OPEN Characterization of argon direct-current

SUBJECT AREAS:
glow discharge with a longitudinal
PLASMA PHYSICS
APPLIED PHYSICS
electric field applied at ambient air
Weiman Jiang1, Jie Tang1, Yishan Wang1, Wei Zhao1 & Yixiang Duan1,2
Received
7 May 2014 1
State Key Laboratory of Transient Optics and Photonics, Xi’an Institute of Optics and Precision Mechanics of CAS, Xi’an 710119,
Accepted China, 2Research Center of Analytical Instrumentation, Sichuan University, Chengdu 610064, China.
20 August 2014
Published A direct-current-driven plasma jet is developed by applying a longitudinal electric field on the flowing argon
10 September 2014 at ambient air. This plasma shows a torch shape with its cross-section increased from the anode to the
cathode. Comparison with its counterparts indicates that the gas flow plays a key role in variation of the
plasma structure and contributes much to enlarging the plasma volume. It is also found that the circular
hollow metal base promotes generation of plasma with a high-power volume density in a limited space. The
Correspondence and optical emission spectroscopy (OES) diagnosis indicates that the plasma comprises many reactive species,
requests for materials such as OH, O, excited N2, and Ar metastables. Examination of the rotational and vibrational temperature
should be addressed to indicates that the plasma is under nonequilibrium condition and the excited species OH(A 2S1), O(5P), and
J.T. (tangjie1979@opt. N2(C 3Pu) are partly generated by energy transfer from argon metastables. The spatially resolved OES of
ac.cn)
plasma reveals that the negative glow, Faraday dark space, and positive column are distributed across the gas
gap. The absence of the anode glow is attributed to the fact that many electrons in the vicinity of the anode
follow ions into the positive column due to the ambipolar diffusion in the flowing gas.

A
tmospheric pressure nonequilibrium plasmas recently have attracted a great interest largely because it can
be used for a wide range of applications, such as surface modification, thin film deposition, and biological
decontamination, without the need for an expensive vacuum system1–4. Such plasmas are usually pro-
duced by different kinds of discharges like corona, capillary, direct-current (DC), radio frequency, microwave,
and dielectric-barrier discharges5. DC glow discharge is a popular one among them, with the voltage applied
between two naked electrodes. The DC glow discharge was first observed with helium, neon, and nitrogen used as
working gas in a tube at the low pressure, and characterized by different regions depending on the discharge
parameters (e.g., the geometry of the electrodes, the gas type, and the pressure)6. This kind of discharge was also
successfully generated at high pressure, even at atmospheric pressure in the ambient air, though there exist
undesirable instabilities which lead a glow to arc transition. Different geometries of electrode and different types
of gas were employed to characterize the DC glow discharge in laboratory. A DC microhollow cathode discharge
(MHCD) in atmospheric pressure air has been reported by Stark and Schoenbach7–8. The stability of this plasma is
attributed to the fact that the microhollow cathode supplies electrons to the positive column of the discharge
rather than the instability prone cathode region as in a traditional glow discharge. Another DC glow discharge was
generated between a thin cylindrical anode and a flat cathode with helium, argon, hydrogen, nitrogen and air used
as working gas respectively9. The discharges appeared to operate as temperature and pressure scaled versions of
low pressure discharges. It is possible to distinguish negative glow, Faraday dark space, and positive column
regions of the discharge in the normal glow discharges. Investigations of atmospheric pressure glow discharges in
helium, argon, nitrogen and air in the similar electrode configuration were presented10. Experiment results
showed that for all the gases, plasma non-equilibrium degree in a positive column decreases with discharge
current increase.
It is generally accepted that a high speed gas flow is beneficial to improvement of discharge stabilities due to
sufficient cooling of discharges at high pressures. A stable brush-shaped plasma jet was achieved by introducing a
flowing argon through the narrow slit with two cylindrical electrodes set opposite at its ends and powered by a DC
supply11. Here, a transverse electric field was applied on the flowing gas with its flow direction perpendicular to the
field. The spatially resolved optical emission spectroscopy (OES) of the plasma revealed that the negative glow,
positive column, and anode glow exist across the gas gap. Li et al. employed the similar device as that used in Ref.
11 to generate a brush-shaped plasma jet12, where the same spatial discharge structure was observed. Another

