Noble Gas Discharges Research Articles

Ionization waves in low-current dc discharges in noble gases obtained with a hybrid kinetic-fluid model.

A hybrid kinetic-fluid model is used to study ionization waves (striations) in a low-current plasma column of dc discharges in noble gases. Coupled solutions of a kinetic equation for electrons, a drift-diffusion equation for ions, and a Poisson equation for the electric field are obtained to clarify the nature of plasma stratification in the positive column. A simplified two-level excitation-ionization model is used for the conditions when the nonlinear effects due to stepwise ionization, gas heating, and Coulomb interactions among electrons are negligible. It is confirmed that the nonlocal effects are responsible for the formation of moving striations in dc discharges at low plasma densities and low values of pR (the product of gas pressure and tube radius). The calculated properties of self-excited waves of S-, P-, and R types in neon and S type in argon agree with available experimental data. The reason for helium plasma stability to stratification is clarified. It is shown that sustaining stratified plasma is more efficient than striation-free plasma when the ionization rate is a nonlinear function of the electric field. However, the nonlinear dependence of the ionization rate on the electric field is not required for plasma stratification. Striations of S-, P-, and R types in neon exist with minimal or no ionization enhancement. Effects of the column length and plasma density on the wave properties are demonstrated.

A self-consistent hybrid model of kinetic striations in low-current argon discharges

A self-consistent hybrid model of standing and moving striations was developed for low-current DC discharges in noble gases. We introduced the concept of surface diffusion in phase space (r, u) (where u denotes the electron kinetic energy) described by a tensor diffusion in the nonlocal Fokker–Planck kinetic equation for electrons in the collisional plasma. Electrons diffuse along surfaces of constant total energy ɛ = u − eφ(r) between energy jumps in inelastic collisions with atoms. Numerical solutions of the 1d1u kinetic equation for electrons were obtained by two methods and coupled to ion transport and Poisson solver. We studied the dynamics of striation formation in Townsend and glow discharges in argon gas at low discharge currents using a two-level excitation-ionization model and a ‘full-chemistry’ model, which includes stepwise and Penning ionization. Standing striations appeared in Townsend and glow discharges at low currents, and moving striations were obtained for the discharge currents exceeding a critical value. These waves originate at the anode and propagate towards the cathode. We have seen two types of moving striations with the two-level and full-chemistry models, which resemble the s and p striations previously observed in the experiments. Simulations indicate that processes in the anode region could control moving striations in the positive column plasma. The developed model helps clarify the nature of standing and moving striations in DC discharges of noble gases at low discharge currents and low gas pressures.

Measurement of plasma densities by dual frequency multichannel boxcar THz time domain spectroscopy

In this paper we show the development and the application of the terahertz time domain spectroscopy (THz TDS) diagnostic technique for the determination of plasma densities in low-pressure discharges. A commercially available system was modified to reach a better signal-to-noise ratio. For that the THz emitter and the detection method were changed and a fast lock-in amplifier was used to reach 38 MHz lock-in frequency. These modifications in a combination with the novel method of dual frequency multichannel boxcar embedded as a feature in the lock-in amplifier allowed us to make also time-resolved measurements. The temporal resolution can potentially go down to 100 ps and is limited only by the spectral range that needs to be recovered for the measurement of low electron densities. Further, the cause of artefacts found in all THz TDS based systems, but not understood until now, is identified and explained.As an application the electron densities in inductively coupled plasmas sustained in a magnetic multi-cusp chamber are determined. Results from steady-state discharges in noble gases (He, Ne, Ar, Kr, Xe) and time-resolved measurements in pulsed discharges in Ar and Ne are presented. The technique is benchmarked against microwave interferometry with good agreement in the applicability range of both techniques. The THz TDS performs reliably also in much denser plasmas where standard microwave interferometry fails. The lower limit for the technique is at a line-integrated electron density of 1012 cm−2, corresponding to about 1011 cm−3 for typical plasma dimensions.

The Effects of Added Hydrogen on Noble Gas Discharges Used as Ambient Desorption/Ionization Sources for Mass Spectrometry.

