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Direct measurement of electron density in microdischarge at atmospheric pressure by Stark broadening

Lifang Dong, Junxia Ran, and Zhiguo Mao Citation: Appl. Phys. Lett. 86, 161501 (2005); doi: 10.1063/1.1906299 View online: http://dx.doi.org/10.1063/1.1906299 View Table of Contents: http://apl.aip.org/resource/1/APPLAB/v86/i16 Published by the American Institute of Physics.

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APPLIED PHYSICS LETTERS 86, 161501 2005

Direct measurement of electron density in microdischarge at atmospheric pressure by Stark broadening


Lifang Dong,a Junxia Ran, and Zhiguo Mao
College of Physics Science & Technology, Hebei University, Baoding 071002, China

Received 26 August 2004; accepted 7 March 2005; published online 14 April 2005 We present a method and results for measurement of electron density in atmospheric-pressure dielectric barrier discharge. The electron density of microdischarge in atmospheric pressure argon is measured by using the spectral line prole method. The asymmetrical deconvolution is used to obtain Stark broadening. The results show that the electron density in single lamentary microdischarge at atmospheric pressure argon is 3.05 1015 cm3 if the electron temperature is 10 000 K. The result is in good agreement with the simulation. The electron density in dielectric barrier discharge increases with the increase of applied voltage. 2005 American Institute of Physics. DOI: 10.1063/1.1906299 with a frequency of 23 kHz. A high voltage probe Tektronix P6015A, 1000X is used to measure applied voltage. A resistance is used to measure the discharge current. The light emitted from the discharge is detected by a photomultiplier tube Hamamatsu, H7826-01 and is recorded with an oscilloscope Tektronix TDS3054, 500 MHz . The visible emission spectrum from the discharge is obtained through a monochromator WDS-8, 1200 groove/ mm grating with a photomultiplier tube. The entrance slit width is 0.06 mm. A digital camera Canon Powershot G1: 1024 768 pixels is used to record images of the discharge. An argon gas ow of 2 slm is maintained to prevent impurity accumulation during operation. Plasma-broadened and shifted spectral line proles have been used for a number of years as a basis of an important noninterfering plasma diagnostic technique.913 In the plasmas with electron density higher than 1015 cm3, where the Stark effect plays an important role on the atom spectral line broadening, the Stark broadening characteristics of atoms can be used for purposes of plasma diagnostics.11 Stark broadening is caused by the Coulomb interaction of the emitting atoms with the charged particles present in the plasma. For nonhydrogenic atoms, the full width at half maximum Stark nm is a complex FWHM of Stark broadening L function of the electron density Ne cm3 and electron temperature Te K . The expression for the Stark broadening can be approximated by12,13

In recent years, atmospheric-pressure dielectric barrier discharge DBD has been paid much attention due to its numerous potential industry applications such as plasma processing, ozone generation, pollution control, and sterilization of biological samples.13 It is also a system in the study of pattern formation, an important eld of nonlinear science.4,5 The discharge operated in atmospheric pressure consists of a lot of microdischarges, in which all physical and chemical processes including excitations, ionizations, and chemical reactions occur. Any knowledge of the plasma parameters of microdischarge, especially electron density and electron temperature, is desirable for understanding the physical and chemical processes. It is believed that the electron density of a microdischarge usually is in the order of 10141015 cm3 through the numerical simulation.6 However, there is no report on measurement of the absolute value of electron density of a microdischarge at atmospheric pressure up to now. Maybe there are two reasons resulting in the above fact, one is that the single microdischarge is hardly obtained in DBD, the other is the difculties of the usual electron density measurement method applied to a microdischarge. The general methods to measure the electron density in plasma are electrostatic Langmuir probes,7 laser Thomson scattering,8 and spectral line prole method.913 However the electrostatic Langmuir probe method that is widely used for low-pressure plasmas is generally less useful for plasma produced at atmospheric pressure.7 The laser Thomson scattering is a very complex method and hard to measure a microdischarge.8 The spectral line prole method should be the most convenient method for measuring a microdischarge because of its simple equipment and nonintrusive characteristic. In this article, we report the measurement of electron density of a microdischarge in atmospheric-pressure DBD by using the spectral line prole method. The schematic diagram of experimental device is shown in Fig. 1. Two cylindrical containers with diameters of 47 mm are lled with tap water. There is a metallic ring immersed in each of the containers and connected to a power supply. Thus, the water acts as liquid electrode. The parallel glass with a thickness of 1.5 mm serves as dielectric layer. An ac power supply has a maximum peak voltage of 10 kV
a

Electronic mail: Donglf@mail.hbu.edu.cn

FIG. 1. Schematic diagram of the experimental setup: HVhigh voltage high frequency power supply. 86, 161501-1 2005 American Institute of Physics

