2212 IEEE TRANSACTIONS ON PLASMA SCIENCE, VOL. 43, NO. 7, JULY 2015 Nanosecond-Resolved Discharge Processes Revealing Detailed Mechanisms of Nonequilibrium Atmospheric-Pressure Plasma Jet of Helium Nan Jiang, Xianjun Shao, Guan-Jun Zhang, and Zexian Cao Abstract— Nanosecond-resolved photographs of the nonequilibrium atmospheric-pressure plasma jet of helium, generated with the conventional dielectric barrier discharge device, were obtained at different sections of the experimental setup and at different development stages of the discharges, showing that various distinct mechanisms are simultaneous in operation. The streamer from the outer edge of active electrode sitting at downstream side forms a jet in air, which only turns out to be hollow when approaching the orifice of the gas conduct. The streamer from the inner edge temporally lags behind, and it propagates along a helical path and initiates the glow discharge when arriving at the ground electrode. The electron deposit beneath the active electrode expands inward from both sides, displaying a soliton-like behavior; while the very compact ion deposit beneath the ground electrode, a typical ionic streamer, extends outward from the inner edge of the electrode. The velocities of the jet in air and of the streamer between electrodes are much larger than those at other parts of the device. The resolution of these particular processes and features can improve the implementation of this valuable cold plasma source. Index Terms— Atmospheric-pressure plasma jet (APPJ), dielectric barrier discharge (DBD), helium, streamer. I. I NTRODUCTION T THE beginning of 1990s, Koinuma et al. [1] devised an equipment that could generate a microbeam plasma, and thus initiated the subsequent research of the nonequilibrium atmospheric-pressure plasma jet (APPJ). Many similar devices have since then been designed, aiming mostly at the implementation of this intriguing cold plasma source [2]. Teschke et al. [3] found with the help of an intensified charge-coupled device (ICCD) that the plasma plumes, A Manuscript received July 12, 2014; revised October 2, 2014; accepted April 1, 2015. Date of publication June 23, 2015; date of current version July 7, 2015. This work was supported in part by the National Natural Science Foundation of China under Grant 10904165, Grant 11290161, and Grant 51172272, in part by the National Basic Research Program of China under Grant 2012CB933002, in part by the Knowledge Innovation Project through the Chinese Academy of Sciences, and in part by the China National Fund for Distinguished Young Scientists under Grant 51125029. N. Jiang and Z. Cao are with the Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China (e-mail: jiangnan@iphy.ac.cn; zxcao@iphy.ac.cn). X. Shao and G.-J. Zhang are with the State Key Laboratory of Electrical Insulation and Power Equipment, Xi’an Jiaotong University, Xi’an 710049, China (e-mail: shaodbd@gmail.com; gjzhang@mail.xjtu.edu.cn). Color versions of one or more of the figures in this paper are available online at http://ieeexplore.ieee.org. Digital Object Identifier 10.1109/TPS.2015.2419639 there comprise a train of bullets. Since then, many reports on the characterization of such plasma bullets, essentially as guided ionization waves, have been published [4]–[13]. In 2009, Jiang et al. [14] pointed out that the nonequilibrium APPJs generated with the apparatus used by Teschke et al. [3] actually comprise three, instead of two, distinct zones and that the plasma in each of the three zones arises from a different mechanism. At that time, the observation was made using two photoelectron multiplier tubes to measure the optical emission from different positions on the path of gas flow, and the conclusion was arrived by comparing the initial moments of light emission from some specific positions [14]. In due time, a temporally resolved photography was successfully applied to investigate the formation and development phases of plasma bullets, for instance, forward bullet and backward bullet, the latter is also known as return stroke, were identified in a helium atmospheric pressure needle-to-plane discharge [15]. The influence of voltage waveform, pulse polarity, and pulse repetition rate has been studied using nanosecond ICCD imaging and plasma-front velocity measurement [16]. In this paper, using an ICCD, the observations in our previous publication [14] are confirmed in a straightforward manner, and more details concerning the nonequilibrium APPJ of helium, especially the seeding process revealed to a resolution of nanosecond, are provided. These results can help illuminate the true mechanisms governing the discharges, and also the dynamics involved, in distinct parts of this very useful cold plasma source. II. E XPERIMENT The setup for the generation of nonequilibrium APPJ is similar to that used in [3], and has been described in our previous publications [14], [17]. Briefly, high-purity (5N) gas of He was introduced at a flow rate of 3.0 L/min into a quartz tube with an outer diameter of 