Direct-current glow discharges in atmospheric pressure air plasmas

Lan Yu, Christophe O. Laux, Denis M. Packan, and Charles H. Kruger

Citation: J. Appl. Phys. 91, 2678 (2002); doi: 10.1063/1.1435421

View online: http://dx.doi.org/10.1063/1.1435421
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JOURNAL OF APPLIED PHYSICS VOLUME 91, NUMBER 5 1 MARCH 2002

Direct-current glow discharges in atmospheric pressure air plasmas

Lan Yu,a) Christophe O. Laux, Denis M. Packan, and Charles H. Kruger
Mechanical Engineering Department, High Temperature Gasdynamics Laboratory, Stanford University,
Stanford, California 94305-3032
共Received 28 June 2001; accepted for publication 27 November 2001兲
Investigations have been conducted to experimentally validate the mechanisms of ionization in
two-temperature atmospheric pressure air plasmas in which the electron temperature is elevated
with respect to the gas temperature. To test a predicted S-shaped dependence of steady-state electron
number density on the electron temperature and its macroscopic interpretation in terms of current
density versus electric field, direct-current 共dc兲 glow discharge experiments have been conducted in
flowing low temperature, atmospheric pressure air plasmas. These experiments show that it is
feasible to create stable diffuse glow discharges with electron number densities in excess of 1012
cm⫺3 in atmospheric pressure air plasmas. Electrical characteristics were measured and the
thermodynamic parameters of the discharge were obtained by spectroscopic measurements. The
measured gas temperature is not noticeably affected by whether or not the dc discharge is applied.
The discharge area was determined from spatially resolved optical measurements of plasma
emission during discharge excitation. The measured discharge characteristics are found to be in
good agreement with the predicted electrical characteristics. © 2002 American Institute of Physics.
关DOI: 10.1063/1.1435421兴

I. INTRODUCTION eters, namely current density j and the electric field E, by

There has been considerable interest in finding methods
for efficiently producing large volumes of atmospheric pres-
sure air plasmas with free electron densities greater than
1012/cm3 at gas temperatures below 2000 K.1 Such plasmas
are of practical significance in applications ranging from
electromagnetic wave shielding to biodecontamination.2–5
Currently achievable electron number densities in these low
temperature air plasmas are on the order of 1010 cm⫺3. 5–11 In
order to produce and sustain electron number densities
greater than 1012 cm⫺3 in air without significantly heating the
gas, the energy must be added in a targeted fashion. One
approach is to apply the energy addition to the free electrons
by means of electrical discharge. Under appropriate condi-
tions, the energetic electrons produced by the discharge can
increase ionization reactions without significantly heating the
gas.1 Such plasmas are sometimes referred to as two-
temperature plasmas, with the kinetic temperature of the free
electrons T e being higher than the kinetic temperature of
heavy species T g . The chemical mechanisms of ionization
and recombination in air plasmas with energetic electrons
were modeled in Ref. 1. The numerical simulations of these
mechanisms yield the surprising result that the electron num-
ber density n e exhibits an S-shaped dependence on the elec-
tron temperature T e as shown in Fig. 1. This S-shaped be-
havior is caused by competing ionization and charge transfer
reactions, and by the importance of two-body dissociative
recombination relative to three-body electron recombination
reactions. The predicted steady state n e versus T e curves
were interpreted in terms of macroscopic discharge param-
a兲
Author to whom correspondence should be addressed; electronic mail:
yu@saha.stanford.edu
means of Ohm’s law and the electron energy equation. Ac-
cordingly, the resulting current density versus electric field
characteristic also exhibits a nonmonotonic behavior as can
be seen in Fig. 2, where the predicted discharge characteris-
tics in atmospheric pressure air at 2000 and 3000 K are
shown.1
In this article, we describe direct-current 共dc兲 glow dis-
charge experiments in which spectroscopic and electrical
measurements were made to determine temperatures, species
concentrations, electrical conductivity, and electron number
densities. The results of these experiments were then com-
pared with the theoretical discharge characteristics of Ref. 1.
The discharge experiments were conducted in a preheated
flowing air plasma 共velocity around 400 m/s兲 at adjustable
temperatures between 1800 and 3000 K.
II. dc DISCHARGE EXPERIMENT SETUP
The ionization process in the discharge region is accom-
panied by energy transfer to the gas through collisions be-
tween electrons and heavy particles. Reference 1 shows that
the electrons lose more than 99.9% of the energy gained
from the electric field to molecular N2 through vibrational
excitation, and the vibrationally excited N2 transfers energy
to translational mode through vibrational relaxation. Thus the
degree of gas heating ⌬T g is a function of the volumetric
power jE deposited into the plasma by the discharge and the
competition of the vibrational relaxation time and the resi-
dence time ␶ of the plasma in the discharge region. To limit
gas heating to acceptable levels of given volumetric power, it
is desirable to flow the plasma at high velocity through the
discharge region.
The experimental setup is shown schematically in Fig. 3.
Atmospheric pressure air is heated with a 50 kW radio-