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Figure 1 | The experimental setup. Figure 3 | Photographs of (a) the experimental apparatus and (b) the
plasma jet generated between two rod electrodes with the electrode spacing
electrode configuration was reported by Lu et al.13. A high-voltage of 6 mm (with the exposure time of 20 ms).(c) shows the isointensity map
pulsed DC power supply was connected to the blades that serve as the of the plasma image out of the quartz tube.
anode and the treated objects were connected to the ground, where a
longitudinal electric field was applied on the flowing gas. The nega- curve becomes essentially flat and the discharge voltage approxi-
tive glow, Faraday dark space and positive column in the brush- mately maintains a constant with the increasing current.
shaped plasma are clearly visible to the naked eye. Additionally, a Figure 3(a) shows the experimental apparatus without discharge.
DC-driven plasma source equipped with hollow-needle-plate elec- When the apparatus works at an operating point with the discharge
trodes was developed by Li et al.14, where the gas flows along the voltage of 234 V and current of 22 mA, the discharge operates in the
cavity of the hollow needle and rushes to the plate. This plasma normal glow mode and a stable plasma jet is formed between the two
presents us a diffuse plume in cup shape in the discharge space. As electrodes, as shown in Fig. 3(b). The plasma photograph was taken
mentioned above, in order to obtain a stable plasma, the working gas by using a digital camera (Nikon D5200) with the exposure time of
was allowed to flow through the discharge space with either a trans- 20 ms. The plasma appears to eject out of the quartz tube from the
verse or a longitudinal electric field applied on. As for the longit- end face of the anode and run towards the cathode, and gradually
udinal electric field, the working gas flows from one electrode to the becomes thick from the top to the bottom, looking like an inverted
other, where the needle-plate (or rod-plate) electrodes are usually torch. The diameter of the plasma jet is approximately linearly
used. In this work, a plasma jet is generated by using a longitudinal increased from 1 mm close to the anode to about 3 mm around
electric field that is generated between two rod electrodes. This the cathode, exhibiting an increasing cross-section. A closer obser-
plasma shows quite different physical structure in comparison with vation indicates that parts of the plasma run out of the discharge
those observed in the traditional DC glow discharge. space between the electrodes along the gas flow direction and sur-
round the cathode end face. Figure 3(c) shows the isointensity map of
Results the plasma image out of the quartz tube (with x varied from 1 to
To demonstrate the unique DC-driven plasma jet, we used the atmo- 7 mm). It is found that the luminance of the plasma is weakened
spheric-pressure plasma device sketched in Fig. 1. The voltage-cur- along the radial direction.
rent (V-I) characteristic of the DC discharge was examined at the gas To investigate reactive species in the plasma, the OES was exam-
flow 2 L/min, with the relationship between the discharge voltage ined by using a moderate-resolution spectrometer with its fiber
and current shown in Fig. 2. It is found that only subnormal (zone I) arranged at the specific spot (x 5 3 mm and y 5 0 mm) in accord-
and normal (zone II) glow discharge modes appear in the examined ance with the axe labeled in Fig. 3. Typical emission spectra with the
current scope of 9–33 mA, where the Townsend mode is not wavelength range from 200 to 1000 nm are depicted in Fig. 4. In the
observed. In the subnormal glow discharge (9–18 mA), the V–I ultraviolet and visible region, between 200 and 450 nm, the spectra
curve assumes a negative differential resistance and the discharge are dominated by N2(C 3Pu R B 3Pg) emissions. Additionally, the
voltage across the gas gap drops with the increasing current. When OH emission lines, resulted from OH(A 2S1 R X 2P) transition, are
the discharge is transformed to the normal one (18–33 mA), the V–I also visible. In the visible and infrared region between 690 and
950 nm, we can easily observe various excited argon atomic lines
(e.g., l 5 763.7, 772.7, and 811.7 nm) from the 4 p R 4 s transitions.
Meanwhile, a group of oxygen atomic lines around 777.8 nm, which
correspond to O(I) triplet state transitions (O(5P) R O(5S0)), are also
observed in close wavelength to one another, but cannot be distin-
guished due to the resolution limit of the spectrometer.

