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Analysis of microdischarges in asymmetric dielectric barrier discharges in argon

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2013 J. Phys. D: Appl. Phys. 46 355203

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IOP PUBLISHING JOURNAL OF PHYSICS D: APPLIED PHYSICS
J. Phys. D: Appl. Phys. 46 (2013) 355203 (15pp) doi:10.1088/0022-3727/46/35/355203

Analysis of microdischarges in
asymmetric dielectric barrier
discharges in argon
M M Becker, T Hoder, R Brandenburg and D Loffhagen
INP Greifswald e.V., Felix-Hausdorff-Str. 2, 17489 Greifswald, Germany
E-mail: markus.becker@inp-greifswald.de

Received 25 April 2013, in final form 1 July 2013

Published 14 August 2013
Online at stacks.iop.org/JPhysD/46/355203

Abstract
Theoretical and experimental studies of two different discharge modes in asymmetric dielectric
barrier discharges in argon at atmospheric pressure have been performed. The first mode
appears to be the well-known filamentary microdischarge with non-striated positive column
whereas the second mode is characterized by discharge instabilities and the appearance of
striations. Both experiment and model calculations predict a transition from the first mode to
the second mode when the applied voltage amplitude is increased above approximately 2 kV.
The reliability of the employed fluid model is confirmed by comparison of the current–voltage
characteristics obtained by model calculations and measurements for different applied voltage
amplitudes. The results of the model calculations point out that in the second discharge mode
the ionization of excited argon atoms prevents the total recombination of charge carriers
between two subsequent discharge events. This leads to the occurrence of the memory from
one discharge to the following one, which plays an important role in mode transition.
(Some figures may appear in colour only in the online journal)

1. Introduction different discharge modes takes place. Phenomena like period

Besides the fact that dielectric barrier discharges (DBDs)
are of high technological importance in many applications,
their physics and chemistry is very interesting from the
physical point of view. In particular, the formation of
structures and instabilities as well as the study of volume
and surface processes is an issue of high complexity. It is
well known that different discharge modes can occur in DBDs
at atmospheric pressure including diffuse, filamentary and
mixed modes [1–3]. In contrast to the typical filamentary
regime, which is characterized by a large number of individual
discharge channels, the plasma of a diffuse barrier discharge
covers the entire electrode area uniformly [2]. Two different
diffuse modes can occur, namely, the atmospheric pressure
Townsend discharge and the atmospheric pressure glow
discharge [2, 4–6]. The mentioned discharge modes occur in
dependence on the cell geometry [7], amplitude and frequency
of the applied voltage [2, 8, 9], gas composition [2, 3] and gas
pressure [1], respectively. Quite complex discharge dynamics
can occur when periodic or even chaotic switching between
multiplication, mixed-mode oscillations and transitions to
chaotic states in electrical discharges in gases have been
observed in experimental [10–14] as well as theoretical
[15–19] investigations. In most cases, a detailed analysis of the
discharge properties is necessary to explain such behaviour.
Recently, the alternate occurrence of two different
discharge modes in a DBD in atmospheric pressure argon
has been observed experimentally [20, 21]. The first mode
appears to be a normal filamentary microdischarge with non-
striated plasma channel known from the literature [22–24],
while the second mode is characterized by a comparatively
low discharge current exhibiting a multi-peak structure and
a striated positive column. Figure 1 represents typical
pictures of non-striated (a) and striated (b) microdischarges
in argon. Unlike striations in low-pressure plasmas [25, 26],
striated structures in discharges at atmospheric pressure are
rarely observed and their generation mechanisms are not
fully understood [20, 21, 27–31]. It should be noted that the
appearance of the striated structure is not related to the presence
of the metallic electrode in asymmetric barrier discharge

