H.-E. Wagner

The barrier discharge: basic properties and applications to surface treatment

Abstract Barrier discharges (BDs) produce highly non-equilibrium plasmas in a controllable way at atmospheric pressure, and at moderate gas temperature. They provide the effective generation of atoms, radicals and excited species by energetic electrons. In the case of operation in noble gases (or noble gas/halogen gas mixtures), they are sources of an intensive UV and VUV excimer radiation. There are two different modes of BDs. Generally they are operated in the filamentary one. Under special conditions, a diffuse mode can be generated. Their physical properties are discussed, and the main electric parameters, necessary for the controlled BD operation, are listed. Recent results on spatially and temporally resolved spectroscopic investigations by cross-correlation technique are presented. BDs are applied for a long time in the wide field of plasma treatment and layer deposition. An overview on these applications is given. Selected representative examples are outlined in more detail. In particular, the surface treatment by filamentary and diffuse BDs, and the VUV catalyzed deposition of metallic layers are discussed. BDs have a great flexibility with respect to their geometrical shape, working gas mixture and operation parameters. Generally, the scaling-up to large dimensions is of no problem. The possibility to treat or coat surfaces at low gas temperature and pressures close to atmospheric once is an important advantage for their application.

Spatio-temporally resolved spectroscopic diagnostics of the barrier discharge in air at atmospheric pressure

The technique of spatially resolved cross-correlation spectroscopy (CCS) is used to carry out diagnostic measurements of the barrier discharge (BD) in air at atmospheric pressure. Quantitative estimates for electric field strength E(x,t) and for relative electron density ne(x,t)/nemax are derived from the experimentally determined spatio-temporal distributions of the luminosity for the spectral bands of the 0-0 transitions of the second positive system of N2 (λ = 337.1 nm) and the first negative system of N2+ (λ = 391.5 nm). These results are used to test the validity of some physical models of electrical breakdown in a BD. The influence of the spatio-temporal structure of the discharge on the chemical kinetics of ozone synthesis is studied by means of a semi-empirical method based on the results of spatially resolved CCS measurements.

Investigation of the filamentary and diffuse mode of barrier discharges in N2/O2 mixtures at atmospheric pressure by cross-correlation spectroscopy

The techniques of spatially resolved cross-correlation spectroscopy (CCS) and current pulse oscillography were used to carry out systematic investigations of the barrier discharge (BD) in the binary gas mixtures N2/O2 at atmospheric pressure. At very low oxygen concentrations (<500 ppm), the BD was observed in a so-called diffuse mode (also referred to as atmospheric pressure glow discharge, glow silent discharge or homogeneous BD). In the case of the BD filamentary mode, the spatio-temporal distributions of the BD radiation intensities were recorded for the spectral bands of the 0–0 transitions of the second positive (λ = 337 nm) and first negative system of molecular nitrogen (λ = 391 nm). In the case of the diffuse mode, the spectral bands λ = 337 nm, λ = 260 nm (0–3 transition of the γ -system of NO) and λ = 557 nm (radiation of ON2 excimer) were used for this purpose. The velocities of the cathode-directed ionizing waves as well as the effective lifetimes of the excited states N2(C 3 � u)υ� =0 and N + (B 2 � + u )υ � =0 were evaluated from the CCS data. Special attention was devoted to the investigation of the transition between the filamentary and diffuse modes of the BD, this transition being caused by the variation of oxygen content within the range 500–1000 ppm. (Some figures in this article are in colour only in the electronic version)

Intensity ratio of spectral bands of nitrogen as a measure of electric field strength in plasmas

The ratios of intensities of the spectral bands of molecular nitrogen corresponding to transitions N + (B 2 � + g ,v = 0) → N + (X 2 � + ,v = 0), N2(C 3 � u ,v = 0) → N2(B 3 � g ,v = 0) and N2(C 3 � u ,v = 2) → N2(B 3 � g ,v = 5) as a function of the applied electric field strength were measured for air in the pressure range of 300 to 10 5 Pa. The non-self-sustaining dc discharge in a parallel-plane gap was used for excitation of gas molecules. The reduced field strength was varied in the range of (150–5000) × 10 −21 Vm 2 . The measured ratio of intensities as a function of electric field strength is compared with the theoretical estimates made by other authors. The obtained intensity ratio versus field strength curves can be used for field strength estimation in plasmas if the nitrogen molecules are excited dominantly from the ground state directly by the electron impact. (Some figures in this article are in colour only in the electronic version)

Diffuse barrier discharges in nitrogen with small admixtures of oxygen: discharge mechanism and transition to the filamentary regime

Diffuse barrier discharges (BDs) are characterized by the periodicity of their discharge current and by the uniform coverage of the entire electrode surface by the plasma. Up to now the discharge development, their appearance and dynamics cannot be adequately explained by elementary processes. Different processes are discussed in the literature controversially, in particular the importance of volume and surface processes on the pre-ionization (Penning-ionization, secondary (?-) processes, role of surface charges). Diffuse BDs in nitrogen with small admixtures of oxygen are investigated by plasma diagnostics (current/voltage-oscillography, optical emission spectroscopy) and numerical modelling. Special attention is paid to the transition to the usual filamentary mode, characterized by the presence of micro-discharges and caused by the admixture of oxygen in the range of 0?1200?ppm (parts-per-million). This transition starts at low values of O2 (about 450?ppm) and is introduced by an oscillative multi-peak mode. At higher admixtures (about 1000?ppm) the micro-discharges are generated. According to the results of numerical modelling, secondary electron emission by N2(A?3?u) metastable states plays a major role in discharge maintenance. Due to the much more effective quenching of these states by O2 and NO than by N2 the subsequent delivery of electrons will be decreased when the oxygen amount is increased.