Figure 2 | Voltage-current characteristic of the plasma source with Figure 4 | The emission spectrum of the plasma jet examined at the spot
2 L/min argon as working gas at atmospheric pressure. with x 5 3 mm and y 5 0 mm.

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Figure 5 | The comparison of experimental and simulated spectra of (a)

OH(A 2S1 R X 2P, Dv 5 0) transition for Trot measurement and (b)
N2(C 3Pu R B 3Pg, Dv 5 22) transition for Tvib measurement.

Due to frequent collisions among heavy particles at atmospheric

pressure, the rotational temperature (Trot) of the OH radical has a
value which is generally close to the gas temperature15,16. This tem-
perature can be measured by using the OH(A 2S1 R X 2P, Dv 5 0)
band transition from 306 to 312 nm. This band is easily isolated
under various experimental conditions to give useful information.
The vibrational temperature (Tvib) provides the information of the
energy transfer between electrons and heavy particles, especially
molecules17. It was obtained by the typical Boltzmann plot method
of the nitrogen second positive system N2(C 3Pu R B 3Pg, Dv 5 22)
in the range 370–382 nm18. Based on the emission spectrum mea-
Figure 6 | Emission profiles of the radical OH (309.7 nm), excited N2
sured by using the high-resolution spectrometer with the fiber probe
(337.1 nm), and excited argon (763.7 nm) along x axis with a
arranged at the same spot (x 5 3 mm and y 5 0 mm), the rotational
longitudinal (a) and transverse (b) electric field applied on the flowing
temperature and vibrational temperature of the plasma were
gas, respectively.
obtained through the analysis of OH and N2 molecular emission
spectrum, respectively. As seen from Fig. 5, the simulated spectra
at Trot 5 810 6 32 K and Tvib 5 2200 6 45 K give a good fit to the The spatially resolved OES showed that all of these reactive species
experimental spectra, indicating that the vibrational temperature is presented a near-symmetrical distribution of emission profile, with
higher than the rotational temperature. the greatest emission intensity at the edges.
The spatially resolved OES of reactive species such as OH The spatially resolved OES of these reactive species was also exam-
(309.7 nm), N2 (337.1 nm), and Ar (763.7 nm) was examined along ined along the y axis with x 5 3 and 6 mm labeled in Fig. 3. Figure 7
the x axis or axial direction at y 5 0 mm (from the anode to the shows that the emission intensity of all the reactive species presents a
cathode labeled in Fig. 3), with the result shown in Fig. 6(a), where symmetric distribution with its maximum at the center. Along the y
the discharge current is 22 mA. It is found that the OH and Ar direction at x 5 3 mm, the light emitted from the excited argon
assume the similar spatial distribution of emission profile. Their exceeds that from other species and the N2 exhibits the weakest
OES intensity first increases along the x axis (0–1 mm), and then emission intensity, as shown in Fig. 7 (a). With x 5 6 mm, as seen
approximately maintains unvaried (1–4 mm). After a slight drop (4– from Fig. 7 (b), the light emitted from excited N2 is relatively
5 mm), the intensity rises largely, reaches its maximum around x 5 increased considerably and overwhelms both other species of light
6 mm, afterwards gradually declines, and tends to be zero near the along the y axis. The OH emission intensity becomes the weakest one.
cathode (6–7 mm). This spatial distribution feature of OES indir- The spatial distribution of rotational and vibrational temperature
ectly reveals that the negative glow (around x 5 6 mm), Faraday dark was measured through the spectral fitting method along the x axis at
space (around x 5 5 mm), and positive column (1–4 mm) are dis- y 5 0 mm, with the results depicted in Fig. 8. The errors in the
tributed from the cathode to the anode. The OES intensity of N2 measured rotational and vibrational temperature are less than 640
exhibits a quite different spatial distribution, in comparison with that and 650 K, respectively. As seen from Fig. 8 (a), the highest rota-
of OH and Ar. Its intensity maintains very low and nearly unvaried tional temperature (1050 K) is located in the negative glow region
from x 5 0 to 3 mm. After a slow increase (3–5 mm), the intensity and there is a decrease of temperature close to the Faraday dark
rises sharply (5–6 mm), approaches its maximum around 6 mm, space. After the Faraday dark space, this temperature rises gradually
and drops rapidly near the cathode (6–7 mm). and approaches about 810 K in the positive column. Approaching
Figure 6(b) shows the OES spatial distribution of a stable brush- the anode, the temperature decreases to about 630 K. Figure 8 (b)
shaped plasma jet generated in an extended DC discharge by apply- shows a distinct increase of vibrational temperature from the nega-
ing a transverse electric field on the flowing argon, which was pre- tive glow region to the Faraday dark space where the temperature
sented in our previous work11. This DC discharge was supported by a arrives at its maximum of 2450 K. This temperature reduces after the
DBD one and operated in a normal glow mode at discharge current Faraday dark space and reaches about 2200 K in the positive column.
22 mA. The OES of the plasma was examined along the x axis (from The measured rotational and vibrational temperature profiles are in
the cathode to the anode) with the distance 2 mm away from the exit. well agreement with those reported by Staack et al.19.

