Numerical and Experimental Study of Atmospheric Pressure

Glows in Helium
P. Zhang, C. Anderson, J. Heberlein, U. Kortshagen
Department of Mechanical Engineering, University of Minnesota
111 Church St. S.E.
Minneapolis, Minnesota 55455 USA

ABSTRACT. In this study, we investigate atmospheric pressure glow (APG) discharges in

helium, comparing numerical simulations with experimental data. Our two-dimensional fluid
model includes the dielectric barriers and the discharge gap in the simulation domain. We
compare numerical results to space and time-resolved optical emission spectroscopy (OES)
measurements. The emission lines from He I (3s3S - 2p3P: = 706 nm) and N2 (C3u - B3g:
= 337 nm) are used to show qualitatively the distributions of electrons at various threshold
energies. The relative distribution of He (23S) within the gas gap is mapped by the observation
of the emission from N2+ ((0,0) B2u+ - X2g+: = 391 nm), which is produced through
Penning ionization involving He (23S). Both numerical and experimental results show that
the breakdown first appears at the center of the gap, followed by the axial and radial
propagation of the ionization wave. Additionally, the influence of increasing the driving
frequency manifests in a shift from a non-uniform discharge to a uniform glow discharge.
This transition is attributed to the increased density of seed electrons remaining in the
discharge gap before the subsequent breakdown. The effects of nitrogen impurities and the
Penning ionization are also discussed.
INTRODUCTION
The dielectric barrier discharge (DBD) is an atmospheric pressure discharge in which an
insulating layer covers one or both of two parallel plate or coaxial electrodes in the discharge
system [1]. DBDs exhibit a filamentary structure, characterized by individual microdischarges.
This behavior is highly transient and non-uniform over the electrode surface, hence highpressure DBDs are not suited for application that require good spatial plasma uniformity. First
demonstrated in the late 1960s [2], the atmospheric pressure glow (APG) discharge has
attracted great attention due to its diffuse, transversely uniform structure. Already APGs have
found applications in thin film deposition [3], VLSI processing [4], and biological sterilization
or decontamination [5].
Despite their uniform appearance, two-dimensional effects have been observed in APGs in
helium [6]. Using high-speed camera images, such effects as a radial spreading of the
ionization front and a secondary breakdown observed at the electrode edges were reported. In
order to study the discharge behavior in the axial direction, Tochikubo et al. [7] used timeresolved spectroscopic measurements of He I and N2 to show the distributions of high and low
energy electrons, respectively. For this work we use a similar measurement technique to study
the both the axial and radial behavior of the discharge emission species.

Numerical simulation is another tool for interpreting the underlying physics of APGs. In
order to identify the conditions essential to create a uniform glow discharge, and to investigate
the mechanism of transition to the filamentary mode, two-dimensional simulations of the
discharge initiation and comparisons with experimental results are necessary.
In the current paper, we demonstrate results of two-dimensionally resolved time-dependent
spectroscopic measurements as well as the two-dimensional numerical simulation results. The
paper is organized as follows: Section 2 describes the experimental set-up and the twodimensional model, results and their interpretation are also presented. Section 3 summarizes
the main conclusions.
PROCEDURES AND RESULTS DISCUSSION
Experimental set-up

Figure 1. Experimental apparatus.

A general schematic of the apparatus used in this study is shown in Figure 1. The details of
the discharge chamber can be found in reference [6]. For the spectroscopic measurements, the
system consists primarily of a .5 meter focal length spectrometer (SpectraPro 500, Acton
Research Corporation) and a high-speed intensified CCD camera (PIMAX, Roper Scientific).
The CCD is synchronized with the electrical signal from the discharge such that the current
maximum is defined as 0.0 s in time. The electrical signal is shown in Figure 2 noting that
the discharge current follows a similar periodic behavior as has been observed by others (see
reference [8]); a single current pulse is observed during each half cycle of applied voltage.
The emission from the discharge gap was focused onto the entrance slit of the spectrometer
using two plano-convex lenses (fL 35 cm and 45 cm). Since the slit is vertically oriented, this
focusing system allows a time sequence measurement of the discharge in the axial direction at
a single radial location. By scanning incrementally across the radial direction, the twodimensional behavior of a desired spectral emission line can be recorded. These images were
then converted to numerical ASCII format, and combined into sequential animations using
simple C commands. Prior to recording these images, the discharge is allowed to run for an
appropriate length of time to clean the dielectric surfaces of any contaminants, as well as
eliminate any long-range transient behavior. During the measurement process, great care was
taken to ensure that the synchronization between the CCD and discharge current remained
accurate and constant.

Fig. 2 Electrical signal from APG.

