properties for detection of dopamine

NASA Astrophysics Data System (ADS)

Li, Meixia; Zhu, Jun E.; Zhang, Lili; Chen, Xu; Zhang, Huimin; Zhang, Fazhi; Xu, Sailong; Evans, David G.

2011-10-01

Layered double hydroxides (LDHs), also known as hydrotalcite-like anionic clays, have been investigated widely as promising electrochemical active materials. Due to the inherently weak conductivity, the electrochemical properties of LDHs were improved typically by utilization of either functional molecules intercalated between LDH interlayer galleries, or proteins confined between exfoliated LDH nanosheets. Here, we report a facile protocol to prepare NiAl-LDH/graphene (NiAl-LDH/G) nanocomposites using a conventional coprecipitation process under low-temperature conditions and subsequent reduction of the supporting graphene oxide. Electrochemical tests showed that the NiAl-LDH/G modified electrode exhibited highly enhanced electrochemical performance of dopamine electrooxidation in comparison with the pristine NiAl-LDH modified electrode. Results of high-resolution transmission electron microscopy and Raman spectra provide convincing information on the nanostructure and composition underlying the enhancement. Our results of the NiAl-LDH/G modified electrodes with the enhanced electrochemical performance may allow designing a variety of promising hybrid sensors via a simple and feasible approach.Layered double hydroxides (LDHs), also known as hydrotalcite-like anionic clays, have been investigated widely as promising electrochemical active materials. Due to the inherently weak conductivity, the electrochemical properties of LDHs were improved typically by utilization of either functional molecules intercalated between LDH interlayer galleries, or proteins confined between exfoliated LDH nanosheets. Here, we report a facile protocol to prepare NiAl-LDH/graphene (NiAl-LDH/G) nanocomposites using a conventional coprecipitation process under low-temperature conditions and subsequent reduction of the supporting graphene oxide. Electrochemical tests showed that the NiAl-LDH/G modified electrode exhibited highly enhanced electrochemical performance of dopamine electrooxidation in comparison with the pristine NiAl-LDH modified electrode. Results of high-resolution transmission electron microscopy and Raman spectra provide convincing information on the nanostructure and composition underlying the enhancement. Our results of the NiAl-LDH/G modified electrodes with the enhanced electrochemical performance may allow designing a variety of promising hybrid sensors via a simple and feasible approach. Electronic supplementary information (ESI) available: Fig. S1 showing 2D fast Fourier transform (FFT) image of NiAl-LDH phase in NiAl-LDH/G composites, and Fig. S2 showing CV curve of the pristine G modified electrode. See DOI: 10.1039/c1nr10592b.

Graphene device and method of using graphene device

DOEpatents

Bouchiat, Vincent; Girit, Caglar; Kessler, Brian; Zettl, Alexander K.

2015-08-11

An embodiment of a graphene device includes a layered structure, first and second electrodes, and a dopant island. The layered structure includes a conductive layer, an insulating layer, and a graphene layer. The electrodes are coupled to the graphene layer. The dopant island is coupled to an exposed surface of the graphene layer between the electrodes. An embodiment of a method of using a graphene device includes providing the graphene device. A voltage is applied to the conductive layer of the graphene device. Another embodiment of a method of using a graphene device includes providing the graphene device without the dopant island. A dopant island is placed on an exposed surface of the graphene layer between the electrodes. A voltage is applied to the conductive layer of the graphene device. A response of the dopant island to the voltage is observed.

Phonon Self-Energy Corrections to Nonzero Wave-Vector Phonon Modes in Single-Layer Graphene

NASA Astrophysics Data System (ADS)

Araujo, P. T.; Mafra, D. L.; Sato, K.; Saito, R.; Kong, J.; Dresselhaus, M. S.

2012-07-01

Phonon self-energy corrections have mostly been studied theoretically and experimentally for phonon modes with zone-center (q=0) wave vectors. Here, gate-modulated Raman scattering is used to study phonons of a single layer of graphene originating from a double-resonant Raman process with q≠0. The observed phonon renormalization effects are different from what is observed for the zone-center q=0 case. To explain our experimental findings, we explored the phonon self-energy for the phonons with nonzero wave vectors (q≠0) in single-layer graphene in which the frequencies and decay widths are expected to behave oppositely to the behavior observed in the corresponding zone-center q=0 processes. Within this framework, we resolve the identification of the phonon modes contributing to the G⋆ Raman feature at 2450cm-1 to include the iTO+LA combination modes with q≠0 and also the 2iTO overtone modes with q=0, showing both to be associated with wave vectors near the high symmetry point K in the Brillouin zone.

van der Waals Heterostructures with High Accuracy Rotational Alignment.

PubMed

Kim, Kyounghwan; Yankowitz, Matthew; Fallahazad, Babak; Kang, Sangwoo; Movva, Hema C P; Huang, Shengqiang; Larentis, Stefano; Corbet, Chris M; Taniguchi, Takashi; Watanabe, Kenji; Banerjee, Sanjay K; LeRoy, Brian J; Tutuc, Emanuel

2016-03-09

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.

Structure of Room Temperature Ionic Liquids on Charged Graphene: An integrated experimental and computational study

NASA Astrophysics Data System (ADS)

Uysal, Ahmet; Zhou, Hua; Lee, Sang Soo; Fenter, Paul; Feng, Guang; Li, Song; Cummings, Peter; Fulvio, Pasquale; Dai, Sheng; McDonough, Jake; Gogotsi, Yury

2014-03-01

Electrical double layer capacitors (EDLCs) with room temperature ionic liquid (RTIL) electrolytes and carbon electrodes are promising candidates for energy storage devices with high power density and long cycle life. We studied the potential and time dependent changes in the electric double layer (EDL) structure of an imidazolium-based room temperature ionic liquid (RTIL) electrolyte at an epitaxial graphene (EG) surface. We used in situ x-ray reflectivity (XR) to determine the EDL structure at static potentials, during cyclic voltammetry (CV) and potential step measurements. The static potential structures were also investigated with fully atomistic molecular dynamics (MD) simulations. Combined XR and MD results show that the EDL structure has alternating anion/cation layers within the first nanometer of the interface. The dynamical response of the EDL to potential steps has a slow component (>10 s) and the RTIL structure shows hysteresis during CV scans. We propose a conceptual model that connects nanoscale interfacial structure to the macroscopic measurements. This material is based upon work supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy (DOE), Office of Science (SC), Office of Basic Energy

Nanoporous graphene obtained by hydrothermal process in H2O2 and its application for supercapacitors

NASA Astrophysics Data System (ADS)

Lv, Jinlong; Liang, Tongxiang

2016-08-01

Nanohole graphene oxide (NHGO) was obtained in a homogeneous aqueous mixture of graphene oxide (GO) and H2O2 at 120 °C. Supercapacitors were fabricated as the electrode material by using NHGO. A specific capacitance of 240.1 F g-1 was obtained at a current density of 1 A g-1 in 6 m KOH electrolyte and specific capacitance remained 193.6 F g-1 at the current density of 20 A g-1. This was attributed to reducing the inner space between the double-layers, enhanced ion diffusion and large specific surface area. Supercapacitor prepared with NHGO electrodes also exhibited an excellent cycle stability.

Strongly Enhanced Tunneling at Total Charge Neutrality in Double-Bilayer Graphene-WSe_{2} Heterostructures.

PubMed

Burg, G William; Prasad, Nitin; Kim, Kyounghwan; Taniguchi, Takashi; Watanabe, Kenji; MacDonald, Allan H; Register, Leonard F; Tutuc, Emanuel

2018-04-27

We report the experimental observation of strongly enhanced tunneling between graphene bilayers through a WSe_{2} barrier when the graphene bilayers are populated with carriers of opposite polarity and equal density. The enhanced tunneling increases sharply in strength with decreasing temperature, and the tunneling current exhibits a vertical onset as a function of interlayer voltage at a temperature of 1.5 K. The strongly enhanced tunneling at overall neutrality departs markedly from single-particle model calculations that otherwise match the measured tunneling current-voltage characteristics well, and suggests the emergence of a many-body state with condensed interbilayer excitons when electrons and holes of equal densities populate the two layers.

Strongly Enhanced Tunneling at Total Charge Neutrality in Double-Bilayer Graphene-WSe2 Heterostructures

NASA Astrophysics Data System (ADS)

Burg, G. William; Prasad, Nitin; Kim, Kyounghwan; Taniguchi, Takashi; Watanabe, Kenji; MacDonald, Allan H.; Register, Leonard F.; Tutuc, Emanuel

2018-04-01

We report the experimental observation of strongly enhanced tunneling between graphene bilayers through a WSe2 barrier when the graphene bilayers are populated with carriers of opposite polarity and equal density. The enhanced tunneling increases sharply in strength with decreasing temperature, and the tunneling current exhibits a vertical onset as a function of interlayer voltage at a temperature of 1.5 K. The strongly enhanced tunneling at overall neutrality departs markedly from single-particle model calculations that otherwise match the measured tunneling current-voltage characteristics well, and suggests the emergence of a many-body state with condensed interbilayer excitons when electrons and holes of equal densities populate the two layers.

Functionalization of graphene by size and doping control and its optoelectronic applications

NASA Astrophysics Data System (ADS)

Tang, Libin; Ji, Rongbin; Tian, Pin; Kong, Jincheng; Xiang, Jinzhong

2017-02-01

Graphene has received intensive attention in recent years because of the special physical and chemical properties. However, up to now graphene has not been widely used in optoelectronic fields yet, which is mainly caused by its semimetal properties. Therefore, changing its properties from semimetal to semiconductor is becoming a focal point. Recently, aiming at tuning the energy band of graphene, we have carried out systematic studies on the preparations of graphene based materials and devices, the CVD growth techniques of monolayer and double layer graphenes have been developed, the large-area doped graphene films have been fabricated to tune the structure-related optical and electrical properties. A novel graphene oxide (GO) preparation method namely "Tang-Lau method" has been invented, the graphene quantum dots growths by microwave assisted hydrothermal method and "Soft-Template method" have been developed, the Cl, S and K doped graphene quantum dots preparations by hydrothermal methods have also been invented. Systematic investigations have been carried out for the effect of preparation parameters on the properties of graphene based materials, the effects of size, doping elements on the energy level of graphene based materials have been explored and discussed. Based on the semiconducting graphene based materials, some novel room temperature photodetectors covering detection wavebands from UV, Vis and NIR have been designed and fabricated.

Early patterns of commercial activity in graphene

NASA Astrophysics Data System (ADS)

Shapira, Philip; Youtie, Jan; Arora, Sanjay

2012-03-01

Graphene, a novel nanomaterial consisting of a single layer of carbon atoms, has attracted significant attention due to its distinctive properties, including great strength, electrical and thermal conductivity, lightness, and potential benefits for diverse applications. The commercialization of scientific discoveries such as graphene is inherently uncertain, with the lag time between the scientific development of a new technology and its adoption by corporate actors revealing the extent to which firms are able to absorb knowledge and engage in learning to implement applications based on the new technology. From this perspective, we test for the existence of three different corporate learning and activity patterns: (1) a linear process where patenting follows scientific discovery; (2) a double-boom phenomenon where corporate (patenting) activity is first concentrated in technological improvements and then followed by a period of technology productization; and (3) a concurrent model where scientific discovery in publications occurs in parallel with patenting. By analyzing corporate publication and patent activity across country and application lines, we find that, while graphene as a whole is experiencing concurrent scientific development and patenting growth, country- and application-specific trends offer some evidence of the linear and double-boom models.

A thin film approach for SiC-derived graphene as an on-chip electrode for supercapacitors

NASA Astrophysics Data System (ADS)

Ahmed, Mohsin; Khawaja, Mohamad; Notarianni, Marco; Wang, Bei; Goding, Dayle; Gupta, Bharati; Boeckl, John J.; Takshi, Arash; Motta, Nunzio; Saddow, Stephen E.; Iacopi, Francesca

2015-10-01

We designed a nickel-assisted process to obtain graphene with sheet resistance as low as 80 Ω square-1 from silicon carbide films on Si wafers with highly enhanced surface area. The silicon carbide film acts as both a template and source of graphitic carbon, while, simultaneously, the nickel induces porosity on the surface of the film by forming silicides during the annealing process which are subsequently removed. As stand-alone electrodes in supercapacitors, these transfer-free graphene-on-chip samples show a typical double-layer supercapacitive behaviour with gravimetric capacitance of up to 65 F g-1. This work is the first attempt to produce graphene with high surface area from silicon carbide thin films for energy storage at the wafer-level and may open numerous opportunities for on-chip integrated energy storage applications.

A thin film approach for SiC-derived graphene as an on-chip electrode for supercapacitors.

PubMed

Ahmed, Mohsin; Khawaja, Mohamad; Notarianni, Marco; Wang, Bei; Goding, Dayle; Gupta, Bharati; Boeckl, John J; Takshi, Arash; Motta, Nunzio; Saddow, Stephen E; Iacopi, Francesca

2015-10-30

We designed a nickel-assisted process to obtain graphene with sheet resistance as low as 80 Ω square(-1) from silicon carbide films on Si wafers with highly enhanced surface area. The silicon carbide film acts as both a template and source of graphitic carbon, while, simultaneously, the nickel induces porosity on the surface of the film by forming silicides during the annealing process which are subsequently removed. As stand-alone electrodes in supercapacitors, these transfer-free graphene-on-chip samples show a typical double-layer supercapacitive behaviour with gravimetric capacitance of up to 65 F g(-1). This work is the first attempt to produce graphene with high surface area from silicon carbide thin films for energy storage at the wafer-level and may open numerous opportunities for on-chip integrated energy storage applications.

Theoretical investigation of structural and optical properties of semi-fluorinated bilayer graphene

NASA Astrophysics Data System (ADS)

Xiao-Jiao, San; Bai, Han; Jing-Geng, Zhao

2016-03-01

We have studied the structural and optical properties of semi-fluorinated bilayer graphene using density functional theory. When the interlayer distance is 1.62 Å, the two graphene layers in AA stacking can form strong chemical bonds. Under an in-plane stress of 6.8 GPa, this semi-fluorinated bilayer graphene becomes the energy minimum. Our calculations indicate that the semi-fluorinated bilayer graphene with the AA stacking sequence and rectangular fluorinated configuration is a nonmagnetic semiconductor (direct gap of 3.46 eV). The electronic behavior at the vicinity of the Fermi level is mainly contributed by the p electrons of carbon atoms forming C=C double bonds. We compare the optical properties of the semi-fluorinated bilayer graphene with those of bilayer graphene stacked in the AA sequence and find that the semi-fluorinated bilayer graphene is anisotropic for the polarization vector on the basal plane of graphene and a red shift occurs in the [010] polarization, which makes the peak at the low-frequency region located within visible light. This investigation is useful to design polarization-dependence optoelectronic devices. Project supported by the Program of Educational Commission of Heilongjiang Province, China (Grant No. 12541131).

All-solid-state supercapacitors on silicon using graphene from silicon carbide

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Bei; Ahmed, Mohsin; Iacopi, Francesca, E-mail: f.iacopi@griffith.edu.au

2016-05-02

Carbon-based supercapacitors are lightweight devices with high energy storage performance, allowing for faster charge-discharge rates than batteries. Here, we present an example of all-solid-state supercapacitors on silicon for on-chip applications, paving the way towards energy supply systems embedded in miniaturized electronics with fast access and high safety of operation. We present a nickel-assisted graphitization method from epitaxial silicon carbide on a silicon substrate to demonstrate graphene as a binder-free electrode material for all-solid-state supercapacitors. We obtain graphene electrodes with a strongly enhanced surface area, assisted by the irregular intrusion of nickel into the carbide layer, delivering a typical double-layer capacitancemore » behavior with a specific area capacitance of up to 174 μF cm{sup −2} with about 88% capacitance retention over 10 000 cycles. The fabrication technique illustrated in this work provides a strategic approach to fabricate micro-scale energy storage devices compatible with silicon electronics and offering ultimate miniaturization capabilities.« less

In situ self-sacrificed template synthesis of vanadium nitride/nitrogen-doped graphene nanocomposites for electrochemical capacitors.

PubMed

Liu, Hong-Hui; Zhang, Hong-Ling; Xu, Hong-Bin; Lou, Tai-Ping; Sui, Zhi-Tong; Zhang, Yi

2018-03-15

Vanadium nitride and graphene have been widely used as pseudo-capacitive and electric double-layer capacitor electrode materials for electrochemical capacitors, respectively. However, the poor cycling stability of vanadium nitride and the low capacitance of graphene impeded their practical applications. Herein, we demonstrated an in situ self-sacrificed template method for the synthesis of vanadium nitride/nitrogen-doped graphene (VN/NGr) nanocomposites by the pyrolysis of a mixture of dicyandiamide, glucose, and NH 4 VO 3 . Vanadium nitride nanoparticles of the size in the range of 2 to 7 nm were uniformly embedded into the nitrogen-doped graphene skeleton. Furthermore, the VN/NGr nanocomposites with a high specific surface area and pore volume showed a high specific capacitance of 255 F g -1 at 10 mV s -1 , and an excellent cycling stability (94% capacitance retention after 2000 cycles). The excellent capacitive properties were ascribed to the excellent conductivity of nitrogen-doped graphene, high surface area, high pore volume, and the synergistic effect between vanadium nitride and nitrogen-doped graphene.

Graphene-oxide-supported CuAl and CoAl layered double hydroxides as enhanced catalysts for carbon-carbon coupling via Ullmann reaction

NASA Astrophysics Data System (ADS)

Ahmed, Nesreen S.; Menzel, Robert; Wang, Yifan; Garcia-Gallastegui, Ainara; Bawaked, Salem M.; Obaid, Abdullah Y.; Basahel, Sulaiman N.; Mokhtar, Mohamed

2017-02-01

Two efficient catalyst based on CuAl and CoAl layered double hydroxides (LDHs) supported on graphene oxide (GO) for the carbon-carbon coupling (Classic Ullmann Homocoupling Reaction) are reported. The pure and hybrid materials were synthesised by direct precipitation of the LDH nanoparticles onto GO, followed by a chemical, structural and physical characterisation by electron microscopy, X-ray diffraction (XRD), thermogravimetric analysis (TGA), surface area measurements and X-ray photoelectron spectroscopy (XPS). The GO-supported and unsupported CuAl-LDH and CoAl-LDH hybrids were tested over the Classic Ullman Homocoupling Reaction of iodobenzene. In the current study CuAl- and CoAl-LDHs have shown excellent yields (91% and 98%, respectively) at very short reaction times (25 min). GO provides a light-weight, charge complementary and two-dimensional material that interacts effectively with the 2D LDHs, in turn enhancing the stability of LDH. After 5 re-use cycles, the catalytic activity of the LDH/GO hybrid is up to 2 times higher than for the unsupported LDH.

Facile synthesis of three dimensional hierarchical Co-Al layered double hydroxides on graphene as high-performance materials for supercapacitor electrode.

PubMed

Hao, Jinhui; Yang, Wenshu; Zhang, Zhe; Lu, Baoping; Ke, Xi; Zhang, Bailin; Tang, Jilin

2014-07-15

A facile simple hydrothermal method combined with a post-solution reaction is developed to grow interconnected three dimensional (3D) hierarchical Co-Al layered double hydroxides (LDHs) on reduced graphene oxide (rGO). The obtained 3D hierarchical rGO-LDHs are characterized by field emission scanning electron microscopy, X-ray diffraction, and X-ray photo-electron spectroscopy. As LDHs nanosheets directly grow on the surface of rGO via chemical covalent bonding, the rGO could provide facile electron transport paths in the electrode for the fast Faradaic reaction. Moreover, benefiting from the rational 3D hierarchical structural, the rGO-LDHs demonstrate excellent electrochemical properties with a combination of high charge storage capacitance, fast rate capability and stable cycling performance. Remarkably, the 3D hierarchical rGO-LDHs exhibit specific capacitance values of 599 F g(-1) at a constant current density of 4 A g(-1). The rGO-LDHs also show high charge-discharge reversibility with an efficiency of 92.4% after 5000 cycles. Copyright © 2014 Elsevier Inc. All rights reserved.

High-surface-area nitrogen-doped reduced graphene oxide for electric double-layer capacitors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Youn, Hee-Chang; Bak, Seong-Min; Kim, Myeong-Seong

A two-step method consisting of solid-state microwave irradiation and heat treatment under NH₃ gas was used to prepare nitrogen-doped reduced graphene oxide (N-RGO) with a high specific surface area (1007m²g⁻¹), high electrical conductivity (1532S m⁻¹), and low oxygen content (1.5 wt%) for electric double-layer capacitor applications. The specific capacitance of N-RGO was 291 Fg⁻¹ at a current density of 1 A g⁻¹, and a capacitance of 261 F g⁻¹ was retained at 50 A g⁻¹, indicating a very good rate capability. N-RGO also showed excellent cycling stability, preserving 96% of the initial specific capacitance after 100,000 cycles. Near-edge X-ray absorptionmore » fine-structure spectroscopy evidenced the recover of π-conjugation in the carbon networks with the removal of oxygenated groups and revealed the chemical bonding of the nitrogen atoms in N-RGO. The good electrochemical performance of N-RGO is attributed to its high surface area, high electrical conductivity, and low oxygen content.« less

High-surface-area nitrogen-doped reduced graphene oxide for electric double-layer capacitors

DOE PAGES

Youn, Hee-Chang; Bak, Seong-Min; Kim, Myeong-Seong; ...

2015-06-08

A two-step method consisting of solid-state microwave irradiation and heat treatment under NH₃ gas was used to prepare nitrogen-doped reduced graphene oxide (N-RGO) with a high specific surface area (1007m²g⁻¹), high electrical conductivity (1532S m⁻¹), and low oxygen content (1.5 wt%) for electric double-layer capacitor applications. The specific capacitance of N-RGO was 291 Fg⁻¹ at a current density of 1 A g⁻¹, and a capacitance of 261 F g⁻¹ was retained at 50 A g⁻¹, indicating a very good rate capability. N-RGO also showed excellent cycling stability, preserving 96% of the initial specific capacitance after 100,000 cycles. Near-edge X-ray absorptionmore » fine-structure spectroscopy evidenced the recover of π-conjugation in the carbon networks with the removal of oxygenated groups and revealed the chemical bonding of the nitrogen atoms in N-RGO. The good electrochemical performance of N-RGO is attributed to its high surface area, high electrical conductivity, and low oxygen content.« less

Electronic and Optical Properties of Twisted Bilayer Graphene

NASA Astrophysics Data System (ADS)

Huang, Shengqiang

The ability to isolate single atomic layers of van der Waals materials has led to renewed interest in the electronic and optical properties of these materials as they can be fundamentally different at the monolayer limit. Moreover, these 2D crystals can be assembled together layer by layer, with controllable sequence and orientation, to form artificial materials that exhibit new features that are not found in monolayers nor bulk. Twisted bilayer graphene is one such prototype system formed by two monolayer graphene layers placed on top of each other with a twist angle between their lattices, whose electronic band structure depends on the twist angle. This thesis presents the efforts to explore the electronic and optical properties of twisted bilayer graphene by Raman spectroscopy and scanning tunneling microscopy measurements. We first synthesize twisted bilayer graphene with various twist angles via chemical vapor deposition. Using a combination of scanning tunneling microscopy and Raman spectroscopy, the twist angles are determined. The strength of the Raman G peak is sensitive to the electronic band structure of twisted bilayer graphene and therefore we use this peak to monitor changes upon doping. Our results demonstrate the ability to modify the electronic and optical properties of twisted bilayer graphene with doping. We also fabricate twisted bilayer graphene by controllable stacking of two graphene monolayers with a dry transfer technique. For twist angles smaller than one degree, many body interactions play an important role. It requires eight electrons per moire unit cell to fill up each band instead of four electrons in the case of a larger twist angle. For twist angles smaller than 0.4 degree, a network of domain walls separating AB and BA stacking regions forms, which are predicted to host topologically protected helical states. Using scanning tunneling microscopy and spectroscopy, these states are confirmed to appear on the domain walls when inversion symmetry is broken with an external electric field. We observe a double-line profile of these states on the domain walls, only occurring when the AB and BA regions are gaped. These states give rise to channels that could transport charge in a dissipationless manner making twisted bilayer graphene a promising platform to realize controllable topological networks for future applications.

Multilayered nano-architecture of variable sized graphene nanosheets for enhanced supercapacitor electrode performance.

PubMed

Biswas, Sanjib; Drzal, Lawrence T

2010-08-01

The diverse physical and chemical aspects of graphene nanosheets such as particle size surface area and edge chemistry were combined to fabricate a new supercapacitor electrode architecture consisting of a highly aligned network of large-sized nanosheets as a series of current collectors within a multilayer configuration of bulk electrode. Capillary driven self-assembly of monolayers of graphene nanosheets was employed to create a flexible, multilayer, free-standing film of highly hydrophobic nanosheets over large macroscopic areas. This nanoarchitecture exhibits a high-frequency capacitative response and a nearly rectangular cyclic voltammogram at 1000 mV/s scanning rate and possesses a rapid current response, small equivalent series resistance (ESR), and fast ionic diffusion for high-power electrical double-layer capacitor (EDLC) application.

Carbon Capsules of Ionic Liquid for Enhanced Performance of Electrochemical Double-Layer Capacitors.

PubMed

Luo, Qinmo; Wei, Peiran; Huang, Qianwen; Gurkan, Burcu; Pentzer, Emily B

2018-05-16

Ion accessibility, large surface area, and complete wetting of a carbonaceous electrode by the electrolyte are crucial for high-performance electrochemical double-layer capacitors. Herein, we report a facile and scalable method to prepare electrode-electrolyte hybrid materials, where an ionic liquid (IL) electrolyte is encapsulated within a shell of reduced graphene oxide (rGO) nanosheets as the active electrode material (called rGO-IL capsules). These structures were templated using a Pickering emulsion consisting of a dispersed phase of 1-methyl-3-butylimidazolium hexafluorophosphate ([bmim][PF 6 ]) and a continuous water phase; graphene oxide nanosheets were used as the surfactant, and interfacial polymerization yielded polyurea that bound the nanosheets together to form the capsule shell. This method prevents the aggregation and restacking of GO nanosheets and allows wetting of the materials by IL. The chemical composition, thermal properties, morphology, and electrochemical behavior of these new hybrid architectures are fully characterized. Specific capacitances of 80 F g -1 at 18 °C and 127 F g -1 at 60 °C were achieved at a scan rate of 10 mV s -1 for symmetric coin cells of rGO-IL capsules. These architected materials have higher capacitance at low temperature (18 °C) across many scan rates (10-500 mV s -1 ) compared with analogous cells with the porous carbon YP-50. These results demonstrate a distinct and important methodology to enhance the performance of electrochemical double-layer capacitors by incorporating electrolyte and carbon material together during synthesis.

Eco-friendly synthesis of size-controllable amine-functionalized graphene quantum dots with antimycoplasma properties

NASA Astrophysics Data System (ADS)

Jiang, Feng; Chen, Daiqin; Li, Ruimin; Wang, Yucheng; Zhang, Guoqiang; Li, Shumu; Zheng, Junpeng; Huang, Naiyan; Gu, Ying; Wang, Chunru; Shu, Chunying

2013-01-01

Size-controllable amine-functionalized graphene quantum dots (GQDs) are prepared by an eco-friendly method with graphene oxide sheets, ammonia and hydrogen peroxide as starting materials. Using a Sephadex G-25 gel column for fine separation, for the first time we obtain GQDs with either single or double layers. By atomic force microscopy characterization, we confirm that hydrogen peroxide and ammonia play a synergistic role on graphene oxide (GO), in which the former cuts the GO into small pieces and the latter passivates the active surface to give amine-modified GQDs. Due to the low cytotoxicity and excellent biocompatibility of the obtained amine-functionalized GQDs, besides the multiwavelength imaging properties of GQDs, for the first time we find that this kind of GQD exhibits good antimycoplasma properties. Given the superior antimycoplasma effect of the GQDs and their eco-friendly mass production with low cost, these new GQDs may offer opportunities for the development of new antimycoplasma agents, thus extending their widespread application in biomedicine.Size-controllable amine-functionalized graphene quantum dots (GQDs) are prepared by an eco-friendly method with graphene oxide sheets, ammonia and hydrogen peroxide as starting materials. Using a Sephadex G-25 gel column for fine separation, for the first time we obtain GQDs with either single or double layers. By atomic force microscopy characterization, we confirm that hydrogen peroxide and ammonia play a synergistic role on graphene oxide (GO), in which the former cuts the GO into small pieces and the latter passivates the active surface to give amine-modified GQDs. Due to the low cytotoxicity and excellent biocompatibility of the obtained amine-functionalized GQDs, besides the multiwavelength imaging properties of GQDs, for the first time we find that this kind of GQD exhibits good antimycoplasma properties. Given the superior antimycoplasma effect of the GQDs and their eco-friendly mass production with low cost, these new GQDs may offer opportunities for the development of new antimycoplasma agents, thus extending their widespread application in biomedicine. Electronic supplementary information (ESI) available: Experimental details and additional characterization data. See DOI: 10.1039/c2nr33191h

Freestanding polyaniline nanorods grown on graphene for highly capacitive energy storage

NASA Astrophysics Data System (ADS)

Li, Zijiong; Qin, Zhen; Yang, Baocheng; Guo, Jian; Wang, Haiyan; Zhang, Weiyang; Lv, Xiaowei; Stack, Alison

2015-02-01

Freestanding polyaniline (PANI) nanorods grown in situ on microwave-expanded graphene oxide (MEGO) sheets were prepared through a facile solution method. The morphological characterization indicates that large quantity of free-standing PANI nanorods with average diameter of 50 nm were uniformly deposited onto the double sides of the MEGO nanosheets to form a sandwich structure. The hybrid of PANI/MEGO (GPANI) exhibit high specific surface area and high electrical conductivity, compared with pristine PANI nanorods. When evaluated as electrodes for supercapacitors, the GPANI demonstrate high specific capacitance of 628 F g-1 at a current density of 1.1 A g-1, high-rate performance, and excellent cycle stability compared to individual component. Such excellent electrochemical performance should be attributed to the combined double-layer capacitance and pseudo -capacitance mechanisms from the MEGO sheets and PANI nanorods.

Graphene can wreak havoc with cell membranes.

PubMed

Dallavalle, Marco; Calvaresi, Matteo; Bottoni, Andrea; Melle-Franco, Manuel; Zerbetto, Francesco

2015-02-25

Molecular dynamics--coarse grained to the level of hydrophobic and hydrophilic interactions--shows that small hydrophobic graphene sheets pierce through the phospholipid membrane and navigate the double layer, intermediate size sheets pierce the membrane only if a suitable geometric orientation is met, and larger sheets lie mainly flat on the top of the bilayer where they wreak havoc with the membrane and create a patch of upturned phospholipids. The effect arises in order to maximize the interaction between hydrophobic moieties and is quantitatively explained in terms of flip-flops by the analysis of the simulations. Possible severe biological consequences are discussed.

Processing and Characterization of Graphene/Polyimide-Nickel Oxide Hybrid Nanocomposites for Advanced Energy Storage in Supercapacitor Applications

NASA Astrophysics Data System (ADS)

Okafor, Patricia A.

This research is focused on enhancing electrochemical properties/energy storage capabilities of graphene-polyimide composites. The composite's dense morphology/structure limits ionic penetration owing to high bulk resistances resulting in poor electrochemical performance. Modification of the composite's morphology by incorporation of facile pores during curing increases total available surface area to electrolyte species. Presence of pores increases adsorption sites for double layer formation and increases overall capacitance. In this work, aromatic polyimide precursors were reacted in the presence of nano-graphene fillers to synthesize graphene-polyimide composite films. The resulting composite was very stiff and dense with a high glass transition temperature (Tg) of 400 °C and storage modulus of 7.20 GPa. Selective decomposition of a thermally labile poly(acrylic ester) resin introduced into the composite during synthesis creates pores of varying size and shapes which increases available surface area of embedded stacked graphene sheets available for ion adsorption and double layer formation. Proper control over pore size and specific surface area of pores was required to ensure good performance in terms of both power delivery rate and energy storage capacity. Dynamic mechanical studies on modified composite showed very good mechanical property while shifts in imide peaks to lower wave numbers in Raman and Fourier transform spectroscopy (FTIR) confirms presence of chemical interaction between graphene filler and polymer matrix confirming uniform dispersion of fillers in the material. Thermogravimetric analysis (TGA) shows thermal stability for the composite systems at temperatures above 700°C. To further optimize material's energy storage capabilities, a hybrid composite was formed by depositing relatively cheap nickel oxide onto the modified porous composite system by a two-step process. A remarkable improvement in electrochemical properties up to an order of magnitude was observed. Electrochemical performance of the hybrid system showed strong dependence on deposition current density, deposition time and substrate pore morphology. Increased NiO particle size (aggregates) was observed with increased deposition time and current density which had a significant impact on charge transfer resistance and specific capacitance. Several correlations were made between composite's morphology and obtained properties. The material's morphology showed direct correlation with double layer capacitance, charge capacity, bulk resistance and sheet conductivity measured using cyclic voltammetry (CV), cyclic charge discharge (CCD), electrochemical impedance spectroscopy (EIS) and four probe measurements respectively. It was observed that smaller well distributed pores showed enhanced properties compared to larger pores. Material's overall performance shows a linear dependence on porosity. The overall electrochemical and electrical behavior of the system is directly linked to the composite's morphology and structure as will be demonstrated in this thesis work.

Insights into the effects of solvent properties in graphene based electric double-layer capacitors with organic electrolytes

NASA Astrophysics Data System (ADS)

Zhang, Shuo; Bo, Zheng; Yang, Huachao; Yang, Jinyuan; Duan, Liangping; Yan, Jianhua; Cen, Kefa

2016-12-01

Organic electrolytes are widely used in electric double-layer capacitors (EDLCs). In this work, the microstructure of planar graphene-based EDLCs with different organic solvents are investigated with molecular dynamics simulations. Results show that an increase of solvent polarity could weaken the accumulation of counter-ions nearby the electrode surface, due to the screen of electrode charges and relatively lower ionic desolvation. It thus suggests that solvents with low polarity could be preferable to yield high EDL capacitance. Meanwhile, the significant effects of the size and structure of solvent molecules are reflected by non-electrostatic molecule-electrode interactions, further influencing the adsorption of solvent molecules on electrode surface. Compared with dimethyl carbonate, γ-butyrolactone, and propylene carbonate, acetonitrile with relatively small-size and linear structure owns weak non-electrostatic interactions, which favors the easy re-orientation of solvent molecules. Moreover, the shift of solvent orientation in surface layer, from parallel orientation to perpendicular orientation relative to the electrode surface, deciphers the solvent twin-peak behavior near negative electrode. The as-obtained insights into the roles of solvent properties on the interplays among particles and electrodes elucidate the solvent influences on the microstructure and capacitive behavior of EDLCs using organic electrolytes.

Water-gel for gating graphene transistors.

PubMed

Kim, Beom Joon; Um, Soong Ho; Song, Woo Chul; Kim, Yong Ho; Kang, Moon Sung; Cho, Jeong Ho

2014-05-14

Water, the primary electrolyte in biology, attracts significant interest as an electrolyte-type dielectric material for transistors compatible with biological systems. Unfortunately, the fluidic nature and low ionic conductivity of water prevents its practical usage in such applications. Here, we describe the development of a solid state, megahertz-operating, water-based gate dielectric system for operating graphene transistors. The new electrolyte systems were prepared by dissolving metal-substituted DNA polyelectrolytes into water. The addition of these biocompatible polyelectrolytes induced hydrogelation to provide solid-state integrity to the system. They also enhanced the ionic conductivities of the electrolytes, which in turn led to the quick formation of an electric double layer at the graphene/electrolyte interface that is beneficial for modulating currents in graphene transistors at high frequencies. At the optimized conditions, the Na-DNA water-gel-gated flexible transistors and inverters were operated at frequencies above 1 MHz and 100 kHz, respectively.

Electromechanically generating electricity with a gapped-graphene electric generator

NASA Astrophysics Data System (ADS)

Dressen, Donald; Golovchenko, Jene

2015-03-01

We demonstrate the fabrication and operation of a gapped-graphene electric generator (G-GEG) device. The G-GEG generates electricity from the mechanical oscillation of droplets of electrolytes and ionic liquids. The spontaneous adsorption of ionic species on graphene charges opposing electric double-layer capacitors (EDLCs) on each half of the device. Modulating the area of contact between the droplet and graphene leads to adsorption/desorption of ions, effectively charging/discharging each EDLC and generating a current. The flow of current supports a potential difference across the G-GEG due to the device's internal impedance. Both the magnitude and polarity of the induced current and voltage show a strong dependence on the type of ionic species used, suggesting that certain ions interact more strongly with graphene than others. We find that a simple model circuit consisting of an AC current source in series with a resistor and a time-varying capacitor accurately predicts the device's dynamic behavior. Additionally, we discuss the effect of graphene's intrinsic quantum capacitance on the G-GEG's performance and speculate on the utility of the device in the context of energy harvesting.

High-concentration boron doping of graphene nanoplatelets by simple thermal annealing and their supercapacitive properties.

PubMed

Yeom, Da-Young; Jeon, Woojin; Tu, Nguyen Dien Kha; Yeo, So Young; Lee, Sang-Soo; Sung, Bong June; Chang, Hyejung; Lim, Jung Ah; Kim, Heesuk

2015-05-05

For the utilization of graphene in various energy storage and conversion applications, it must be synthesized in bulk with reliable and controllable electrical properties. Although nitrogen-doped graphene shows a high doping efficiency, its electrical properties can be easily affected by oxygen and water impurities from the environment. We here report that boron-doped graphene nanoplatelets with desirable electrical properties can be prepared by the simultaneous reduction and boron-doping of graphene oxide (GO) at a high annealing temperature. B-doped graphene nanoplatelets prepared at 1000 °C show a maximum boron concentration of 6.04 ± 1.44 at %, which is the highest value among B-doped graphenes prepared using various methods. With well-mixed GO and g-B2O3 as the dopant, highly uniform doping is achieved for potentially gram-scale production. In addition, as a proof-of-concept, highly B-doped graphene nanoplatelets were used as an electrode of an electrochemical double-layer capacitor (EDLC) and showed an excellent specific capacitance value of 448 F/g in an aqueous electrolyte without additional conductive additives. We believe that B-doped graphene nanoplatelets can also be used in other applications such as electrocatalyst and nano-electronics because of their reliable and controllable electrical properties regardless of the outer environment.

High-concentration boron doping of graphene nanoplatelets by simple thermal annealing and their supercapacitive properties

NASA Astrophysics Data System (ADS)

Yeom, Da-Young; Jeon, Woojin; Tu, Nguyen Dien Kha; Yeo, So Young; Lee, Sang-Soo; Sung, Bong June; Chang, Hyejung; Lim, Jung Ah; Kim, Heesuk

2015-05-01

For the utilization of graphene in various energy storage and conversion applications, it must be synthesized in bulk with reliable and controllable electrical properties. Although nitrogen-doped graphene shows a high doping efficiency, its electrical properties can be easily affected by oxygen and water impurities from the environment. We here report that boron-doped graphene nanoplatelets with desirable electrical properties can be prepared by the simultaneous reduction and boron-doping of graphene oxide (GO) at a high annealing temperature. B-doped graphene nanoplatelets prepared at 1000 °C show a maximum boron concentration of 6.04 ± 1.44 at %, which is the highest value among B-doped graphenes prepared using various methods. With well-mixed GO and g-B2O3 as the dopant, highly uniform doping is achieved for potentially gram-scale production. In addition, as a proof-of-concept, highly B-doped graphene nanoplatelets were used as an electrode of an electrochemical double-layer capacitor (EDLC) and showed an excellent specific capacitance value of 448 F/g in an aqueous electrolyte without additional conductive additives. We believe that B-doped graphene nanoplatelets can also be used in other applications such as electrocatalyst and nano-electronics because of their reliable and controllable electrical properties regardless of the outer environment.

Electrochemical characteristics of amorphous carbon nanorod synthesized by radio frequency magnetron sputtering

NASA Astrophysics Data System (ADS)

Chang, Hsin-Yueh; Huang, Yung-Jui; Chang, Hsuan-Chen; Su, Wei-Jhih; Shih, Yi-Ting; Chen, John L.; Honda, Shin-ichi; Huang, Ying-Sheng; Lee, Kuei-Yi

2015-01-01

Amorphous carbon nanorods (CNRs) were deposited directly using radio frequency magnetron sputtering. The synthesized CNR electrochemical properties were investigated using graphene as the current collector for an electric double layer capacitor. The CNRs were vertically aligned to the graphene to achieve higher specific surface area. The capacitor performance was characterized using electrochemical impedance spectroscopy, cyclic voltammetry, and galvanostatic charge-discharge testing in 1 M KOH electrolyte at 30°C, 40°C, 50°C, and 60°C. The CNR specific capacitance was observed to increase with increasing measurement temperature and could reach up to 830 F/g at 60°C. Even after extensive measurements, the CNR electrode maintained good adhesion to the graphene current collector thereby suggesting electrode material stability.

Graphene based 2D-materials for supercapacitors

NASA Astrophysics Data System (ADS)

Palaniselvam, Thangavelu; Baek, Jong-Beom

2015-09-01

Ever-increasing energy demands and the depletion of fossil fuels are compelling humanity toward the development of suitable electrochemical energy conversion and storage devices to attain a more sustainable society with adequate renewable energy and zero environmental pollution. In this regard, supercapacitors are being contemplated as potential energy storage devices to afford cleaner, environmentally friendly energy. Recently, a great deal of attention has been paid to two-dimensional (2D) nanomaterials, including 2D graphene and its inorganic analogues (transition metal double layer hydroxides, chalcogenides, etc), as potential electrodes for the development of supercapacitors with high electrochemical performance. This review provides an overview of the recent progress in using these graphene-based 2D materials as potential electrodes for supercapacitors. In addition, future research trends including notable challenges and opportunities are also discussed.

Multilayer graphene as an effective corrosion protection coating for copper

NASA Astrophysics Data System (ADS)

Ravishankar, Vasumathy; Ramaprabhu, S.; Jaiswal, Manu

2018-04-01

Graphene grown by chemical vapor deposition (CVD) has been studied as a protective layer against corrosion of copper. The layer number dependence on the protective nature of graphene has been investigated using techniques such as Tafel analysis and Electroimpedance Spectroscopy. Multiple layers of graphene were achieved by wet transfer above CVD grown graphene. Though this might cause grain boundaries, the sites where corrosion is initiated, to be staggered, wet transfer inherently carries the disadvantage of tearing of graphene, as confirmed by Raman spectroscopy measurements. However, Electroimpedance Spectroscopy (EIS) reflects that graphene protected copper has a layer dependent resistance to corrosion. Decrease in corrosion current (Icorr) for graphene protected copper is presented. There is only small dependence of corrosion current on the layer number, Tafel plots clearly indicate passivation in the presence of graphene, whether it be single layer or multiple layers. Notwithstanding the crystallite size, defect free layers of graphene with staggered grain boundaries combined with passivation could offer good corrosion protection for metals.

High-performance metal mesh/graphene hybrid films using prime-location and metal-doped graphene.

PubMed

Min, Jung-Hong; Jeong, Woo-Lim; Kwak, Hoe-Min; Lee, Dong-Seon

2017-08-31

We introduce high-performance metal mesh/graphene hybrid transparent conductive layers (TCLs) using prime-location and metal-doped graphene in near-ultraviolet light-emitting diodes (NUV LEDs). Despite the transparency and sheet resistance values being similar for hybrid TCLs, there were huge differences in the NUV LEDs' electrical and optical properties depending on the location of the graphene layer. We achieved better physical stability and current spreading when the graphene layer was located beneath the metal mesh, in direct contact with the p-GaN layer. We further improved the contact properties by adding a very thin Au mesh between the thick Ag mesh and the graphene layer to produce a dual-layered metal mesh. The Au mesh effectively doped the graphene layer to create a p-type electrode. Using Raman spectra, work function variations, and the transfer length method (TLM), we verified the effect of doping the graphene layer after depositing a very thin metal layer on the graphene layers. From our results, we suggest that the nature of the contact is an important criterion for improving the electrical and optical performance of hybrid TCLs, and the method of doping graphene layers provides new opportunities for solving contact issues in other semiconductor devices.

Hybrid phosphorene/graphene nanocomposite as an anode material for Na-ion batteries: a first-principles study

NASA Astrophysics Data System (ADS)

Wang, Linxia; Jiang, Zhiqiang; Li, Wei; Gu, Xiao; Huang, Li

2017-04-01

The potential application of the hybrid phosphorene/graphene (P/G) composites as an anode material in Na-ion batteries (NIBs) has been explored based on first-principles calculations. The calculated elastic constants reveal that the P/G has an ultrahigh stiffness, which can effectively suppress the undesirable structural deformation during the sodiation and desodiation cycles. Na atoms can strongly bind with the phosphorene single-layer (SP), double-layer (DP), and their composites with graphene (SP/G, DP/G, G/DP/G), and can even cause a sliding between the layers when the DP/G accommodate more Na atoms. The migration of Na in P/G is anisotropic with the minimum energy path along the zigzag channel. The low diffusion barriers of only about several tens of meV ensure the high mobility of Na within the layers, and thus lead to rapid charge/discharge capacity of P/G. The electronic structures show that the hybrid P/G becomes metallic with the Na incorporation, which contributes to the good electric conductivity in P/G. We further demonstrate that the average open circuit voltage (OCV) of DP/G is 0.53 V, which is comparable to other anode materials. These results suggest that P/G composites hold great potential to be a good anode material in NIBs.

Vertically Oriented Graphene Electrochemical Double Layer Capacitor with Very Fast Dynamic Response

DTIC Science & Technology

2013-01-01

cauliflower type of morphology (see Figure A-2c). Figure A-3. (a) The intensity of D to G peak ratio in Raman spectra and the thickness (height) of...in a random, cauliflower type of morphology (see Figure A-2c). Figure A-2. (a) The intensity of D to G peak ratio in Raman spectra and the

High-Surface-Area Nitrogen-Doped Reduced Graphene Oxide for Electric Double-Layer Capacitors.

PubMed

Youn, Hee-Chang; Bak, Seong-Min; Kim, Myeong-Seong; Jaye, Cherno; Fischer, Daniel A; Lee, Chang-Wook; Yang, Xiao-Qing; Roh, Kwang Chul; Kim, Kwang-Bum

2015-06-08

A two-step method consisting of solid-state microwave irradiation and heat treatment under NH3 gas was used to prepare nitrogen-doped reduced graphene oxide (N-RGO) with a high specific surface area (1007 m(2)  g(-1) ), high electrical conductivity (1532 S m(-1) ), and low oxygen content (1.5 wt %) for electrical double-layer capacitor applications. The specific capacitance of N-RGO was 291 F g(-1) at a current density of 1 A g(-1) , and a capacitance of 261 F g(-1) was retained at 50 A g(-1) , which indicated a very good rate capability. N-RGO also showed excellent cycling stability and preserved 96 % of the initial specific capacitance after 100 000 cycles. Near-edge X-ray absorption fine-structure spectroscopy results provided evidenced for the recovery of π conjugation in the carbon networks with the removal of oxygenated groups and revealed chemical bonding of the nitrogen atoms in N-RGO. The good electrochemical performance of N-RGO is attributed to its high surface area, high electrical conductivity, and low oxygen content. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Solvothermal one-step synthesis of Ni-Al layered double hydroxide/carbon nanotube/reduced graphene oxide sheet ternary nanocomposite with ultrahigh capacitance for supercapacitors.

PubMed

Yang, Wanlu; Gao, Zan; Wang, Jun; Ma, Jing; Zhang, Milin; Liu, Lianhe

2013-06-26

A Ni-Al layered double hydroxide (LDH), mutil-wall carbon nanotube (CNT), and reduced graphene oxide sheet (GNS) ternary nanocomposite electrode material has been developed by a facile one-step ethanol solvothermal method. The obtained LDH/CNT/GNS composite displayed a three-dimensional (3D) architecture with flowerlike Ni-Al LDH/CNT nanocrystallites gradually self-assembled on GNS nanosheets. GNS was used as building blocks to construct 3D nanostructure, and the LDH/CNT nanoflowers in turn separated the two-dimensional (2D) GNS sheets, which preserved the high surface area of GNSs. Furthermore, the generated porous networks with a narrow pore size distribution in the LDH/CNT/GNS composite were also demonstrated by the N2 adsorption/desorption experiment. Such morphology would be favorable to improve the mass transfer and electrochemical action of the electrode. As supercapacitor electrode material, the LDH/CNT/GNS hybrid exhibited excellent electrochemical performance, including ultrahigh specific capacitance (1562 F/g at 5 mA/cm(2)), excellent rate capability, and long-term cycling performance, which could be a promising energy storage/conversion material for supercapacitor application.

Reduced graphene oxide modified NiFe-calcinated layered double hydroxides for enhanced photocatalytic removal of methylene blue

NASA Astrophysics Data System (ADS)

Zhao, Guoqing; Li, Caifeng; Wu, Xia; Yu, Jingang; Jiang, Xinyu; Hu, Wenjihao; Jiao, Feipeng

2018-03-01

Calcined layered double hydroxides (CLDH) are one of the remarkable photocatalysts passionately studied for photodecolorization of organic dyes. NiFe-CLDH was successfully modified by reduced graphene oxide (RGO) through a facile in situ crystallization technique. The obtained RGO/NiFe-CLDH composites were fully characterized by powder X-ray diffraction (XRD), Scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), Fourier transform infrared (FT-IR), and UV-vis diffuse reflectance spectroscopy (DRS). The results analysis indicated that RGO sheets could work as base course to prompt the growth of LDH crystallites and NiFe-LDH lamellar crystal promiscuously distributed on the sheets with a strong interplay between each other. The photocatalytic performance of RGO/NiFe-CLDH composites toward decolorization of methylene blue tightly depended on the mass fraction of RGO and calcinated temperature. At the RGO weight loading of 1%, calcination temperature of 500 °C, the photocatalytic degradation efficiency of RGO/NiFe-CLDH composites reached 93.0% within 5.0 h. The enhanced activity of RGO/NiFe-CLDH composites may be due to the concerted catalysis effect between two constituents of as-prepared composites.

Evaluation of layered double hydroxide/graphene hybrid as a sorbent in membrane-protected stir-bar supported micro-solid-phase extraction for determination of organochlorine pesticides in urine samples.

PubMed

Sajid, Muhammad; Basheer, Chanbasha; Daud, Muhammad; Alsharaa, Abdulnaser

2017-03-17

In this work, the potential of layered double hydroxide/graphene (LDH-G) hybrid as a sorbent for extraction and preconcentration of fifteen organochlorine pesticides (OCPs) in urine samples was evaluated. The LDH-G hybrid was synthesized by co-precipitation method and it was then characterized by Fourier transform infrared spectroscopy, scanning electron microscopy, transmission electron microscopy and X-ray diffraction. The sorbent was then employed in membrane-protected stir-bar supported micro-solid-phase extraction (SB-μ-SPE) of OCPs in urine samples. This extraction approach is highly suitable for the samples representing matrix complexity such as urine because the sorbent is effectively protected inside the membrane. The extracted samples were analyzed by gas chromatography mass spectrometry. The factors that affect the performance of SB-μ-SPE were suitably optimized. This method demonstrated good linearity with coefficients of determination up to 0.9996. The limits of detection ranged between 0.22 and 1.38ngmL -1 . The RSD values for intra and inter-day precision were also in a satisfactory range (2.7-9.5%). Copyright © 2017 Elsevier B.V. All rights reserved.

Synthesis and characterization of graphene quantum dots/CoNiAl-layered double-hydroxide nanocomposite: Application as a glucose sensor.

PubMed

Samuei, Sara; Fakkar, Jila; Rezvani, Zolfaghar; Shomali, Ashkan; Habibi, Biuck

2017-03-15

In the present work, a novel nanocomposite based on the graphene quantum dots and CoNiAl-layered double-hydroxide was successfully synthesized by co-precipitation method. To achieve the morphological, structural and compositional information, the resulted nanocomposite was characterized by scanning electron microscopy X-ray diffraction, thermal gravimetric analysis, Fourier transform infrared spectroscopy, and photoluminescence. Then, the nanocomposite was used as a modifier to fabricate a modified carbon paste electrode as a non-enzymatic sensor for glucose determination. Electrochemical behavior and determination of glucose at the nanocomposite modified carbon paste electrode were investigated by cyclic voltammetry and chronoamperometry methods, respectively. The prepared sensor offered good electrocatalytic properties, fast response time, high reproducibility and stability. At the optimum conditions, the constructed sensor exhibits wide linear range; 0.01-14.0 mM with a detection limit of 6 μM (S/N = 3) and high sensitivity of 48.717 μAmM -1 . Finally, the sensor was successfully applied to determine the glucose in real samples which demonstrated its applicability. Copyright © 2017 Elsevier Inc. All rights reserved.

Ceramic Composite Thin Films

NASA Technical Reports Server (NTRS)

Dikin, Dmitriy A. (Inventor); Nguyen, SonBinh T. (Inventor); Ruoff, Rodney S. (Inventor); Stankovich, Sasha (Inventor)

2013-01-01

A ceramic composite thin film or layer includes individual graphene oxide and/or electrically conductive graphene sheets dispersed in a ceramic (e.g. silica) matrix. The thin film or layer can be electrically conductive film or layer depending the amount of graphene sheets present. The composite films or layers are transparent, chemically inert and compatible with both glass and hydrophilic SiOx/silicon substrates. The composite film or layer can be produced by making a suspension of graphene oxide sheet fragments, introducing a silica-precursor or silica to the suspension to form a sol, depositing the sol on a substrate as thin film or layer, at least partially reducing the graphene oxide sheets to conductive graphene sheets, and thermally consolidating the thin film or layer to form a silica matrix in which the graphene oxide and/or graphene sheets are dispersed.

Flexible Textile-Based Organic Transistors Using Graphene/Ag Nanoparticle Electrode

PubMed Central

Kim, Youn; Kwon, Yeon Ju; Lee, Kang Eun; Oh, Youngseok; Um, Moon-Kwang; Seong, Dong Gi; Lee, Jea Uk

2016-01-01

Highly flexible and electrically-conductive multifunctional textiles are desirable for use in wearable electronic applications. In this study, we fabricated multifunctional textile composites by vacuum filtration and wet-transfer of graphene oxide films on a flexible polyethylene terephthalate (PET) textile in association with embedding Ag nanoparticles (AgNPs) to improve the electrical conductivity. A flexible organic transistor can be developed by direct transfer of a dielectric/semiconducting double layer on the graphene/AgNP textile composite, where the textile composite was used as both flexible substrate and conductive gate electrode. The thermal treatment of a textile-based transistor enhanced the electrical performance (mobility = 7.2 cm2·V−1·s−1, on/off current ratio = 4 × 105, and threshold voltage = −1.1 V) due to the improvement of interfacial properties between the conductive textile electrode and the ion-gel dielectric layer. Furthermore, the textile transistors exhibited highly stable device performance under extended bending conditions (with a bending radius down to 3 mm and repeated tests over 1000 cycles). We believe that our simple methods for the fabrication of graphene/AgNP textile composite for use in textile-type transistors can potentially be applied to the development of flexible large-area electronic clothes. PMID:28335276

Gold nano particle decorated graphene core first generation PAMAM dendrimer for label free electrochemical DNA hybridization sensing.

PubMed

Jayakumar, K; Rajesh, R; Dharuman, V; Venkatasan, R; Hahn, J H; Pandian, S Karutha

2012-01-15

A novel first generation (G1) poly(amidoamine) dendrimer (PAMAM) with graphene core (GG1PAMAM) was synthesized for the first time. Single layer of GG1PAMAM was immobilized covalently on mercaptopropionic acid (MPA) monolayer on Au transducer. This allows cost effective and easy deposition of single layer graphene on the Au transducer surface than the advanced vacuum techniques used in the literature. Au nano particles (17.5 nm) then decorated the GG1PAMAM and used for electrochemical DNA hybridization sensing. The sensor discriminates selectively and sensitively the complementary double stranded DNA (dsDNA, hybridized), non-complementary DNA (ssDNA, un-hybridized) and single nucleotide polymorphism (SNP) surfaces. Interactions of the MPA, GG1PAMAM and the Au nano particles were characterized by Ultra Violet (UV), Fourier Transform Infrared (FTIR), Raman spectroscopy (RS), Thermo gravimetric analysis (TGA), Scanning Electron Microscopy (SEM), Atomic Force Microscopy (AFM), Cyclic Voltmetric (CV), Impedance spectroscopy (IS) and Differntial Pulse Voltammetry (DPV) techniques. The sensor showed linear range 1×10(-6) to 1×10(-12) M with lowest detection limit 1 pM which is 1000 times lower than G1PAMAM without graphene core. Copyright © 2011 Elsevier B.V. All rights reserved.

Recent progress in layered double hydroxide based materials for electrochemical capacitors: design, synthesis and performance.