The transition between different modes of barrier discharges at atmospheric pressure

Barrier discharges (BDs) can be operated in so-called diffuse modes. In contrast to the usual filamentary regime, which is characterized by a large number of individual microdischarges, the plasma of a diffuse BD covers the entire electrode area uniformly. Depending on the operation conditions (gas composition, amplitude and frequency of applied voltage), different diffuse modes can be investigated, namely, the atmospheric pressure Townsend discharge (APTD) and the atmospheric pressure glow discharge (APGD). The subject of the paper is the study of the transition between APTD and APGD as well as between diffuse and filamentary BD modes. Therefore, BDs were studied in the gas mixtures N2/H2, N2/He, N2/Ne and N2/Ar. It is shown that APGD in the noble gases helium and neon is formed due to high ionization rate at a comparatively low electric field, assisted by indirect ionization mechanisms involving metastable states of inert gases and nitrogen impurities, while the existence of APTD is coupled to the existence of metastable states of molecular nitrogen. Furthermore, a similar memory effect of residual surface charges on the dielectric barriers as described for filamentary BDs was observed in diffuse BDs.

Surface charge accumulation and discharge development in diffuse and filamentary barrier discharges operating in He, N2 and mixtures

A new discharge cell configuration was developed which allows the joint investigation of important volume and surface processes of the barrier discharge (BD) operation. In particular, the spatio-temporal and spectrally resolved discharge emission in the volume was studied together with the temporally resolved formation of surface charges on a dielectric BSO crystal. This was possible by the application of the cross-correlation spectroscopy and the electro-optic Pockels effect for surface charge measurement, respectively. Surface charges play an important role for the re-ignition of BDs. In pure nitrogen and helium, the diffuse Townsend-like discharge mode was studied, characterized by an emission maximum near the anode. Small admixtures of nitrogen to helium resulted in the filamentary discharge operation. Under these conditions, the importance of the so-called memory effect has been verified.The lateral extent of the discharge spots in the filamentary mode differs significantly for the positive and negative charges. Both can be approximated by Gaussian profiles. The deposited surface charges are in good agreement with the transferred charge of subsequent discharge breakdowns.

A computational model of a barrier discharge in air at atmospheric pressure: the role of residual surface charges in microdischarge formation

A two-dimensional (axially symmetric) computational model of the microdischarge formation in a barrier discharge for short (1–2 mm) gaps in air at atmospheric pressure is proposed. A non-homogeneous electric field, caused by a residual non-uniform charging of the dielectric barriers, is considered as an important reason for the filament formation by a Townsend mechanism. The ion–electron emission from the dielectric covering the cathode is treated as the principal secondary process; the secondary emission coefficient in the model is selected to be consistent with the Paschen voltage. For an applied sinusoidal voltage, this follows the microdischarge development on a microsecond scale. It is shown that even a slight inhomogeneity of the initial electric field leads to the formation of a narrow microdischarge channel.The two-dimensional dynamics of the radiation from a microdischarge for the case of the second positive and the first negative systems of nitrogen is simulated and compared with recent experimental data. The effects of the secondary emission coefficient and of a distribution of residual surface charges are investigated. It is shown that the level of inhomogeneity of the residual surface charge distribution does not affect the radius of the microdischarge channel, but affects its two-dimensional structure.The proposed model explains satisfactorily the experimental results for the velocity of the cathode-directed ionizing wave and the emission of the N2 second positive system from a microdischarge.

Comparative study of diffuse barrier discharges in neon and helium

Diffuse dielectric barrier discharges in neon and helium at atmospheric pressure were studied. The discharges were generated between two metal electrodes, both covered by an alumina layer and driven by ac voltage of frequency 10 kHz. The discharge gap was 2.2 mm and 5 mm, respectively. The discharges were investigated by electrical measurements and by temporally and spatially resolved optical emission spectroscopy. The experimental results revealed similar discharge behaviour in both gases being considered. Although the discharges were ignited at slightly different electric field strengths, their evolutions were found to be similar. At maximum discharge current the spatial light intensity distribution was characterized by the formation of a cathode fall. A difference was observed in the magnitudes of the current density only. In addition to the regime with a single discharge pulse per voltage half period T/2, a discharge mode with two and more subsequent current pulses per T/2 (also referred to as the pseudoglow discharge regime in the literature) was obtained due to an increase in the voltage amplitude or an admixture of nitrogen.

Systematic investigation of the barrier discharge operation in helium, nitrogen, and mixtures: discharge development, formation and decay of surface charges

As a logical extension to previous investigations of the barrier discharge (BD) in helium and nitrogen, the present work reports on the operation in any mixtures of both pure gases. Using a well-established plane-parallel discharge cell configuration allows to study the influence of the He/N2 mixing ratio on the formation of different discharge modes. Their characterization was made by measuring the discharge emission development together with the formation and decay of surface charges on a bismuth silicon oxide (Bi12SiO20, BSO) crystal. This was realized by the simultaneous application of the spatio-temporally resolved optical emission spectroscopy, and the electro-optic Pockels effect in combination with a CCD high speed camera. The existence diagram for diffuse and filamentary BDs was determined by varying the amplitude and shape of the applied voltage. Over the entire range of the He/N2 ratio, the diffuse mode can be operated at moderate voltage amplitudes whereas filamentation occurs at significant overvoltage and is favoured by a high voltage slew rate. Irrespective of the discharge mode, the overall charge transfer during a discharge breakdown is found to be in excellent agreement with the amount of accumulated surface charges. An exponential decay of the surface charge deposited on the BSO crystal is induced by LED illumination beyond a typical discharge cycle. During the decay process, a broadening of the radial profiles of positive as well as negative surface charge spots originating from previous microdischarges is observed. The investigations contribute to a better understanding of the charge accumulation at a dielectric.