4.0 mm and an inner diameter of 2.0 mm. The two electrodes, made of either a 50 μ-thick copper foil or a net of metal nickel with a transparency of 90% wrapping the quartz tube, are both 2.0-cm wide and separated for 2.0 cm, with the outer edge of the electrode at the downstream side being 1.0 cm away from the orifice of the quartz tube. The electrode at the upstream side was grounded, and the one at the downstream side was connected 0093-3813 © 2015 IEEE. Personal use is permitted, but republication/redistribution requires IEEE permission. See http://www.ieee.org/publications_standards/publications/rights/index.html for more information. JIANG et al.: NANOSECOND-RESOLVED DISCHARGE PROCESSES REVEALING MECHANISMS OF NONEQUILIBRIUM APPJ OF He 2213 Fig. 1. Characteristic curve of discharge current of the nonequilibrium APPJ of He generated with the electrode configuration of the DBD drawn against the applied voltage. Applied voltage: 3.2 kV. to a power supply operated at 17 KHz (the period measures ∼58.82 μs). The discharge current and the applied voltage were monitored using an oscilloscope (Tek4104): the voltage was directly measured using a HV-probe (Tek, P6015A), while the discharge current was obtained by measuring the voltage on a resistor Ri = 100 connecting the ground electrode to the ground [14, Fig. 2]. The device was photographed using a digital camera (Canon 5DII) and the discharges, both inside the quartz tube and outside in the air, were dynamically resolved using an ICCD system (PI-Max II, Princeton Instruments). For taking the side-view photographs for the discharge inside quartz tube, the gate time of ICCD was set, with deliberately chosen delay times, with regard to the zero time that corresponds to the moment of appearance for the onrising front of the discharge current (Fig. 1). The ICCD has a low resolution (512 × 512 pixels), and thus to raise the resolution of the photographs, the whole setup was photographed in five sections, and the results were then synthesized into one picture using Photoshop without introducing any other alteration. The sectional images of the plasma jet in the ambient were taken with the ICCD positioned on the line through the axis of the quartz tube. The discussions here concern with discharges obtained at, but not limited to, an applied voltage of 3.2 kV under which the discharge is very stable. Other working parameters would be specified at proper places. III. R ESULTS AND D ISCUSSION Fig. 1 shows the characteristic curve of discharge current for the nonequilibrium APPJ of helium drawn against the applied voltage, which shows a pronounced peak in the positive half period. The zero time for one period of the applied voltage in the following discussion is set at the onrising front of this positive pulse of discharge current. The gate time for ICCD photographs was also settled this way. In fact, given other parameters, the discharge currents obtained with those voltages that can sustain the discharge are usually unstable. The moment for the appearance of the first pulse (referring to Fig. 2. (a) Six ICCD photographs (pseudo color) in series taken at the moments specified in (b), overlapping the photograph of the device. (b) Characteristic curve of the discharge current in a time interval of 4 μs, with labels showing the gate-ON times for the corresponding ICCD photographs in (a). Exposure times: 10×10 = 100 ns for the ICCD photographs and 0.125 s for the photograph of the device. the phase of the applied voltage) and its intensity are quite random and irregular [18]. This instability at microscopic scale is probably related to some nonlinear processes in this particular kind of discharge; the precise reason for this phenomenon needs be clarified, but it is beyond the scope of this paper. Under some distinct voltages, however, the discharge current can be very stable and the characteristic curve of the discharge current is well reproducible, as the one obtained at 3.2 kV, which is shown in Fig. 1. Thanks to this property, we could obtain ICCD photographs of a stable discharge, which furnishes the basis for the discussion here. Fig. 2(a) shows six ICCD photographs in series showing the plasma bullet moving from the active electrode at downstream side (left) to the ground electrode, overlying on a conventional digital photograph of the whole device. As the discharge process is well reproducible, the taking of ICCD photographs was triggered by the onrising front of a previous positive current pulse, and the first shot occurred at ∼58 μs later. Then with the help of a timing controller (ST-133, Princeton Instruments) a time delay of 20 ns was set to make each next photograph. In the time interval between 58–62 μs corresponding to the development phase of the positive pulse, 200 such photographs had been taken. To achieve a better quality of the photographs, what is presented here is the accumulated record of the ICCD in 10 periods of applied voltage, and thus the total exposure time amounts to 100 ns. We choose six ICCD photographs to present