PubMed

Zhao, Mingming; Zhao, Qunxing; Li, Bing; Xue, Huaiguo; Pang, Huan; Chen, Changyun

2017-10-19

As representative two-dimensional (2D) materials, layered double hydroxides (LDHs) have received increasing attention in electrochemical energy storage and conversion because of the facile tunability between their composition and morphology. The high dispersion of active species in layered arrays, the simple exfoliation into monolayer nanosheets and chemical modification offer the LDHs an opportunity as active electrode materials in electrochemical capacitors (ECs). LDHs are favourable in providing large specific surface areas, good transport features as well as attractive physicochemical properties. In this review, our purpose is to provide a detailed summary of recent developments in the synthesis and electrochemical performance of the LDHs. Their composites with carbon (carbon quantum dots, carbon black, carbon nanotubes/nanofibers, graphene/graphene oxides), metals (nickel, platinum, silver), metal oxides (TiO 2 , Co 3 O 4 , CuO, MnO 2 , Fe 3 O 4 ), metal sulfides/phosphides (CoS, NiCo 2 S 4 , NiP), MOFs (MOF derivatives) and polymers (PEDOT:PSS, PPy (polypyrrole), P(NIPAM-co-SPMA) and PET) are also discussed in this review. The relationship between structures and electrochemical properties as well as the associated charge-storage mechanisms is discussed. Moreover, challenges and prospects of the LDHs for high-performance ECs are presented. This review sheds light on the sustainable development of ECs with LDH based electrode materials.

Scanning electrochemical microscopy of graphene/polymer hybrid thin films as supercapacitors: Physical-chemical interfacial processes

NASA Astrophysics Data System (ADS)

Gupta, Sanju; Price, Carson

2015-10-01

Hybrid electrode comprising an electric double-layer capacitor of graphene nanosheets and a pseudocapacitor of the electrically conducting polymers namely, polyaniline; PAni and polypyrrole; PPy are constructed that exhibited synergistic effect with excellent electrochemical performance as thin film supercapacitors for alternative energy. The hybrid supercapacitors were prepared by layer-by-layer (LbL) assembly based on controlled electrochemical polymerization followed by reduction of graphene oxide electrochemically producing ErGO, for establishing intimate electronic contact through nanoscale architecture and chemical stability, producing a single bilayer of (PAni/ErGO)1, (PPy/ErGO)1, (PAni/GO)1 and (PPy/GO)1. The rationale design is to create thin films that possess interconnected graphene nanosheets (GNS) with polymer nanostructures forming well-defined tailored interfaces allowing sufficient surface adsorption and faster ion transport due to short diffusion distances. We investigated their electrochemical properties and performance in terms of gravimetric specific capacitance, Cs, from cyclic voltammograms. The LbL-assembled bilayer films exhibited an excellent Cs of ≥350 F g-1 as compared with constituents (˜70 F g-1) at discharge current density of 0.3 A g-1 that outperformed many other hybrid supercapacitors. To gain deeper insights into the physical-chemical interfacial processes occurring at the electrode/electrolyte interface that govern their operation, we have used scanning electrochemical microscopy (SECM) technique in feedback and probe approach modes. We present our findings from viewpoint of reinforcing the role played by heterogeneous electrode surface composed of nanoscale graphene sheets (conducting) and conducting polymers (semiconducting) backbone with ordered polymer chains via higher/lower probe current distribution maps. Also targeted is SECM imaging that allowed to determine electrochemical (re)activity of surface ion adsorption sites density at solid/liquid interface.

Solving the Controversy on the Wetting Transparency of Graphene.

PubMed

Kim, Donggyu; Pugno, Nicola M; Buehler, Markus J; Ryu, Seunghwa

2015-10-26

Since its discovery, the wetting transparency of graphene, the transmission of the substrate wetting property over graphene coating, has gained significant attention due to its versatility for potential applications. Yet, there have been debates on the interpretation and validity of the wetting transparency. Here, we present a theory taking two previously disregarded factors into account and elucidate the origin of the partial wetting transparency. We show that the liquid bulk modulus is crucial to accurately calculate the van der Waals interactions between the liquid and the surface, and that various wetting states on rough surfaces must be considered to understand a wide range of contact angle measurements that cannot be fitted with a theory considering the flat surface. In addition, we reveal that the wetting characteristic of the substrate almost vanishes when covered by any coating as thick as graphene double layers. Our findings reveal a more complete picture of the wetting transparency of graphene as well as other atomically thin coatings, and can be applied to study various surface engineering problems requiring wettability-tuning.

Graphene-Based Ultra-Light Batteries for Aircraft

NASA Technical Reports Server (NTRS)

Calle, Carlos I.; Kaner, Richard B.

2014-01-01

Develop a graphene-based ultracapacitor prototype that is flexible, thin, lightweight, durable, low cost, and safe and that will demonstrate the feasibility for use in aircraft center dot These graphene-based devices store charge on graphene sheets and take advantage of the large accessible surface area of graphene (2,600 m2/g) to increase the electrical energy that can be stored. center dot The proposed devices should have the electrical storage capacity of thin-film-ion batteries but with much shorter charge/discharge cycle times as well as longer lives center dot The proposed devices will be carbon-based and so will not have the same issues with flammability or toxicity as the standard lithium-based storage cells There are two main established methods for the storage and delivery of electrical energy: center dot Batteries - Store energy with electrochemical reactions - High energy densities - Slow charge/discharge cycles - Used in applications requiring large amounts of energy ? aircraft center dot Electrochemical capacitors - Store energy in electrochemical double layers - Fast charge/discharge cycles - Low energy densities - Used in electronics devices - Large capacitors are used in truck engine cranking

Solving the Controversy on the Wetting Transparency of Graphene

PubMed Central

Kim, Donggyu; Pugno, Nicola M.; Buehler, Markus J.; Ryu, Seunghwa

2015-01-01

Since its discovery, the wetting transparency of graphene, the transmission of the substrate wetting property over graphene coating, has gained significant attention due to its versatility for potential applications. Yet, there have been debates on the interpretation and validity of the wetting transparency. Here, we present a theory taking two previously disregarded factors into account and elucidate the origin of the partial wetting transparency. We show that the liquid bulk modulus is crucial to accurately calculate the van der Waals interactions between the liquid and the surface, and that various wetting states on rough surfaces must be considered to understand a wide range of contact angle measurements that cannot be fitted with a theory considering the flat surface. In addition, we reveal that the wetting characteristic of the substrate almost vanishes when covered by any coating as thick as graphene double layers. Our findings reveal a more complete picture of the wetting transparency of graphene as well as other atomically thin coatings, and can be applied to study various surface engineering problems requiring wettability-tuning. PMID:26496835

Electronic nanobiosensors based on two-dimensional materials

NASA Astrophysics Data System (ADS)

Ping, Jinglei

Atomically-thick two-dimensional (2D) nanomaterials have tremendous potential to be applied as transduction elements in biosensors and bioelectronics. We developed scalable methods for synthesis and large-area transfer of two-dimensional nanomaterials, particularly graphene and metal dichalcogenides (so called ``MX2'' materials). We also developed versatile fabrication methods for large arrays of field-effect transistors (FETs) and micro-electrodes with these nanomaterials based on either conventional photolithography or innovative approaches that minimize contamination of the 2D layer. By functionalizing the FETs with a computationally redesigned water-soluble mu-opioid receptor, we created selective and sensitive biosensors suitable for detection of the drug target naltrexone and the neuropeptide enkephalin at pg/mL concentrations. We also constructed DNA-functionalized biosensors and nano-particle decorated biosensors by applying related bio-nano integration techniques. Our methodology paves the way for multiplexed nanosensor arrays with all-electronic readout suitable for inexpensive point-of-care diagnostics, drug-development and biomedical research. With graphene field-effect transistors, we investigated the graphene/solution interface and developed a quantitative model for the effect of ionic screening on the graphene carrier density based on theories of the electric double layer. Finally, we have developed a technique for measuring low-level Faradaic charge-transfer current (fA) across the graphene/solution interface via real-time charge monitoring of graphene microelectrodes in ionic solution. This technique enables the development of flexible and transparent pH sensors that are promising for in vivo applications. The author acknowledges the support from the Defense Advanced Research Projects Agency (DARPA) and the U. S. Army Research Office under Grant Number W911NF1010093.

Evaluation of Graphene/WO3 and Graphene/CeO x Structures as Electrodes for Supercapacitor Applications

NASA Astrophysics Data System (ADS)

Chaitoglou, Stefanos; Amade, Roger; Bertran, Enric

2017-12-01

The combination of graphene with transition metal oxides can result in very promising hybrid materials for use in energy storage applications thanks to its intriguing properties, i.e., highly tunable surface area, outstanding electrical conductivity, good chemical stability, and excellent mechanical behavior. In the present work, we evaluate the performance of graphene/metal oxide (WO3 and CeO x ) layered structures as potential electrodes in supercapacitor applications. Graphene layers were grown by chemical vapor deposition (CVD) on copper substrates. Single and layer-by-layer graphene stacks were fabricated combining graphene transfer techniques and metal oxides grown by magnetron sputtering. The electrochemical properties of the samples were analyzed and the results suggest an improvement in the performance of the device with the increase in the number of graphene layers. Furthermore, deposition of transition metal oxides within the stack of graphene layers further improves the areal capacitance of the device up to 4.55 mF/cm2, for the case of a three-layer stack. Such high values are interpreted as a result of the copper oxide grown between the copper substrate and the graphene layer. The electrodes present good stability for the first 850 cycles before degradation.

Controllable poly-crystalline bilayered and multilayered graphene film growth by reciprocal chemical vapor deposition

NASA Astrophysics Data System (ADS)

Wu, Qinke; Jung, Seong Jun; Jang, Sung Kyu; Lee, Joohyun; Jeon, Insu; Suh, Hwansoo; Kim, Yong Ho; Lee, Young Hee; Lee, Sungjoo; Song, Young Jae

2015-06-01

We report the selective growth of large-area bilayered graphene film and multilayered graphene film on copper. This growth was achieved by introducing a reciprocal chemical vapor deposition (CVD) process that took advantage of an intermediate h-BN layer as a sacrificial template for graphene growth. A thin h-BN film, initially grown on the copper substrate using CVD methods, was locally etched away during the subsequent graphene growth under residual H2 and CH4 gas flows. Etching of the h-BN layer formed a channel that permitted the growth of additional graphene adlayers below the existing graphene layer. Bilayered graphene typically covers an entire Cu foil with domain sizes of 10-50 μm, whereas multilayered graphene can be epitaxially grown to form islands a few hundreds of microns in size. This new mechanism, in which graphene growth proceeded simultaneously with h-BN etching, suggests a potential approach to control graphene layers for engineering the band structures of large-area graphene for electronic device applications.We report the selective growth of large-area bilayered graphene film and multilayered graphene film on copper. This growth was achieved by introducing a reciprocal chemical vapor deposition (CVD) process that took advantage of an intermediate h-BN layer as a sacrificial template for graphene growth. A thin h-BN film, initially grown on the copper substrate using CVD methods, was locally etched away during the subsequent graphene growth under residual H2 and CH4 gas flows. Etching of the h-BN layer formed a channel that permitted the growth of additional graphene adlayers below the existing graphene layer. Bilayered graphene typically covers an entire Cu foil with domain sizes of 10-50 μm, whereas multilayered graphene can be epitaxially grown to form islands a few hundreds of microns in size. This new mechanism, in which graphene growth proceeded simultaneously with h-BN etching, suggests a potential approach to control graphene layers for engineering the band structures of large-area graphene for electronic device applications. Electronic supplementary information (ESI) available: The growth conditions, statistical studies of OM images and high-resolution STM/TEM measurements for multi-/bi-layered graphene are discussed in detail. See DOI: 10.1039/c5nr02716k

Atomic layer deposited oxide films as protective interface layers for integrated graphene transfer

NASA Astrophysics Data System (ADS)

Cabrero-Vilatela, A.; Alexander-Webber, J. A.; Sagade, A. A.; Aria, A. I.; Braeuninger-Weimer, P.; Martin, M.-B.; Weatherup, R. S.; Hofmann, S.

2017-12-01

The transfer of chemical vapour deposited graphene from its parent growth catalyst has become a bottleneck for many of its emerging applications. The sacrificial polymer layers that are typically deposited onto graphene for mechanical support during transfer are challenging to remove completely and hence leave graphene and subsequent device interfaces contaminated. Here, we report on the use of atomic layer deposited (ALD) oxide films as protective interface and support layers during graphene transfer. The method avoids any direct contact of the graphene with polymers and through the use of thicker ALD layers (≥100 nm), polymers can be eliminated from the transfer-process altogether. The ALD film can be kept as a functional device layer, facilitating integrated device manufacturing. We demonstrate back-gated field effect devices based on single-layer graphene transferred with a protective Al2O3 film onto SiO2 that show significantly reduced charge trap and residual carrier densities. We critically discuss the advantages and challenges of processing graphene/ALD bilayer structures.

Ultrafast electron-optical phonon scattering and quasiparticle lifetime in CVD-grown graphene.

PubMed

Shang, Jingzhi; Yu, Ting; Lin, Jianyi; Gurzadyan, Gagik G

2011-04-26

Ultrafast quasiparticle dynamics in graphene grown by chemical vapor deposition (CVD) has been studied by UV pump/white-light probe spectroscopy. Transient differential transmission spectra of monolayer graphene are observed in the visible probe range (400-650 nm). Kinetics of the quasiparticle (i.e., low-energy single-particle excitation with renormalized energy due to electron-electron Coulomb, electron-optical phonon (e-op), and optical phonon-acoustic phonon (op-ap) interactions) was monitored with 50 fs resolution. Extending the probe range to near-infrared, we find the evolution of quasiparticle relaxation channels from monoexponential e-op scattering to double exponential decay due to e-op and op-ap scattering. Moreover, quasiparticle lifetimes of mono- and randomly stacked graphene films are obtained for the probe photon energies continuously from 1.9 to 2.3 eV. Dependence of quasiparticle decay rate on the probe energy is linear for 10-layer stacked graphene films. This is due to the dominant e-op intervalley scattering and the linear density of states in the probed electronic band. A dimensionless coupling constant W is derived, which characterizes the scattering strength of quasiparticles by lattice points in graphene.

Eco-friendly synthesis of size-controllable amine-functionalized graphene quantum dots with antimycoplasma properties.

PubMed

Jiang, Feng; Chen, Daiqin; Li, Ruimin; Wang, Yucheng; Zhang, Guoqiang; Li, Shumu; Zheng, Junpeng; Huang, Naiyan; Gu, Ying; Wang, Chunru; Shu, Chunying

2013-02-07

Size-controllable amine-functionalized graphene quantum dots (GQDs) are prepared by an eco-friendly method with graphene oxide sheets, ammonia and hydrogen peroxide as starting materials. Using a Sephadex G-25 gel column for fine separation, for the first time we obtain GQDs with either single or double layers. By atomic force microscopy characterization, we confirm that hydrogen peroxide and ammonia play a synergistic role on graphene oxide (GO), in which the former cuts the GO into small pieces and the latter passivates the active surface to give amine-modified GQDs. Due to the low cytotoxicity and excellent biocompatibility of the obtained amine-functionalized GQDs, besides the multiwavelength imaging properties of GQDs, for the first time we find that this kind of GQD exhibits good antimycoplasma properties. Given the superior antimycoplasma effect of the GQDs and their eco-friendly mass production with low cost, these new GQDs may offer opportunities for the development of new antimycoplasma agents, thus extending their widespread application in biomedicine.

Conductance of graphene-based double-barrier nanostructures.

PubMed

Setare, M R; Jahani, D

2010-12-22

The effect of a mass gap on the conductance of graphene double-barrier heterojunctions is studied. By obtaining the 2D expression for the electronic transport of the low energy excitations of pure graphene through double-barrier systems, it is found that the conductivity of these structures does not depend on the type of charge carriers in the zones of the electric field. However, a finite induced gap in the graphene spectrum makes conductivity dependent on the energy band index. We also discuss a few controversies concerning double-barrier systems stemming from an improper choice of the scattering angle. Then it is observed that, for some special values of the incident energy and potential's height, graphene junctions behave like left-handed materials, resulting in a maximum value for the conductivity.

Modification of the contact surfaces for improving the puncture resistance of laminar structures.

PubMed

Wang, Pengfei; Yang, Jinglei; Li, Xin; Liu, Mao; Zhang, Xin; Sun, Dawei; Bao, Chenlu; Gao, Guangfa; Yahya, Mohd Yazid; Xu, Songlin

2017-07-26

Uncovering energy absorption and surface effects of various penetrating velocities on laminar structures is essential for designing protective structures. In this study, both quasi-static and dynamic penetration tests were systematical conducted on the front surfaces of metal sheets coated with a graphene oxide (GO) solution and other media. The addition of a GO fluid film to the front impact surface aided in increasing the penetration strength, improving the failure extension and dissipating additional energy under a wide-range of indentation velocity, from 3.33 × 10 -5  m/s to 4.42 m/s. The coated -surfaces improved the specific energy dissipation by approximately 15~40% relative to the dry-contact configuration for both single-layer and double-layer configurations, and specific energy dissipations of double-layer configurations were 20~30% higher than those of the single-layer configurations. This treatment provides a facile strategy in changing the contact state for improving the failure load and dissipate additional energy.

Covalent modification and exfoliation of graphene oxide using ferrocene

NASA Astrophysics Data System (ADS)

Avinash, M. B.; Subrahmanyam, K. S.; Sundarayya, Y.; Govindaraju, T.

2010-09-01

Large scale preparation of single-layer graphene and graphene oxide is of great importance due to their potential applications. We report a simple room temperature method for the exfoliation of graphene oxide using covalent modification of graphene oxide with ferrocene to obtain single-layer graphene oxide sheets. The samples were characterized by FESEM, HRTEM, AFM, EDAX, FT-IR, Raman and Mössbauer spectroscopic studies. HRTEM micrograph of the covalently modified graphene oxide showed increased interlayer spacing of ~2.4 nm due to ferrocene intercalation. The presence of single-layer graphene oxide sheets were confirmed by AFM studies. The covalently modified ferrocene-graphene oxide composite showed interesting magnetic behavior.Large scale preparation of single-layer graphene and graphene oxide is of great importance due to their potential applications. We report a simple room temperature method for the exfoliation of graphene oxide using covalent modification of graphene oxide with ferrocene to obtain single-layer graphene oxide sheets. The samples were characterized by FESEM, HRTEM, AFM, EDAX, FT-IR, Raman and Mössbauer spectroscopic studies. HRTEM micrograph of the covalently modified graphene oxide showed increased interlayer spacing of ~2.4 nm due to ferrocene intercalation. The presence of single-layer graphene oxide sheets were confirmed by AFM studies. The covalently modified ferrocene-graphene oxide composite showed interesting magnetic behavior. Electronic supplementary information (ESI) available: Magnetic data; AFM images; TEM micrographs; and Mössbauer spectroscopic data. See DOI: 10.1039/c0nr00024h

Benzocyclobutene (BCB) Polymer as Amphibious Buffer Layer for Graphene Field-Effect Transistor.

PubMed

Wu, Yun; Zou, Jianjun; Huo, Shuai; Lu, Haiyan; Kong, Yuecan; Chen, Tangshen; Wu, Wei; Xu, Jingxia

2015-08-01

Owing to the scattering and trapping effects, the interfaces of dielectric/graphene or substrate/graphene can tailor the performance of field-effect transistor (FET). In this letter, the polymer of benzocyclobutene (BCB) was used as an amphibious buffer layer and located at between the layers of substrate and graphene and between the layers of dielectric and graphene. Interestingly, with the help of nonpolar and hydrophobic BCB buffer layer, the large-scale top-gated, chemical vapor deposited (CVD) graphene transistors was prepared on Si/SiO2 substrate, its cutoff frequency (fT) and the maximum cutoff frequency (fmax) of the graphene field-effect transistor (GFET) can be reached at 12 GHz and 11 GHz, respectively.

High-temperature electron-hole superfluidity with strong anisotropic gaps in double phosphorene monolayers

NASA Astrophysics Data System (ADS)

Saberi-Pouya, S.; Zarenia, M.; Perali, A.; Vazifehshenas, T.; Peeters, F. M.

2018-05-01

Excitonic superfluidity in double phosphorene monolayers is investigated using the BCS mean-field equations. Highly anisotropic superfluidity is predicted where we found that the maximum superfluid gap is in the Bose-Einstein condensate (BEC) regime along the armchair direction and in the BCS-BEC crossover regime along the zigzag direction. We estimate the highest Kosterlitz-Thouless transition temperature with maximum value up to ˜90 K with onset carrier densities as high as 4 ×1012cm-2 . This transition temperature is significantly larger than what is found in double electron-hole few-layers graphene. Our results can guide experimental research toward the realization of anisotropic condensate states in electron-hole phosphorene monolayers.

Direct growth of graphene-dielectric bi-layer structure on device substrates from Si-based polymer

NASA Astrophysics Data System (ADS)

Seo, Hong-Kyu; Kim, Kyunghun; Min, Sung-Yong; Lee, Yeongjun; Eon Park, Chan; Raj, Rishi; Lee, Tae-Woo

2017-06-01

To facilitate the utilization of graphene films in conventional semiconducting devices (e.g. transistors and memories) which includes an insulating layer such as gate dielectric, facile synthesis of bi-layers composed of a graphene film and an insulating layer by one-step thermal conversion will be very important. We demonstrate a simple, inexpensive, scalable and patternable process to synthesize graphene-dielectric bi-layer films from solution-processed polydimethylsiloxane (PDMS) under a Ni capping layer. This method fabricates graphene-dielectric bi-layer structure simultaneously directly on substrate by thermal conversion of PDMS without using additional graphene transfer and patterning process or formation of an expensive dielectric layer, which makes the device fabrication process much easier. The graphene-dielectric bi-layer on a conducting substrate was used in bottom-contact pentacene field-effect transistors that showed ohmic contact and small hysteresis. Our new method will provide a way to fabricate flexible electronic devices simply and inexpensively.

A review of molecular modelling of electric double layer capacitors.

PubMed

Burt, Ryan; Birkett, Greg; Zhao, X S

2014-04-14

Electric double-layer capacitors are a family of electrochemical energy storage devices that offer a number of advantages, such as high power density and long cyclability. In recent years, research and development of electric double-layer capacitor technology has been growing rapidly, in response to the increasing demand for energy storage devices from emerging industries, such as hybrid and electric vehicles, renewable energy, and smart grid management. The past few years have witnessed a number of significant research breakthroughs in terms of novel electrodes, new electrolytes, and fabrication of devices, thanks to the discovery of innovative materials (e.g. graphene, carbide-derived carbon, and templated carbon) and the availability of advanced experimental and computational tools. However, some experimental observations could not be clearly understood and interpreted due to limitations of traditional theories, some of which were developed more than one hundred years ago. This has led to significant research efforts in computational simulation and modelling, aimed at developing new theories, or improving the existing ones to help interpret experimental results. This review article provides a summary of research progress in molecular modelling of the physical phenomena taking place in electric double-layer capacitors. An introduction to electric double-layer capacitors and their applications, alongside a brief description of electric double layer theories, is presented first. Second, molecular modelling of ion behaviours of various electrolytes interacting with electrodes under different conditions is reviewed. Finally, key conclusions and outlooks are given. Simulations on comparing electric double-layer structure at planar and porous electrode surfaces under equilibrium conditions have revealed significant structural differences between the two electrode types, and porous electrodes have been shown to store charge more efficiently. Accurate electrolyte and electrode models which account for polarisation effects are critical for future simulations which will consider more complex electrode geometries, particularly for the study of dynamics of electrolyte transport, where the exclusion of electrode polarisation leads to significant artefacts.

Layer-controllable graphene by plasma thinning and post-annealing

NASA Astrophysics Data System (ADS)

Zhang, Lufang; Feng, Shaopeng; Xiao, Shaoqing; Shen, Gang; Zhang, Xiumei; Nan, Haiyan; Gu, Xiaofeng; Ostrikov, Kostya (Ken)

2018-05-01

The electronic structure of graphene depends crucially on its layer number and therefore engineering the number of graphene's atomic stacking layers is of great importance for the preparation of graphene-based devices. In this paper, we demonstrated a relatively less invasive, high-throughput and uniform large-area plasma thinning of graphene based on direct bombardment effect of fast-moving ionic hydrogen or argon species. Any desired number of graphene layers including trilayer, bilayer and monolayer can be obtained. Structural changes of graphene layers are studied by optical microscopy, Raman spectroscopy and atomic force microscopy. Post annealing is adopted to self-heal the lattice defects induced by the ion bombardment effect. This plasma etching technique is efficient and compatible with semiconductor manufacturing processes, and may find important applications for graphene-based device fabrication.

Electronic resonant tunneling on graphene superlattice heterostructures with a tunable graphene layer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Shan; Cui, Liyong; Liu, Fen

We have theoretically investigated the electronic resonant tunneling effect in graphene superlattice heterostructures, where a tunable graphene layer is inserted between two different superlattices. It is found that a complete tunneling state appears inside the enlarged forbidden gap of the heterostructure by changing the thickness of the inserted graphene layer and the transmittance of the tunneling state depends on the thickness of the inserted layer. Furthermore, the frequency of the tunneling state changes with the thickness of the inserted graphene layer but it always located in the little overlapped forbidden gap of two graphene superlattices. Therefore, both a perfect tunnelingmore » state and an ultrawide forbidden gap are realized in such heterostrutures. Since maximum probability densities of the perfect tunneling state are highly localized near the interface between the inserted graphene layer and one graphene superlattice, it can be named as an interface-like state. Such structures are important to fabricate high-Q narrowband electron wave filters.« less

Temperature Dependence of Raman-Active In-Plane E2g Phonons in Layered Graphene and h-BN Flakes

NASA Astrophysics Data System (ADS)

Li, Xiaoli; Liu, Jian; Ding, Kai; Zhao, Xiaohui; Li, Shuai; Zhou, Wenguang; Liang, Baolai

2018-01-01

Thermal properties of sp2 systems such as graphene and hexagonal boron nitride (h-BN) have attracted significant attention because of both systems being excellent thermal conductors. This research reports micro-Raman measurements on the in-plane E2g optical phonon peaks ( 1580 cm-1 in graphene layers and 1362 cm-1 in h-BN layers) as a function of temperature from - 194 to 200 °C. The h-BN flakes show higher sensitivity to temperature-dependent frequency shifts and broadenings than graphene flakes. Moreover, the thermal effect in the c direction on phonon frequency in h-BN layers is more sensitive than that in graphene layers but on phonon broadening in h-BN layers is similar as that in graphene layers. These results are very useful to understand the thermal properties and related physical mechanisms in h-BN and graphene flakes for applications of thermal devices.

Monitoring the layer-by-layer self-assembly of graphene and graphene oxide by spectroscopic ellipsometry.

PubMed

Zhou, Kai-Ge; Chang, Meng-Jie; Wang, Hang-Xing; Xie, Yu-Long; Zhang, Hao-Li

2012-01-01

Thin films of graphene oxide, graphene and copper (II) phthalocyanine dye have been successfully fabricated by electrostatic layer-by-layer (LbL) assembly approach. We present the first variable angle spectroscopic ellipsometry (VASE) investigation on these graphene-dye hybrid thin films. The thickness evaluation suggested that our LbL assembly process produces highly uniform and reproducible thin films. We demonstrate that the refractive indices of the graphene-dye thin films undergo dramatic variation in the range close to the absorption of the dyes. This investigation provides new insight to the optical properties of graphene containing thin films and shall help to establish an appropriate optical model for graphene-based hybrid materials.

Layer-dependent supercapacitance of graphene films grown by chemical vapor deposition on nickel foam

NASA Astrophysics Data System (ADS)

Chen, Wei; Fan, Zhongli; Zeng, Gaofeng; Lai, Zhiping

2013-03-01

High-quality, large-area graphene films with few layers are synthesized on commercial nickel foams under optimal chemical vapor deposition conditions. The number of graphene layers is adjusted by varying the rate of the cooling process. It is found that the capacitive properties of graphene films are related to the number of graphene layers. Owing to the close attachment of graphene films on the nickel substrate and the low charge-transfer resistance, the specific capacitance of thinner graphene films is almost twice that of the thicker ones and remains stable up to 1000 cycles. These results illustrate the potential for developing high-performance graphene-based electrical energy storage devices.

Reversible loss of Bernal stacking during the deformation of few-layer graphene in nanocomposites.

PubMed

Gong, Lei; Young, Robert J; Kinloch, Ian A; Haigh, Sarah J; Warner, Jamie H; Hinks, Jonathan A; Xu, Ziwei; Li, Li; Ding, Feng; Riaz, Ibtsam; Jalil, Rashid; Novoselov, Kostya S

2013-08-27

The deformation of nanocomposites containing graphene flakes with different numbers of layers has been investigated with the use of Raman spectroscopy. It has been found that there is a shift of the 2D band to lower wavenumber and that the rate of band shift per unit strain tends to decrease as the number of graphene layers increases. It has been demonstrated that band broadening takes place during tensile deformation for mono- and bilayer graphene but that band narrowing occurs when the number of graphene layers is more than two. It is also found that the characteristic asymmetric shape of the 2D Raman band for the graphene with three or more layers changes to a symmetrical shape above about 0.4% strain and that it reverts to an asymmetric shape on unloading. This change in Raman band shape and width has been interpreted as being due to a reversible loss of Bernal stacking in the few-layer graphene during deformation. It has been shown that the elastic strain energy released from the unloading of the inner graphene layers in the few-layer material (~0.2 meV/atom) is similar to the accepted value of the stacking fault energies of graphite and few layer graphene. It is further shown that this loss of Bernal stacking can be accommodated by the formation of arrays of partial dislocations and stacking faults on the basal plane. The effect of the reversible loss of Bernal stacking upon the electronic structure of few-layer graphene and the possibility of using it to modify the electronic structure of few-layer graphene are discussed.

Reversible Loss of Bernal Stacking during the Deformation of Few-Layer Graphene in Nanocomposites

PubMed Central

2013-01-01

The deformation of nanocomposites containing graphene flakes with different numbers of layers has been investigated with the use of Raman spectroscopy. It has been found that there is a shift of the 2D band to lower wavenumber and that the rate of band shift per unit strain tends to decrease as the number of graphene layers increases. It has been demonstrated that band broadening takes place during tensile deformation for mono- and bilayer graphene but that band narrowing occurs when the number of graphene layers is more than two. It is also found that the characteristic asymmetric shape of the 2D Raman band for the graphene with three or more layers changes to a symmetrical shape above about 0.4% strain and that it reverts to an asymmetric shape on unloading. This change in Raman band shape and width has been interpreted as being due to a reversible loss of Bernal stacking in the few-layer graphene during deformation. It has been shown that the elastic strain energy released from the unloading of the inner graphene layers in the few-layer material (∼0.2 meV/atom) is similar to the accepted value of the stacking fault energies of graphite and few layer graphene. It is further shown that this loss of Bernal stacking can be accommodated by the formation of arrays of partial dislocations and stacking faults on the basal plane. The effect of the reversible loss of Bernal stacking upon the electronic structure of few-layer graphene and the possibility of using it to modify the electronic structure of few-layer graphene are discussed. PMID:23899378

Very large scale characterization of graphene mechanical devices using a colorimetry technique.

PubMed

Cartamil-Bueno, Santiago Jose; Centeno, Alba; Zurutuza, Amaia; Steeneken, Peter Gerard; van der Zant, Herre Sjoerd Jan; Houri, Samer

2017-06-08

We use a scalable optical technique to characterize more than 21 000 circular nanomechanical devices made of suspended single- and double-layer graphene on cavities with different diameters (D) and depths (g). To maximize the contrast between suspended and broken membranes we used a model for selecting the optimal color filter. The method enables parallel and automatized image processing for yield statistics. We find the survival probability to be correlated with a structural mechanics scaling parameter given by D 4 /g 3 . Moreover, we extract a median adhesion energy of Γ = 0.9 J m -2 between the membrane and the native SiO 2 at the bottom of the cavities.

Boron supercapacitors

DOE PAGES

Zhan, Cheng; Zhang, Pengfei; Dai, Sheng; ...

2016-11-16

Supercapacitors based on the electric double-layer mechanism use porous carbons or graphene as electrodes. To move beyond this paradigm, we propose boron supercapacitors to leverage two-dimensional (2D) boron sheets’ metallicity and low weight. Six 2D boron sheets from both previous theoretical design and experimental growth are chosen as test electrodes. By applying joint density functional theory (JDFT) to the electrode–electrolyte system, we examine how the 2D boron sheets charge up against applied potential. JDFT predicts that these 2D boron sheets exhibit specific capacitance on the order of 400 F/g, about four times that of graphene. As a result, our workmore » suggests that 2D boron sheets are promising electrodes for supercapacitor applications.« less

Nonvolatile memory with graphene oxide as a charge storage node in nanowire field-effect transistors

NASA Astrophysics Data System (ADS)

Baek, David J.; Seol, Myeong-Lok; Choi, Sung-Jin; Moon, Dong-Il; Choi, Yang-Kyu

2012-02-01

Through the structural modification of a three-dimensional silicon nanowire field-effect transistor, i.e., a double-gate FinFET, a structural platform was developed which allowed for us to utilize graphene oxide (GO) as a charge trapping layer in a nonvolatile memory device. By creating a nanogap between the gate and the channel, GO was embedded after the complete device fabrication. By applying a proper gate voltage, charge trapping, and de-trapping within the GO was enabled and resulted in large threshold voltage shifts. The employment of GO with FinFET in our work suggests that graphitic materials can potentially play a significant role for future nanoelectronic applications.

Boron supercapacitors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhan, Cheng; Zhang, Pengfei; Dai, Sheng

Supercapacitors based on the electric double-layer mechanism use porous carbons or graphene as electrodes. To move beyond this paradigm, we propose boron supercapacitors to leverage two-dimensional (2D) boron sheets’ metallicity and low weight. Six 2D boron sheets from both previous theoretical design and experimental growth are chosen as test electrodes. By applying joint density functional theory (JDFT) to the electrode–electrolyte system, we examine how the 2D boron sheets charge up against applied potential. JDFT predicts that these 2D boron sheets exhibit specific capacitance on the order of 400 F/g, about four times that of graphene. As a result, our workmore » suggests that 2D boron sheets are promising electrodes for supercapacitor applications.« less

Hierarchical MnO2 nanowire/graphene hybrid fibers with excellent electrochemical performance for flexible solid-state supercapacitors

NASA Astrophysics Data System (ADS)

Ma, Wujun; Chen, Shaohua; Yang, Shengyuan; Chen, Wenping; Cheng, Yanhua; Guo, Yiwei; Peng, Shengjie; Ramakrishna, Seeram; Zhu, Meifang

2016-02-01

Towards rapid development of lightweight, flexible, and even wearable electronics, a highly efficient energy-storage device is required for their energy supply management. Graphene fiber-based supercapacitor is considered as one of the promising candidates because of the remarkable mechanical and electrical properties of graphene fibers. However, supercapacitors based on bare graphene fibers generally suffer a low capacitance, which certainly restricts their potentially wide applications. In this work, hierarchically structured MnO2 nanowire/graphene hybrid fibers are fabricated through a simple, scalable wet-spinning method. The hybrid fibers form mesoporous structure with large specific surface area of 139.9 m2 g-1. The mass loading of MnO2 can be as high as 40 wt%. Due to the synergistic effect between MnO2 nanowires and graphene, the main pseudocapacitance of MnO2 and the electric double-layer capacitance of graphene are improved simultaneously. In view of the practical demonstration, a highly flexible solid-state supercapacitor is fabricated by twisting of two MnO2/graphene fibers coated by polyvinyl alcohol/H3PO4 electrolyte. The supercapacitor exhibits a high volumetric capacitance (66.1 F cm-3, normalized by the total volume of two fiber electrodes), excellent cycling stability (96% capacitance retention over 10,000 cycles), high energy and power density (5.8 mWh cm-3 and 0.51 W cm-3, respectively).

Stacking sequence and interlayer coupling in few-layer graphene revealed by in situ imaging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Zhu-Jun; Dong, Jichen; Cui, Yi

In the transition from graphene to graphite, the addition of each individual graphene layer modifies the electronic structure and produces a different material with unique properties. Controlled growth of few-layer graphene is therefore of fundamental interest and will provide access to materials with engineered electronic structure. Here we combine isothermal growth and etching experiments with in situ scanning electron microscopy to reveal the stacking sequence and interlayer coupling strength in few-layer graphene. The observed layer-dependent etching rates reveal the relative strength of the graphene graphene and graphene substrate interaction and the resulting mode of adlayer growth. Scanning tunnelling microscopy andmore » density functional theory calculations confirm a strong coupling between graphene edge atoms and platinum. Simulated etching confirms that etching can be viewed as reversed growth. This work demonstrates that real-time imaging under controlled atmosphere is a powerful method for designing synthesis protocols for sp2 carbon nanostructures in between graphene and graphite.« less

Stacking sequence and interlayer coupling in few-layer graphene revealed by in situ imaging

DOE PAGES

Wang, Zhu-Jun; Dong, Jichen; Cui, Yi; ...

2016-10-19

In the transition from graphene to graphite, the addition of each individual graphene layer modifies the electronic structure and produces a different material with unique properties. Controlled growth of few-layer graphene is therefore of fundamental interest and will provide access to materials with engineered electronic structure. Here we combine isothermal growth and etching experiments with in situ scanning electron microscopy to reveal the stacking sequence and interlayer coupling strength in few-layer graphene. The observed layer-dependent etching rates reveal the relative strength of the graphene graphene and graphene substrate interaction and the resulting mode of adlayer growth. Scanning tunnelling microscopy andmore » density functional theory calculations confirm a strong coupling between graphene edge atoms and platinum. Simulated etching confirms that etching can be viewed as reversed growth. This work demonstrates that real-time imaging under controlled atmosphere is a powerful method for designing synthesis protocols for sp2 carbon nanostructures in between graphene and graphite.« less

Unusual Enhancement in Intrinsic Thermal Conductivity of Multilayer Graphene by Tensile Strains

DOE PAGES

Kuang, Youdi; Lindsay, Lucas R.; Huang, Baoling

2015-01-01

High basal plane thermal conductivity k of multi-layer graphene makes it promising for thermal management applications. Here we examine the effects of tensile strain on thermal transport in this system. Using a first principles Boltzmann-Peierls equation for phonon transport approach, we calculate the room-temperature in-plane lattice k of multi-layer graphene (up to four layers) and graphite under different isotropic tensile strains. The calculated in-plane k of graphite, finite mono-layer graphene and 3-layer graphene agree well with previous experiments. The dimensional transitions of the intrinsic k and the extent of the diffusive transport regime from mono-layer graphene to graphite are presented.more » We find a peak enhancement of intrinsic k for multi-layer graphene and graphite with increasing strain and the largest enhancement amplitude is about 40%. In contrast the calculated intrinsic k with tensile strain decreases for diamond and diverges for graphene, we show that the competition between the decreased mode heat capacities and the increased lifetimes of flexural phonons with increasing strain contribute to this k behavior. Similar k behavior is observed for 2-layer hexagonal boron nitride systems, suggesting that it is an inherent thermal transport property in multi-layer systems assembled of purely two dimensional atomic layers. This study provides insights into engineering k of multi-layer graphene and boron nitride by strain and into the nature of thermal transport in quasi-two-dimensional and highly anisotropic systems.« less

Synergistic Effect between Ultra-Small Nickel Hydroxide Nanoparticles and Reduced Graphene Oxide sheets for the Application in High-Performance Asymmetric Supercapacitor.

PubMed

Liu, Yonghuan; Wang, Rutao; Yan, Xingbin

2015-06-08

Nanoscale electrode materials including metal oxide nanoparticles and two-dimensional graphene have been employed for designing supercapacitors. However, inevitable agglomeration of nanoparticles and layers stacking of graphene largely hamper their practical applications. Here we demonstrate an efficient co-ordination and synergistic effect between ultra-small Ni(OH)2 nanoparticles and reduced graphene oxide (RGO) sheets for synthesizing ideal electrode materials. On one hand, to make the ultra-small Ni(OH)2 nanoparticles work at full capacity as an ideal pseudocapacitive material, RGO sheets are employed as an suitable substrate to anchor these nanoparticles against agglomeration. As a consequence, an ultrahigh specific capacitance of 1717 F g(-1) at 0.5 A g(-1) is achieved. On the other hand, to further facilitate ion transfer within RGO sheets as an ideal electrical double layer capacitor material, the ultra-small Ni(OH)2 nanoparticles are introduced among RGO sheets as the recyclable sacrificial spacer to prevent the stacking. The resulting RGO sheets exhibit superior rate capability with a high capacitance of 182 F g(-1) at 100 A g(-1). On this basis, an asymmetric supercapacitor is assembled using the two materials, delivering a superior energy density of 75 Wh kg(-1) and an ultrahigh power density of 40 000 W kg(-1).

Synergistic Effect between Ultra-Small Nickel Hydroxide Nanoparticles and Reduced Graphene Oxide sheets for the Application in High-Performance Asymmetric Supercapacitor

PubMed Central

Liu, Yonghuan; Wang, Rutao; Yan, Xingbin

2015-01-01

Nanoscale electrode materials including metal oxide nanoparticles and two-dimensional graphene have been employed for designing supercapacitors. However, inevitable agglomeration of nanoparticles and layers stacking of graphene largely hamper their practical applications. Here we demonstrate an efficient co-ordination and synergistic effect between ultra-small Ni(OH)2 nanoparticles and reduced graphene oxide (RGO) sheets for synthesizing ideal electrode materials. On one hand, to make the ultra-small Ni(OH)2 nanoparticles work at full capacity as an ideal pseudocapacitive material, RGO sheets are employed as an suitable substrate to anchor these nanoparticles against agglomeration. As a consequence, an ultrahigh specific capacitance of 1717 F g−1 at 0.5 A g−1 is achieved. On the other hand, to further facilitate ion transfer within RGO sheets as an ideal electrical double layer capacitor material, the ultra-small Ni(OH)2 nanoparticles are introduced among RGO sheets as the recyclable sacrificial spacer to prevent the stacking. The resulting RGO sheets exhibit superior rate capability with a high capacitance of 182 F g−1 at 100 A g−1. On this basis, an asymmetric supercapacitor is assembled using the two materials, delivering a superior energy density of 75 Wh kg−1 and an ultrahigh power density of 40 000 W kg−1. PMID:26053847

Electrochemical detection of DNA damage induced by acrylamide and its metabolite at the graphene-ionic liquid-Nafion modified pyrolytic graphite electrode.

PubMed

Qiu, Yanyan; Qu, Xiangjin; Dong, Jing; Ai, Shiyun; Han, Ruixia

2011-06-15

A new electrochemical biosensor for directly detecting DNA damage induced by acrylamide (AA) and its metabolite was presented in this work. The graphene-ionic liquid-Nafion modified pyrolytic graphite electrode (PGE) was prepared, and then horseradish peroxidase (HRP) and natural double-stranded DNA were alternately assembled on the modified electrode by the layer-by-layer method. The PGE/graphene-ionic liquid-Nafion and the construction of the (HRP/DNA)(n) film were characterized by electrochemical impedance spectroscopy. With the guanine signal in DNA as an indicator, the damage of DNA was detected by differential pulse voltammetry after PGE/graphene-ionic liquid-Nafion/(HRP/DNA)(n) was incubated in AA solution or AA+H(2)O(2) solution at 37°C. This method provides a new model to mimic and directly detect DNA damage induced by chemical pollutants and their metabolites in vitro. The results indicated that, in the presence of H(2)O(2), HRP was activated and catalyzed the transformation of AA to glycidamide, which could form DNA adducts and induce more serious damage of DNA than AA. In order to further verify these results, UV-vis spectrophotometry was also used to investigate DNA damage induced by AA and its metabolites in solution and the similar results were obtained. Copyright © 2011 Elsevier B.V. All rights reserved.

Interfacial ionic 'liquids': connecting static and dynamic structures.

PubMed

Uysal, Ahmet; Zhou, Hua; Feng, Guang; Lee, Sang Soo; Li, Song; Cummings, Peter T; Fulvio, Pasquale F; Dai, Sheng; McDonough, John K; Gogotsi, Yury; Fenter, Paul

2015-01-28

It is well known that room temperature ionic liquids (RTILs) often adopt a charge-separated layered structure, i.e. with alternating cation- and anion-rich layers, at electrified interfaces. However, the dynamic response of the layered structure to temporal variations in applied potential is not well understood. We used in situ, real-time x-ray reflectivity to study the potential-dependent electric double layer (EDL) structure of an imidazolium-based RTIL on charged epitaxial graphene during potential cycling as a function of temperature. The results suggest that the graphene-RTIL interfacial structure is bistable in which the EDL structure at any intermediate potential can be described by the combination of two extreme-potential structures whose proportions vary depending on the polarity and magnitude of the applied potential. This picture is supported by the EDL structures obtained by fully atomistic molecular dynamics simulations at various static potentials. The potential-driven transition between the two structures is characterized by an increasing width but with an approximately fixed hysteresis magnitude as a function of temperature. The results are consistent with the coexistence of distinct anion- and cation-adsorbed structures separated by an energy barrier (∼0.15 eV).

Supramolecular self-assembly of graphene oxide and metal nanoparticles into stacked multilayers by means of a multitasking protein ring.

PubMed

Ardini, Matteo; Golia, Giordana; Passaretti, Paolo; Cimini, Annamaria; Pitari, Giuseppina; Giansanti, Francesco; Di Leandro, Luana; Ottaviano, Luca; Perrozzi, Francesco; Santucci, Sandro; Morandi, Vittorio; Ortolani, Luca; Christian, Meganne; Treossi, Emanuele; Palermo, Vincenzo; Angelucci, Francesco; Ippoliti, Rodolfo

2016-03-28

Graphene oxide (GO) is rapidly emerging worldwide as a breakthrough precursor material for next-generation devices. However, this requires the transition of its two-dimensional layered structure into more accessible three-dimensional (3D) arrays. Peroxiredoxins (Prx) are a family of multitasking redox enzymes, self-assembling into ring-like architectures. Taking advantage of both their symmetric structure and function, 3D reduced GO-based composites are hereby built up. Results reveal that the "double-faced" Prx rings can adhere flat on single GO layers and partially reduce them by their sulfur-containing amino acids, driving their stacking into 3D multi-layer reduced GO-Prx composites. This process occurs in aqueous solution at a very low GO concentration, i.e. 0.2 mg ml(-1). Further, protein engineering allows the Prx ring to be enriched with metal binding sites inside its lumen. This feature is exploited to both capture presynthesized gold nanoparticles and grow in situ palladium nanoparticles paving the way to straightforward and "green" routes to 3D reduced GO-metal composite materials.

Assessment of bilayer silicene to probe as quantum spin and valley Hall effect

NASA Astrophysics Data System (ADS)

Rehman, Majeed Ur; Qiao, Zhenhua

2018-02-01

Silicene takes precedence over graphene due to its buckling type structure and strong spin orbit coupling. Motivated by these properties, we study the silicene bilayer in the presence of applied perpendicular electric field and intrinsic spin orbit coupling to probe as quantum spin/valley Hall effect. Using analytical approach, we calculate the spin Chern-number of bilayer silicene and then compare it with monolayer silicene. We reveal that bilayer silicene hosts double spin Chern-number as compared to single layer silicene and therefore accordingly has twice as many edge states in contrast to single layer silicene. In addition, we investigate the combined effect of intrinsic spin orbit coupling and the external electric field, we find that bilayer silicene, likewise single layer silicene, goes through a phase transitions from a quantum spin Hall state to a quantum valley Hall state when the strength of the applied electric field exceeds the intrinsic spin orbit coupling strength. We believe that the results and outcomes obtained for bilayer silicene are experimentally more accessible as compared to bilayer graphene, because of strong SO coupling in bilayer silicene.

Edge effects in vertically-oriented graphene based electric double-layer capacitors

NASA Astrophysics Data System (ADS)

Yang, Huachao; Yang, Jinyuan; Bo, Zheng; Zhang, Shuo; Yan, Jianhua; Cen, Kefa

2016-08-01

Vertically-oriented graphenes (VGs) have been demonstrated as a promising active material for electric double-layer capacitors (EDLCs), partially due to their edge-enriched structure. In this work, the 'edge effects', i.e., edges as the promoters of high capacitance, in VG based EDLCs are investigated with experimental research and numerical simulations. VGs with diverse heights (i.e., edge-to-basal ratios) and edge densities are prepared with varying the plasma-enabled growth time and employing different plasma sources. Electrochemical measurements show that the edges play a predominant role on the charge storage behavior of VGs. A simulation is further conducted to unveil the roles of the edges on the separation and adsorption of ions within VG channels. The initial charge distribution of a VG plane is obtained with density functional theory (DFT) calculations, which is subsequently applied to a molecular dynamics (MD) simulation system to gain the insights into the microscope EDLC structures. Compared with the basal planes, the edges present higher initial charge density (by 4.2 times), higher ion packing density (by 2.6 times), closer ion packing location (by 0.8 Å), and larger ion separation degree (by 14%). The as-obtained findings will be instructive in designing the morphology and structure of VGs for enhanced capacitive performances.

Development of efficient electrocatalysts via molecular hybridization of NiMn layered double hydroxide nanosheets and graphene.

PubMed

Ma, Wei; Ma, Renzhi; Wu, Jinghua; Sun, Pengzhan; Liu, Xiaohe; Zhou, Kechao; Sasaki, Takayoshi

2016-05-21

Ni(2+)Mn(3+) layered double hydroxide (LDH) nanoplatelets have been hydrothermally synthesized in a homogeneous precipitation of mixed Ni(2+)/Mn(2+) salts at a molar ratio of 2 : 1 via the hydrolysis of hexamethylenetetramine (HMT) and in situ oxidation with H2O2. After anion-exchange, NiMn LDH was exfoliated into unilamellar nanosheets. Subsequent flocculation of NiMn LDH nanosheets with (reduced) graphene oxide (GO/rGO) into superlattice composites was achieved and further tested as electrocatalysts for oxygen evolution reaction (OER). The face-to-face heteroassembly of NiMn LDH nanosheets with conductive rGO at an alternating sequence resulted in a small overpotential of 0.26 V and a Tafel slope of 46 mV per decade, which is much superior to as-exfoliated nanosheets. The analyses of electrochemical activity surface area (ECSA) and impedance spectra clearly indicated that the superlattice structure was ideal in facilitating the migration/transfer of the charge and reactants, revealing the electrochemical energetics and mechanism behind the synergistic effect arising from molecular hybridization. The proof of concept toward total water splitting using the newly developed hybrid electrocatalyst was demonstrated by an electrolysis cell powered by a single AA battery.

Preparation of graphene foam with high performance by modified self-assembly method

NASA Astrophysics Data System (ADS)

Zhang, Wenhui; Sun, Youyi; Liu, Tantan; Li, Diansen; Hou, Chunlin; Gao, Li; Liu, Yaqing

2016-03-01

Recently, self-assembly method was applied for preparation of graphene foam. However, it is still a great challenge to obtain a three-dimensional graphene network with high performance (e.g., low density, high mechanical strength and high conductivity together) for the self-assembly method. Herein, a modified self-assembly method applied for preparation of graphene foam was investigated, in which, L-ascorbic acid and HI were firstly chosen as the reducing agent, and further reduced by hydrazine hydrate. The results demonstrated that the graphene foam showed high compressive strength (ca. 320 kPa), high electrical conductivity (20.6 S/m) and low density (14.7 mg/cm-1). Especially, the obtained compressive strength (ca. 320 kPa) is the highest value compared to the data of graphene foam reported in previous works. This phenomenon may be due to following three reasons: (1) the reaction between hydrazine hydrate and graphene brought some covalent bonds among graphene sheets; (2) graphene foam was achieved by high hydrophobicity and electrostatic repulsion which inhibit the restacking of graphene sheets; (3) the removal of the oxygen groups by hydrazine hydrate efficiently restores conjugation of sp2 regions and the π-π interaction in the cross-linking sites, which tightly bonds the sheets together. The obtained graphene foam not only had good porous structure and mechanical strength, but also showed excellent satisfactory double-layer capacitive behavior with good electrochemical cyclic stability and high specific capacitance of 171.0 F/g for application in electrode of supercapacitors and absorption capacities for the removal of various oils and dyes from water.

Graphene interfaced perovskite solar cells: Role of graphene flake size

NASA Astrophysics Data System (ADS)

Sakorikar, Tushar; Kavitha, M. K.; Tong, Shi Wun; Vayalamkuzhi, Pramitha; Loh, Kian Ping; Jaiswal, Manu

2018-04-01

Graphene interfaced inverted planar heterojunction perovskite solar cells are fabricated by facile solution method and studied its potential as hole conducting layer. Reduced graphene oxide (rGO) with small and large flake size and Polyethylenedioxythiophene:polystyrene sulfonate (PEDOT:PSS) are utilized as hole conducting layers in different devices. For the solar cell employing PEDOT:PSS as hole conducting layer, 3.8 % photoconversion efficiency is achieved. In case of solar cells fabricated with rGO as hole conducting layer, the efficiency of the device is strongly dependent on flake size. With all other fabrication conditions kept constant, the efficiency of graphene-interfaced solar cell improves by a factor of 6, by changing the flake size of graphene oxide. We attribute this effect to uniform coverage of graphene layer and improved electrical percolation network.

The optical properties of transferred graphene and the dielectrics grown on it obtained by ellipsometry

NASA Astrophysics Data System (ADS)

Kasikov, Aarne; Kahro, Tauno; Matisen, Leonard; Kodu, Margus; Tarre, Aivar; Seemen, Helina; Alles, Harry

2018-04-01

Graphene layers grown by chemical vapour deposition (CVD) method and transferred from Cu-foils to the oxidized Si-substrates were investigated by spectroscopic ellipsometry (SE), Raman and X-Ray Photoelectron Spectroscopy (XPS) methods. The optical properties of transferred CVD graphene layers do not always correspond to the ones of the exfoliated graphene due to the contamination from the chemicals used in the transfer process. However, the real thickness and the mean properties of the transferred CVD graphene layers can be found using ellipsometry if a real thickness of the SiO2 layer is taken into account. The pulsed laser deposition (PLD) and atomic layer deposition (ALD) methods were used to grow dielectric layers on the transferred graphene and the obtained structures were characterized using optical methods. The approach demonstrated in this work could be useful for the characterization of various materials grown on graphene.

Preparation and electrical transport properties of quasi free standing bilayer graphene on SiC (0001) substrate by H intercalation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yu, Cui; Liu, Qingbin; Li, Jia

2014-11-03

We investigate the temperature dependent electrical transport properties of quasi-free standing bilayer graphene on 4H-SiC (0001) substrate. Three groups of monolayer epitaxial graphene and corresponding quasi-free standing bilayer graphene with different crystal quality and layer number homogeneity are prepared. Raman spectroscopy and atomic-force microscopy are used to obtain their morphologies and layer number, and verify the complete translation of buffer layer into graphene. The highest room temperature mobility reaches 3700 cm{sup 2}/V·s for the quasi-free standing graphene. The scattering mechanism analysis shows that poor crystal quality and layer number inhomogeneity introduce stronger interacting of SiC substrate to the graphene layer andmore » more impurities, which limit the carrier mobility of the quasi-free standing bilayer graphene samples.« less

Ultrahard carbon film from epitaxial two-layer graphene

NASA Astrophysics Data System (ADS)

Gao, Yang; Cao, Tengfei; Cellini, Filippo; Berger, Claire; de Heer, Walter A.; Tosatti, Erio; Riedo, Elisa; Bongiorno, Angelo

2018-02-01

Atomically thin graphene exhibits fascinating mechanical properties, although its hardness and transverse stiffness are inferior to those of diamond. So far, there has been no practical demonstration of the transformation of multilayer graphene into diamond-like ultrahard structures. Here we show that at room temperature and after nano-indentation, two-layer graphene on SiC(0001) exhibits a transverse stiffness and hardness comparable to diamond, is resistant to perforation with a diamond indenter and shows a reversible drop in electrical conductivity upon indentation. Density functional theory calculations suggest that, upon compression, the two-layer graphene film transforms into a diamond-like film, producing both elastic deformations and sp2 to sp3 chemical changes. Experiments and calculations show that this reversible phase change is not observed for a single buffer layer on SiC or graphene films thicker than three to five layers. Indeed, calculations show that whereas in two-layer graphene layer-stacking configuration controls the conformation of the diamond-like film, in a multilayer film it hinders the phase transformation.

First-principles simulations of Graphene/Transition-metal-Dichalcogenides/Graphene Field-Effect Transistor

NASA Astrophysics Data System (ADS)

Li, Xiangguo; Wang, Yun-Peng; Zhang, X.-G.; Cheng, Hai-Ping

A prototype field-effect transistor (FET) with fascinating properties can be made by assembling graphene and two-dimensional insulating crystals into three-dimensional stacks with atomic layer precision. Transition metal dichalcogenides (TMDCs) such as WS2, MoS2 are good candidates for the atomically thin barrier between two layers of graphene in the vertical FET due to their sizable bandgaps. We investigate the electronic properties of the Graphene/TMDCs/Graphene sandwich structure using first-principles method. We find that the effective tunnel barrier height of the TMDC layers in contact with the graphene electrodes has a layer dependence and can be modulated by a gate voltage. Consequently a very high ON/OFF ratio can be achieved with appropriate number of TMDC layers and a suitable range of the gate voltage. The spin-orbit coupling in TMDC layers is also layer dependent but unaffected by the gate voltage. These properties can be important in future nanoelectronic device designs. DOE/BES-DE-FG02-02ER45995; NERSC.