0021-8979/2002/91(5)/2678/9/$19.00 2678 © 2002 American Institute of Physics

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J. Appl. Phys., Vol. 91, No. 5, 1 March 2002
FIG. 1. Predicted steady-state electron number density n e as a function of
electron temperature T e for air at T g ⫽2000 K.
frequency inductively coupled plasma torch operating at a
frequency of 4 MHz. A 2 cm exit diameter nozzle is mounted
at the exit of the torch head. The flow rate injected in the
torch was approximately 96 standard liters per minute 共slpm兲
共64 slpm radial and 32 slpm swirl兲 and the plate power set-
tings were 8.9 kV ⫻ 4.1 A, with approximately 14 kW of
power deposited into the plasma. Under these conditions, the
temperature of the plasma at the exit of the 2 cm diam nozzle
is about 5000 K and its velocity is ⬃100 m/s.
The plasma then enters a quartz test section where it is
cooled to the desired temperature by mixing with an adjust-
able amount of cold air injected into the plasma stream
through a radial mixing ring. The quartz test section length
of 18 cm ensures that the flow residence time 共approximately
1.6 ms here兲 is greater than the characteristic time for chemi-
cal and thermal equilibration of the plasma 共⬍1 ms兲. Thus at
the exit of the quart test section the air flow is close to local
thermodynamic equilibrium 共LTE兲 conditions. Finally, a 1
cm exit diameter converging water-cooled copper nozzle is
mounted at the exit of the mixing test section. The nozzle is
used to control the velocity, hence the residence time, of the
flow within the discharge region. Two-dimensional computa-
tional fluid dynamics 共CFD兲 calculations performed at the
University of Minnesota showed that the axial velocity at the
entrance of the discharge region is approximately 445 m/s.12
FIG. 2. Predicted E – j characteristics at T g ⫽2000 and 3000 K.
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Yu et al. 2679
FIG. 3. Setup 共not to scale兲 for discharge experiments showing the torch
head, the injection ring, the 2 cm diam, 18 cm long water-cooled quartz
mixing test section, the 2→1 cm converging nozzle, electrodes, voltage pins,
and electrical circuit.
The discharge itself is produced between two platinum pin
electrodes of 0.5 mm diameter held along the axis of the air
stream by two water-cooled 1/16 in. stainless-steel tubes
placed crosswise to the plasma flow. The bottom electrode is
mounted on the copper nozzle and the upper electrode is
affixed to a Lucite ring itself mounted on a vertical transla-
tion stage in order to provide adjustable distance between
electrodes. The distance was set to 3.5 cm.
The discharge was driven by a Del Electronics Model
RHSV10-2500R power supply with reversible polarities, ca-
pable of operation in control current or control voltage mode,
with current and voltage outputs in the ranges of 0–250 mA
and 0–10 kV, respectively. For the present experiments, the
cathode 共bottom electrode兲 was biased to negative potentials
with respect to ground.
The electric field within the discharge region is mea-
sured from the potential on a high purity platinum wire 共0.02
in. diameter兲 that extends to the center of the discharge re-
gion. The platinum wire is held by a small ceramic tube
installed on a two-way 共horizontal and vertical兲 translation
stage. Horizontal translation moves the pin into the discharge
region for electric field measurements, and out of the dis-
charge during spectral emission measurements. Vertical
translation moves the pin along the discharge axis to deter-
mine the electric field from potential measurements. Al-
though pure platinum melts at ⬃2045 K, radiation cooling
prevents melting of the platinum wires for plasma tempera-
tures up to at least 3000 K. The voltage measurements re-
ported here were made with a Tektronix Model P6015A high
voltage 共20 kV dc, 40 kV peak pulse兲 probe and a Hewlett
Packard Model 54510A, digitizing oscilloscope. The current
2680 J. Appl. Phys., Vol. 91, No. 5, 1 March 2002
FIG. 4. NEQAIR2 simulations of the OH A→X emission spectrum as a
