22nd International Symposium on Plasma Chemistry July 5-10, 2015; Antwerp, Belgium 2D time-resolved measurement and modeling of electric fields associated with atmospheric pressure plasma streams propagation in dielectric capillaries T. Darny1, E. Robert1, F. Pechereau2, S. Dozias1, A. Bourdon3 and J.-M. Pouvesle1 1 GREMI UMR 7344 CNRS / Université d’Orléans, Orléans, FR-45067, France 2 CERFACS, 42 Av Coriolis, FR-31057 Toulouse, France 3 LPP UMR7648 CNRS / Ecole Polytechnique, Palaiseau / Université Pierre et Marie Curie, Paris, France Abstract: This work reports on time-resolved measurement of longitudinal and radial electric fields (EF) associated with plasma propagation in dielectric capillaries. Plasma propagation occurs in a region where longitudinal EF exists ahead the ionization front position usually revealed from plasma emission with ICCD measurement. The ionization front propagation induces the sudden rise of a radial EF component. Both of these EF components have a few kV/cm in amplitude for helium or neon plasmas. Their amplitude is kept almost constant along a few tens of cm long capillary. All these experimental measurements are in excellent agreement with electrostatic and 2D fluid model calculations which are used to infer EF data on capillary axis. Keywords: plasma jet, electric field, ionization wave 1. Introduction While cold atmospheric pressure plasma jets have shown their great potential for many biomedical applications, there still exists a strong need for their diagnostics. Excited and reactive species quantification [1,2], interplay between plasma jets and the carrying gas flow [3,4],interaction of plasma jets with targets of various nature [5], electric field measurement [6,7] are some of the most exciting but challenging topics under study targeting a deeper characterization of plasma properties and potential optimization for relevant applications. This work presents a preliminary non intrusive experimental and modelling analysis of electric fields associated with the generation and propagation of atmospheric pressure plasma streams in dielectric tubes and ambient air. Dealing with electric field diagnostics, several techniques have been already proposed. Shashurin et al. [6] proposed a method based on stopping ionization front propagation with DC potential applied on external metallic ring surrounding plasma plume. Very intense electric field amplitude as high as 100 kV/cm were deduced in [6]. The method may suffer severe limitation for some plasma jets, where the use of metal ring may strongly modify the plasma plume features. Other technique based onStark polarization spectroscopy has been proposed by Ivkovic et al. [7], based on He line and its forbidden counterpart in a helium plane to plane DBD. This optical method is non intrusive and give access to spatial resolution of electric field amplitude in the cathode sheath region. However, homogenous discharge is required, in appropriate pressure range (200 and 800 mbar pressure), and the technique is limited with lower detection rate of 3kV/cm and the only use of helium gases or helium and hydrogen admixture [8]. Authors indicate a good agreement between their O-2-2 experimental value and the usual local electrical field calculates by numerical models in this condition (around 10 kV/cm). A large effort has also been addressed on the development of adequate models likely to give insight for some hard to reach experimental parameters [8-12]. In the present work, we report and analyse first electric field measurements with a new device (bi component EOP Kapteos probe) for the diagnostics of pulsed atmosphericpressure plasma streams inside long dielectric tube, produced by the Plasma Gun (PG). PG is a coaxial dielectric barrier discharge reactor with a quartz capillary, flushed with rare gas and powered, in this work by μs duration voltage pulses in the kHz regime. 2. Experimental Setup Figure 1 shows the experimental setup. A 42 cm long dielectric quartz capillary with a 4 mm inner diameter and 6 mm outer diameter is used. The inner electrode, 2cm long, is set inside the capillary. The rare gas (helium or neon) buffer (1 L/min) is injected through in the inner hollowed electrode (0,8 mm inner diameter). Grounded ring electrode is set on the outer surface of the quartz capillary at the tip of the inner electrode. Some experiments have also been performed with the use of a single HV cylindrical electrode set on the outer surface of the quartz capillary, the discharge reactor being positioned on the axis of a grounded cylinder, 20 cm in diameter, in order to get the best agreement with the model discharge configuration. Data discussed in this work have been measured with a 16 kV peak voltage amplitude applied across the PG powered at a constant 1 kHz repetition rate. 1 usually detected from ICCD measurement or plasma emission optical detection, expanding over a distance of about 5 cm. This was previously revealed from model calculation [9] where the existence of the higher energy electrons was reported ahead the electron density and ionization