Characteristics of Atmospheric Microplasma in Small Discharge Gaps Marius Blajan and Kazuo Shimizu Organization for Innovation and Social Collaboration, Shizuoka University, Japan Abstract: Emission spectroscopy analysis and imaging technique were used to study the microplasma phenomena. The microplasma discharge in Ar and N2/Ar was analyzed along the discharge gap area and also for specific periods of time during the discharge. Microplasma showed characteristics specific with an atmospheric glow discharge: positive column, Faraday dark space and negative glow. Spatial and temporal distribution showed the propagation of light emission from anode towards cathode. The light emission was measured up to 365 ns as long as the discharge current was measured. The intensity of N2 Second Positive Band System (N2 SPS) peak at 337.1 nm was measured along the discharge gap and at various time intervals during the discharge using an effective shutter opening time of high-speed ICCD camera of 3 ns. The peak of Ar I at 696.5 nm was used to estimate the value of electron density using Stark broadening method. The calculated value of electron density ne=1.338x1015 /cm3 is specific for atmospheric pressure nonthermal plasmas. Keywords: dielectric barrier discharge, microplasma, emission spectroscopy 1. Introduction Microplasma applications are ranging from NOx removal to indoor air treatment, sterilization of bacteria or surface treatment of polymers [1-3]. Among nonthermal plasma technologies microplasma has advantages due to its small size of reactor and power supply and the operation at atmospheric pressure. This makes it suitable to be integrated easily with other devices and economical to use. Our microplasma is a dielectric barrier discharge at atmospheric pressure [4]. Analysis of microplasma could be performed by various techniques but due to the small discharge gaps emission spectroscopy and the use of high speed imaging camera is suitable for microplasma analysis [5-6]. This could lead to a better understanding of phenomena and furthermore to a development and optimization of the application processes. 2. Experimental Setup Emission spectra were measured by an ICCD camera (Ryoushi-giken, SMCP–ICCD 1024 HAMNDS/UV) and a spectrometer to which was attached a fiber optic (Fig. 1). Photos of microdischarges were taken using a high speed ICCD camera for imaging (Princeton Instruments, PI-MAX 3). A fiber optic with diameter of about 100 µm was used in order to have an accurate measurement of a small part of the microplasma discharge. A negative pulse Marx Generator was used to energize the electrodes [7]. Experiments were carried out at atmospheric pressure in Ar, N2/Ar. Discharge voltage was negative pulse, rise time 100 ns, width 1 µs at 1 kHz. The pulse width can be varied from 200 ns to 2 µs. Microplasma electrodes are perforated metallic plates covered with a dielectric layer. Due to small discharge gaps (0~100 μm) and to the assumed specific dielectric constant of εr = 104, a high intensity electric field (107~108 V/m) could be obtained with relatively low discharge voltages around 1 kV [1]. The electrode size was 20 mm versus 40 mm. They have holes to flow the gas, with a diameter of Ø 3mm and an aperture ratio of 36%. The discharge gap was set at about 100 μm in our study using a spacer. Microplasma was measured in different points along X axis by varying the position of the fiber optic in 20 µm incremental steps. Figure 2 shows side views of the microplasma electrodes thus X axis was considered to be along the discharge gap. The position of fiber optic was perpendicular on X axis. The position of fiber optic was perpendicular on X axis. Relative intensity of emission peak of the N2 Second Positive Band System (N2 SPS) peak at 337.1 nm was plotted for each incremental step of 20 µm. The opening time of ICCD camera for emission spectroscopy measurements was 15 ns considering rise time and fall time of 6 ns each thus it could be considered that the effective opening time was 3 ns. Fig. 1. An experimental setup. Fig. 2. Electrode arrangement