in Fig. 2(a), in which the corresponding triggering moments are labeled with letters a–f on the curve of the discharge current [Fig. 2(b)]. The ICCD photograghs in Fig. 2(a) clearly show the process of the plasma bullet developing on the way from the active electrode to the ground electrode. One sees that the discharge in between the two electrodes is essentially a bulk discharge 2214 instead of a surface discharge [14], [19] as we speculated previously based on the consideration of the device configuration. This is a typical streamer discharge process in helium [16], starting with an almost invisible seed discharge and developing into a discharge channel connecting the two electrodes at the final stage. That this essentially streamer-type discharge appears in average as a bright spot-bullet is termed bullet-streamer dualism [20]. From Fig. 2(a), one can conclude that in between the electrodes, the streamer is initiated at the outer edge of the active electrode, in the neighborhood of the central axis of the glass tube. Here, the discharge is very weak. On the way propagating toward the ground electrode, the streamer head steadily becomes larger and brighter. The clear photographing of this very important, rather the universal process for helium gas discharge has not been reported, to the best knowledge of the authors. From the pictures available in the literature, it is usually impossible to tell assuredly whether the plasma bullet arises from a surfacial discharge or from a bulk discharge [16]. Here, we see that at the initial stage of the discharge in a period of applied voltage, the discharge, being a streamer, is initiated at the inner edge of the active electrode; it develops toward the ground electrode and grows in intensity all the way. The bullet, or strictly speaking, the streamer head, does not propagate along the axis of the quartz tube, rather it whirls around the axis, i.e., the path is helical. This helical path maybe results from the irregularity of the gas flow inside the tube. The disturbance to the gas flow is probably induced by the dielectric barrier discharge (DBD), which essentially is an electrohydrodynamic effect [21]. Fig. 2 reveals only the process of the streamer-triggered discharge in a very short time interval within a period of the applied voltage. When the plasma bullet arrives at the inner edge of the ground electrode, a conducting channel is established between the electrodes, the discharge between the electrodes turns into a glow discharge, and a large discharge current is measured. The DBD is generally more violent than the streamer, which, besides causing a turbulent flow, has an effect on the subsequent discharge in different aspects [22]. The correlation of the streamer path to the turbulent flow pattern is a factor of practical importance for atmospheric-pressure plasma sources [23]. In Fig. 2, the bullet grows larger on the way forward to the ground electrode. This is related to the generation of seed electrons around the bullet initiated by metastable He∗ atoms (see [22] for detailed discussion). The impurity gases lurked into the quartz tube, mainly O2 and N2 , provide seed electrons when ionized by metastable He∗ atoms via the Penning process, since their ionization energies, 12.2 and 15.58 eV, respectively, are much lower those of He [24]. As the He∗ atoms are neutral, their distribution is indifferent to the electrical field, and thus the range of discharge can become larger, and an enlarged diameter of the streamer head results from a weakened electrical field. Consequently, the plasma bullet, whether in helium confined inside the quartz tube or in He/air mixture outside is much slower than the streamers generated in air, of which the typical velocities fall in the range of 106 –107 m/s. This velocity of bullet is a few times lower than the reported values in the literature since here only a IEEE TRANSACTIONS ON PLASMA SCIENCE, VOL. 43, NO. 7, JULY 2015 Fig. 3. Synthesized picture from the ICCD photographs for the whole nonequilibrium APPJ taken on five zones. In particular, zone C is the active electrode on the downstream side and zone E is the ground electrode. Insets: magnified ICCD pictures for the plasma jet in zone B, for the approaching electron deposits beneath the active electrode, and for the ionic wave front beneath the ground electrode. The discharge current and the applied voltage are presented for reference. smaller voltage was applied [16]. The diameter of the streamer in air under a pressure of one atmosphere is estimated to be 0.1 mm [25], but that of the steamer in helium in Fig. 2 is definitely larger than 1.0 mm. The reason for this difference lies in the presence of metastable He∗ atoms in the discharge of helium. To reveal the generation, development, and propagation of the discharges at different parts of the setup, ICCD photographs of the whole device in operation should be obtained. Since our ICCD has only a resolution of 512 ×512, we divided the device into five zones, labeled A–E, namely, zone A is the