function of temperature in LTE air, normalized to the peak of the P branch.
was measured from the voltage drop across the 12 k⍀ ballast
resistor of the dc circuit.
The setup for optical emission spectroscopy diagnostics
include a SPEX model 750 M, 3/4 m monochromator fitted
with a 1200 lines/mm grating blazed at 200 nm and a back-
thinned Spectrum One thermoelectrically cooled charge-
coupled device 共CCD兲 camera. The 30⫻12 mm CCD chip
contains 2000⫻800 pixels of dimension 15⫻15 ␮m. The
dispersion of the optical system is ⬃1.1 nm/mm. The mono-
chromator entrance slit width was set at 200 ␮m, and 26
columns of 800 pixels were binned to produce an equivalent
exit slit width of 390 ␮m. The spatial resolution was ⬃0.5
mm as determined by the monochromator entrance slit width
and the magnification of the optical train 共2.5 for two lenses
of focal length 50 and 20 cm兲. Absolute spectral intensity
calibrations were obtained with an Optronics model OL550
tungsten filament lamp and a 1 kW argon arcjet, with radi-
ance calibrations traceable to National Institute of Standards
and Technology 共NIST兲 standards.
III. SPECTROSCOPIC MEASUREMENTS
A. Measurements without dc discharge applied
The gas temperature 共rotational temperature兲 without dc
discharge applied was measured by emission spectroscopy of
the OH (A→X) transition. The OH (A→X) transition is one
of most intense emission systems in low temperature (T
⭐4000 K兲 air plasmas containing even a small amount
共⬃1%兲 of H2 or H2O. In the present experiments, the water
content of the air injected into the torch was sufficient to
produce intense OH radiation. Rotational temperatures can
be obtained from the relative intensities of two groups of
rotational lines, corresponding to the R (R 1 and R 2 ) and P
( P 1 and P 2 ) branches of the 共0,0兲 vibrational band, that form
distinct peaks at 306.8 and 309.2 nm, respectively. Figure 4
shows a simulation of the OH A→X bands obtained with the
NEQAIR2 radiation code13 which incorporates an accurate
model for this transition.14 One advantage of this rotational
temperature measurement technique is that it does not re-
quire the measured signal to be corrected for the spectral
intensity response of the detection system because the re-
sponse of the detection system used is nearly constant over
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Yu et al.
FIG. 5. Intensity ratio of the R/ P band head as a function of the rotational
temperature 共NEQAIR2 simulations for an instrumental slit function of
HWHM⫽0.21 nm兲.
the less than 3 nm spectral range of interest. The relative
intensity of the two peaks is fairly sensitive to the rotational
temperature, as can be seen from Fig. 5.
Line-of-sight OH emission spectra were recorded with
the discharge off. The amount of cold air mixing was ad-
justed to vary the temperature of the preheated air. The mea-
sured OH spectra were later fitted with NEQAIR2. As shown
in Fig. 6, the gas temperature can be varied from 1800 to
2900 K by adjusting the amount of cold air mixing.
Absolute spectral measurements were made of plasma
emission between 200 and 400 nm in order to verify that the
preheated air is chemical or thermal equilibrium. Compari-
sons are shown in Fig. 7 with spectral simulations made with
the NEQAIR2 code, assuming LTE conditions, and using the
measured temperature profile and corresponding equilibrium
concentrations for the case of 145 slpm mixing cold air. As
can be seen from Fig. 7, the numerical LTE simulations re-
produce the experimental spectrum both in shape and abso-
lute intensity, thus indicating that the preheated air 共with no
discharge applied兲 is close to LTE. Thus the electron number
density is close to the equilibrium value, when the discharge
is not applied. At 2000 K for instance, this equilibrium value
is ⬃3⫻106 cm⫺3.
FIG. 6. Measured OH A→X emission spectra without discharge applied as
a function of the amount of cold air mixing.
J. Appl. Phys., Vol. 91, No. 5, 1 March 2002 Yu et al. 2681