Two-dimensional fluid model
z

Dielectric Plates

electrode
Gap

r
-3

-2

-1

Figure 3. Numerical simulation domain.

A two-dimensional fluid model has been developed for the simulation of APGs. The
simulation domain includes two dielectric barriers and the discharge gap as shown in Fig. 2.
The electrodes with 2-cm radius are embedded in dielectrics. The gap is filled with
atmospheric-pressure helium. Assuming azimuthal symmetry, cylindrical coordinates (r-z) are
used.
The model involves the self-consistent solution of Poisson equation for electric field and the
continuity and momentum equation for all the species. The momentum equations are
simplified by using the drift-diffusion approximation. Due to the small leak rate of the
experimental system, the known effects of nitrogen impurities must be considered in the
simulation of a helium discharge. The following species are then used for the model: electrons
(e-), atomic and molecular helium ions (He+, He2+), helium metastables (He*), and molecular
nitrogen ions (N2+). Here helium excited states of 23S and 21S are lumped into one single state
for simplification (denoted He*). The reactions and the corresponding rate coefficients are the
same as in the ref [9].
The secondary electron emission at the dielectric surface due to ion bombardment is
regarded as the main source for self-sustaining the glow discharge. The space charge
deposited on the plates is obtained from the drift-diffusion flux to the dielectrics. The surface
recombination coefficient of the electron and ions is set to 1 for simplification.
The transport terms in the continuity equations are discretized using the ScharfetterGummel exponential scheme [10] on a set of non-uniform meshes. To increase the timestepping efficiency, an adaptive time step and a semi-implicit time integration scheme [11] are
3

used. All the numerical simulations were implemented on an IBM Power4 supercomputer at
the University of Minnesota Supercomputing Institute. Simulations were run until a periodic
solution was reached, usually occurring after 8-10 AC cycles.
Experiment results
The applied signal voltage and frequency for the case presented was 1.9 kV at 15 kHz. The
dielectric plates used were 0.635 mm thick alumina, separated by a fixed gap distance of 6.35
mm. Figures 4-6 show the two-dimensional spectral emissions from the three lines chosen for
this study; namely He I (706 nm), N2 (337 nm), and N2+ (391 nm).
From He I emission (Figure 4), with its high threshold energy (24.8 eV), we can observe
qualitatively the regions of high electric field strength in the gap. This line emission also
indicates the instantaneous production rate of He* metastable states during the discharge pulse.
It is apparent that the initiation of the cathode layer is in the center region, and propagates
radially outward with time. This sheath quickly collapses in the center, so the profile takes on
a ring-like structure as it ultimately decays. By 3.0 s after the current maximum, the sheath
has almost completely vanished.
In order to observe the distribution of lower energy electrons throughout the gap region, we
have measured the emission from N2 (Figure 5). In addition to the intensity seen near the
momentary cathode, there is significant intensity in the positive column region where the
electric field is much weaker.
With the known effect of Penning ionization in this system, we can observe the relative
distribution of He* metastables from the emission of N2+ at 391 nm (Figure 6). Again the
profile shows that the emission is initiated in the center region, and spreads radially outward
in time, as with He I at 706 nm. However, in this case the emission remains strong in the
center, as well as showing significant intensity further into the gap region. In this way, the
emission from N2+ shows the cumulative effect of the production of He* metastables.

Figure 4. He I line emission at 706 nm.

Figure 5. N2 line emission at 337 nm.

Figure 6. N2+ line emission at 391 nm.

Model results
As an initial condition for the model, the electron density is set equal to 106 cm-3, and is
distributed uniformly in the gap. It takes several AC cycles to build up the electron density
and to initiate the gas breakdown. In this way, the influence of the assumed initial electron
density can be reduced. Generally, 8-10 voltage cycles are required to reach a steady state
condition. The two-dimensional plots presented here are all obtained under steady state.
The evolution of the electron density profile (Figure 7) mirrors the ionization processes in
the discharge. The breakdown first appears in the center of the gap region, followed by the
fast axially propagation. The radial movement of the ionization wave becomes more
pronounced close to the dielectrics, where a sheath rapidly develops.
0.6

Gap [cm]

Gap [cm]

0.6
0.4
0.2

Gap [cm]

0.4
0.2

0.4
0.2
0

0.6

0.6

Gap [cm]

0.4
0.2

0.4
0.2

0.6

0.6

Gap [cm]

Gap [cm]
Gap [cm]

0.2
0

Gap [cm]

0.4

0.4
0.2
0

0.5

1.5

2.5

Radius [cm]

0.4
0.2
0

Excitation rate of He*

0.5

1.5

2.5

Radius [cm]

ne
5.0E+09 9.0E+09 1.6E+10 2.9E+10 5.1E+10 9.2E+10 1.6E+11

Figure 7. Electron density evolution.