source function peak position during ionization wave propagation. Fig. 1. PG with the probe set 10 cm downstream from the grounded electrode, 2 mm from the capillary wall. The probe is represented by it space orientation, here allowing Ex and Er measurements. A Pockels effect based fiber-like sensor equipped with an isotropic crystal probed by a laser beam give simultaneous access to two orthogonal components of the electric field. A specially designed 1.75 mm in diameter, 1 mm long crystal embedded in an alumina tube, set at one end of an optical fiber was used as a sensor. The sensor was move along the quartz capillary, with a constant 2 mm gap from the quartz outer surface. This corresponds to a distance between the capillary axis and the crystal center of 6 mm. This 2 mm gap was checked, through ICCD measurement, to induce no detectable modification of the plasma front propagation emission pattern and velocity. Thus, the probe allow for the nonintrusive, non perturbative measurement of the longitudinal (Ex) and radial (Er) EF components. The EF field amplitude necessarily reflects space averaged (1.75 mm3) value while the full detection system affords nanosecond temporal resolution. 3. Results Figure 2 presents the voltage pulse and the temporal evolutions of longitudinal and radial EF for the probe set 10 cm downstream from the inner electrode tip. For this probe position, the peak longitudinal EF amplitude, 5 kV/cm, is measured with an 1800 ns delay from the voltage onset. This delay should be assigned to the combination of the discharge production delay around 4 kV applied voltage and the consecutive plasma propagation along the first 10 cm path. For the helium buffer and a 16 kV amplitude, the mean velocity of the plasma is around 107cm/s, inducing a 1 µs delay for 10 cm long plasma propagation. One can note that the EF probe detects longitudinal EF increase about 500 ns before the 1800 ns peak. This indicates that there exists a significant longitudinal EF ahead the ionization front 2 Fig. 2. Ex and Er time evolutions for the probe set at the 10 cm position. The time evolution of the voltage pulse is also superimposed on the graphic. Helium buffer is used. Figure 2 also indicates the sudden rise of an intense radial EF component, presenting a very sharp rising front and appearing almost synchronously with the peak of the longitudinal EF component, i.e. around 1800 ns for the present experimental conditions. The rise of such radial component following the ionization wave propagation was also reported in [9] where EF was shown to essentially consists in a radial component all along the ionization channel following the ionization front while a rather extended region where longitudinal EF component predominates ahead the ionization front. At longer delays, the probe detects the EF associated with the combination of the electric field imposed across the PG electrodes, and the EF induced through the plasma column following the ionization front. The voltage applied to this plasma column is controlled by the voltage applied across the PG. Equipotential line calculation have been performed using Comsol multiphysics® for two situations corresponding first, to the start of the ionization wave propagation and second, after an 8 cm long ionization front propagation. In this rough calculation, constant voltage of 10 kV in amplitude is applied on an on axis 2 mm wide HV electrode. Ground potential is imposed in a cylindrical region 1 cm high, 2 mm wide, mimicking the PG ground electrode. The plasma column is considered as an equipotential downstream extension of the HV electrode. As awaited, the electric field is basically longitudinal ahead the ionization front, while following plasma propagation, the plasma column induces an almost radial EF pattern, in agreement with results in fig.2. This confirms the role in high potential extension of O-2-2 the plasma column in between the ionization front and the discharge reactor. Fig. 3. Equipotential line patterns at the beginning of plasma propagation (top) and after an 8 cm path (bottom). Color scale ranges from 0.1 to 10 kV (applied voltage). Both the longitudinal and radial EF measured 6 mm from the capillary axis, exhibit amplitudes of a few kV/cm with no direct relationship with the electric field imposed across the PG electrodes, this latter being essential intense in the electrode zone and quite undetectable a few cm away from this region without plasma propagation. This confirms that transient intense electric field could be delivered a few tens of cm away from the DBD reactor and may play a critical role for biomedical applications. Figure 4 presents the longitudinal and radial EF for different downstream distances from the HV electrode tip for helium and neon buffer gases. At a first glance, the EF components behaviour and amplitude are close for the two rare gases. The faster propagation of neon plasma is confirmed by the sooner appearance of the EF components for the same downstream positions (10 or 25 cm). Sudden rise of radial EF holds true for neon plasma