We demonstrate the effectiveness of using hydrogen-doped argon as the support gas for the dielectric barrier discharge (DBD) ambient desorption/ionization (ADI) source in mass spectrometry. Also, we explore the chemistry responsible for the signal enhancement observed when using both hydrogen-doped argon and hydrogen-doped helium. The hydrogen-doped argon was tested for five analytes representing different classes of molecules. Addition of hydrogen to the argon plasma gas enhanced signals for gas-phase analytes and for analytes coated onto glass slides in positive and negative ion mode. The enhancements ranged from factors of 4 to 5 for gas-phase analytes and factors of 2 to 40 for coated slides. There was no significant increase in the background. The limit of detection for caffeine was lowered by a factor of 79 using H2/Ar and 2 using H2/He. Results are shown that help explain the fundamental differences between the pure-gas discharges and those that are hydrogen-doped for both argon and helium. Experiments with different discharge geometries and grounding schemes indicate that observed signal enhancements are strongly dependent on discharge configuration. Graphical Abstract ᅟ.

An experimental study on the influence of trace impurities on ionization of atmospheric noble gas dielectric barrier discharges.

While the influence of trace impurities in noble gas discharges is well established in theoretical work, experimental approaches are difficult. Particularly the effects of trace concentrations of N2 on He discharges are complicated to investigate due to the fact that for He 5.0 the purity of He is only 99.999%. This corresponds to a residual concentration of 10 ppm, thereof 3 ppm of N2, in He. Matters are made difficult by the fact that He DBD plasmajets are normally operated under an ambient atmosphere, which has a high abundance of N2. This work tackles these problems from two sides. The first approach is to operate a DBD plasmajet under a quasi-controlled He atmosphere, therefore diminishing the effect of atmospheric N2 and making a defined contamination with N2 possible. The second approach is using Ar as the operating gas and introducing propane (C3H8) as a suitable substitute impurity like N2 in He. As will be shown both discharges in either He or Ar, with their respective impurity show the same qualitative behaviour.

Stratification of discharge in noble gases from the viewpoint of the discrete dynamics

Based on the analysis of electron phase trajectories in sinusoidal electric fields, a new point of view on discharge stratification is proposed. It is shown that the positive column can be considered as a spatial resonator in which electric fields with a fundamental period length LS or higher mode length qpLS establish, where p and q are integers and p > q. The fundamental mode length LS is equivalent to the distance on which electrons gain energy equal to the lowest excitation threshold. This distance determines a length of the S-striation. Unlike kinetic theory, in the presented model resonance properties of the discharge column are not connected with elastic collision energy losses. A point map is used to obtain the resonance trajectories of electrons in the phase plane. Stable points for the positions of inelastic collisions in the resonance trajectories have been found at the positions of field maxima in the case of integer ratios pq. For non-integer ratios pq, multiple resonance trajectories arise according to a more complex stability criterion. From this point of view, S-, P-, and R-striations in noble gas discharges can be explained. Due to energy losses in elastic collisions, initial electron energy distribution functions converge to the resonance trajectories (the so-called “bunch effect”). The findings of the discrete model agree with results of kinetic theory and experiment. The new approach avoids difficulties of the kinetic theory in the case of exceptionally large relaxation lengths which can even exceed the positive column length.

Nonlocal control of electron temperature in short direct current glow discharge plasma

To demonstrate controlling the electron temperature in nonlocal plasma, experiments have been performed on a short (without positive column) dc glow discharge with a cold cathode by applying different voltages to the conducting discharge wall. The experiments have been performed for low-pressure noble gas discharges. The applied voltage can modify trapping the energetic electrons emitted from the cathode sheath and arising from the atomic and molecular processes in the plasma within the device volume. This phenomenon results in the energetic electrons heating the slow plasma electrons, which consequently modifies the electron temperature. Furthermore, a numerical model of the discharge has demonstrated the electron temperature modification for the above case.

The positive-column plasma in low-pressure noble gas d.c. discharge as an integral plasma-field system

A one-dimension model for positive-column plasma is analyzed. In the framework of this model, a complete, self-consistent set of equations for the plasma column is proposed and justified. Basic prerequisites for the model and the equations used in it are discussed at length to clarify the mathematics and physics that underlie the proposed generalized description of plasma states. A study of the equations has unveiled the existence of two structurally stable types of steady states and three integrals of motion in the plasma system. The first type of states corresponds to spatially homogeneous plasma, and the second type, to the self-forming plasma structure with striations. Analysis of spatio-temporal plasma structures (spatially homogeneous and stratified stationary plasma states) and their attendant phenomena is given in detail. It is shown that the equations offer a more penetrating insight into the physical states and properties of positive-column plasma in dc-driven gas discharges, and into the various phenomena proceeding in the discharge system. Such a behavior is intimately related to the influence which the electric field has on the rate of ionization reactions. The theoretical results are compared to experimental data and can be used for to place the great body of experimental data in their proper framework. The modern fluid bifurcation model proposed to describe the properties of non-isothermic positive-column plasma in dc-driven low-pressure noble-gas discharges proved to be rather realistic, capable of adequately reproducing the basic properties of real field-plasma systems.