Evaluating Graphene as a Channel Material in Spintronic Logic Devices

NASA Astrophysics Data System (ADS)

Anugrah, Yoska

Spintronics, a class of devices that exploit the spin properties of electrons in addition to the charge properties, promises the possibility for nonvolatile logic and memory devices that operate at low power. Graphene is a material in which the spin orientation of electrons can be conserved over a long distance, which makes it an attractive channel material in spintronics devices. In this dissertation, the properties of graphene that are interesting for spintronics applications are explored. A robust fabrication process is described for graphene spin valves using Al2O3 tunnel tunnel barriers and Co ferromagnetic contacts. Spin transport was characterized in both few-layer exfoliated and single-layer graphene, and spin diffusion lengths and spin relaxation times were extracted using the nonlocal spin valve geometry and Hanle measurements. The effect of input-output asymmetry on the spin transport was investigated. The effect of an applied drift electric field on spin transport was investigated and the spin diffusion length was found to be tunable by a factor of 8X (suppressed to 1.6 microm and enhanced to 13 microm from the intrinsic length of 4.6 microm using electric field of +/-1800 V/cm). A mechanism to induce asymmetry without excess power dissipation is also described which utilizes a double buried-gate structure to tune the Fermi levels on the input and output sides of a graphene spin logic device independently. It was found that different spin scattering mechanisms were at play in the two halves of a small graphene strip. This suggests that the spin properties of graphene are strongly affected by its local environment, e.g. impurities, surface topography, defects. Finally, two-dimensional materials beyond graphene have been explored as spin channels. One such material is phosphorene, which has low spin-orbit coupling and high mobility, and the interface properties of ferromagnets (cobalt and permalloy) with this material were explored. This work could potentially enable spin injection without the need for a physical tunnel barrier to solve the conductivity mismatch problem inherent to graphene.

Enhanced model for determining the number of graphene layers and their distribution from X-ray diffraction data

PubMed Central

Ademi, Abdulakim; Grozdanov, Anita; Paunović, Perica; Dimitrov, Aleksandar T

2015-01-01

Summary A model consisting of an equation that includes graphene thickness distribution is used to calculate theoretical 002 X-ray diffraction (XRD) peak intensities. An analysis was performed upon graphene samples produced by two different electrochemical procedures: electrolysis in aqueous electrolyte and electrolysis in molten salts, both using a nonstationary current regime. Herein, the model is enhanced by a partitioning of the corresponding 2θ interval, resulting in significantly improved accuracy of the results. The model curves obtained exhibit excellent fitting to the XRD intensities curves of the studied graphene samples. The employed equation parameters make it possible to calculate the j-layer graphene region coverage of the graphene samples, and hence the number of graphene layers. The results of the thorough analysis are in agreement with the calculated number of graphene layers from Raman spectra C-peak position values and indicate that the graphene samples studied are few-layered. PMID:26665083

Parametric Investigation of the Isothermal Kinetics of Growth of Graphene on a Nickel Catalyst in the Process of Chemical Vapor Deposition of Hydrocarbons

NASA Astrophysics Data System (ADS)

Futko, S. I.; Shulitskii, B. G.; Labunov, V. A.; Ermolaeva, E. M.

2016-11-01

A kinetic model of isothermal synthesis of multilayer graphene on the surface of a nickel foil in the process of chemical vapor deposition, on it, of hydrocarbons supplied in the pulsed regime is considered. The dependences of the number of graphene layers formed and the time of their growth on the temperature of the process, the concentration of acetylene, and the thickness of the nickel foil were calculated. The regime parameters of the process of chemical vapor deposition, at which single-layer graphene and bi-layer graphene are formed, were determined. The dynamics of growth of graphene domains at chemical-vapor-deposition parameters changing in wide ranges was investigated. It is shown that the time dependences of the rates of growth of single-layer graphene and bi-layer graphene are nonlinear in character and that they are determined by the kinetics of nucleation and growth of graphene and the diffusion flow of carbon atoms in the nickel foil.

Precise Control of the Number of Layers of Graphene by Picosecond Laser Thinning.

PubMed

Lin, Zhe; Ye, Xiaohui; Han, Jinpeng; Chen, Qiao; Fan, Peixun; Zhang, Hongjun; Xie, Dan; Zhu, Hongwei; Zhong, Minlin

2015-06-26

The properties of graphene can vary as a function of the number of layers (NOL). Controlling the NOL in large area graphene is still challenging. In this work, we demonstrate a picosecond (ps) laser thinning removal of graphene layers from multi-layered graphene to obtain desired NOL when appropriate pulse threshold energy is adopted. The thinning process is conducted in atmosphere without any coating and it is applicable for graphene films on arbitrary substrates. This method provides many advantages such as one-step process, non-contact operation, substrate and environment-friendly, and patternable, which will enable its potential applications in the manufacturing of graphene-based electronic devices.

Precise Control of the Number of Layers of Graphene by Picosecond Laser Thinning

NASA Astrophysics Data System (ADS)

Lin, Zhe; Ye, Xiaohui; Han, Jinpeng; Chen, Qiao; Fan, Peixun; Zhang, Hongjun; Xie, Dan; Zhu, Hongwei; Zhong, Minlin

2015-06-01

The properties of graphene can vary as a function of the number of layers (NOL). Controlling the NOL in large area graphene is still challenging. In this work, we demonstrate a picosecond (ps) laser thinning removal of graphene layers from multi-layered graphene to obtain desired NOL when appropriate pulse threshold energy is adopted. The thinning process is conducted in atmosphere without any coating and it is applicable for graphene films on arbitrary substrates. This method provides many advantages such as one-step process, non-contact operation, substrate and environment-friendly, and patternable, which will enable its potential applications in the manufacturing of graphene-based electronic devices.

Supramolecular self-assembly of graphene oxide and metal nanoparticles into stacked multilayers by means of a multitasking protein ring

NASA Astrophysics Data System (ADS)

Ardini, Matteo; Golia, Giordana; Passaretti, Paolo; Cimini, Annamaria; Pitari, Giuseppina; Giansanti, Francesco; Leandro, Luana Di; Ottaviano, Luca; Perrozzi, Francesco; Santucci, Sandro; Morandi, Vittorio; Ortolani, Luca; Christian, Meganne; Treossi, Emanuele; Palermo, Vincenzo; Angelucci, Francesco; Ippoliti, Rodolfo

2016-03-01

Graphene oxide (GO) is rapidly emerging worldwide as a breakthrough precursor material for next-generation devices. However, this requires the transition of its two-dimensional layered structure into more accessible three-dimensional (3D) arrays. Peroxiredoxins (Prx) are a family of multitasking redox enzymes, self-assembling into ring-like architectures. Taking advantage of both their symmetric structure and function, 3D reduced GO-based composites are hereby built up. Results reveal that the ``double-faced'' Prx rings can adhere flat on single GO layers and partially reduce them by their sulfur-containing amino acids, driving their stacking into 3D multi-layer reduced GO-Prx composites. This process occurs in aqueous solution at a very low GO concentration, i.e. 0.2 mg ml-1. Further, protein engineering allows the Prx ring to be enriched with metal binding sites inside its lumen. This feature is exploited to both capture presynthesized gold nanoparticles and grow in situ palladium nanoparticles paving the way to straightforward and ``green'' routes to 3D reduced GO-metal composite materials.Graphene oxide (GO) is rapidly emerging worldwide as a breakthrough precursor material for next-generation devices. However, this requires the transition of its two-dimensional layered structure into more accessible three-dimensional (3D) arrays. Peroxiredoxins (Prx) are a family of multitasking redox enzymes, self-assembling into ring-like architectures. Taking advantage of both their symmetric structure and function, 3D reduced GO-based composites are hereby built up. Results reveal that the ``double-faced'' Prx rings can adhere flat on single GO layers and partially reduce them by their sulfur-containing amino acids, driving their stacking into 3D multi-layer reduced GO-Prx composites. This process occurs in aqueous solution at a very low GO concentration, i.e. 0.2 mg ml-1. Further, protein engineering allows the Prx ring to be enriched with metal binding sites inside its lumen. This feature is exploited to both capture presynthesized gold nanoparticles and grow in situ palladium nanoparticles paving the way to straightforward and ``green'' routes to 3D reduced GO-metal composite materials. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr08632a

Metal-doped graphene layers composed with boron nitride-graphene as an insulator: a nano-capacitor.

PubMed

Monajjemi, Majid

2014-11-01

A model of a nanoscale dielectric capacitor composed of a few dopants has been investigated in this study. This capacitor includes metallic graphene layers which are separated by an insulating medium containing a few h-BN layers. It has been observed that the elements from group IIIA of the periodic table are more suitable as dopants for hetero-structures of the {metallic graphene/hBN/metallic graphene} capacitors compared to those from groups IA or IIA. In this study, we have specifically focused on the dielectric properties of different graphene/h-BN/graphene including their hetero-structure counterparts, i.e., Boron-graphene/h-BN/Boron-graphene, Al-graphene/h-BN/Al-graphene, Mg-graphene/h-BN/Mg-graphene, and Be-graphene/h-BN/Be-graphene stacks for monolayer form of dielectrics. Moreover, we studied the multi dielectric properties of different (h-BN)n/graphene hetero-structures of Boron-graphene/(h-BN)n/Boron-graphene.

Three-dimensional reduced graphene oxide/polyaniline nanocomposite film prepared by diffusion driven layer-by-layer assembly for high-performance supercapacitors

NASA Astrophysics Data System (ADS)

Hong, Xiaodong; Zhang, Binbin; Murphy, Elizabeth; Zou, Jianli; Kim, Franklin

2017-03-01

As a simple and versatile method, diffusion driven Layer-by-Layer assembly (dd-LbL) is developed to assemble graphene oxide (GO) into three-dimensional (3D) structure. The assembled GO macrostructure can be reduced through a hydrothermal treatment and used as a high volumetric capacitance electrode in supercapacitors. In this report we use rGO framework created from dd-LbL as a scaffold for in situ polymerization of aniline within the pores of the framework to form rGO/polyaniline (rGO/PANI) composite. The rGO/PANI composite affords a robust and porous structure, which facilitates electrolyte diffusion and exhibits excellent electrochemical performance as binder-free electrodes in a sandwich-configuration supercapacitor. Combining electric double layer capacitance and pseudo-capacitance, rGO/PANI electrodes exhibit a specific capacitance of 438.8 F g-1 at discharge rate of 5 mA (mass of electrodes were 10.0 mg, 0.5 A g-1) in 1 mol L-1 H2SO4 electrolyte; furthermore, the generated PANI nanoparticles in rGO template achieve a higher capacitance of 763 F g-1. The rGO/PANI composite electrodes also show an improved recyclability, 76.5% of capacitance retains after recycled 2000 times.

Two-dimensional layered semiconductor/graphene heterostructures for solar photovoltaic applications.

PubMed

Shanmugam, Mariyappan; Jacobs-Gedrim, Robin; Song, Eui Sang; Yu, Bin

2014-11-07

Schottky barriers formed by graphene (monolayer, bilayer, and multilayer) on 2D layered semiconductor tungsten disulfide (WS2) nanosheets are explored for solar energy harvesting. The characteristics of the graphene-WS2 Schottky junction vary significantly with the number of graphene layers on WS2, resulting in differences in solar cell performance. Compared with monolayer or stacked bilayer graphene, multilayer graphene helps in achieving improved solar cell performance due to superior electrical conductivity. The all-layered-material Schottky barrier solar cell employing WS2 as a photoactive semiconductor exhibits efficient photon absorption in the visible spectral range, yielding 3.3% photoelectric conversion efficiency with multilayer graphene as the Schottky contact. Carrier transport at the graphene/WS2 interface and the interfacial recombination process in the Schottky barrier solar cells are examined.

Interface and interaction of graphene layers on SiC(0001[combining macron]) covered with TiC(111) intercalation.

PubMed

Wang, Lu; Wang, Qiang; Huang, Jianmei; Li, Wei-Qi; Chen, Guang-Hui; Yang, Yanhui

2017-10-11

It is important to understand the interface and interaction between the graphene layer, titanium carbide [TiC(111)] interlayer, and silicon carbide [SiC(0001[combining macron])] substrates in epitaxial growth of graphene on silicon carbide (SiC) substrates. In this study, the fully relaxed interfaces which consist of up to three layers of TiC(111) coatings on the SiC(0001[combining macron]) as well as the graphene layers interactions with these TiC(111)/SiC(0001[combining macron]) were systematically studied using the density functional theory-D2 (DFT-D2) method. The results showed that the two layers of TiC(111) coating with the C/C-terminated interfaces were thermodynamically more favorable than one or three layers of TiC(111) on the SiC(0001[combining macron]). Furthermore, the bonding of the Ti-hollow-site stacked interfaces would be a stronger link than that of the Ti-Fcc-site stacked interfaces. However, the formation of the C/Ti/C and Ti/C interfaces implied that the first upper carbon layer can be formed on TiC(111)/SiC(0001[combining macron]) using the decomposition of the weaker Ti-C and C-Si interfacial bonds. When growing graphene layers on these TiC(111)/SiC(0001[combining macron]) substrates, the results showed that the interaction energy depended not only on the thickness of the TiC(111) interlayer, but also on the number of graphene layers. Bilayer graphene on the two layer thick TiC(111)/SiC(0001[combining macron]) was thermodynamically more favorable than a monolayer or trilayer graphene on these TiC(111)/SiC(0001[combining macron]) substrates. The adsorption energies of the bottom graphene layers with the TiC(111)/SiC(0001[combining macron]) substrates increased with the decrease of the interface vertical distance. The interaction energies between the bottom, second and third layers of graphene on the TiC(111)/SiC(0001[combining macron]) were significantly higher than that of the freestanding graphene layers. All of these findings provided insight into the growth of epitaxial graphene on TiC(111)/SiC(0001[combining macron]) substrates and the design of graphene/TiC/SiC-based electronic devices.

Tailoring graphene-based electrodes from semiconducting to metallic to increase the energy density in supercapacitors

NASA Astrophysics Data System (ADS)

Vatamanu, Jenel; Ni, Xiaojuan; Liu, Feng; Bedrov, Dmitry

2015-11-01

The semiconducting character of graphene and some carbon-based electrodes can lead to noticeably lower total capacitances and stored energy densities in electric double layer (EDL) capacitors. This paper discusses the chemical and electronic structure modifications that enhance the available energy bands, density of states and quantum capacitance of graphene substrates near the Fermi level, therefore restoring the conducting character of these materials. The doping of graphene with p or n dopants, such as boron and nitrogen atoms, or the introduction of vacancy defects that introduce zigzag edges, can significantly increase the quantum capacitance within the potential range of interest for the energy storage applications by either shifting the Dirac point away from the Fermi level or by eliminating the Dirac point. We show that a combination of doping and vacancies at realistic concentrations is sufficient to increase the capacitance of a graphene-based electrode to within 1 μF cm-2 from that of a metallic surface. Using a combination of ab initio calculations and classical molecular dynamics simulations we estimate how the changes in the quantum capacitance of these electrode materials affect the total capacitance stored by the open structure EDL capacitors containing room temperature ionic liquid electrolytes.

Efficient small molecular organic light emitting diode with graphene cathode covered by a Sm layer with nano-hollows and n-doped by Bphen:Cs2CO3 in the hollows

NASA Astrophysics Data System (ADS)

Yao, Li; Li, Lei; Qin, Laixiang; Ma, Yaoguang; Wang, Wei; Meng, Hu; Jin, Weifeng; Wang, Yilun; Xu, Wanjin; Ran, Guangzhao; You, Liping; Qin, Guogang

2017-03-01

Graphene is a favorable candidate for electrodes of organic light emitting diodes (OLEDs). Graphene has quite a high work function of ˜4.5 eV, and has been extensively studied when used as anodes of OLEDs. In order to use graphene as a cathode, the electron injection barrier between the graphene cathode and the electron transport layer has to be low enough. Using 4,7-diphenyl-1,10-phenanthroline (Bphen):Cs2CO3 to n-dope graphene is a very good method, but the electron injection barrier between the n-doped graphene and Bphen:Cs2CO3 is still too high to be ˜1.0 eV. In this work, in order to further reduce the electron injection barrier, a novel method is suggested. On the graphene cathode, a Sm layer with a lot of nano-hollows, and subsequently a layer of Bphen:Cs2CO3, are deposited. The Bphen:Cs2CO3 can n-dope graphene in the nano-hollows, and the Fermi level of the graphene rises. The nano Sm layer is very easily oxidized. Oxygen adsorbed on the surface of graphene may react with Sm to form an O--Sm+ dipole layer. On the areas of the Sm oxide dipole layer without nano-hollows, the electron injection barrier can be further lowered by the dipole layer. Electrons tend to mainly inject through the lower electron barrier where the dipole layer exists. Based on this idea, an effective inverted small molecular OLED with the structure of graphene/1 nm Sm layer with a lot of nano-hollows/Bphen:Cs2CO3/Alq3:C545T/NPB/MoO3/Al is presented. The maximum current efficiency and maximum power efficiency of the OLED with a 1 nm Sm layer are about two and three times of those of the reference OLED without any Sm layer, respectively.

Self assembled multi-layer nanocomposite of graphene and metal oxide materials

DOEpatents

Liu, Jun; Aksay, Ilhan A; Choi, Daiwon; Kou, Rong; Nie, Zimin; Wang, Donghai; Yang, Zhenguo

2013-10-22

Nanocomposite materials having at least two layers, each layer consisting of one metal oxide bonded to at least one graphene layer were developed. The nanocomposite materials will typically have many alternating layers of metal oxides and graphene layers, bonded in a sandwich type construction and will be incorporated into an electrochemical or energy storage device.

Self assembled multi-layer nanocomposite of graphene and metal oxide materials

DOEpatents

Liu, Jun; Aksay, Ilhan A; Choi, Daiwon; Kou, Rong; Nie, Zimin; Wang, Donghai; Yang, Zhenguo

2015-04-28

Nanocomposite materials having at least two layers, each layer consisting of one metal oxide bonded to at least one graphene layer were developed. The nanocomposite materials will typically have many alternating layers of metal oxides and graphene layers, bonded in a sandwich type construction and will be incorporated into an electrochemical or energy storage device.

Self assembled multi-layer nanocomposite of graphene and metal oxide materials

DOEpatents

Liu, Jun; Choi, Daiwon; Kou, Rong; Nie, Zimin; Wang, Donghai; Yang, Zhenguo

2014-09-16

Nanocomposite materials having at least two layers, each layer consisting of one metal oxide bonded to at least one graphene layer were developed. The nanocomposite materials will typically have many alternating layers of metal oxides and graphene layers, bonded in a sandwich type construction and will be incorporated into an electrochemical or energy storage device.

New X-ray insight into oxygen intercalation in epitaxial graphene grown on 4H-SiC(0001)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kowalski, G., E-mail: kowal@fuw.edu.pl; Tokarczyk, M.; Dąbrowski, P.

Efficient control of intercalation of epitaxial graphene by specific elements is a way to change properties of the graphene. Results of several experimental techniques, such as X-ray photoelectron spectroscopy, micro-Raman mapping, reflectivity, attenuated total reflection, X-ray diffraction, and X-ray reflectometry, gave a new insight into the intercalation of oxygen in the epitaxial graphene grown on 4H-SiC(0001). These results confirmed that oxygen intercalation decouples the graphene buffer layer from the 4H-SiC surface and converts it into the graphene layer. However, in contrast to the hydrogen intercalation, oxygen does not intercalate between carbon planes (in the case of few layer graphene) andmore » the interlayer spacing stays constant at the level of 3.35–3.32 Å. Moreover, X-ray reflectometry showed the presence of an oxide layer having the thickness of about 0.8 Å underneath the graphene layers. Apart from the formation of the nonuniform thin oxide layer, generation of defects in graphene caused by oxygen was also evidenced. Last but not least, water islands underneath defected graphene regions in both intercalated and non-intercalated samples were most probably revealed. These water islands are formed in the case of all the samples stored under ambient laboratory conditions. Water islands can be removed from underneath the few layer graphene stacks by relevant thermal treatment or by UV illumination.« less

The impact of hydrogen and oxidizing impurities in chemical vapor deposition of graphene on copper

NASA Astrophysics Data System (ADS)

Choubak, Saman

Graphene, the single-atom layer of carbon, has attracted scientists and technologists due to its outstanding physical and opto/electronic properties. The use of graphene in practical applications requires a reliable and cost-effective method to produce large area graphene films with low defects and controlled thicknesses. Direct growth of graphene using chemical vapor deposition (CVD) on copper, in which carbonaceous gaseous species react with the metal substrate in the presence of hydrogen at high temperatures (850-1100° C), led to high coverage of high quality graphene, opening up a promising future for methods of this type and a large step towards commercial realization of graphene products. The present thesis deals with the synthesis of graphene via low pressure CVD (LP-CVD) on copper catalyst using methane as the carbon precursor. The focus is mainly on the determination of the role of hydrogen and oxidizing impurities during graphene formation with an ultimate purpose: to elucidate a viable and reproducible method for the production of high quality graphene films compatible with industrial manufacturing processes. The role of molecular hydrogen in graphene CVD is explored in the first part of the thesis. Few studies claimed that molecular hydrogen etches graphene films on copper by conducting annealing experiments. On the other hand, we speculated that this graphene etching reaction is due to the presence of trace amount of oxygen in the furnace atmosphere. Thus, we took another approach and designed systematic annealing experiments to investigate the role of hydrogen in the etching reaction of graphene on copper foils. No evidence of graphene etching on copper was observed when purified ultra high purity (UHP) hydrogen was used at 825 °C and 500 mTorr. Nevertheless, graphene films exposed to the unpurified UHP hydrogen were etched due to the presence of oxidizing impurities. Our results show that hydrogen is not responsible for graphene etching reaction and oxygen impurities are the main cause of this etching reaction. We have also determined that graphene etching reaction is catalyzed by the copper surface. Next, we systematically investigated the role that hydrogen plays during the growth and coolingdown stage of LP-CVD of graphene on copper. We show that a flow of CH4/H2 is necessary during cooling for preventing graphene etching likely by the means of a competitive action with carbon growth. After graphene formation, the film can be preserved from detrimental effect of oxygen in the absence of methane by its exposure to purified ultra high purity (UHP) hydrogen flow during cooling. In conditions where the level of oxidizing impurities is low, we have obtained continuous and uniform graphene films using solely purified methane (O2<1ppbV) serving a double role as a copper oxide reducer and carbon supply for the growth in the absence of hydrogen gas. This result shows that the presence of hydrogen is not necessary for graphene growth in a controlled atmosphere. Differences in graphene film morphology in purified conditions, where the level of oxidizing impurities is low (O2<1ppb) compare to standard conditions (O2<1ppm), have also been observed. A larger bilayer and multilayer coverage was noticed when only purified methane was used. These bi- and multi-layer graphene islands appeared to be twisted with respect to the first graphene layer. These overall results suggest a different graphene growth behavior in purified and controlled conditions. Having investigated and understood the role of hydrogen and oxidizing impurities in LP-CVD of graphene on copper, we show a rapid and efficient growth of continuous monolayer graphene on copper within 1 min. This was achieved by minimizing the presence of oxidizing impurities with using gas purifiers installed on the gas lines and maintaining a flow of purified UHP hydrogen during the cooling down stage. With this method, we have reduced the graphene growth process time between 5 to 45 times compared to the current recipes in literature. Note that the installation of gas purifiers is entirely compatible with industrial manufacturing processes and is extremely profitable since it can lower graphene production cost by reducing process time and saving energy. Moreover, the crystalline quality and uniformity of the graphene films, determined by Raman spectroscopy and Scanning Electron Microscopy, stayed similar even at this short growth time. Lastly, by gathering all the results during the evolution of this thesis, we notice that graphene multilayer growth is mainly occurring in highly purified conditions and most importantly when a flow of methane gas is present during the cool down stage. Based on these observations, a significant number of bi/multi layer formation can potentially arise when graphene is completed in the cooling stage. These results, although preliminary, point toward the influence of the cooling stage on graphene bi/multi layer formation. The collection of our results presented in this thesis show that oxidizing impurities play a significant role in graphene LP-CVD and explain inconsistencies between growth recipes reported in the literature. They also provide a rational about the need to control the balance between oxygen and hydrogen pressures, for graphene growth pointing toward a general method for improving graphene layer thickness and uniformity on polycrystalline copper substrates.

Watering Graphene for Devices and Electricity

NASA Astrophysics Data System (ADS)

Guo, Wanlin; Yin, Jun; Li, Xuemei; Zhang, Zhuhua

2013-03-01

Graphene bring us into a fantastic two-dimensional (2D) age of nanotechnology, which can be fabricated and applied at wafer scale, visible at single layer but showing exceptional properties distinguished from its bulk form graphite, linking the properties of atomic layers with the engineering scale of our mankind. We shown that flow-induced-voltage in graphene can be 20 folds higher than in graphite, not only due to the giant Seebeck coefficient of single layer graphene, but also the exceptional interlayer interaction in few layer graphene. Extremely excitingly, water flow over graphene can generate electricity through unexpected interaction of the ions in the water with the graphene. We also find extraordinary mechanical-electric-magnetic coupling effects in graphene and BN systems. Such extraordinary multifield coupling effects in graphene and functional nanosystems open up new vistas in nanotechnology for efficient energy conversion, self-powering flexible devices and novel functional systems.

Enhanced transconductance in a double-gate graphene field-effect transistor

NASA Astrophysics Data System (ADS)

Hwang, Byeong-Woon; Yeom, Hye-In; Kim, Daewon; Kim, Choong-Ki; Lee, Dongil; Choi, Yang-Kyu

2018-03-01

Multi-gate transistors, such as double-gate, tri-gate and gate-all-around transistors are the most advanced Si transistor structure today. Here, a genuine double-gate transistor with a graphene channel is experimentally demonstrated. The top and bottom gates of the double-gate graphene field-effect transistor (DG GFET) are electrically connected so that the conductivity of the graphene channel can be modulated simultaneously by both the top and bottom gate. A single-gate graphene field-effect transistor (SG GFET) with only the top gate is also fabricated as a control device. For systematical analysis, the transfer characteristics of both GFETs were measured and compared. Whereas the maximum transconductance of the SG GFET was 17.1 μS/μm, that of the DG GFET was 25.7 μS/μm, which is approximately a 50% enhancement. The enhancement of the transconductance was reproduced and comprehensively explained by a physics-based compact model for GFETs. The investigation of the enhanced transfer characteristics of the DG GFET in this work shows the possibility of a multi-gate architecture for high-performance graphene transistor technology.

Preparation of graphene by electrical explosion of graphite sticks.

PubMed

Gao, Xin; Xu, Chunxiao; Yin, Hao; Wang, Xiaoguang; Song, Qiuzhi; Chen, Pengwan

2017-08-03

Graphene nanosheets were produced by electrical explosion of high-purity graphite sticks in distilled water at room temperature. The as-prepared samples were characterized by various techniques to find different forms of carbon phases, including graphite nanosheets, few-layer graphene, and especially, mono-layer graphene with good crystallinity. Delicate control of energy injection is critical for graphene nanosheet formation, whereas mono-layer graphene was produced under the charging voltage of 22.5-23.5 kV. On the basis of electrical wire explosion and our experimental results, the underlying mechanism that governs the graphene generation was carefully illustrated. This work provides a simple but innovative route for producing graphene nanosheets.

Reducing the layer number of AB stacked multilayer graphene grown on nickel by annealing at low temperature.

PubMed

Velasco, J Marquez; Giamini, S A; Kelaidis, N; Tsipas, P; Tsoutsou, D; Kordas, G; Raptis, Y S; Boukos, N; Dimoulas, A

2015-10-09

Controlling the number of layers of graphene grown by chemical vapor deposition is crucial for large scale graphene application. We propose here an etching process of graphene which can be applied immediately after growth to control the number of layers. We use nickel (Ni) foil at high temperature (T = 900 °C) to produce multilayer-AB-stacked-graphene (MLG). The etching process is based on annealing the samples in a hydrogen/argon atmosphere at a relatively low temperature (T = 450 °C) inside the growth chamber. The extent of etching is mainly controlled by the annealing process duration. Using Raman spectroscopy we demonstrate that the number of layers was reduced, changing from MLG to few-layer-AB-stacked-graphene and in some cases to randomly oriented few layer graphene near the substrate. Furthermore, our method offers the significant advantage that it does not introduce defects in the samples, maintaining their original high quality. This fact and the low temperature our method uses make it a good candidate for controlling the layer number of already grown graphene in processes with a low thermal budget.

Graphene-coated coupling coil for AC resistance reduction

DOEpatents

Miller, John M

2014-03-04

At least one graphene layer is formed to laterally surround a tube so that the basal plane of each graphene layer is tangential to the local surface of the tube on which the graphene layer is formed. An electrically conductive path is provided around the tube for providing high conductivity electrical path provided by the basal plane of each graphene layer. The high conductivity path can be employed for high frequency applications such as coupling coils for wireless power transmission to overcome skin depth effects and proximity effects prevalent in high frequency alternating current paths.

DC conductivity of twisted bilayer graphene: Angle-dependent transport properties and effects of disorder

NASA Astrophysics Data System (ADS)

Andelković, M.; Covaci, L.; Peeters, F. M.

2018-03-01

The in-plane dc conductivity of twisted bilayer graphene is calculated using an expansion of the real-space Kubo-Bastin conductivity in terms of Chebyshev polynomials. We investigate within a tight-binding approach the transport properties as a function of rotation angle, applied perpendicular electric field, and vacancy disorder. We find that for high-angle twists, the two layers are effectively decoupled, and the minimum conductivity at the Dirac point corresponds to double the value observed in monolayer graphene. This remains valid even in the presence of vacancies, hinting that chiral symmetry is still preserved. On the contrary, for low twist angles, the conductivity at the Dirac point depends on the twist angle and is not protected in the presence of disorder. Furthermore, for low angles and in the presence of an applied electric field, we find that the chiral boundary states emerging between AB and BA regions contribute to the dc conductivity, despite the appearance of localized states in the AA regions. The results agree qualitatively with recent transport experiments in low-angle twisted bilayer graphene.

A Study on Field Emission Characteristics of Planar Graphene Layers Obtained from a Highly Oriented Pyrolyzed Graphite Block

PubMed Central

2009-01-01

This paper describes an experimental study on field emission characteristics of individual graphene layers for vacuum nanoelectronics. Graphene layers were prepared by mechanical exfoliation from a highly oriented pyrolyzed graphite block and placed on an insulating substrate, with the resulting field emission behavior investigated using a nanomanipulator operating inside a scanning electron microscope. A pair of tungsten tips controlled by the nanomanipulator enabled electric connection with the graphene layers without postfabrication. The maximum emitted current from the graphene layers was 170 nA and the turn-on voltage was 12.1 V. PMID:20596315

Stacking sequence and interlayer coupling in few-layer graphene revealed by in situ imaging

PubMed Central

Wang, Zhu-Jun; Dong, Jichen; Cui, Yi; Eres, Gyula; Timpe, Olaf; Fu, Qiang; Ding, Feng; Schloegl, R.; Willinger, Marc-Georg

2016-01-01

In the transition from graphene to graphite, the addition of each individual graphene layer modifies the electronic structure and produces a different material with unique properties. Controlled growth of few-layer graphene is therefore of fundamental interest and will provide access to materials with engineered electronic structure. Here we combine isothermal growth and etching experiments with in situ scanning electron microscopy to reveal the stacking sequence and interlayer coupling strength in few-layer graphene. The observed layer-dependent etching rates reveal the relative strength of the graphene–graphene and graphene–substrate interaction and the resulting mode of adlayer growth. Scanning tunnelling microscopy and density functional theory calculations confirm a strong coupling between graphene edge atoms and platinum. Simulated etching confirms that etching can be viewed as reversed growth. This work demonstrates that real-time imaging under controlled atmosphere is a powerful method for designing synthesis protocols for sp2 carbon nanostructures in between graphene and graphite. PMID:27759024

Role of humidity in reducing the friction of graphene layers on textured surfaces

NASA Astrophysics Data System (ADS)

Li, Zheng-yang; Yang, Wen-jing; Wu, Yan-ping; Wu, Song-bo; Cai, Zhen-bing

2017-05-01

A multiple-layer graphene was prepared on steel surface to reduce friction and wear. A graphene-containing ethanol solution was dripped on the steel surface, and several layers of graphene flakes were deposited on the surface after ethanol evaporated. Tribological performance of graphene-contained surface (GCS) was induced by reciprocating ball against plate contact in different RH (0% (dry nitrogen), 30%, 60%, and 90%). Morphology and wear scar were analyzed by OM, 2D profile, SEM, Raman spectroscopy, and XPS. Results show that GCS can substantially reduce the wear and coefficient of friction (COF) in 60% relative humidity (RH). Low COF occurs due to graphene layer providing a small shear stress on the friction interface. Meanwhile, conditions of high RH and textured surface could make the low COF persist for a longer time. High moisture content can stabilize and protect the graphene C-network from damage due to water dissociative chemisorption with carbon dangling bonds, and the textured surface was attributed to release graphene layer stored in the dimple.

Supercritical fluid extraction of bi & multi-layer graphene sheets from graphite by using exfoliation technique

NASA Astrophysics Data System (ADS)

Xavier, Gauravi; Dave, Bhoomi; Khanna, Sakshum

2018-05-01

In recent times, researchers have turned to explore the possibility of using Supercritical Fluid (SCFs) system to penetrate into the inert-gaping of graphite and exfoliate it into a number of layer graphene sheets. The supercritical fluid holds excellent wetting surfaces with low interfacial tension and high diffusion coefficients. Although SCFs exfoliation approach looks promising to developed large scale & low-cost graphene sheet but has not received much attention. To arouse interest and reflection on this approach, this review is organized to summarize the recent progress in graphene production by SCF technology. Here we present the simplest route to obtained layers of graphene sheets by intercalating and exfoliating graphite using supercritical CO2 processing. The layers graphene nano-sheets were collected in dichloromethane (DCM) solution which prevents the restocking of sheets. The obtained graphene sheets show the desired characteristics and thus can be used in physical, chemical and biological sciences. Thus this method provides an effortless and eco-friendly approach for the synthesis of layers of graphene sheets.

Traditional Semiconductors in the Two-Dimensional Limit.

PubMed

Lucking, Michael C; Xie, Weiyu; Choe, Duk-Hyun; West, Damien; Lu, Toh-Ming; Zhang, S B

2018-02-23

Interest in two-dimensional materials has exploded in recent years. Not only are they studied due to their novel electronic properties, such as the emergent Dirac fermion in graphene, but also as a new paradigm in which stacking layers of distinct two-dimensional materials may enable different functionality or devices. Here, through first-principles theory, we reveal a large new class of two-dimensional materials which are derived from traditional III-V, II-VI, and I-VII semiconductors. It is found that in the ultrathin limit the great majority of traditional binary semiconductors studied (a series of 28 semiconductors) are not only kinetically stable in a two-dimensional double layer honeycomb structure, but more energetically stable than the truncated wurtzite or zinc-blende structures associated with three dimensional bulk. These findings both greatly increase the landscape of two-dimensional materials and also demonstrate that in the double layer honeycomb form, even ordinary semiconductors, such as GaAs, can exhibit exotic topological properties.

A solid dielectric gated graphene nanosensor in electrolyte solutions.

PubMed

Zhu, Yibo; Wang, Cheng; Petrone, Nicholas; Yu, Jaeeun; Nuckolls, Colin; Hone, James; Lin, Qiao

2015-03-23

This letter presents a graphene field effect transistor (GFET) nanosensor that, with a solid gate provided by a high- κ dielectric, allows analyte detection in liquid media at low gate voltages. The gate is embedded within the sensor and thus is isolated from a sample solution, offering a high level of integration and miniaturization and eliminating errors caused by the liquid disturbance, desirable for both in vitro and in vivo applications. We demonstrate that the GFET nanosensor can be used to measure pH changes in a range of 5.3-9.3. Based on the experimental observations and quantitative analysis, the charging of an electrical double layer capacitor is found to be the major mechanism of pH sensing.

Layer-selective synthesis of bilayer graphene via chemical vapor deposition

NASA Astrophysics Data System (ADS)

Yang, Ning; Choi, Kyoungjun; Robertson, John; Park, Hyung Gyu

2017-09-01

A controlled synthesis of high-quality AB-stacked bilayer graphene by chemical vapor deposition demands a detailed understanding of the mechanism and kinetics. By decoupling the growth of the two layers via a growth-and-regrowth scheme, we report the kinetics and termination mechanisms of the bilayer graphene growth on copper. We observe, for the first time, that the secondary layer growth follows Gompertzian kinetics. Our observations affirm the postulate of a time-variant transition from a mass-transport-limited to a reaction-limited regimes and identify the mechanistic disparity between the monolayer growth and the secondary-layer expansion underneath the monolayer cover. It is the continuous carbon supply that drives the expansion of the graphene secondary layer, rather than the initially captured carbon amount, suggesting an essential role of the surface diffusion of reactant adsorbates in the interspace between the top graphene layer and the underneath copper surface. We anticipate that the layer selectivity of the growth relies on the entrance energetics of the adsorbed reactants to the graphene-copper interspace across the primary-layer edge, which could be engineered by tailoring the edge termination state. The temperature-reliant saturation area of the secondary-layer expansion is understood as a result of competitive attachment of carbon and hydrogen adatoms to the secondary-layer graphene edge.

Layer-Dependent Third-Harmonic Generation in Graphene

NASA Astrophysics Data System (ADS)

Yang, Hao; Guan, Honghua; Dadap, Jerry; Osgood, Richard; Richard Osgood Team

Graphene has become a subject of intense interest and study because of its remarkable 2D electronic properties. Multilayer graphene also offers an array of properties that are also of interest for optical physics and devices. Despite its second-order-nonlinear optical response is intrinsically weak, third-order nonlinear optical effects in graphene are symmetry-allowed thus leading to studies of several third-order process in few-layer graphene. In this work, we report third-harmonic generation in multilayer graphene mounted on fused silica and with thicknesses which approach the bulk continuum. THG signals show cubic power dependence with respect to the intensity of fundamental beam. Third-harmonic generation spectroscopy enables a good fit using linear optical detection, which shows strong contrast for different layer number graphene. The maximum THG efficiency appears at layer number around 30. Two models are used for describing this layer dependent phenomenon and shows absorption plays a key role in THG of multilayer graphene. This work also provides a new imaging technology for graphene detection and identification with better contrast and resolution. U.S. Department of Energy under Contract No. DE-FG 02-04-ER-46157.

Methods of fabrication of graphene nanoribbons

DOEpatents

Zhang, Yuegang

2015-06-23

Methods of fabricating graphene nanoribbons include depositing a catalyst layer on a substrate. A masking layer is deposited on the catalyst layer. The masking layer and the catalyst layer are etched to form a structure on the substrate, the structure comprising a portion of the catalyst layer and a portion of the masking layer disposed on the catalyst layer, with sidewalls of the catalyst layer being exposed. A graphene layer is formed on a sidewall of the catalyst layer with a carbon-containing gas.

Role of Defects on Regioselectivity of Nano Pristine Graphene.

PubMed

Kudur Jayaprakash, Gururaj; Casillas, Norberto; Astudillo-Sánchez, Pablo D; Flores-Moreno, Roberto

2016-11-17

Here analytical Fukui functions based on density functional theory are applied to investigate the redox reactivity of pristine and defected graphene lattices. A carbon H-terminated graphene structure (with 96 carbon atoms) and a graphene defected surface with Stone-Wales rearrangement and double vacancy defects are used as models. Pristine sp 2 -hybridized, hexagonal arranged carbon atoms exhibit a symmetric reactivity. In contrast, common carbon atoms at reconstructed polygons in Stone-Wales and double vacancy graphene display large reactivity variations. The improved reactivity and the regioselectivity at defected graphene is correlated to structural changes that caused carbon-carbon bond length variations at defected zones.

Epitaxially Self-Assembled Alkane Layers for Graphene Electronics.

PubMed

Yu, Young-Jun; Lee, Gwan-Hyoung; Choi, Ji Il; Shim, Yoon Su; Lee, Chul-Ho; Kang, Seok Ju; Lee, Sunwoo; Rim, Kwang Taeg; Flynn, George W; Hone, James; Kim, Yong-Hoon; Kim, Philip; Nuckolls, Colin; Ahn, Seokhoon

2017-02-01

The epitaxially grown alkane layers on graphene are prepared by a simple drop-casting method and greatly reduce the environmentally driven doping and charge impurities in graphene. Multiscale simulation studies show that this enhancement of charge homogeneity in graphene originates from the lifting of graphene from the SiO 2 surface toward the well-ordered and rigid alkane self-assembled layers. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Graphene oxide/graphene vertical heterostructure electrodes for highly efficient and flexible organic light emitting diodes

NASA Astrophysics Data System (ADS)

Jia, S.; Sun, H. D.; Du, J. H.; Zhang, Z. K.; Zhang, D. D.; Ma, L. P.; Chen, J. S.; Ma, D. G.; Cheng, H. M.; Ren, W. C.

2016-05-01

The relatively high sheet resistance, low work function and poor compatibility with hole injection layers (HILs) seriously limit the applications of graphene as transparent conductive electrodes (TCEs) for organic light emitting diodes (OLEDs). Here, a graphene oxide/graphene (GO/G) vertical heterostructure is developed as TCEs for high-performance OLEDs, by directly oxidizing the top layer of three-layer graphene films with ozone treatment. Such GO/G heterostructure electrodes show greatly improved optical transmittance, a large work function, high stability, and good compatibility with HIL materials (MoO3 in this work). Moreover, the conductivity of the heterostructure is not sacrificed compared to the pristine three-layer graphene electrodes, but is significantly higher than that of pristine two-layer graphene films. In addition to high flexibility, OLEDs with different emission colors based on the GO/G heterostructure TCEs show much better performance than those based on indium tin oxide (ITO) anodes. Green OLEDs with GO/G heterostructure electrodes have the maximum current efficiency and power efficiency, as high as 82.0 cd A-1 and 98.2 lm W-1, respectively, which are 36.7% (14.8%) and 59.2% (15.0%) higher than those with pristine graphene (ITO) anodes. These findings open up the possibility of using graphene for next generation high-performance flexible and wearable optoelectronics with high stability.The relatively high sheet resistance, low work function and poor compatibility with hole injection layers (HILs) seriously limit the applications of graphene as transparent conductive electrodes (TCEs) for organic light emitting diodes (OLEDs). Here, a graphene oxide/graphene (GO/G) vertical heterostructure is developed as TCEs for high-performance OLEDs, by directly oxidizing the top layer of three-layer graphene films with ozone treatment. Such GO/G heterostructure electrodes show greatly improved optical transmittance, a large work function, high stability, and good compatibility with HIL materials (MoO3 in this work). Moreover, the conductivity of the heterostructure is not sacrificed compared to the pristine three-layer graphene electrodes, but is significantly higher than that of pristine two-layer graphene films. In addition to high flexibility, OLEDs with different emission colors based on the GO/G heterostructure TCEs show much better performance than those based on indium tin oxide (ITO) anodes. Green OLEDs with GO/G heterostructure electrodes have the maximum current efficiency and power efficiency, as high as 82.0 cd A-1 and 98.2 lm W-1, respectively, which are 36.7% (14.8%) and 59.2% (15.0%) higher than those with pristine graphene (ITO) anodes. These findings open up the possibility of using graphene for next generation high-performance flexible and wearable optoelectronics with high stability. Electronic supplementary information (ESI) available: XPS spectra, Raman spectra, sheet resistance and transmittance of graphene films with different numbers of layers and different ozone treatment times, doping effect of MoO3 on graphene and GO/G electrodes, performance of green OLEDs with different graphene anodes, a movie showing the flexibility of device. See DOI: 10.1039/c6nr01649a

Bonding between graphene and MoS 2 monolayers without and with Li intercalation

DOE PAGES

Ahmed, Towfiq; Modine, N. A.; Zhu, Jian-Xin

2015-07-27

We performed density functional theory (DFT) calculations for a bi-layered heterostructure combining a graphene layer with a MoS 2 layer with and without intercalated Li atoms. Our calculations demonstrate the importance of the van der Waals (vdW) interaction, which is crucial for forming stable bonding between the layers. Our DFT calculation correctly reproduces the linear dispersion, or Dirac cone, feature at the Fermi energy for the isolated graphene monolayer and the band gap for the MoS 2 monolayer. For the combined graphene/MoS 2 bi-layer, we observe interesting electronic structure and density of states (DOS) characteristics near the Fermi energy, showingmore » both the gap like features of the MoS 2 layer and in-gap states with linear dispersion contributed mostly by the graphene layer. Our calculated total DOS in this vdW heterostructure reveals that the graphene layer significantly contributes to pinning the Fermi energy at the center of the band gap of MoS 2. We also find that intercalating Li ions in between the layers of the graphene/MoS2 heterostructure enhances the binding energy through orbital hybridizations between cations (Li adatoms) and anions (graphene and MoS 2 monolayers). Moreover, we calculate the dielectric function of the Li intercalated graphene/MoS 2 heterostructure, the imaginary component of which can be directly compared with experimental measurements of optical conductivity in order to validate our theoretical prediction. We observe sharp features in the imaginary component of the dielectric function, which shows the presence of a Drude peak in the optical conductivity, and therefore metallicity in the lithiated graphene/MoS 2 heterostructure.« less

Scanning electrochemical microscopy of graphene/polymer hybrid thin films as supercapacitors: Physical-chemical interfacial processes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gupta, Sanju, E-mail: sanju.gupta@wku.edu; Price, Carson

2015-10-15

Hybrid electrode comprising an electric double-layer capacitor of graphene nanosheets and a pseudocapacitor of the electrically conducting polymers namely, polyaniline; PAni and polypyrrole; PPy are constructed that exhibited synergistic effect with excellent electrochemical performance as thin film supercapacitors for alternative energy. The hybrid supercapacitors were prepared by layer-by-layer (LbL) assembly based on controlled electrochemical polymerization followed by reduction of graphene oxide electrochemically producing ErGO, for establishing intimate electronic contact through nanoscale architecture and chemical stability, producing a single bilayer of (PAni/ErGO){sub 1}, (PPy/ErGO){sub 1}, (PAni/GO){sub 1} and (PPy/GO){sub 1}. The rationale design is to create thin films that possess interconnectedmore » graphene nanosheets (GNS) with polymer nanostructures forming well-defined tailored interfaces allowing sufficient surface adsorption and faster ion transport due to short diffusion distances. We investigated their electrochemical properties and performance in terms of gravimetric specific capacitance, C{sub s}, from cyclic voltammograms. The LbL-assembled bilayer films exhibited an excellent C{sub s} of ≥350 F g{sup −1} as compared with constituents (∼70 F g{sup −1}) at discharge current density of 0.3 A g{sup −1} that outperformed many other hybrid supercapacitors. To gain deeper insights into the physical-chemical interfacial processes occurring at the electrode/electrolyte interface that govern their operation, we have used scanning electrochemical microscopy (SECM) technique in feedback and probe approach modes. We present our findings from viewpoint of reinforcing the role played by heterogeneous electrode surface composed of nanoscale graphene sheets (conducting) and conducting polymers (semiconducting) backbone with ordered polymer chains via higher/lower probe current distribution maps. Also targeted is SECM imaging that allowed to determine electrochemical (re)activity of surface ion adsorption sites density at solid/liquid interface.« less

Improved functionality of graphene and carbon nanotube hybrid foam architecture by UV-ozone treatment

NASA Astrophysics Data System (ADS)

Wang, Wei; Ruiz, Isaac; Lee, Ilkeun; Zaera, Francisco; Ozkan, Mihrimah; Ozkan, Cengiz S.

2015-04-01

Optimization of the electrode/electrolyte double-layer interface is a key factor for improving electrode performance of aqueous electrolyte based supercapacitors (SCs). Here, we report the improved functionality of carbon materials via a non-invasive, high-throughput, and inexpensive UV generated ozone (UV-ozone) treatment. This process allows precise tuning of the graphene and carbon nanotube hybrid foam (GM) transitionally from ultrahydrophobic to hydrophilic within 60 s. The continuous tuning of surface energy can be controlled by simply varying the UV-ozone exposure time, while the ozone-oxidized carbon nanostructure maintains its integrity. Symmetric SCs based on the UV-ozone treated GM foam demonstrated enhanced rate performance. This technique can be readily applied to other CVD-grown carbonaceous materials by taking advantage of its ease of processing, low cost, scalability, and controllability.Optimization of the electrode/electrolyte double-layer interface is a key factor for improving electrode performance of aqueous electrolyte based supercapacitors (SCs). Here, we report the improved functionality of carbon materials via a non-invasive, high-throughput, and inexpensive UV generated ozone (UV-ozone) treatment. This process allows precise tuning of the graphene and carbon nanotube hybrid foam (GM) transitionally from ultrahydrophobic to hydrophilic within 60 s. The continuous tuning of surface energy can be controlled by simply varying the UV-ozone exposure time, while the ozone-oxidized carbon nanostructure maintains its integrity. Symmetric SCs based on the UV-ozone treated GM foam demonstrated enhanced rate performance. This technique can be readily applied to other CVD-grown carbonaceous materials by taking advantage of its ease of processing, low cost, scalability, and controllability. Electronic supplementary information (ESI) available. See DOI: 10.1039/c4nr06795a

Synergistic effect of temperature and point defect on the mechanical properties of single layer and bi-layer graphene

NASA Astrophysics Data System (ADS)

Debroy, Sanghamitra; Pavan Kumar, V.; Vijaya Sekhar, K.; Acharyya, Swati Ghosh; Acharyya, Amit

2017-10-01

The present study reports a comprehensive molecular dynamics simulation of the effect of a) temperature (300-1073 K at intervals of every 100 K) and b) point defect on the mechanical behaviour of single (armchair and zigzag direction) and bilayer layer graphene (AA and AB stacking). Adaptive intermolecular reactive bond order (AIREBO) potential function was used to describe the many-body short-range interatomic interactions for the single layer graphene sheet. Moreover, Lennard Jones model was considered for bilayer graphene to incorporate the van der Waals interactions among the interlayers of graphene. The effect of temperature on the strain energy of single layer and bilayer graphene was studied in order to understand the difference in mechanical behaviour of the two systems. The strength of the pristine single layer graphene was found to be higher as compared to bilayer AA stacked graphene at all temperatures. It was observed at 1073 K and in the presence of vacancy defect the strength for single layer armchair sheet falls by 30% and for bilayer armchair sheet by 33% as compared to the pristine sheets at 300 K. The AB stacked graphene sheet was found to have a two-step rupture process. The strength of pristine AB sheet was found to decrease by 22% on increase of temperature from 300 K to 1073 K.

Atomic layer deposited high-k dielectric on graphene by functionalization through atmospheric plasma treatment

NASA Astrophysics Data System (ADS)

Shin, Jeong Woo; Kang, Myung Hoon; Oh, Seongkook; Yang, Byung Chan; Seong, Kwonil; Ahn, Hyo-Sok; Lee, Tae Hoon; An, Jihwan

2018-05-01

Atomic layer-deposited (ALD) dielectric films on graphene usually show noncontinuous and rough morphology owing to the inert surface of graphene. Here, we demonstrate the deposition of thin and uniform ALD ZrO2 films with no seed layer on chemical vapor-deposited graphene functionalized by atmospheric oxygen plasma treatment. Transmission electron microscopy showed that the ALD ZrO2 films were highly crystalline, despite a low ALD temperature of 150 °C. The ALD ZrO2 film served as an effective passivation layer for graphene, which was shown by negative shifts in the Dirac voltage and the enhanced air stability of graphene field-effect transistors after ALD of ZrO2. The ALD ZrO2 film on the functionalized graphene may find use in flexible graphene electronics and biosensors owing to its low process temperature and its capacity to improve device performance and stability.

Electrochemistry at Edge of Single Graphene Layer in a Nanopore

PubMed Central

Banerjee, Shouvik; Shim, Jiwook; Rivera, Jose; Jin, Xiaozhong; Estrada, David; Solovyeva, Vita; You, Xiuque; Pak, James; Pop, Eric; Aluru, Narayana; Bashir, Rashid

2013-01-01

We study the electrochemistry of single layer graphene edges using a nanopore-based structure consisting of stacked graphene and Al2O3 dielectric layers. Nanopores, with diameters ranging from 5 to 20 nm, are formed by an electron beam sculpting process on the stacked layers. This leads to unique edge structure which, along with the atomically thin nature of the embedded graphene electrode, demonstrates electrochemical current densities as high as 1.2 × 104 A/cm2. The graphene edge embedded structure offers a unique capability to study the electrochemical exchange at an individual graphene edge, isolated from the basal plane electrochemical activity. We also report ionic current modulation in the nanopore by biasing the embedded graphene terminal with respect to the electrodes in the fluid. The high electrochemical specific current density for a graphene nanopore-based device can have many applications in sensitive chemical and biological sensing, and energy storage devices. PMID:23249127

Raman study of annealed two-dimensional heterostructure of graphene on hexagonal boron nitride

NASA Astrophysics Data System (ADS)

Souibgui, Mourad; Ajlani, Hosni; Cavanna, Antonnella; Oueslati, Meherzi; Meftah, Abdelaziz; Madouri, Ali

2017-12-01

In this paper, we investigate stacked 2D graphene layers on hexagonal boron nitride (h-BN). The graphene is obtained by high-quality chemical vapor deposition (CVD) and transferred to the h-BN substrate. We focus our attention on annealing effect at 1040 °C on single graphene layer (SGL) and bilayer graphene (BLG) on h-BN substrate using Raman spectroscopy. Our results show, before annealing, a twist angle θ = 0.63 ° between the SGL and the h-BN substrate and a twist angle 3 ° <θG1G2 < 8 ° between the two graphene layers of the BLG. After annealing, the analysis of the graphene G and 2D bands show a rotational reorientation of the graphene layer with respect to the h-BN substrate. Raman mapping also shows that the rotational reorientation is spatially dependent.

Atomic layer deposited high-k dielectric on graphene by functionalization through atmospheric plasma treatment.

PubMed

Shin, Jeong Woo; Kang, Myung Hoon; Oh, Seongkook; Yang, Byung Chan; Seong, Kwonil; Ahn, Hyo-Sok; Lee, Tae Hoon; An, Jihwan

2018-05-11

Atomic layer-deposited (ALD) dielectric films on graphene usually show noncontinuous and rough morphology owing to the inert surface of graphene. Here, we demonstrate the deposition of thin and uniform ALD ZrO 2 films with no seed layer on chemical vapor-deposited graphene functionalized by atmospheric oxygen plasma treatment. Transmission electron microscopy showed that the ALD ZrO 2 films were highly crystalline, despite a low ALD temperature of 150 °C. The ALD ZrO 2 film served as an effective passivation layer for graphene, which was shown by negative shifts in the Dirac voltage and the enhanced air stability of graphene field-effect transistors after ALD of ZrO 2 . The ALD ZrO 2 film on the functionalized graphene may find use in flexible graphene electronics and biosensors owing to its low process temperature and its capacity to improve device performance and stability.

Pressure sensing element based on the BN-graphene-BN heterostructure

NASA Astrophysics Data System (ADS)

Li, Mengwei; Wu, Chenggen; Zhao, Shiliang; Deng, Tao; Wang, Junqiang; Liu, Zewen; Wang, Li; Wang, Gao

2018-04-01

In this letter, we report a pressure sensing element based on the graphene-boron nitride (BN) heterostructure. The heterostructure consists of monolayer graphene sandwiched between two layers of vertically stacked dielectric BN nanofilms. The BN layers were used to protect the graphene layer from oxidation and pollution. Pressure tests were performed to investigate the characteristics of the BN-graphene-BN pressure sensing element. A sensitivity of 24.85 μV/V/mmHg is achieved in the pressure range of 130-180 kPa. After exposing the BN-graphene-BN pressure sensing element to the ambient environment for 7 days, the relative resistance change in the pressure sensing element is only 3.1%, while that of the reference open-faced graphene device without the BN protection layers is 15.7%. Thus, this strategy is promising for fabricating practical graphene pressure sensors with improved performance and stability.

Large-Area Growth of Turbostratic Graphene on Ni(111) via Physical Vapor Deposition

DOE Office of Scientific and Technical Information (OSTI.GOV)

Garlow, Joseph A.; Barrett, Lawrence K.; Wu, Lijun

Single-layer graphene has demonstrated remarkable electronic properties that are strongly influenced by interfacial bonding and break down for the lowest energy configuration of stacked graphene layers (AB Bernal). Multilayer graphene with relative rotations between carbon layers, known as turbostratic graphene, can effectively decouple the electronic states of adjacent layers, preserving properties similar to that of SLG. While the growth of AB Bernal graphene through chemical vapor deposition has been widely reported, we investigate the growth of turbostratic graphene on heteroepitaxial Ni(111) thin films utilizing physical vapor deposition. By varying the carbon deposition temperature between 800–1100°C, we report an increase inmore » the graphene quality concomitant with a transition in the size of uniform thickness graphene, ranging from nanocrystallites to thousands of square microns. Combination Raman modes of as-grown graphene within the frequency range of 1650 cm ₋1 to 2300 cm ₋1, along with features of the Raman 2D mode, were employed as signatures of turbostratic graphene. Bilayer and multilayer graphene were directly identified from areas that exhibited Raman characteristics of turbostratic graphene using high-resolution TEM imaging. Lastly, Raman maps of the pertinent modes reveal large regions of turbostratic graphene on Ni(111) thin films at a deposition temperature of 1100°C.« less

Large-Area Growth of Turbostratic Graphene on Ni(111) via Physical Vapor Deposition

DOE PAGES

Garlow, Joseph A.; Barrett, Lawrence K.; Wu, Lijun; ...

