22nd International Symposium on Plasma Chemistry July 5-10, 2015; Antwerp, Belgium Spatio-temporal diagnostics of dielectric barrier discharges R. Brandenburg1, H. Höft1, H. Toder2, M. Kettlitz1, A. Sarani1, H.-E. Wagner3 and K.-D. Weltmann1 1 Leibniz Institute for Plasma Science and Technology (INP Greifswald), Greifswald, Germany 2 Masaryk University Brno, Brno, Czech Republic 3 University of Greifswald, Greifswald, Germany Abstract: The principles and limitations of methods for the spatio-temporal spectroscopy and the recording of discharge luminosity are summarized. Selected examples on the application of such methods for dielectric barrier discharges in nitrogen-oxygen gas mixtures are discussed. In particular the capabilities of a novel Time-Correlated Single Photon Counting set-up with automatic scanning of spatial discharge coordinate are presented. Keywords: dielectric barrier discharge, streak recording, time-correlated single photon counting, microdischarge, microplasma 1. Introduction Many plasmas, in particular those operated at atmospheric pressure are often transient, small scale and of short duration [1]. Dielectric barrier discharges (DBDs), corona discharges and plasma jets are typical examples of filamentary plasmas with irregular appearing distinct discharge channels. They obtain strong gradients in local plasma parameters that can be affected by instabilities. Its key parameters and important species must be studied with sufficient spatial and/or temporal resolution, accordingly. Depending on the plasma source and the operating conditions a resolution down to the submm and sub-ns range is desired. Special techniques are required which will be summarized and d emonstrated on selected examples in this contribution. In particular a novel time-correlated single photon counting system will be presented. 2. Methods and methodology The principal approach to study filamentary plasmas is to study the most fundamental element, the single filament or microdischarge. To generate localized and repetitive filaments special electrode arrangements with pin-electrodes or semi-spherical dielectric bodies can be used. To study the morphology and development of single discharge channels in principle three methods are available: gated intensified charge coupled device (ICCD) cameras, streak cameras and time-correlated single photon counting (TC-SPC) based cross-correlation spectroscopy (CCS). ICCD cameras allow photography by means of image intensification using a micro-channel plate before CCD detection. For temporally resolved studies the microchannel plate can be gated down to 1 ns, (some modern ICCD cameras even reach 100 ps). To resolve the spatial structure of individual discharge channels it can be magnified by lens systems, far-field microscopes or classical microscope. ICCD cameras are limited by their read-out times. Temporally resolved studies must be IN-09 done by investigation of subsequent discharge events with variable gating with respect to a defined trigger event. Thus, spatio-temporally resolved studies by ICCD cameras are typically limited to discharges with a defined inception in time such as pulsed driven discharges. Multichannel or framing ICCD cameras enable the recording of few (usually up to eight) images for one discharge cycle, but a limited number of recordings is often not sufficient to describe the discharge development as a whole in detail. ICCD cameras which can be operated in stroboscopic regime overcome read-out time limitations and reach time resolutions of about 80 ps [2, 3]. Stroboscopic images are well suited if nonreproducible discharges that propagate in multiple directions (e.g., branching streamer in corona discharges) are studied. Streak cameras enable to resolve the spatio-temporally development of the luminosity of discharges along a chosen dimension (usually the discharge axis). Optoelectronic streak cameras transform the temporal profile of a light signal into a spatial profile on the CCD array by causing a time-varying deflection of the photoelectrons which are generated at a photocathode and intensified by a microchannel plate before CCD detection. In principal streak camera imaging is the only method which enables the spatio-temporally resolved study of single or individual discharges with high resolution (down to 50 ps) in one exposure [4]. Streak cameras need to be triggered similar to ICCD cameras. If the discharge event is well localized and reproducible, the accumulation over many events can be performed with a reasonable accumulation time. Even irregular appearing discharge events can be accumulated by using the so-called jitter correction function. For the temporally resolved optical emission spectroscopy of pulsed operated discharges with low inception jitter (e.g., nanosecond pulsed discharges between two steel pin electrodes operated with a high voltage with rise/fall times of 5 ns) a triggered 1 photomultiplier with sufficient rise time at the monochromator exit can be used [5]. In this case a trigger generator is controlling the high voltage device and the photomultiplier. However, the synchronization between the discharge event and the detection system (ICCD camera, spectrometer) cannot be provided by an external trigger generator in case of irregular or self-pulsing discharges. In such cases the current pulse of the discharge can be used to trigger the detection unit [6]. Such methods are limited due to delay and transmission times