Thermometry in noble gas dielectric barrier discharges at atmospheric pressure using optical emission spectroscopy

We measure the temperature, T, of dielectric barrier discharges (DBD), in noble gases using optical emission spectroscopy (OES), by analysing rotational bands in the emission spectra of the first negative system (FNS) of N <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">+</sup> . This has the advantage that rotational structure can be fully resolved even with a spectrograph of average performance, and that the rotational temperature, T <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">rot</sub> (~ T <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">gas</sub> ) can then be determined from a conventional Boltzmann plot. Ionization of N2 occurs mainly via Penning transfer from metastable excited states of He (ca. 20 eV) or Ne (ca. 16.6 eV). Using two glass-walled DBD chambers of very different volumes (0.1 and 20 liters), we have studied atmospheric-pressure discharges in flowing helium (He) or neon (Ne) containing traces of nitrogen. Discharges were excited by audio-frequency (10 kHz) high voltage (HV) using a needle as the HV electrode and a dielectric (alumina)-covered planar grounded counter-electrode. OE spectra were acquired with a 0.5 m focal length spectrograph, coupled to an intensified charge coupled device (ICCD) detector. Using the (0-0) R-branch of the FNS N <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">+</sup> (B <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sup> Σ <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">u</sub> <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">+</sup> - X <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sup> Σ <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">g</sub> <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">+</sup> ) bands near a wavelength of 391.4 nm, we have measured axial (inter-electrode) distributions of T <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">rot</sub> for the two different reactor volumes in both He and Ne. T <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">rot</sub> values were found to be highest at the needle electrode, of about 450 K and 740 K for He and Ne, respectively; in He, T <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">rot</sub> dropped to a minimum of about 405 K at the mid-gap position in the small chamber, and ~ 360 K near the planar electrode in the large chamber. We conclude that temperatures in noble gas discharges depend critically on thermal conductivities of the particular gases (K <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">He</sub> = 1.9; K <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">Ne</sub> = 0.6, both in mW.cm <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">-1</sup> .K <sup xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">-1</sup> ) and on other experimental factors that influence heat transfer.

Feasibility Study of VUV Sensitization Effect of Tb3+

ABSTRACT The possibility to use Tb3+ as luminescence sensitizer for enhancement of the conversion efficiency of vacuum-ultraviolet (VUV) radiation into visible light was examined. We studied the luminescence properties of K3Tb(PO4)2 and Ba3Tb(PO4)3 activated by Eu3+, and of SrAl12O19 co-doped with Mn2+ and Tb3+ at excitation over the 120 to 300 nm wavelength range. It is shown that Tb3+ ions, exhibiting a strong absorption band in the VUV, can provide efficient sensitization of Eu3+ and Mn2+ emissions for excitation in this spectral range, giving rise to intense red and green luminescence, respectively. This study provides a proof for the concept of VUV sensitization, which enables the engineering of luminescence materials with improved efficiency for excitation from a noble gas discharge.

Concerning the width of spark channels with different polarities in submicrosecond sliding discharges in noble gases

Previously, the parameters of submicrosecond (with a duration of <200 ns) multichannel high-current discharges sliding along a ceramic surface in Ne, Ar, and Xe were studied only for the negative polarity of the applied voltage. The experimental data indicate that the channels expand in the transverse direction mainly due to electron drift from the channel surface layer under the action of the electric field perpendicular to the channel axis and subsequent gas ionization by these electrons. To investigate mechanisms for the channel development in a sliding discharge—in particular, to determine the contribution of electron drift—it is necessary to carry out experiments similar to those performed earlier for the opposite polarity of the applied voltage. Here, the results of measurements of the widths of the spark channels of negativeand positive-polarity sliding discharges excited in Ne, Ar, and Xe at pressures of 30 and 100 kPa are presented and discussed. It is shown that, depending on the pressure and sort of gas, the averaged optical width of positive-polarity channels is smaller by a factor of 1.27–1.60 than that of negative-polarity channels. The experimental data are analyzed using the theory of propagation of ionization waves with different polarities in gases. Analysis has shown that electron diffusion contributes insignificantly to channel expansion and that, for both polarities, the channel expansion rate exceeds the electron drift velocity in the transverse electric field near the channel. In the framework of the so-called approximation of nonlocalized initial conditions, the measured ratio between of the widths of negativeand positive-polarity channels and their relation to the electron mobility are explained by the channel expansion governed by both electron drift and primary free electrons produced by a short-term source in a narrow region ahead of the front of the expansion wave. Numerical simulations show that the width of this region is comparable with that of the wave front and is more than one order of magnitude smaller than the observed channel radius. Gas photoionization by the channel radiation can serve as a source of primary electrons.