2016-01-29

Single-layer graphene has demonstrated remarkable electronic properties that are strongly influenced by interfacial bonding and break down for the lowest energy configuration of stacked graphene layers (AB Bernal). Multilayer graphene with relative rotations between carbon layers, known as turbostratic graphene, can effectively decouple the electronic states of adjacent layers, preserving properties similar to that of SLG. While the growth of AB Bernal graphene through chemical vapor deposition has been widely reported, we investigate the growth of turbostratic graphene on heteroepitaxial Ni(111) thin films utilizing physical vapor deposition. By varying the carbon deposition temperature between 800–1100°C, we report an increase inmore » the graphene quality concomitant with a transition in the size of uniform thickness graphene, ranging from nanocrystallites to thousands of square microns. Combination Raman modes of as-grown graphene within the frequency range of 1650 cm ₋1 to 2300 cm ₋1, along with features of the Raman 2D mode, were employed as signatures of turbostratic graphene. Bilayer and multilayer graphene were directly identified from areas that exhibited Raman characteristics of turbostratic graphene using high-resolution TEM imaging. Lastly, Raman maps of the pertinent modes reveal large regions of turbostratic graphene on Ni(111) thin films at a deposition temperature of 1100°C.« less

Large-Area Growth of Turbostratic Graphene on Ni(111) via Physical Vapor Deposition

PubMed Central

Garlow, Joseph A.; Barrett, Lawrence K.; Wu, Lijun; Kisslinger, Kim; Zhu, Yimei; Pulecio, Javier F.

2016-01-01

Single-layer graphene has demonstrated remarkable electronic properties that are strongly influenced by interfacial bonding and break down for the lowest energy configuration of stacked graphene layers (AB Bernal). Multilayer graphene with relative rotations between carbon layers, known as turbostratic graphene, can effectively decouple the electronic states of adjacent layers, preserving properties similar to that of SLG. While the growth of AB Bernal graphene through chemical vapor deposition has been widely reported, we investigate the growth of turbostratic graphene on heteroepitaxial Ni(111) thin films utilizing physical vapor deposition. By varying the carbon deposition temperature between 800 –1100 °C, we report an increase in the graphene quality concomitant with a transition in the size of uniform thickness graphene, ranging from nanocrystallites to thousands of square microns. Combination Raman modes of as-grown graphene within the frequency range of 1650 cm−1 to 2300 cm−1, along with features of the Raman 2D mode, were employed as signatures of turbostratic graphene. Bilayer and multilayer graphene were directly identified from areas that exhibited Raman characteristics of turbostratic graphene using high-resolution TEM imaging. Raman maps of the pertinent modes reveal large regions of turbostratic graphene on Ni(111) thin films at a deposition temperature of 1100 °C. PMID:26821604

Graphene photonics for resonator-enhanced electro-optic devices and all-optical interactions

DOEpatents

Englund, Dirk R.; Gan, Xuetao

2017-03-21

Techniques for coupling light into graphene using a planar photonic crystal having a resonant cavity characterized by a mode volume and a quality factor and at least one graphene layer positioned in proximity to the planar photonic crystal to at least partially overlap with an evanescent field of the resonant cavity. At least one mode of the resonant cavity can couple into the graphene layer via evanescent coupling. The optical properties of the graphene layer can be controlled, and characteristics of the graphene-cavity system can be detected. Coupling light into graphene can include electro-optic modulation of light, photodetection, saturable absorption, bistability, and autocorrelation.

The edge- and basal-plane-specific electrochemistry of a single-layer graphene sheet

PubMed Central

Yuan, Wenjing; Zhou, Yu; Li, Yingru; Li, Chun; Peng, Hailin; Zhang, Jin; Liu, Zhongfan; Dai, Liming; Shi, Gaoquan

2013-01-01

Graphene has a unique atom-thick two-dimensional structure and excellent properties, making it attractive for a variety of electrochemical applications, including electrosynthesis, electrochemical sensors or electrocatalysis, and energy conversion and storage. However, the electrochemistry of single-layer graphene has not yet been well understood, possibly due to the technical difficulties in handling individual graphene sheet. Here, we report the electrochemical behavior at single-layer graphene-based electrodes, comparing the basal plane of graphene to its edge. The graphene edge showed 4 orders of magnitude higher specific capacitance, much faster electron transfer rate and stronger electrocatalytic activity than those of graphene basal plane. A convergent diffusion effect was observed at the sub-nanometer thick graphene edge-electrode to accelerate the electrochemical reactions. Coupling with the high conductivity of a high-quality graphene basal plane, graphene edge is an ideal electrode for electrocatalysis and for the storage of capacitive charges. PMID:23896697

Ultrahigh-throughput exfoliation of graphite into pristine 'single-layer' graphene using microwaves and molecularly engineered ionic liquids.

PubMed

Matsumoto, Michio; Saito, Yusuke; Park, Chiyoung; Fukushima, Takanori; Aida, Takuzo

2015-09-01

Graphene has shown much promise as an organic electronic material but, despite recent achievements in the production of few-layer graphene, the quantitative exfoliation of graphite into pristine single-layer graphene has remained one of the main challenges in developing practical devices. Recently, reduced graphene oxide has been recognized as a non-feasible alternative to graphene owing to variable defect types and levels, and attention is turning towards reliable methods for the high-throughput exfoliation of graphite. Here we report that microwave irradiation of graphite suspended in molecularly engineered oligomeric ionic liquids allows for ultrahigh-efficiency exfoliation (93% yield) with a high selectivity (95%) towards 'single-layer' graphene (that is, with thicknesses <1 nm) in a short processing time (30 minutes). The isolated graphene sheets show negligible structural deterioration. They are also readily redispersible in oligomeric ionic liquids up to ~100 mg ml(-1), and form physical gels in which an anisotropic orientation of graphene sheets, once induced by a magnetic field, is maintained.

Manipulation of Dirac cones in metal-intercalated epitaxial graphene

NASA Astrophysics Data System (ADS)

Wang, Cai-Zhuang; Kim, Minsung; Tringides, Michael; Ho, Kai-Ming

Graphene is one of the most attractive materials from both fundamental and practical points of view due to its characteristic Dirac cones. The electronic property of graphene can be modified through the interaction with substrate or another graphene layer as illustrated in few-layer epitaxial graphene. Recently, metal intercalation became an effective method to manipulate the electronic structure of graphene by modifying the coupling between the constituent layers. In this work, we show that the Dirac cones of epitaxial graphene can be manipulated by intercalating rare-earth metals. We demonstrate that rare-earth metal intercalated epitaxial graphene has tunable band structures and the energy levels of Dirac cones as well as the linear or quadratic band dispersion can be controlled depending on the location of the intercalation layer and density. Our results could be important for applications and characterizations of the intercalated epitaxial graphene. Supported by the U.S. DOE-BES under Contract No. DE-AC02-07CH11358.

Nucleation of graphene layers on magnetic oxides: Co 3O 4(111) and Cr 2O 3(0001) from theory and experiment

DOE Office of Scientific and Technical Information (OSTI.GOV)

Beatty, John; Cheng, Tao; Cao, Yuan

We report directly grown strongly adherent graphene on Co 3O 4(111) by carbon molecular beam epitaxy (C MBE) at 850 K and density functional theory (DFT) findings that the first graphene layer is reconstructed to fit the Co 3O 4 surface, while subsequent layers retain normal graphene structure. This adherence to the Co 3O 4 structure results from partial bonding of half the carbons to top oxygens of the substrate. This structure is validated by X-ray photoelectron spectroscopy and low-energy electron diffraction studies, showing layer-by-layer graphene growth with ~0.08 electrons/carbon atom transferred to the oxide from the first graphene layer,more » in agreement with DFT. In contrast, for Cr 2O 3 DFT finds no strong bonding to the surface and C MBE on Cr 2O 3(0001) yields only graphite formation at 700 K, with C desorption above 800 K. As a result, strong graphene-to-oxide charge transfer aids nucleation of graphene on incommensurate oxide substrates and may have implications for spintronics.« less

Nucleation of graphene layers on magnetic oxides: Co 3O 4(111) and Cr 2O 3(0001) from theory and experiment

DOE PAGES

Beatty, John; Cheng, Tao; Cao, Yuan; ...

2016-12-14

We report directly grown strongly adherent graphene on Co 3O 4(111) by carbon molecular beam epitaxy (C MBE) at 850 K and density functional theory (DFT) findings that the first graphene layer is reconstructed to fit the Co 3O 4 surface, while subsequent layers retain normal graphene structure. This adherence to the Co 3O 4 structure results from partial bonding of half the carbons to top oxygens of the substrate. This structure is validated by X-ray photoelectron spectroscopy and low-energy electron diffraction studies, showing layer-by-layer graphene growth with ~0.08 electrons/carbon atom transferred to the oxide from the first graphene layer,more » in agreement with DFT. In contrast, for Cr 2O 3 DFT finds no strong bonding to the surface and C MBE on Cr 2O 3(0001) yields only graphite formation at 700 K, with C desorption above 800 K. As a result, strong graphene-to-oxide charge transfer aids nucleation of graphene on incommensurate oxide substrates and may have implications for spintronics.« less

Remote catalyzation for direct formation of graphene layers on oxides.

PubMed

Teng, Po-Yuan; Lu, Chun-Chieh; Akiyama-Hasegawa, Kotone; Lin, Yung-Chang; Yeh, Chao-Hui; Suenaga, Kazu; Chiu, Po-Wen

2012-03-14

Direct deposition of high-quality graphene layers on insulating substrates such as SiO(2) paves the way toward the development of graphene-based high-speed electronics. Here, we describe a novel growth technique that enables the direct deposition of graphene layers on SiO(2) with crystalline quality potentially comparable to graphene grown on Cu foils using chemical vapor deposition (CVD). Rather than using Cu foils as substrates, our approach uses them to provide subliming Cu atoms in the CVD process. The prime feature of the proposed technique is remote catalyzation using floating Cu and H atoms for the decomposition of hydrocarbons. This allows for the direct graphitization of carbon radicals on oxide surfaces, forming isolated low-defect graphene layers without the need for postgrowth etching or evaporation of the metal catalyst. The defect density of the resulting graphene layers can be significantly reduced by tuning growth parameters such as the gas ratios, Cu surface areas, and substrate-to-Cu distance. Under optimized conditions, graphene layers with nondiscernible Raman D peaks can be obtained when predeposited graphite flakes are used as seeds for extended growth. © 2012 American Chemical Society

Layered Chalcogenides beyond Graphene: from Electronic Structure Evolution to the Spin Transport

NASA Astrophysics Data System (ADS)

Yuan, Hongtao

2014-03-01

Recent efforts on graphene-like atomic layer materials, aiming at novel electronic properties and quantum phenomena beyond graphene, have attracted much attention for potential electronics/spintronics applications. Compared to the weak spin-orbit-interaction (SOI) in graphene, metal chalcogenides MX2 have heavy 4d/5d elements with strong atomic SOI, providing a unique way for generating spin polarization based on valleytronics physics. Indeed, such a spin-polarized band structure has been demonstrated theoretically and supported by optical investigations. However, despite these exciting progresses, following two important issues in MX2 community remain elusive: 1. the quantitative band structure of MX2 compounds (where are the valleys -band maxima/minima- locating in the BZ) have not been experimentally confirmed. Especially for those cleaved ultrathin mono- and bi-layer flakes hosting most of recently-reported exotic phenomena at the 2D limit, the direct detection for band dispersion becomes of great importance for valleytronics. 2. Spin transports have seldom been reported even though such a strong SOI system can serve as an ideal platform for the spin polarization and spin transport. In this work, we started from the basic electronic structures of representative MX2, obtained by ARPES, and investigated both the band variation between these compounds and their band evolution from bulk to the monolayer limit. After having a systematic understanding on band structures, we reported a giant Zeeman-type spin-polarization generated and modulated by an external electric field in WSe2 electric-double-layer transistors. The non-magnetic approach for realizing such an intriguing spin splitting not only keeps the system time-reversally invariant but also suggests a new paradigm for manipulating the spin-degrees of freedom of electrons. Acknowledge the support from DoE, BES, Division of MSE under contract DE-AC02-76SF00515.

A flexible and transparent graphene/ZnO nanorod hybrid structure fabricated by exfoliating a graphite substrate

NASA Astrophysics Data System (ADS)

Nam, Gwang-Hee; Baek, Seong-Ho; Cho, Chang-Hee; Park, Il-Kyu

2014-09-01

We demonstrate the fabrication of a graphene/ZnO nanorod (NR) hybrid structure by mechanical exfoliation of ZnO NRs grown on a graphite substrate. We confirmed the existence of graphene sheets on the hybrid structure by analyzing the Raman spectra and current-voltage (I-V) characteristics. The Raman spectra of the exfoliated graphene/ZnO NR hybrid structure show G and 2D band peaks that are shifted to lower wavenumbers, indicating that the exfoliated graphene layer exists under a significant amount of strain. The I-V characteristics of the graphene/ZnO NR hybrid structure show current flow through the graphene layer, while no current flow is observed on the ZnO NR/polydimethylsiloxane (PDMS) composite without graphene, thereby indicating that the few-layer graphene was successfully transferred onto the hybrid structure. A piezoelectric nanogenerator is demonstrated by using the fabricated graphene/ZnO NR hybrid structure. The nanogenerator exhibits stable output voltage up to 3.04 V with alternating current output characteristics.We demonstrate the fabrication of a graphene/ZnO nanorod (NR) hybrid structure by mechanical exfoliation of ZnO NRs grown on a graphite substrate. We confirmed the existence of graphene sheets on the hybrid structure by analyzing the Raman spectra and current-voltage (I-V) characteristics. The Raman spectra of the exfoliated graphene/ZnO NR hybrid structure show G and 2D band peaks that are shifted to lower wavenumbers, indicating that the exfoliated graphene layer exists under a significant amount of strain. The I-V characteristics of the graphene/ZnO NR hybrid structure show current flow through the graphene layer, while no current flow is observed on the ZnO NR/polydimethylsiloxane (PDMS) composite without graphene, thereby indicating that the few-layer graphene was successfully transferred onto the hybrid structure. A piezoelectric nanogenerator is demonstrated by using the fabricated graphene/ZnO NR hybrid structure. The nanogenerator exhibits stable output voltage up to 3.04 V with alternating current output characteristics. Electronic supplementary information (ESI) available. See DOI: 10.1039/c4nr02318h

Damage evaluation in graphene underlying atomic layer deposition dielectrics

PubMed Central

Tang, Xiaohui; Reckinger, Nicolas; Poncelet, Olivier; Louette, Pierre; Ureña, Ferran; Idrissi, Hosni; Turner, Stuart; Cabosart, Damien; Colomer, Jean-François; Raskin, Jean-Pierre; Hackens, Benoit; Francis, Laurent A.

2015-01-01

Based on micro-Raman spectroscopy (μRS) and X-ray photoelectron spectroscopy (XPS), we study the structural damage incurred in monolayer (1L) and few-layer (FL) graphene subjected to atomic-layer deposition of HfO2 and Al2O3 upon different oxygen plasma power levels. We evaluate the damage level and the influence of the HfO2 thickness on graphene. The results indicate that in the case of Al2O3/graphene, whether 1L or FL graphene is strongly damaged under our process conditions. For the case of HfO2/graphene, μRS analysis clearly shows that FL graphene is less disordered than 1L graphene. In addition, the damage levels in FL graphene decrease with the number of layers. Moreover, the FL graphene damage is inversely proportional to the thickness of HfO2 film. Particularly, the bottom layer of twisted bilayer (t-2L) has the salient features of 1L graphene. Therefore, FL graphene allows for controlling/limiting the degree of defect during the PE-ALD HfO2 of dielectrics and could be a good starting material for building field effect transistors, sensors, touch screens and solar cells. Besides, the formation of Hf-C bonds may favor growing high-quality and uniform-coverage dielectric. HfO2 could be a suitable high-K gate dielectric with a scaling capability down to sub-5-nm for graphene-based transistors. PMID:26311131

Interaction Between Graphene-Coated SiC Single Crystal and Liquid Copper

NASA Astrophysics Data System (ADS)

Homa, M.; Sobczak, N.; Sobczak, J. J.; Kudyba, A.; Bruzda, G.; Nowak, R.; Pietrzak, K.; Chmielewski, M.; Strupiński, W.

2018-04-01

The wettability of graphene-coated SiC single crystal (CGn/SiCsc) by liquid Cu (99.99%) was investigated by a sessile drop method in vacuum conditions at temperature of 1100 °C. The graphene layer was produced via a chemical vapor deposition routine using 4H-SiC single crystal cut out from 6″ wafer. A dispensed drop technique combined with a non-contact heating of a couple of materials was applied. The Cu drop was squeezed from a graphite capillary and deposited on the substrate directly in a vacuum chamber. The first Cu drop did not wet the CGn/SiCsc substrate and showed a lack of adhesion to the substrate: the falling Cu drop only touched the substrate forming a contact angle of θ 0 = 121° and then immediately rolled like a ball along the substrate surface. After settling near the edge of the substrate in about 0.15 s, the Cu drop formed an asymmetric shape with the right and left contact angles of different values (θ R = 86° and θ L = 70°, respectively), while in the next 30 min, θ R and θ L achieved the same final value of 52°. The second Cu drop was put down on the displacement path of the first drop, and immediately after the deposition, it also did not wet the substrate (θ = 123°). This drop kept symmetry and the primary position, but its wetting behavior was unusual: both θ R and θ L decreased in 17 min to the value of 23° and next, they increased to a final value of 65°. Visual observations revealed a presence of 2.5-mm-thick interfacial phase layer reactively formed under the second drop. Scanning electron microscopy (SEM) investigations revealed the presence of carbon-enriched precipitates on the top surface of the first Cu drop. These precipitates were identified by the Raman spectroscopy as double-layer graphene. The Raman spectrum taken from the substrate far from the drop revealed the presence of graphene, while that obtained from the first drop displacement path exhibited a decreased intensity of 2D peak. The results of SEM investigations and Raman spectroscopy studies suggest that the presence of graphene layer on the SiC substrate suppresses but does not completely prevent chemical interaction between liquid Cu drop and SiC. Both chemical degradation (etching) and mechanical degradation of the graphene layer during drop rolling due to high adhesion of the Cu drop to the SiC substrate are responsible for mass transfer through the 2nd drop/substrate interface that in turn results in significant changes of structure and chemistry of the drop and the interface.

Interaction Between Graphene-Coated SiC Single Crystal and Liquid Copper

NASA Astrophysics Data System (ADS)

Homa, M.; Sobczak, N.; Sobczak, J. J.; Kudyba, A.; Bruzda, G.; Nowak, R.; Pietrzak, K.; Chmielewski, M.; Strupiński, W.

2018-05-01

The wettability of graphene-coated SiC single crystal (CGn/SiCsc) by liquid Cu (99.99%) was investigated by a sessile drop method in vacuum conditions at temperature of 1100 °C. The graphene layer was produced via a chemical vapor deposition routine using 4H-SiC single crystal cut out from 6″ wafer. A dispensed drop technique combined with a non-contact heating of a couple of materials was applied. The Cu drop was squeezed from a graphite capillary and deposited on the substrate directly in a vacuum chamber. The first Cu drop did not wet the CGn/SiCsc substrate and showed a lack of adhesion to the substrate: the falling Cu drop only touched the substrate forming a contact angle of θ 0 = 121° and then immediately rolled like a ball along the substrate surface. After settling near the edge of the substrate in about 0.15 s, the Cu drop formed an asymmetric shape with the right and left contact angles of different values ( θ R = 86° and θ L = 70°, respectively), while in the next 30 min, θ R and θ L achieved the same final value of 52°. The second Cu drop was put down on the displacement path of the first drop, and immediately after the deposition, it also did not wet the substrate ( θ = 123°). This drop kept symmetry and the primary position, but its wetting behavior was unusual: both θ R and θ L decreased in 17 min to the value of 23° and next, they increased to a final value of 65°. Visual observations revealed a presence of 2.5-mm-thick interfacial phase layer reactively formed under the second drop. Scanning electron microscopy (SEM) investigations revealed the presence of carbon-enriched precipitates on the top surface of the first Cu drop. These precipitates were identified by the Raman spectroscopy as double-layer graphene. The Raman spectrum taken from the substrate far from the drop revealed the presence of graphene, while that obtained from the first drop displacement path exhibited a decreased intensity of 2D peak. The results of SEM investigations and Raman spectroscopy studies suggest that the presence of graphene layer on the SiC substrate suppresses but does not completely prevent chemical interaction between liquid Cu drop and SiC. Both chemical degradation (etching) and mechanical degradation of the graphene layer during drop rolling due to high adhesion of the Cu drop to the SiC substrate are responsible for mass transfer through the 2nd drop/substrate interface that in turn results in significant changes of structure and chemistry of the drop and the interface.

Environmental Synthesis of Few Layers Graphene Sheets Using Ultrasonic Exfoliation with Enhanced Electrical and Thermal Properties.

PubMed

Noroozi, Monir; Zakaria, Azmi; Radiman, Shahidan; Abdul Wahab, Zaidan

2016-01-01

In this paper, we report how few layers graphene that can be produced in large quantity with low defect ratio from exfoliation of graphite by using a high intensity probe sonication in water containing liquid hand soap and PVP. It was founded that the graphene powder obtained by this simple exfoliation method after the heat treatment had an excellent exfoliation into a single or layered graphene sheets. The UV-visible spectroscopy, FESEM, TEM, X-ray powder diffraction and Raman spectroscopy was used to analyse the graphene product. The thermal diffusivity of the samples was analysed using a highly accurate thermal-wave cavity photothermal technique. The data obtained showed excellent enhancement in the thermal diffusivity of the graphene dispersion. This well-dispersed graphene was then used to fabricate an electrically conductive polymer-graphene film composite. The results demonstrated that this low cost and environmental friendly technique allowed to the production of high quality layered graphene sheets, improved the thermal and electrical properties. This may find use in the wide range of applications based on graphene.

Environmental Synthesis of Few Layers Graphene Sheets Using Ultrasonic Exfoliation with Enhanced Electrical and Thermal Properties

PubMed Central

Noroozi, Monir; Zakaria, Azmi; Radiman, Shahidan; Abdul Wahab, Zaidan

2016-01-01

In this paper, we report how few layers graphene that can be produced in large quantity with low defect ratio from exfoliation of graphite by using a high intensity probe sonication in water containing liquid hand soap and PVP. It was founded that the graphene powder obtained by this simple exfoliation method after the heat treatment had an excellent exfoliation into a single or layered graphene sheets. The UV-visible spectroscopy, FESEM, TEM, X-ray powder diffraction and Raman spectroscopy was used to analyse the graphene product. The thermal diffusivity of the samples was analysed using a highly accurate thermal-wave cavity photothermal technique. The data obtained showed excellent enhancement in the thermal diffusivity of the graphene dispersion. This well-dispersed graphene was then used to fabricate an electrically conductive polymer-graphene film composite. The results demonstrated that this low cost and environmental friendly technique allowed to the production of high quality layered graphene sheets, improved the thermal and electrical properties. This may find use in the wide range of applications based on graphene. PMID:27064575

Structural consequences of hydrogen intercalation of epitaxial graphene on SiC(0001)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Emery, Jonathan D., E-mail: jdemery@anl.gov, E-mail: bedzyk@northwestern.edu; Johns, James E.; McBriarty, Martin E.

2014-10-20

The intercalation of various atomic species, such as hydrogen, to the interface between epitaxial graphene (EG) and its SiC substrate is known to significantly influence the electronic properties of the graphene overlayers. Here, we use high-resolution X-ray reflectivity to investigate the structural consequences of the hydrogen intercalation process used in the formation of quasi-free-standing (QFS) EG/SiC(0001). We confirm that the interfacial layer is converted to a layer structurally indistinguishable from that of the overlying graphene layers. This newly formed graphene layer becomes decoupled from the SiC substrate and, along with the other graphene layers within the film, is vertically displacedmore » by ∼2.1 Å. The number of total carbon layers is conserved during the process, and we observe no other structural changes such as interlayer intercalation or expansion of the graphene d-spacing. These results clarify the under-determined structure of hydrogen intercalated QFS-EG/SiC(0001) and provide a precise model to inform further fundamental and practical understanding of the system.« less

Comparison of VVV Auger electron spectra from single and multilayer graphene and graphite.

NASA Astrophysics Data System (ADS)

Chirayath, V. A.; Callewaert, V.; Fairchild, A. J.; Chrysler, M. D.; Gladen, R. W.; Imam, S. K.; Koymen, A. R.; Saniz, R.; Barbiellini, B.; Rajeshwar, K.; Partoens, B.; Weiss, A. H.

A direct observation of a low energy electron peak in the positron annihilation induced Auger electron spectra (PAES) from a single layer of graphene was made recently. A low energy positron beam (<1.25 eV) was used to deposit the positron on single layer graphene on a Cu substrate and the low energy peak was designated as VVV following the X-ray notation. The PAES signal is almost entirely from the top graphene layer due to the trapping of positrons in the image potential well on the surface of graphene. We utilize this monolayer sensitivity of PAES to compare the shape of the VVV Auger peak from the single layer graphene to the shapes of the VVV Auger peak obtained from multilayer graphene on Cu and from highly oriented pyrolytic graphite (HOPG). The VVV Auger peak from multilayer graphene on Cu and HOPG shows a systematic shift towards lower energies relative to the VVV Auger peak from the single layer graphene. The influence of the hole-hole interaction in distorting and shifting the VVV Auger spectra are discussed in relation to this observed shift. NSF Grant No. DMR 1508719 and DMR 1338130.

Modeling optical transmissivity of graphene grate in on-chip silicon photonic device

NASA Astrophysics Data System (ADS)

Amiri, Iraj S.; Ariannejad, M. M.; Jalil, M. A.; Ali, J.; Yupapin, P.

2018-06-01

A three-dimensional (3-D) finite-difference-time-domain (FDTD) analysis was used to simulate a silicon photonic waveguide. We have calculated power and transmission of the graphene used as single or multilayers to study the light transmission behavior. A new technique has been developed to define the straight silicon waveguide integrated with grate graphene layer. The waveguide has a variable grate spacing to be filled by the graphene layer. The number of graphene atomic layers varies between 100 and 1000 (or 380 nm and 3800 nm), the transmitted power obtained varies as ∼30% and ∼80%. The ∼99%, blocking of the light was occurred in 10,000 (or 38,000 nm) atomic layers of the graphene grate.

Side-gate modulation effects on high-quality BN-Graphene-BN nanoribbon capacitors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Yang; Chen, Xiaolong; Ye, Weiguang

High-quality BN-Graphene-BN nanoribbon capacitors with double side-gates of graphene have been experimentally realized. The double side-gates can effectively modulate the electronic properties of graphene nanoribbon capacitors. By applying anti-symmetric side-gate voltages, we observed significant upward shifting and flattening of the V-shaped capacitance curve near the charge neutrality point. Symmetric side-gate voltages, however, only resulted in tilted upward shifting along the opposite direction of applied gate voltages. These modulation effects followed the behavior of graphene nanoribbons predicted theoretically for metallic side-gate modulation. The negative quantum capacitance phenomenon predicted by numerical simulations for graphene nanoribbons modulated by graphene side-gates was not observed,more » possibly due to the weakened interactions between the graphene nanoribbon and side-gate electrodes caused by the Ga{sup +} beam etching process.« less

Optical control of graphene plasmon using liquid crystal layer 29K New One

DTIC Science & Technology

2017-03-01

AFRL-AFOSR-UK-TR-2017-0014 Optical control of graphene plasmon using liquid crystal layer 29K New One Viktor Yuriyovych Reshetnyak SCIENCE AND... plasmon using liquid crystal layer 29K New One 5a.  CONTRACT NUMBER 5b.  GRANT NUMBER STCU-P652 5c.  PROGRAM ELEMENT NUMBER 61102F 6. AUTHOR(S) Viktor...the basic research and establishes possible optical ways to control the surface plasmon polariton in graphene layer. A system comprises the graphene

Probing the interaction of noble gases with pristine and nitrogen-doped graphene through Raman spectroscopy

NASA Astrophysics Data System (ADS)

Cunha, Renato; Perea-López, Néstor; Elías, Ana Laura; Fujisawa, Kazunori; Carozo, Victor; Feng, Simin; Lv, Ruitao; dos Santos, Maria Cristina; Terrones, Mauricio; Araujo, Paulo T.

2018-05-01

The interactions of adsorbates with graphene have received increasing attention due to its importance in the development of applications involving graphene-based coatings. Here, we present a study of the adsorption of noble gases on pristine and nitrogen-doped graphene. Single-layer graphene samples were synthesized by chemical vapor deposition (CVD) and transferred to transmission electron microscopy (TEM) grids. Several noble gases were allowed to adsorb on the suspended graphene substrate at very low temperatures. Raman spectra show distinct frequency blue shifts in both the 2D and G bands, which are induced by gas adsorption onto high quality single layer graphene (1LG). These shifts, which we associate with compressive biaxial strain in the graphene layers induced by the noble gases, are negligible for nitrogen-doped graphene. Additionally, a thermal depinning transition, which is related to the desorption of a noble gas layer from the graphene surface at low temperatures (ranging from 20 to 35 K), was also observed at different transition temperatures for different noble gases. These transition temperatures were found to be 25 K for argon and 35 K for xenon. Moreover, we were able to obtain values for the compressive biaxial strain in graphene induced by the adsorbed layer of noble gases, using Raman spectroscopy. Ab initio calculations confirmed the correlation between the noble gas-induced strain and the changes in the Raman features observed.

The preparation and application of white graphene

NASA Astrophysics Data System (ADS)

Zhou, Chenghong

2014-12-01

In this article, another thin film named white graphene is introduced, containing its properties, preparation and potential applications. White graphene, which has the same structure with graphene but quite different electrical properties, can be exfoliated from its layered crystal, hexagonal boron nitride. Here two preparation methods of white graphene including supersonic cleavage and supercritical cleavage are presented. Inspired by the cleavage of graphene oxide, supersonic is applied to BN and few-layered films are obtained. Compared with supersonic cleavage, supercritical cleavage proves to be more successful. As supercritical fluid can diffuse into interlayer space of the layered hexagonal boron nitride easily, once reduce the pressure of the supercritical system fast, supercritical fluid among layers expands and escapes form interlayer, consequently exfoliating the hexagonal boron nitride into few layered structure. A series of characterization demonstrate that the monolayer white graphene prepared in the process matches its theoretical thickness 0.333nm and has lateral sizes at the order of 10μm. Supercritical cleavage proves to be successful and shows many advantages, such as good production quality and fast production cycle. Furthermore, the band energy of white graphene, which shows quite different from graphene, is simulated via tight-bonding in theory. The excellent properties will lead to extensive applications of white graphene. As white graphene has not received enough concern and exploration, it's potential to play a significant role in the fields of industry and science.

An Approach to Solid-State Electrical Double Layer Capacitors Fabricated with Graphene Oxide-Doped, Ionic Liquid-Based Solid Copolymer Electrolytes

PubMed Central

Fattah, N. F. A.; Ng, H. M.; Mahipal, Y. K.; Numan, Arshid; Ramesh, S.; Ramesh, K.

2016-01-01

Solid polymer electrolyte (SPE) composed of semi-crystalline poly (vinylidene fluoride-hexafluoropropylene) [P(VdF-HFP)] copolymer, 1-ethyl-3-methylimidazolium bis (trifluoromethyl sulphonyl) imide [EMI-BTI] and graphene oxide (GO) was prepared and its performance evaluated. The effects of GO nano-filler were investigated in terms of enhancement in ionic conductivity along with the electrochemical properties of its electrical double layer capacitors (EDLC). The GO-doped SPE shows improvement in ionic conductivity compared to the P(VdF-HFP)-[EMI-BTI] SPE system due to the existence of the abundant oxygen-containing functional group in GO that assists in the improvement of the ion mobility in the polymer matrix. The complexation of the materials in the SPE is confirmed in X-ray diffraction (XRD) and thermogravimetric analysis (TGA) studies. The electrochemical performance of EDLC fabricated with GO-doped SPE is examined using cyclic voltammetry and charge–discharge techniques. The maximum specific capacitance obtained is 29.6 F∙g−1, which is observed at a scan rate of 3 mV/s in 6 wt % GO-doped, SPE-based EDLC. It also has excellent cyclic retention as it is able keep the performance of the EDLC at 94% even after 3000 cycles. These results suggest GO doped SPE plays a significant role in energy storage application. PMID:28773573

An Approach to Solid-State Electrical Double Layer Capacitors Fabricated with Graphene Oxide-Doped, Ionic Liquid-Based Solid Copolymer Electrolytes.

PubMed

Fattah, N F A; Ng, H M; Mahipal, Y K; Numan, Arshid; Ramesh, S; Ramesh, K

2016-06-06

Solid polymer electrolyte (SPE) composed of semi-crystalline poly (vinylidene fluoride-hexafluoropropylene) [P(VdF-HFP)] copolymer, 1-ethyl-3-methylimidazolium bis (trifluoromethyl sulphonyl) imide [EMI-BTI] and graphene oxide (GO) was prepared and its performance evaluated. The effects of GO nano-filler were investigated in terms of enhancement in ionic conductivity along with the electrochemical properties of its electrical double layer capacitors (EDLC). The GO-doped SPE shows improvement in ionic conductivity compared to the P(VdF-HFP)-[EMI-BTI] SPE system due to the existence of the abundant oxygen-containing functional group in GO that assists in the improvement of the ion mobility in the polymer matrix. The complexation of the materials in the SPE is confirmed in X-ray diffraction (XRD) and thermogravimetric analysis (TGA) studies. The electrochemical performance of EDLC fabricated with GO-doped SPE is examined using cyclic voltammetry and charge-discharge techniques. The maximum specific capacitance obtained is 29.6 F∙g -1 , which is observed at a scan rate of 3 mV/s in 6 wt % GO-doped, SPE-based EDLC. It also has excellent cyclic retention as it is able keep the performance of the EDLC at 94% even after 3000 cycles. These results suggest GO doped SPE plays a significant role in energy storage application.

Significantly improved photovoltaic performance in polymer bulk heterojunction solar cells with graphene oxide /PEDOT:PSS double decked hole transport layer

PubMed Central

Rafique, Saqib; Abdullah, Shahino Mah; Shahid, Muhammad Mehmood; Ansari, Mohammad Omaish; Sulaiman, Khaulah

2017-01-01

This work demonstrates the high performance graphene oxide (GO)/PEDOT:PSS doubled decked hole transport layer (HTL) in the PCDTBT:PC71BM based bulk heterojunction organic photovoltaic device. The devices were tested on merits of their power conversion efficiency (PCE), reproducibility, stability and further compared with the devices with individual GO or PEDOT:PSS HTLs. Solar cells employing GO/PEDOT:PSS HTL yielded a PCE of 4.28% as compared to either of individual GO or PEDOT:PSS HTLs where they demonstrated PCEs of 2.77 and 3.57%, respectively. In case of single GO HTL, an inhomogeneous coating of ITO caused the poor performance whereas PEDOT:PSS is known to be hygroscopic and acidic which upon direct contact with ITO reduced the device performance. The improvement in the photovoltaic performance is mainly ascribed to the increased charge carriers mobility, short circuit current, open circuit voltage, fill factor, and decreased series resistance. The well matched work function of GO and PEDOT:PSS is likely to facilitate the charge transportation and an overall reduction in the series resistance. Moreover, GO could effectively block the electrons due to its large band-gap of ~3.6 eV, leading to an increased shunt resistance. In addition, we also observed the improvement in the reproducibility and stability. PMID:28084304

Significantly improved photovoltaic performance in polymer bulk heterojunction solar cells with graphene oxide /PEDOT:PSS double decked hole transport layer.

PubMed

Rafique, Saqib; Abdullah, Shahino Mah; Shahid, Muhammad Mehmood; Ansari, Mohammad Omaish; Sulaiman, Khaulah

2017-01-13

This work demonstrates the high performance graphene oxide (GO)/PEDOT:PSS doubled decked hole transport layer (HTL) in the PCDTBT:PC 71 BM based bulk heterojunction organic photovoltaic device. The devices were tested on merits of their power conversion efficiency (PCE), reproducibility, stability and further compared with the devices with individual GO or PEDOT:PSS HTLs. Solar cells employing GO/PEDOT:PSS HTL yielded a PCE of 4.28% as compared to either of individual GO or PEDOT:PSS HTLs where they demonstrated PCEs of 2.77 and 3.57%, respectively. In case of single GO HTL, an inhomogeneous coating of ITO caused the poor performance whereas PEDOT:PSS is known to be hygroscopic and acidic which upon direct contact with ITO reduced the device performance. The improvement in the photovoltaic performance is mainly ascribed to the increased charge carriers mobility, short circuit current, open circuit voltage, fill factor, and decreased series resistance. The well matched work function of GO and PEDOT:PSS is likely to facilitate the charge transportation and an overall reduction in the series resistance. Moreover, GO could effectively block the electrons due to its large band-gap of ~3.6 eV, leading to an increased shunt resistance. In addition, we also observed the improvement in the reproducibility and stability.

Significantly improved photovoltaic performance in polymer bulk heterojunction solar cells with graphene oxide /PEDOT:PSS double decked hole transport layer

NASA Astrophysics Data System (ADS)

Rafique, Saqib; Abdullah, Shahino Mah; Shahid, Muhammad Mehmood; Ansari, Mohammad Omaish; Sulaiman, Khaulah

2017-01-01

This work demonstrates the high performance graphene oxide (GO)/PEDOT:PSS doubled decked hole transport layer (HTL) in the PCDTBT:PC71BM based bulk heterojunction organic photovoltaic device. The devices were tested on merits of their power conversion efficiency (PCE), reproducibility, stability and further compared with the devices with individual GO or PEDOT:PSS HTLs. Solar cells employing GO/PEDOT:PSS HTL yielded a PCE of 4.28% as compared to either of individual GO or PEDOT:PSS HTLs where they demonstrated PCEs of 2.77 and 3.57%, respectively. In case of single GO HTL, an inhomogeneous coating of ITO caused the poor performance whereas PEDOT:PSS is known to be hygroscopic and acidic which upon direct contact with ITO reduced the device performance. The improvement in the photovoltaic performance is mainly ascribed to the increased charge carriers mobility, short circuit current, open circuit voltage, fill factor, and decreased series resistance. The well matched work function of GO and PEDOT:PSS is likely to facilitate the charge transportation and an overall reduction in the series resistance. Moreover, GO could effectively block the electrons due to its large band-gap of ~3.6 eV, leading to an increased shunt resistance. In addition, we also observed the improvement in the reproducibility and stability.

Burning Graphene Layer-by-Layer

PubMed Central

Ermakov, Victor A.; Alaferdov, Andrei V.; Vaz, Alfredo R.; Perim, Eric; Autreto, Pedro A. S.; Paupitz, Ricardo; Galvao, Douglas S.; Moshkalev, Stanislav A.

2015-01-01

Graphene, in single layer or multi-layer forms, holds great promise for future electronics and high-temperature applications. Resistance to oxidation, an important property for high-temperature applications, has not yet been extensively investigated. Controlled thinning of multi-layer graphene (MLG), e.g., by plasma or laser processing is another challenge, since the existing methods produce non-uniform thinning or introduce undesirable defects in the basal plane. We report here that heating to extremely high temperatures (exceeding 2000 K) and controllable layer-by-layer burning (thinning) can be achieved by low-power laser processing of suspended high-quality MLG in air in “cold-wall” reactor configuration. In contrast, localized laser heating of supported samples results in non-uniform graphene burning at much higher rates. Fully atomistic molecular dynamics simulations were also performed to reveal details of oxidation mechanisms leading to uniform layer-by-layer graphene gasification. The extraordinary resistance of MLG to oxidation paves the way to novel high-temperature applications as continuum light source or scaffolding material. PMID:26100466

Enhancement in sensitivity of graphene-based zinc oxide assisted bimetallic surface plasmon resonance (SPR) biosensor

NASA Astrophysics Data System (ADS)

Kumar, Rajeev; Kushwaha, Angad S.; Srivastava, Monika; Mishra, H.; Srivastava, S. K.

2018-03-01

In the present communication, a highly sensitive surface plasmon resonance (SPR) biosensor with Kretschmann configuration having alternate layers, prism/zinc oxide/silver/gold/graphene/biomolecules (ss-DNA) is presented. The optimization of the proposed configuration has been accomplished by keeping the constant thickness of zinc oxide (32 nm), silver (32 nm), graphene (0.34 nm) layer and biomolecules (100 nm) for different values of gold layer thickness (1, 3 and 5 nm). The sensitivity of the proposed SPR biosensor has been demonstrated for a number of design parameters such as gold layer thickness, number of graphene layer, refractive index of biomolecules and the thickness of biomolecules layer. SPR biosensor with optimized geometry has greater sensitivity (66 deg/RIU) than the conventional (52 deg/RIU) as well as other graphene-based (53.2 deg/RIU) SPR biosensor. The effect of zinc oxide layer thickness on the sensitivity of SPR biosensor has also been analysed. From the analysis, it is found that the sensitivity increases significantly by increasing the thickness of zinc oxide layer. It means zinc oxide intermediate layer plays an important role to improve the sensitivity of the biosensor. The sensitivity of SPR biosensor also increases by increasing the number of graphene layer (upto nine layer).

Chirality and grain boundary effects on indentation mechanical properties of graphene coated on nickel foil

NASA Astrophysics Data System (ADS)

Yan, Yuping; Lv, Jiajiang; Liu, Sheng

2018-04-01

We investigate chirality and grain boundary (GB) effects on indentation mechanical properties of graphene coated on nickel foil using molecular dynamics simulations. The models of graphene with different chirality angles, different numbers of layers and tilt GBs were established. It was found that the chirality angle of few-layer graphene had a significant effect on the load bearing capacity of graphene/nickel systems, and this turns out to be more significant when the number of layers is greater than one. The enhancement to the contact stiffness, elastic capacity and the load bearing capacity of graphene with tilt GBs was lower than that of pristine graphene.

Graphene-epoxy flexible transparent capacitor obtained by graphene-polymer transfer and UV-induced bonding.

PubMed

Sangermano, Marco; Chiolerio, Alessandro; Veronese, Giulio Paolo; Ortolani, Luca; Rizzoli, Rita; Mancarella, Fulvio; Morandi, Vittorio

2014-02-01

A new approach is reported for the preparation of a graphene-epoxy flexible transparent capacitor obtained by graphene-polymer transfer and UV-induced bonding. SU8 resin is employed for realizing a well-adherent, transparent, and flexible supporting layer. The achieved transparent graphene/SU8 membrane presents two distinct surfaces: one homogeneous conductive surface containing a graphene layer and one dielectric surface typical of the epoxy polymer. Two graphene/SU8 layers are bonded together by using an epoxy photocurable formulation based on epoxy resin. The obtained material showed a stable and clear capacitive behavior. © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

An ultrasensitive and low-cost graphene sensor based on layer-by-layer nano self-assembly

NASA Astrophysics Data System (ADS)

Zhang, Bo; Cui, Tianhong

2011-02-01

The flexible cancer sensor based on layer-by-layer self-assembled graphene reported in this letter demonstrates features including ultrahigh sensitivity and low cost due to graphene material properties in nature, self-assembly technique, and polyethylene terephthalate substrate. According to the conductance change of self-assembled graphene, the label free and labeled graphene sensors are capable of detecting very low concentrations of prostate specific antigen down to 4 fg/ml (0.11 fM) and 0.4 pg/ml (11 fM), respectively, which are three orders of magnitude lower than carbon nanotube sensors under the same conditions of design, manufacture, and measurement.

Spectral properties of excitons in the bilayer graphene

NASA Astrophysics Data System (ADS)

Apinyan, V.; Kopeć, T. K.

2018-01-01

In this paper, we consider the spectral properties of the bilayer graphene with the local excitonic pairing interaction between the electrons and holes. We consider the generalized Hubbard model, which includes both intralayer and interlayer Coulomb interaction parameters. The solution of the excitonic gap parameter is used to calculate the electronic band structure, single-particle spectral functions, the hybridization gap, and the excitonic coherence length in the bilayer graphene. We show that the local interlayer Coulomb interaction is responsible for the semimetal-semiconductor transition in the double layer system, and we calculate the hybridization gap in the band structure above the critical interaction value. The formation of the excitonic band gap is reported as the threshold process and the momentum distribution functions have been calculated numerically. We show that in the weak coupling limit the system is governed by the Bardeen-Cooper-Schrieffer (BCS)-like pairing state. Contrary, in the strong coupling limit the excitonic condensate states appear in the semiconducting phase, by forming the Dirac's pockets in the reciprocal space.

Green Synthesis of Three-Dimensional MnO2/Graphene Hydrogel Composites as a High-Performance Electrode Material for Supercapacitors.

PubMed

Meng, Xiaoyi; Lu, Liang; Sun, Chunwen

2018-05-16

Graphene hydrogels (GHs) and their composites have attracted wide attention because of the special structure of graphene assembly and exceptional electrochemical performance as electrodes for energy storage devices. Here, we report a GH with three-dimensional architecture prepared by a hydrothermal method via a self-assembled process in glucose and ammonia system as well as subsequent freeze-drying. The δ-MnO 2 /GH composite was then obtained by immersing GH in KMnO 4 solution with a certain concentration under heat treatment. The asymmetric supercapacitor MnO 2 /GH//GH consisting of pseudocapacitive nanosheet-like δ-MnO 2 /GH as the cathode and electric double-layer capacitive GH as the anode provides high energy density of 34.7 W h/kg at a power density of 1.0 kW/kg. Importantly, it is found that the pseudocapacitive behavior of MnO 2 has great effects on the rate performance of the supercapacitor, which is identified by kinetic analysis.

Supercapacitors based on pillared graphene nanostructures.

PubMed

Lin, Jian; Zhong, Jiebin; Bao, Duoduo; Reiber-Kyle, Jennifer; Wang, Wei; Vullev, Valentine; Ozkan, Mihrimah; Ozkan, Cengiz S

2012-03-01

We describe the fabrication of highly conductive and large-area three dimensional pillared graphene nanostructure (PGN) films from assembly of vertically aligned CNT pillars on flexible copper foils for applications in electric double layer capacitors (EDLC). The PGN films synthesized via a one-step chemical vapor deposition process on flexible copper foils exhibit high conductivity with sheet resistance as low as 1.6 ohms per square and possessing high mechanical flexibility. Raman spectroscopy indicates the presence of multi walled carbon nanotubes (MWCNT) and their morphology can be controlled by the growth conditions. It was discovered that nitric acid treatment can significantly increase the specific capacitance of the devices. EDLC devices based on PGN electrodes (surface area of 565 m2/g) demonstrate enhanced performance with specific capacitance value as high as 330 F/g extracted from the current density-voltage (CV) measurements and energy density value of 45.8 Wh/kg. The hybrid graphene-CNT nanostructures are attractive for applications including supercapacitors, fuel cells and batteries.

Ultrahigh-rate supercapacitors based on eletrochemically reduced graphene oxide for ac line-filtering.

PubMed

Sheng, Kaixuan; Sun, Yiqing; Li, Chun; Yuan, Wenjing; Shi, Gaoquan

2012-01-01

The recent boom in multifunction portable electronic equipments requires the development of compact and miniaturized electronic circuits with high efficiencies, low costs and long lasting time. For the operation of most line-powered electronics, alternating current (ac) line-filters are used to attenuate the leftover ac ripples on direct current (dc) voltage busses. Today, aluminum electrolytic capacitors (AECs) are widely applied for this purpose. However, they are usually the largest components in electronic circuits. Replacing AECs by more compact capacitors will have an immense impact on future electronic devices. Here, we report a double-layer capacitor based on three-dimensional (3D) interpenetrating graphene electrodes fabricated by electrochemical reduction of graphene oxide (ErGO-DLC). At 120-hertz, the ErGO-DLC exhibited a phase angle of -84 degrees, a specific capacitance of 283 microfaradays per centimeter square and a resistor-capacitor (RC) time constant of 1.35 milliseconds, making it capable of replacing AECs for the application of 120-hertz filtering.

Ultrahigh-rate supercapacitors based on eletrochemically reduced graphene oxide for ac line-filtering

NASA Astrophysics Data System (ADS)

Sheng, Kaixuan; Sun, Yiqing; Li, Chun; Yuan, Wenjing; Shi, Gaoquan

2012-02-01

The recent boom in multifunction portable electronic equipments requires the development of compact and miniaturized electronic circuits with high efficiencies, low costs and long lasting time. For the operation of most line-powered electronics, alternating current (ac) line-filters are used to attenuate the leftover ac ripples on direct current (dc) voltage busses. Today, aluminum electrolytic capacitors (AECs) are widely applied for this purpose. However, they are usually the largest components in electronic circuits. Replacing AECs by more compact capacitors will have an immense impact on future electronic devices. Here, we report a double-layer capacitor based on three-dimensional (3D) interpenetrating graphene electrodes fabricated by electrochemical reduction of graphene oxide (ErGO-DLC). At 120-hertz, the ErGO-DLC exhibited a phase angle of -84 degrees, a specific capacitance of 283 microfaradays per centimeter square and a resistor-capacitor (RC) time constant of 1.35 milliseconds, making it capable of replacing AECs for the application of 120-hertz filtering.

Ultrahigh-rate supercapacitors based on eletrochemically reduced graphene oxide for ac line-filtering

PubMed Central

Sheng, Kaixuan; Sun, Yiqing; Li, Chun; Yuan, Wenjing; Shi, Gaoquan

2012-01-01

The recent boom in multifunction portable electronic equipments requires the development of compact and miniaturized electronic circuits with high efficiencies, low costs and long lasting time. For the operation of most line-powered electronics, alternating current (ac) line-filters are used to attenuate the leftover ac ripples on direct current (dc) voltage busses. Today, aluminum electrolytic capacitors (AECs) are widely applied for this purpose. However, they are usually the largest components in electronic circuits. Replacing AECs by more compact capacitors will have an immense impact on future electronic devices. Here, we report a double-layer capacitor based on three-dimensional (3D) interpenetrating graphene electrodes fabricated by electrochemical reduction of graphene oxide (ErGO-DLC). At 120-hertz, the ErGO-DLC exhibited a phase angle of −84 degrees, a specific capacitance of 283 microfaradays per centimeter square and a resistor-capacitor (RC) time constant of 1.35 milliseconds, making it capable of replacing AECs for the application of 120-hertz filtering. PMID:22355759

Tailoring the Oxygen Content of Graphite and Reduced Graphene Oxide for Specific Applications.

PubMed

Morimoto, Naoki; Kubo, Takuya; Nishina, Yuta

2016-02-25

Graphene oxide (GO) is widely recognized as a promising material in a variety of fields, but its structure and composition has yet to be fully controlled. We have developed general strategies to control the oxidation degree of graphene-like materials via two methods: oxidation of graphite by KMnO4 in H2SO4 (oGO), and reduction of highly oxidized GO by hydrazine (rGO). Even though the oxygen content may be the same, oGO and rGO have different properties, for example the adsorption ability, oxidation ability, and electron conductivity. These differences in property arise from the difference in the underlying graphitic structure and the type of defect present. Our results can be used as a guideline for the production of tailor-made graphitic carbons. As an example, we show that rGO with 23.1 wt% oxygen showed the best performance as an electrode of an electric double-layer capacitor.

Tailoring the Oxygen Content of Graphite and Reduced Graphene Oxide for Specific Applications

NASA Astrophysics Data System (ADS)

Morimoto, Naoki; Kubo, Takuya; Nishina, Yuta

2016-02-01

Graphene oxide (GO) is widely recognized as a promising material in a variety of fields, but its structure and composition has yet to be fully controlled. We have developed general strategies to control the oxidation degree of graphene-like materials via two methods: oxidation of graphite by KMnO4 in H2SO4 (oGO), and reduction of highly oxidized GO by hydrazine (rGO). Even though the oxygen content may be the same, oGO and rGO have different properties, for example the adsorption ability, oxidation ability, and electron conductivity. These differences in property arise from the difference in the underlying graphitic structure and the type of defect present. Our results can be used as a guideline for the production of tailor-made graphitic carbons. As an example, we show that rGO with 23.1 wt% oxygen showed the best performance as an electrode of an electric double-layer capacitor.

Graphene oxide--MnO2 nanocomposites for supercapacitors.

PubMed

Chen, Sheng; Zhu, Junwu; Wu, Xiaodong; Han, Qiaofeng; Wang, Xin

2010-05-25

A composite of graphene oxide supported by needle-like MnO(2) nanocrystals (GO-MnO(2) nanocomposites) has been fabricated through a simple soft chemical route in a water-isopropyl alcohol system. The formation mechanism of these intriguing nanocomposites investigated by transmission electron microscopy and Raman and ultraviolet-visible absorption spectroscopy is proposed as intercalation and adsorption of manganese ions onto the GO sheets, followed by the nucleation and growth of the crystal species in a double solvent system via dissolution-crystallization and oriented attachment mechanisms, which in turn results in the exfoliation of GO sheets. Interestingly, it was found that the electrochemical performance of as-prepared nanocomposites could be enhanced by the chemical interaction between GO and MnO(2). This method provides a facile and straightforward approach to deposit MnO(2) nanoparticles onto the graphene oxide sheets (single layer of graphite oxide) and may be readily extended to the preparation of other classes of hybrids based on GO sheets for technological applications.

Functionalization Pattern of Graphene Oxide Sheets Controls Entry or Produces Lipid Turmoil in Phospholipid Membranes.

PubMed

Dallavalle, Marco; Bottoni, Andrea; Calvaresi, Matteo; Zerbetto, Francesco

2018-05-09

Molecular dynamics, coarse-grained to the level of hydrophobic and hydrophilic interactions, shows that graphene oxide sheets, GOSs, can pierce through the phospholipid membrane and navigate the double layer only if the hydrophilic groups are randomly dispersed in the structure. Their behavior resembles that found in similar calculations for pristine graphene sheets. If the oxidation is located at the edge of the sheets, GOSs hover over the membrane and trigger a major reorganization of the lipids. The reorganization is the largest when the radius of the edge-functionalized sheet is similar to the length of the lipophilic chain of the lipids. In the reorganization, the heads of the lipid chains form dynamical structures that pictorially resemble the swirl of water flowing down a drain. All effects maximize the interaction between hydrophobic moieties on the one hand and lipophilic fragments on the other and are accompanied by a large number of lipid flip-flops. Possible biological consequences are discussed.

Ni Foam-Ni3 S2 @Ni(OH)2 -Graphene Sandwich Structure Electrode Materials: Facile Synthesis and High Supercapacitor Performance.

PubMed

Wang, Xiaobing; Hu, Jiangjiang; Su, Yichang; Hao, Jin; Liu, Fanggang; Han, Shuang; An, Jian; Lian, Jianshe

2017-03-23

A novel Ni foam-Ni 3 S 2 @Ni(OH) 2 -graphene sandwich-structured electrode (NF-NN-G) with high areal mass loading (8.33 mg cm -2 ) has been developed by sulfidation and hydrolysis reactions. The conductivity of Ni 3 S 2 and Ni(OH) 2 were both improved. The upper layer of Ni(OH) 2 , covered with a thin graphene film, is formed in situ from the surface of the lower layer of Ni 3 S 2 , whereas the Ni 3 S 2 grown on Ni foam substrate mainly acts as a rough support bridging the Ni(OH) 2 and Ni foam. The graphene stabilized the Ni(OH) 2 and the electrochemical properties were effectively enhanced. The as-synthesized NF-NN-G-5mg electrode shows a high specific capacitance (2258 F g -1 at 1 A g -1 or 18.81 F cm -2 at 8.33 mA cm -2 ) and an outstanding rate property (1010 F g -1 at 20 Ag -1 or 8.413 F cm -2 at 166.6 mA cm -2 ). This result is around double the capacitance achieved in previous research on Ni 3 S 2 @Ni(OH) 2 /3DGN composites (3DGN=three-dimensional graphene network). In addition, the as-fabricated NF-NN-G-5mg composite electrode has an excellent cycle life with no capacitance loss after 3000 cycles, indicating a potential application as an efficient electrode. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Wearable supercapacitors on polyethylene terephthalate fabrics with good wash fastness and high flexibility

NASA Astrophysics Data System (ADS)

Wang, Guixia; Babaahmadi, Vahid; He, Nanfei; Liu, Yixin; Pan, Qin; Montazer, Majid; Gao, Wei

2017-11-01

All solid-state micro-supercapacitors (MSC) have emerged as attractive energy-storage units for portable and wearable electronics. Here, we describe a textile-based solid-state MSC via laser scribing of graphene oxide (GO) coatings on a flexible polyethylene terephthalate (PET) fabric. The laser-scribed graphene oxide layers (LGO) possess three-dimensionally porous structure suitable for electrochemical-double-layer formation. To improve the wash fastness and the flexibility of the as-prepared MSCs, glutaraldehyde (GA) was employed to crosslink the GO layers and PVA-gel electrolyte onto the PET fabric. The resultant all solid-state MSCs exhibited excellent flexibility, high areal specific capacitance (756 μF·cm-2 at 20 mV·s-1), and good rate capability when subject to bending and laundering. Furthermore, the MSC device showed a high power density of about 1.4 W·cm-3 and an energy density of 5.3 × 10-5 Wh·cm-3, and retained 98.3% of its initial capacitance after 1000 cycles at a current density of 0.5 mA·cm-2. This work is the first demonstration of in-plane MSCs on PET fabric surfaces with enhanced durability and flexibility.

Covalently functionalized single-walled carbon nanotubes and graphene composite electrodes for pseudocapacitor application

NASA Astrophysics Data System (ADS)

Le Barny, Pierre; Servet, Bernard; Campidelli, Stéphane; Bondavalli, Paolo; Galindo, Christophe

2013-09-01

The use of carbon-based materials in electrochemical double-layer supercapacitors (EDLC) is currently being the focus of much research. Even though activated carbon (AC) is the state of the art electrode material, AC suffers from some drawbacks including its limited electrical conductivity, the need for a binder to ensure the expected electrode cohesion and its limited accessibility of its pores to solvated ions of the electrolyte. Owing to their unique physical properties, carbon nanotubes (CNTs) or graphene could overcome these drawbacks. It has been demonstrated that high specific capacitance could be obtained when the carbon accessible surface area of the electrode was finely tailored by using graphene combined with other carbonaceous nanoparticles such as CNTs12.In this work, to further increase the specific capacitance of the electrode, we have covalently grafted onto the surface of single-walled carbon nanotubes (SWCNTs), exfoliated graphite or graphene oxide (GO), anthraquinone (AQ) derivatives which are electrochemically active materials. The modified SWCNTs and graphene-like materials have been characterized by Raman spectroscopy, X-ray photoemission and cyclic voltammetry . Then suspensions based on mixtures of modified SWCNTs and modified graphene-like materials have been prepared and transformed into electrodes either by spray coating or by filtration. These electrodes have been characterized by SEM and by cyclic voltammetry in 0.1M H2S04 electrolyte.