FIG. 9. Emission spectrum of N2 second positive (C→B) bands and com-

parisons with NEQAIR2 spectral simulations.
FIG. 7. Measured emission spectra without discharge applied, and compari-
sons with NEQAIR2 spectral simulations assuming LTE.

⫽Tr,measured) to the shape of the measured 共0,2兲,共1,3兲,共2,4兲,

B. Measurements with dc discharge applied and 共3,5兲 bands spectra, the N2 C state vibrational tempera-
ture T v ,measured was obtained.
Emission spectra were also measured with the discharge
The absolute intensity of the spectrum can then be used
applied 共discharge current of 150 mA兲, and results are shown
to determine the population of the N2 C electronic state. As
in Fig. 8. As can be seen in the figure, a factor of ⬃104
discussed in Ref. 13, the integrated intensity of a spectra line
enhancement of the emission due to NO gamma (A→X) and
is defined as
a factor of ⬃105 enhancement of the emission due to N2
(C→B) bands were observed. It is also shown in Fig. 8 that n u A ul ⌬E ul
I 共 W/cm3 sr兲 ⫽ , 共1兲
the N2 second positive system (C→B) bands overlap the 4␲
OH (A→X) feature around 308 nm. This overlap precludes
the accurate measurements of the rotational temperature where A ul (s⫺1) is the Einstein A coefficient representing the
from the OH (A→X) transition. Therefore the gas tempera- probability of a radiative transition from level u to level l,
ture 共rotational temperature兲 was measured by means of ⌬E ul is the energy difference between the level u and l, and
emission spectroscopy of the 共0,0兲 band of the N2 second n u is the population of electronic level u. The intensity of the
positive system — the N2 (C→B) transition. Line-of-sight transition gives a measurement of the number density of the
N2 emission spectra were recorded along lateral chords of the upper electronic energy level, which can then be used to
plasma. The spectra were fitted with NEQAIR2 to obtain a determine an electronic temperature T el defined by the Bolt-
rotational temperature T r . Figure 9 shows a typical experi- zmann relation
mental spectrum and NEQAIR2 fit for 150 mA discharge
current and 145 slpm of cold air mixing.
The vibrational structure of the N2 second positive (C
nu gu
⫽ exp
n0 g0
⫺␧ u
k B T el
,冉 冊 共2兲

→B) system can be used to determine the vibrational tem- where ␧ u is the electronic energy of the level u; k B is Bolt-
perature of the C state. As shown in Fig. 9, the 共0,2兲, 共1,3兲, zmann’s constant; n 0 is the population of the ground state;
共2,4兲 and 共3,5兲 vibrational sequences were utilized here. By and g u and g 0 are the degeneracies of the upper and ground
matching NEQAIR2 spectra 共calculated with T r level, respectively.
The absolute 共0,0兲 bandhead intensity I model can be ob-
tained from NEQAIR2 modeling by assuming T r
⫽T r,measured , T v ⫽T v ,measured , and T el⫽T r . Thus from Eqs.
共1兲 and 共2兲 we can obtain the measured N2 C state electronic
temperature T el,N2(C) via
I exp
I model
⫽exp 冉 冉
⫺␧ u 1
⫺
1
k B T el,N2共 C 兲 T r 冊冊 . 共3兲