Plasma series resonance in the E mode of low-pressure inductively coupled noble gas discharges

When operated at low pressure, plasma discharges bounded by radiofrequency (rf)-driven sheaths exhibit high harmonics in the discharge current, which occur due to the nonlinear charge–voltage relation of the sheath. This phenomenon is well known from capacitive rf discharges and commonly called the plasma series resonance (PSR) effect. Rf inductively coupled plasmas (ICPs) operated at low power are usually mainly driven capacitively (E mode) and act similar to capacitive discharges (CCPs), which includes the occurrence of the series resonance effect. In this communication the effect is investigated experimentally and compared with a simple global model which is an extension of existing CCP models to the ICP. Additionally, the influence of the series resonance on the electron energy distribution is investigated.

The effects of traces of molecular gases (H2, N2 & O2) in glow discharges in noble gases

A brief introduction is given on the use of glow discharges in noble gases for spectrochemical analysis, with particular emphasis on Glow Discharge Optical Emission Spectroscopy (GD-OES). This explains the relevance of investigations on the effect of small quantities of molecular gases on the performance of discharges in noble gases, mainly in argon. The chief effects are on the electrical characteristics, the sputtering rate and the spectrum emitted. Earlier work is briefly reviewed, the options for spectral investigations discussed and the current state-of-the-art described for some samples (cathodes) of analytical importance (copper, iron and titanium) The main emphasis is on the addition of hydrogen to discharges in argon, with brief comments on other gas mixtures. A great deal of work remains to be done, both to produce empirical data for analytical use and to gain a fuller understanding of the discharge processes involved.

Electron scattering from argon: Data evaluation and consistency

The demand for coherent scattering data for modeling electron transport in matter has increased in recent years. While much effort has been devoted to the improvement of models describing electron transport and scattering, the updating of fundamental data sets on the basis of recent experimental results has often been neglected. The use of a well-validated set of electron cross sections ensures accurate calculations of transport parameters and ionization yields, with typical applications in material analysis, detector response studies, plasma diagnostics, physics of the atmosphere, and radiotherapy. Data consistency can be verified on the basis of various theoretical requirements, and systematic errors can be minimized by cross-checking results obtained from independent experiments. For example, the oscillator strength distribution of an atom can be obtained both from photoabsorption experiments and from zero-angle electron-atom collisions at high energy, on the basis of the Bethe theory. A considerable number of all electron-scattering experiments are concerned with light noble gases, in particular with argon. This gas is a dominant constituent of noble-gas discharge plasmas and plays an important role in rare-gas halide lasers and proportional scintillator counters. This work reviews electron-scattering cross sections and optical data for the argon atom, discusses the progress made in the field of electron scattering and photoabsorption, and focuses on the most appropriate criteria for verifying data consistency.

Effects of fast neutral particles in low-pressure gas discharges

The effects of fast neutral (heavy) particles on the characteristics of low-pressure noble gas discharges are reviewed. Complementing experimental observations, numerical simulations are applied to demonstrate the importance of these species in the (i) surface reactions causing cathodic electron emission and (ii) gas-phase reactions leading to the creation of charged particles and to light emission through excitation processes. All these processes are found to be important at high values of the electric field to gas density ratio, E/n, under which conditions positive ions - being the primary species creating fast neutrals in collision processes - acquire high energy in the cathode region.

Grain surface temperature in noble gas discharges: Refined analytical model

A model of grain surface temperature in a low-pressure weakly ionized complex plasma is refined by taking into account the effect of rare ion-neutral collisions in the vicinity of the grain. These collisions enhance plasma collection by the grain and can result in a considerable increase of the grain temperature. It is shown that the collision enhanced plasma collection model yields generally better agreement with the results of existing experiments. The effect of the temperature difference between the grain surface and the surrounding gas on the grain-grain interaction potential is also briefly discussed.