which exhibits slightly higher EF amplitudes and shorter duration and rising front partly associated with the faster propagation velocity in front of the EF probe. The measurements in long tubes for neon plasma indicate that the EF amplitudes are almost constant along a few tens of cm propagation, in agreement with previous calculation [9]. This confirms the specific nature and peculiar interest of plasma streams generated in confined dielectric tubes, having the ability to preserved most of plasma parameters along very long distances. O-2-2 Fig. 4. Ex and Er time evolutions for different downstream probe positions with helium (a) and neon (b) buffer gas. New calculations and experiments have been performed with a specific attention for plasma propagation analysis and associated electric fields properties. Figure 5 presents the experimental EF measurements obtained with the single outer HV electrode PG configuration and their comparison with the results of a 2D fluid model [12] in the same setup. An excellent agreement is observed concerning the time evolution of the EF components, the calculation also confirms the sudden rise of the radial EF following ionization wave propagation. A good agreement is also found concerning the EF amplitudes, confirming that radial peak amplitude is higher than the longitudinal one. Considering the already achieved good simulation of the experimental ionization wave propagation and EF nature, model has been used to infer the on axis EF. Figure 6 presents such on axis longitudinal EF evolution along the axis of the quartz capillary. Besides the electric field induced in the electrode region, an intense (9 kV/cm in amplitude) longitudinal component is generated presenting some ahead extension over distance of a few cm. 3 Fig. 5. Experimental (top) and 2D fluid model calculation (bottom) of Ex and Er in the single electrode PG configuration. The probe was set 3 cm downstream the HV electrode tip, voltage amplitude was 16 kV, helium buffer was used. 0 -1 0 2 4 6 8 10 12 14 16 18 20 Ex (kV/cm) -2 -3 -4 -5 -6 5. Acknowlegments This work is supported by ANR BLAN 093003 PAMPA, APR PLASMEDNORM, TD is supported by MENSR. The authors are grateful to N. Semmar for Comsol calculation implementation, and L. Duvillaret (Kapteos) for EOS probe design and validation. -7 -8 -9 -10 Distance from electrode (cm) Fig. 6. 2D fluid model calculation of on capillary axis Ex profile along a 10 cm long capillary. Discharge propagation from left to right. Work is in progress to extend EF characterization for the plasma plume delivered in ambient air but also over targets relevant for biomedical applications. While the non perturbative setting of the optical probe has not yet been fully demonstrated, preliminary measurements indicate first that EF having peak amplitudes in the range from 10 to 20 kV/cm are detected in the plasma plume, and second, that EF amplitudes around 1kV/cm persists below 3 mm thick tissue layers. 4. Conclusion Time-resolved experimental non intrusive and non perturbative measurement of longitudinal and radial electric field components associated with helium and neon atmospheric pressure plasma propagation in long 4 dielectric tubes has been achieved using a new probe based on Pockels effect. Peak voltage amplitudes of a few kV/cm have been measured for both components a few mm apart from capillary axis, for both rare gas buffers. The experimental measurements reveal that plasma propagates in region where an intense longitudinal component exists a few cm ahead the ionization front usually revealed by strong plasma emission in optical diagnostics. Correlated with the ionization front propagation, the extension of a plasma tail connecting this latter with the powered electrode of the plasma jet device, induces the sudden generation of an intense radial electric field component. These observations are in good agreement with electrostatic calculations and confirm that electric field amplitudes are almost constant along the full plasma propagation over distances of a few tens of cm. Calculations with a 2D fluid model, in a configuration very close to the experimental setup and including the temporal evolution of the voltage pulse delivered across the discharge reactor, indicate very good correlation of the electric field temporal profiles, electric field amplitude and allow inferring electric field on capillary axis. On axis longitudinal and radial electric field amplitude around 10 kV/cm have been obtained inside helium fed capillaries while electric field amplitude in the plume region ranges from 10 to 20 kV/cm, in our experimental conditions. 6. References [1] S. Iseni et al New Journal of Physics16 123011 (2014) [2] S.Hubner et al J.Phys.D :Appl Phys. 47 432001 (2014) [3] E. Robert et al. Plasma Sources Sci. Technol. 23 012003 (2014) [4] S Zhang et al J. Phys. D: Appl. Phys. 48 015203 (2015) [5] S. Bornholdt et al Eur. Phys. J. D10.1140/epjd/e201000245-x (2010) [6] A.Shashurin et al Plasma Sources Sci. Technol. 21 034006 (2012) [7] B M. 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