0003-6951/2005/86 16 /161501/3/$22.50

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161501-2

Dong, Ran, and Mao

Appl. Phys. Lett. 86, 161501 2005 TABLE II. Broadening coefcient / N for van der Waals broadening of Ar I 696.54 nm spectral line, in units of 1020 cm1 / cm3. Authors Lee 2.9 0.8 Copley 2.8 0.3 Hindmarsh 2.0 0.3 Stacey 1.67 0.05 Theory 1.9

TABLE I. Stark broadening parameters of Ar I 696.54 nm as a function of electron temperature and the electron density corresponding to Stark broadening under different electron temperature. Te K 5000 10 000 40 000 w nm/ 1016 cm3 0.004 09 0.005 37 0.008 73 0.040 0.032 0.023 Ne 1015 cm3 / 3.55/ 3 2.71/ 3 1.68/ 3
Stark =3 L Stark L

0.001 nm /N 4.73/ 4 3.61/ 4 2.24/ 4

Note: 3.55/ 3 represents Ne = 3.55


Stark = L

1015 cm3 if

0.001 nm.

1 + 1.75 0.068N1/6T1/2 e e

104N1/4 e 10
16

1 wNe , 1

where is the static ion-broadening parameter, w is electron impact half-width. Both are the function of electron temperature and listed in Table I.10 Approximately, electron density Stark under certain electron temperais a linear function of L ture. The Stark broadening is determined by electrons impact broadening and plasma ions impact broadening. In dense plasmas, isolated spectral lines of neutral atoms other than hydrogen are mostly broadened by electron impact. This electron impact broadening gives a symmetrical Lorentzian prole. In addition, smaller contribution to the line broadening arises from the plasma ions, which is asymmetrical in nature. So the Stark prole is described by the sum of these two broadenings leading to asymmetrical Lorentzian spectral line prole j j = 1
0

1+

WR d 0 d /w

2 2,

represents the microeld strength distribution where WR function,14 0 is the central wavelength of the prole, and d is the electron impact Stark shift. In experiment, the spectral line emitted from plasma are subject to various broadening mechanisms such as natural broadening, Doppler broadening, instrumental broadening, and pressure broadening, which includes resonance, van der Waals, and Stark broadening. The natural broadening and resonance broadening are generally negligible in high density plasma.13 Doppler and instrumental broadening follow Gaussian prole. van der Waals broadening follows Lorentzian prole and Stark broadening follows the asymmetrical Lorentzian prole j . It is obvious that the sum of the van der Waals Lorentzian prole and Stark prole j is also a . Based on Eq. 2 and asymmetrical Lorentzian prole L should be in the following form: its deducing process, L L = 1
0

where G , w , d , and are tted to the experiment data. We compiled a deconvolution procedure to separate the prole from the total spectral line prole. The Stark L broadening can be obtained by extracting van der Waals Van from FWHM . As is well broadening L of L L known, the van der Waals broadening is proportional to neutral particle number density and the broadening coefcient of 696.54 nm linewidth is listed in Table II.15 According to Ref. 12, the gas temperature in discharge channel in argon at atmospheric pressure in our experiment will be estimated to be about 2300 K and the van der Waals broadening is about 0.003 nm when the moderate coefcient value 2.0 1020 cm1 / cm3 is chosen. In general, dielectric barrier discharge at atmospheric pressure consists of a lot of microdischarges or laments moving stochastically. It is hard to select a single microdischarge for spectral measurement. To obtain a stable single microdischarge the stable time is more than one minute , the cleaning discharge technology is used in our experiment.16 At rst, the applied voltage is raised to a high value for example 3000 V and a cleaning discharge at this high voltage is conducted for several minutes. Then the voltage is decreased slowly until several stable laments are formed. The laments expire one by one by continually decreasing the voltage. Finally, single lamentary microdischarge is formed. In order to obtain good spectral line prole, the slits of the monochromator are set 60 m to enhance the spectrum intensity. The 696.54 nm Ar I transition 2P2 1S5 is chosen to diagnose the electron density because it is a strong and well isolated spectrum line of the neutral argon. Figure 2 gives the measurement result of the electron

1+

WR d 0 d /w

2 2.

The total spectral line prole is the convolution of the Gaussand described by ian prole and L K =
+

y L y dy 1
0 G

/2

exp

2 y
2 G

WR d 1 + y 0 d /w

2 2 dy,

FIG. 2. a Wave forms of voltage, current, and light of single lamentary microdischarge. b Deconvolution result for Ar I 696.54 nm and timeintegrated photograph of single lamentary microdischarge. Exposure time= 1 / 15 s , applied voltage= 1800 V . Cconvolution prole, GGaussian prole, Lasymmetrical Lorentzian prole.