Characterization of few-layered graphene grown by carbon implantation

NASA Astrophysics Data System (ADS)

Lee, Kin Kiong; McCallum, Jeffrey C.; Jamieson, David N.

2014-02-01

Graphene is considered to be a very promising material for applications in nanotechnology. The properties of graphene are strongly dependent on defects that occur during growth and processing. These defects can be either detrimental or beneficial to device performance depending on defect type, location and device application. Here we present experimental results on formation of few-layered graphene by carbon ion implantation into nickel films and characteristics of graphene devices formed by graphene transfer and lithographic patterning. Micro-Raman spectroscopy was used to determine the number of graphene layers formed and identify defects arising from the device processing. The graphene films were cleaned by annealing in vacuum. Transport properties of cleaned graphene films were investigated by fabrication of back-gated field-effect transistors, which exhibited high hole and electron mobility of 1935 and 1905 cm2/Vs, respectively.

Growing vertical ZnO nanorod arrays within graphite: efficient isolation of large size and high quality single-layer graphene.

PubMed

Ding, Ling; E, Yifeng; Fan, Louzhen; Yang, Shihe

2013-07-18

We report a unique strategy for efficiently exfoliating large size and high quality single-layer graphene directly from graphite into DMF dispersions by growing ZnO nanorod arrays between the graphene layers in graphite.

Reducing graphene device variability with yttrium sacrificial layers

NASA Astrophysics Data System (ADS)

Wang, Ning C.; Carrion, Enrique A.; Tung, Maryann C.; Pop, Eric

2017-05-01

Graphene technology has made great strides since the material was isolated more than a decade ago. However, despite improvements in growth quality and numerous "hero" devices, challenges of uniformity remain, restricting the large-scale development of graphene-based technologies. Here, we investigate and reduce the variability of graphene transistors by studying the effects of contact metals (with and without a Ti layer), resist, and yttrium (Y) sacrificial layers during the fabrication of hundreds of devices. We find that with optical photolithography, residual resist and process contamination are unavoidable, ultimately limiting the device performance and yield. However, using Y sacrificial layers to isolate the graphene from processing conditions improves the yield (from 73% to 97%), the average device performance (three-fold increase of mobility and 58% lower contact resistance), and the device-to-device variability (standard deviation of Dirac voltage reduced by 20%). In contrast to other sacrificial layer techniques, the removal of the Y sacrificial layer with dilute HCl does not harm surrounding materials, simplifying large-scale graphene fabrication.

Mass production of highly-porous graphene for high-performance supercapacitors

NASA Astrophysics Data System (ADS)

Amiri, Ahmad; Shanbedi, Mehdi; Ahmadi, Goodarz; Eshghi, Hossein; Kazi, S. N.; Chew, B. T.; Savari, Maryam; Zubir, Mohd Nashrul Mohd

2016-09-01

This study reports on a facile and economical method for the scalable synthesis of few-layered graphene sheets by the microwave-assisted functionalization. Herein, single-layered and few-layered graphene sheets were produced by dispersion and exfoliation of functionalized graphite in ethylene glycol. Thermal treatment was used to prepare pure graphene without functional groups, and the pure graphene was labeled as thermally-treated graphene (T-GR). The morphological and statistical studies about the distribution of the number of layers showed that more than 90% of the flakes of T-GR had less than two layers and about 84% of T-GR were single-layered. The microwave-assisted exfoliation approach presents us with a possibility for a mass production of graphene at low cost and great potentials in energy storage applications of graphene-based materials. Owing to unique surface chemistry, the T-GR demonstrates an excellent energy storage performance, and the electrochemical capacitance is much higher than that of the other carbon-based nanostructures. The nanoscopic porous morphology of the T-GR-based electrodes made a significant contribution in increasing the BET surface as well as the specific capacitance of graphene. T-GR, with a capacitance of 354.1 Fg-1 at 5 mVs-1 and 264 Fg-1 at 100 mVs-1, exhibits excellent performance as a supercapacitor.

Tailoring graphene-based electrodes from semiconducting to metallic to increase the energy density in supercapacitors.

PubMed

Vatamanu, Jenel; Ni, Xiaojuan; Liu, Feng; Bedrov, Dmitry

2015-11-20

The semiconducting character of graphene and some carbon-based electrodes can lead to noticeably lower total capacitances and stored energy densities in electric double layer (EDL)capacitors. This paper discusses the chemical and electronic structure modifications that enhance the available energy bands, density of states and quantum capacitance of graphene substrates near the Fermi level, therefore restoring the conducting character of these materials. The doping of graphene with p or n dopants, such as boron and nitrogen atoms, or the introduction of vacancy defects that introduce zigzag edges, can significantly increase the quantum capacitance within the potential range of interest for the energy storage applications by either shifting the Dirac point away from the Fermi level or by eliminating the Dirac point. We show that a combination of doping and vacancies at realistic concentrations is sufficient to increase the capacitance of a graphene-based electrode to within 1 μF cm(−2) from that of a metallic surface.Using a combination of ab initio calculations and classical molecular dynamics simulations we estimate how the changes in the quantum capacitance of these electrode materials affect the total capacitance stored by the open structure EDL capacitors containing room temperature ionic liquid electrolytes.

Hexagonal boron nitride intercalated multi-layer graphene: a possible ultimate solution to ultra-scaled interconnect technology

NASA Astrophysics Data System (ADS)

Li, Yong-Jun; Sun, Qing-Qing; Chen, Lin; Zhou, Peng; Wang, Peng-Fei; Ding, Shi-Jin; Zhang, David Wei

2012-03-01

We proposed intercalation of hexagonal boron nitride (hBN) in multilayer graphene to improve its performance in ultra-scaled interconnects for integrated circuit. The effect of intercalated hBN layer in bilayer graphene is investigated using non-equilibrium Green's functions. We find the hBN intercalated bilayer graphene exhibit enhanced transport properties compared with pristine bilayer ones, and the improvement is attributed to suppression of interlayer scattering and good planar bonding condition of inbetween hBN layer. Based on these results, we proposed a via structure that not only benefits from suppressed interlayer scattering between multilayer graphene, but also sustains the unique electrical properties of graphene when many graphene layers are stacking together. The ideal current density across the structure can be as high as 4.6×109 A/cm2 at 1V, which is very promising for the future high-performance interconnect.

Interaction driven quantum Hall effect in artificially stacked graphene bilayers

PubMed Central

Iqbal, Muhammad Zahir; Iqbal, Muhammad Waqas; Siddique, Salma; Khan, Muhammad Farooq; Ramay, Shahid Mahmood; Nam, Jungtae; Kim, Keun Soo; Eom, Jonghwa

2016-01-01

The honeycomb lattice structure of graphene gives rise to its exceptional electronic properties of linear dispersion relation and its chiral nature of charge carriers. The exceptional electronic properties of graphene stem from linear dispersion relation and chiral nature of charge carries, originating from its honeycomb lattice structure. Here, we address the quantum Hall effect in artificially stacked graphene bilayers and single layer graphene grown by chemical vapor deposition. The quantum Hall plateaus started to appear more than 3 T and became clearer at higher magnetic fields up to 9 T. Shubnikov-de Hass oscillations were manifestly observed in graphene bilayers texture. These unusual plateaus may have been due to the layers interaction in artificially stacked graphene bilayers. Our study initiates the understanding of interactions between artificially stacked graphene layers. PMID:27098387

Interaction driven quantum Hall effect in artificially stacked graphene bilayers.

PubMed

Iqbal, Muhammad Zahir; Iqbal, Muhammad Waqas; Siddique, Salma; Khan, Muhammad Farooq; Ramay, Shahid Mahmood; Nam, Jungtae; Kim, Keun Soo; Eom, Jonghwa

2016-04-21

The honeycomb lattice structure of graphene gives rise to its exceptional electronic properties of linear dispersion relation and its chiral nature of charge carriers. The exceptional electronic properties of graphene stem from linear dispersion relation and chiral nature of charge carries, originating from its honeycomb lattice structure. Here, we address the quantum Hall effect in artificially stacked graphene bilayers and single layer graphene grown by chemical vapor deposition. The quantum Hall plateaus started to appear more than 3 T and became clearer at higher magnetic fields up to 9 T. Shubnikov-de Hass oscillations were manifestly observed in graphene bilayers texture. These unusual plateaus may have been due to the layers interaction in artificially stacked graphene bilayers. Our study initiates the understanding of interactions between artificially stacked graphene layers.

Effect of layer number and metal-chloride dopant on multiple layers of graphene/porous Si solar cells

NASA Astrophysics Data System (ADS)

Shin, Dong Hee; Kim, Jong Min; Jang, Chan Wook; Kim, Ju Hwan; Kim, Sung; Choi, Suk-Ho

2018-03-01

Porous silicon (PSi) is an attractive building block for Si-based solar cells due to its low reflectance. Here, PSi is prepared by metal-assisted chemical etching of a Si wafer on which Au nanoparticles are formed by sputtering for 5 s. The layer number (Ln) of graphene is varied to optimize multiple layers of graphene/PSi Schottky junction solar cells because the sheet resistance, work function, transmittance, and reflectance of graphene strongly depend on Ln. At Ln = 2, the best condition for the highest power conversion efficiency (PCE), various metal chlorides are employed as dopants for graphene. The PCE is maximally enhanced to 9.15% by doping the graphene with RhCl3 and is reduced by only 20% of its original value (absolutely from 9.15% to 7.23%) during 10 days in air. These results are very meaningful in that even a single doping for graphene can be effective for achieving high PCE from graphene/PSi solar cells by controlling Ln.

Chemical and morphological modifications of single layer graphene submitted to annealing in water vapor

NASA Astrophysics Data System (ADS)

Rolim, Guilherme Koszeniewski; Corrêa, Silma Alberton; Galves, Lauren Aranha; Lopes, João Marcelo J.; Soares, Gabriel Vieira; Radtke, Cláudio

2018-01-01

Modifications of single layer graphene transferred to SiO2/Si substrates resulting from annealing in water vapor were investigated. Near edge X-ray absorption fine structure spectroscopy evidenced graphene puckering between 400 and 500 °C. Synchrotron radiation based X-ray photoelectron spectroscopy showed variation of sp2 and sp3C bonding configurations specially in this same temperature range. Moreover, oxygen related functionalities are formed as a result of water vapor annealing. Based on these results and complementary Raman and nuclear reaction analysis, one distinguishes three different regimes of water interaction with graphene concerning modifications of the graphene layer. In the low temperature range (200-400 °C), no prominent modification of graphene itself is observed. At higher temperatures (400-500 °C), to accommodate newly formed oxygen functionalities, the flat and continuous sp2 bonding network of graphene is disrupted, giving rise to a puckered layer. For 600 °C and above, shrinking of graphene domains and a higher doping level take place.

Incommensurate Graphene Foam as a High Capacity Lithium Intercalation Anode

PubMed Central

Paronyan, Tereza M.; Thapa, Arjun Kumar; Sherehiy, Andriy; Jasinski, Jacek B.; Jangam, John Samuel Dilip

2017-01-01

Graphite’s capacity of intercalating lithium in rechargeable batteries is limited (theoretically, 372 mAh g−1) due to low diffusion within commensurately-stacked graphene layers. Graphene foam with highly enriched incommensurately-stacked layers was grown and applied as an active electrode in rechargeable batteries. A 93% incommensurate graphene foam demonstrated a reversible specific capacity of 1,540 mAh g−1 with a 75% coulombic efficiency, and an 86% incommensurate sample achieves above 99% coulombic efficiency exhibiting 930 mAh g−1 specific capacity. The structural and binding analysis of graphene show that lithium atoms highly intercalate within weakly interacting incommensurately-stacked graphene network, followed by a further flexible rearrangement of layers for a long-term stable cycling. We consider lithium intercalation model for multilayer graphene where capacity varies with N number of layers resulting LiN+1C2N stoichiometry. The effective capacity of commonly used carbon-based rechargeable batteries can be significantly improved using incommensurate graphene as an anode material. PMID:28059110

Magnetoresistance effect in Fe{sub 20}Ni{sub 80}/graphene/Fe{sub 20}Ni{sub 80} vertical spin valves

DOE Office of Scientific and Technical Information (OSTI.GOV)

Entani, Shiro, E-mail: entani.shiro@qst.go.jp; Naramoto, Hiroshi; Sakai, Seiji

2016-08-22

Vertical spin valve devices with junctions of single- and bi-layer graphene interlayers sandwiched with Fe{sub 20}Ni{sub 80} (Permalloy) electrodes were fabricated by exploiting the direct growth of graphene on the Permalloy. The linear current-voltage characteristics indicated that ohmic contacts were realized at the interfaces. The systematic characterization revealed the significant modification of the electronic state of the interfacial graphene layer on the Permalloy surface, which indicates the strong interactions at the interface. The ohmic transport was attributable to the strong interface-interaction. The vertical resistivity of the graphene interlayer and the spin asymmetry coefficient at the graphene/Permalloy interface were obtained tomore » be 0.13 Ω cm and 0.06, respectively. It was found that the strong interface interaction modifies the electronic structure and metallic properties in the vertical spin valve devices with bi-layer graphene as well as single-layer graphene.« less

Potassium-doped n-type bilayer graphene

NASA Astrophysics Data System (ADS)

Yamada, Takatoshi; Okigawa, Yuki; Hasegawa, Masataka

2018-01-01

Potassium-doped n-type bilayer graphene was obtained. Chemical vapor deposited bilayer and single layer graphene on copper (Cu) foils were used. After etching of Cu foils, graphene was dipped in potassium hydroxide aqueous solutions to dope potassium. Graphene on silicon oxide was characterized by X-ray photoelectron spectroscopy (XPS), energy dispersive X-ray spectroscopy (EDX), and Raman spectroscopy. Both XPS and EDX spectra indicated potassium incorporation into the bilayer graphene via intercalation between the graphene sheets. The downward shift of the 2D peak position of bilayer graphene after the potassium hydroxide (KOH) treatment was confirmed in Raman spectra, indicating that the KOH-treated bilayer graphene was doped with electrons. Electrical properties were measured using Hall bar structures. The Dirac points of bilayer graphene were shifted from positive to negative by the KOH treatment, indicating that the KOH-treated bilayer graphene was n-type conduction. For single layer graphene after the KOH treatment, although electron doping was confirmed from Raman spectra, the peak of potassium in the X-ray photoelectron spectroscopy (XPS) spectrum was not detected. The Dirac points of single layer graphene with and without the KOH treatment showed positive.

Effect of Strong Acid Functional Groups on Electrode Rise Potential in Capacitive Mixing by Double Layer Expansion

DOE PAGES

Hatzell, Marta C.; Raju, Muralikrishna; Watson, Valerie J.; ...

2014-11-03

We report that the amount of salinity-gradient energy that can be obtained through capacitive mixing based on double layer expansion depends on the extent the electric double layer (EDL) is altered in a low salt concentration (LC) electrolyte (e.g., river water). We show that the electrode-rise potential, which is a measure of the EDL perturbation process, was significantly (P = 10 –5) correlated to the concentration of strong acid surface functional groups using five types of activated carbon. Electrodes with the lowest concentration of strong acids (0.05 mmol g –1) had a positive rise potential of 59 ± 4 mVmore » in the LC solution, whereas the carbon with the highest concentration (0.36 mmol g –1) had a negative rise potential (₋31 ± 5 mV). Chemical oxidation of a carbon (YP50) using nitric acid decreased the electrode rise potential from 46 ± 2 mV (unaltered) to ₋6 ± 0.5 mV (oxidized), producing a whole cell potential (53 ± 1.7 mV) that was 4.4 times larger than that obtained with identical electrode materials (from 12 ± 1 mV). Changes in the EDL were linked to the behavior of specific ions in a LC solution using molecular dynamics and metadynamics simulations. The EDL expanded in the LC solution when a carbon surface (pristine graphene) lacked strong acid functional groups, producing a positive-rise potential at the electrode. In contrast, the EDL was compressed for an oxidized surface (graphene oxide), producing a negative-rise electrode potential. In conclusion, these results established the linkage between rise potentials and specific surface functional groups (strong acids) and demonstrated on a molecular scale changes in the EDL using oxidized or pristine carbons.« less

Catalyst-free one step synthesis of large area vertically stacked N-doped graphene-boron nitride heterostructures from biomass source.

PubMed

Esteve-Adell, Ivan; He, Jinbao; Ramiro, Fernando; Atienzar, Pedro; Primo, Ana; García, Hermenegildo

2018-03-01

A procedure for the one-step preparation of films of few-layer N-doped graphene on top of nanometric hexagonal boron nitride sheets ((N)graphene/h-BN) based on the pyrolysis at 900 °C under an inert atmosphere of a film of chitosan containing about 20 wt% of ammonium borate salt as a precursor is reported. During the pyrolysis a spontaneous segregation of (N)graphene and boron nitride layers takes place. The films were characterized by optical microscopy that shows a thin graphene overlayer covering the boron nitride layer, the latter showing characteristic cracks, and by XPS measurements at different monitoring angles from 0° to 50° where an increase in the proportion of C vs. B and N was observed. The resulting (N)graphene/h-BN films were also characterized by Raman, HRTEM, SEM, FIB-SEM and AFM. The thickness of the (N)graphene and h-BN layers can be controlled by varying the concentration of precursors and the spin coating rate and is typically below 5 nm. Electrical conductivity measurements using microelectrodes can cause the burning of the graphene layer at high intensities, while lower intensities show that (N)graphene/h-BN films behave as capacitors in the range of positive voltages.

High-contrast terahertz wave modulation by gated graphene enhanced by extraordinary transmission through ring apertures.

PubMed

Gao, Weilu; Shu, Jie; Reichel, Kimberly; Nickel, Daniel V; He, Xiaowei; Shi, Gang; Vajtai, Robert; Ajayan, Pulickel M; Kono, Junichiro; Mittleman, Daniel M; Xu, Qianfan

2014-03-12

Gate-controllable transmission of terahertz (THz) radiation makes graphene a promising material for making high-speed THz wave modulators. However, to date, graphene-based THz modulators have exhibited only small on/off ratios due to small THz absorption in single-layer graphene. Here we demonstrate a ∼50% amplitude modulation of THz waves with gated single-layer graphene by the use of extraordinary transmission through metallic ring apertures placed right above the graphene layer. The extraordinary transmission induced ∼7 times near-filed enhancement of THz absorption in graphene. These results promise complementary metal-oxide-semiconductor compatible THz modulators with tailored operation frequencies, large on/off ratios, and high speeds, ideal for applications in THz communications, imaging, and sensing.

Rocking-Chair Configuration in Ultrathin Lithium Vanadate-Graphene Hybrid Nanosheets for Electrical Modulation

PubMed Central

Zhu, Haiou; Qin, Xinming; Sun, Xu; Yan, Wensheng; Yang, Jinlong; Xie, Yi

2013-01-01

The ability to control electronic property of a material by externally applied voltage is greatly anticipated in modern electronics, and graphene provide potential application foreground for this issue on account of its exotic ambipolar transport property. In this study, we proposed that inorganic-graphene intercalated nanosheet is an effective solution to optimize the transport property of graphene. As an example, lithium vanadate-graphene (LiVO-graphene) alternately intercalated nanosheets were designed and successfully synthesized. Theoretical calculation implied that its rocking chair configuration may provide a new pathway to switch the carrier in graphene layer between p-type and n-type while the position of embedded Li ions is controlled by an external field. Thus, a demo transistor was fabricated with layer-by-layer overlapping of LiVO-graphene nanosheets which proved that this inorganic-graphene structure could be used for electrical modulation in electronic devices. PMID:23409237

Clean Transfer of Wafer-Scale Graphene via Liquid Phase Removal of Polycyclic Aromatic Hydrocarbons.

PubMed

Kim, Hyun Ho; Kang, Boseok; Suk, Ji Won; Li, Nannan; Kim, Kwang S; Ruoff, Rodney S; Lee, Wi Hyoung; Cho, Kilwon

2015-05-26

Pentacene (C22H14), a polycyclic aromatic hydrocarbon, was used as both supporting and sacrificing layers for the clean and doping-free graphene transfer. After successful transfer of graphene to a target substrate, the pentacene layer was physically removed from the graphene surface by using intercalating organic solvent. This solvent-mediated removal of pentacene from graphene surface was investigated by both theoretical calculation and experimental studies with various solvents. The uses of pentacene and appropriate intercalation solvent enabled graphene transfer without forming a residue from the supporting layer. Such residues tend to cause charged impurity scattering and unintentional graphene doping effects. As a result, this clean graphene exhibited extremely homogeneous surface potential profiles over a large area. A field-effect transistor fabricated using this graphene displayed a high hole (electron) mobility of 8050 cm(2)/V·s (9940 cm(2)/V·s) with a nearly zero Dirac point voltage.

Electronic screening in stacked graphene flakes revealed by scanning tunneling microscopy

NASA Astrophysics Data System (ADS)

Feng, Xiaofeng; Salmeron, Miquel

2013-02-01

Electronic doping and screening effects in stacked graphene flakes on Ru and Cu substrates have been observed using scanning tunneling microscopy (STM). The screening affects the apparent STM height of each flake in successive layers reflecting the density of states near the Fermi level and thus the doping level. It is revealed in this way that the strong doping of the first graphene layer on Ru(0001) is attenuated in the second one, and almost eliminated in the third and fourth layers. Similar effect is also observed in graphene flakes on Cu(111). In contrast, the strong doping effect is suppressed immediately by a water layer intercalated between the graphene and Ru.

Protecting nickel with graphene spin-filtering membranes: A single layer is enough

DOE Office of Scientific and Technical Information (OSTI.GOV)

Martin, M.-B.; Dlubak, B.; Piquemal-Banci, M.

2015-07-06

We report on the demonstration of ferromagnetic spin injectors for spintronics which are protected against oxidation through passivation by a single layer of graphene. The graphene monolayer is directly grown by catalytic chemical vapor deposition on pre-patterned nickel electrodes. X-ray photoelectron spectroscopy reveals that even with its monoatomic thickness, monolayer graphene still efficiently protects spin sources against oxidation in ambient air. The resulting single layer passivated electrodes are integrated into spin valves and demonstrated to act as spin polarizers. Strikingly, the atom-thick graphene layer is shown to be sufficient to induce a characteristic spin filtering effect evidenced through the signmore » reversal of the measured magnetoresistance.« less

Monolayer and/or few-layer graphene on metal or metal-coated substrates

DOEpatents

Sutter, Peter Werner; Sutter, Eli Anguelova

2015-04-14

Disclosed is monolayer and/or few-layer graphene on metal or metal-coated substrates. Embodiments include graphene mirrors. In an example, a mirror includes a substrate that has a surface exhibiting a curvature operable to focus an incident beam onto a focal plane. A graphene layer conformally adheres to the substrate, and is operable to protect the substrate surface from degradation due to the incident beam and an ambient environment.

Improving Fire Resistance of Cotton Fabric through Layer-by-Layer Assembled Graphene Multilayer Nanocoating

NASA Astrophysics Data System (ADS)

Jang, Wonjun; Chung, Il Jun; Kim, Junwoo; Seo, Seongmin; Park, Yong Tae; Choi, Kyungwho

2018-05-01

In this study, thin films containing poly(vinyl alcohol) (PVA) and graphene nanoplatelets (GNPs), stabilized with poly(4-styrene-sulfonic acid) (PSS), were assembled by a simple and cost-effective layer-by-layer (LbL) technique in order to introduce the anti-flammability to cotton. These antiflammable layers were characterized by using UV-vis spectrometry and quartz crystal microbalance as a function of the number of bilayers deposited. Scanning electron microscopy was used to visualize the morphology of the thin film coatings on the cotton fabric. The graphene-polymer thin films introduced anti-flammable properties through thermally stable carbonaceous layers at a high temperature. The thermal stability and flame retardant property of graphene-coated cotton was demonstrated by thermogravimetric analysis, cone calorimetry, and vertical flame test. The results indicate that LbL-assembled graphene-polymer thin films can be applied largely in the field of flame retardant.

Interlayer interaction and mechanical properties in multi-layer graphene, Boron-Nitride, Aluminum-Nitride and Gallium-Nitride graphene-like structure: A quantum-mechanical DFT study

NASA Astrophysics Data System (ADS)

Ghorbanzadeh Ahangari, Morteza; Fereidoon, A.; Hamed Mashhadzadeh, Amin

2017-12-01

In present study, we investigated mechanical, electronic and interlayer properties of mono, bi and 3layer of Boron-Nitride (B-N), Aluminum-Nitride (Al-N) and Gallium-Nitride (Ga-N) graphene sheets and compared these results with results obtained from carbonic graphenes (C-graphenes). For reaching this purpose, first we optimized the geometrical parameters of these graphenes by using density functional theory (DFT) method. Then we calculated Young's modulus of graphene sheet by compressing and then elongating these sheets in small increment. Our results indicates that Young's modulus of graphenes didn't changed obviously by increasing the number of layer sheet. We also found that carbonic graphene has greatest Young's modulus among another mentioned sheets because of smallest equilibrium distance between its elements. Next we modeled the van der Waals interfacial interaction exist between two sheets with classical spring model by using general form of Lennard-Jones (L-J) potential for all of mentioned graphenes. For calculating L-J parameters (ε and σ), the potential energy between layers of mentioned graphene as a function of the separation distance was plotted. Moreover, the density of states (DOS) are calculated to understand the electronic properties of these systems better.

Layer-by-layer evolution of structure, strain, and activity for the oxygen evolution reaction in graphene-templated Pt monolayers.

PubMed

Abdelhafiz, Ali; Vitale, Adam; Joiner, Corey; Vogel, Eric; Alamgir, Faisal M

2015-03-25

In this study, we explore the dimensional aspect of structure-driven surface properties of metal monolayers grown on a graphene/Au template. Here, surface limited redox replacement (SLRR) is used to provide precise layer-by-layer growth of Pt monolayers on graphene. We find that after a few iterations of SLRR, fully wetted 4-5 monolayer Pt films can be grown on graphene. Incorporating graphene at the Pt-Au interface modifies the growth mechanism, charge transfers, equilibrium interatomic distances, and associated strain of the synthesized Pt monolayers. We find that a single layer of sandwiched graphene is able to induce a 3.5% compressive strain on the Pt adlayer grown on it, and as a result, catalytic activity is increased due to a greater areal density of the Pt layers beyond face-centered-cubic close packing. At the same time, the sandwiched graphene does not obstruct vicinity effects of near-surface electron exchange between the substrate Au and adlayers Pt. X-ray photoelectron spectroscopy (XPS) and extended X-ray absorption fine structure (EXAFS) techniques are used to examine charge mediation across the Pt-graphene-Au junction and the local atomic arrangement as a function of the Pt adlayer dimension. Cyclic voltammetry (CV) and the oxygen reduction reaction (ORR) are used as probes to examine the electrochemically active area of Pt monolayers and catalyst activity, respectively. Results show that the inserted graphene monolayer results in increased activity for the Pt due to a graphene-induced compressive strain, as well as a higher resistance against loss of the catalytically active Pt surface.

Drude conductivity exhibited by chemically synthesized reduced graphene oxide

NASA Astrophysics Data System (ADS)

Younas, Daniyal; Javed, Qurat-ul-Ain; Fatima, Sabeen; Kalsoom, Riffat; Abbas, Hussain; Khan, Yaqoob

2017-09-01

Electrical conductance in graphene layers having Drude like response due to massless Dirac fermions have been well explained theoretically as well as experimentally. In this paper Drude like electrical conductivity response of reduced graphene oxide synthesized by chemical route is presented. A method slightly different from conventional methods is used to synthesize graphene oxide which is then converted to reduced graphene oxide. Various analytic techniques were employed to verify the successful oxidation and reductions in the process and were also used to measure various parameters like thickness of layers and conductivity. Obtained reduced graphene oxide has very thin layers of thickness around 13 nm on average and reduced graphene oxide has average thickness below 20 nm. Conductivity of the reduced graphene was observed to have Drude like response which is explained on basis of Drude model for conductors.

Design and comparative study of vertical LEDs with graphene, ITO and Ni/Au as contact/current spreading layer

NASA Astrophysics Data System (ADS)

Singh, Sumitra; Mahala, Pramila; Pal, Suchandan

2018-01-01

This work evaluates the effect of graphene, indium tin oxide (ITO) and Ni/Au as contact/current spreading layer/current spreading layer for GaN vertical light emitting diodes (V-LEDs). In this simulation study, the effect of these contact/current spreading layers on different performance parameters of GaN V-LEDs has been studied. By using these three different types of contact/current spreading layers, we have comparatively studied the effect on light extraction efficiency (LEE), optical output power, wall plug efficiency and radiant intensity of V-LEDs. As per the simulation results, it shows that using graphene contact/current spreading layers, it is possible to achieve better performance than using ITO and Ni/Au contact/current spreading layers. For graphene/(Ni/Au) contact/current spreading layers, the LEE is improved by 36.77% whereas for ITO/(Ni/Au) contact/current spreading layers it is improved by 13.74%. Also, by using graphene/(Ni/Au) contact/current spreading layers, the optical output power of LEDs improved by 11.11% whereas for ITO/(Ni/Au) contact/current spreading layers shown 4.16% improvement. The radiant intensity is enhanced by 37.65% for graphene/(Ni/Au) contact/current spreading layers and 13.5% for ITO/(Ni/Au) contact/current spreading layers. In this report, we have given a detailed analysis of the obtained simulation results. The simulation was carried out in SimuLED tool.

Large-area, freestanding, single-layer graphene-gold: a hybrid plasmonic nanostructure.

PubMed

Iyer, Ganjigunte R Swathi; Wang, Jian; Wells, Garth; Guruvenket, Srinivasan; Payne, Scott; Bradley, Michael; Borondics, Ferenc

2014-06-24

Graphene-based plasmonic devices have recently drawn great attention. However, practical limitations in fabrication and device architectures prevent studies from being carried out on the intrinsic properties of graphene and their change by plasmonic structures. The influence of a quasi-infinite object (i.e., the substrate) on graphene, being a single sheet of carbon atoms, and the plasmonic device is overwhelming. To address this and put the intrinsic properties of the graphene-plasmonic nanostructures in focus, we fabricate large-area, freestanding, single-layer graphene-gold (LFG-Au) sandwich structures and Au nanoparticle decorated graphene (formed via thermal treatment) hybrid plasmonic nanostructures. We observed two distinct plasmonic enhancement routes of graphene unique to each structure via surface-enhanced Raman spectroscopy. The localized electronic structure variation in the LFG due to graphene-Au interaction at the nanoscale is mapped using scanning transmission X-ray microscopy. The measurements show an optical density of ∼0.007, which is the smallest experimentally determined for single-layer graphene thus far. Our results on freestanding graphene-Au plasmonic structures provide great insight for the rational design and future fabrication of graphene plasmonic hybrid nanostructures.

Organic solar cells with graphene electrodes and vapor printed poly(3,4-ethylenedioxythiophene) as the hole transporting layers.

PubMed

Park, Hyesung; Howden, Rachel M; Barr, Miles C; Bulović, Vladimir; Gleason, Karen; Kong, Jing

2012-07-24

For the successful integration of graphene as a transparent conducting electrode in organic solar cells, proper energy level alignment at the interface between the graphene and the adjacent organic layer is critical. The role of a hole transporting layer (HTL) thus becomes more significant due to the generally lower work function of graphene compared to ITO. A commonly used HTL material with ITO anodes is poly(3,4-ethylenedioxythiophene) (PEDOT) with poly(styrenesulfonate) (PSS) as the solid-state dopant. However, graphene's hydrophobic surface renders uniform coverage of PEDOT:PSS (aqueous solution) by spin-casting very challenging. Here, we introduce a novel, yet simple, vapor printing method for creating patterned HTL PEDOT layers directly onto the graphene surface. Vapor printing represents the implementation of shadow masking in combination with oxidative chemical vapor deposition (oCVD). The oCVD method was developed for the formation of blanket (i.e., unpatterened) layers of pure PEDOT (i.e., no PSS) with systematically variable work function. In the unmasked regions, vapor printing produces complete, uniform, smooth layers of pure PEDOT over graphene. Graphene electrodes were synthesized under low-pressure chemical vapor deposition (LPCVD) using a copper catalyst. The use of another electron donor material, tetraphenyldibenzoperiflanthene, instead of copper phthalocyanine in the organic solar cells also improves the power conversion efficiency. With the vapor printed HTL, the devices using graphene electrodes yield comparable performances to the ITO reference devices (η(p,LPCVD) = 3.01%, and η(p,ITO) = 3.20%).

Layer speciation and electronic structure investigation of freestanding hexagonal boron nitride nanosheets

NASA Astrophysics Data System (ADS)

WangEqual Contribution To This Work., Jian; Wang, Zhiqiang; Cho, Hyunjin; Kim, Myung Jong; Sham, T. K.; Sun, Xuhui

2015-01-01

Chemical imaging, thickness mapping, layer speciation and polarization dependence have been performed on single and multilayered (up to three layers and trilayered nanosheets overlapping to form 6 and 9 layers) hexagonal boron nitride (hBN) nanosheets by scanning transmission X-ray microscopy. Spatially-resolved XANES directly from freestanding regions of different layers has been extracted and compared with sample normal and 30° tilted configurations. Notably a double feature σ* excitonic state and a stable high energy σ* state were observed at the boron site in addition to the intense π* excitonic state. The boron projected σ* DOS, especially the first σ* exciton, is sensitive to surface modification, particularly in the single layered hBN nanosheet which shows more significant detectable contaminants and defects such as tri-coordinated boron/nitrogen oxide. The nitrogen site has shown very weak or no excitonic character. The distinct excitonic effect on boron and nitrogen was interpreted to the partly ionic state of hBN. Bulk XANES of hBN nanosheets was also measured to confirm the spectro-microscopic STXM result. Finally, the unoccupied electronic structures of hBN and graphene were compared.Chemical imaging, thickness mapping, layer speciation and polarization dependence have been performed on single and multilayered (up to three layers and trilayered nanosheets overlapping to form 6 and 9 layers) hexagonal boron nitride (hBN) nanosheets by scanning transmission X-ray microscopy. Spatially-resolved XANES directly from freestanding regions of different layers has been extracted and compared with sample normal and 30° tilted configurations. Notably a double feature σ* excitonic state and a stable high energy σ* state were observed at the boron site in addition to the intense π* excitonic state. The boron projected σ* DOS, especially the first σ* exciton, is sensitive to surface modification, particularly in the single layered hBN nanosheet which shows more significant detectable contaminants and defects such as tri-coordinated boron/nitrogen oxide. The nitrogen site has shown very weak or no excitonic character. The distinct excitonic effect on boron and nitrogen was interpreted to the partly ionic state of hBN. Bulk XANES of hBN nanosheets was also measured to confirm the spectro-microscopic STXM result. Finally, the unoccupied electronic structures of hBN and graphene were compared. Electronic supplementary information (ESI) available. See DOI: 10.1039/c4nr04445b

A flexible and transparent graphene/ZnO nanorod hybrid structure fabricated by exfoliating a graphite substrate.

PubMed

Nam, Gwang-Hee; Baek, Seong-Ho; Cho, Chang-Hee; Park, Il-Kyu

2014-10-21

We demonstrate the fabrication of a graphene/ZnO nanorod (NR) hybrid structure by mechanical exfoliation of ZnO NRs grown on a graphite substrate. We confirmed the existence of graphene sheets on the hybrid structure by analyzing the Raman spectra and current-voltage (I-V) characteristics. The Raman spectra of the exfoliated graphene/ZnO NR hybrid structure show G and 2D band peaks that are shifted to lower wavenumbers, indicating that the exfoliated graphene layer exists under a significant amount of strain. The I-V characteristics of the graphene/ZnO NR hybrid structure show current flow through the graphene layer, while no current flow is observed on the ZnO NR/polydimethylsiloxane (PDMS) composite without graphene, thereby indicating that the few-layer graphene was successfully transferred onto the hybrid structure. A piezoelectric nanogenerator is demonstrated by using the fabricated graphene/ZnO NR hybrid structure. The nanogenerator exhibits stable output voltage up to 3.04 V with alternating current output characteristics.

Application of graphene oxide in water treatment

NASA Astrophysics Data System (ADS)

Liu, Yongchen

2017-11-01

Graphene oxide has good hydrophilicity and has been tried to use it into thin films for water treatment in recent years. In this paper, the preparation methods of graphene oxide membrane are reviewed, including vacuum suction filtration, spray coating, spin coating, dip coating and the layer by layer method. Secondly, the mechanism of mass transfer of graphene membrane is introduced in detail. The application of the graphene oxide membrane, modified graphene oxide membrane and graphene hybrid membranes were discussed in RO, vaporization, nanofiltration and other aspects. Finally, the development and application of graphene membrane in water treatment were discussed.

A platform for large-scale graphene electronics--CVD growth of single-layer graphene on CVD-grown hexagonal boron nitride.

PubMed

Wang, Min; Jang, Sung Kyu; Jang, Won-Jun; Kim, Minwoo; Park, Seong-Yong; Kim, Sang-Woo; Kahng, Se-Jong; Choi, Jae-Young; Ruoff, Rodney S; Song, Young Jae; Lee, Sungjoo

2013-05-21

Direct chemical vapor deposition (CVD) growth of single-layer graphene on CVD-grown hexagonal boron nitride (h-BN) film can suggest a large-scale and high-quality graphene/h-BN film hybrid structure with a defect-free interface. This sequentially grown graphene/h-BN film shows better electronic properties than that of graphene/SiO2 or graphene transferred on h-BN film, and suggests a new promising template for graphene device fabrication. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Method of preparing graphene-sulfur nanocomposites for rechargeable lithium-sulfur battery electrodes

DOEpatents

Liu, Jun; Lemmon, John P; Yang, Zhenguo; Cao, Yuliang; Li, Xiaolin

2015-04-07

A method of preparing a graphene-sulfur nanocomposite for a cathode in a rechargeable lithium-sulfur battery comprising thermally expanding graphite oxide to yield graphene layers, mixing the graphene layers with a first solution comprising sulfur and carbon disulfide, evaporating the carbon disulfide to yield a solid nanocomposite, and grinding the solid nanocomposite to yield the graphene-sulfur nanocomposite. Rechargeable-lithium-sulfur batteries having a cathode that includes a graphene-sulfur nanocomposite can exhibit improved characteristics. The graphene-sulfur nanocomposite can be characterized by graphene sheets with particles of sulfur adsorbed to the graphene sheets. The sulfur particles have an average diameter of less than 50 nm.

First-principles study of graphene under c-HfO{sub 2}(111) layers: Electronic structures and transport properties

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kaneko, Tomoaki, E-mail: kaneko@flex.phys.tohoku.ac.jp; Materials Research Consortium for Energy Efficient Electronic Devices; Ohno, Takahisa, E-mail: OHNO.Takahisa@nims.go.jp

2016-08-22

We investigated the electronic properties, stability, and transport of graphene under c-HfO{sub 2}(111) layers by performing first-principles calculations with special attention to the chemical bonding between graphene and HfO{sub 2} surfaces. When the interface of HfO{sub 2}/graphene is terminated by an O layer, the linear dispersion of graphene is preserved and the degradation of transport is suppressed. For other interface structures, HfO{sub 2} is tightly adsorbed on graphene and the transport is strictly limited. In terms of the stability of the interface structures, an O-terminated interface is preferable, which is achieved under an O-deficient condition.

Polyelectrolyte/Graphene Oxide Barrier Film for Flexible OLED.

PubMed

Yang, Seung-Yeol; Park, Jongwhan; Kim, Yong-Seog

2015-10-01

Ultra-thin flexible nano-composite barrier layer consists of graphene oxide and polyelectrolyte was prepared using the layer-by-layer processing method. Microstructures of the barrier layer was optimized via modifying coating conditions and inducing chemical reactions. Although the barrier layer consists of hydrophilic polyelectrolyte was not effective in blocking the water vapor permeation, the chemical reduction of graphene oxide as well as conversion of polyelectrolyte to hydrophobic nature were very effective in reducing the permeation.

Laser induced forward transfer of graphene

NASA Astrophysics Data System (ADS)

Smits, Edsger C. P.; Walter, Arnaud; de Leeuw, Dago M.; Asadi, Kamal

2017-10-01

Transfer of graphene and other two-dimensional materials is still a technical challenge. The 2D-materials are typically patterned after transfer, which leads to a major loss of material. Here, we present laser induced forward transfer of chemical vapor deposition grown graphene layers with well-defined shapes and geometries. The transfer is based on photo-decomposition of a triazene-based transfer layer that produces N2 gas, which propels a graphene layer from the donor to the acceptor substrate. The functionality of the graphene-metal junction was verified by realizing functional bottom contact bottom gate field-effect transistors.

Selective growth of Pb islands on graphene/SiC buffer layers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, X. T.; Miao, Y. P.; Ma, D. Y.

2015-02-14

Graphene is fabricated by thermal decomposition of silicon carbide (SiC) and Pb islands are deposited by Pb flux in molecular beam epitaxy chamber. It is found that graphene domains and SiC buffer layer coexist. Selective growth of Pb islands on SiC buffer layer rather than on graphene domains is observed. It can be ascribed to the higher adsorption energy of Pb atoms on the 6√(3) reconstruction of SiC. However, once Pb islands nucleate on graphene domains, they will grow very large owing to the lower diffusion barrier of Pb atoms on graphene. The results are consistent with first-principle calculations. Sincemore » Pb atoms on graphene are nearly free-standing, Pb islands grow in even-number mode.« less

Controlled surface oxidation of multi-layered graphene anode to increase hole injection efficiency in organic electronic devices

NASA Astrophysics Data System (ADS)

Han, Tae-Hee; Kwon, Sung-Joo; Seo, Hong-Kyu; Lee, Tae-Woo

2016-03-01

Ultraviolet ozone (UVO) surface treatment of graphene changes its sp2-hybridized carbons to sp3-bonded carbons, and introduces oxygen-containing components. Oxidized graphene has a finite energy band gap, so UVO modification of the surface of a four-layered graphene anode increases its surface ionization potential up to ∼5.2 eV and improves the hole injection efficiency (η) in organic electronic devices by reducing the energy barrier between the graphene anode and overlying organic layers. By controlling the conditions of the UVO treatment, the electrical properties of the graphene can be tuned to improve η. This controlled surface modification of the graphene will provide a way to achieve efficient and stable flexible displays and solid-state lighting.

Resonant tunneling structures based on epitaxial graphene on SiC

NASA Astrophysics Data System (ADS)

Nguyen, V. Hung; Bournel, A.; Dollfus, P.

2011-12-01

Recently some experiments have suggested that graphene epitaxially grown on SiC can exhibit an energy bandgap of 260 meV, which enhances the potential of this material for electronic applications. On this basis, we propose to use spatial doping to generate graphene-on-SiC double-barrier structures. The non-equilibrium Green's function technique for solving the massive Dirac model is applied to highlight typical transport phenomena such as the electron confinement and the resonant tunneling effects. The I-V characteristics of graphene resonant tunneling diodes were then investigated and the effect of different device parameters was discussed. It is finally shown that this kind of double-barrier junction provides an efficient way to confine the charge carriers in graphene and to design graphene resonant tunneling structures.

Unfolding energy spectra of double-periodicity two-dimensional systems: Twisted bilayer graphene and MoS2 on graphene

NASA Astrophysics Data System (ADS)

Matsushita, Yu-ichiro; Nishi, Hirofumi; Iwata, Jun-ichi; Kosugi, Taichi; Oshiyama, Atsushi

2018-01-01

We propose an unfolding scheme to analyze energy spectra of complex large-scale systems which are inherently of double periodicity on the basis of the density-functional theory. Applying our method to a twisted bilayer graphene (tBLG) and a stack of monolayer MoS2 on graphene (MoS2/graphene) as examples, we first show that the conventional unfolding scheme in the past using a single primitive-cell representation causes serious problems in analyses of the energy spectra. We then introduce our multispace representation scheme in the unfolding method and clarify its validity. Velocity renormalization of Dirac electrons in tBLG and mini gaps of Dirac cones in MoS2/graphene are elucidated in the present unfolding scheme.

Role of graphene inter layer on the formation of the MoS2-CZTS interface during growth

NASA Astrophysics Data System (ADS)

Vishwakarma, Manoj; Thota, Narayana; Karakulina, Olesia; Hadermann, Joke; Mehta, B. R.

2018-05-01

The growth of MoS2 layer near the Mo/CZTS interface during sulphurization process can have an impact on back contact cell parameters (series resistance and fill factor) depending upon the thickness or quality of MoS2. This study reports the dependence of the thickness of interfacial MoS2 layer on the growth of graphene at the interface between molybdenum back contact and deposited CZTS layer. The graphene layer reduces the accumulation of Zn/ZnS, Sn/SnO2 and formation of pores near the MoS2-CZTS interface. The use of graphene as interface layer can be potentially useful for improving the quality of Mo/MoS2/CZTS interface.

Multilayer Nanoporous Graphene Membranes for Water Desalination.

PubMed

Cohen-Tanugi, David; Lin, Li-Chiang; Grossman, Jeffrey C

2016-02-10

While single-layer nanoporous graphene (NPG) has shown promise as a reverse osmosis (RO) desalination membrane, multilayer graphene membranes can be synthesized more economically than the single-layer material. In this work, we build upon the knowledge gained to date toward single-layer graphene to explore how multilayer NPG might serve as a RO membrane in water desalination using classical molecular dynamic simulations. We show that, while multilayer NPG exhibits similarly promising desalination properties to single-layer membranes, their separation performance can be designed by manipulating various configurational variables in the multilayer case. This work establishes an atomic-level understanding of the effects of additional NPG layers, layer separation, and pore alignment on desalination performance, providing useful guidelines for the design of multilayer NPG membranes.

Graphene-on-semiconductor substrates for analog electronics

DOEpatents

Lagally, Max G.; Cavallo, Francesca; Rojas-Delgado, Richard

2016-04-26

Electrically conductive material structures, analog electronic devices incorporating the structures and methods for making the structures are provided. The structures include a layer of graphene on a semiconductor substrate. The graphene layer and the substrate are separated by an interfacial region that promotes transfer of charge carriers from the surface of the substrate to the graphene.

Magnetoresistance of vertical Co-graphene-NiFe junctions controlled by charge transfer and proximity-induced spin splitting in graphene

NASA Astrophysics Data System (ADS)

Asshoff, P. U.; Sambricio, J. L.; Rooney, A. P.; Slizovskiy, S.; Mishchenko, A.; Rakowski, A. M.; Hill, E. W.; Geim, A. K.; Haigh, S. J.; Fal'ko, V. I.; Vera-Marun, I. J.; Grigorieva, I. V.

2017-09-01

Graphene is hailed as an ideal material for spintronics due to weak intrinsic spin-orbit interaction that facilitates lateral spin transport and tunability of its electronic properties, including a possibility to induce magnetism in graphene. Another promising application of graphene is related to its use as a spacer separating ferromagnetic metals (FMs) in vertical magnetoresistive devices, the most prominent class of spintronic devices widely used as magnetic sensors. In particular, few-layer graphene was predicted to act as a perfect spin filter. Here we show that the role of graphene in such devices (at least in the absence of epitaxial alignment between graphene and the FMs) is different and determined by proximity-induced spin splitting and charge transfer with adjacent ferromagnetic metals, making graphene a weak FM electrode rather than a spin filter. To this end, we report observations of magnetoresistance (MR) in vertical Co-graphene-NiFe junctions with 1-4 graphene layers separating the ferromagnets, and demonstrate that the dependence of the MR sign on the number of layers and its inversion at relatively small bias voltages is consistent with spin transport between weakly doped and differently spin-polarized layers of graphene. The proposed interpretation is supported by the observation of an MR sign reversal in biased Co-graphene-hBN-NiFe devices and by comprehensive structural characterization. Our results suggest a new architecture for vertical devices with electrically controlled MR.

Ultra-large nonlinear parameter in graphene-silicon waveguide structures.

PubMed

Donnelly, Christine; Tan, Dawn T H

2014-09-22

Mono-layer graphene integrated with optical waveguides is studied for the purpose of maximizing E-field interaction with the graphene layer, for the generation of ultra-large nonlinear parameters. It is shown that the common approach used to minimize the waveguide effective modal area does not accurately predict the configuration with the maximum nonlinear parameter. Both photonic and plasmonic waveguide configurations and graphene integration techniques realizable with today's fabrication tools are studied. Importantly, nonlinear parameters exceeding 10(4) W(-1)/m, two orders of magnitude larger than that in silicon on insulator waveguides without graphene, are obtained for the quasi-TE mode in silicon waveguides incorporating mono-layer graphene in the evanescent part of the optical field. Dielectric loaded surface plasmon polariton waveguides incorporating mono-layer graphene are observed to generate nonlinear parameters as large as 10(5) W(-1)/m, three orders of magnitude larger than that in silicon on insulator waveguides without graphene. The ultra-large nonlinear parameters make such waveguides promising platforms for nonlinear integrated optics at ultra-low powers, and for previously unobserved nonlinear optical effects to be studied in a waveguide platform.

Three-dimensionally networked graphene hydroxide with giant pores and its application in supercapacitors

PubMed Central

Lee, Dongwook; Seo, Jiwon

2014-01-01

The three-dimensionally networked and layered structure of graphene hydroxide (GH) was investigated. After lengthy immersion in a NaOH solution, most of the epoxy groups in the graphene oxide were destroyed, and more hydroxyl groups were generated, transforming the graphene oxide into graphene hydroxide. Additionally, benzoic acid groups were formed, and the ether groups link the neighboring layers, creating a near-3D structure in the GH. To utilize these unique structural features, electrodes with large pores for use in supercapacitors were fabricated using thermal reduction in vacuum. The reduced GH maintained its layered structure and developed a lot of large of pores between/inside the layers. The GH electrodes exhibited high gravimetric as well as high volumetric capacitance. PMID:25492227

Three-dimensionally networked graphene hydroxide with giant pores and its application in supercapacitors

NASA Astrophysics Data System (ADS)

Lee, Dongwook; Seo, Jiwon

2014-12-01

The three-dimensionally networked and layered structure of graphene hydroxide (GH) was investigated. After lengthy immersion in a NaOH solution, most of the epoxy groups in the graphene oxide were destroyed, and more hydroxyl groups were generated, transforming the graphene oxide into graphene hydroxide. Additionally, benzoic acid groups were formed, and the ether groups link the neighboring layers, creating a near-3D structure in the GH. To utilize these unique structural features, electrodes with large pores for use in supercapacitors were fabricated using thermal reduction in vacuum. The reduced GH maintained its layered structure and developed a lot of large of pores between/inside the layers. The GH electrodes exhibited high gravimetric as well as high volumetric capacitance.

Three-dimensionally networked graphene hydroxide with giant pores and its application in supercapacitors.

PubMed

Lee, Dongwook; Seo, Jiwon

2014-12-10

The three-dimensionally networked and layered structure of graphene hydroxide (GH) was investigated. After lengthy immersion in a NaOH solution, most of the epoxy groups in the graphene oxide were destroyed, and more hydroxyl groups were generated, transforming the graphene oxide into graphene hydroxide. Additionally, benzoic acid groups were formed, and the ether groups link the neighboring layers, creating a near-3D structure in the GH. To utilize these unique structural features, electrodes with large pores for use in supercapacitors were fabricated using thermal reduction in vacuum. The reduced GH maintained its layered structure and developed a lot of large of pores between/inside the layers. The GH electrodes exhibited high gravimetric as well as high volumetric capacitance.

Synthesis of Different Layers of Graphene on Stainless Steel Using the CVD Method

NASA Astrophysics Data System (ADS)

Ghaemi, Ferial; Abdullah, Luqman Chuah; Tahir, Paridah Md; Yunus, Robiah

2016-11-01

In this study, different types of graphene, including single-, few-, and multi-layer graphene, were grown on a stainless steel (SS) mesh coated with Cu catalyst by using the chemical vapor deposition (CVD) method. Even though the SS mesh consisted of different types of metals, such as Fe, Ni, and Cr, which can also be used as catalysts, the reason for coating Cu catalyst on the SS surface had been related to the nature of the Cu, which promotes the growth of graphene with high quality and quantity at low temperature and time. The reaction temperature and run time, as the most important parameters of the CVD method, were varied, and thus led to the synthesis of different layers of graphene. Moreover, the presence of single-, few-, and multi-layer graphene was confirmed by employing two techniques, namely transmission electron microscopy (TEM) and Raman spectroscopy. On top of that, electron dispersive X-ray (EDX) was further applied to establish the influence of the CVD parameters on the growth of graphene.

In-plane heterostructures of graphene and hexagonal boron nitride with controlled domain sizes

NASA Astrophysics Data System (ADS)

Liu, Zheng; Ma, Lulu; Shi, Gang; Zhou, Wu; Gong, Yongji; Lei, Sidong; Yang, Xuebei; Zhang, Jiangnan; Yu, Jingjiang; Hackenberg, Ken P.; Babakhani, Aydin; Idrobo, Juan-Carlos; Vajtai, Robert; Lou, Jun; Ajayan, Pulickel M.

2013-02-01

Graphene and hexagonal boron nitride (h-BN) have similar crystal structures with a lattice constant difference of only 2%. However, graphene is a zero-bandgap semiconductor with remarkably high carrier mobility at room temperature, whereas an atomically thin layer of h-BN is a dielectric with a wide bandgap of ~5.9 eV. Accordingly, if precise two-dimensional domains of graphene and h-BN can be seamlessly stitched together, hybrid atomic layers with interesting electronic applications could be created. Here, we show that planar graphene/h-BN heterostructures can be formed by growing graphene in lithographically patterned h-BN atomic layers. Our approach can create periodic arrangements of domains with size ranging from tens of nanometres to millimetres. The resulting graphene/h-BN atomic layers can be peeled off the growth substrate and transferred to various platforms including flexible substrates. We also show that the technique can be used to fabricate two-dimensional devices, such as a split closed-loop resonator that works as a bandpass filter.

Synthesis of Different Layers of Graphene on Stainless Steel Using the CVD Method.

PubMed

Ghaemi, Ferial; Abdullah, Luqman Chuah; Tahir, Paridah Md; Yunus, Robiah

2016-12-01

In this study, different types of graphene, including single-, few-, and multi-layer graphene, were grown on a stainless steel (SS) mesh coated with Cu catalyst by using the chemical vapor deposition (CVD) method. Even though the SS mesh consisted of different types of metals, such as Fe, Ni, and Cr, which can also be used as catalysts, the reason for coating Cu catalyst on the SS surface had been related to the nature of the Cu, which promotes the growth of graphene with high quality and quantity at low temperature and time. The reaction temperature and run time, as the most important parameters of the CVD method, were varied, and thus led to the synthesis of different layers of graphene. Moreover, the presence of single-, few-, and multi-layer graphene was confirmed by employing two techniques, namely transmission electron microscopy (TEM) and Raman spectroscopy. On top of that, electron dispersive X-ray (EDX) was further applied to establish the influence of the CVD parameters on the growth of graphene.

Electrochemical exfoliation of graphite to stage-III graphite bisulfate flakes in low concentration sulfuric acid solution: A novel synthesis route to completely trilayer graphene suspension

NASA Astrophysics Data System (ADS)

Mir, Afkham; Shukla, Anupam

2018-06-01

Graphene produced from electrochemical exfoliation of graphite show a scatter in the number of layers. This scatter is a serious drawback for sensor and opto-electronic applications since the electronic properties of graphene change with number of layers. The scatter in the layer number of graphene is caused by formation of the intermediate graphite intercalation compounds (GIC) of different stage numbers as well as simultaneous cleaving of the GICs in the dispersion-unsuitable aqueous environment. In this work, we show the synthesis of stage-III graphite bisulfate (GB) enriched flakes by electrochemical exfoliation of graphite in low concentration (0.1 M) sulfuric acid from two different routes. We further show that the intercalated bisulfate planes provide sites for selective cleaving of the GB particles to trilayer graphene in DMF, a solvent favorable for graphene dispersion. Morphological characterizations show that while GB particles from one of the routes give graphene with a small scatter in the layer numbers, the other route provides a completely trilayer graphene dispersion. TEM and optical micrographs show graphene flakes have linear dimensions of several micrometers and a low aspect ratio suitable for use in sensor applications.

Gate-Tunable Spin Transport and Giant Electroresistance in Ferromagnetic Graphene Vertical Heterostructures

PubMed Central

Myoung, Nojoon; Park, Hee Chul; Lee, Seung Joo

2016-01-01

Controlling tunneling properties through graphene vertical heterostructures provides advantages in achieving large conductance modulation which has been known as limitation in lateral graphene device structures. Despite of intensive research on graphene vertical heterosturctures for recent years, the potential of spintronics based on graphene vertical heterostructures remains relatively unexplored. Here, we present an analytical device model for graphene-based spintronics by using ferromagnetic graphene in vertical heterostructures. We consider a normal or ferroelectric insulator as a tunneling layer. The device concept yields a way of controlling spin transport through the vertical heterostructures, resulting in gate-tunable spin-switching phenomena. Also, we revealed that a ‘giant’ resistance emerges through a ferroelectric insulating layer owing to the anti-parallel configuration of ferromagnetic graphene layers by means of electric fields via gate and bias voltages. Our findings discover the prospect of manipulating the spin transport properties in vertical heterostructures without use of magnetic fields. PMID:27126101

Enhanced photovoltaic performances of graphene/Si solar cells by insertion of a MoS₂ thin film.

