22nd International Symposium on Plasma Chemistry July 5-10, 2015; Antwerp, Belgium Precise calorimetric measurements in dielectric barrier discharges (DBD) at atmospheric pressure M. Archambault-Caron, H. Gagnon, B. Nisol, K. Piyakis and M.R. Wertheimer Polytechnique Montréal, Groupe des Couches Minces (GCM) and Department of Engineering Physics, P.O. 6079, Station Centre-Ville, Québec, H3C 3A7, Canada Abstract: A special dielectric barrier discharge (DBD) cell has been used to carry out precise measurements of electrical energy, πΈg , dissipated per a.c. voltage cycle in helium atmospheric pressure glow discharges (APGD). Aided by multiple thermometric probes, a surprisingly accurate energy balance has been achieved, to our knowledge, for the first time. Keywords: helium APGD, discharge energy, thermometry, energy balance 1. Introduction The cold nature of atmospheric-pressure (AP) dielectric barrier discharge (DBD) plasmas is of key importance when they are put to use in many of their current applications, for example in biomedical (therapeutic) contexts [1, 2]. We refer to recent work by Wertheimer et al.[3], where they confronted their own and other workersβ gas temperature (π) measurements carried out by optical emission spectroscopy (OES) with π measurements based on the use of fiber-optic thermometers. The latter were developed for use in conditions involving high voltages and/or intense electromagnetic fields, where conventional (e.g., thermocouple) instrumentation should be disqualified. Surprisingly, even to this day, only a few workers in plasma processing science use fiber-optic thermometers, even though it was clearly shown that π based on OES invariably overestimates the true gas temperature, often very grossly [3, 4]. Beside knowledge of π, it is also clearly important for the operator of a (AP) plasma system to know the exact amount of electrical power, π, delivered to the plasma and hence to a substrate. In this present work, a specially designed dielectric barrier discharge (DBD) cell has been used to carry out precise measurements of electrical energy, πΈg , dissipated per discharge cycle of the applied a.c. voltage, V a over the frequency range 5 β€ π β€ 50 kHz. Twin pairs of several different dielectric materials (2.54 cm diameter discs, thicknesses = 2.0 or ca. 0.1 mm with relative permittivities between 2.1 β€ πΎ β² β€ 9.5) were used as dielectric barriers in DBDs of four different gases: He, Ne, Ar and N 2 . Much of this research, the part that is reported in this presentation, relates to the study of atmospheric pressure glow discharge (APGD) plasma in flowing helium; five separate thermometers (including two fiber-optic probes in sensitive locations) have enabled us to perform a detailed calorimetric (heat balance) investigation in He APGD, believed to be the first of its kind. R O-9-4 2. Experimental Methodology Fig. 1 shows a schematic diagram of the DBD cell, thermometric and electrical probes, and other associated components. The discharge chamber is an hermetic Pyrex glass cylinder (inner diameter = 32 mm) with metallic end plates, connected to a gas supply and flow-control unit with which gases can be maintained at a constant flow rate, πΉ (in liters per minute, L/min), slightly above atmospheric pressure. Small holes in the Pyrex vessel wall permit insertion of thermometric probes at appropriate locations, namely in the discharge gap (πplasma ) and in the effluent gas stream (πgas ). The two fiber-optic thermometric probes (OpSens Inc., model OTG-F, Quebec City, Canada) in these two critical locations were based on the T-dependence of the optical band gap of GaAs. The reader is referred to a recent article by Gagnon et al. [5] for information about the electrical measurement system, and some of the details about the refined algorithms that permit rapid data acquisition and processing. Ttop Gas out HV probe Oscilloscope Gap LV probe PC Tgas Tglass Tplasma Telec 50 β¦ Gas in Metal Dielectric Micrometer T Thermocouple screw T Optical Fiber Probe Fig. 1. Schematic diagram of the DBD cell, thermometric and electrical probes, and other associated components. 