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161501-3

Dong, Ran, and Mao

Appl. Phys. Lett. 86, 161501 2005

FIG. 3. a Snapshots exposure time= 1 / 50 s of seven lamentary microdischarges applied voltage= 1870 V and eight lamentary microdischarges applied voltage= 1900 V . Deconvolution result for Ar I 696.54 nm of b seven lamentary microdischarges and c eight lamentary microdischarges.

be calculated for a certain electron temperature according to Eq. 1 and Table I. For example the electron density of the microdischarge is 3.05 1015 cm3 for electron temperature of 10 000 K. This result is in good agreement with the simulation results.6 It is found that the electron density decreases with the decrease of applied voltage. Figure 3 gives the electron density measurement results of discharge pattern organized by seven and eight lamentary microdischarges. The electron density is 3.43 1015 cm3 in seven lamentary microdischarges under an applied voltage of 1870 V. The electron density is 3.48 1015 cm3 in eight lamentary microdischarges under an applied voltage of 1900 V. In addition, the estimated relative error of electron density is about 40% by considering the error of measurement, uncertainty of van der Waals broadening coefcient see also Table II and the process of deconvolution procedure. In conclusion, the electron density of microdischarge in atmospheric pressure argon is measured by Stark broadening. The electron density in single lamentary microdischarge at atmospheric pressure argon is 3.05 1015 cm3 if the electron temperature is 10 000 K. The result is in good agreement with the simulation. The electron density in DBD increases with the increase of applied voltage. It is believed that above method and the results will be of great importance to applications of DBD. This work is supported by the Natural Science Foundation of China under Grant No. 10375015, the Key Project of Chinese Ministry of Education. No. 02020 , and the Natural Science Foundation of Hebei Province, China under Grant No. A2004000086.
U. Kogelschatz, IEEE Trans. Plasma Sci. 30, 1400 2002 . S. Y. Moon, W. Choe, and B. K. Kang, Appl. Phys. Lett. 84, 188 2004 . 3 J. Reece Roth, Phys. Plasmas 10, 2117 2003 . 4 L. F Dong, Z. G Mao, Z. Q. Yin, and J. X. Ran, Appl. Phys. Lett. 84, 5142 2004 . 5 T. Shirafuji, T. Kitagawa, T. Wakai, and K. Tachibana, Appl. Phys. Lett. 83, 2309 2003 . 6 B. Eliasson and U. Kogelschatz, IEEE Trans. Plasma Sci. 19, 309 1991 . 7 S. Y. Moon, W. Choe, H. S. Uhm, Y. S. Hwang, and J. J. Choi, Phys. Plasmas 9, 4045 2002 . 8 Y. Noguchi, A. Matsuoka, K. Uchino, and K. Muraoka, J. Appl. Phys. 91, 613 2002 . 9 N. Konjevi, Plasma Sources Sci. Technol. 10, 356 2001 . 10 H. R. Griem, Plasma Spectroscopy McGraw-Hill, New York 1964 , p. 492. 11 V. Milosavljevi and S. Djenie, Eur. Phys. J. D 23, 385 2003 . 12 C. Penache, M. Miclea A. Bruning-Demian, O. Hohn, S. Schssler, T. Jahnke, K. Niemax, and H. Schmidt-Bcking, Plasma Sources Sci. Technol. 11, 476 2002 . 13 S. Pellerin, K. Musiol, B. Pokrzywka, and J. Chapelle, J. Phys. B 29, 3911 1996 . 14 A. Y. Potekhin, G. Chabrier, and D. Gilles, Phys. Rev. E 65, 1 2002 . 15 C. S. Lee, D. M. Camm, and G. H. Copley, J. Quant. Spectrosc. Radiat. Transf. 15, 211 1975 . 16 L. F. Dong, Z. Q. Yin, X. C. Li, and L. Wang, Plasma Sources Sci. Technol. 12, 380 2003 . 17 K. Hamano, S. Sugita, and T. Kadono, Lunar Planet. Sci.34 Annual Lunar and Planetary Science Conference, March 1721, 2003, League City, Texas, Abstract no. 1647.
2 1

density of single lamentary microdischarge under applied voltage of 1800 V. Figure 2 a shows the wave forms of voltage, current, and light emission during spectrum collecting. The current is the superposition of displacement current and the single microdischarge current spike. It can be seen that the uctuation in discharge current is less than 10%. It indicates that the microdischarge is stable enough to ensure that good spectral line prole can be obtained in spectral measurement. Figure 2 b shows the side-view timeintegrated photograph of the microdischarge and deconvolution result for Ar I 696.54 nm. It should be noticed that the latter is also time average since the duration of spectral measurement is about 1.0 104 times of the cycle of applied voltage. The photo shows that an almost axially symmetrical single lamentary microdischarge spreads out like H shaped. The channel is about 0.4 mm, but the diameter of the luminescence at the dielectric surface is about 5 mm. The FWHM of the Gaussian prole is very broad due to the large monochromator slit width leading to the broad instrument broadening . It is familiar in the spectral line prole measurement of weak light.17 The Stark broadening FWHM is about 0.00337 nm after extracting van der Waals broadening Van 0.003 nm from L. The electron excited temperaL ture is estimated to be in the range of 500010 000 K by the intensity ratio of 763.72 and 772.63 nm of the argon atom in our experiment. It is generally believed that the electron temperature in DBD is greater than the electron excited temperature and is in the range of 110 eV.6 The electron density can

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