0022-3727/13/355203+15$33.00 1 © 2013 IOP Publishing Ltd Printed in the UK & the USA
J. Phys. D: Appl. Phys. 46 (2013) 355203
Figure 1. ICCD pictures of single non-striated (a) and striated (b) discharge events in an asymmetric DBD in argon for metal cathode and
dielectric anode (both in M-D+ configuration).
arrangements, where one electrode is covered by a dielectric.
Indeed, in the case of symmetric barrier discharges, where both
electrodes are covered by a dielectric, the striated structure
has been found as well [21]. However, the appearance of
striated microdischarges in the symmetric setup was rare and
unstable [21].
In the present paper the two discharge modes are analysed
in more detail with the aid of measurements and fluid modelling
describing self-consistently the spatiotemporal development
of microdischarges in the DBD arrangement considered.
The experimental studies were performed using the same
equipment as published in [21]. A brief description of the
experimental setup is given in section 2.
For the theoretical description of the discharge a fluid-
Poisson model was adapted. Due to the much higher
computational efficiency of fluid models compared to a
kinetic description, the former are preferred for modelling of
atmospheric pressure discharges. In the literature, global [32]
as well as spatially one-dimensional [33, 34], two-dimensional
[35–37] and three-dimensional [38] fluid descriptions are
considered for modelling of DBDs. Two- and three-
dimensional descriptions provide the possibility to study both
the axial and the radial discharge structure. But simple reaction
kinetics, taking into account the most relevant excitation and
ionization processes, only, has to be applied then to keep the
computing time within a feasible limit. The advantage of
global and spatially one-dimensional models is that all relevant
collision and radiation processes can be taken into account
without increasing the computing time too much. Therefore,
a one-dimensional fluid description is preferred here which
allows both the analysis of the axial plasma structure and of
the reaction kinetics. Details of the fluid model are given in
section 3.
Measurements as well as model calculations were
performed for a wide range of applied voltage amplitudes.
It is analysed in detail how the amplitude of the applied
voltage influences the basic characteristics and the stability
of the discharge and which effects give rise to the multi-peak
discharge mode that has been observed in the experiment.
The experimental and theoretical results for the current-
voltage characteristics of the discharge under consideration
are compared and discussed in section 4.1. Furthermore, the
spatiotemporal evolution of particle densities, electric field
and ionization processes is investigated in section 4.2 with the
assistance of the modelling results.
2
M M Becker et al
Figure 2. Electrode setup with electrode gap d = 1.5 mm and
thickness of dielectric layer
= 0.5 mm.
2. Experimental setup
The experimental investigations were performed in a sealed
glass chamber as shown in figure 2. The mutual distance of
the pure metal (stainless steel) and alumina covered electrode
was d = 1.5 mm. The metal electrode was energized by
high voltage and the alumina covered electrode was grounded.
The thickness of the dielectric layer was
= 0.5 mm. The
curvature of both electrode tips was 2 mm. The sealed glass
chamber was evacuated to high vacuum (10−5 mbar), heated
to 700 K for several hours (baked out to reduce residual
gaseous impurities) and then filled with argon gas of purity
of 99.9999% to atmospheric pressure. In order to ensure
direct comparability with the model neglecting gas flow, the
experiments were performed without gas flow as described
in [21]. The barrier discharge was generated by a 60 kHz
sinusoidal voltage using a Softal AT6003 transformer, QSC
Powerlight 9.0 PFC amplifier, and Toellner TOE 7711A
function generator. The voltage and current characteristics
were measured by Tektronix probes P6015A and CT-1,
respectively. All signals were recorded by a Tektronix TDS
3052 oscilloscope. An intensified charge-coupled device
(iCCD) DiCam Pro 25 SVGA camera was used in combination
with a Questar QM 100BK7 far-field microscope to study
the two-dimensional structure of a single microdischarge
simultaneously with identical current pulse measurements.
3. Fluid description of microdischarges
3.1. Basic relations
For the theoretical description of the spatiotemporal
development of microdischarges, a time- and space-dependent
J. Phys. D: Appl. Phys. 46 (2013) 355203 M M Becker et al

Table 1. List of argon species considered in the model.