Additional discharge experiments were conducted with

different gas temperatures. Figure 10 shows the measured N2
second positive system spectra and their rotational and vibra-
tional temperatures at a discharge current of 150 mA, as a
function of the amount of mixing air. It can be seen in the
figure that both the rotational and vibrational temperatures
are lower with higher amount of mixing cold air. Figure 11
FIG. 8. Line-of-sight emission spectra measured at a discharge current I shows the measured spectrum as a function of the discharge
⫽150 mA. current for 145 slpm of mixing air. As can be seen from the

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2682 J. Appl. Phys., Vol. 91, No. 5, 1 March 2002
FIG. 10. Measured N2 second positive (C→B) bands with discharge on as
a function of the amount of cold air mixing (I⫽150 mA兲.
figure, the rotational temperature remains the same at all cur-
rents, but the vibrational temperature increases with increas-
ing discharge current.
Radial rotational temperature profiles with an without
the discharge applied were measured along chords of the
plasma from Abel-inverted N2 second positive system emis-
sion spectra and OH emission spectrum, respectively. Figure
12 shows the measured radial temperature profiles at a dis-
tance of 1.5 cm downstream of the cathode 共i.e., along mid-
way between the two electrodes兲. As can be seen from the
figure, the applied discharge does not noticeably increase the
rotational temperature of the plasma at this location. Figure
13 shows the radial N2 C state electronic and vibrational
temperature profiles. On the axis of the discharge, the elec-
tronic temperature of the N2 C state reaches about 5000 K,
and the vibrational temperature is about 3000 K.
Figure 14共a兲 shows a photograph of the air plasma
plume at a temperature of approximately 2200 K in the re-
gion between the two electrodes without the discharge ap-
plied. Figure 14共b兲 shows the same region when a dc dis-
charge of 5.2 kV and 200 mA is applied between the two
electrodes. In these experiments, the distance between elec-
trodes is 3.5 cm. The bright region in Fig. 14共b兲 corresponds
to the discharge-excited plasma. As shown in Fig. 14, the
plasma plume without discharge applied appears to be homo-
geneous over a larger diameter than the plasma plume with
FIG. 11. Measured N2 second positive (C→B) bands with discharge on as
a function of discharge current for the case of 145 slpm cold air mixing.
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Yu et al.
FIG. 12. Rotational temperature profiles with and without the applied dc
discharge at 1.5 cm downstream of the bottom electrode. The temperature
profile without the discharge was measured from rotational lines of the OH
(A→X) transition. With the discharge applied, the rotational temperature
was measured from lines of the N2 (C→B) transition in the ultraviolet.
the discharge applied. However, Fig. 12 showed that the gas
temperature profile is practically the same as in the discharge
applied case. The increased brightness in Fig. 14共b兲 is due to
the emission of excited electronic states of molecular NO
and N2 共see Fig. 13兲. Thus the applied discharge increases
excited state populations without significantly increasing the
gas temperature.
C. Current density measurements
The current density at the center of the plasma was de-
termined by dividing the measured current by the effective
discharge area A * , i.e., j(r⫽0)⫽I/A * . The effective dis-
charge area is obtained from the following relation,
关 j 共 r⫽0 兲 ⫻A * 兴 ⫽ 冕 0
R
2 ␲ r j 共 r 兲 dr, 共4兲
where j(r) is the local current density and it was shown in
Ref. 1 that j(r) is approximately proportional to n e (r).
Thus, A * can be calculated as
A *⫽ 冉冕 0
R
冊
n e 共 r 兲 2 ␲ r dr /n e 共 r⫽0 兲 . 共5兲
FIG. 13. Electronic, vibrational, and rotational temperature profiles of N2 C
state with an applied discharge current of I⫽150 mA.
J. Appl. Phys., Vol. 91, No. 5, 1 March 2002
FIG. 14. 共a兲 Air plasma at 2000 K without electrical discharge. 共b兲 Air
plasma at 2000 K with applied discharge 共1.4 kV/cm, 200 mA兲. Interelec-
trode distance ⫽ 3.5 cm. The measured electron number density in the
bright discharge region is around 1012 cm⫺3.
In separate discharge experiments conducted with a ni-
trogen plasma,15 the electron number density profile n e was