of cables, electronics and detection system, which can be overcome by an optical delay of the emission. However, this results in a complicated optical system and a weak signal. The cross-correlation spectroscopy (CCS) is the most sensitive technique for the spatio-temporal and spectral resolved recording of irregular single discharge channels. It was first applied to corona discharges and independently on these studies Kozlov proposed this method for the investigation of single DBDs. The CCS method substitutes the real-time measurement of discharge events by the statistically averaged determination of a cross-correlation function between two optical signals, both originating from the same source [7]. One of these is used to define a relative time scale (synchronizing signal) while the second one is consisting of single photons that are spatially and spectrally resolved (main signal). The measured quantity is the time delay between these two signals, which is determined by the TC-SPC module. Consequently, a time histogram of counted photons for all positions is accumulated (technical time resolution about 12 ps), which is the probability density function for the light pulse luminosity evolution. If the repetitive light pulses reproduce each other sufficiently exact, and if the synchronization signal detection is adjusted in such a way that it occurs always at the same moment of a single light pulse evolution, then the recorded probability density function is proportional to the light intensity of the source. CCS provides a method for the accumulation and thus averaging over a great number of elementary events by the measurement procedure itself. Therefore it requires a high reproducibility and long-time spatial stability of the repetitive discharge events and is therefore very time consuming. A similar method was realized in [8] by means of photomultipliers connected to an analogue–digital recorder and digital oscilloscopes. The oscilloscopes and recorders were triggered by current pulses measured by fast current probes. Within recent years we used ICCD imaging, streak camera and CCS simultaneously together with electrical diagnostics to the same discharge configuration. The developed methodology is shown in Fig. 1. The current pulse measurements and the ICCD camera imaging were used to provide information about the current duration and amplitude, mean current density, discharge morphology but also on the reproducibility and 2 Fig. 1. Used methodology of the investigation of single discharges in DBD arrangements. spatial localization of discharge channels. If this criteria was fulfilled the accumulation of streak camera images could be performed. The streak recording was used to yield only information along the discharge channel but has the advantage of short accumulation times (usually in the range of several seconds to minutes) which are favourable if systematic measurements for variation of several process parameters are necessary. CCS is even more sensitive, offers a larger dynamic range and enables higher spectral resolution. However, the accumulation of single photons for many different positions can be very time consuming. Therefore, CCS is more appropriate for a more detailed investigation of specific aspects of discharge development (see section 3) for selected conditions. Furthermore, CCS is mandatory in case of erratically appearing discharge events with a large jitter of discharge inception (e.g., sinusoidal operated DBDs). To get a two dimensional development the discharge can be scanned in spatial coordinates (radial and axial along the discharge channel). 3. Selected examples The first example demonstrates the prospects of the methods and the methodology in Fig. 1 itself. The discharge being investigated is shown in Fig. 2a. Single repetitive discharge channels are generated in a symmetric electrode arrangement with semi-spherical electrodes [9]. The dielectric is alumina (Al 2 O 3 ) with a thickness of about 0.5 mm. The minimum distance between the electrodes amounts to 1 mm. The electrodes can be flushed with defined gas mixtures in a discharge cell. Electrical measurements (current and applied voltage) are performed with fast probes and recorded with a digital sampling oscilloscope [9]. The current probe is directly embedded in one of the electrodes which reduce stray capacitances and inductances. The measured current and voltage are shown in Fig. 2c. A rectangular voltage with IN-09 Fig. 2. Investigation of rectangular pulsed single discharges in N 2 with 0.1 vol.% O 2 admixture (a) by means of ICCD camera (b), electrical diagnostics (c), individual (d), accumulated streak camera recording (e), and CCS (wavelength of 337 nm (f)). a rise time of 250 V/ns and amplitude of 10 kV (10 kHz frequency) is applied and the measured current I tot consists of the displacement I dis (which can be obtained from the derivation of applied voltage or measured, when no discharge is ignited) and the plasma induced current IN-09 (obtained by subtraction of I dis from I tot and multiplication with a factors including barrier and total capacitance of the arrangement) [9]. As outlined above the discharges are either investigated simultaneously by ICCD camera and streak camera system by using a beam splitter or by means of CCS. The ICCD camera photo in Fig. 2b is for an individual discharge channel. It expands in the gas gap (diameter about 70 µm) towards the electrodes and spread into several discharge