Index Species Energy level (eV)
∆
1 Ar[1p0 ] 0
2 Ar[1s5 ] 11.55
3 Ar[1s4 ] 11.62
x=0 x x=d 4 Ar[1s3 ] 11.72
5 Ar[1s2 ] 11.82
6 Ar[2p] 12.90
7 Ar[2p
] 13.28
8 Ar ∗ [hl] 13.84
9 Ar + 15.76
powered grounded
10 Ar2∗ [3 u+ , v  0] 9.76
electrode electrode 11 Ar2∗ [1 u+ , v  0] 9.84
Figure 3. Spatially one-dimensional discharge geometry with 12 Ar2∗ [3 u+ , v = 0] 11.37
electrode gap d = 1.5 mm and thickness of dielectric layer 13 Ar2∗ [1 u+ , v = 0] 11.45

= 0.5 mm. 14 Ar2+ 14.50

hydrodynamic model was employed taking into account the

spatially one-dimensional discharge geometry depicted in
figure 3. The one-dimensional description considering the
axial component x of the plasma, only, assumes in a first
approach that the main characteristics of the discharge are not
influenced by radial effects.
The nonlinear system of partial differential equations
comprises the continuity equations
∂t ns (x, t) + ∂x s (x, t) = Ss (x, t) (1)
for particle densities ns of considered species s listed in table 1,
the electron energy balance equation
∂t we (x, t) + ∂x Qe (x, t) = −e0 E(x, t)e (x, t) + S̃e (x, t)
(2)
determining the spatiotemporal evolution of the electron
energy density we and Poisson’s equation providing self-
consistently the electric potential φ and the electric field
E(x, t) = −∂x φ(x, t) according to
1

− ∂x2 φ(x, t) = qs ns (x, t), (3)
ε0 s
where ε0 denotes the permittivity of free space and qs is
the particle charge. The particle fluxes s and the electron
energy flux Qe in the x-direction are given in drift-diffusion
approximation by [39]
 
s (x, t) = −∂x Ds (x, t)ns (x, t)
 
+sgn qs bs (x, t)E(x, t)ns (x, t), (4)
 
Qe (x, t) = −∂x D̃e (x, t)ne (x, t) − b̃e (x, t)E(x, t)ne (x, t).
(5)
Here, Ds and bs denote the diffusion coefficient and the
mobility of species s, respectively and D̃e and b̃e are the
diffusion coefficient and the mobility for energy transport of
electrons. The function sgn(qs ) gives the sign of the particle
charge qs . The changes of particle densities and electron
energy density due to collisional and radiation processes are
included by means of the source terms Ss in the particle balance
equation (1) and the term S̃e in the electron energy balance
equation (2). The first term on the right-hand side of (2) denotes
the power input from the electric field.
3.2. Reaction kinetics model
To achieve an adequate description of atmospheric pressure
argon plasmas, atomic and molecular argon ions as well as
seven excited atomic and four excited molecular argon states
were taken into account. Table 1 lists all species that are
considered in the model in addition to the electron component.
The lumped states Ar[2p] and Ar[2p
] include the 2p10 –2p5 and
2p4 –2p1 levels, respectively. All higher energetic atomic argon
levels are summarized in Ar ∗ [hl] according to Hayashi [40].
The reaction kinetic scheme takes into account 70 electron
collision processes. Besides elastic collisions contributing
directly to the electron energy balance equation (2), it includes
excitation, deexcitation, ionization and recombination
processes with rate coefficients depending on the mean electron
energy ε̄ = we /ne . In addition, 20 radiation and 24 heavy
particle collision processes are considered. A list of all
processes is given in the appendix in tables A1 and A2.
The mean energy dependent transport coefficients for
electrons as well as the rate coefficients of elastic collisions,
exciting, de-exciting and ionizing collision processes have
been obtained by solution of the stationary, spatially
homogeneous electron Boltzmann equation in a convergent
multi-term approach using a modified version of the method
presented in [41]. It has been adapted to take into account
nonconservative electron collision processes. More details
on the particular form of the coefficients as well as graphical
representation are provided in [42]. In order to avoid numerical
instabilities, the common simplified expressions [43]
b̃e = 53 ε̄be , (6)
D̃e = 53 ε̄De (7)
are used for the electron energy transport coefficients.
The mobility of atomic and molecular argon ions is
determined as function of the reduced electric field E/N during
the model calculations using the data given in [44] and [45],
respectively, where N is the total gas density. Furthermore, it is
assumed that the ion diffusion coefficients Di satisfy Einstein’s
relation [46]
kB Tg bi
Di = , (8)
e0