PubMed

Tsuboi, Yuka; Wang, Feijiu; Kozawa, Daichi; Funahashi, Kazuma; Mouri, Shinichiro; Miyauchi, Yuhei; Takenobu, Taishi; Matsuda, Kazunari

2015-09-14

Transition-metal dichalcogenides exhibit great potential as active materials in optoelectronic devices because of their characteristic band structure. Here, we demonstrated that the photovoltaic performances of graphene/Si Schottky junction solar cells were significantly improved by inserting a chemical vapor deposition (CVD)-grown, large MoS2 thin-film layer. This layer functions as an effective electron-blocking/hole-transporting layer. We also demonstrated that the photovoltaic properties are enhanced with the increasing number of graphene layers and the decreasing thickness of the MoS2 layer. A high photovoltaic conversion efficiency of 11.1% was achieved with the optimized trilayer-graphene/MoS2/n-Si solar cell.

Salt-assisted direct exfoliation of graphite into high-quality, large-size, few-layer graphene sheets.

PubMed

Niu, Liyong; Li, Mingjian; Tao, Xiaoming; Xie, Zhuang; Zhou, Xuechang; Raju, Arun P A; Young, Robert J; Zheng, Zijian

2013-08-21

We report a facile and low-cost method to directly exfoliate graphite powders into large-size, high-quality, and solution-dispersible few-layer graphene sheets. In this method, aqueous mixtures of graphite and inorganic salts such as NaCl and CuCl2 are stirred, and subsequently dried by evaporation. Finally, the mixture powders are dispersed into an orthogonal organic solvent solution of the salt by low-power and short-time ultrasonication, which exfoliates graphite into few-layer graphene sheets. We find that the as-made graphene sheets contain little oxygen, and 86% of them are 1-5 layers with lateral sizes as large as 210 μm(2). Importantly, the as-made graphene can be readily dispersed into aqueous solution in the presence of surfactant and thus is compatible with various solution-processing techniques towards graphene-based thin film devices.

Mixing Of Mode Symmetries In Top Gated Bilayer And Multilayer Graphene Field Effect Devices

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chakraborty, Biswanath; Das, Anindya; Sood, A. K.

2011-07-15

We report Raman study to investigate the influence of stacking on the inversion symmetry breaking in top gated bi- and multi-layer ({approx}10 layers) graphene field effect transistors. The G phonon mode splits into a low frequency (G{sub low}) and a high frequency (G{sub high}) mode in bi- and multi-layer graphene and the two modes show different dependence on doping. The mode splitting is explained in terms of mixing of zone-center in-plane optical phonons representing in-phase and out-of-phase inter-layer atomic motions. Unlike in bilayer graphene, there is no transfer of intensity from G{sub low} to G{sub high} in multilayer graphene. Amore » comparison is made for the bilayer graphene data with the recent theory of Gava et al. [Phys. Rev. B 80, 155422 (2009)].« less

Landau quantization of Dirac fermions in graphene and its multilayers

NASA Astrophysics Data System (ADS)

Yin, Long-Jing; Bai, Ke-Ke; Wang, Wen-Xiao; Li, Si-Yu; Zhang, Yu; He, Lin

2017-08-01

When electrons are confined in a two-dimensional (2D) system, typical quantum-mechanical phenomena such as Landau quantization can be detected. Graphene systems, including the single atomic layer and few-layer stacked crystals, are ideal 2D materials for studying a variety of quantum-mechanical problems. In this article, we review the experimental progress in the unusual Landau quantized behaviors of Dirac fermions in monolayer and multilayer graphene by using scanning tunneling microscopy (STM) and scanning tunneling spectroscopy (STS). Through STS measurement of the strong magnetic fields, distinct Landau-level spectra and rich level-splitting phenomena are observed in different graphene layers. These unique properties provide an effective method for identifying the number of layers, as well as the stacking orders, and investigating the fundamentally physical phenomena of graphene. Moreover, in the presence of a strain and charged defects, the Landau quantization of graphene can be significantly modified, leading to unusual spectroscopic and electronic properties.

Design of a Tunable Ultra-Broadband Terahertz Absorber Based on Multiple Layers of Graphene Ribbons

NASA Astrophysics Data System (ADS)

Xu, Zenghui; Wu, Dong; Liu, Yumin; Liu, Chang; Yu, Zhongyuan; Yu, Li; Ye, Han

2018-05-01

We propose and numerically demonstrate an ultra-broadband graphene-based metamaterial absorber, which consists of multi-layer graphene/dielectric on the SiO2 layer supported by a metal substrate. The simulated result shows that the proposed absorber can achieve a near-perfect absorption above 90% with a bandwidth of 4.8 Thz. Owing to the flexible tunability of graphene sheet, the state of the absorber can be switched from on (absorption > 90%) to off (reflection > 90%) in the frequencies range of 3-7.8 Thz by controlling the Fermi energy of graphene. Moreover, the absorber is insensitive to the incident angles. The broadband absorption can be maintained over 90% up to 50°. Importantly, the design is scalable to develop broader tunable terahertz absorbers by adding more graphene layers which may have wide applications in imaging, sensors, photodetectors, and modulators.

Selenium-assisted controlled growth of graphene-Bi2Se3 nanoplates hybrid Dirac materials by chemical vapor deposition

NASA Astrophysics Data System (ADS)

Sun, Zhencui; Man, Baoyuan; Yang, Cheng; Liu, Mei; Jiang, Shouzhen; Zhang, Chao; Zhang, Jiaxin; Liu, Fuyan; Xu, Yuanyuan

2016-03-01

Se seed layers were used to synthesize the high-quality graphene-Bi2Se3 nanoplates hybrid Dirac materials via chemical vapor deposition (CVD) method. The morphology, crystallization and structural properties of the hybrid Dirac materials were characterized by SEM, EDS, Raman, XRD, AFM and HRTEM. The measurement results verify that the Se seed layer on the graphene surface can effectively saturate the surface dangling bonds of the graphene, which not only impel the uniform Bi2Se3 nanoplates growing along the horizontal direction but also can supply enough Se atoms to fill the Se vacancies. We also demonstrate the Se seed layer can effectively avoid the interaction of Bi2Se3 and the graphene. Further experiments testify the different Se seed layer on the graphene surface can be used to control the density of the Bi2Se3 nanoplates.

A pentacene monolayer trapped between graphene and a substrate.

PubMed

Zhang, Qicheng; Peng, Boyu; Chan, Paddy Kwok Leung; Luo, Zhengtang

2015-09-21

A self-assembled pentacene monolayer can be fabricated between the solid-solid interface of few-layered graphene (FLG) and the mica substrate, through a diffusion-spreading method. By utilizing a transfer method that allows us to sandwich pentacene between graphene and mica, followed by controlled annealing, we enabled the diffused pentacene to be trapped in the interfaces and led to the formation of a stable monolayer. We found that the formation of a monolayer is kinetically favored by using a 2D Ising lattice gas model for pentacene trapped between the graphene-substrate interfaces. This kinetic Monte Carlo simulation results indicate that, due to the graphene substrate enclosure, the spreading of the first layer proceeds faster than the second layer, as the kinetics favors the filling of voids by molecules from the second layer. This graphene assisted monolayer assembly method provides a new avenue for the fabrication of two-dimensional monolayer structures.

Work function of few layer graphene covered nickel thin films measured with Kelvin probe force microscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Eren, B.; Material Sciences Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720; Gysin, U.

2016-01-25

Few layer graphene and graphite are simultaneously grown on a ∼100 nm thick polycrystalline nickel film. The work function of few layer graphene/Ni is found to be 4.15 eV with a variation of 50 meV by local measurements with Kelvin probe force microscopy. This value is lower than the work function of free standing graphene due to peculiar electronic structure resulting from metal 3d-carbon 2p(π) hybridization.

Molecular dynamics simulation of amino acid ionic liquids near a graphene electrode: effects of alkyl side-chain length.

PubMed

Sadeghi Moghadam, Behnoosh; Razmkhah, Mohammad; Hamed Mosavian, Mohammad Taghi; Moosavi, Fatemeh

2016-12-07

Electric double layer (EDL) supercapacitors, using ionic liquid electrolytes, have been receiving a great deal of attention in response to the growing demand for energy storage systems. In the present study, the nanoscopic structure of amino acid ionic liquids (AAILs) as biodegradable electrolytes near a neutral graphene surface was studied by molecular dynamics (MD) simulation. In order to explore the influence of the anion type and structure, the effect of the alkyl side-chain length of amino acids on the EDL was investigated. The results for the AAILs, composed of 1-ethyl-3-methylimidazolium ([EMIM]) cations near alanine ([ALA]) and isoleucine ([ILE]) anions, were compared to a conventional electrolyte, [EMIM][PF 6 ]. A lower mobility of AAIL compared to [EMIM][PF 6 ], with diffusions as low as 10 -11 m 2 s -1 , was observed. The structural results demonstrated a layered structure near the surface and most of the adsorbed imidazolium cation rings lay flat on the graphene surface. Both MD and quantum computations were performed to shed light on the charge behavior of AAIL electrolytes. As the current results demonstrate, an increase in the anion side-chain length leads to a decrease in both the number of adsorbed ions on the surface and the thickness of the first adsorbed layer. More impressively, it was observed that a low charge concentration in the EDL of AAILs is due to more side-side interactions. This remarkable feature could introduce AAILs as more efficient electrolyte materials than conventional [EMIM][PF 6 ].

Ultrathin planar graphene supercapacitors.

PubMed

Yoo, Jung Joon; Balakrishnan, Kaushik; Huang, Jingsong; Meunier, Vincent; Sumpter, Bobby G; Srivastava, Anchal; Conway, Michelle; Reddy, Arava Leela Mohana; Yu, Jin; Vajtai, Robert; Ajayan, Pulickel M

2011-04-13

With the advent of atomically thin and flat layers of conducting materials such as graphene, new designs for thin film energy storage devices with good performance have become possible. Here, we report an "in-plane" fabrication approach for ultrathin supercapacitors based on electrodes comprised of pristine graphene and multilayer reduced graphene oxide. The in-plane design is straightforward to implement and exploits efficiently the surface of each graphene layer for energy storage. The open architecture and the effect of graphene edges enable even the thinnest of devices, made from as grown 1-2 graphene layers, to reach specific capacities up to 80 μFcm(-2), while much higher (394 μFcm(-2)) specific capacities are observed multilayer reduced graphene oxide electrodes. The performances of devices with pristine as well as thicker graphene-based structures are examined using a combination of experiments and model calculations. The demonstrated all solid-state supercapacitors provide a prototype for a broad range of thin-film based energy storage devices.

Schottky barrier contrasts in single and bi-layer graphene contacts for MoS{sub 2} field-effect transistors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Du, Hyewon; Kim, Taekwang; Shin, Somyeong

We have investigated single- and bi-layer graphene as source-drain electrodes for n-type MoS{sub 2} transistors. Ti-MoS{sub 2}-graphene heterojunction transistors using both single-layer MoS{sub 2} (1M) and 4-layer MoS{sub 2} (4M) were fabricated in order to compare graphene electrodes with commonly used Ti electrodes. MoS{sub 2}-graphene Schottky barrier provided electron injection efficiency up to 130 times higher in the subthreshold regime when compared with MoS{sub 2}-Ti, which resulted in V{sub DS} polarity dependence of device parameters such as threshold voltage (V{sub TH}) and subthreshold swing (SS). Comparing single-layer graphene (SG) with bi-layer graphene (BG) in 4M devices, SG electrodes exhibited enhancedmore » device performance with higher on/off ratio and increased field-effect mobility (μ{sub FE}) due to more sensitive Fermi level shift by gate voltage. Meanwhile, in the strongly accumulated regime, we observed opposing behavior depending on MoS{sub 2} thickness for both SG and BG contacts. Differential conductance (σ{sub d}) of 1M increases with V{sub DS} irrespective of V{sub DS} polarity, while σ{sub d} of 4M ceases monotonic growth at positive V{sub DS} values transitioning to ohmic-like contact formation. Nevertheless, the low absolute value of σ{sub d} saturation of the 4M-graphene junction demonstrates that graphene electrode could be unfavorable for high current carrying transistors.« less

Moving towards the magnetoelectric graphene transistor

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cao, Shi; Xiao, Zhiyong; Kwan, Chun -Pui

Here, the interfacial charge transfer between mechanically exfoliated few-layer graphene and Cr 2O 3 (0001) surfaces has been investigated. Electrostatic force microscopy and Kelvin probe force microscopy studies point to hole doping of few-layer graphene, with up to a 150 meV shift in the Fermi level, an aspect that is confirmed by Raman spectroscopy. Density functional theory calculations furthermore confirm the p-type nature of the graphene/chromia interface and suggest that the chromia is able to induce a significant carrier spin polarization in the graphene layer. A large magnetoelectrically controlled magneto-resistance can therefore be anticipated in transistor structures based on thismore » system, a finding important for developing graphene-based spintronic applications.« less

Moving towards the magnetoelectric graphene transistor

DOE PAGES

Cao, Shi; Xiao, Zhiyong; Kwan, Chun -Pui; ...

2017-10-30

Here, the interfacial charge transfer between mechanically exfoliated few-layer graphene and Cr 2O 3 (0001) surfaces has been investigated. Electrostatic force microscopy and Kelvin probe force microscopy studies point to hole doping of few-layer graphene, with up to a 150 meV shift in the Fermi level, an aspect that is confirmed by Raman spectroscopy. Density functional theory calculations furthermore confirm the p-type nature of the graphene/chromia interface and suggest that the chromia is able to induce a significant carrier spin polarization in the graphene layer. A large magnetoelectrically controlled magneto-resistance can therefore be anticipated in transistor structures based on thismore » system, a finding important for developing graphene-based spintronic applications.« less

Graphene enhanced surface plasmon resonance sensing based on Goos-Hänchen shift

NASA Astrophysics Data System (ADS)

Chen, Huifang; Tong, Jinguang; Wang, Yiqin; Jiang, Li

2018-03-01

A graphene/Ag structure is engineered as an enhanced platform for surface plasmon resonance sensing due to the high impermeability nature of graphene and the superior surface plasmon resonance performance of Ag. This structure is ultrasensitive to even tiny refractive index change of analytes based on Goos-Hänchen shift measurement compared to the traditional SPR sensor with bare Au film. The graphene/Ag configuration is consisted of five components, including BK7 glass slide, titanium thin film, silver thin film, two-dimensional graphene layers and biomolecular analyte layer. We have optimized the parameters of each layer and theoretically analyzed Goos-Hänchen shift of the plasmonic structure under surface plasmon resonance effect. The optimized graphene/Ag structure is monolayer graphene coated on Ag thin film with the thickness of 42 nm.

Charge Induced Dynamics of Water in a Graphene–Mica Slit Pore

PubMed Central

2017-01-01

We use atomic force microscopy to in situ investigate the dynamic behavior of confined water at the interface between graphene and mica. The graphene is either uncharged, negatively charged, or positively charged. At high humidity, a third water layer will intercalate between graphene and mica. When graphene is negatively charged, the interface fills faster with a complete three layer water film, compared to uncharged graphene. As charged positively, the third water layer dewets the interface, either by evaporation into the ambient or by the formation of three-dimensional droplets under the graphene, on top of the bilayer. Our experimental findings reveal novel phenomena of water at the nanoscale, which are interesting from a fundamental point of view and demonstrate the direct control over the wetting properties of the graphene/water interface. PMID:28985466

Observing the Heterogeneous Electro-redox of Individual Single-Layer Graphene Sheets.

PubMed

Chen, Tao; Zhang, Yuwei; Xu, Weilin

2016-09-27

Electro-redox-induced heterogeneous fluorescence of an individual single-layer graphene sheet was observed in real time by a total internal reflection fluorescence microscope. It was found that the fluorescence intensity of an individual sheet can be tuned reversibly by applying periodic voltages to control the redox degree of graphene sheets. Accordingly, the oxidation and reduction kinetics of an individual single-layer graphene sheet was studied at different voltages. The electro-redox-induced reversible variation of fluorescence intensity of individual sheets indicates a reversible band gap tuning strategy. Furthermore, correlation analysis of redox rate constants on individual graphene sheets revealed a redox-induced spatiotemporal heterogeneity or dynamics of graphene sheets. The observed controllable redox kinetics can rationally guide the precise band gap tuning of individual graphene sheets and then help their extensive applications in optoelectronics and devices for renewable energy.

Homoepitaxial graphene tunnel barriers for spin transport

NASA Astrophysics Data System (ADS)

Friedman, Adam

Tunnel barriers are key elements for both charge-and spin-based electronics, offering devices with reduced power consumption and new paradigms for information processing. Such devices require mating dissimilar materials, raising issues of heteroepitaxy, interface stability, and electronic states that severely complicate fabrication and compromise performance. Graphene is the perfect tunnel barrier. It is an insulator out-of-plane, possesses a defect-free, linear habit, and is impervious to interdiffusion. Nonetheless, true tunneling between two stacked graphene layers is not possible in environmental conditions (magnetic field, temperature, etc.) usable for electronics applications. However, two stacked graphene layers can be decoupled using chemical functionalization. We demonstrate successful tunneling, charge, and spin transport with a fluorinated graphene tunnel barrier on a graphene channel. We show that while spin transport stops short of room temperature, spin polarization efficiency values are the highest of any graphene spin devices. We also demonstrate that hydrogenation of graphene can also be used to create a tunnel barrier. We begin with a four-layer stack of graphene and hydrogenate the top few layers to decouple them from the graphene transport channel beneath. We demonstrate successful tunneling by measuring non-linear IV curves and a weakly temperature dependent zero-bias resistance. We demonstrate lateral transport of spin currents in non-local spin-valve structures and determine spin lifetimes with the non-local Hanle effect to be commensurate with previous studies. The measured spin polarization efficiencies for hydrogenated graphene are higher than most oxide tunnel barriers on graphene, but not as high as with fluorinated graphene tunnel barriers. However, here we show that spin transport persists up to room temperature. Our results for the hydrogenated graphene tunnel barriers are compared with fluorinated tunnel barriers and we discuss the possibility that magnetic moments in the graphene tunnel barriers affect the spin transport of our devices.

Architecture engineering of supercapacitor electrode materials

NASA Astrophysics Data System (ADS)

Chen, Kunfeng; Li, Gong; Xue, Dongfeng

2016-02-01

The biggest challenge for today’s supercapacitor systems readily possessing high power density is their low energy density. Their electrode materials with controllable structure, specific surface area, electronic conductivity, and oxidation state, have long been highlighted. Architecture engineering of functional electrode materials toward powerful supercapacitor systems is becoming a big fashion in the community. The construction of ion-accessible tunnel structures can microscopically increase the specific capacitance and materials utilization; stiff 3D structures with high specific surface area can macroscopically assure high specific capacitance. Many exciting findings in electrode materials mainly focus on the construction of ice-folded graphene paper, in situ functionalized graphene, in situ crystallizing colloidal ionic particles and polymorphic metal oxides. This feature paper highlights some recent architecture engineering strategies toward high-energy supercapacitor electrode systems, including electric double-layer capacitance (EDLC) and pseudocapacitance.

Deposition of thin silicon layers on transferred large area graphene

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lupina, Grzegorz, E-mail: lupina@ihp-microelectronics.com; Kitzmann, Julia; Lukosius, Mindaugas

2013-12-23

Physical vapor deposition of Si onto transferred graphene is investigated. At elevated temperatures, Si nucleates preferably on wrinkles and multilayer graphene islands. In some cases, however, Si can be quasi-selectively grown only on the monolayer graphene regions while the multilayer islands remain uncovered. Experimental insights and ab initio calculations show that variations in the removal efficiency of carbon residuals after the transfer process can be responsible for this behavior. Low-temperature Si seed layer results in improved wetting and enables homogeneous growth. This is an important step towards realization of electronic devices in which graphene is embedded between two Si layers.

Dynamically tunable dendritic graphene-based absorber with thermal stability at infrared regions

NASA Astrophysics Data System (ADS)

Huang, Hailong; Xia, Hui; Guo, Zhibo; Xie, Ding; Li, Hongjian

2018-06-01

The infrared polarization-insensitive absorber, which is composed of dendritic metal, graphene layer, silicon dioxides layer, gallium arsenide substrate, and metal plate, is investigated theoretically and numerically. The tunability can be realized by loading a graphene layer into the structure. The position of absorption peak can be tuned by manipulating the graphene's Fermi energy. Compared with the previously reported graphene-based absorbers, the system has the advantage of temperature-independent high absorption. The results indicate that the proposed absorber can be used in the applications of the refractive index sensor with a sensitivity of 587.8 nm/refractive index unit and temperature-insensitive infrared absorber.

Changes in the reflectivity of a lithium niobate crystal decorated with a graphene layer

NASA Astrophysics Data System (ADS)

Salas, O.; Garcés, E.; Castillo, F. L.; Magaña, L. F.

2017-01-01

Density functional theory and molecular dynamics were used to study the interaction of a graphene layer with the surface of lithium niobate. The simulations were performed at atmospheric pressure and 300K. We found that the graphene layer is physisorbed with an adsorption energy of -0.8205 eV/C-atom. Subsequently, the optical absorption of the graphene-(lithium niobate) system was calculated and compared with that of graphene solo and lithium niobate alone, respectively. The calculations were performed using the Quantum Espresso code with the GGA approximation and Vdw-DF2 (which includes long-range correlation effects as Van der Waals interactions).

Highly air stable passivation of graphene based field effect devices.

PubMed

Sagade, Abhay A; Neumaier, Daniel; Schall, Daniel; Otto, Martin; Pesquera, Amaia; Centeno, Alba; Elorza, Amaia Zurutuza; Kurz, Heinrich

2015-02-28

The sensitivity of graphene based devices to surface adsorbates and charge traps at the graphene/dielectric interface requires proper device passivation in order to operate them reproducibly under ambient conditions. Here we report on the use of atomic layer deposited aluminum oxide as passivation layer on graphene field effect devices (GFETs). We show that successful passivation produce hysteresis free DC characteristics, low doping level GFETs stable over weeks though operated and stored in ambient atmosphere. This is achieved by selecting proper seed layer prior to deposition of encapsulation layer. The passivated devices are also demonstrated to be robust towards the exposure to chemicals and heat treatments, typically used during device fabrication. Additionally, the passivation of high stability and reproducible characteristics is also shown for functional devices like integrated graphene based inverters.

NiFe layered double hydroxide/reduced graphene oxide nanohybrid as an efficient bifunctional electrocatalyst for oxygen evolution and reduction reactions

NASA Astrophysics Data System (ADS)

Zhan, Tianrong; Zhang, Yumei; Liu, Xiaolin; Lu, SiSi; Hou, Wanguo

2016-11-01

Highly active and low-cost bifunctional electrocatalysts for oxygen evolution and reduction reactions (OER and ORR) hold a heart position for the renewable energy technologies such as metal-air batteries and fuel cells. Here, we reported the synthesis of NiFe layered double hydroxide/reduced graphene oxide (NiFe-LDH/rGO) nanohybrid via the facile solvothermal method followed by chemical reduction. The template role of surfactant and the hybridization of rGO supplied the NiFe-LDH/rGO catalyst with a porous nanostructure and an enhanced conductivity, favoring both mass transport and charge communication of electrocatalytic reactions. The NiFe-LDH/rGO composite not only displayed highly efficient OER activity in alkaline solution with a low onset overpotential of 240 mV, but also only needed an overpotential of 250 mV to reach the 10 mA cm-2 current density. The NiFe-LDH/rGO nanohybrid also offered excellent ORR catalytic activity with onset potential at 0.796 V in alkaline media. The rotating-disk and rotating-ring-disk electrodes both revealed that the ORR on NiFe-LDH/rGO mainly involved a direct four-electron reaction pathways accompanying part of the two-electron process. The excellent bifunctional activity of the NiFe-LDH/rGO nanohybrid could be attributed to the synergistic effects of rGO and NiFe-LDH components due to the strongly coupled interactions.

Solid-Solution Sulfides Derived from Tunable Layered Double Hydroxide Precursors/Graphene Aerogel for Pseudocapacitors and Sodium-Ion Batteries.

PubMed

Song, Yajie; Li, Hui; Yang, Lan; Bai, Daxun; Zhang, Fazhi; Xu, Sailong

2017-12-13

Transition-metal sulfides (TMSs) are suggested as promising electrode materials for electrochemical pseudocapacitors and lithium- and sodium-ion batteries; however, they typically involve mixed composites or conventionally stoichiometric TMSs (such as NiCo 2 S 4 and Ni 2 CoS 4 ). Herein we demonstrate a preparation of solid-solution sulfide (Ni 0.7 Co 0.3 )S 2 supported on three-dimensional graphene aerogel (3DGA) via a sulfuration of NiCo-layered double hydroxide (NiCo-LDH) precursor/3DGA. The electrochemical tests show that the (Ni 0.7 Co 0.3 )S 2 /3DGA electrode exhibits a capacitance of 2165 F g -1 at 1 A g -1 , 2055 F g -1 at 2 A g -1 , and 1478 F g -1 at 10 A g -1 ; preserves 78.5% capacitance retention upon 1000 cycles for pseudocapacitors; and in particular, possesses a relatively high charge capacity of 388.7 mA h g -1 after 50 cycles at 100 mA g -1 as anode nanomaterials for sodium-ion batteries. Furthermore, the electrochemical performances are readily tuned by varying the cationic type of the tunable LDH precursors to prepare different solid-solution sulfides, such as (Ni 0.7 Fe 0.3 )S 2 /3DGA and (Co 0.7 Fe 0.3 )S 2 /3DGA. Our results show that engineering LDH precursors can offer an alternative for preparing diverse transition-metal sulfides for energy storage.

Visible-light-responsive photocatalysts toward water oxidation based on NiTi-layered double hydroxide/reduced graphene oxide composite materials.

PubMed

Li, Bei; Zhao, Yufei; Zhang, Shitong; Gao, Wa; Wei, Min

2013-10-23

A visible-light responsive photocatalyst was fabricated by anchoring NiTi-layered double hydroxide (NiTi-LDH) nanosheets to the surface of reduced graphene oxide sheets (RGO) via an in situ growth method; the resulting NiTi-LDH/RGO composite displays excellent photocatalytic activity toward water splitting into oxygen with a rate of 1.968 mmol g(-1) h(-1) and a quantum efficiency as high as 61.2% at 500 nm, which is among the most effective visible-light photocatalysts. XRD patterns and SEM images indicate that the NiTi-LDH nanosheets (diameter: 100-200 nm) are highly dispersed on the surface of RGO. UV-vis absorption spectroscopy exhibits that the introduction of RGO enhances the visible-light absorption range of photocatalysts, which is further verified by the largely decreased band gap (∼1.78 eV) studied by cyclic voltammetry measurements. Moreover, photoluminescence (PL) measurements indicate a more efficient separation of electron-hole pairs; electron spin resonance (ESR) and Raman scattering spectroscopy confirm the electrons transfer from NiTi-LDH nanosheets to RGO, accounting for the largely enhanced carrier mobility and the resulting photocatalytic activity in comparison with pristine NiTi-LDH material. Therefore, this work demonstrates a facile approach for the fabrication of visible-light responsive NiTi-LDH/RGO composite photocatalysts, which can be used as a promising candidate in solar energy conversion and environmental science.

Stability of hydrogenated graphene: a first-principles study

DOE PAGES

Yi, Ding; Yang, Liu; Xie, Shijie; ...

2015-02-10

In order to explain the disagreement between present theoretical and experimental investigations on the stability of hydrogenated graphene, we have systematically studied hydrogenated graphene with different configurations from the consideration of single-side and double-side adsorption using first-principles calculations. Both binding energy and formation energy are calculated to characterize the stability of the system. It is found that single-side hydrogenated graphene is always unstable. However, for double-side hydrogenation, some configurations are stable due to the increased carbon–carbon sp 3 hybridization compared to single-side hydrogenation. Furthermore, it is found that the system is energetically favorable when an equal number of hydrogen atomsmore » are adsorbed on each side of the graphene.« less

Nitrogen-Doping Enables Covalent-Like pi-pi Bonding between Graphenes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tian, Yong-Hui; Huang, Jingsong; Sumpter, Bobby G

The neighboring layers in bi-layer (and few-layer) graphenes of both AA and AB stacking motifs are known to be separated at a distance corresponding to van der Waals (vdW) interactions. In this Letter, we present for the first time a new aspect of graphene chemistry in terms of a special chemical bonding between the giant graphene molecules . Through rigorous theoretical calculations, we demonstrate that the N-doped graphenes (NGPs) with various doping levels can form an unusual two-dimensional (2D) pi pi bonding in bi-layer NGPs bringing the neighboring NGPs to significantly reduced interlayer separations. The interlayer binding energies can bemore » enhanced by up to 50% compared to the pristine graphene bi-layers that are characterized by only vdW interactions. Such an unusual chemical bonding arises from the pi pi overlap across the vdW gap while the individual layers maintain their in-plane pi-conjugation and are accordingly planar. The existence of the resulting interlayer covalent-like bonding is corroborated by electronic structure calculations and crystal orbital overlap population (COOP) analyses. In NGP-based graphite with the optimal doping level, the NGP layers are uniformly stacked and the 3D bulk exhibits metallic characteristics both in the in-plane and along the stacking directions.« less

Nonlocal thermal transport across embedded few-layer graphene sheets

DOE PAGES

Liu, Ying; Huxtable, Scott T.; Yang, Bao; ...

2014-11-13

Thermal transport across the interfaces between few-layer graphene sheets and soft materials exhibits intriguing anomalies when interpreted using the classical Kapitza model, e.g., the conductance of the same interface differs greatly for different modes of interfacial thermal transport. Using atomistic simulations, we show that such thermal transport follows a nonlocal flux-temperature drop constitutive law and is characterized jointly by a quasi-local conductance and a nonlocal conductance instead of the classical Kapitza conductance. Lastly, the nonlocal model enables rationalization of many anomalies of the thermal transport across embedded few-layer graphene sheets and should be used in studies of interfacial thermal transportmore » involving few-layer graphene sheets or other ultra-thin layered materials.« less

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

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jung, I.; Pelton, M.; Piner, R.

2007-12-01

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.

Terahertz magneto-optical properties of bi- and tri-layer graphene

NASA Astrophysics Data System (ADS)

Mei, Hongying; Xu, Wen; Wang, Chao; Yuan, Haifeng; Zhang, Chao; Ding, Lan; Zhang, Jin; Deng, Chao; Wang, Yifan; Peeters, Francois M.

2018-05-01

Magneto-optical (MO) properties of bi- and tri-layer graphene are investigated utilizing terahertz time-domain spectroscopy (THz TDS) in the presence of a strong magnetic field at room-temperature. In the Faraday configuration and applying optical polarization measurements, we measure the real and imaginary parts of the longitudinal and transverse MO conductivities of different graphene samples. The obtained experimental data fits very well with the classical MO Drude formula. Thus, we are able to obtain the key sample and material parameters of bi- and tri-layer graphene, such as the electron effective mass, the electronic relaxation time and the electron density. It is found that in high magnetic fields the electronic relaxation time τ for bi- and tri-layer graphene increases with magnetic field B roughly in a form τ∼ B2 . Most importantly, we obtain the electron effective mass for bi- and tri-layer graphene at room-temperature under non-resonant conditions. This work shows how the advanced THz MO techniques can be applied for the investigation into fundamental physics properties of atomically thin 2D electronic systems.

Graphene-based multilayer resonance structure to enhance the optical pressure on a Mie particle

NASA Astrophysics Data System (ADS)

Hassanzadeh, Abdollah; Mohammadnezhad, Mohammadbagher

2016-04-01

We theoretically investigate the optical force exerted on a Mie dielectric particle in the evanescent field of a graphene-based resonance multilayer structure using the arbitrary beam theory and the theory of multilayer films. The resonance structure consists of several thin films including a dielectric film (MgF2), a metal film (silver or gold), and several graphene layers which are located on a prism base. The effects of the metal film thickness and the number of graphene layers on the optical force are numerically investigated. The thickness of the metal layer and the number of graphene layers are optimized to reach the highest optical force. The numerical results show that an optimized composition of graphene and gold leads to a higher optical force compared to that of the graphene and silver. The optical force was enhanced resonantly by four orders of magnitude for the resonance structure containing graphene and a gold film and by three orders of magnitude for the structure containing graphene and a silver film compared to other similar resonance structures. We hope that the results presented in this paper can provide an excellent means of improving the optical manipulation of particles and enable the provision of effective optical tweezers, micromotors, and microaccelelators.

Opening a band gap without breaking lattice symmetry: a new route toward robust graphene-based nanoelectronics.

PubMed

Kou, Liangzhi; Hu, Feiming; Yan, Binghai; Frauenheim, Thomas; Chen, Changfeng

2014-07-07

Developing graphene-based nanoelectronics hinges on opening a band gap in the electronic structure of graphene, which is commonly achieved by breaking the inversion symmetry of the graphene lattice via an electric field (gate bias) or asymmetric doping of graphene layers. Here we introduce a new design strategy that places a bilayer graphene sheet sandwiched between two cladding layers of materials that possess strong spin-orbit coupling (e.g., Bi2Te3). Our ab initio and tight-binding calculations show that a proximity enhanced spin-orbit coupling effect opens a large (44 meV) band gap in bilayer graphene without breaking its lattice symmetry, and the band gap can be effectively tuned by an interlayer stacking pattern and significantly enhanced by interlayer compression. The feasibility of this quantum-well structure is demonstrated by recent experimental realization of high-quality heterojunctions between graphene and Bi2Te3, and this design also conforms to existing fabrication techniques in the semiconductor industry. The proposed quantum-well structure is expected to be especially robust since it does not require an external power supply to open and maintain a band gap, and the cladding layers provide protection against environmental degradation of the graphene layer in its device applications.

Examination of humidity effects on measured thickness and interfacial phenomena of exfoliated graphene on silicon dioxide via amplitude modulation atomic force microscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jinkins, K.; Farina, L.; Wu, Y., E-mail: wuy@uwplatt.edu

2015-12-14

The properties of Few-Layer Graphene (FLG) change with the number of layers and Amplitude Modulation (AM) Atomic Force Microscopy (AFM) is commonly used to determine the thickness of FLG. However, AFM measurements have been shown to be sensitive to environmental conditions such as relative humidity (RH). In the present study, AM-AFM is used to measure the thickness and loss tangent of exfoliated graphene on silicon dioxide (SiO{sub 2}) as RH is increased from 10% to 80%. We show that the measured thickness of graphene is dependent on RH. The loss tangent values of the graphene and oxide regions are bothmore » affected by humidity, with generally higher loss tangent for graphene than SiO{sub 2}. As RH increases, we observe the loss tangent of both materials approaches the same value. We hypothesize that there is a layer of water trapped between the graphene and SiO{sub 2} substrate to explain this observation. Using this interpretation, the loss tangent images also indicate movement and change in this trapped water layer as RH increases, which impacts the measured thickness of graphene using AM-AFM.« less

Characterisation of thin films of graphene–surfactant composites produced through a novel semi-automated method

PubMed Central

Nabok, Alexei; Davis, Frank; Higson, Séamus P J

2016-01-01

Summary In this paper we detail a novel semi-automated method for the production of graphene by sonochemical exfoliation of graphite in the presence of ionic surfactants, e.g., sodium dodecyl sulfate (SDS) and cetyltrimethylammonium bromide (CTAB). The formation of individual graphene flakes was confirmed by Raman spectroscopy, while the interaction of graphene with surfactants was proven by NMR spectroscopy. The resulting graphene–surfactant composite material formed a stable suspension in water and some organic solvents, such as chloroform. Graphene thin films were then produced using Langmuir–Blodgett (LB) or electrostatic layer-by-layer (LbL) deposition techniques. The composition and morphology of the films produced was studied with SEM/EDX and AFM. The best results in terms of adhesion and surface coverage were achieved using LbL deposition of graphene(−)SDS alternated with polyethyleneimine (PEI). The optical study of graphene thin films deposited on different substrates was carried out using UV–vis absorption spectroscopy and spectroscopic ellipsometry. A particular focus was on studying graphene layers deposited on gold-coated glass using a method of total internal reflection ellipsometry (TIRE) which revealed the enhancement of the surface plasmon resonance in thin gold films by depositing graphene layers. PMID:26977378

Graphene Based Reversible Nano-Switch/Sensor Schottky Diode (NANOSSSD) Device

NASA Technical Reports Server (NTRS)

Miranda, Felix A. (Inventor); Theofylaktos, Onoufrios (Inventor); Pinto, Nicholas J. (Inventor); Mueller, Carl H. (Inventor); Santos, Javier (Inventor); Meador, Michael A. (Inventor)

2015-01-01

A nanostructure device is provided and performs dual functions as a nano-switching/sensing device. The nanostructure device includes a doped semiconducting substrate, an insulating layer disposed on the doped semiconducting substrate, an electrode formed on the insulating layer, and at least one layer of graphene formed on the electrode. The at least one layer of graphene provides an electrical connection between the electrode and the substrate and is the electroactive element in the device.

Pulsed-Plasma Physical Vapor Deposition Approach Toward the Facile Synthesis of Multilayer and Monolayer Graphene for Anticoagulation Applications.

PubMed

Vijayaraghavan, Rajani K; Gaman, Cezar; Jose, Bincy; McCoy, Anthony P; Cafolla, Tony; McNally, Patrick J; Daniels, Stephen

2016-02-01

We demonstrate the growth of multilayer and single-layer graphene on copper foil using bipolar pulsed direct current (DC) magnetron sputtering of a graphite target in pure argon atmosphere. Single-layer graphene (SG) and few-layer graphene (FLG) films are deposited at temperatures ranging from 700 °C to 920 °C within <30 min. We find that the deposition and post-deposition annealing temperatures influence the layer thickness and quality of the graphene films formed. The films were characterized using atomic force microscopy (AFM), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and optical transmission spectroscopy techniques. Based on the above studies, a diffusion-controlled mechanism was proposed for the graphene growth. A single-step whole blood assay was used to investigate the anticoagulant activity of graphene surfaces. Platelet adhesion, activation, and morphological changes on the graphene/glass surfaces, compared to bare glass, were analyzed using fluorescence microscopy and SEM techniques. We have found significant suppression of the platelet adhesion, activation, and aggregation on the graphene-covered surfaces, compared to the bare glass, indicating the anticoagulant activity of the deposited graphene films. Our production technique represents an industrially relevant method for the growth of SG and FLG for various applications including the biomedical field.

Dark-field transmission electron microscopy and the Debye-Waller factor of graphene

PubMed Central

Hubbard, William A.; White, E. R.; Dawson, Ben; Lodge, M. S.; Ishigami, Masa; Regan, B. C.

2014-01-01

Graphene's structure bears on both the material's electronic properties and fundamental questions about long range order in two-dimensional crystals. We present an analytic calculation of selected area electron diffraction from multi-layer graphene and compare it with data from samples prepared by chemical vapor deposition and mechanical exfoliation. A single layer scatters only 0.5% of the incident electrons, so this kinematical calculation can be considered reliable for five or fewer layers. Dark-field transmission electron micrographs of multi-layer graphene illustrate how knowledge of the diffraction peak intensities can be applied for rapid mapping of thickness, stacking, and grain boundaries. The diffraction peak intensities also depend on the mean-square displacement of atoms from their ideal lattice locations, which is parameterized by a Debye-Waller factor. We measure the Debye-Waller factor of a suspended monolayer of exfoliated graphene and find a result consistent with an estimate based on the Debye model. For laboratory-scale graphene samples, finite size effects are sufficient to stabilize the graphene lattice against melting, indicating that ripples in the third dimension are not necessary. PMID:25242882

Dark-field transmission electron microscopy and the Debye-Waller factor of graphene.

PubMed

Shevitski, Brian; Mecklenburg, Matthew; Hubbard, William A; White, E R; Dawson, Ben; Lodge, M S; Ishigami, Masa; Regan, B C

2013-01-15

Graphene's structure bears on both the material's electronic properties and fundamental questions about long range order in two-dimensional crystals. We present an analytic calculation of selected area electron diffraction from multi-layer graphene and compare it with data from samples prepared by chemical vapor deposition and mechanical exfoliation. A single layer scatters only 0.5% of the incident electrons, so this kinematical calculation can be considered reliable for five or fewer layers. Dark-field transmission electron micrographs of multi-layer graphene illustrate how knowledge of the diffraction peak intensities can be applied for rapid mapping of thickness, stacking, and grain boundaries. The diffraction peak intensities also depend on the mean-square displacement of atoms from their ideal lattice locations, which is parameterized by a Debye-Waller factor. We measure the Debye-Waller factor of a suspended monolayer of exfoliated graphene and find a result consistent with an estimate based on the Debye model. For laboratory-scale graphene samples, finite size effects are sufficient to stabilize the graphene lattice against melting, indicating that ripples in the third dimension are not necessary.

Defect-enhanced performance of a 3D graphene anode in a lithium-ion battery

NASA Astrophysics Data System (ADS)

Guo, Hongchen; Long, Deng; Zheng, Zongmin; Chen, Xinyi; Ng, Alan M. C.; Lu, Miao

2017-12-01

Morphological defects were generated in an undoped 3D graphene structure via the involvement of a ZnO and Mg(OH)2 intermediate nanostructure layer placed between two layers of vapor-deposited graphene. Once the intermediate layer was etched, the 3D graphene lost support and shrank; during this process many morphological defects were formed. The electrochemical performance of the derived defective graphene utilized as the anode of a lithium (Li)-ion battery was significantly improved from ˜382 mAh g-1 to ˜2204 mAh g-1 at 0.5 A g-1 compared to normal 3D graphene. The derived defective graphene exhibited an initial capacity of 1009 mAh g-1 and retention of 83% at 4 A g-1 for 500 cycles, and ˜330 mAh g-1 at a high rate of 20 A g-1. Complicated defects such as wrinkles, pores, and particles formed during the etching of the intermediate layer, were considered to contribute to the improvement of the electrochemical performance.

Graphene-ferromagnet interfaces: hybridization, magnetization and charge transfer.

PubMed

Abtew, Tesfaye; Shih, Bi-Ching; Banerjee, Sarbajit; Zhang, Peihong

2013-03-07

Electronic and magnetic properties of graphene-ferromagnet interfaces are investigated using first-principles electronic structure methods in which a single layer graphene is adsorbed on Ni(111) and Co(111) surfaces. Due to the symmetry matching and orbital overlap, the hybridization between graphene pπ and Ni (or Co) d(z(2)) states is very strong. This pd hybridization, which is both spin and k dependent, greatly affects the electronic and magnetic properties of the interface, resulting in a significantly reduced (by about 20% for Ni and 10% for Co) local magnetic moment of the top ferromagnetic layer at the interface and an induced spin polarization on the graphene layer. The calculated induced magnetic moment on the graphene layer agrees well with a recent experiment. In addition, a substantial charge transfer across the graphene-ferromagnet interfaces is observed. We also investigate the effects of thickness of the ferromagnet slab on the calculated electronic and magnetic properties of the interface. The strength of the pd hybridization and the thickness-dependent interfacial properties may be exploited to design structures with desirable magnetic and transport properties for spintronic applications.

Graphene-silicon layered structures on single-crystalline Ir(111) thin films

DOE PAGES

Que, Yande D.; Tao, Jing; Zhang, Yong; ...

2015-01-20

Epitaxial growth of graphene on transition metal crystals, such as Ru,⁽¹⁻³⁾ Ir,⁽⁴⁻⁶⁾ and Ni,⁽⁷⁾ provides large-area, uniform graphene layers with controllable defect density, which is crucial for practical applications in future devices. To decrease the high cost of single-crystalline metal bulks, single-crystalline metal films are strongly suggested as the substrates for epitaxial growth large-scale high-quality graphene.⁽⁸⁻¹⁰⁾ Moreover, in order to weaken the interactions of graphene with its metal host, which may result in a suppression of the intrinsic properties of graphene,⁽¹¹ ¹²⁾ the method of element intercalation of semiconductors at the interface between an epitaxial graphene layer and a transitionmore » metal substrate has been successfully realized.⁽¹³⁻¹⁶⁾« less

Infrared spectroscopy of wafer-scale graphene.

PubMed

Yan, Hugen; Xia, Fengnian; Zhu, Wenjuan; Freitag, Marcus; Dimitrakopoulos, Christos; Bol, Ageeth A; Tulevski, George; Avouris, Phaedon

2011-12-27

We report spectroscopy results from the mid- to far-infrared on wafer-scale graphene, grown either epitaxially on silicon carbide or by chemical vapor deposition. The free carrier absorption (Drude peak) is simultaneously obtained with the universal optical conductivity (due to interband transitions) and the wavelength at which Pauli blocking occurs due to band filling. From these, the graphene layer number, doping level, sheet resistivity, carrier mobility, and scattering rate can be inferred. The mid-IR absorption of epitaxial two-layer graphene shows a less pronounced peak at 0.37 ± 0.02 eV compared to that in exfoliated bilayer graphene. In heavily chemically doped single-layer graphene, a record high transmission reduction due to free carriers approaching 40% at 250 μm (40 cm(-1)) is measured in this atomically thin material, supporting the great potential of graphene in far-infrared and terahertz optoelectronics.

Graphene on silicon dioxide via carbon ion implantation in copper with PMMA-free transfer

NASA Astrophysics Data System (ADS)

Lehnert, Jan; Spemann, Daniel; Hamza Hatahet, M.; Mändl, Stephan; Mensing, Michael; Finzel, Annemarie; Varga, Aron; Rauschenbach, Bernd

2017-06-01

In this work, a synthesis method for the growth of low-defect large-area graphene using carbon ion beam implantation into metallic Cu foils is presented. The Cu foils (1 cm2 in size) were pre-annealed in a vacuum at 950 °C for 2 h, implanted with 35 keV carbon ions at room temperature, and subsequently annealed at 850 °C for 2 h to form graphene layers with the layer number controlled by the implantation fluence. The graphene was then transferred to SiO2/Si substrates by a PMMA-free wet chemical etching process. The obtained regions of monolayer graphene are of ˜900 μm size. Raman spectroscopy, atomic force microscopy, scanning electron microscopy, and optical microscopy performed at room temperature demonstrated a good quality and homogeneity of the graphene layers, especially for monolayer graphene.

Epitaxial Graphene: A New Material for Electronics

NASA Astrophysics Data System (ADS)

de Heer, Walt A.

2007-10-01

Graphene multilayers are grown epitaxially on single crystal silicon carbide. This system is composed of several graphene layers of which the first layer is electron doped due to the built-in electric field and the other layers are essentially undoped. Unlike graphite the charge carriers show Dirac particle properties (i.e. an anomalous Berry's phase, weak anti-localization and square root field dependence of the Landau level energies). Epitaxial graphene shows quasi-ballistic transport and long coherence lengths; properties that may persists above cryogenic temperatures. Paradoxically, in contrast to exfoliated graphene, the quantum Hall effect is not observed in high mobility epitaxial graphene. It appears that the effect is suppressed due to absence of localized states in the bulk of the material. Epitaxial graphene can be patterned using standard lithography methods and characterized using a wide array of techniques. These favorable features indicate that interconnected room temperature ballistic devices may be feasible for low dissipation high-speed nano-electronics.

Epitaxial graphene

NASA Astrophysics Data System (ADS)

de Heer, Walt A.; Berger, Claire; Wu, Xiaosong; First, Phillip N.; Conrad, Edward H.; Li, Xuebin; Li, Tianbo; Sprinkle, Michael; Hass, Joanna; Sadowski, Marcin L.; Potemski, Marek; Martinez, Gérard

2007-07-01

Graphene multilayers are grown epitaxially on single crystal silicon carbide. This system is composed of several graphene layers of which the first layer is electron doped due to the built-in electric field and the other layers are essentially undoped. Unlike graphite the charge carriers show Dirac particle properties (i.e. an anomalous Berry's phase, weak anti-localization and square root field dependence of the Landau level energies). Epitaxial graphene shows quasi-ballistic transport and long coherence lengths; properties that may persist above cryogenic temperatures. Paradoxically, in contrast to exfoliated graphene, the quantum Hall effect is not observed in high-mobility epitaxial graphene. It appears that the effect is suppressed due to the absence of localized states in the bulk of the material. Epitaxial graphene can be patterned using standard lithography methods and characterized using a wide array of techniques. These favorable features indicate that interconnected room temperature ballistic devices may be feasible for low-dissipation high-speed nanoelectronics.

Transfer-free synthesis of multilayer graphene using a single-step process in an evaporator and formation confirmation by laser mode-locking.

PubMed

Kim, Won-Jun; Debnath, Pulak C; Lee, Junsu; Lee, Ju Han; Lim, Dae-Soon; Song, Yong-Won

2013-09-13

Multilayer graphene is synthesized by a simplified process employing an evaporator in which a target substrate is deposited with a Ni catalyst layer before being heated to grow graphene directly. Carbon atoms adsorbed onto the surface of the Ni source as impurities from the atmosphere are incorporated into the catalyst layer during the deposition, and diffuse toward the catalyst/substrate interface, where they crystallize as graphene with a thickness of less than 2 nm. The need for a transfer process and external carbon supply is eliminated. The graphene is characterized by conventional analysis approaches, including nano-scale visualization and Raman spectroscopy, and utilizing photonics, graphene-functionalized passive laser mode-locking is demonstrated to confirm the successful synthesis of the graphene layer, resulting in an operating center wavelength of 1569.4 nm, a pulse duration of 1.35 ps, and a repetition rate of 31.6 MHz.

Thermoacoustic and photoacoustic characterizations of few-layer graphene by pulsed excitations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Xiong; Department of Medical Imaging, The University of Arizona, Tucson, Arizona 85724; School of Information Science and Technology, ShanghaiTech University, Shanghai 200031

2016-04-04

We characterized the thermoacoustic and photoacoustic properties of large-area, few-layer graphene by pulsed microwave and optical excitations. Due to its high electric conductivity and low heat capacity per unit area, graphene lends itself to excellent microwave and optical energy absorption and acoustic signal emanation due to the thermoacoustic effect. When exposed to pulsed microwave or optical radiation, distinct thermoacoustic and photoacoustic signals generated by the few-layer graphene are obtained due to microwave and laser absorption of the graphene, respectively. Clear thermoacoustic and photoacoustic images of large-area graphene sample are achieved. A numerical model is developed and the simulated results aremore » in good accordance with the measured ones. This characterization work may find applications in ultrasound generator and detectors for microwave and optical radiation. It may also become an alternative characterization approach for graphene and other types of two-dimensional materials.« less

Interactions between C and Cu atoms in single-layer graphene: direct observation and modelling.

PubMed

Kano, Emi; Hashimoto, Ayako; Kaneko, Tomoaki; Tajima, Nobuo; Ohno, Takahisa; Takeguchi, Masaki

2016-01-07

Metal doping into the graphene lattice has been studied recently to develop novel nanoelectronic devices and to gain an understanding of the catalytic activities of metals in nanocarbon structures. Here we report the direct observation of interactions between Cu atoms and single-layer graphene by transmission electron microscopy. We document stable configurations of Cu atoms in the graphene sheet and unique transformations of graphene promoted by Cu atoms. First-principles calculations based on density functional theory reveal a reduction of energy barrier that caused rotation of C-C bonds near Cu atoms. We discuss two driving forces, electron irradiation and in situ heating, and conclude that the observed transformations were mainly promoted by electron irradiation. Our results suggest that individual Cu atoms can promote reconstruction of single-layer graphene.

Direct synthesis of few-layer graphene supported platinum nanocatalyst for methanol oxidation

NASA Astrophysics Data System (ADS)

Tan, Hong; Ma, Xiaohui; Sheng, Leimei; An, Kang; Yu, Liming; Zhao, Hongbin; Xu, Jiaqiang; Ren, Wei; Zhao, Xinluo

2014-11-01

High-crystalline few-layer graphene supported Pt nanoparticles have been synthesized by arc discharge evaporation of carbon electrodes containing Pt element. A high-temperature treatment under hydrogen atmosphere has been carried out to obtain a new type of Pt/graphene catalyst for methanol oxidation in direct methanol fuel cell. The morphology and structure characterizations of as-grown few-layer graphene supported Pt nanoparticles and Pt/graphene catalysts have been studied by Raman spectroscopy, scanning electron microscopy with energy-dispersive spectroscopy, and high-resolution transmission electron microscopy. Cyclic voltammograms and chronoamperometric curves show that our present Pt/graphene catalysts have larger current density for methanol oxidation, higher tolerance to carbon monoxide poisoning, and better stability during the operating procedure, compared to commercial Pt/C catalysts.

Direct graphene growth from highly ordered pyrolytic graphite using pulsed Nd: YAG laser on p-Si (100) substrate at 700°c

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kumar, Pramod, E-mail: kumarpramod.iitd@gmail.com; Lahiri, Indranil; Mitra, Anirban

Few layer graphene was deposited on p-type Si (100) substrates by pulsed laser deposition of highly ordered pyrolytic graphite (HOPG) target at a relatively low temperature of 700 °C, without any catalytic layer. Effect of laser energy on the ability to produce the crystalline graphene was studied. It was observed that a laser energy of 220 mJ/pulse lead to form few layer graphene while higher laser energy of 440 mJ/pulse was detrimental to precipitation process. The reasons behind this observation are also discussed. Graphene samples were analyzed using Raman spectroscopy and surface morphology of graphene samples was confirmed using fieldmore » emission scanning electron microscope (FE-SEM).« less

Three-Dimensional Expanded Graphene-Metal Oxide Film via Solid-State Microwave Irradiation for Aqueous Asymmetric Supercapacitors.

PubMed

Yang, MinHo; Lee, Kyoung G; Lee, Seok Jae; Lee, Sang Bok; Han, Young-Kyu; Choi, Bong Gill

2015-10-14

Carbon-based electrochemical double-layer capacitors and pseudocapacitors, consisting of a symmetric configuration of electrodes, can deliver much higher power densities than batteries, but they suffer from low energy densities. Herein, we report the development of high energy and power density supercapacitors using an asymmetric configuration of Fe2O3 and MnO2 nanoparticles incorporated into 3D macroporous graphene film electrodes that can be operated in a safe and low-cost aqueous electrolyte. The gap in working potential windows of Fe2O3 and MnO2 enables the stable expansion of the cell voltage up to 1.8 V, which is responsible for the high energy density (41.7 Wh kg(-1)). We employ a household microwave oven to simultaneously create conductivity, porosity, and the deposition of metal oxides on graphene films toward 3D hybrid architectures, which lead to a high power density (13.5 kW kg(-1)). Such high energy and power densities are maintained for over 5000 cycles, even during cycling at a high current density of 16.9 A g(-1).

Enrichment of Pyrrolic Nitrogen by Hole Defects in Nitrogen and Sulfur Co-Doped Graphene Hydrogel for Flexible Supercapacitors.

PubMed

Tran, Ngoc Quang; Kang, Bong Kyun; Woo, Moo Hyun; Yoon, Dae Ho

2016-08-23

The effect of the doping configuration and concentration of nitrogen (N) and sulfur (S) on the electrochemical performance of 3 D N and S co-doped hole defect graphene hydrogel (NS-HGH) electrodes is investigated. Surprisingly, by introducing a hole defect on the graphene surface, the difference in the doping concentrations of N and S can be used to effectively modulate the electrochemical behavior of the NS-HGH. The hole defects provide a rapid ion diffusion path. Finally, we showed that the intriguing specific capacitance (536 F g(-1) ) of the NS-HGH could enhance the overall performance of the pseudocapacitance and electric double layer capacitance. The rational design of the NS-HGH-based flexible solid state supercapacitor results in not only outstanding electrochemical performance with a maximum energy density of 14.8 Wh kg(-1) and power density of 5.2 KW kg(-1) but also in extraordinary mechanical flexibility and excellent cycle stability. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Enhancing Graphene Capacitance by Nitrogen: Effects of Doping Configuration and Concentration

DOE PAGES

Zhan, Cheng; Cummings, Peter; Jiang, De-en

2016-01-08

Recent experiments have shown that nitrogen doping enhances capacitance in carbon electrode supercapacitors. However, a detailed study of the effect of N-doping on capacitance is still lacking. In this paper, we study the doping concentration and the configuration effect on the electric double-layer (EDL) capacitance, quantum capacitance, and total capacitance. It is found that pyridinic and graphitic nitrogens can increase the total capacitance by increasing quantum capacitance, but pyrrolic configuration limits the total capacitance due to its much lower quantum capacitance than the other two configurations. We also find that, unlike the graphitic and pyridinic nitrogens, the pyrrolic configuration's quantummore » capacitance does not depend on the nitrogen concentration, which may explain why some capacitance versus voltage measurements of N-doped graphene exhibit a V-shaped curve similar to that of undoped graphene. Our investigation provides a deeper understanding of the capacitance enhancement of the N-doping effect in carbon electrodes and suggests a potentially effective way to optimize the capacitance by controlling the type of N-doping.« less

Highly electroconductive mesoporous graphene nanofibers and their capacitance performance at 4 V.