1 3. Results, Discussion and Conclusions Calorimetric calculations have been carried out on the basis of T measurements accumulated at ½-minute intervals by the five thermometric probes during a He APGD experiment at f = 50 kHz, V a = 780 V rms that lasted for 20 minutes, and during which E g was found to remain rigorously constant at 18.3 ± 0.2 µJ per period of the applied a.c. voltage. For these experiments, the gas entered at the bottom of the reactor at a flow rate, πΉ, of 3.1 L/min and ambient (laboratory) temperature, π = 295 K. The plasma temperature, T plasma , was found to be a maximum of 5.5 K above ambient, i.e., merely 300 K. This stands in striking contrast with OES-based values that are reported to be at least 360 K, several tens of K higher [4]. Power delivered by the plasma, π1 , at 5 × 104 periods per second, was π1 = 18.3 × 10β6 × 5 × 104 = 0.915 W. The energy budget corresponding to an arbitrarily chosen time, π‘ = 1000 s (16.7 min) is represented by the vertical line in Fig. 2, where the cumulative value of electrical energy dissipated was πΈ1 = π1 × π‘ = 915 J. The five thermometers permitted the various energy components E 2 to E 5 to be calculated and this, in turn, allowed the following overall energy balance to be performed: β πΈπ = πΈ2 + πΈ3 + πΈ4 + πΈ5 = 66.7 + 415.6 + 230 + 190 = 902.3 J; βπΈ = πΈ1 β β πΈπ = 12.7 J. In Fig. 2, the lowest (Energy Balance) curve representing βE reveals that the astonishing (+1.5%) numerical agreement was coincidental. Nevertheless, even the largest deviation (βπΈ/πΈ1 ~ -20%) was small enough to confirm that the procedure and results were on sound footing. We do not have the space here to go into further details regarding Fig. 2, but these will be reported in detail elsewhere [6]. In that same pending report, we show that E g depends on the energy stored in the DBD cellβs capacitance, C, where Fig. 2. Plot showing the various contributions to the overall energy balance, βπΈ = πΈ1 β β πΈπ , versus time. The lowest curve represents βπΈ. 4. Acknowledgements The authors are grateful for financial support from the Natural Sciences and Engineering Research Council of Canada (NSERC), namely research grants to M.R.W. and an undergraduate research scholarship to M. A.-C. Financial support was also provided by the Fonds de recherche du Québec β Nature et technologies (FRQNT) via Plasma Québec. Skilled technical help by Yves Leblanc and Francis Boutet is also gratefully acknowledged. The authors thank Dr. Claude Hudon (Hydro Quebec Research Institute, IREQ) for loan of the OpSens thermometers. R πΆ= and πΆdie πΆgap πΆdie +πΆgap = πΈ = β« πππ = π0 π΄πΎ β²πΎ1β² (1) πΎ β² π+πΎ1β² π· 1 π0 π΄πΎ β²πΎ1β² οΏ½ 2 πΎ β²π+πΎ1β² π· οΏ½ π2 (2) Eqs. (1) and (2) pertain to a planar DBD cell of area π΄, consisting of a dielectric (thickness π·, relative permittivity πΎβ²) and a gas gap (spacing distance π, relative permittivity πΎ1β² Μ΄ 1.0). We further demonstrate that eq. (2) permits inter-laboratory comparisons to be made, which have revealed good agreement with power data presented by other authors for He APGD [7, 8], and which enable scale-up of reactors. 2 5. References [1] G. Fridman, G. Friedman, A. Gutsol, A.B. Shekhter, V.N. Vasilets, A. Fridman, Plasma Processes and Polymers, 5, 503 (2008) [2] K. Landsberg, C. Scharf, K. Darm, K. Wende, G. Daeschlein, E. Kindel, et al., Plasma Medicine, 1, 55 (2011) [3] M.R. Wertheimer, M. Ahlawat, B. Saoudi, R. Kashyap, Applied Physics Letters, 100, 201112 (2012) [4] A. Berchtikou, J. Lavoie, V. Poenariu, B. Saoudi, R. Kashyap, M.R. Wertheimer, IEEE Transactions on Dielectrics and Electrical Insulation, 18, 24 (2011) [5] H. Gagnon, K. Piyakis, M.R. Wertheimer., Plasma Processes and Polymers, 11, 106 (2014) [6] M. Archambault-Caron, H. Gagnon, B. Nisol, K. Piyakis, M.R. Wertheimer, Plasma Sources Sci. Technol. (submitted) [7] P. Decomps, F. Massines, C. Mayoux, Acta Physica Universitatis Comenianae, 35, 47 (1994) [8] G. Nersisyan, W.G. Graham, Plasma Sources Science and Technology, 13, 582 (2004) O-9-4
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