3
J. Phys. D: Appl. Phys. 46 (2013) 355203 M M Becker et al

where kB is the Boltzmann constant, e0 denotes the elementary and 

charge and Tg is the gas temperature which is assumed to be 8kB Te
constant during the discharge event. To estimate the maximum ṽth,e = 2kB Te , (14)
π me
effect caused by gas heating during one discharge pulse, a
balance equation for the neutral gas temperature neglecting respectively, assuming a Maxwellian energy distribution
temperature loss due to heat transfer was solved. It was function at the boundaries with kB Te = 2ε̄/3. In equation (12),
found that due to the short duration of the microdischarges ε̄γ = 2 eV denotes the mean energy of secondary electrons.
the maximum increase of temperature in a single filament is The electron reflection coefficient is set to 0.3 at the metallic
smaller than 0.5 K. For metastable argon atoms the diffusion surface and it takes the value 0.7 at the dielectric [48].
coefficient is set to N Dm = 1.7×1018 s−1 cm−1 in accordance Approximately, the secondary electron emission coefficient
with [44]. The diffusive transport of excited particles in for argon is 0.07 at metallic surfaces [44, 49] and 0.02 at
radiative argon states has been neglected due to their short an alumina covered surface [50]. Recently it has been
lifetimes. pointed out that due to charge accumulation the secondary
electron emission coefficient of a dielectric changes during
3.3. Boundary conditions different stages of the discharge [51]. However, the accurate
description of this effect is an ambitious task and left for future
In order to solve the system of partial differential equations (1)– investigations.
(3) taking into account the drift–diffusion fluxes (4) and (5), At the powered electrode located at x = 0 a sinusoidal
an adequate set of boundary conditions has to be added. For voltage Va is applied in accordance with the experimental
the heavy particle densities as well as for the particle and setup. The effect of surface charge accumulation on top of
energy densities of electrons, boundary conditions according to the alumina covered grounded electrode is described by Gauss
Hagelaar et al [36, 47] have been applied. For heavy particles law [35, 36]
h with the mass mh the boundary condition applied at the
electrodes takes the form εD ED (d, t) · ν − ε0 E(d, t) · ν = σ (t) (15)
1 − rh  1 
h · ν = |sgn(qh )bh Enh | + vth,h nh . (9) for the space-charge field E and the electric field ED inside the
1 + rh 2
dielectric. Since charge carriers are almost absent within the
Here, ν is equal to −1 at x = 0 (powered electrode) and dielectric [52], the electric field ED is determined by means of
equal to 1 at the dielectric surface in front of the grounded the Laplace equation
electrode located at x = 2 mm. In accordance with [48],
the reflection coefficient rh for ions is set to 5 × 10−4 and ∂x ED = −∂x2 φD = 0. (16)
5 × 10−3 at the metallic and the dielectric covered electrode
surface, respectively. For metastable argon atoms the reflection Equation (15) is used as boundary condition for the electric
coefficient is set to 0.3. Boundary condition (9) takes potential at x = d. The surface charge density σ results from
into account the partial reflexion of particles considering a particle currents striking the dielectric. It is incorporated by
drift–diffusion flux as well as a thermal flux with thermal the equation
velocity 

8kB Tg ∂t σ (t) = qs s (d, t) · ν, (17)
vth,h = . (10) s
πmh
which includes the legitimate assumption that the surface
The boundary conditions for electrons having the mass
charge density does not diffuse along the surface on time scales
me look almost the same. In addition to partial reflection, the
emission of secondary electrons due to ion bombardment at relevant for this study [53].
the walls with the secondary electron emission coefficient γ
has been considered 3.4. Spatiotemporal discretization
 in the form 
1 − re 1
e · ν = |b |
e Ene + vth,e ne The coupled system of partial differential equations (1)–(5),
1 + re 2 equipped with the boundary conditions discussed in
2
section 3.3, is discretized in time and space by means of
− γ max(i · ν, 0), (11)
1 + re finite-difference methods. Spatial discretization of the drift-
i
  diffusion equations for charge carrier densities as well as
1 − re 1
Qe · ν = b̃e Ene + ṽth,e ne the electron energy balance equation (2) has been performed
1 + re 2 by an exponential scheme based on the Scharfetter–Gummel
2

