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Sorption of 4He, H2, Ne, N2, CH4 and Kr impurities in graphene oxide at low temperatures. Quantum effects

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 Added by Alexander Dolbin V.
 Publication date 2013
  fields Physics
and research's language is English
 Authors A.V. Dolbin




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Sorption and the subsequent desorption of 4He, H2,Ne, N2, CH4 and Kr gas impurities by graphene oxide (GO), glucose-reduced GO (RGO-Gl) and hydrazine-reduced GO (RGO-Hz) powders have been investigated in the temperature interval 2-290 K. It has been found that the sorptive capacity of the reduced sample RGO-Hz is three to six times higher than that of GO. The reduction of GO with glucose has only a slight effect on its sorptive properties. The temperature dependences of the diffusion coefficients of the GO, RGO-Gl and RGO-Hz samples have been obtained using the measured characteristic times of sorption. It is assumed that the temperature dependences of the diffusion coefficients are determined by the competition of the thermally activated and tunneling mechanisms, the tunneling contribution being dominant at low temperatures.



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150 - A.V. Dolbin 2016
The kinetics of the sorption and the subsequent desorption of 4He by the starting graphite oxide (GtO) and the thermally reduced graphene oxide samples (TRGO, Treduction = 200, 300, 500, 700 and 900 C) have been investigated in the temperature interval 1.5 - 20 K. The effect of the annealing temperature on the structural characteristics of the samples was examined by the X-ray diffraction (XRD) technique. On lowering the temperature from 20 K to 11-12 K, the time of 4He sorption increased for all the samples, which is typically observed under the condition of thermally activated diffusion. Below 5 K the characteristic times of 4He sorption by the GtO and TRGO-200 samples were only weakly dependent on temperature, suggesting the dominance of the tunnel mechanism. In the same region (T<5 K) the characteristic times of the TRGOs reduced at higher temperatures (300, 500, 700 and 900 C) were growing with lowering temperature, presumably due to the defects generated in the carbon planes on removing the oxygen functional groups (oFGs). The estimates of the activation energy (Ea) of 4He diffusion show that in the TRGO-200 sample the Ea value is 2.9 times lower as compared to the parent GtO, which is accounted for by GtO exfoliation due to evaporation of the water intercalated in the interlayer space of carbon. The nonmonotonic dependences Ea vs T for the GtO samples treated above 200 C are determined by a competition between two processes - the recovery of the graphite carbon structure, which increases the activation energy, and the generation of defects, which decreases the activation energy by opening additional surface areas and ways for sorption. The dependence of the activation energy on treatment temperature correlates well with the contents of the crystalline phase in GtO varying with a rise of the annealing temperature.
The operation of Thick Gaseous Electron Multipliers (THGEM) in Ne and Ne/CH4 mixtures, features high multiplication factors at relatively low operation potentials, in both single- and double-THGEM configurations. We present some systematic data measured with UV-photons and soft x-rays, in various Ne mixtures. It includes gain dependence on hole diameter and gas purity, photoelectron extraction efficiency from CsI photocathodes into the gas, long-term gain stability and pulse rise-time. Position resolution of a 100x100 mm^2 X-rays imaging detector is presented. Possible applications are discussed.
We report the design and development of a piezoelectric sample rotation system, and its integration into an Oxford Instruments Kelvinox 100 dilution refrigerator, for orientation-dependent studies of quantum transport in semiconductor nanodevices at millikelvin temperatures in magnetic fields up to 10T. Our apparatus allows for continuous in situ rotation of a device through >100deg in two possible configurations. The first enables rotation of the field within the plane of the device, and the second allows the field to be rotated from in-plane to perpendicular to the device plane. An integrated angle sensor coupled with a closed-loop feedback system allows the device orientation to be known to within +/-0.03deg whilst maintaining the sample temperature below 100mK.
Electron paramagnetic resonance (EPR) study of air-physisorbed defective carbon nano-onions evidences in favor of microwave assisted formation of weakly-bound paramagnetic complexes comprising negatively-charged O2- ions and edge carbon atoms carrying pi-electronic spins. These complexes being located on the graphene edges are stable at low temperatures but irreversibly dissociate at temperatures above 50-60 K. These EPR findings are justified by density functional theory (DFT) calculations demonstrating transfer of an electron from the zigzag edge of graphene-like material to oxygen molecule physisorbed on the graphene sheet edge. This charge transfer causes changing the spin state of the adsorbed oxygen molecule from S = 1 to S = 1/2 one. DFT calculations show significant changes of adsorption energy of oxygen molecule and robustness of the charge transfer to variations of the graphene-like substrate morphology (flat and corrugated mono- and bi-layered graphene) as well as edges passivation. The presence of H- and COOH- terminated edge carbon sites with such corrugated substrate morphology allows formation of ZE-O2- paramagnetic complexes characterized by small (<50 meV) binding energies and also explains their irreversible dissociation as revealed by EPR.
We present the magnetoresistance (MR) of highly doped monolayer graphene layers grown by chemical vapor deposition on 6H-SiC. The magnetotransport studies are performed on a large temperature range, from $T$ = 1.7 K up to room temperature. The MR exhibits a maximum in the temperature range $120-240$ K. The maximum is observed at intermediate magnetic fields ($B=2-6$ T), in between the weak localization and the Shubnikov-de Haas regimes. It results from the competition of two mechanisms. First, the low field magnetoresistance increases continuously with $T$ and has a purely classical origin. This positive MR is induced by thermal averaging and finds its physical origin in the energy dependence of the mobility around the Fermi energy. Second, the high field negative MR originates from the electron-electron interaction (EEI). The transition from the diffusive to the ballistic regime is observed. The amplitude of the EEI correction points towards the coexistence of both long and short range disorder in these samples.
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