measured using various techniques 共from H␤ Stark broaden-
ing and N2 first positive emission spectra兲 to calculate A *
using Eq. 共5兲. The discharge area A * was also estimated
from the full width at half maximum 共FWHM兲 of the N2
C – B 共0,0兲 bandhead intensity profile. In these nitrogen dis-
charge experiments, the effective area A * obtained with Eq.
共5兲 and the measured n e profile was found to be equal to the
effective area obtained from the N2 C – B 共0,0兲 emission in-
tensity measurement. Thus for the present air plasma dis-
charge experiments, we estimate the effective discharge area
from the spatially resolved optical measurements of N2 C
state emission. Spectroscopic measurements of N2 C – B
共0,0兲 emission with the applied discharge are shown in Fig.
15. It can be seen from the figure that the diameter 共FWHM兲
of the discharge is approximately 3.2 mm. This diameter was
monitored and found to be constant for all discharge currents
ranging from 5 to 250 mA. The discharge diameter was
therefore taken to be 3.2 mm and assumed constant through-
out the extent of the discharge.
FIG. 15. Spatial extent of the plasma produced by the discharge.
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Yu et al. 2683
FIG. 16. Measured potentials as a function of applied current in the dis-
charge section.
IV. VOLTAGE AND CURRENT MEASUREMENTS
Electrode and pin potentials were measured as a function
of the applied discharge current which was varied from 0 to
250 mA. The cathode current was measured from the voltage
drop across the 12 k⍀ ballast resistor placed in series with
the discharge 共see Fig. 3兲. There is a small difference of 7
mA between the anode and the cathode currents that was
found to be due to a current leak through the water cooling
circuit of the anode. All results reported below are based on
the measured cathode current, which is not affected by cur-
rent losses to the cooling circuit.
Figure 16 shows the measured pin voltage as a function
of the applied current along the axis of the discharge. The
potential varies approximately linearly along the axis of the
discharge, indicating that the electric field is approximately
uniform in the discharge region. The electric field measure-
ments reported here were determined from the slope of a
linear fit of the pin potentials. In the vicinity of the cathodes,
voltage falls of up to several hundred volts were observed.
These values are typical of the cathode fall voltage in glow
discharges.16
The total voltage across the discharge was also measured
as a function of electrode separation, by translating the top
electrode 共anode兲 vertically. The voltage–length characteris-
tic for a discharge current of 150 mA is shown in Fig. 17.
The lowest voltage reading as the electrodes are brought
FIG. 17. Voltage–length characteristic in the discharge region.
2684 J. Appl. Phys., Vol. 91, No. 5, 1 March 2002
FIG. 18. Measured 共symbols兲 and predicted 共solid lines兲 electrical discharge
characteristics in atmospheric pressure air plasmas generated by dc electric
discharges.
within less than 0.2 mm from one another provides an ap-
proximation to the discharge voltage at zero gap length.17,18
The value of this voltage is found to be 285 V and is inde-
pendent of the current in the current range investigated 共10–
250 mA兲. This value agrees with the cathode fall voltage
reported in the literature19,20 for glow discharges in air with a
platinum cathode. The voltage gradient in the positive col-
umn, given by the slope of the voltage-length characteristic,
is constant as the discharge length is increased. For a dis-
charge current of 150 mA, the gradient is about 1400 V/cm
共see Fig. 17兲 and is consistent with the electric field value
determined from the pin measurements.
V. RESULTS
The electric field versus current density characteristics
determined in the manner described above for the case of
140 slpm mixing air as well as several additional experimen-
tal conditions at plasma temperatures ranging from 1800 to
2900 K are shown in Fig. 18. The solid curves in Fig. 18
correspond to the predicted discharge characteristics in atmo-
spheric pressure air plasmas at temperatures of 2000 and
3000 K, respectively. A detailed description of the theoretical
work on discharge characteristics was presented in Ref. 1.
Good agreement is obtained between the measured and pre-