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cathode. The backflow gas and the large-area plate cathode are
responsible for the large-volume diffuse plasma generated in the
vicinity of the cathode. In our case, the circular hollow metal base
avoids the gas backflow and gas dispersion to a larger open space
around the discharge region. This promotes the formation of a thin
gas flow channel around the column of the discharge region, leading
to the generation of plasma with a high-power volume density in a
limited space. This feature is crucial in applications such as surface
modification, where a high-power-density plasma is required.
As we know, reactive species, such as OH and O, are the indis-
pensable components and main enablers for industrial and medical
plasma treatment applications. The OES of the torch-shaped plasma
jet indicates that many reactive species, including OH, O, excited N2,
and argon metastables, are produced in the glow discharge, as shown
in Fig. 4. All these reactive species are desirable in the applications
such as surface modification and biological decontamination. Since
the plasma jet is generated in the ambient air, the presence of OH, O
and excited N2 spectra is attributed to the interaction of the argon
plasma with the ambient air that contains nitrogen, oxygen, water
vapor, and other components, which will be addressed in detail in the
following section.
Examination of the rotational temperature and vibrational tem-
perature of the plasma in Fig. 5 shows that the plasma jet is under
nonequilibrium condition. This feature is favorable for enhanced
plasma chemistry. The electronic excitation temperature Texc of
plasma is determined according to the double-line method21:
ajj1 {j2 j
Texc ~ , ð1Þ
lg gg12 AA12 { lg ll12 { lg ii12