part outside in the ambient air, zone B is the part from the outer edge of the active electrode to the orifice, zone C is the part over active electrode, zone D is the region between the electrodes, and zone E is the part over ground electrode. The zone-specific photographs were then digitally synthesized (Fig. 3). Under a low voltage of only 3.2 kV, no charge overflow beyond the ground electrode could be observed [21]. From Fig. 3, one notices that in zone A, i.e., in the ambient air, the plasma jet propagates as a bullet with an attenuating intensity and a shrinking size. This is right the plasma jet of interest for application, thus it has been intensively investigated [2]–[6]. Plasma dynamics in a helium jet are probably very similar to the streamer propagation in a dielectric tube filled with helium [26], and the attenuating helium jet in air leads to a shrinking size of the plasma bullet [27]. Jiang et al. [14] pointed out that the plasmas on the two sides of the active electrode are independent from each other, and this will be confirmed in Fig. 3. In the first half period of the applied voltage, it is the outer edge of the active electrode that first triggers a streamer, a feature of the corona discharge. From zones B and C in Fig. 3, one sees that it becomes visible at ∼50 μs. Following Raizer [24], the head of a positive streamer comprises ions. At the same time, the electrons are accelerated toward the temporal anode, now the active electrode, and then deposit on the inner surface of the quartz tube beneath that electrode. The electrons first landed at the outer edge of the electrode and then proceeded forward. JIANG et al.: NANOSECOND-RESOLVED DISCHARGE PROCESSES REVEALING MECHANISMS OF NONEQUILIBRIUM APPJ OF He As electron propagation can induce light emission via excitation and/or ionization of the surrounding gas atoms, we see that the illuminated part develops inward gradually from the outer edge of the active electrode (see zone C in Fig. 3), indicating on the process of electron deposition. The discharge in between the electrodes, i.e, in the so-called DBD zone (zone D in Fig. 3), begins at the inner edge of the active electrode. Its triggering time, a little earlier before the moment of 55 μs, lags behind that initiated at the outer edge of the active electrode for ∼5 μs. This observation is consistent with the simulation [26] and our experimental demonstration that the streamer can be initiated from a single electrode. The streamer from there also induces electron deposition beneath the active electrode, which propagates inward from the inner edge. Thus, we have the chance to observe a very interesting phenomenon in zone C: the deposited electrons beneath the active electrode expand inward from both sides that at some moment later, they finally meet at a position nearer to the inner edge, since the streamer at the inner edge of the active electrode occurs ∼5 μs later. The deposited electrons from the two edges do not merge into a whole; rather they cross each other to continue to propagate forward with their own profiles well preserved, a behavior similar to the interaction of solitary waves of water. More experimental evidences, in conjunction with theoretical considerations [28]–[31], are required to elucidate this phenomenon. Naidis’s simulation [31] of the interaction between two counter-porpagating streamers may provide some hints for further simulation of the situation in Fig. 3. When the streamer from the inner edge of the active electrode arrives at the ground electrode, a conducting channel is formed, and the discharge changes from a streamer to a glow discharge, and the discharge current suddenly becomes large, resulting in a sharp peak (Fig. 1). At the same time, more charges are generated that they deposit beneath the active electrode. From Fig. 3, one observes that the luminescence caused by the charge deposit from the inner edge of the active electrode suddenly becomes very bright and expands toward the outer side very fast. Following this, the jet in the ambient air comes to the farthest end and the electron deposit from the outer edge of the active electrode then becomes weakened and gets slowed down. Clearly, the transition of the discharge in the DBD zone into a glow discharge casts no influence on the jet outside in ambient, or we can say that the streamers from the two edges of the active electrode are mutually independent. First, a few ICCD shots for zone D reflects the process discussed above before the readers are referring to Fig. 2(a). When the head of the streamer arrives at the ground electrode, a spike appears on the discharge current curve. After that, the region near the active electrode immediately turns brighter. Now, a conducting channel is formed between the electrodes and the discharge has turned into a glow discharge. As mentioned before, the negative charges, dominantly electrons, flow to the temporal anode. The positive ions deposit beneath the temporal cathode, currently the ground electrode, and expand inward. At sufficiently large applied voltages, the charge deposition may expand beyond the ground electrode to form a jet outside, which we called an overflow jet [21]. 