dicted discharge characteristics over a range of experiments
spanning over 3 orders of magnitude in current density. Fig-
ure 18 共dashed curve兲 also shows the resistive characteristic
of equilibrium air at 3000 K, given by the relation
j field E required to generate 1013 electrons/cm3 in 2000 K
E⫽ , 共6兲
␴ equilibrium,3000 K
where ␴ equilibrium,3000 K , the electrical conductivity of equi-
librium air at 300 K, is calculated as
n equil,3000 K 2
e heating in small scale stationary dc discharges where con-
e
␴ equilibrium,3000 K⫽ , 共7兲
m e¯␯ e-air
where n equil,3000
e
K
⫽6.3⫻1010 cm⫺3 and the collision fre-
quency ¯␯ e-air as shown in Ref. 1 is well approximated by
冉 冊
p
¯␯ e-air⫽ g 共 1⫻10⫺15共 cm2兲兲 , 共8a兲
kT g e
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Yu et al.
where p is the pressure 共1 atm兲, T g ⫽3000 K is the gas tem-
perature, and g e ⫽ 冑8kT e / ␲ m e is the electron thermal veloc-
ity. For the T g ⫽3000 K case, as can be seen from Fig. 18,
the predicted E versus j characteristic is close to the resistive
equilibrium characteristic for current densities below 0.2
A/cm2. In this current density range, the predicted electron
temperature remains below approximately 8000 K and
electron-impact reactions are inefficient in ionizing the
plasma. Thus the electron number density increases only by a
few percent. As the electron temperature increases, the fre-
quency of collisions increases with 冑T e , resulting in a de-
crease of the electrical conductivity of the plasma. This ex-
plains why the E versus j characteristic is higher than the
resistive equilibrium characteristic for j below ⬃0.2 A/cm2.
At higher values of the current density, where the discharge
produces a significant increase in the electron density, the
conductivity increases dramatically and the slope of the E
versus j characteristic decreases. Thus the region to the right
of the resistive equilibrium characteristic is where the dis-
charge increases the electron number density. The experi-
mental data at T g between 1800 and 2900 K all show the
turning trends of the nonresistive discharge characteristics.
Additional experimental data from Gambling and
Edels18 and Stark and Schoenbach21 are also plotted in Fig.
18. The data of Gambling and Edels were obtained in ambi-
ent atmospheric pressure air glow discharges generated be-
tween parallel electrodes made of copper or tungsten. Al-
though the authors did not report measurements of the gas
temperature, it is likely that the local gas temperature was
higher than room temperature because of Joule heating. As
the location of the transition region from high to low fields
seems to be a weak function of the gas temperature 共at least
judging from the predicted characteristics at 2000 and 3000
K兲, the data of Gambling and Edels add further support to
the predicted E/ j characteristics.
The datum from Stark and Schoenbach in Fig. 18 was
obtained in an atmospheric pressure glow discharge in air.
The discharge was produced between a microhollow cathode
and a positively biased electrode, as described in Ref. 22.
The measured gas temperature is around 2000 K, and center
electron number density is above 1012 cm⫺3. 21,23 This mea-
surement adds further support to the kinetic mechanism pre-
dictions.
The dashed line in Fig. 18 indicates the current density
corresponding to an electron number density of 1013 cm⫺3. It
can be seen that the predicted current density j and electric
atmospheric pressure air are equal to 16 A/cm 2 and 1.5 kV/
cm, respectively. The corresponding power budget, equal to
the product jE, is therefore approximately 24 kW/cm3. This
level of Joule heating may not lead to significant overall gas
duction to ambient air and to the electrodes is high. This was
the case for instance in Gambling and Edel’s experiments
where the positive column was several millimeters in length
and approximately 0.2 mm2 in area. In larger volume dc
discharges, however, it is necessary to control the effect of
Joule heating of the gas, for instance by flowing the gas
through the discharge at high velocities. For air at 2000 K
J. Appl. Phys., Vol. 91, No. 5, 1 March 2002
FIG. 19. Measured electron number densities as a function of applied cur-
rent density.
flowing through a 1 cm diam region of length 3.5 cm at a
velocity of 450 m/s, the residence time is 78 ␮s. The vibra-
