st 21 International Symposium on Plasma Chemistry (ISPC 21) Sunday 4 August – Friday 9 August 2013 Cairns Convention Centre, Queensland, Australia Time resolved ion density and electrical field determination by electrical current measurements in a self-pulsing plasma at atmospheric pressure air T Gerling, R Bussiahn, C. Wilke, and K-D Weltmann Leibniz Institute for Plasma Science and Technology (INP Greifswald), Greifswald, Germany Abstract: High resolution current signals of a self-pulsing discharge revealed characteristic oscillations in the pulse decay phase. These oscillations appear with decreasing frequency between 250 MHz and 75 MHz. It is expected, that these oscillations are the result of ion acoustic waves. From frequency and current amplitude measurements, the ion density and electric field strength is calculated over time. Keywords: Electrical characterization, ion acoustic wave, ion density, electrical field strength 1. Introduction Atmospheric pressure plasmas are a field of great potential in the industrial and medical sector [1]. A challenging part for the characterization of plasma sources remains the determination of plasma parameters like species densities. The variety of techniques to determine these parameters is still very limited and mostly involves costly equipment. Current and voltage measurements are a simple method to gain first information about a plasma discharge. In previous experiments, we observed weak oscillations in the current and voltage signals [2]. The oscillations were interpreted to be a result from ion acoustic waves, with densities well in the range of estimated electron densities. The experimental setup and new results on the oscillations will be presented here. Possible sources of errors will be discussed along with the setup to underline the sensitivity of highly resolved electrical measurements. Afterwards, the origin of the oscillations is evaluated. Finally, the resulting ion density and electrical field calculations are presented. 2. Experimental Setup For this investigation, a self-pulsing, discharge as in [2,3] is used (see figure 1). A negative DC voltage (-5 … -10 kV) is applied by a high resistive power supply to a hollow needle electrode (0.8 mm outer diameter). The grounded counter electrode is a 4x4 mm² copper plate in a distance of 8 mm. A quartz capillary surrounds the needle electrode (3 mm outer diameter) and is placed 5 mm from the needle tip [2]. An argon gas flow between 0.2 and 0.5 slm is supplied through the needle electrode. The created discharge filament (transient spark [2,4]) has a diameter of 60 μm (measured by photography). Current amplitudes between 0.2 A and 3.8 A are possible. The applied voltage charges the device capacity until the breakdown voltage is reached. Since the discharge operates in flowing argon, the breakdown conditions are not stable and the repetition frequency varies between 0.5 and 3 kHz. The electrical measurements were done with two dif- Fig.1: ground loop free experimental setup ferent setups. In accordance with the arrangement in [2], the first setup consisted of a high voltage probe (Tektronix P6015A) mounted in open air as an antenna and a second voltage probe (Tektronix P5100) was connected before a 100 Ω resistor at the grounded electrode. The discharge was grounded in the same spot as the oscilloscope (both probes connected, Tektronix DPO7104) and the power supply. For the second setup, the voltage probes were removed and only a current probe (Tektronix CT1) placed after the resistor (see figure 1). For some measurements the signal of the probe was split on two channels of the oscilloscope to have high resolution for small changes on the one and low resolution but therefore absolute peak values on the other channel. 3. Results of electrical Measurements Typical current and voltage slopes for the measurement with voltage probes are shown in figure 2. The voltage slope of the antenna probe (red curve) shows the voltage breakdown after a discharge event. The voltage jumps from its negative value (around -5 kV [2]) to 0 kV (figure 2 has only relative values) within 30 ns. After the breakdown, some oscillations are observed on the voltage signal. The current signal for the discharge is overexposed to record the oscillations with higher resolution. While the scale in figure 2 is limited to a current amplitude of 50 mA, the discharge current peak in this case is about -400 st 21 International Symposium on Plasma Chemistry (ISPC 21) Sunday 4 August – Friday 9 August 2013 Cairns Convention Centre, Queensland, Australia mA. At the beginning of the current signal, the breakdown is visible by a steep drop. Afterwards, the current decays towards zero in damped oscillations with obviously different, overlapping frequencies. Fig.4: current signal of the discharge with measurement of the peak value (160 mA) and overexposed signal with weak current spikes (some mA amplitude). QAr = 500 sccm, UA = -10 kV Fig.2: current and relative voltage signal (antenna) for the breakdown. The current signal is overexposed to enhance the visibility of the oscillations (QAr = 500 sccm, UA = -10 kV) In figure 3, the fast Fourier transformation (FFT) of the signals from figure 2 is shown. Several characteristic frequencies are observed, whereas the peak at 73 MHz was seen on both