for measuring spatial and temporal distribution of microplasma. Measurements for time incremental steps were performed up to 190 ns considering as the time origin the rise of the discharge current. Images of microplasma were taken using a high speed ICCD camera with an opening gate time of 2 ns, for 200 gates per exposure and 5 ns time incremental steps up to 365 ns. The surface plot depicted in Figure 5 represents only the relative intensities for each time step measurement thus measurement corresponding to one time step could not be compared in term of absolute intensity with other one. The plot shows how the area with highest intensity at a given moment varies inside the discharge gap. Thus it could be observed that at the beginning of discharge the highest intensity was measured near anode and after 25 ns it started to shift towards cathode and back to anode after 130 ns. Dynamics of microdischarge was observed with high speed ICCD camera for microplasma in 1% N 2 in Ar at 1 kV. Trigger signal for ICCD camera was set at 2 ns as shown in Figure 6(a). The trigger signal was set initially at the time when the discharge current started to rise and this was considered as time origin. The time setting was then increased for each measurement. Relative Intensity Scale 0.5-0.55 0.55-0.6 0.6-0.65 0.65-0.7 0.7-0.75 0.75-0.8 0.8-0.85 0.85-0.9 0.9-0.95 0.95-1 190 160 130 100 70 60 50 40 35 30 25 20 15 10 5 0 Cathode Anode Time (ns) 3. Results and Discussion The emission spectrum of the microplasma discharge generated at 1 kV in Ar and 1% N2 in Ar mixture showed high intensity peaks of N2 second positive band system (N2 SPS 315.9 nm, 337.1 nm, 357.7 nm, 380.4 nm) [8] and OH peaks (306 ~ 309 nm) [9] (Fig. 3). For the discharge in pure Ar (purity 99.999%) high intensity peaks corresponding to ArI were measured in the violet and red regions (Fig.4) [10]. The intensity if N2 SPS peak at 337.1 nm was measured along X axis using experimental setup shown in Fig. 2 by varying across X axis with 20 µm incremental steps the position of electrodes versus the fiber optic. Microplasma was generated in 1% N2 in Ar at 1 kV. Fig. 4. Emission spectrum of microplasma discharge in Ar at -1.2 kV in red region. 0 40 80 120 160 200 240 280 Distance X (um) Fig. 3. Emission spectrum of microplasma in Ar and N2/Ar mixture at -1.2 kV. . Fig. 5. Spatial and temporal evolution of the relative intensity for N2 SPS peak at 337.1 nm. (a) 1 ns 2 ns 3 ns 4 ns Anode Cathode 100 µm 10 ns 20 ns 25 ns 35 ns 45 ns 55 ns 100 ns 365 ns (b) Fig. 6. Discharge voltage, corresponding discharge current and ICCD camera trigger signal (a) and spatial and temporal evolution of light intensity (b) during microplasma discharge in 1% N2 in Ar. Images show that with various incremental steps the distribution of light emission in the gap was different suggesting the waves of light intensity that started directly from the anode (grounded) and propagate towards the negative one (cathode) (Fig. 6(b)). The gating of the ICCD camera was set at 2 ns and it was placed in time for the first image at -1 ns thus first image showed the phenomena up to 1 ns. Then the cathode layer development, cathode layer enhancement and cathode layer decay were observed. The initial phenomena of electron avalanche from cathode and the cathode directed streamer are difficult to capture mainly due to the small discharge gap characteristic to our microplasma. The cathode layer development could be observed up to 35 ns. The highest intensity was observed between 35 and 70 ns which corresponded to cathode layer enhancement stage. Finally the post discharge phenomena was observed starting from about 70 ns. Weak light intensity was measured up to 365 ns. This could be due to the long life active species that remained during the afterglow. The discharge gap was about 100 µm but due to the asperities on the dielectric the discharge gap could vary. The asperities on the dielectric could favor due to an increase of the electric field in certain spots the apparition of microdischarges. According to N. Sewraj et al. the