tional relaxation times ␶ reported by Park,24 indicate that the
fastest vibrational relaxation rate of molecular N2 is through
collisions with atomic oxygen. The rate constant is given by
p 0 ␶ ⫽10⫺6 共atm s兲, where p 0 is the partial pressure of atomic
oxygen. In our discharge experiments, the atomic oxygen
mole fraction is less than 1%, according to our two-
temperature kinetic model1 predictions. Thus, the vibrational
relaxation time ␶ 共⬎100 ␮s兲 is larger than flow time 共78 ␮s兲.
This is consistent with the observation that significant gas
heating was not observed in the experiment. To limit gas
heating to acceptable levels for a given volumetric power, it
is desirable to flow the plasma at high velocity through the
discharge region.
An alternate way to present the results of Fig. 14 is to
plot the measured electron number density as a function of
the applied current density, which can be inferred from the
measured E – j characteristics using the following equations:
¯␯ e-air⬵ 共 P/kT g 兲 g e 共 10⫺15共 cm2兲兲 ,
n ee 2
j⫽ ␴ E⫽ E,
m e¯␯ e-air
E⬵
me
e
冑 3k 共 T e ⫺T g 兲
␦
m air
共 ¯␯ e-air兲 2 ,
where ␦ is an inelastic energy loss factor1 defined as the ratio
of total energy losses to elastic energy losses. The results,
shown in Fig. 19, confirm that the electron number density
increases by 1 order of magnitude when the applied current
density is increased by 1 order of magnitude.
VI. CONCLUSION
Investigations have been made of the mechanisms of
ionization in two-temperature air plasmas with electron tem-
peratures elevated with respect to the gas temperature. Nu-
merical simulations of these mechanisms yield the notable
result that the electron number density exhibits an S-shape
dependence on the electron temperature at fixed gas tempera-
ture. This S-shaped behavior is caused by competing ioniza-
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Yu et al. 2685
tion and charge transfer reactions. The characteristic of elec-
tric field versus current density also exhibits a nonmonotonic
dependence.1
Discharge experiments were conducted in air at atmo-
spheric pressure and temperatures ranging from 1800 to
3000 K. In these experiments, a dc electric field was applied
to flowing air plasmas with initial equilibrium electron con-
centrations. These experiments showed that it is possible to
obtain stable diffuse glow discharges in atmospheric pressure
air with electron number densities of up to 2.5⫻1012 cm⫺3,
which is up to 6 orders of magnitude higher than in the
absence of the discharge. The value of 2.5⫻1012 cm⫺3 cor-
responds to the maximum current that can be drawn from the
250 mA power supply used in these experiments. The diffuse
discharges are approximately 3.5 cm in length and 3.2 mm in
diameter. No significant degree of gas heating was noticed as
the measured gas temperature remained within a few hun-
dred Kelvin of its value without the discharge applied. Re-
sults from these experiments are in excellent agreement with
the predicted E versus j characteristics. Additional compari-
sons were made with results from glow discharge experi-
ments in atmospheric pressure ambient air by Stark and
Schoenbach,21 and Gambling and Edels.18 The measurements
of these authors are also consistent with the predicted E ver-
sus j characteristics. As these measurements were made in
the reactive region of the E versus j curve, they support our
proposed mechanism of ionization for two-temperature air.
As the power budget for dc electron heating is higher
than desired for the practical use of air plasmas in most ap-
plications, methods to reduce the power budget are currently
being explored in our laboratory. Based on the predictions of
our chemical kinetics and electrical discharge models, it is
found that a repetitively pulsed electron heating strategy can
provide significant power budget reductions by several or-
ders of magnitude with respect to dc electron heating. Re-
petitively pulsed discharge experiments are now being con-
ducted in our laboratory to verify this data.
共8b兲
ACKNOWLEDGMENT
共9兲 This work was funded by the Director of Defense Re-
search & Engineering 共DDR&E兲 within the Air Plasma Ram-
共10兲
parts MURI program managed by the Air Force Office of
Scientific Research under the cognizance of Dr. R. Barker
共Grant No. AF-F49620-97-10-316兲.
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