2215 Fig. 4. Sectional images of the plasma jet in air taken at different distances from the orifice of the quartz tube. The plasma jet shows a hollow structure in the neighborhood of the orifice of the quartz tube. Exposure time: 100 ns. Though we first coined this term, the charge overflow process has already been simulated in [19]. Unlike the jets from edges of the active electrode, here it involves a typical surfacial discharge process. The ICCD photographs in Fig. 3 help us inspect this process more closely. In comparison with those in zone C, the deposition of ions in zone E looks more compact, and the head of the ionic wave can be seen clearly. This is just the difference between the positive streamer and the negative streamer [13], [16], [19]. Fig. 3 shows that the discharges in different zones of the APPJ setup occur at variable moment within a period of the applied voltage. By measuring the positions of the brighter parts, i.e., the streamer heads and charge deposits, the velocities for the discharges at different zones can be roughly estimated. In the ambient air, i.e., in zone A, the maximum velocity, under given conditions, grows to ∼25 km/s at 58 μs and drops to zero at 59.4 μs. The plasma bullet visible in zone B develops to the moment of ∼56.5 μs with the velocity growing to ∼4.4 km/s. This difference is larger than only by twice as observed in a similar device [32]. In zone C, i.e., beneath the active electrode, the situation is a little complicated. The velocity of the deposited charges starting from the outer edge of the active electrode, visible from the moment of ∼50 μs, grows to 4.5 km/s at ∼59.5 μs and then drops to zero within 2 μs, whereas that from the inner edge, measurable at about 58 μs, grows steadily to a value of 2.4 km/s. In zone D, the streamer flies from the active electrode to the ground electrode within 58.1–59.1 μs with a velocity steadily growing to ∼40 km/s. In zone E, the charge overflow is detectable within the time interval between 59.4–64 μs, and the velocity grows to a maximum value of only 8.3 km/s at 60.6 μs and then drops to zero. It should be emphasized again that at the outer edge of the active electrode, the initiation and development of the streamer are quite the same as at the inner edge. The plasma bullet takes form in the neighborhood of the axis of the glass tube, and it flies along the axial line toward the orifice of the tube. It turns into a hollow structure only when it approaches the orifice of the tube (Fig. 4). The plasma jet maintains its hollow structure for a while in the ambient air (within a distance of 18 mm in Fig. 4), and it merges into a solid structure further into the air because of the narrowing helium channel. Evidence of the hollow structure of the jet and its contraction was also acquired by spatially resolved optical emission measurements [27]. 2216 IEEE TRANSACTIONS ON PLASMA SCIENCE, VOL. 43, NO. 7, JULY 2015 IV. C ONCLUSION In summary, the discharge processes occurring in the generation of nonequilibrium APPJ with a DBD device, also in regions beneath the two electrodes, have been resolved to nanosecond and recorded with the aid of the ICCD, which reveals very interesting phenomena concerning the discharge details that can help understand the true mechanisms underlying this intriguing cold plasma source. At both edges of the active electrode, under given conditions, the streamer starts as a weak bulk discharge at the neighborhood of the axis of the quartz tube. The streamer from the outer edge of the active electrode starts earlier, and in approaching the orifice of the glass tube, it turns into a hollow structure due to the invasion of air. After leaving the orifice of the quartz tube, it attenuates in intensity and shrinks its size, but its velocity grows to a maximum value a few times larger than that measured within the quartz tube. The streamer from the inner edge temporally lags behind that from the outer edge, and it propagates along the axis of the gas conduct, growing larger and brighter on the way to the ground electrode to eventually launch the glow discharge. At that moment, a large discharge current peak appears. Electron deposition beneath the active electrode, the temporal anode, occurs from both edges, and the fronts of the electron deposit run across each other like solitary waves of water. Ionic charge deposit beneath the ground electrode, the temporal cathode, looks more compact, and can expand beyond the electrode to form an overflow jet when the applied voltage is sufficiently large. The velocities of the plasma bullet running from the active electrode to the ground electrode, and of the plasma jet running from the active electrode to protrude into the ambient air, are an order of magnitude larger than the propagation velocities of deposited charges beneath the electrodes. 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