1.0E+06 8.4E+06 7.0E+07 5.8E+08 4.9E+09 4.1E+10 3.4E+11 2.9E+12 2.4E+13 2.0E+14

Figure 8. Generation rate of He*.

The helium metastable production rate is shown in Figure 8. Before the breakdown, the
helium metastables generation is low and the peak is located some distance away from the
cathode. After the gas breakdown, due to the formation of sheath, helium generation rate is
increased and the peak moves to the cathode. The radial propagation of the distribution is also
5

observed. The result is qualitatively consistent with the experiment. Figure 9 shows the
electron temperature distribution during these four sequences. The collapse of the cathode
layer and the formation of the sheath can be clearly seen. It should be pointed out that the
local maximum at the edge of the electrodes in both figures are mainly due to the edge effect
of the finite length of the electrodes.
Gap [cm]

0.6
0.4
0.2

Gap [cm]

0.4
0.2
0

Gap [cm]

0.6
0.4
0.2
0

Gap [cm]

0.6
0.4
0.2
0

0.5

1.5

2.5

Radius [cm]
Te
5.0E-01 7.2E-01 1.0E+00 1.5E+00 2.1E+00 3.1E+00 4.4E+00

Figure 9. Electron temperature distribution.

The existence of nitrogen impurities has a large effect on the discharge behavior, manifested
in a decrease in the gas breakdown voltage due to Penning ionization. As pointed out in
reference [8], high pre-ionization at a low electric field through Penning ionization is
important for obtaining a glow discharge. To study this effect of pre-ionization, we
intentionally increased the recombination coefficient of the nitrogen molecular ions to =
5x10-6 cm3 s-1. Since the recombination process is dominant during post-glow, using a higher
recombination rate will decrease the electron density in the gap before the next breakdown, i.e.
decrease the pre-ionization level. The result is shown in Figure 10; a filamentary discharge
appears as seen in Figure 10(a). Figure 10(b) shows the non-uniform distribution of the
surface charge on the powered dielectric.
For a filamentary discharge, if we increase the driving frequency, holding all other
parameters constant, the surface charge distribution becomes uniform, and the discharge
appears diffuse once again (see Figure 11). Two reasons for this are: (1) the pre-ionization
level is increased because of the reduced time for recombination during discharge pulses. As a
result the seed electron density before the breakdown in this case increases from less than 109
to 1010 cm-3. (2) The number of filaments increases with the driving frequency. The
overlapping of these filaments results in a uniform discharge, which we will discuss elsewhere.

2E-09

4.5s

0
3.0 s
2

[ C/cm ]

-2E-09

-4E-09
1.5s

-6E-09

-8E-09
0 s

-1E-08
0

0.5

1.5

2.5

Radius [cm]

(a)

(b)

Figure 10. (a) Electron density profile evolution and (b) surface charge density on the
powered dielectric. = 5x10-6 cm3 s-1, f = 15 kHz for both plots.

Gap [cm]

0.6

0s

0.4
0.2

1.5E-08

18s

1E-08
9s

0.4
0.2

12 s

5E-09
2

[ C/cm ]

Gap [cm]

0.6

Gap [cm]

0.6

18s

0.4
0.2

0
6s

-5E-09

Gap [cm]

0.6

36s

0.4

-1E-08
0 s

0.2
00

0.5

1.5

2.5

Radius [cm]

-1.5E-08

0.5

1.5

2.5

Radius [cm]
ne: 5.0E+09 7.5E+09 1.1E+10 1.7E+10 2.6E+10 3.9E+10 5.8E+10 8.8E+10 1.3E+11 2.0E+11

(a)

(b)

Figure 11. (a) Electron density profile evolution and (b) surface charge density on the
powered dielectric. = 5x10-6 cm3 s-1, f = 25 kHz for both plots.
CONCLUSIONS
We have studied an APG in helium using both experimental and numerical simulation
methods. From the OES measurements, we have seen qualitatively the distributions of high
and low energy electrons, as well as helium metastable atoms. The results show evidence of
Penning ionization of N2. Perhaps most significant is the observation of a ring-like cathode
layer, initiating at the center and moving outwards in time. A similar phenomenon is seen
from the numerical simulations. Further results from the model show that sufficient preionization between half cycles is necessary in sustaining a uniform discharge. This is provided
primarily by helium metastables, owing to their slow decay and long diffusion time. The pre7

ionization level is also affected by the driving frequency. Increasing the frequency favors a
transition from a filamentary to homogenous glow discharge.
ACKOWNLEDGEMENTS
This work is supported by the Department of Energy under grant DE-FG02-00ER54583 and
by the University of Minnesota Supercomputing Institute.
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