electron avalanche from cathode has an average speed of 2.5 × 105 m/s and the cathode directed streamer an average speed of 5 × 105 m/s [6]. This data was obtained at 50 torr in pure nitrogen and for atmospheric pressure it is expected that due to higher molecule density the phenomena should be slower. In a 100 µm discharge gap the electron avalanche from cathode needs 0.4 ns to reach the anode and after the cathode directed streamer reaches the cathode in 0.2 ns if we consider the above mentioned speeds and slower for atmospheric pressure. Considering this the phenomena of electron avalanche towards anode and first streamer reaching cathode was captured in the first image of Figure 6(b). The addition of N2 in Ar contributed to a filamentary discharge due to N2 instead of a diffuse one in the case of pure Ar discharge. This allowed us to observe the phenomena of microdischarges. As shown in Figure 6(b) the narrowest diameter of the microdischarge is under 30 µm, thinner than other researchers reported [11]. Stark-broadened spectra can be used to determine microplasma density [12],[13],[15],[16]. Considering the dimensions of microplasma only spectroscopy techniques can be used to measure the plasma density. In addition to their Stark profiles, the spectra are also convolutions of instrument broadening and Doppler broadening. Electric microfields of neighbouring particles give rise to Stark broadened line profiles. Stark broadening is characterized by a Lorentzian profile, whose full width at half max (FWHM) is directly related to electron density. A Lorentzian and Gaussian convolution is a Voigt function [12], [13]: V( ) exp( G L( ) 4 ln 2( ' G 2W ' G( )L( 0) 2 )d ' A* L2W ) 4( ' 0) 2 L2W d ' (1) where A is amplitude of Voigt profile, Gw is FWHM of the Gaussian function, Lw is FWHM of the Lorentzian function, λ is the wavelength and λ0 is the centroid wavelength. A pseudo Voigt function was used to determine Lw by applying least square fit and optimizing the parameters to fit the Ar I peak at 696.5 nm spectra: LW 2 V( ) V0 S(m u 2 4( L2W 0) 4 ln 2 4 ln 2 2 (2) ( 0) ) GW G 2W where V0 is offset, S area and mu profile shape factor [14]. After optimizing the parameters to fit the spectra using Scilab as shown in Figure 7 to optimum value of Lw = 0.0042564 nm. Considering van der Waals broadening Ww= 0.003 nm and extracting it from Lw, the value of Stark width resulted Sw=0.0012564 nm. (1 m u ) exp( Fig. 7. Measured and fitted spectra of Ar I peak at 696.5 nm. The Stark width equation was approximated by [13],[15]: 2(1 1.75 *10 4 * 4 ne * * 1 (1 0.0068 * 6 ne )) *10 16 * w * ne (3) Te where ne is the electron density, α is the static ion broadening parameter, Te is the electron temperature and w is electron impact half-width. Previously we reported the electron temperature for microplasma discharge in Ar at atmospheric pressure Te=10000~23000 K [2]. Considering also α=0.032, w=0.00537 nm/1016 cm−3 [13],[15],[16], and Sw=0.0012564 nm in equation (3) electron density was calculated ne=1.338x1015 /cm3. SW 4. Conclusion The analysis of the spatial and temporal behavior of the dielectric barrier discharge microplasma showed its particularities regarding dynamics and characteristics of microdischarges: 1) Spatial and temporal distribution of light emission from microplasma was observed for about 365 ns corresponding to the duration of discharge current. Light near the negative electrode was preceded by the waves of light intensity that started directly from the anode and propagated towards the cathode. 2) Spatial and temporal distribution for the N2 SPS peak at 337.1 nm inside the discharge gap shown a maximum intensity towards the anode for the 25 ns. 3) Electron density measured a specific value for atmospheric pressure nonthermal plasmas of ne=1.338x1015 /cm3. Acknowledgment The authors would like to thank Prof. M. Nagatsu from Shizuoka University for the fruitful discussions. 5. References [1] K. Shimizu, M. Yamada, M. Kanamori, M. Blajan, IEEE Trans. Ind. Appl., 46, 641 (2010). [2] M. 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