A chamber for studying planetary environments and its applications to astrobiology

We have built a versatile environmental simulation chamber capable of reproducing atmospheric compositions and surface temperatures for most of the planetary objects. It has been especially developed to make feasible in situ irradiation and characterization of the sample under study. The total pressure in the chamber can range from 5 to 5 × 10−9 mbar. The required atmospheric composition is regulated via a residual gas analyser with ca ppm precision. Temperatures can be set from 4 K to 325 K. The sample under study can be irradiated with ion and electron sources, a deuterium ultraviolet (UV) lamp and a noble-gas discharge UV lamp. One of the main technological challenges of this device is to provide the user the possibility of performing ion and electron irradiation at a total pressure of 0.5 mbar. This is attained by means of an efficient differential pumping system. The in situ analysis techniques implemented are UV spectroscopy and infrared spectroscopy (IR). This machine is especially suitable for following the chemical changes induced in a particular sample by irradiation in a controlled environment. Therefore, it can be used in different disciplines such as planetary geology, astrobiology, environmental chemistry, materials science and for instrumentation testing.

Different modes of arc attachment at HID cathodes: simulation and comparison with measurements

Based on a model for the plasma boundary layer of high intensity discharge cathodes, simulations are performed and compared with experimental results. To solve the power balance of the cathode body different methods are used, namely a 1D integral solution as well as 1D, 2D and 3D finite-element calculations. The simulations are done for cylindrical tungsten cathodes operated in different pure noble gas discharges (0.1–1.0 MPa) and with currents between 0.5 and 10 A. Under these conditions different modes of arc attachment are found, both in simulations and experiments.For the diffuse mode of arc attachment an excellent quantitative agreement between measurements and the simulations is obtained, reflecting an improved accuracy of measurements and simulation. In addition, different spot modes are found. At least one of these modes is also observed in the experiment. Also for this spot mode the agreement between measurements and simulation for the integral quantities is good. There are still some open questions concerning the spot mode of cathodic arc attachment.Varying the geometric dimensions of the cathode, the proper simulation of the heat conduction problem of the cathode body is shown. Variations of the plasma properties, like gas type and pressure, prove the conceptional capability of the boundary layer model for the simulation of different modes of arc attachment. Evaluating the cathode fall characteristics, regions of existence for the different modes are found, which are similar to the experiments.

Removal of volatile organic compounds in atmospheric pressure air by means of direct current glow discharges

A nonthermal plasma with an electron density on the order of 10/sup 12/ cm/sup -3/ and a gas temperature of 2000 K was generated in atmospheric pressure air, using a microhollow cathode discharge as plasma cathode. The plasma was sustained in a /spl sim/1 mm/sup 3/ micro reactor, by a voltage of 470 V between the plasma cathode and a planar anode, and at currents ranging from 12 to 22 mA. This direct current glow discharge has been used to study the remediation of methane and benzene, two of the most stable volatile organic compounds (VOCs). The removal fraction for 300-ppm methane in atmospheric pressure air, flowing through the 0.5-mm thick plasma layer, with a residence time of the gas in the plasma of less than 0.5 ms, was measured at 80% with an energy density of 4 kJ/L. For benzene, the remediation rate is as high as 90%, comparable to results obtained with low pressure glow discharges. The energy efficiency for benzene remediation is 0.9 g/kWh, higher than that obtained for benzene remediation in low pressure glow discharges in noble gases. However, the VOC fraction remaining was found to be limited to values of approximately 0.1 and 0.05 for methane and benzene, respectively. In addition to experimental studies, the VOC dissociation mechanism in a VOC/dry air mixture plasma was modeled using a zero-dimensional plasma chemistry code. The modeling results have shown that atomic oxygen impact reactions are the dominant dissociation reactions for VOC destruction in this kind of glow discharge. Diffusion of atomic oxygen to the dielectric walls of the reactor is assumed to cause the observed limitation in the VOC destruction rate and efficiency.

Control of dissociation by varying oxygen pressure in noble gas admixtures for plasma processing

The electron density, electron temperature, and atomic oxygen density are measured in mixtures of oxygen and noble gas discharges as a function of the input power and the oxygen partial pressure. The atomic oxygen density is measured by both actinometry and appearance mass spectrometry and plasma density and electron temperature are monitored with Langmuir probes. The background noble gas determines the electron density and temperature as long as the partial pressure of oxygen remains small. The dissociated atomic neutral oxygen density is highest in O2∕Xe mixtures and lowest in O2∕He mixtures, increases with electron density, and decreases with electron temperature. Estimates of the dominant source and sink rates of atomic oxygen are used to explain these results using a simple zero-dimensional dissociation kinetics and transport model. The use of noble gas/oxygen mixtures allows for a larger range of atomic oxygen density and ion density than in pure oxygen plasmas, and also allows for independent control of the ion density and the atomic oxygen density.