channels on the dielectric surfaces. The streak photo of an individual discharge event (axial coordinate is ordinate, abscissa is relative time scale and number of counted photons/luminosity is colour coded in logarithmic scale) is shown in Fig. 2d. The formation of the bulk plasma in front of the anode and a weak emission at the cathode can be observed, but details of discharge development are obtained only by the accumulation of streak photos over about 103 events (see Fig. 2e). The recording of multiple discharges could be excluded and sufficient reproducibility as well as stability of spatial localization could be confirmed due to current and ICCD measurements. Furthermore, the streak camera system handles a temporal jitter of the discharges in the ns-range (jitter correction function) [10]. The CCS image (Fig. 2f) is for the most intensive emission in the optical emission spectrum at 337 nm (0-0 transition of molecular bands of second positive system of nitrogen). The advantage of CCS is the high sensitivity which is beneficial if studying the weak pre-phase of discharge development or in case of spectrally resolved measurements of weak signals. The example in Fig. 2f shows a pre-phase, which is located at the anode. More precise measurements show that it is about 35 ns long [10] which correlated with the time window between the start of the voltage slope and the inception of the discharge. For sinusoidal generation of DBDs more than 100 ns long pre-phase has been obtained [7]. It is clearly seen in CCS image and streak photo that the cathode directed ionization wave is starting at the anode and reaching a maximum velocity of about 2 106 m/s in front of the cathode. The differences in both plots are most likely due to the fact that the streak image is recorded along the central line of the discharge channel while CCS accumulated over the full width of the discharge channel in this case. In order to reduce accumulation times of CCS measurements a new set-up has recently been developed (see Fig. 3). The recording is based on a multi-dimensional TC-SPC process that records the photon distribution over the time in the discharge emission pulses, the applied voltage, and the position along the discharge gap. Scanning over the gap is performed by a galvanometer mirror and controlled by a scan controller which generates both the scan ramp for the mirror and a sinusoidal signal that is amplified to generate the discharge (sinusoidal operation at about 12 kV pp amplitude and 7 kHz frequency). The photon distribution is built up by the TC-SPC module. 3 Fig. 5 shows the discharge development (resolved along position in the gap and fine time scale) for 337 nm, consisting of pre-phase, streamer phase, bulk plasma and decay. The origin of the weak discharges several 10 ns before the main discharge are still unclear but most probably artefacts of the discharge accumulation caused b several discharge channels per half-period. Fig. 3. Novel TC-SPC set-up with automatic spatial scanning along discharge axis. Fig. 4 shows the integral intensity over the phase of the applied voltage and the position along the gap for a DBD in air. The figure should be interpreted as the mean distribution of photons (and thus discharge events) over the phase and the position. It shows that for sinusoidal operated DBD in symmetric electrode arrangement the discharges are distributed over about one quarter of the voltage period. Each pixel of this image consists of a curve with the temporally resolved emission signal (fine time scale of 50 ns duration). These data are used to compose Fig. 5. Fig. 4. Integral intensity versus phase in sinusoidal high voltage and position along the gap (1 mm) in logarithmic intensity scale. 4. Conclusions The techniques for spatio-temporally resolved imaging and/or spectroscopy of transient and short-living discharge events (e.g., single DBDs) have been presented. Different techniques in simultaneous application on the same discharge configuration offer the possibility to get a complete picture on discharge morphology, reproducibility, localization and development. A new CCS set-up with first results was presented. The set-up provides automatic scanning over phase of the applied voltage and the position along the discharge gap. 5. Acknowledgement Partly supported by the European Union's 7th Framework Programme (Project “PlasmaShape”, 3162169). We are grateful to Dr Kirill V. Kozlov (Moscow State University) as well as Dr W. Becker and H. Netz (Becker & Hickl GmbH Berlin). 6. References [1] P. Bruggeman and R. Brandenburg. J. Phys. D: Appl. Phys, 399, 26 (2013) [2] S. Pancheshnyi, et al. Phys. Rev. E, 71, 16407 (2005) [3] D. Trienekens, et al. IEEE Trans. Plasma Sci., 99 (2014) [4] V. Gibalov and G. Pietsch. J. Phys. D: Appl. Phys., 33, 2618-2636 (2000) [5] D. Pai, et al. J. Appl. Phys., 107, 093303 (2010) [6] M. Janda, et al. in: Proc. 20th Symp. Applications of Plasma Processes (SAPP). (Tatranska Lomnica) IL-06 (2015) [7] K. Kozlov, et al. J. Phys. D: Appl. Phys., 34, 3164 (2001) [8] Yu. Shcherbakov and R. Sigmond. J. Phys. D: Appl. Phys., 40, 460-473 (2007) [9] M. Kettlitz, et al. J. Phys. D: Appl. Phys., 45, 245201 (2012) [10] R. Brandenburg, et al. J. Phys. D: Appl. Phys., 46, 464015 (2013) Fig. 5. Spatio-temporally resolved discharge development of a single DBD in air (at 337 nm). Cathode is top electrode, logarithmic intensity scale. 4 IN-09
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