Figure 7 | Emission profiles of the radical OH (309.7 nm), excited N2 where two close spectral lines (l1 5 763.7 nm, 2P6 R 1S5, and l2 5
(337.1 nm), and excited argon (763.7 nm) along the y axis with x fixed at 772.7 nm, 2P2 R 1S3) are used; excitation potentials of the spectral
(a) 3 mm and (b) 6 mm, respectively. lines j1 5 13.17 eV and j2 5 13.328 eV; the coefficient a is 5040 for
j in eV; the weighting factor g1 5 5 and g2 5 3; transition probability
Discussion of the two spectral lines A1 5 24.5 and A2 5 11.7; and i is the relative
In the traditional DC normal glow discharge in a still argon at atmo- intensity of spectral line with i1 < 45800 and i2 < 1710022, The
spheric pressure, the contraction of the positive column, which is electronic excitation temperature is estimated to be 0.57 6 0.02 eV
attributed to the recombination process, allows the gas discharge to (6586 6 240 K) and far beyond the vibrational temperature. This
occur only in the discharge space between two opposite plane elec- also indicates the nonequilibrium characteristic of the plasma jet.
trodes6,20. The cross-section of the positive column has been changed However, the vibrational temperature determined through ana-
little along the axial direction (from the anode to the cathode)10. lysis of N2 emission spectra as a result of electron impact excitation is
Comparison with the torch-shaped plasma jet in our case (see usually measured to be about 3000 K23, and much higher than the
Fig. 3(b)) indicates that the gas flow plays a key role in variation of temperature examined in our case. This suggests that the excited
the plasma structure and contributes much to enlarging the plasma species OH(A 2S1), O(5P), and N2(C 3Pu) are partly generated by
volume along the radial direction especially in the vicinity of the energy transfer from argon metastables, in addition to the electron
cathode. In the work performed by Li et al.14, a cup-shaped plasma excitation. As is well known, the energy carried by the argon meta-
could be formed between the hollow-needle anode and the plate stables (11.5–13.5 eV)24, which are produced effectively in our case
indicated by the spectrum shown in Fig. 4, is slightly higher than that
of energy level of N2(C 3Pu) (,11.1 eV) from the ground state25. The
argon metastables can easily transfer energy to the ground state
nitrogen molecules to generate abundant excited state N2(C 3Pu)
molecules. Besides, the energy required to dissociate H2C from the
ambient air into OH and H, and subsequently excite the ground state
OH to the excited state OH(A 2S1) is only 5.1 and 4.2 eV respect-
ively24. Sufficient excited state OH(A 2S1) molecules can be produced
by energy transfer from argon metastabels. Thus, the emission spec-
tra arising from the excited OH and N2 are distinctively presented.
The energy threshold is 15.9 eV for the production of O(5P) from O2,
and is beyond the energy level of the argon metastables25. Therefore,
the direct generation of excited O from O2 through energy transfer
with excited argon atoms is ignorable in our case. However, the
energy for dissociation of an oxygen molecule to oxygen atoms is
5.58 eV and that required to subsequently produce O(5P) from
ground state O is about 10.7 eV25,26. Since the two potential levels
Figure 8 | The spatial distributions of (a) rotational temperature and (b) are in the range of the energy carried by argon metastables, the
vibrational temperature along the x axis at y 5 0 mm. excited O can be produced from their ground state atoms through