PubMed

Cui, Chaojie; Qian, Weizhong; Yu, Yuntao; Kong, Chuiyan; Yu, Bo; Xiang, Lan; Wei, Fei

2014-02-12

We report the fabrication of one-dimensional highly electroconductive mesoporous graphene nanofibers (GNFs) by a chemical vapor deposition method using MgCO3·3H2O fibers as the template. The growth of such a unique structure underwent the first in situ decomposition of MgCO3·3H2O fibers to porous MgO fibers, followed by the deposition of carbon on the MgO surface, the removal of MgO by acidic washing, and the final self-assembly of wet graphene from single to double layer in drying process. GNFs exhibited good structural stability, high surface area, mesopores in large amount, and electrical conductivity 3 times that of carbon nanotube aggregates. It, used as an electrode in a 4 V supercapacitor, exhibited high energy density in a wide range of high power density and excellent cycling stability. The short diffusion distance for ions of ionic liquids electrolyte to the surface of GNFs yielded high surface utilization efficiency and a capacitance up to 15 μF/cm(2), higher than single-walled carbon nanotubes.

The improved electrochemical performance of cross-linked 3D graphene nanoribbon monolith electrodes

NASA Astrophysics Data System (ADS)

Vineesh, Thazhe Veettil; Alwarappan, Subbiah; Narayanan, Tharangattu N.

2015-04-01

Technical advancement in the field of ultra-small sensors and devices demands the development of novel micro- or nano-based architectures. Here we report the design and assembly of cross-linked three dimensional graphene nanoribbons (3D GNRs) using solution based covalent binding of individual 2D GNRs and demonstrate its electrochemical application as a 3D electrode. The enhanced performance of 3D GNRs over individual 2D GNRs is established using standard redox probes - [Ru(NH3)6]3+/2+, [Fe(CN)6]3-/4- and important bio-analytes - dopamine and ascorbic acid. 3D GNRs are found to have high double layer capacitance (2482 μF cm-2) and faster electron transfer kinetics; their exceptional electrocatalytic activity towards the oxygen reduction reaction is indicative of their potential over a wide range of electrochemical applications. Moreover, this study opens a new platform for the design of novel point-of-care devices and electrodes for energy devices.Technical advancement in the field of ultra-small sensors and devices demands the development of novel micro- or nano-based architectures. Here we report the design and assembly of cross-linked three dimensional graphene nanoribbons (3D GNRs) using solution based covalent binding of individual 2D GNRs and demonstrate its electrochemical application as a 3D electrode. The enhanced performance of 3D GNRs over individual 2D GNRs is established using standard redox probes - [Ru(NH3)6]3+/2+, [Fe(CN)6]3-/4- and important bio-analytes - dopamine and ascorbic acid. 3D GNRs are found to have high double layer capacitance (2482 μF cm-2) and faster electron transfer kinetics; their exceptional electrocatalytic activity towards the oxygen reduction reaction is indicative of their potential over a wide range of electrochemical applications. Moreover, this study opens a new platform for the design of novel point-of-care devices and electrodes for energy devices. Electronic supplementary information (ESI) available. See DOI: 10.1039/c4nr07315k

Optical transparency of graphene layers grown on metal surfaces

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rut’kov, E. V.; Lavrovskaya, N. P.; Sheshenya, E. S., E-mail: sheshenayket@gmail.ru

It is shown that, in contradiction with the fundamental results obtained for free graphene, graphene films grown on the Rh(111) surface to thicknesses from one to ~(12–15) single layers do not absorb visible electromagnetic radiation emitted from the surface and influence neither the brightness nor true temperature of the sample. At larger thicknesses, such absorption occurs. This effect is observed for the surfaces of other metals, specifically, Pt(111), Re(1010), and Ni(111) and, thus, can be considered as being universal. It is thought that the effect is due to changes in the electronic properties of thin graphene layers because of electronmore » transfer between graphene and the metal substrate.« less

Bending stiffness and interlayer shear modulus of few-layer graphene

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, Xiaoming; Yi, Chenglin; Ke, Changhong, E-mail: cke@binghamton.edu

2015-03-09

Interlayer shear deformation occurs in the bending of multilayer graphene with unconstrained ends, thus influencing its bending rigidity. Here, we investigate the bending stiffness and interlayer shear modulus of few-layer graphene through examining its self-folding conformation on a flat substrate using atomic force microscopy in conjunction with nonlinear mechanics modeling. The results reveal that the bending stiffness of 2–6 layers graphene follows a square-power relationship with its thickness. The interlayer shear modulus is found to be in the range of 0.36–0.49 GPa. The research findings show that the weak interlayer shear interaction has a substantial stiffening effect for multilayer graphene.

Carbon Displacement-Induced Single Carbon Atomic Chain Formation and its Effects on Sliding of SiC Fibers in SiC/graphene/SiC Composite

DOE PAGES

Wallace, Joseph B.; Chen, Di; Shao, Lin

2015-11-03

Understanding radiation effects on the mechanical properties of SiC composites is important to their application in advanced reactor designs. By means of molecular dynamics simulations, we found that due to strong interface bonding between the graphene layers and SiC, the sliding friction of SiC fibers is largely determined by the frictional behavior between graphene layers. Upon sliding, carbon displacements between graphene layers can act as seed atoms to induce the formation of single carbon atomic chains (SCACs) by pulling carbon atoms from the neighboring graphene planes. The formation, growth, and breaking of SCACs determine the frictional response to irradiation.

Metal oxide induced charge transfer doping and band alignment of graphene electrodes for efficient organic light emitting diodes.

PubMed

Meyer, Jens; Kidambi, Piran R; Bayer, Bernhard C; Weijtens, Christ; Kuhn, Anton; Centeno, Alba; Pesquera, Amaia; Zurutuza, Amaia; Robertson, John; Hofmann, Stephan

2014-06-20

The interface structure of graphene with thermally evaporated metal oxide layers, in particular molybdenum trioxide (MoO3), is studied combining photoemission spectroscopy, sheet resistance measurements and organic light emitting diode (OLED) characterization. Thin (<5 nm) MoO3 layers give rise to an 1.9 eV large interface dipole and a downwards bending of the MoO3 conduction band towards the Fermi level of graphene, leading to a near ideal alignment of the transport levels. The surface charge transfer manifests itself also as strong and stable p-type doping of the graphene layers, with the Fermi level downshifted by 0.25 eV and sheet resistance values consistently below 50 Ω/sq for few-layer graphene films. The combination of stable doping and highly efficient charge extraction/injection allows the demonstration of simplified graphene-based OLED device stacks with efficiencies exceeding those of standard ITO reference devices.

Epitaxial ferromagnetic single clusters and smooth continuous layers on large area MgO/CVD graphene substrates

NASA Astrophysics Data System (ADS)

Godel, Florian; Meny, Christian; Doudin, Bernard; Majjad, Hicham; Dayen, Jean-François; Halley, David

2018-02-01

We report on the fabrication of ferromagnetic thin layers separated by a MgO dielectric barrier from a graphene-covered substrate. The growth of ferromagnetic metal layers—Co or Ni0.8Fe0.2—is achieved by Molecular Beam Epitaxy (MBE) on a 3 nm MgO(111) epitaxial layer deposited on graphene. In the case of a graphene, grown by chemical vapor deposition (CVD) over Ni substrates, an annealing at 450 °C, under ultra-high-vacuum (UHV) conditions, leads to the dewetting of the ferromagnetic layers, forming well-defined flat facetted clusters whose shape reflects the substrate symmetry. In the case of CVD graphene transferred on SiO2, no dewetting is observed after same annealing. We attribute this difference to the mechanical stress states induced by the substrate, illustrating how it matters for epitaxial construction through graphene. Controlling the growth parameters of such magnetic single objects or networks could benefit to new architectures for catalysis or spintronic applications.

Fabrication of bi-layer graphene and theoretical simulation for its possible application in thin film solar cell.

PubMed

Behura, Sanjay K; Mahala, Pramila; Nayak, Sasmita; Yang, Qiaoqin; Mukhopadhyay, Indrajit; Janil, Omkar

2014-04-01

High quality graphene film is fabricated using mechanical exfoliation of highly-oriented pyrolytic graphite. The graphene films on glass substrates are characterized using field-emission scanning electron microscopy, atomic force microscopy, Raman spectroscopy, UV-vis spectroscopy and Fourier transform infrared spectroscopy. A very high intensity ratio of 2D to G-band (to approximately 1.67) and narrow 2D-band full-width at half maximum (to approximately 40 cm(-1)) correspond to the bi-layer graphene formation. The bi-layer graphene/p-GaN/n-InGaN/n-GaN/GaN/sAl2O3 system is studied theoretically using TCAD Silvaco software, in which the properties of exfoliated bi-layer graphene are used as transparent and conductive film, and the device exhibits an efficiency of 15.24% compared to 13.63% for ITO/p-GaN/n-InGaN/n-GaN/GaN/Al2O3 system.

Switching of Photonic Crystal Lasers by Graphene.

PubMed

Hwang, Min-Soo; Kim, Ha-Reem; Kim, Kyoung-Ho; Jeong, Kwang-Yong; Park, Jin-Sung; Choi, Jae-Hyuck; Kang, Ju-Hyung; Lee, Jung Min; Park, Won Il; Song, Jung-Hwan; Seo, Min-Kyo; Park, Hong-Gyu

2017-03-08

Unique features of graphene have motivated the development of graphene-integrated photonic devices. In particular, the electrical tunability of graphene loss enables high-speed modulation of light and tuning of cavity resonances in graphene-integrated waveguides and cavities. However, efficient control of light emission such as lasing, using graphene, remains a challenge. In this work, we demonstrate on/off switching of single- and double-cavity photonic crystal lasers by electrical gating of a monolayer graphene sheet on top of photonic crystal cavities. The optical loss of graphene was controlled by varying the gate voltage V g , with the ion gel atop the graphene sheet. First, the fundamental properties of graphene were investigated through the transmittance measurement and numerical simulations. Next, optically pumped lasing was demonstrated for a graphene-integrated single photonic crystal cavity at V g below -0.6 V, exhibiting a low lasing threshold of ∼480 μW, whereas lasing was not observed at V g above -0.6 V owing to the intrinsic optical loss of graphene. Changing quality factor of the graphene-integrated photonic crystal cavity enables or disables the lasing operation. Moreover, in the double-cavity photonic crystal lasers with graphene, switching of individual cavities with separate graphene sheets was achieved, and these two lasing actions were controlled independently despite the close distance of ∼2.2 μm between adjacent cavities. We believe that our simple and practical approach for switching in graphene-integrated active photonic devices will pave the way toward designing high-contrast and ultracompact photonic integrated circuits.

Graphene Oxide Nanoribbon as Hole Extraction Layer to Enhance Efficiency and Stability of Polymer Solar Cells

DTIC Science & Technology

2013-01-01

Oxide Nanoribbon as Hole Extraction Layer to Enhance Effi ciency and Stability of Polymer Solar Cells Jun Liu , Gi-Hwan Kim , Yuhua Xue , Jin...circumvented by oxidizing graphene with acids (e.g., H 2 SO 4 /KMnO 4 ) to produce graphene oxide (GO) with oxygen-containing groups (e.g., –COOH, –OH...introducing the oxygen-rich groups around a graphene nanoribbon, the resultant graphene oxide nanoribbon (GOR) should show a synergistic effect to have

Electrostatic force assisted deposition of graphene

DOEpatents

Liang, Xiaogan [Berkeley, CA

2011-11-15

An embodiment of a method of depositing graphene includes bringing a stamp into contact with a substrate over a contact area. The stamp has at least a few layers of the graphene covering the contact area. An electric field is developed over the contact area. The stamp is removed from the vicinity of the substrate which leaves at least a layer of the graphene substantially covering the contact area.

Chemical gating of epitaxial graphene through ultrathin oxide layers.

PubMed

Larciprete, Rosanna; Lacovig, Paolo; Orlando, Fabrizio; Dalmiglio, Matteo; Omiciuolo, Luca; Baraldi, Alessandro; Lizzit, Silvano

2015-08-07

We achieved a controllable chemical gating of epitaxial graphene grown on metal substrates by exploiting the electrostatic polarization of ultrathin SiO2 layers synthesized below it. Intercalated oxygen diffusing through the SiO2 layer modifies the metal-oxide work function and hole dopes graphene. The graphene/oxide/metal heterostructure behaves as a gated plane capacitor with the in situ grown SiO2 layer acting as a homogeneous dielectric spacer, whose high capacity allows the Fermi level of graphene to be shifted by a few hundreds of meV when the oxygen coverage at the metal substrate is of the order of 0.5 monolayers. The hole doping can be finely tuned by controlling the amount of interfacial oxygen, as well as by adjusting the thickness of the oxide layer. After complete thermal desorption of oxygen the intrinsic doping of SiO2 supported graphene is evaluated in the absence of contaminants and adventitious adsorbates. The demonstration that the charge state of graphene can be changed by chemically modifying the buried oxide/metal interface hints at the possibility of tuning the level and sign of doping by the use of other intercalants capable of diffusing through the ultrathin porous dielectric and reach the interface with the metal.

Self-Organization of Ions at the Interface between Graphene and Ionic Liquid DEME-TFSI.

PubMed

Hu, Guangliang; Pandey, Gaind P; Liu, Qingfeng; Anaredy, Radhika S; Ma, Chunrui; Liu, Ming; Li, Jun; Shaw, Scott K; Wu, Judy

2017-10-11

Electrochemical effects manifest as nonlinear responses to an applied electric field in electrochemical devices, and are linked intimately to the molecular orientation of ions in the electric double layer (EDL). Herein, we probe the origin of the electrochemical effect using a double-gate graphene field effect transistor (GFET) of ionic liquid N,N-diethyl-N-(2-methoxyethyl)-N-methylammonium bis(trifluoromethylsulfonyl)imide (DEME-TFSI) top-gate, paired with a ferroelectric Pb 0.92 La 0.08 Zr 0.52 Ti 0.48 O 3 (PLZT) back-gate of compatible gating efficiency. The orientation of the interfacial molecular ions can be extracted by measuring the GFET Dirac point shift, and their dynamic response to ultraviolet-visible light and a gate electric field was quantified. We have observed that the strong electrochemical effect is due to the TFSI anions self-organizing on a treated GFET surface. Moreover, a reversible order-disorder transition of TFSI anions self-organized on the GFET surface can be triggered by illuminating the interface with ultraviolet-visible light, revealing that it is a useful method to control the surface ion configuration and the overall performance of the device.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Lifeng, E-mail: walfe@nuaa.edu.cn; Hu, Haiyan

The thermal vibration of a rectangular single-layered graphene sheet is investigated by using a rectangular nonlocal elastic plate model with quantum effects taken into account when the law of energy equipartition is unreliable. The relation between the temperature and the Root of Mean Squared (RMS) amplitude of vibration at any point of the rectangular single-layered graphene sheet in simply supported case is derived first from the rectangular nonlocal elastic plate model with the strain gradient of the second order taken into consideration so as to characterize the effect of microstructure of the graphene sheet. Then, the RMS amplitude of thermalmore » vibration of a rectangular single-layered graphene sheet simply supported on an elastic foundation is derived. The study shows that the RMS amplitude of the rectangular single-layered graphene sheet predicted from the quantum theory is lower than that predicted from the law of energy equipartition. The maximal relative difference of RMS amplitude of thermal vibration appears at the sheet corners. The microstructure of the graphene sheet has a little effect on the thermal vibrations of lower modes, but exhibits an obvious effect on the thermal vibrations of higher modes. The quantum effect is more important for the thermal vibration of higher modes in the case of smaller sides and lower temperature. The relative difference of maximal RMS amplitude of thermal vibration of a rectangular single-layered graphene sheet decreases monotonically with an increase of temperature. The absolute difference of maximal RMS amplitude of thermal vibration of a rectangular single-layered graphene sheet increases slowly with the rising of Winkler foundation modulus.« less

Liquid-phase growth of few-layered graphene on sapphire substrates using SiC micropowder source

NASA Astrophysics Data System (ADS)

Maruyama, Takahiro; Yamashita, Yutaka; Saida, Takahiro; Tanaka, Shin-ichiro; Naritsuka, Shigeya

2017-06-01

We demonstrated direct synthesis of graphene films consisting of a few layers (few-layered graphene) on sapphire substrates by liquid-phase growth (LPG), using liquid Ga as the melt and SiC micropowder as the source material. When the dissolution temperature was above 700 °C, almost all Si atoms of SiC diffused into the Ga melt and only carbon atoms remained at the interface beneath the liquid Ga. Above 800 °C, X-ray photoelectron spectra showed that most of the remaining carbon was graphitized. When the dissolution temperature was 1000 °C, Raman spectra showed that few-layered graphene films grew on the sapphire substrates.

Porous graphene-based membranes for water purification from metal ions at low differential pressures.

PubMed

Park, Jaewoo; Bazylewski, Paul; Fanchini, Giovanni

2016-05-14

A new generation of membranes for water purification based on weakly oxidized and nanoporous few-layer graphene is here introduced. These membranes dramatically decrease the high energy requirements of water purification by reverse osmosis. They combine the advantages of porous and non-oxidized single-layer graphene, offering energy-efficient water filtration at relatively low differential pressures, and highly oxidized graphene oxide, exhibiting high performance in terms of impurity adsorption. In the reported fabrication process, leaks between juxtaposed few-layer graphene flakes are sealed by thermally annealed colloidal silica, in a treatment that precedes the opening of (sub)nanometre-size pores in graphene. This process, explored for the first time in this work, results in nanoporous graphene flakes that are water-tight at the edges without occluding the (sub)nanopores. With this method, removal of impurities from water occurs through a combination of size-based pore rejection and pore-edge adsorption. Thinness of graphene flakes allows these membranes to achieve water purification from metal ions in concentrations of few parts-per-million at differential pressures as low as 30 kPa, outperforming existing graphene or graphene oxide purification systems with comparable flow rates.

Porous graphene-based membranes for water purification from metal ions at low differential pressures

NASA Astrophysics Data System (ADS)

Park, Jaewoo; Bazylewski, Paul; Fanchini, Giovanni

2016-05-01

A new generation of membranes for water purification based on weakly oxidized and nanoporous few-layer graphene is here introduced. These membranes dramatically decrease the high energy requirements of water purification by reverse osmosis. They combine the advantages of porous and non-oxidized single-layer graphene, offering energy-efficient water filtration at relatively low differential pressures, and highly oxidized graphene oxide, exhibiting high performance in terms of impurity adsorption. In the reported fabrication process, leaks between juxtaposed few-layer graphene flakes are sealed by thermally annealed colloidal silica, in a treatment that precedes the opening of (sub)nanometre-size pores in graphene. This process, explored for the first time in this work, results in nanoporous graphene flakes that are water-tight at the edges without occluding the (sub)nanopores. With this method, removal of impurities from water occurs through a combination of size-based pore rejection and pore-edge adsorption. Thinness of graphene flakes allows these membranes to achieve water purification from metal ions in concentrations of few parts-per-million at differential pressures as low as 30 kPa, outperforming existing graphene or graphene oxide purification systems with comparable flow rates.

Plasmon Excitations of Multi-layer Graphene on a Conducting Substrate

PubMed Central

Gumbs, Godfrey; Iurov, Andrii; Wu, Jhao-Ying; Lin, M. F.; Fekete, Paula

2016-01-01

We predict the existence of low-frequency nonlocal plasmons at the vacuum-surface interface of a superlattice of N graphene layers interacting with conducting substrate. We derive a dispersion function that incorporates the polarization function of both the graphene monolayers and the semi-infinite electron liquid at whose surface the electrons scatter specularly. We find a surface plasmon-polariton that is not damped by particle-hole excitations or the bulk modes and which separates below the continuum mini-band of bulk plasmon modes. The surface plasmon frequency of the hybrid structure always lies below , the surface plasmon frequency of the conducting substrate. The intensity of this mode depends on the distance of the graphene layers from the conductor’s surface, the energy band gap between valence and conduction bands of graphene monolayer and, most importantly, on the number of two-dimensional layers. For a sufficiently large number of layers the hybrid structure has no surface plasmon. The existence of plasmons with different dispersion relations indicates that quasiparticles with different group velocity may coexist for various ranges of wavelengths determined by the number of layers in the superlattice. PMID:26883086

Highly sensitive transient absorption imaging of graphene and graphene oxide in living cells and circulating blood.

PubMed

Li, Junjie; Zhang, Weixia; Chung, Ting-Fung; Slipchenko, Mikhail N; Chen, Yong P; Cheng, Ji-Xin; Yang, Chen

2015-07-23

We report a transient absorption (TA) imaging method for fast visualization and quantitative layer analysis of graphene and GO. Forward and backward imaging of graphene on various substrates under ambient condition was imaged with a speed of 2 μs per pixel. The TA intensity linearly increased with the layer number of graphene. Real-time TA imaging of GO in vitro with capability of quantitative analysis of intracellular concentration and ex vivo in circulating blood were demonstrated. These results suggest that TA microscopy is a valid tool for the study of graphene based materials.

Disorder from the Bulk Ionic Liquid in Electric Double Layer Transistors

DOE PAGES

Petach, Trevor A.; Reich, Konstantin V.; Zhang, Xiao; ...

2017-07-28

Ionic liquid gating has a number of advantages over solid-state gating, especially for flexible or transparent devices and for applications requiring high carrier densities. But, the large number of charged ions near the channel inevitably results in Coulomb scattering, which limits the carrier mobility in otherwise clean systems. We develop a model for this Coulomb scattering. We then validate our model experimentally using ionic liquid gating of graphene across varying thicknesses of hexagonal boron nitride, demonstrating that disorder in the bulk ionic liquid often dominates the scattering.

Non-Equilibrium Green’s Function Study of Transport in Disordered Double-Layer Graphene Systems

DTIC Science & Technology

2011-01-01

particles like electrons and holes. The Pauli exclusion principle prevents fermions from occupying the same quantum state, limiting the expectation...sity approximation. In Eq. 6.2, µ represents a vector that isolates each of the Cartesian components of the pairing vector, σµ represents the Pauli spin...devices on SiO2,” Nat. Nano, vol. 3, pp. 206–209, 2008. [35] X. Li, W. Cai, J. An, S. Kim, J. Nah, D. Yang, R. Piner, A. Velamakanni, I. Jung , E

One-step hydrothermal synthesis of three-dimensional porous Ni-Co sulfide/reduced graphene oxide composite with optimal incorporation of carbon nanotubes for high performance supercapacitors.

PubMed

Chiu, Cheng-Ting; Chen, Dong-Hwang

2018-04-27

Three-dimensional (3D) porous Ni-Co sulfide/reduced graphene oxide composite with the appropriate incorporation of carbon nanotubes (NCS/rGO/CNT) was fabricated as a promising material for supercapacitor electrodes. It combined the high pseudo-capacitance of Ni-Co sulfide as well as the large specific surface area and electrical double layer capacitance of reduced graphene oxide (rGO). Carbon nanotubes (CNTs) were incorporated to act as the spacer for hindering the restacking of rGO and to construct a conductive network for enhancing the electron transport. The 3D porous NCS/rGO/CNT composite was fabricated by a facile one-step hydrothermal process in which Ni-Co sulfide nanosheets were synthesized and graphene oxide was reduced simultaneously. It was shown that the capacitance and cyclic performance indeed could be effectively improved via the appropriate addition of CNTs. In addition, a flexible all-solid-state asymmetric supercapacitor based on the NCS/rGO/CNT electrode was fabricated and exhibited the same capacitive electrochemical performance under bending. Also, it could successfully turn on a light-emitting diode light, revealing its feasibility in practical application. All results demonstrated that the developed NCS/rGO/CNT composite has potential application in supercapacitors.

A high energy and power Li-ion capacitor based on a TiO2 nanobelt array anode and a graphene hydrogel cathode.

PubMed

Wang, Huanwen; Guan, Cao; Wang, Xuefeng; Fan, Hong Jin

2015-03-25

A novel hybrid Li-ion capacitor (LIC) with high energy and power densities is constructed by combining an electrochemical double layer capacitor type cathode (graphene hydrogels) with a Li-ion battery type anode (TiO(2) nanobelt arrays). The high power source is provided by the graphene hydrogel cathode, which has a 3D porous network structure and high electrical conductivity, and the counter anode is made of free-standing TiO(2) nanobelt arrays (NBA) grown directly on Ti foil without any ancillary materials. Such a subtle designed hybrid Li-ion capacitor allows rapid electron and ion transport in the non-aqueous electrolyte. Within a voltage range of 0.0-3.8 V, a high energy of 82 Wh kg(-1) is achieved at a power density of 570 W kg(-1). Even at an 8.4 s charge/discharge rate, an energy density as high as 21 Wh kg(-1) can be retained. These results demonstrate that the TiO(2) NBA//graphene hydrogel LIC exhibits higher energy density than supercapacitors and better power density than Li-ion batteries, which makes it a promising electrochemical power source. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

One-step hydrothermal synthesis of three-dimensional porous Ni-Co sulfide/reduced graphene oxide composite with optimal incorporation of carbon nanotubes for high performance supercapacitors

NASA Astrophysics Data System (ADS)

Chiu, Cheng-Ting; Chen, Dong-Hwang

2018-04-01

Three-dimensional (3D) porous Ni-Co sulfide/reduced graphene oxide composite with the appropriate incorporation of carbon nanotubes (NCS/rGO/CNT) was fabricated as a promising material for supercapacitor electrodes. It combined the high pseudo-capacitance of Ni-Co sulfide as well as the large specific surface area and electrical double layer capacitance of reduced graphene oxide (rGO). Carbon nanotubes (CNTs) were incorporated to act as the spacer for hindering the restacking of rGO and to construct a conductive network for enhancing the electron transport. The 3D porous NCS/rGO/CNT composite was fabricated by a facile one-step hydrothermal process in which Ni-Co sulfide nanosheets were synthesized and graphene oxide was reduced simultaneously. It was shown that the capacitance and cyclic performance indeed could be effectively improved via the appropriate addition of CNTs. In addition, a flexible all-solid-state asymmetric supercapacitor based on the NCS/rGO/CNT electrode was fabricated and exhibited the same capacitive electrochemical performance under bending. Also, it could successfully turn on a light-emitting diode light, revealing its feasibility in practical application. All results demonstrated that the developed NCS/rGO/CNT composite has potential application in supercapacitors.

Graphene field-effect devices

NASA Astrophysics Data System (ADS)

Echtermeyer, T. J.; Lemme, M. C.; Bolten, J.; Baus, M.; Ramsteiner, M.; Kurz, H.

2007-09-01

In this article, graphene is investigated with respect to its electronic properties when introduced into field effect devices (FED). With the exception of manual graphene deposition, conventional top-down CMOS-compatible processes are applied. Few and monolayer graphene sheets are characterized by scanning electron microscopy, atomic force microscopy and Raman spectroscopy. The electrical properties of monolayer graphene sandwiched between two silicon dioxide films are studied. Carrier mobilities in graphene pseudo-MOS structures are compared to those obtained from double-gated Graphene-FEDs and silicon metal-oxide-semiconductor field-effect-transistors (MOSFETs).

First-principles study on silicon atom doped monolayer graphene

NASA Astrophysics Data System (ADS)

Rafique, Muhammad; Shuai, Yong; Hussain, Nayyar

2018-01-01

This paper illustrates the structural, electronic and optical properties of individual silicon (Si) atom-doped single layer graphene using density functional theory method. Si atom forms tight bonding with graphene layer. The effect of doping has been investigated by varying the concentration of Si atoms from 3.125% to 9.37% (i.e. From one to three Si atoms in 4 × 4 pure graphene supercell containing 32 carbon atoms), respectively. Electronic structure, partial density of states (PDOS) and optical properties of pure and Si atom-doped graphene sheet were calculated using VASP (Vienna ab-initio Simulation Package). The calculated results for pure graphene sheet were then compared with Si atom doped graphene. It is revealed that upon Si doping in graphene, a finite band gap appears at the high symmetric K-point, thereby making graphene a direct band gap semiconductor. Moreover, the band gap value is directly proportional to the concentration of impurity Si atoms present in graphene lattice. Upon analyzing the optical properties of Si atom-doped graphene structures, it is found that, there is significant change in the refractive index of the graphene after Si atom substitution in graphene. In addition, the overall absorption spectrum of graphene is decreased after Si atom doping. Although a significant red shift in absorption is found to occur towards visible range of radiation when Si atom is substituted in its lattice. The reflectivity of graphene improves in low energy region after Si atom substitution in graphene. These results can be useful for tuning the electronic structure and to manipulate the optical properties of graphene layer in the visible region.

Stable aqueous dispersions of functionalized multi-layer graphene by pulsed underwater plasma exfoliation of graphite

NASA Astrophysics Data System (ADS)

Meyer-Plath, Asmus; Beckert, Fabian; Tölle, Folke J.; Sturm, Heinz; Mülhaupt, Rolf

2016-02-01

A process was developed for graphite particle exfoliation in water to stably dispersed multi-layer graphene. It uses electrohydraulic shockwaves and the functionalizing effect of solution plasma discharges in water. The discharges were excited by 100 ns high voltage pulsing of graphite particle chains that bridge an electrode gap. The underwater discharges allow simultaneous exfoliation and chemical functionalization of graphite particles to partially oxidized multi-layer graphene. Exfoliation is caused by shockwaves that result from rapid evaporation of carbon and water to plasma-excited gas species. Depending on discharge energy and locus of ignition, the shockwaves cause stirring, erosion, exfoliation and/or expansion of graphite flakes. The process was optimized to produce long-term stable aqueous dispersions of multi-layer graphene from graphite in a single process step without requiring addition of intercalants, surfactants, binders or special solvents. A setup was developed that allows continuous production of aqueous dispersions of flake size-selected multi-layer graphenes. Due to the well-preserved sp2-carbon structure, thin films made from the dispersed graphene exhibited high electrical conductivity. Underwater plasma discharge processing exhibits high innovation potential for morphological and chemical modifications of carbonaceous materials and surfaces, especially for the generation of stable dispersions of two-dimensional, layered materials.

Electronic and optical properties of novel carbon allotropes

DOE PAGES

Wang, Zhanyu; Dong, F.; Shen, B.; ...

2016-01-22

The vibrational properties, electronic structures and optical properties of novel carbon allotropes, such as monolayer penta-graphene (PG), double-layer PG and T12-carbon, were studied by first-principles calculations. Results of phonon calculations demonstrate that these exotic carbon allotropes are dynamically stable. The bulk T12 phase is an indirect-gap semiconductor having a quasiparticle (QP) bandgap of ~5.19 eV. When the bulk material transforms to a two-dimensional (2D) phase, the monolayer and double-layer PG become quasi-direct gap semiconductors with smaller QP bandgaps of ~4.48 eV and ~3.67 eV, respectively. Furthermore, the partial charge density analysis indicates that the 2D phases retain part of themore » electronic characteristics of the T12 phase. The linear photon energy-dependent dielectric functions and related optical properties including refractive index, extinction coefficient, absorption spectrum, reflectivity, and energy-loss spectrum were also computed and discussed. Additionally, the chemical stability of monolayer PG and the electronic and optical properties of double-side hydrogenated monolayer PG were also investigated. Furthermore, the results obtained from our calculations are beneficial to practical applications of these exotic carbon allotropes in optoelectronics and electronics.« less

Surface modification of graphene using HBC-6ImBr in solution-processed OLEDs

NASA Astrophysics Data System (ADS)

Cheng, Tsung-Chin; Ku, Ting-An; Huang, Kuo-You; Chou, Ang-Sheng; Chang, Po-Han; Chang, Chao-Chen; Yue, Cheng-Feng; Liu, Chia-Wei; Wang, Po-Han; Wong, Ken-Tsung; Wu, Chih-I.

2018-01-01

In this work, we report a simple method for solution-processed organic light emitting devices (OLEDs), where single-layer graphene acts as the anode and the hexa-peri-hexabenzocoronene exfoliating agent (HBC-6ImBr) provides surface modification. In SEM images, the PEDOT:PSS solution fully covered the graphene electrode after coating with HBC-6ImBr. The fabricated solution-processed OLEDs with a single-layer graphene anode showed outstanding brightness at 3182 cd/m2 and current efficiency up to 6 cd/A which is comparable to that of indium tin oxide films, and the OLED device brightness performance increases six times compared to tri-layer graphene treated with UV-Ozone at the same driving voltage. This method can be used in a wide variety of solution-processed organic optoelectronics on surface-modified graphene anodes.

Direct Growth of Graphene on Silicon by Metal-Free Chemical Vapor Deposition

NASA Astrophysics Data System (ADS)

Tai, Lixuan; Zhu, Daming; Liu, Xing; Yang, Tieying; Wang, Lei; Wang, Rui; Jiang, Sheng; Chen, Zhenhua; Xu, Zhongmin; Li, Xiaolong

2018-06-01

The metal-free synthesis of graphene on single-crystal silicon substrates, the most common commercial semiconductor, is of paramount significance for many technological applications. In this work, we report the growth of graphene directly on an upside-down placed, single-crystal silicon substrate using metal-free, ambient-pressure chemical vapor deposition. By controlling the growth temperature, in-plane propagation, edge-propagation, and core-propagation, the process of graphene growth on silicon can be identified. This process produces atomically flat monolayer or bilayer graphene domains, concave bilayer graphene domains, and bulging few-layer graphene domains. This work would be a significant step toward the synthesis of large-area and layer-controlled, high-quality graphene on single-crystal silicon substrates. [Figure not available: see fulltext.

Chemical storage of hydrogen in few-layer graphene

PubMed Central

Subrahmanyam, K. S.; Kumar, Prashant; Maitra, Urmimala; Govindaraj, A.; Hembram, K. P. S. S.; Waghmare, Umesh V.; Rao, C. N. R.

2011-01-01

Birch reduction of few-layer graphene samples gives rise to hydrogenated samples containing up to 5 wt % of hydrogen. Spectroscopic studies reveal the presence of sp3 C-H bonds in the hydrogenated graphenes. They, however, decompose readily on heating to 500 °C or on irradiation with UV or laser radiation releasing all the hydrogen, thereby demonstrating the possible use of few-layer graphene for chemical storage of hydrogen. First-principles calculations throw light on the mechanism of dehydrogenation that appears to involve a significant reconstruction and relaxation of the lattice. PMID:21282617

Detachment of CVD-grown graphene from single crystalline Ni films by a pure gas phase reaction

NASA Astrophysics Data System (ADS)

Zeller, Patrick; Henß, Ann-Kathrin; Weinl, Michael; Diehl, Leo; Keefer, Daniel; Lippmann, Judith; Schulz, Anne; Kraus, Jürgen; Schreck, Matthias; Wintterlin, Joost

2016-11-01

Despite great previous efforts there is still a high need for a simple, clean, and upscalable method for detaching epitaxial graphene from the metal support on which it was grown. We present a method based on a pure gas phase reaction that is free of solvents and polymer supports and avoids mechanical transfer steps. The graphene was grown on 150 nm thick, single crystalline Ni(111) films on Si(111) wafers with YSZ buffer layers. Its quality was monitored by using low energy electron diffraction and scanning tunneling microscopy. The gas phase etching uses a chemical transport reaction, the so-called Mond process, based on the formation of gaseous nickel tetracarbonyl in 1 bar of CO at 75 °C and by adding small amounts of sulfide catalysts. X-ray photoelectron spectroscopy, Raman spectroscopy and scanning electron microscopy were used to characterize the detached graphene. It was found that the method successfully removes the nickel from underneath the graphene layer, so that the graphene lies on the insulating oxide buffer layer. Small residual particles of nickel sulfide and cracks in the obtained graphene layer were identified. The defect concentrations were comparable to graphene samples obtained by wet chemical etching and by the bubbling transfer.

Nano-Architecture of nitrogen-doped graphene films synthesized from a solid CN source.

PubMed

Maddi, Chiranjeevi; Bourquard, Florent; Barnier, Vincent; Avila, José; Asensio, Maria-Carmen; Tite, Teddy; Donnet, Christophe; Garrelie, Florence

2018-02-19

New synthesis routes to tailor graphene properties by controlling the concentration and chemical configuration of dopants show great promise. Herein we report the direct reproducible synthesis of 2-3% nitrogen-doped 'few-layer' graphene from a solid state nitrogen carbide a-C:N source synthesized by femtosecond pulsed laser ablation. Analytical investigations, including synchrotron facilities, made it possible to identify the configuration and chemistry of the nitrogen-doped graphene films. Auger mapping successfully quantified the 2D distribution of the number of graphene layers over the surface, and hence offers a new original way to probe the architecture of graphene sheets. The films mainly consist in a Bernal ABA stacking three-layer architecture, with a layer number distribution ranging from 2 to 6. Nitrogen doping affects the charge carrier distribution but has no significant effects on the number of lattice defects or disorders, compared to undoped graphene synthetized in similar conditions. Pyridinic, quaternary and pyrrolic nitrogen are the dominant chemical configurations, pyridinic N being preponderant at the scale of the film architecture. This work opens highly promising perspectives for the development of self-organized nitrogen-doped graphene materials, as synthetized from solid carbon nitride, with various functionalities, and for the characterization of 2D materials using a significant new methodology.

Characterization of spatial manipulation on ZnO nanocomposites consisting of Au nanoparticles, a graphene layer, and ZnO nanorods

NASA Astrophysics Data System (ADS)

Huang, Shen-Che; Lu, Chien-Cheng; Su, Wei-Ming; Weng, Chen-Yuan; Chen, Yi-Cian; Wang, Shing-Chung; Lu, Tien-Chang; Chen, Ching-Pang; Chen, Hsiang

2018-01-01

Three types of ZnO-based nanocomposites were fabricated consisting of 80-nm Au nanoparticles (NPs), a graphene layer, and ZnO nanorods (NRs). To investigate interactions between the ZnO NRs and Au nanoparticle, multiple material analysis techniques including field-emission scanning electron microscopy (FESEM), surface contact angle measurements, secondary ion mass spectrometry (SIMS), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopic characterizations were performed. Results indicate that incorporating a graphene layer could block the interaction between the ZnO NRs and the Au NPs. Furthermore, the Raman signal of the Au NPs could be enhanced by inserting a graphene layer on top of the ZnO NRs. Investigation of these graphene-incorporated nanocomposites would be helpful to future studies of the physical properties and Raman analysis of the ZnO-based nanostructure design.

Magnetotransport properties of a few-layer graphene-ferromagnetic metal junctions in vertical spin valve devices

DOE Office of Scientific and Technical Information (OSTI.GOV)

Entani, Shiro, E-mail: entani.shiro@jaea.go.jp; Naramoto, Hiroshi; Sakai, Seiji

2015-05-07

Magnetotransport properties were studied for the vertical spin valve devices with two junctions of permalloy electrodes and a few-layer graphene interlayer. The graphene layer was directly grown on the bottom electrode by chemical vapor deposition. X-ray photoelectron spectroscopy showed that the permalloy surface fully covered with a few-layer graphene is kept free from oxidation and contamination even after dispensing and removing photoresist. This enabled fabrication of the current perpendicular to plane spin valve devices with a well-defined interface between graphene and permalloy. Spin-dependent electron transport measurements revealed a distinct spin valve effect in the devices. The magnetotransport ratio was 0.8%more » at room temperature and increased to 1.75% at 50 K. Linear current-voltage characteristics and resistance increase with temperature indicated that ohmic contacts are realized at the relevant interfaces.« less

Fine-tuning the Wall Thickness of Ordered Mesoporous Graphene by Exploiting Ligand Exchange of Colloidal Nanocrystals

NASA Astrophysics Data System (ADS)

Han, Dandan; Yan, Yancui; Wei, Jishi; Wang, Biwei; Li, Tongtao; Guo, Guannan; Yang, Dong; Xie, Songhai; Dong, Angang

2017-12-01

Because of their unique physical properties, three-dimensional (3D) graphene has attracted enormous attention over the past years. However, it is still a challenge to precisely control the layer thickness of 3D graphene. Here, we report a novel strategy to rationally adjust the wall thickness of ordered mesoporous graphene (OMG). By taking advantage of ligand exchange capability of colloidal Fe3O4 nanocrystals, we are able to fine-tune the wall thickness of OMG from 2 to 6 layers of graphene by tailoring the hydrocarbon ligands attached to the nanocrystal surface. When evaluated as electrocatalyst for oxygen reduction reaction upon S and N doping, the 4-layer OMG is found to show better catalytic performance compared with its 2- and 6-layer counterparts, which we attribute to the enhanced exposure of active sites resulting from its ultrathin wall thickness and high surface area.

Voltage contrast X-ray photoelectron spectroscopy reveals graphene-substrate interaction in graphene devices fabricated on the C- and Si- faces of SiC

DOE Office of Scientific and Technical Information (OSTI.GOV)

Aydogan, Pinar; Suzer, Sefik, E-mail: suzer@fen.bilkent.edu.tr; Arslan, Engin

2015-09-21

We report on an X-ray photoelectron spectroscopy (XPS) study of two graphene based devices that were analyzed by imposing a significant current under +3 V bias. The devices were fabricated as graphene layers(s) on hexagonal SiC substrates, either on the C- or Si-terminated faces. Position dependent potential distributions (IR-drop), as measured by variations in the binding energy of a C1s peak are observed to be sporadic for the C-face graphene sample, but very smooth for the Si-face one, although the latter is less conductive. We attribute these sporadic variations in the C-face device to the incomplete electrical decoupling between the graphenemore » layer(s) with the underlying buffer and/or substrate layers. Variations in the Si2p and O1s peaks of the underlayer(s) shed further light into the electrical interaction between graphene and other layers. Since the potential variations are amplified only under applied bias (voltage-contrast), our methodology gives unique, chemically specific electrical information that is difficult to obtain by other techniques.« less

Tuning electronic properties by oxidation-reduction reactions at graphene-ruthenium interface

DOE PAGES

Kandyba, Viktor; Al-Mahboob, Abdullah; Giampietri, Alessio; ...

2018-06-06

Mass production of graphene is associated with the growth on catalysts used also in other chemical reactions. In this study, we exploit the oxidation-reduction to tailor the properties of single layer graphene domains with incorporated bi-layer patches on ruthenium. Using photoelectron spectromicroscopy techniques, we find that oxygen, intercalating under single layer and making it p-doped by the formation of Ru-O x, does not intercalate under the bilayer patches with n-doped upper layer, but decorates them under single layer surrounding creating lateral p-n junctions with chemical potential difference of 1.2 eV. O-reduction by thermal treatment in vacuum results in C-vacancy defectsmore » enhancing electronic coupling of remained graphene to Ru, whereas in H 2, vacancy formation is suppressed. Also, for the domains below 15–25 μm size, after O-reduction in H 2, graphene/Ru coupling is restored, while wrinkle pattern produced by O-intercalation is irreversible and can trap reaction products between the wrinkles and Ru surface step edges. In fact, in certain regions of bigger domains, the products, containing H 2O and/or its fragments, remain at the interface, making graphene decoupled and undoped.« less

Electrically tunable coherent optical absorption in graphene with ion gel.

PubMed

Thareja, Vrinda; Kang, Ju-Hyung; Yuan, Hongtao; Milaninia, Kaveh M; Hwang, Harold Y; Cui, Yi; Kik, Pieter G; Brongersma, Mark L

2015-03-11

We demonstrate electrical control over coherent optical absorption in a graphene-based Salisbury screen consisting of a single layer of graphene placed in close proximity to a gold back reflector. The screen was designed to enhance light absorption at a target wavelength of 3.2 μm by using a 600 nm-thick, nonabsorbing silica spacer layer. An ionic gel layer placed on top of the screen was used to electrically gate the charge density in the graphene layer. Spectroscopic reflectance measurements were performed in situ as a function of gate bias. The changes in the reflectance spectra were analyzed using a Fresnel based transfer matrix model in which graphene was treated as an infinitesimally thin sheet with a conductivity given by the Kubo formula. The analysis reveals that a careful choice of the ionic gel layer thickness can lead to optical absorption enhancements of up to 5.5 times for the Salisbury screen compared to a suspended sheet of graphene. In addition to these absorption enhancements, we demonstrate very large electrically induced changes in the optical absorption of graphene of ∼3.3% per volt, the highest attained so far in a device that features an atomically thick active layer. This is attributable in part to the more effective gating achieved with the ion gel over the conventional dielectric back gates and partially by achieving a desirable coherent absorption effect linked to the presence of the thin ion gel that boosts the absorption by 40%.

Thickness scaling of atomic-layer-deposited HfO2 films and their application to wafer-scale graphene tunnelling transistors

PubMed Central

Jeong, Seong-Jun; Gu, Yeahyun; Heo, Jinseong; Yang, Jaehyun; Lee, Chang-Seok; Lee, Min-Hyun; Lee, Yunseong; Kim, Hyoungsub; Park, Seongjun; Hwang, Sungwoo

2016-01-01

The downscaling of the capacitance equivalent oxide thickness (CET) of a gate dielectric film with a high dielectric constant, such as atomic layer deposited (ALD) HfO2, is a fundamental challenge in achieving high-performance graphene-based transistors with a low gate leakage current. Here, we assess the application of various surface modification methods on monolayer graphene sheets grown by chemical vapour deposition to obtain a uniform and pinhole-free ALD HfO2 film with a substantially small CET at a wafer scale. The effects of various surface modifications, such as N-methyl-2-pyrrolidone treatment and introduction of sputtered ZnO and e-beam-evaporated Hf seed layers on monolayer graphene, and the subsequent HfO2 film formation under identical ALD process parameters were systematically evaluated. The nucleation layer provided by the Hf seed layer (which transforms to the HfO2 layer during ALD) resulted in the uniform and conformal deposition of the HfO2 film without damaging the graphene, which is suitable for downscaling the CET. After verifying the feasibility of scaling down the HfO2 thickness to achieve a CET of ~1.5 nm from an array of top-gated metal-oxide-graphene field-effect transistors, we fabricated graphene heterojunction tunnelling transistors with a record-low subthreshold swing value of <60 mV/dec on an 8″ glass wafer. PMID:26861833

Rebar graphene from functionalized boron nitride nanotubes.

PubMed

Li, Yilun; Peng, Zhiwei; Larios, Eduardo; Wang, Gunuk; Lin, Jian; Yan, Zheng; Ruiz-Zepeda, Francisco; José-Yacamán, Miguel; Tour, James M

2015-01-27

The synthesis of rebar graphene on Cu substrates is described using functionalized boron nitride nanotubes (BNNTs) that were annealed or subjected to chemical vapor deposition (CVD) growth of graphene. Characterization shows that the BNNTs partially unzip and form a reinforcing bar (rebar) network within the graphene layer that enhances the mechanical strength through covalent bonds. The rebar graphene is transferrable to other substrates without polymer assistance. The optical transmittance and conductivity of the hybrid rebar graphene film was tested, and a field effect transistor was fabricated to explore its electrical properties. This method of synthesizing 2D hybrid graphene/BN structures should enable the hybridization of various 1D nanotube and 2D layered structures with enhanced mechanical properties.

FAST TRACK COMMUNICATION: Graphene based quantum dots

NASA Astrophysics Data System (ADS)

Zhang, H. G.; Hu, H.; Pan, Y.; Mao, J. H.; Gao, M.; Guo, H. M.; Du, S. X.; Greber, T.; Gao, H.-J.

2010-08-01

Laterally localized electronic states are identified on a single layer of graphene on ruthenium by low temperature scanning tunneling spectroscopy (STS). The individual states are separated by 3 nm and comprise regions of about 90 carbon atoms. This constitutes a highly regular quantum dot-array with molecular precision. It is evidenced by quantum well resonances (QWRs) with energies that relate to the corrugation of the graphene layer. The dI/dV conductance spectra are modeled by a layer height dependent potential-well with a delta-function potential that describes the barrier for electron penetration into graphene. The resulting QWRs are strongest and lowest in energy on the isolated 'hill' regions with a diameter of 2 nm, where the graphene is decoupled from the surface.

Strong Fermi-Level Pinning at Metal/n-Si(001) Interface Ensured by Forming an Intact Schottky Contact with a Graphene Insertion Layer.

PubMed

Yoon, Hoon Hahn; Jung, Sungchul; Choi, Gahyun; Kim, Junhyung; Jeon, Youngeun; Kim, Yong Soo; Jeong, Hu Young; Kim, Kwanpyo; Kwon, Soon-Yong; Park, Kibog

2017-01-11

We report the systematic experimental studies demonstrating that a graphene layer inserted at metal/n-Si(001) interface is efficient to explore interface Fermi-level pinning effect. It is confirmed that an inserted graphene layer prevents atomic interdiffusion to form an atomically abrupt Schottky contact. The Schottky barriers of metal/graphene/n-Si(001) junctions show a very weak dependence on metal work-function, implying that the metal Fermi-level is almost completely pinned at charge neutrality level close to the valence band edge of Si. The atomically impermeable and electronically transparent properties of graphene can be used generally to form an intact Schottky contact for all semiconductors.

Graphene based quantum dots.

PubMed

Zhang, H G; Hu, H; Pan, Y; Mao, J H; Gao, M; Guo, H M; Du, S X; Greber, T; Gao, H-J

2010-08-04

Laterally localized electronic states are identified on a single layer of graphene on ruthenium by low temperature scanning tunneling spectroscopy (STS). The individual states are separated by 3 nm and comprise regions of about 90 carbon atoms. This constitutes a highly regular quantum dot-array with molecular precision. It is evidenced by quantum well resonances (QWRs) with energies that relate to the corrugation of the graphene layer. The dI/dV conductance spectra are modeled by a layer height dependent potential-well with a delta-function potential that describes the barrier for electron penetration into graphene. The resulting QWRs are strongest and lowest in energy on the isolated 'hill' regions with a diameter of 2 nm, where the graphene is decoupled from the surface.

Raman spectroscopy of few-layer graphene prepared by C2-C6 cluster ion implantation

NASA Astrophysics Data System (ADS)

Wang, Z. S.; Zhang, R.; Zhang, Z. D.; Huang, Z. H.; Liu, C. S.; Fu, D. J.; Liu, J. R.

2013-07-01

Few-layer graphene has been prepared on 300 nm-thick Ni films by C2-C6 cluster ion implantation at 20 keV/cluster. Raman spectroscopy reveals significant influence of the number of atoms in the cluster, the implantation dose, and thermal treatment on the structure of the graphene layers. In particular, the graphene samples exhibit a sharp G peak at 1584 cm-1 and 2D peaks at 2711-2717 cm-1. The IG/I2D ratios higher than 1.70 and IG/ID ratio as high as 1.95 confirm that graphene sheets with low density of defects have been synthesized with much improved quality by ion implantation with larger clusters of C4-C6.

Utilizing boron nitride sheets as thin supports for high resolution imaging of nanocrystals.

PubMed

Wu, Yimin A; Kirkland, Angus I; Schäffel, Franziska; Porfyrakis, Kyriakos; Young, Neil P; Briggs, G Andrew D; Warner, Jamie H

2011-05-13

We demonstrate the use of thin BN sheets as supports for imaging nanocrystals using low voltage (80 kV) aberration-corrected high resolution transmission electron microscopy. This provides an alternative to the previously utilized 2D crystal supports of graphene and graphene oxide. A simple chemical exfoliation method is applied to get few layer boron nitride (BN) sheets with micrometer-sized dimensions. This generic approach of using BN sheets as supports is shown by depositing Mn doped ZnSe nanocrystals directly onto the BN sheets and resolving the atomic structure from both the ZnSe nanocrystals and the BN support. Phase contrast images reveal moiré patterns of interference between the beams diffracted by the nanocrystals and the BN substrate that are used to determine the relative orientation of the nanocrystals with respect to the BN sheets and interference lattice planes. Double diffraction is observed and has been analyzed.

Three-dimensional sulphur/nitrogen co-doped reduced graphene oxide as high-performance supercapacitor binder-free electrodes

NASA Astrophysics Data System (ADS)

Huo, Jinghao; Zheng, Peng; Wang, Xiaofei; Guo, Shouwu

2018-06-01

Sulphur/nitrogen co-doped reduced graphene oxide (SNG) aerogels were prepared by a simple solvothermal method with l-cysteine-assisted in ethylene glycol. The morphology and composition tests showed that the S/N heteroatoms were evenly distributed on SNG microsheets, and these microsheets were further composed of SNG aerogels with three-dimensional (3D) porous structure. The cyclic voltammetry and galvanostatic charge/discharge tests illustrated the SNG bind-free electrode possessed electric double-layer capacitance and pseudocapacitance, and had a capacitance of 254 F g-1 at a current density of 1 A g-1. After the 5000 cycles tests, the capacitance retained 83.54% at a current density of 2 A g-1. Meanwhile, the electrochemical impedance spectroscopy data shown the electrode materials had excellent capacity and good conductivity. Hence, the SNG aerogel prepared by l-cysteine-assisted solvothermal method is a great material for high-performance supercapacitors.

Highly Enhanced Electromechanical Stability of Large-Area Graphene with Increased Interfacial Adhesion Energy by Electrothermal-Direct Transfer for Transparent Electrodes.

PubMed

Kim, Jangheon; Kim, Gi Gyu; Kim, Soohyun; Jung, Wonsuk

2016-09-07

Graphene, a two-dimensional sheet of carbon atoms in a hexagonal lattice structure, has been extensively investigated for research and industrial applications as a promising material with outstanding electrical, mechanical, and chemical properties. To fabricate graphene-based devices, graphene transfer to the target substrate with a clean and minimally defective surface is the first step. However, graphene transfer technologies require improvement in terms of uniform transfer with a clean, nonfolded and nontorn area, amount of defects, and electromechanical reliability of the transferred graphene. More specifically, uniform transfer of a large area is a key challenge when graphene is repetitively transferred onto pretransferred layers because the adhesion energy between graphene layers is too low to ensure uniform transfer, although uniform multilayers of graphene have exhibited enhanced electrical and optical properties. In this work, we developed a newly suggested electrothermal-direct (ETD) transfer method for large-area high quality monolayer graphene with less defects and an absence of folding or tearing of the area at the surface. This method delivers uniform multilayer transfer of graphene by repetitive monolayer transfer steps based on high adhesion energy between graphene layers and the target substrate. To investigate the highly enhanced electromechanical stability, we conducted mechanical elastic bending experiments and reliability tests in a highly humid environment. This ETD-transferred graphene is expected to replace commercial transparent electrodes with ETD graphene-based transparent electrodes and devices such as a touch panels with outstanding electromechanical stability.

Improvement of Energy Capacity with Vitamin C Treated Dual-Layered Graphene-Sulfur Cathodes in Lithium-Sulfur Batteries.

PubMed

Kim, Jin Won; Ocon, Joey D; Kim, Ho-Sung; Lee, Jaeyoung

2015-09-07

A graphene-based cathode design for lithium-sulfur batteries (LSB) that shows excellent electrochemical performance is proposed. The dual-layered cathode is composed of a sulfur active layer and a polysulfide absorption layer, and both layers are based on vitamin C treated graphene oxide at various degrees of reduction. By controlling the degree of reduction of graphene, the dual-layered cathode can increase sulfur utilization dramatically owing to the uniform formation of nanosized sulfur particles, the chemical bonding of dissolved polysulfides on the oxygen-rich sulfur active layer, and the physisorption of free polysulfides on the absorption layer. This approach enables a LSB with a high specific capacity of over 600 mAh gsulfur (-1) after 100 cycles even under a high current rate of 1C (1675 mA gsulfur (-1) ). An intriguing aspect of our work is the synthesis of a high-performance dual-layered cathode by a green chemistry method, which could be a promising approach to LSBs with high energy and power densities. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Reduced electron back-injection in Al2O3/AlOx/Al2O3/graphene charge-trap memory devices

NASA Astrophysics Data System (ADS)

Lee, Sejoon; Song, Emil B.; Min Kim, Sung; Lee, Youngmin; Seo, David H.; Seo, Sunae; Wang, Kang L.

2012-12-01

A graphene charge-trap memory is devised using a single-layer graphene channel with an Al2O3/AlOx/Al2O3 oxide stack, where the ion-bombarded AlOx layer is intentionally added to create an abundance of charge-trap sites. The low dielectric constant of AlOx compared to Al2O3 reduces the potential drop in the control oxide Al2O3 and suppresses the electron back-injection from the gate to the charge-storage layer, allowing the memory window of the device to be further extended. This shows that the usage of a lower dielectric constant in the charge-storage layer compared to that of the control oxide layer improves the memory performance for graphene charge-trap memories.

Quantitative secondary electron imaging for work function extraction at atomic level and layer identification of graphene

PubMed Central

Zhou, Yangbo; Fox, Daniel S; Maguire, Pierce; O’Connell, Robert; Masters, Robert; Rodenburg, Cornelia; Wu, Hanchun; Dapor, Maurizio; Chen, Ying; Zhang, Hongzhou

2016-01-01

Two-dimensional (2D) materials usually have a layer-dependent work function, which require fast and accurate detection for the evaluation of their device performance. A detection technique with high throughput and high spatial resolution has not yet been explored. Using a scanning electron microscope, we have developed and implemented a quantitative analytical technique which allows effective extraction of the work function of graphene. This technique uses the secondary electron contrast and has nanometre-resolved layer information. The measurement of few-layer graphene flakes shows the variation of work function between graphene layers with a precision of less than 10 meV. It is expected that this technique will prove extremely useful for researchers in a broad range of fields due to its revolutionary throughput and accuracy. PMID:26878907

Graphene decorated microelectrodes for simultaneous detection of ascorbic, dopamine, and folic acids by means of chemical vapor deposition

NASA Astrophysics Data System (ADS)

Namdar, N.; Hassanpour Amiri, M.; Dehghan Nayeri, F.; Gholizadeh, A.; Mohajerzadeh, S.

2015-09-01

In this paper, high quality and large area graphene layers were synthesized using thermal chemical vapour deposition on copper foil substrates. We use graphene incorporated electrodes to measure simultaneously ascorbic acid, dopamine and folic acid. Cyclic voltammetry and differential pulse voltammetry methods were used to evaluate electrochemical behaviour of the grown graphene layers. The graphene-modified electrode shows large electrochemical potential difference compared to bare gold electrodes with higher current responses. Also our fabricated electrodes configuration can be used easily for microfluidic analysis.