signals. By changing cable lengths and grounding conditions, differences in the frequencies could be observed. But even with a single voltage probe, the oscillation with its sensitivity towards cable length and grounding remained. Fig.3: FFT analysis of current and voltage signal from figure 2. When all voltage probes were removed and only the current probe inserted (see figure 1), the signal was almost free of oscillations. This indicates, that the reason for the oscillations were ground loops with lengths in the order of some 10 m. Nevertheless, this new setup revealed some even smaller signals on the decaying current peak. Examples are shown in figure 4. The main current peak is about 160 mA and decays within 150 ns. The same signal is given onto a second channel of the oscilloscope and the sensitivity increased many times, shown in figure 4 as well. A very weak oscillation is detected with amplitudes up to 3 mA. In general, the cycle duration increases (repetition frequency decreases) while the amplitude is slightly reduced. To be precise, the signal presented in figure 4 is not the regular signal of the setup. It is more like a rare exception, only occurring every ten or twenty discharges. The trigger for this type of discharge seems to be very sensible. With this setup, the observed signal is invariant to the variation of the cable length or grounding. The conditions for its appearance were found to be strongly dependent on the gas flow. While for small argon flow rates from 200 sccm up to 450 sccm, the signal was not visible, above 450 sccm argon it could be observed with a higher rate. For the measurements presented here, the trigger of the oscilloscope was set to glitch mode for peaks faster then 10 ns. The interpretation of these peaks is quite sensitive. To extinguish electrical reasons like low resolution of the applied equipment, a 4 GHz oscilloscope (Tektronix DPO70404B) together with a 2 GHz current probe (Tektronix CT6) were used. The observed current peaks stayed the same. Therefore, we believe the peaks to result from plasma activity under very sensitive, external conditions. 4. Discussion Figure 4 shows electrical current oscillations with a repetition frequency from 250 down to 75 MHz. This range of repetition frequency was measured for several series. Meanwhile the peak amplitudes range from 4 down to 0.5 mA, decreasing with time. st 21 International Symposium on Plasma Chemistry (ISPC 21) Sunday 4 August – Friday 9 August 2013 Cairns Convention Centre, Queensland, Australia One possible explanation for a plasma caused oscillation in this frequency range is the presence of ion acoustic waves. Within some discharges, the system seems to generate resonance conditions for an ion acoustic wave. While their observation in low temperature plasma discharges was done under quasi static conditions with nearly no damping, atmospheric pressure with great damping constants has to be considered here. Until now, the observation is rarely reported and the aspect of save electrical setups not discussed [5]. For our experiment, we assume the observed pulse repetition frequency to be the ion plasma frequency f pi 1 e² n 2 m (1) i 0 i where e is the elementary charge, ni the ion density, ε0 the dielectric permittivity and mi the ion mass. Argon is assumed to be the dominant ion in these calculations. By measuring the times between the oscillation maxima in figure 4, it is thus possible to analyze the time dependence of the plasma ion frequency and therefore the ion density. In the moment of maximal discharge current, the discharge gap is bridged by a glow discharge like structure [2]. Therefore the plasma is considered to be a conducting channel with a diameter of 60 μm. The current density is proportional to the electron density with (e – elementary charge and c – speed of light): I A e n c (2) e An electron density of 1.18 * 1012 cm-3 is calculated. To evaluate the current peaks in the decay slope, the velocity in equation (2) is exchanged by the drift velocity of the electrons: I A en v en E 1 I (t ) E (t ) (3) e A n (t ) e d ,e e e e e The electron mobility in argon is taken from [6] (Nair=2.44*1019 cm-³ at 300°K): μe=613 cm²/Vs. For the current peaks, the underground created by the main discharge current is subtracted from the current peaks. Based on the assumption of quasi neutrality, the electron density in equation (3) is equal to the ion density from equation (1). Observed current oscillation amplitudes as well as the results from equation 1 and 3 are shown in figure 5. The current signal shows an increase at the beginning before it decays from 3 mA to 0.6 mA. The increase of the peak values at the beginning indicates the build up of the ion acoustic wave. After the maximum value, the current value decreases, especially through collisions and diffusion. The argon ion density decreases with the oscillation frequency (equation (1)) exponentially from 5*1013 cm-3 Fig.5: current value of the peaks in the decay phase (rectangular), calculated argon ion densities and electrical field strength according to equation (1) and (3) down to 2*1012 cm-3. The values for the ion density are one order of magnitude higher then the calculated electron density from equation (2). This great difference is explained by the uncertainty of the filament cross