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energy transfer processes with excited Ar. As a result, the oxygen duced there. When these reactive species are deexcited, they emit a
emission spectra are observed. brighter light, as illustrated in Fig. 3(c).
The spatially resolved OES of the plasma in Fig. 6(a) presents the The spatially resolved rotational and vibrational temperature mea-
spatial emission spectrum distribution of reactive species. As dis- surements in Fig. 8 show that the discharge is nonthermal through-
cussed above, the excited OH and N2 are produced from water vapor out the discharge space. The peak and valley in the profile of
and nitrogen in the ambient air through complex reaction channels. rotational temperature are associated with heating of the gas by
The corresponding reaction coefficients are largely dependent on the energetic electrons6. The rotational temperature peak in the negative
reaction conditions, such as reactant concentration and energy glow region is attributed to the more energetic electrons due to the
required for reaction onset. The distinct spatial distribution of OH high electric field there. In the Faraday dark space, the electrons are
and N2 emission spectra is probable due to the largely different less energetic with a low electric field, resulting in a falling of tem-
volume percent between water vapor and nitrogen in ambient air perature. The decrease of rotational temperature close to the anode is
and different energy required to pump them from the ground state to probably due to the higher gas flow velocity which is beneficial to
an excited one16. In our experiment, the argon ejects into the ambient cooling the plasma. A correspondence between higher vibrational
air from the end face of the anode with a certain velocity and mixes temperature and lower rotational temperature is observed probably
with the ambient air. The un-fully mixing partly contributes to the due to the increased vibration-translation relaxation rates at higher
low and slowly increasing intensity of N2 emission spectra in the gas temperature19,29.
positive column. In addition, the gas flow brings parts of the excited
N2 downward and few are left upward in the positive column. This Methods
contributes much to assembling most of the excited N2 in the vicinity A schematic of the experiment setup is shown in Fig. 1. The plasma source mainly
of the cathode. comprises two parts. One is the anode unit and the other is the cathode unit. In the
In our previous work, as shown in Fig. 6(b), a near-symmetrical anode unit, a cylindrical metal rod (with the diameter of 1 mm) serves as the anode
that is centered inside a quartz tube (with the inner diameter of 1.7 mm and outer
distribution of emission profile of reactive species (radical OH, diameter of 3.3 mm). The metal rod is connected to a high-voltage DC power supply
excited N2, and excited argon) was presented in front of us, with a through a 100 MV ballast resistor which is used to limit the discharge current. As for
flat area located in the middle and two peaks situated at the edges. It is the cathode unit, a metal (iron) spring acts as the cathode and is embedded in the
considered that the flat area is correlated with the positive column of hollow cylindrical metal base (with the hollow diameter of 7 mm) that is connected to
the ground. It should be noted that the metal spring is fixed tightly in the metal base
the DC glow discharge, while the two peaks at the edges is attributed and could hardly be deformed by the gas flow. The anode unit is set above the cathode
to the negative and anode glow, where there exist many energetic one with the electrode spacing of 6 mm. Argon (with the purity of 99.999%), which is
electrons. In this work, the near-symmetrical distribution of emis- controlled by a mass flow controller (fixed at 2 L/min), enters by inlet port, flows
sion profile cannot be found, because the peak of emission intensity through the circular region between the quartz tube and the anode, and rushes out
into the discharge space, where argon and ambient air are mixed. The volume fraction
appears only near the cathode. The absence of the emission intensity of water vapor in ambient air is estimated to be 1.9%, based on the temperature of
peak near the anode suggests that the anode glow does not exist. 25uC and the relative humidity of 60% recorded by a humidity/temperature trans-
Since the gas flow is fixed at 2 L/min and the inner diameter of mitter. With a proper voltage applied to the two electrodes, a stable plasma jet,
quartz tube is 1.7 mm, the gas flow velocity near the anode is esti- indicated by the red pattern, can be formed between them. In our experiment, the gas
mixture flows from the anode to the cathode and the flow has the same direction with
mated to be about 1.7 3 103 cm/s. The electric field in the positive the electric field. After travelling across the discharge space, the gas mixture will flow
column can be expressed as E 5 (Vdis 2 Vn)/D, with the value of along the original direction and into the circular hollow space of the metal base, rather
172 V/cm. Here, Vdis is the sustaining voltage (234 V) between the than flow back in the case where needle-plate (or rod-plate) electrodes are used. The
electrodes, Vn is the cathode fall (,165 V) for the iron electrode6 and flow behavior of argon is indicated by the light blue bar with an arrow downstream.
The plasma is imaged with a digital camera (Nikon D5200). The emission spectra
D is the length of the positive column (,4 mm). The electron drift from the plasma are recorded by using two different resolution spectrometers. For the
velocity is given by ve 5 meE. With the electron mobility me of 4.3 3 large emission spectrum range (200–1000 nm), an Avantes spectrometer (AvaSpec-
102 cm2/(V?s)6, the electron drift velocity is approximately equal to ULS2048-USB2) with a moderate resolution of 0.8 nm is used to identify various
0.7 3 105 cm/s and far beyond the gas flow velocity. This means the reactive species. In order to obtain the rotational and vibrational temperature of the
plasma, another Avantes spectrometer (AvaSpec-ULS2048-3-usb2) with a high
gas flow has practically no direct effect on the motion of electrons. As resolution of 0.1 nm is used. Both their fiber probes are placed at 1.0 cm away and
far as the ion motion is concerned, the ion drift velocity vi 5 miE< 0.3 perpendicular to the plasma. The radius of observation spot of fiber probe is 2.3 mm,
3 103 cm/s, where only one sort of ions Ar1 is considered for sim- with the fiber diameter of 200 mm and the fiber numerical aperture of 0.22.
plicity and the ion mobility mi 5 1.9 cm2/(V?s)27. It is found that the
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24. Xian, Y., Lu, X., Tang, Z., Xiong, Q., Gong, W., Liu, D., Jiang, Z. & Pan Y. Optical otherwise in the credit line; if the material is not included under the Creative
and electrical diagnostics of an atmospheric pressure room temperature plasma Commons license, users will need to obtain permission from the license holder
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photographing of an open-air argon plasma plume by a grating–ICCD camera
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