Atomistic simulation on the plastic deformation and fracture of bio-inspired graphene/Ni nanocomposites

NASA Astrophysics Data System (ADS)

Yang, Zhenyu; Wang, Dandan; Lu, Zixing; Hu, Wenjun

2016-11-01

Molecular dynamics simulations were performed to investigate the plastic deformation and fracture behaviors of bio-inspired graphene/metal nanocomposites, which have a "brick-and-mortar" nanostructure, consisting of hard graphene single-layers embedded in a soft Ni matrix. The plastic deformation mechanisms of the nanocomposites were analyzed as well as their effects on the mechanical properties with various geometrical variations. It was found that the strength and ductility of the metal matrix can be highly enhanced with the addition of the staggered graphene layers, and the plastic deformation can be attributed to the interfacial sliding, dislocation nucleation, and cracks' combination. The strength of the nanocomposites strongly depends on the length scale of the nanostructure and the interlayer distance as well. In addition, slip at the interface releases the stress in graphene layers, leading to the stress distribution on the graphene more uniform. The present results are expected to contribute to the design of the nanolayered graphene/metal composites with high performance.

Microwave-Assisted Synthesis of Highly-Crumpled, Few-Layered Graphene and Nitrogen-Doped Graphene for Use as High-Performance Electrodes in Capacitive Deionization

NASA Astrophysics Data System (ADS)

Amiri, Ahmad; Ahmadi, Goodarz; Shanbedi, Mehdi; Savari, Maryam; Kazi, S. N.; Chew, B. T.

2015-12-01

Capacitive deionization (CDI) is a promising procedure for removing various charged ionic species from brackish water. The performance of graphene-based material in capacitive deionization is lower than the expectation of the industry, so highly-crumpled, few-layered graphene (HCG) and highly-crumpled nitrogen-doped graphene (HCNDG) with high surface area have been introduced as promising candidates for CDI electrodes. Thus, HCG and HCNDG were prepared by exfoliation of graphite in the presence of liquid-phase, microwave-assisted methods. An industrially-scalable, cost-effective, and simple approach was employed to synthesize HCG and HCNDG, resulting in few-layered graphene and nitrogen-doped graphene with large specific surface area. Then, HCG and HCNDG were utilized for manufacturing a new class of carbon nanostructure-based electrodes for use in large-scale CDI equipment. The electrosorption results indicated that both the HCG and HCNDG have fairly large specific surface areas, indicating their huge potential for capacitive deionization applications.

Superconductivity at 7.4 K in few layer graphene by Li-intercalation.

PubMed

Tiwari, Anand P; Shin, Soohyeon; Hwang, Eunhee; Jung, Soon-Gil; Park, Tuson; Lee, Hyoyoung

2017-11-08

Superconductivity in graphene has been highly sought after for its promise in various device applications and for general scientific interest. Ironically, the simple electronic structure of graphene, which is responsible for novel quantum phenomena, hinders the emergence of superconductivity. Theory predicts that doping the surface of the graphene effectively alters the electronic structure, thus promoting propensity towards Cooper pair instability (Profeta et al (2012) Nat. Phys. 8 131-4; Nandkishore et al (2012) Nat. Phys. 8 158-63) [1, 2]. Here we report the emergence of superconductivity at 7.4 K in Li-intercalated few-layer-graphene (FLG). The absence of superconductivity in 3D Li-doped graphite underlines that superconductivity in Li-FLG arises from the novel electronic properties of the 2D graphene layer. These results are expected to guide future research on graphene-based superconductivity, both in theory and experiments. In addition, easy control of the Li-doping process holds promise for various device applications.

Graphene quantum blisters: A tunable system to confine charge carriers

NASA Astrophysics Data System (ADS)

Abdullah, H. M.; Van der Donck, M.; Bahlouli, H.; Peeters, F. M.; Van Duppen, B.

2018-05-01

Due to Klein tunneling, electrostatic confinement of electrons in graphene is not possible. This hinders the use of graphene for quantum dot applications. Only through quasi-bound states with finite lifetime has one achieved to confine charge carriers. Here, we propose that bilayer graphene with a local region of decoupled graphene layers is able to generate bound states under the application of an electrostatic gate. The discrete energy levels in such a quantum blister correspond to localized electron and hole states in the top and bottom layers. We find that this layer localization and the energy spectrum itself are tunable by a global electrostatic gate and that the latter also coincides with the electronic modes in a graphene disk. Curiously, states with energy close to the continuum exist primarily in the classically forbidden region outside the domain defining the blister. The results are robust against variations in size and shape of the blister which shows that it is a versatile system to achieve tunable electrostatic confinement in graphene.

Photoinduced doping in heterostructures of graphene and boron nitride.

PubMed

Ju, L; Velasco, J; Huang, E; Kahn, S; Nosiglia, C; Tsai, Hsin-Zon; Yang, W; Taniguchi, T; Watanabe, K; Zhang, Y; Zhang, G; Crommie, M; Zettl, A; Wang, F

2014-05-01

The design of stacks of layered materials in which adjacent layers interact by van der Waals forces has enabled the combination of various two-dimensional crystals with different electrical, optical and mechanical properties as well as the emergence of novel physical phenomena and device functionality. Here, we report photoinduced doping in van der Waals heterostructures consisting of graphene and boron nitride layers. It enables flexible and repeatable writing and erasing of charge doping in graphene with visible light. We demonstrate that this photoinduced doping maintains the high carrier mobility of the graphene/boron nitride heterostructure, thus resembling the modulation doping technique used in semiconductor heterojunctions, and can be used to generate spatially varying doping profiles such as p-n junctions. We show that this photoinduced doping arises from microscopically coupled optical and electrical responses of graphene/boron nitride heterostructures, including optical excitation of defect transitions in boron nitride, electrical transport in graphene, and charge transfer between boron nitride and graphene.

The design of a Li-ion full cell battery using a nano silicon and nano multi-layer graphene composite anode

NASA Astrophysics Data System (ADS)

Eom, KwangSup; Joshi, Tapesh; Bordes, Arnaud; Do, Inhwan; Fuller, Thomas F.

2014-03-01

In this study, a Si-graphene composite, which is composed of nano Si particles and nano-sized multi-layer graphene particles, and micro-sized multi-layer graphene plate conductor, was used as the anode for Li-ion battery. The Si-graphene electrode showed the high capacity and stable cyclability at charge/discharge rate of C/2 in half cell tests. Nickel cobalt aluminum material (NCA) was used as a cathode in the full cell to evaluate the practicality of the new Si-graphene material. Although the Si-graphene anode has more capacity than the NCA cathode in this designed full cell, the Si-graphene anode had a greater effect on the full-cell performance due to its large initial irreversible capacity loss and continuous SEI formation during cycling. When fluoro-ethylene carbonate was added to the electrolyte, the cyclability of the full cell was much improved due to less SEI formation, which was confirmed by the decreases in the 1st irreversible capacity loss, overpotential for the 1st lithiation, and the resistance of the SEI.

Interaction of bimetallic PtCo layers with bare and graphene-covered ZnO(0001) supports

NASA Astrophysics Data System (ADS)

Luo, Wen; Mélart, Christophe; Rach, Alain; Sutter, Christophe; Zafeiratos, Spyridon

2018-03-01

PtCo bimetallic overlayers supported on bare and graphene covered ZnO(0001) substrates have been successfully prepared and used to investigate the effect of graphene interlayer on the arrangement and the redox behaviour of PtCo. We found that Co is readily oxidized at the PtCo/ZnO interface during annealing in ultra-high vacuum (UHV) and low pressure O2 atmosphere, while after inserting a layer of graphene in-between, the oxidation of Co is restricted. In addition, the reduction of Co oxides by H2 is more pronounced when PtCo is supported on graphene covered ZnO. Apart from the cobalt oxidation state, graphene insertion at the interface also influences the PtCo arrangement by favouring their intermixing. Raman spectra show that low intensity defects are introduced into graphene layer after the deposition of PtCo and are enhanced by high temperature annealing. This study highlights the prospect of using graphene to tune the interaction between alloys and oxide supports which finds potential applications in catalysis.

High-quality graphene flakes exfoliated on a flat hydrophobic polymer

NASA Astrophysics Data System (ADS)

Pedrinazzi, Paolo; Caridad, José M.; Mackenzie, David M. A.; Pizzocchero, Filippo; Gammelgaard, Lene; Jessen, Bjarke S.; Sordan, Roman; Booth, Timothy J.; Bøggild, Peter

2018-01-01

We show that graphene supported on a hydrophobic and flat polymer surface results in flakes with extremely low doping and strain as assessed by their Raman spectroscopic characteristics. We exemplify this technique by micromechanical exfoliation of graphene on flat poly(methylmethacrylate) layers and demonstrate Raman peak intensity ratios I(2D)/I(G) approaching 10, similar to pristine freestanding graphene. We verify that these features are not an artifact of optical interference effects occurring at the substrate: they are similarly observed when varying the substrate thickness and are maintained when the environment of the graphene flake is completely changed, by encapsulating preselected flakes between hexagonal boron nitride layers. The exfoliation of clean, pristine graphene layers directly on flat polymer substrates enables high performance, supported, and non-encapsulated graphene devices for flexible and transparent optoelectronic studies. We additionally show that the access to a clean and supported graphene source leads to high-quality van der Waals heterostructures and devices with reproducible carrier mobilities exceeding 50 000 cm2 V-1 s-1 at room temperature.

Mechanical properties of graphene and boronitrene

NASA Astrophysics Data System (ADS)

Andrew, R. C.; Mapasha, R. E.; Ukpong, A. M.; Chetty, N.

2012-03-01

We present an equation of state (EOS) that describes how the hydrostatic change in surface area is related to two-dimensional in-plane pressure (F) and yields the measure of a material's resilience to isotropic stretching (the layer modulus γ) as one of its fit parameters. We give results for the monolayer systems of graphene and boronitrene, and we also include results for Si, Ge, GeC, and SiC in the isostructural honeycomb structure for comparison. Our results show that, of the honeycomb structures, graphene is the most resilient to stretching with a value of γC = 206.6 N m-1, second is boronitrene with γBN = 177.0 N m-1, followed by γSiC = 116.5 N m-1, γGeC = 101.0 N m-1, γSi = 44.5 N m-1, and γGe = 29.6 N m-1. We calculate the Young's and shear moduli from the elastic constants and find that, in general, they rank according to the layer modulus. We also find that the calculated layer modulus matches the one obtained from the EOS. We use the EOS to predict the isotropic intrinsic strength of the various systems and find that, in general, the intrinsic stresses also rank according to the layer modulus. Graphene and boronitrene have comparable strengths with intrinsic stresses of 29.4 and 26.0 N m-1, respectively. We considered four graphene allotropes including pentaheptite and graphdiyne and find that pentaheptite has a value for γ comparable to graphene. We find a phase transition from graphene to graphdiyne at F = -7.0 N m-1. We also consider bilayer, trilayer, and four-layered graphene and find that the addition of extra layers results in a linear dependence of γ with F.

Rational and practical exfoliation of graphite using well-defined poly(3-hexylthiophene) for the preparation of conductive polymer/graphene composite.

PubMed

Iguchi, Hiroki; Higashi, Chisato; Funasaki, Yuichi; Fujita, Keisuke; Mori, Atsunori; Nakasuga, Akira; Maruyama, Tatsuo

2017-01-06

Processing and manipulation of highly conductive pristine graphene in large quantities are still major challenges in the practical application of graphene for electric device. In the present study, we report the liquid-phase exfoliation of graphite in toluene using well-defined poly(3-hexylthiophene) (P3HT) to produce a P3HT/graphene composite. We synthesize and use regioregular P3HT with controlled molecular weights as conductive dispersants for graphene. Simple ultrasonication of graphite flakes with the P3HT successfully produces single-layer and few-layer graphene sheets dispersed in toluene. The produced P3HT/graphene composite can be used as conductive graphene ink, indicating that the P3HT/graphene composite has high electrical conductivity owing to the high conductivity of P3HT and graphene. The P3HT/graphene composite also works as an oxidation-resistant and conductive film for a copper substrate, which is due to the high gas-barrier property of graphene.

Rational and practical exfoliation of graphite using well-defined poly(3-hexylthiophene) for the preparation of conductive polymer/graphene composite

NASA Astrophysics Data System (ADS)

Iguchi, Hiroki; Higashi, Chisato; Funasaki, Yuichi; Fujita, Keisuke; Mori, Atsunori; Nakasuga, Akira; Maruyama, Tatsuo

2017-01-01

Processing and manipulation of highly conductive pristine graphene in large quantities are still major challenges in the practical application of graphene for electric device. In the present study, we report the liquid-phase exfoliation of graphite in toluene using well-defined poly(3-hexylthiophene) (P3HT) to produce a P3HT/graphene composite. We synthesize and use regioregular P3HT with controlled molecular weights as conductive dispersants for graphene. Simple ultrasonication of graphite flakes with the P3HT successfully produces single-layer and few-layer graphene sheets dispersed in toluene. The produced P3HT/graphene composite can be used as conductive graphene ink, indicating that the P3HT/graphene composite has high electrical conductivity owing to the high conductivity of P3HT and graphene. The P3HT/graphene composite also works as an oxidation-resistant and conductive film for a copper substrate, which is due to the high gas-barrier property of graphene.

Rational and practical exfoliation of graphite using well-defined poly(3-hexylthiophene) for the preparation of conductive polymer/graphene composite

PubMed Central

Iguchi, Hiroki; Higashi, Chisato; Funasaki, Yuichi; Fujita, Keisuke; Mori, Atsunori; Nakasuga, Akira; Maruyama, Tatsuo

2017-01-01

Processing and manipulation of highly conductive pristine graphene in large quantities are still major challenges in the practical application of graphene for electric device. In the present study, we report the liquid-phase exfoliation of graphite in toluene using well-defined poly(3-hexylthiophene) (P3HT) to produce a P3HT/graphene composite. We synthesize and use regioregular P3HT with controlled molecular weights as conductive dispersants for graphene. Simple ultrasonication of graphite flakes with the P3HT successfully produces single-layer and few-layer graphene sheets dispersed in toluene. The produced P3HT/graphene composite can be used as conductive graphene ink, indicating that the P3HT/graphene composite has high electrical conductivity owing to the high conductivity of P3HT and graphene. The P3HT/graphene composite also works as an oxidation-resistant and conductive film for a copper substrate, which is due to the high gas-barrier property of graphene. PMID:28059127

Review of Graphene as a Solid State Diffusion Barrier.

PubMed

Morrow, Wayne K; Pearton, Stephen J; Ren, Fan

2016-01-06

Conventional thin-film diffusion barriers consist of 3D bulk films with high chemical and thermal stability. The purpose of the barrier material is to prevent intermixing or penetration from the two materials that encase it. Adhesion to both top and bottom materials is critical to the success of the barrier. Here, the effectiveness of a single atomic layer of graphene as a solid-state diffusion barrier for common metal schemes used in microelectronics is reviewed, and specific examples are discussed. Initial studies of electrical contacts to graphene show a distinct separation in behavior between metallic groups that strongly or weakly bond to it. The two basic classes of metal reactions with graphene are either physisorbed metals, which bond weakly with graphene, or chemisorbed metals, which bond strongly to graphene. For graphene diffusion barrier testing on Si substrates, an effective barrier can be achieved through the formation of a carbide layer with metals that are chemisorbed. For physisorbed metals, the barrier failure mechanism is loss of adhesion at the metal–graphene interface. A graphene layer encased between two metal layers, in certain cases, can increase the binding energy of both films with graphene, however, certain combinations of metal films are detrimental to the bonding with graphene. While the prospects for graphene's future as a solid-state diffusion barrier are positive, there are open questions, and areas for future research are discussed. A better understanding of the mechanisms which influence graphene's ability to be an effective diffusion barrier in microelectronic applications is required, and additional experiments are needed on a broader range of metals, as well as common metal stack contact structures used in microelectronic applications. The role of defects in the graphene is also a key area, since they will probably influence the barrier properties. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Multilayer graphene growth on polar dielectric substrates using chemical vapour deposition

NASA Astrophysics Data System (ADS)

Karamat, S.; Çelik, K.; Shah Zaman, S.; Oral, A.

2018-06-01

High quality of graphene is necessary for its applications at industrial scale production. The most convenient way is its direct growth on dielectrics which avoid the transfer route of graphene from metal to dielectric substrate usually followed by graphene community. The choice of a suitable dielectric for the gate material which can replace silicon dioxide (SiO2) is in high demand. Various properties like permittivity, thermodynamic stability, film morphology, interface quality, bandgap and band alignment of other dielectrics with graphene needs more exploration. A potential dielectric material is required which could be used to grow graphene with all these qualities. Direct growth of graphene on magnesium oxide (MgO) substrates is an interesting idea and will be a new addition in the library of 2D materials. The present work is about the direct growth of graphene on MgO substrates by an ambient pressure chemical vapour deposition (CVD) method. We address the surface instability issue of the polar oxides which is the most challenging factor in MgO. Atomic force microscopy (AFM) measurements showed the topographical features of the graphene coated on MgO. X-ray photoelectron spectroscopy (XPS) study is carried out to extract information regarding the presence of necessary elements, their bonding with substrates and to confirm the sp-2 hybridization of carbon, which is a characteristic feature of graphene film. The chemical shift is due to the surface reconstruction of MgO in the prepared samples. For graphene-MgO interface, valence band offset (VBO) and conduction band offset (CBO) extracted from valence band spectra reported. Further, we predicted the energy band diagram for single layer and thin film of graphene. By using the room-temperature energy band gap values of MgO and graphene, the CBO is calculated to be 6.85 eV for single layer and 5.66 eV for few layer (1-3) of graphene layers.

Continuous roll-to-roll growth of graphene films by chemical vapor deposition

NASA Astrophysics Data System (ADS)

Hesjedal, Thorsten

2011-03-01

Few-layer graphene is obtained in atmospheric chemical vapor deposition on polycrystalline copper in a roll-to-roll process. Raman and x-ray photoelectron spectroscopy were employed to confirm the few-layer nature of the graphene film, to map the inhomogeneities, and to study and optimize the growth process. This continuous growth process can be easily scaled up and enables the low-cost fabrication of graphene films for industrial applications.

Simultaneous measurement of electrical and thermal conductivities of suspended monolayer graphene

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Haidong; Kurata, Kosaku; Fukunaga, Takanobu

2016-06-28

We measured both in-plane electrical and thermal properties of the same suspended monolayer graphene using a novel T-type sensor method. At room temperature, the values are about 240 000 Ω{sup −1} m{sup −1} and 2100 W m{sup −1} K{sup −1} for the electrical and thermal conductivities, respectively. Based on the Wiedemann-Franz law, the electrons have negligible contribution to the thermal conductivity of graphene, while the in-plane LA and TA modes phonons are the dominant heat carriers. In monolayer graphene, the absence of layer-layer and layer-substrate interactions enhances the contribution of long wave-length phonons to the heat transport and increases the thermal conductivity accordingly. The reportedmore » method and experimental data of suspended monolayer graphene are useful for understanding the basic physics and designing the future graphene electronic devices.« less

Ab Initio Investigation of Frictional Properties of Graphene on SiC Surfaces

NASA Astrophysics Data System (ADS)

Sayin, Ceren; Gülseren, Oğuz

The exact origin and nature of various nanotribological observations on graphene such as dependence of friction on layer thickness, direction and surface morphology are yet to be fully understood. In this talk, we report on the frictional properties of graphene on 4H-SiC{0001} surfaces obtained from first principles calculations. We investigate sliding of graphene layers of various thickness along different directions on both the Si- and C-terminated faces including van-der Waals interactions. We observe that upon sliding under certain conditions, the interaction between the surface and graphene layers alternates between van-der Waals and covalent forces which dramatically affects friction. We examine the relation of frictional force to applied normal load, small out-of-plane geometric deformations of graphene and electronic structure of the systems. This work is supported by TUBITAK Project No:114F162.

Highly sensitive transient absorption imaging of graphene and graphene oxide in living cells and circulating blood

PubMed Central

Li, Junjie; Zhang, Weixia; Chung, Ting-Fung; Slipchenko, Mikhail N.; Chen, Yong P.; Cheng, Ji-Xin; Yang, Chen

2015-01-01

We report a transient absorption (TA) imaging method for fast visualization and quantitative layer analysis of graphene and GO. Forward and backward imaging of graphene on various substrates under ambient condition was imaged with a speed of 2 μs per pixel. The TA intensity linearly increased with the layer number of graphene. Real-time TA imaging of GO in vitro with capability of quantitative analysis of intracellular concentration and ex vivo in circulating blood were demonstrated. These results suggest that TA microscopy is a valid tool for the study of graphene based materials. PMID:26202216

Separating nano graphene oxide from the residual strong-acid filtrate of the modified Hummers method with alkaline solution

NASA Astrophysics Data System (ADS)

Hu, Xuebing; Yu, Yun; Wang, Yongqing; Zhou, Jianer; Song, Lixin

2015-02-01

In the modified Hummers method for preparing graphene oxide, the yellow slurry can be obtained. After filtering through a quantitative filter paper, the strong-acid filtrate containing the unprecipitated nano graphene oxide was gained. The corresponding filtrate was added gradually with an alkaline (NaOH or KOH) solution at room temperature. The unprecipitated nano graphene oxide could undergo fast aggregation when the pH value of the filtrate was about 1.7 and formed the stable floccules. X-ray diffraction analysis shows the dominant peak of the floccules is about 11°, which accords to the peak of graphene oxide. Spectra of X-ray photoelectron spectroscopy confirm the presence in the floccules of an abundance of oxygen functional groups and the purified graphene oxide floccules can be obtained. Atomic force microscopy measurement shows the graphene oxide floccules consists of sheet-like objects, mostly containing only a few layers (about 5 layers). Zeta potential analysis demonstrates the surface charge of the graphene oxide is pH-sensitive and its isoelectric point is ∼1.7. The flocculation mechanism of graphene oxide ascribes to the acid-base interaction with the surface functional groups of the carbon layers.

Determination of a refractive index and an extinction coefficient of standard production of CVD-graphene.

PubMed

Ochoa-Martínez, Efraín; Gabás, Mercedes; Barrutia, Laura; Pesquera, Amaia; Centeno, Alba; Palanco, Santiago; Zurutuza, Amaia; Algora, Carlos

2015-01-28

The refractive index and extinction coefficient of chemical vapour deposition grown graphene are determined by ellipsometry analysis. Graphene films were grown on copper substrates and transferred as both monolayers and bilayers onto SiO2/Si substrates by using standard manufacturing procedures. The chemical nature and thickness of residual debris formed after the transfer process were elucidated using photoelectron spectroscopy. The real layered structure so deduced has been used instead of the nominal one as the input in the ellipsometry analysis of monolayer and bilayer graphene, transferred onto both native and thermal silicon oxide. The effect of these contamination layers on the optical properties of the stacked structure is noticeable both in the visible and the ultraviolet spectral regions, thus masking the graphene optical response. Finally, the use of heat treatment under a nitrogen atmosphere of the graphene-based stacked structures, as a method to reduce the water content of the sample, and its effect on the optical response of both graphene and the residual debris layer are presented. The Lorentz-Drude model proposed for the optical response of graphene fits fairly well the experimental ellipsometric data for all the analysed graphene-based stacked structures.

Large area graphene ion sensitive field effect transistors with tantalum pentoxide sensing layers for pH measurement at the Nernstian limit

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fakih, Ibrahim, E-mail: ibrahim.fakih@mail.mcgill.ca; Sabri, Shadi; Szkopek, Thomas, E-mail: thomas.szkopek@mcgill.ca

2014-08-25

We have fabricated and characterized large area graphene ion sensitive field effect transistors (ISFETs) with tantalum pentoxide sensing layers and demonstrated pH sensitivities approaching the Nernstian limit. Low temperature atomic layer deposition was used to deposit tantalum pentoxide atop large area graphene ISFETs. The charge neutrality point of graphene, inferred from quantum capacitance or channel conductance, was used to monitor surface potential in the presence of an electrolyte with varying pH. Bare graphene ISFETs exhibit negligible response, while graphene ISFETs with tantalum pentoxide sensing layers show increased sensitivity reaching up to 55 mV/pH over pH 3 through pH 8. Applying themore » Bergveld model, which accounts for site binding and a Guoy-Chapman-Stern picture of the surface-electrolyte interface, the increased pH sensitivity can be attributed to an increased buffer capacity reaching up to 10{sup 14} sites/cm{sup 2}. ISFET response was found to be stable to better than 0.05 pH units over the course of two weeks.« less

Large area graphene ion sensitive field effect transistors with tantalum pentoxide sensing layers for pH measurement at the Nernstian limit

NASA Astrophysics Data System (ADS)

Fakih, Ibrahim; Sabri, Shadi; Mahvash, Farzaneh; Nannini, Matthieu; Siaj, Mohamed; Szkopek, Thomas

2014-08-01

We have fabricated and characterized large area graphene ion sensitive field effect transistors (ISFETs) with tantalum pentoxide sensing layers and demonstrated pH sensitivities approaching the Nernstian limit. Low temperature atomic layer deposition was used to deposit tantalum pentoxide atop large area graphene ISFETs. The charge neutrality point of graphene, inferred from quantum capacitance or channel conductance, was used to monitor surface potential in the presence of an electrolyte with varying pH. Bare graphene ISFETs exhibit negligible response, while graphene ISFETs with tantalum pentoxide sensing layers show increased sensitivity reaching up to 55 mV/pH over pH 3 through pH 8. Applying the Bergveld model, which accounts for site binding and a Guoy-Chapman-Stern picture of the surface-electrolyte interface, the increased pH sensitivity can be attributed to an increased buffer capacity reaching up to 1014 sites/cm2. ISFET response was found to be stable to better than 0.05 pH units over the course of two weeks.

Free-standing epitaxial graphene on silicon carbide and transport barriers in layered materials

NASA Astrophysics Data System (ADS)

Shivaraman, Shriram

This thesis is based on the topic of layered materials, in which different layers interact with each other via van der Waals forces. The majority of this thesis deals with epitaxial graphene (EG) obtained from silicon carbide (SiC). Free-standing epitaxial graphene (FSEG) structures are produced from EG using a photoelectrochemical (PEC) etching process developed for making suspended graphene structures on a large-scale. These structures are investigated for their mechanical and electrical properties. For doubly-clamped FSEG structures, a unique U-beam effect is observed which causes orders of magnitude increase in their mechanical resonance frequency compared to that expected using simple beam theory. Combined magnetotransport and Raman spectroscopy studies reveal that FSEG devices produced from nominally monolayer graphene on the Si-face of SiC exhibit properties of an inhomogeneously doped bilayer after becoming suspended. This suggests that the buffer layer which precedes graphene growth on the Si-face of SiC gets converted to a graphene layer after the PEC etching process. In the second theme of this thesis, transport barriers in layered materials are investigated. The EG-SiC interface is studied using a combination of electrical (I-V, C-V) and photocurrent spectroscopy techniques. It is shown that the interface may be described as having a Schottky barrier for electron transport with a Gaussian distribution of barrier heights. Another interface explored in this work is that between different layers of MoS 2, a layered material belonging to the class of transition metal dichalcogenides. This interface maybe thought of as a one-dimensional junction. Four-point transport measurements indicate the presence of a barrier for electron transport at this interface. A simple model of the junction as a region with an increased threshold voltage and degraded mobility is suggested. The final chapter is a collection of works based on the topic of layered materials, which are not related to the main theme of the thesis. They include fabrication and characterization details of a dual-gated bilayer graphene device, an investigation of the graphene-Si interface and hexagonal boron nitride-based membranes. These are presented in the hope that they may be useful for further investigations along those directions.

Enhanced Capacitance of Hybrid Layered Graphene/Nickel Nanocomposite for Supercapacitors

NASA Astrophysics Data System (ADS)

Mohd Zaid, Norsaadatul Akmal; Idris, Nurul Hayati

2016-08-01

In this work, Ni nanoparticles were directly decorated on graphene (G) nanosheets via mechanical ball milling. Based on transmission electron microscopy observations, the Ni nanoparticles were well dispersed and attached to the G nanosheet without any agglomerations. Electrochemical results showed that the capacitance of a G/Ni nanocomposite was 275 F g-1 at a current density of 2 A g-1, which is higher than the capacitance of bare G (145 F g-1) and bare Ni (3 F g-1). The G/Ni electrode also showed superior performance at a high current density, exhibiting a capacitance of 190 F g-1 at a current density of 5 A g-1 and a capacitance of 144 F g-1 at a current density of 10 A g-1. The equivalent series resistance for G/Ni nanocomposites also decreased. The enhanced performance of this hybrid supercapacitor is best described by the synergistic effect, i.e. dual charge-storage mechanism, which is demonstrated by electrical double layer and pseudocapacitance materials. Moreover, a high specific surface area and electrical conductivity of the materials enhanced the capacitance. These results indicate that the G/Ni nanocomposite is a potential supercapacitor.

Enhanced Capacitance of Hybrid Layered Graphene/Nickel Nanocomposite for Supercapacitors.

PubMed

Mohd Zaid, Norsaadatul Akmal; Idris, Nurul Hayati

2016-08-24

In this work, Ni nanoparticles were directly decorated on graphene (G) nanosheets via mechanical ball milling. Based on transmission electron microscopy observations, the Ni nanoparticles were well dispersed and attached to the G nanosheet without any agglomerations. Electrochemical results showed that the capacitance of a G/Ni nanocomposite was 275 F g(-1) at a current density of 2 A g(-1), which is higher than the capacitance of bare G (145 F g(-1)) and bare Ni (3 F g(-1)). The G/Ni electrode also showed superior performance at a high current density, exhibiting a capacitance of 190 F g(-1) at a current density of 5 A g(-1) and a capacitance of 144 F g(-1) at a current density of 10 A g(-1). The equivalent series resistance for G/Ni nanocomposites also decreased. The enhanced performance of this hybrid supercapacitor is best described by the synergistic effect, i.e. dual charge-storage mechanism, which is demonstrated by electrical double layer and pseudocapacitance materials. Moreover, a high specific surface area and electrical conductivity of the materials enhanced the capacitance. These results indicate that the G/Ni nanocomposite is a potential supercapacitor.

Phonon self-energy corrections to non-zero wavevector phonon modes in single-layer graphene

NASA Astrophysics Data System (ADS)

Araujo, Paulo; Mafra, Daniela; Sato, Kentaro; Saito, Richiiro; Kong, Jing; Dresselhaus, Mildred

2012-02-01

Phonon self-energy corrections have mostly been studied theoretically and experimentally for phonon modes with zone-center (q = 0) wave-vectors. Here, gate-modulated Raman scattering is used to study phonons of a single layer of graphene (1LG) in the frequency range from 2350 to 2750 cm-1, which shows the G* and the G'-band features originating from a double-resonant Raman process with q 0. The observed phonon renormalization effects are different from what is observed for the zone-center q = 0 case. To explain our experimental findings, we explored the phonon self-energy for the phonons with non-zero wave-vectors (q 0) in 1LG in which the frequencies and decay widths are expected to behave oppositely to the behavior observed in the corresponding zone-center q = 0 processes. Within this framework, we resolve the identification of the phonon modes contributing to the G* Raman feature at 2450 cm-1 to include the iTO+LA combination modes with q 0 and the 2iTO overtone modes with q = 0, showing both to be associated with wave-vectors near the high symmetry point K in the Brillouin zone.

Modification of thermal and electronic properties of bilayer graphene by using slow Na+ ions

NASA Astrophysics Data System (ADS)

Ryu, Mintae; Lee, Paengro; Kim, Jingul; Park, Heemin; Chung, Jinwook

2016-12-01

Bilayer graphene (BLG) has an extensive list of industrial applications in graphene-based nanodevices such as energy storage devices, flexible displays, and thermoelectric devices. By doping slow Na+ ions on Li-intercalated BLG, we find significantly improved thermal and electronic properties of BLG by using angle-resolved photoemission and high-resolution core level spectroscopy (HRCLS) with synchrotron photons. Our HRCLS data reveal that the adsorbed Na+ ions on a BLG produced by Li-intercalation through single layer graphene (SLG) spontaneously intercalate below the BLG, and substitute Li atoms to form Na-Si bonds at the SiC interface while preserving the same phase of BLG. This is in sharp contrast with no intercalation of Na+ ions on SLG though neutral Na atoms intercalate. The Na+-induced BLG is found to be stable upon heating up to T = 400 °C, but returns to SLG when heated at T d = 500 °C. The evolution of the π-bands upon doping the Na+ ions followed by thermal annealing shows that the carrier concentration of the π-band may be artificially controlled without damaging the Dirac nature of the π-electrons. The doubled desorption temperature from that (T d = 250 °C) of the Na-intercalated SLG together with the electronic stability of the Na+-intercalated BLG may find more practical and effective applications in advancing graphene-based thermoelectric devices and anode materials for rechargeable batteries.

Homoepitaxial graphene tunnel barriers for spin transport (Presentation Recording)

NASA Astrophysics Data System (ADS)

Friedman, Adam L.

2015-09-01

Tunnel barriers are key elements for both charge-and spin-based electronics, offering devices with reduced power consumption and new paradigms for information processing. Such devices require mating dissimilar materials, raising issues of heteroepitaxy, interface stability, and electronic states that severely complicate fabrication and compromise performance. Graphene is the perfect tunnel barrier. It is an insulator out-of-plane, possesses a defect-free, linear habit, and is impervious to interdiffusion. Nonetheless, true tunneling between two stacked graphene layers is not possible in environmental conditions (magnetic field, temperature, etc.) usable for electronics applications. However, two stacked graphene layers can be decoupled using chemical functionalization. Here, we demonstrate homoepitaxial tunnel barrier devices in which graphene serves as both the tunnel barrier and the high mobility transport channel. Beginning with multilayer graphene, we fluorinate or hydrogenate the top layer to decouple it from the bottom layer, so that it serves as a single monolayer tunnel barrier for both charge and spin injection into the lower graphene transport channel. We demonstrate successful tunneling by measuring non-linear IV curves, and a weakly temperature dependent zero bias resistance. We perform lateral transport of spin currents in non-local spin-valve structures and determine spin lifetimes with the non-local Hanle effect to be commensurate with previous studies (~200 ps). However, we also demonstrate the highest spin polarization efficiencies (~45%) yet measured in graphene-based spin devices [1]. [1] A.L. Friedman, et al., Homoepitaxial tunnel barriers with functionalized graphene-on-graphene for charge and spin transport, Nat. Comm. 5, 3161 (2014).

Graphene as discharge layer for electron beam lithography on insulating substrate

NASA Astrophysics Data System (ADS)

Liu, Junku; Li, Qunqing; Ren, Mengxin; Zhang, Lihui; Chen, Mo; Fan, Shoushan

2013-09-01

Charging of insulating substrates is a common problem during Electron Beam lithography (EBL), which deflects the beam and distorts the pattern. A homogeneous, electrically conductive, and transparent graphene layer is used as a discharge layer for EBL processes on insulating substrates. The EBL resolution is improved compared with the metal discharge layer. Dense arrays of holes with diameters of 50 nm and gratings with line/space of 50/30 nm are obtained on quartz substrate. The pattern placement errors and proximity effect are suppressed over a large area and high quality complex nanostructures are fabricated using graphene as a conductive layer.

Spin-injection into epitaxial graphene on silicon carbide

NASA Astrophysics Data System (ADS)

Konishi, Keita; Cui, Zhixin; Hiraki, Takahiro; Yoh, Kanji

2013-09-01

We have studied the spin-injection properties in epitaxial graphene on SiC. The ferromagnetic metal (FM) electrodes were composed of a tunnel barrier layer AlOx (14 Å) and a ferromagnetic Co (600 Å) layer. We have successfully observed the clear resistance peaks indicating spin-injection both in the "local" and "non-local" spin measurement set-ups at low temperatures. We estimate spin-injection rate of 1% based on "non-local" measurement and 1.6% based on local measurements. Spin-injection rate of multilayer graphene by mechanical exfoliation method was twice as high as single layer graphene on SiC based on "local" measurement.

Nonreciprocal optical isolation via graphene based photonic crystals

NASA Astrophysics Data System (ADS)

Roshan Entezar, S.; Karimi Habil, M.

2018-03-01

The transmission properties of a one-dimensional photonic crystal containing graphene mono-layers are studied using the transfer matrix method. It is shown that the structure can be used as a polarization-selective nonreciprocal device which discriminates between the two circularly polarized waves with different handedness impinging in the same direction. This structure may be utilized in designing optical isolators for the circularly polarized waves due to the gyrotropic behavior of the graphene mono-layers under the perpendicularly applied external magnetic field. Moreover, the effect of an external magnetic field and the chemical potential of the graphene mono-layers on the band gap of the structure are investigated.

Calculation of electron spectra and some problems in the thermodynamics of graphene layers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Alisultanov, Z. Z., E-mail: zaur0102@gmail.com

The expressions for the energy spectra of monolayer, bilayer, and multilayer graphene, as well as epitaxial graphene, are derived using the quantum Green’s functions method. Analytic expressions are obtained for the densities of states of these systems. It is shown that a bandgap can appear the spectrum of an epitaxial graphene bilayer. A number of problems in the thermodynamics of electrons in free and epitaxial graphene layers are considered as applications. Analytic expressions are obtained for the chemical potential and heat capacity in the limiting cases of low and high temperatures. Quantum oscillations of heat capacity in graphene are analyzedmore » taking into account the Coulomb interaction. The Berry phase of epitaxial graphene is investigated.« less

Rebar Graphene from Functionalized Boron Nitride Nanotubes

PubMed Central

2015-01-01

The synthesis of rebar graphene on Cu substrates is described using functionalized boron nitride nanotubes (BNNTs) that were annealed or subjected to chemical vapor deposition (CVD) growth of graphene. Characterization shows that the BNNTs partially unzip and form a reinforcing bar (rebar) network within the graphene layer that enhances the mechanical strength through covalent bonds. The rebar graphene is transferrable to other substrates without polymer assistance. The optical transmittance and conductivity of the hybrid rebar graphene film was tested, and a field effect transistor was fabricated to explore its electrical properties. This method of synthesizing 2D hybrid graphene/BN structures should enable the hybridization of various 1D nanotube and 2D layered structures with enhanced mechanical properties. PMID:25486451

FAST TRACK COMMUNICATION: Electronic structure of a graphene/hexagonal-BN heterostructure grown on Ru(0001) by chemical vapor deposition and atomic layer deposition: extrinsically doped graphene

NASA Astrophysics Data System (ADS)

Bjelkevig, Cameron; Mi, Zhou; Xiao, Jie; Dowben, P. A.; Wang, Lu; Mei, Wai-Ning; Kelber, Jeffry A.

2010-08-01

A significant BN-to-graphene charge donation is evident in the electronic structure of a graphene/h-BN(0001) heterojunction grown by chemical vapor deposition and atomic layer deposition directly on Ru(0001), consistent with density functional theory. This filling of the lowest unoccupied state near the Brillouin zone center has been characterized by combined photoemission/k vector resolved inverse photoemission spectroscopies, and Raman and scanning tunneling microscopy/spectroscopy. The unoccupied σ*(Γ1 +) band dispersion yields an effective mass of 0.05 me for graphene in the graphene/h-BN(0001) heterostructure, in spite of strong perturbations to the graphene conduction band edge placement.

Electronic transport properties of graphene doped by gallium.

PubMed

Mach, J; Procházka, P; Bartošík, M; Nezval, D; Piastek, J; Hulva, J; Švarc, V; Konečný, M; Kormoš, L; Šikola, T

2017-10-13

In this work we present the effect of low dose gallium (Ga) deposition (<4 ML) performed in UHV (10 -7 Pa) on the electronic doping and charge carrier scattering in graphene grown by chemical vapor deposition. In situ graphene transport measurements performed with a graphene field-effect transistor structure show that at low Ga coverages a graphene layer tends to be strongly n-doped with an efficiency of 0.64 electrons per one Ga atom, while the further deposition and Ga cluster formation results in removing electrons from graphene (less n-doping). The experimental results are supported by the density functional theory calculations and explained as a consequence of distinct interaction between graphene and Ga atoms in case of individual atoms, layers, or clusters.

Electronic transport properties of graphene doped by gallium

NASA Astrophysics Data System (ADS)

Mach, J.; Procházka, P.; Bartošík, M.; Nezval, D.; Piastek, J.; Hulva, J.; Švarc, V.; Konečný, M.; Kormoš, L.; Šikola, T.

2017-10-01

In this work we present the effect of low dose gallium (Ga) deposition (<4 ML) performed in UHV (10-7 Pa) on the electronic doping and charge carrier scattering in graphene grown by chemical vapor deposition. In situ graphene transport measurements performed with a graphene field-effect transistor structure show that at low Ga coverages a graphene layer tends to be strongly n-doped with an efficiency of 0.64 electrons per one Ga atom, while the further deposition and Ga cluster formation results in removing electrons from graphene (less n-doping). The experimental results are supported by the density functional theory calculations and explained as a consequence of distinct interaction between graphene and Ga atoms in case of individual atoms, layers, or clusters.

Interactions of Organic Solvents at Graphene/α-Al 2 O 3 and Graphene Oxide/α-Al 2 O 3 Interfaces Studied by Sum Frequency Generation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Achtyl, Jennifer L.; Vlassiouk, Ivan V.; Dai, Sheng

2014-07-17

The adsorption of 1-hexanol from cyclohexane-d12 at single-layer graphene/α-Al2O3 interfaces was probed at mole percent values as low as 0.05 in the C–H stretching region using vibrational sum frequency generation (SFG). The SFG spectra are indiscernible from those obtained in the absence of graphene, and from those obtained in the presence of graphene oxide films prepared via oxygen plasma treatment of pristine single-layer graphene. A Langmuir adsorption model yields observed free adsorption energies of -19.9(5) to -20.9(3) kJ/mol for the three interfaces. The results indicate that the molecular structure of the hexanol alkyl chain is subject to the same orientationmore » distribution when graphene, oxidized or not, is present or absent at the α-Al2O3/cyclohexane-d12 interface. Moreover, it appears that the adsorption of 1-hexanol in this binary mixture is driven by hexanol interactions with the underlying oxide support, and that a single layer of graphene does not influence the extent of this interaction, even when defects are introduced to it. Finally, our structural and quantitative thermodynamic data provide important benchmarks for theoretical calculations and atomistic simulations of liquid/graphene interfaces. We hypothesize that defects emerging in graphene during operation of any device application that relies on layered solvent/graphene/oxide interfaces have little impact on the interfacial structure or thermodynamics, at least for the binary mixture and over the range of defect densities probed in our studies.« less

Passively mode-locked fiber laser based on a hollow-core photonic crystal fiber filled with few-layered graphene oxide solution.

PubMed

Liu, Zhi-Bo; He, Xiaoying; Wang, D N

2011-08-15

We demonstrate a nanosecond-pulse erbium-doped fiber laser that is passively mode locked by a hollow-core photonic crystal fiber filled with few-layered graphene oxide solution. Owing to the good solution processing capability of few-layered graphene oxide, which can be filled into the core of a hollow-core photonic crystal fiber through a selective hole filling process, a graphene saturable absorber can be successfully fabricated. The output pulses obtained have a center wavelength, pulse width, and repetition rate of 1561.2 nm, 4.85 ns, and 7.68 MHz, respectively. This method provides a simple and efficient approach to integrate the graphene into the optical fiber system. © 2011 Optical Society of America

Water Desalination Using Nanoporous Single-Layer Graphene with Tunable Pore Size

DOE PAGES

Surwade, Sumedh P.; Smirnov, Sergei N.; Vlassiouk, Ivan V.; ...

2015-03-23

Graphene has great potential to serve as a separation membrane due to its unique properties such as chemical and mechanical stability, flexibility and most importantly its one-atom thickness. In this study, we demonstrate first experimental evidence of the use of single-layer porous graphene as a desalination membrane. Nanometer-sized pores are introduced into single layer graphene using a convenient oxygen plasma etching process that permits tuning of the pore size. The resulting porous graphene membrane exhibited high rejection of salt ions and rapid water transport, thus functioning as an efficient water desalination membrane. Salt rejection selectivity of nearly 100% and exceptionallymore » high water fluxes exceeding 105 g m-2 s-1 at 40 C were measured using saturated water vapor as a driving force.« less

Effect of surface morphology on friction of graphene on various substrates

NASA Astrophysics Data System (ADS)

Cho, Dae-Hyun; Wang, Lei; Kim, Jin-Seon; Lee, Gwan-Hyoung; Kim, Eok Su; Lee, Sunhee; Lee, Sang Yoon; Hone, James; Lee, Changgu

2013-03-01

The friction of graphene on various substrates, such as SiO2, h-BN, bulk-like graphene, and mica, was investigated to characterize the adhesion level between graphene and the underlying surface. The friction of graphene on SiO2 decreased with increasing thickness and converged around the penta-layers due to incomplete contact between the two surfaces. However, the friction of graphene on an atomically flat substrate, such as h-BN or bulk-like graphene, was low and comparable to that of bulk-like graphene. In contrast, the friction of graphene folded onto bulk-like graphene was indistinguishable from that of mono-layer graphene on SiO2 despite the ultra-smoothness of bulk-like graphene. The characterization of the graphene's roughness before and after folding showed that the corrugation of graphene induced by SiO2 morphology was preserved even after it was folded onto an atomically flat substrate. In addition, graphene deposited on mica, when folded, preserved the same corrugation level as before the folding event. Our friction measurements revealed that graphene, once exfoliated from the bulk crystal, tends to maintain its corrugation level even after it is folded onto an atomically flat substrate and that ultra-flatness in both graphene and the substrate is required to achieve the intimate contact necessary for strong adhesion.The friction of graphene on various substrates, such as SiO2, h-BN, bulk-like graphene, and mica, was investigated to characterize the adhesion level between graphene and the underlying surface. The friction of graphene on SiO2 decreased with increasing thickness and converged around the penta-layers due to incomplete contact between the two surfaces. However, the friction of graphene on an atomically flat substrate, such as h-BN or bulk-like graphene, was low and comparable to that of bulk-like graphene. In contrast, the friction of graphene folded onto bulk-like graphene was indistinguishable from that of mono-layer graphene on SiO2 despite the ultra-smoothness of bulk-like graphene. The characterization of the graphene's roughness before and after folding showed that the corrugation of graphene induced by SiO2 morphology was preserved even after it was folded onto an atomically flat substrate. In addition, graphene deposited on mica, when folded, preserved the same corrugation level as before the folding event. Our friction measurements revealed that graphene, once exfoliated from the bulk crystal, tends to maintain its corrugation level even after it is folded onto an atomically flat substrate and that ultra-flatness in both graphene and the substrate is required to achieve the intimate contact necessary for strong adhesion. Electronic supplementary information (ESI) available: Sample preparation method, identification of graphene thickness, AFM and FFM measurements. See DOI: 10.1039/c3nr34181j

RNA nanopatterning on graphene

NASA Astrophysics Data System (ADS)

Li, Q.; Froning, J. P.; Pykal, M.; Zhang, S.; Wang, Z.; Vondrák, M.; Banáš, P.; Čépe, K.; Jurečka, P.; Šponer, J.; Zbořil, R.; Dong, M.; Otyepka, M.

2018-07-01

Graphene-based materials enable the sensing of diverse biomolecules using experimental approaches based on electrochemistry, spectroscopy, or other methods. Although basic sensing was achieved, it had until now not been possible to understand and control biomolecules’ structural and morphological organization on graphene surfaces (i.e. their stacking, folding/unfolding, self-assembly, and nano-patterning). Here we present the insight into structural and morphological organization of biomolecules on graphene in water, using an RNA hairpin as a model system. We show that the key parameters governing the RNA’s behavior on the graphene surface are the number of graphene layers, RNA concentration, and temperature. At high concentrations, the RNA forms a film on the graphene surface with entrapped nanobubbles. The density and the size of the bubbles depend on the number of graphene layers. At lower concentrations, unfolded RNA stacks on the graphene and forms molecular clusters on the surface. Such a control over the conformational behavior of interacting biomolecules at graphene/water interfaces would facilitate new applications of graphene derivatives in biotechnology and biomedicine.

Localized in situ polymerization on graphene surfaces for stabilized graphene dispersions.

PubMed

Das, Sriya; Wajid, Ahmed S; Shelburne, John L; Liao, Yen-Chih; Green, Micah J

2011-06-01

We demonstrate a novel in situ polymerization technique to develop localized polymer coatings on the surface of dispersed pristine graphene sheets. Graphene sheets show great promise as strong, conductive fillers in polymer nanocomposites; however, difficulties in dispersion quality and interfacial strength between filler and matrix have been a persistent problem for graphene-based nanocomposites, particularly for pristine graphene. With this in mind, a physisorbed polymer layer is used to stabilize graphene sheets in solution. To create this protective layer, we formed an organic microenvironment around dispersed graphene sheets in surfactant solutions, and created a nylon 6, 10 or nylon 6, 6 coating via interfacial polymerization. Technique lies at the intersection of emulsion and admicellar polymerization; a similar technique was originally developed to protect luminescent properties of carbon nanotubes in solution. These coated graphene dispersions are aggregation-resistant and may be reversibly redispersed in water even after freeze-drying. The coated graphene holds promise for a number of applications, including multifunctional graphene-polymer nanocomposites. © 2011 American Chemical Society

Carbon Papers and Aerogels Based on Graphene Layers and Chitosan: Direct Preparation from High Surface Area Graphite.

PubMed

Barbera, Vincenzina; Guerra, Silvia; Brambilla, Luigi; Maggio, Mario; Serafini, Andrea; Conzatti, Lucia; Vitale, Alessandra; Galimberti, Maurizio

2017-12-11

In this work, carbon papers and aerogels based on graphene layers and chitosan were prepared. They were obtained by mixing chitosan (CS) and a high surface area nanosized graphite (HSAG) in water in the presence of acetic acid. HSAG/CS water dispersions were stable for months. High resolution transmission electron microscopy revealed the presence of few graphene layers in water suspensions. Casting or lyophilization of such suspensions led to the preparation of carbon paper and aerogel, respectively. In X-ray spectra of both aerogels and carbon paper, peaks due to regular stacks of graphene layers were not detected: graphene with unaltered sp 2 structure was obtained directly from graphite without the use of any chemical reaction. The composites were demonstrated to be electrically conductive thanks to the graphene. Chitosan thus makes it possible to obtain monolithic carbon aerogels and flexible and free-standing graphene papers directly from a nanosized graphite by avoiding oxidation to graphite oxide and successive reduction. Strong interaction between polycationic chitosan and the aromatic substrate appears to be at the origin of the stability of HSAG/CS adducts. Cation-π interaction is hypothesized, also on the basis of X-ray photoelectron spectroscopy findings. This work paves the way for the easy large-scale preparation of carbon papers through a method that has a low environmental impact and is based on a biosourced polymer, graphene, and water.

Effect of water layer at the SiO2/graphene interface on pentacene morphology.

PubMed

Chhikara, Manisha; Pavlica, Egon; Matković, Aleksandar; Gajić, Radoš; Bratina, Gvido

2014-10-07

Atomic force microscopy has been used to examine early stages of pentacene growth on exfoliated single-layer graphene transferred to SiO2 substrates. We have observed 2D growth with mean height of 1.5 ± 0.2 nm on as-transferred graphene. Three-dimensional islands of pentacene with an average height of 11 ± 2 nm were observed on graphene that was annealed at 350 °C prior to pentacene growth. Compellingly similar 3D morphology has been observed on graphene transferred onto SiO2 that was treated with hexamethyldisilazane prior to the transfer of graphene. On multilayer graphene we have observed 2D growth, regardless of the treatment of SiO2. We interpret this behavior of pentacene molecules in terms of the influence of the dipolar field that emerges from the water monolayer at the graphene/SiO2 interface on the surface energy of graphene.

Controlled assembly of graphene-capped nickel, cobalt and iron silicides

PubMed Central

Vilkov, O.; Fedorov, A.; Usachov, D.; Yashina, L. V.; Generalov, A. V.; Borygina, K.; Verbitskiy, N. I.; Grüneis, A.; Vyalikh, D. V.

2013-01-01

The unique properties of graphene have raised high expectations regarding its application in carbon-based nanoscale devices that could complement or replace traditional silicon technology. This gave rise to the vast amount of researches on how to fabricate high-quality graphene and graphene nanocomposites that is currently going on. Here we show that graphene can be successfully integrated with the established metal-silicide technology. Starting from thin monocrystalline films of nickel, cobalt and iron, we were able to form metal silicides of high quality with a variety of stoichiometries under a Chemical Vapor Deposition grown graphene layer. These graphene-capped silicides are reliably protected against oxidation and can cover a wide range of electronic materials/device applications. Most importantly, the coupling between the graphene layer and the silicides is rather weak and the properties of quasi-freestanding graphene are widely preserved. PMID:23835625

Graphene: powder, flakes, ribbons, and sheets.

PubMed

James, Dustin K; Tour, James M

2013-10-15

Graphene's unique physical and electrical properties (high tensile strength, Young's modulus, electron mobility, and thermal conductivity) have led to its nickname of "super carbon." Graphene research involves the study of several different physical forms of the material: powders, flakes, ribbons, and sheets and others not yet named or imagined. Within those forms, graphene can include a single layer, two layers, or ≤10 sheets of sp² carbon atoms. The chemistry and applications available with graphene depend on both the physical form of the graphene and the number of layers in the material. Therefore the available permutations of graphene are numerous, and we will discuss a subset of this work, covering some of our research on the synthesis and use of many of the different physical and layered forms of graphene. Initially, we worked with commercially available graphite, with which we extended diazonium chemistry developed to functionalize single-walled carbon nanotubes to produce graphitic materials. These structures were soluble in common organic solvents and were better dispersed in composites. We developed an improved synthesis of graphene oxide (GO) and explored how the workup protocol for the synthesis of GO can change the electronic structure and chemical functionality of the GO product. We also developed a method to remove graphene layers one-by-one from flakes. These powders and sheets of GO can serve as fluid loss prevention additives in drilling fluids for the oil industry. Graphene nanoribbons (GNRs) combine small width with long length, producing valuable electronic and physical properties. We developed two complementary syntheses of GNRs from multiwalled carbon nanotubes: one simple oxidative method that produces GNRs with some defects and one reductive method that produces GNRs that are less defective and more electrically conductive. These GNRs can be used in low-loss, high permittivity composites, as conductive reinforcement coatings on Kevlar fibers and in the fabrication of large area transparent electrodes. Using solid carbon sources such as polymers, food, insects, and waste, we can grow monolayer and bilayer graphene directly on metal catalysts, and carbon-sources containing nitrogen can produce nitrogen-doped graphene. The resulting graphene can be transferred to other surfaces, such as metal grids, for potential use in transparent touch screens for applications in personal electronics and large area photovoltaic devices. Because the transfer of graphene from one surface to another can lead to defects, low yields, and higher costs, we have developed methods for growing graphene directly on the substrates of interest. We can also produce patterned graphene to make GNRs or graphane/graphene superlattices within a single sheet. These superlattices could have multiple functions for use in sensors and other devices. This Account only touches upon this burgeoning area of materials chemistry, and the field will continue to expand as researchers imagine new forms and applications of graphene.

Modification of the electronic properties of hexagonal boron-nitride in BN/graphene vertical heterostructures

DOE PAGES

Pan, Minghu; Liang, Liangbo; Lin, Wenzhi; ...

2016-09-28

Van der Waals (vdW) heterostructures consist of isolated atomic planar structures, assembled layer- by-layer into desired structures in a well-defined sequence. Graphene deposited on hexagonal boron nitride (h-BN) has been first considered as a testbed system for vdW heterostructures, and many others have been demonstrated both theoretically and experimentally, revealing many attractive properties and phenomena. However, much less emphasis has been placed on how graphene actively affects h-BN properties. Here, we perform local probe measurements on single-layer h-BN grown over graphene and highlight the manifestation of a proximity effect that significantly affects the electronic properties of h-BN due to itsmore » coupling with the underlying graphene. We find electronic states originating from the graphene layer and the Cu substrate to be injected into the wide electronic gap of the h-BN top layer. Such proximity effect is further confirmed in a study of the variation of h-BN in-gap states with interlayer couplings, elucidated using a combination of topographical/ spectroscopic measurements and first-principles density functional theory calculations. In conclusion, the findings of this work indicate the potential of mutually engineering electronic properties of the components of vdW heterostructures.« less

Graphene-copper composite with micro-layered grains and ultrahigh strength

PubMed Central

Wang, Lidong; Yang, Ziyue; Cui, Ye; Wei, Bing; Xu, Shichong; Sheng, Jie; Wang, Miao; Zhu, Yunpeng; Fei, Weidong

2017-01-01

Graphene with ultrahigh intrinsic strength and excellent thermal physical properties has the potential to be used as the reinforcement of many kinds of composites. Here, we show that very high tensile strength can be obtained in the copper matrix composite reinforced by reduced graphene oxide (RGO) when micro-layered structure is achieved. RGO-Cu powder with micro-layered structure is fabricated from the reduction of the micro-layered graphene oxide (GO) and Cu(OH)2 composite sheets, and RGO-Cu composites are sintered by spark plasma sintering process. The tensile strength of the 5 vol.% RGO-Cu composite is as high as 608 MPa, which is more than three times higher than that of the Cu matrix. The apparent strengthening efficiency of RGO in the 2.5 vol.% RGO-Cu composite is as high as 110, even higher than that of carbon nanotube, multilayer graphene, carbon nano fiber and RGO in the copper matrix composites produced by conventional MLM method. The excellent tensile and compressive strengths, high hardness and good electrical conductivity are obtained simultaneously in the RGO-Cu composites. The results shown in the present study provide an effective method to design graphene based composites with layered structure and high performance. PMID:28169306