We present a self-consistent formulation to study low-pressure traveling wave (azimuthally symmetric surface transverse magnetic mode) driven discharges in nitrogen. The theoretical model is based on a self-consistent treatment of the electron and heavy particle kinetics, wave electrodynamics, gas thermal balance, and plasma–wall interactions. The solution provides the axial variation (as a result of nonlinear wave power dissipation along the wave path) of all discharge quantities and properties of interest, such as the electron energy distribution function and its moments, population densities of all relevant excited and charged species [N2(X 1Σg+,ν),N2(A 3Σu+,a′ 1Σu−,B 3Πg,C 3Πu,a 1Πg,w 1Δu), N2+, N4+, e], gas temperature, degree of dissociation [N(4S)]/N, mean absorbed power per electron, and wave attenuation. A detailed analysis of the energy exchange channels among the degrees of freedom of the heavy particles is presented. Particular attention is paid to the axial variation of the gas and wall temperatures, which affect in a complex way the discharge operation. For the high electron densities and reduced electric fields achieved at 2.45 GHz, it is shown that the contribution of exothermic reactions involving excited molecules in metastable states to the total gas heating can be significant. The role of the triplet N2(A 3Σu+) metastable state as an energy “reservoir” that pumps translational modes of gas particles is pointed out. A strong correlation between the degree of dissociation, the concentration of metastable N2(A 3Σu+), N(2D,2P) particles, and surface kinetics is shown to exist. Spatially resolved measurements of the gas and wall temperatures, electron density, and wave propagation characteristics provide a validation of the model’s predictions.

A theoretical model for a low pressure surface wave driven N2–Ar discharge accounting in a self-consistent way for electron and heavy particle kinetics, gas thermal balance, and wave electrodynamics is developed. The inhomogeneous wave power transfer along the discharge and the concentrations of active species as a function of the spatial position and mixture composition are investigated. N2+ are the dominant ions over a wide range of Ar percentages in the mixture due to the contributions of charge transfer processes between Ar+ and N2 and an effective associative ionization from N2(A 3Σu+). Dissociative recombination of N2+ with electrons provides an increase in the dissociation degree of nitrogen molecules at high Ar fractional concentration.

A theoretical and experimental study on atmospheric pressure microwave plasma-based assembly of free standing graphene sheets is presented. The synthesis method is based on introducing a carbon-containing precursor (C 2 H 5 OH) through a microwave (2.45 GHz) argon plasma environment, where decomposition of ethanol molecules takes place and carbon atoms and molecules are created and then converted into solid carbon nuclei in the 'colder' nucleation zones. A theoretical model previously developed has been further updated and refined to map the particle and thermal fluxes in the plasma reactor. Considering the nucleation process as a delicate interplay between thermodynamic and kinetic factors, the model is based on a set of non-linear differential equations describing plasma thermodynamics and chemical kinetics. The model predictions were validated by experimental results. Optical emission spectroscopy was applied to detect the plasma emission related to carbon species from the 'hot' plasma zone. Raman spectroscopy, scanning electron microscopy (SEM), and x-ray photoelectron spectroscopy (XPS) techniques have been applied to analyze the synthesized nanostructures. The microstructural features of the solid carbon nuclei collected from the colder zones of plasma reactor vary according to their location. A part of the solid carbon was deposited on the discharge tube wall. The solid assembled from the main stream, which was gradually withdrawn from the hot plasma region in the outlet plasma stream directed to a filter, was composed by 'flowing' graphene sheets. The influence of additional hydrogen, Ar flow rate and microwave power on the concentration of obtained stable species and carbon−dicarbon was evaluated. The ratio of sp 3 /sp 2 carbons in graphene sheets is presented. A correlation between changes in C 2 and C number densities and sp 3 /sp 2 ratio was found.

Self-standing graphene sheets were synthesized using microwave plasmas driven by surface waves at 2.45 GHz stimulating frequency and atmospheric pressure. The method is based on injecting ethanol molecules through a microwave argon plasma environment, where decomposition of ethanol molecules takes place. The evolution of the ethanol decomposition was studied in situ by plasma emission spectroscopy. Free gas-phase carbon atoms created in the plasma diffuse into colder zones, both in radial and axial directions, and aggregate into solid carbon nuclei. The main part of the solid carbon is gradually withdrawn from the hot region of the plasma in the outlet plasma stream where nanostructures assemble and grow. Externally forced heating in the assembly zone of the plasma reactor has been applied to engineer the structural qualities of the assembled nanostructures. The synthesized graphene sheets have been analysed by Raman spectroscopy, scanning electron microscopy, high-resolution transmission electron microscopy and x-ray photoelectron spectroscopy. The presence of sp 3 carbons is reduced by increasing the gas temperature in the assembly zone of the plasma reactor. As a general trend, the number of mono-layers decreases when the wall temperature increases from 60 to 100 • C. The synthesized graphene sheets are stable and highly ordered.

Direct assembling of N-graphene, i.e. nitrogen doped graphene, in a controllable manner was achieved using microwave plasmas at atmospheric pressure conditions. The synthesis is accomplished via a single step using ethanol and ammonia as carbon and nitrogen precursors. Tailoring of the high-energy density plasma environment results in a selective synthesis of N-graphene (~0.4% doping level) in a narrow range of externally controlled operational conditions, i.e. precursor and background gas fluxes, plasma reactor design and microwave power. Applying infrared (IR) and ultraviolet (UV) irradiation to the flow of free-standing sheets in the post-plasma zone carries out changes in the percentage of sp2, the N doping type and the oxygen functionalities. X-ray photoelectron spectroscopy (XPS) revealed the relative extension of the graphene sheets π-system and the type of nitrogen chemical functions present in the lattice structure. Scanning Electron microscopy (SEM), Transmission Electron microscopy (TEM) and Raman spectroscopy were applied to determine morphological and structural characteristics of the sheets. Optical emission and FT-IR spectroscopy were applied for characterization of the high-energy density plasma environment and outlet gas stream. Electrochemical measurements were also performed to elucidate the electrochemical behavior of NG for supercapacitor applications.