section. The used diameter value is evaluated from pictures of the whole discharge (some μs accumulation), while the peaks in the decay phase occur directly after the transient spark breakdown and the created species could not diffuse that far in that short time. Therefore, the diameter of the filament will grow in time by diffusion, as will be discussed later on. From the value of current peaks and densities in figure 5, the electrical field strength is calculated according to equation (3). It shows an increase from 5*103 V/cm up to 15*104 V/cm. Such high values as well as the rising tendency are illogical. A voltage of -6.1 kV was applied over the gap width of 8 mm, hence an electrical field in the order of 8*103 V/cm and a decreasing slope were expected. Again the diameter of the filament was set to a fix value, creating a possible source of error. To account for the radial diffusion in the time scale observed in this investigation, the equation of motion for the ions is solved. The equation of continuity, mass flux and charge balance were involved. For our experiment the filament is assumed to be cylindrical. The radial electrical field is neglected as well. We get: n (n v) 0 t j ( n b E D n ) D n V e / (n n ) 0 e e 0 i e e The solution of this set of equations is: n(t , r ) n exp( t / t ) B 1 /(t D ) r (4) 0 0 0 0 e where B is the Bessel function of the first kind with the root at 1 /(t D ) r 2.405 (5) 0 e 0 st 21 International Symposium on Plasma Chemistry (ISPC 21) Sunday 4 August – Friday 9 August 2013 Cairns Convention Centre, Queensland, Australia The value of the diffusion constant De is accessible from the Einstein relation De=Ue*μe. The electron energy Ue is set to 2 eV. For each time step t, t0 was set to the time, when the exponential decay reaches 1/100 of its start value, with: ln( n / n ) ln(1 / 100) 4.6 t / t t t / 4.6 (6) 0 0 0 Therefore it is possible to get the time dependend increase of the filament radius based on diffusion alone. A second aspect will add up from the radial electrical field component, which is neglected for now. Equation (6) inserted in equation (5) gives r (t ) t D / 4.6 2.405 (7) 0 e For t = 100 ns, an increase of the filament radius about 112μm is calculated. Considering the radial expansion for each instant of a current peak allows the recalculation of electrical field strength according to equation (3). The result is shown in figure 6. Electrical field values around 6.3 kV/cm are calculated. This range is within the expectations. Furthermore, the electrical field strength stays almost constant over the whole range (if the first two values of the data-set are omitted). 5. Conclusions Investigations concerning high frequency oscillations of the discharge current are presented. One source of oscillation are voltage probes. It was found, that ground loops create high frequency oscillations. Therefore special care has to be taken for high sensitive current measurements. An improved setup with only a current probe proved to be sensitive and free of ground loops. This setup revealed weak current oscillations of 3 mA amplitude in the decay phase of a transient spark discharge, where current peaks of typically 200 mA had been observed. The oscillation repetition frequency decreases from 250 down to 75 MHz. This is within the range of the plasma ion frequency. The propagation of an ion acoustic wave within the remaining discharge channel is proposed. From the observed oscillation frequency and the current amplitudes, the electrical field strength and the argon ion density is calculated. Diffusion processes are considered to describe the growth of the discharge channel during the decay of the main discharge peak and to improve the electrical field strength calculations. The presence of ion acoustic waves, despite high collisions at atmospheric pressure, leads us to reasonable results for the argon ion density and hence electrical field strength. 6. Acknowledgements The authors are grateful to P. Holtz for providing practical assistance. This work was realized within the framework of the multi-disciplinary research cooperation, ``Campus PlasmaMed'', supported by German Ministry of Education and Research (BMBF, grant no, 13N11188) which is gratefully acknowledged. Fig.6: calculated electrical field strength according to equation (3) under consideration of radial diffusion (equation 7) This finally shows, that an evaluation based on the ion acoustic wave interpretion gives plausible results. The electrical field strength as well as the argon ion density calculations are within reasonable scales. Furthermore we would like to point out, that smaller peaks with a second frequency were observed, but the evaluation of these signals was not possible until now. 7. References [1] Th. v Woedtke et al, Phys. Rep, (2013) DOI: 10.1016/j.physrep.2013.05.005. [2] T. Gerling et al, J. Phys. D: Appl. Phys., 46, 145205 (2013) DOI: 10.1088/0022-3727/46/14/145205 [3] R. Bussiahn et al, Appl. Phys. Lett., 96, 143701 (2010) DOI: 10.1063/1.3380811 [4] M. Janda et al, Plasma Sources Sci. Technol., 20, 035015 (2011) DOI: 10.1088/0963-0252/20/3/035015 [5] B. Qi et al, Phys. Plasma, 18, 083302 (2011) DOI: 10.1063/1.3622632 [6] S. Pfau and A. Rutscher, Annalen d. Physik, 22, 166 (1969)
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