− γ ε̄ γ max(i · ν, 0). (12) method [54]. The discretization scheme has been adapted to
1 + re i
treat diffusion of electrons in the consistent form −∂x (De ne )
The particle and energy thermal velocities of electrons are rather than neglecting the contribution of thermal diffusion
approximated as −ne ∂x De . The central-difference method [55] has been used
 for spatial discretization of Poisson’s equation as well as for
8kB Te the balance equations of metastable argon atoms. For the
vth,e = (13)
πme temporal discretization an iterative time-stepping scheme has

4
J. Phys. D: Appl. Phys. 46 (2013) 355203 M M Becker et al

50 50
V = 1.5 kV V = 1.6 kV
0 0
25 25
Current [mA]

Current [mA]
0 0

−25 −25

−50 −50

50 50
V = 1.9 kV V = 2.0 kV
0 0
25 25
Current [mA]

Current [mA]
0 0

−25 −25

−50 −50

50 50
V0 = 2.2 kV V0 = 2.5 kV
25 25
Current [mA]

Current [mA]
0 0

−25 −25

−50 −50
−2 −1 0 1 2 −2 −1 0 1 2
Applied voltage [kV] Applied voltage [kV]

Figure 4. Trajectories of measured discharge dynamics in phase space of applied voltage and discharge current for different amplitudes of
the applied voltage.

been applied. Further details on the discretization scheme
considered are given in [56].
The size of the time step is adaptively determined to keep
the relative discretization error in the mean electron energy
below the tolerance of 10−4 . The model calculations have been
performed using 900 non-equidistant intervals for the spatial
grid, which is quadratically refined towards the boundaries to
resolve steep gradients in front of the electrodes.
4. Results and discussion
Measurements and model calculations were performed for
applied voltage amplitudes V0 between 1.5 and 2.5 kV. The
driving frequency f = 60 kHz corresponding to a period of
T = 16.7 µs and the argon pressure of 1 atm were not changed
throughout the investigations. For the model calculations a
constant gas temperature of 300 K has been assumed.
4.1. Current–voltage characteristics
In order to explain the occurrence of the different discharge
modes observed in the asymmetric DBD arrangement under
consideration, the influence of the voltage amplitude on the
current-voltage characteristics has been investigated. Figure 4
represents measured data in phase space of applied voltage
and discharge current for different voltage amplitudes V0 . It
becomes obvious that for low applied voltages near the burning
voltage of about 1.5 kV the discharge dynamics is deterministic
that way that the discharge ignites at virtually fixed values
of the externally applied voltage. The discharge current is
characterized by strong current peaks during the discharge
events and small values of the order of the displacement current
throughout the remaining time. This normal discharge mode
is well known from literature [22]. Between 1.6 and 2 kV
a transition in the discharge dynamics takes place. When
the applied voltage is increased, the discharges become more
and more unstable. Microdischarges ignite no longer at
distinct values of the applied voltage, and current pulses with
several maxima and minima are observed. Furthermore, the
positive column in this discharge mode is characterized by the
appearance of striations as discussed in [21]. Similar transition
to quasi-periodic and chaotic discharge modes in DBDs are
investigated in [14, 17, 18]. However, the mechanisms leading
to mode transition and the observed striated structures are not
yet fully understood [14].
In order to demonstrate that fluid modelling is able
to capture the experimentally observed mode transition,

5
J. Phys. D: Appl. Phys. 46 (2013) 355203
V0 = 1.5 kV V0 = 2 kV
2.5
2 40
1.5
1 20
Voltage [kV]
0.5
0 0
−0.5
−1
−1.5
−2
−2.5
0 10 20 30 40 50 0 10 20 30 40 50
t [µs] t [µs]
Figure 5. Comparison between measured (——) and calculated (- - - -) discharge current for different amplitudes of the applied
voltage (— · —).
calculations using the measured voltage course Va as input
have been performed. Calculated and measured results for
the temporal evolution of the discharge current at voltage
amplitudes of 1.5, 2 and 2.5 kV are directly compared in
figure 5. At V0 = 1.5 kV the model predicts the same
stable discharge dynamics as observed in the experiment. In
positive half-periods, where the dielectric electrode is the
cathode (M+D-), even the quantitative agreement between
model prediction and experiment is excellent. In negative
half-periods, where the metallic electrode is the cathode (M-
D+) the model overestimates the amplitude of the discharge
current peaks by a factor of two. This is due to the fact that
the surface area of a hemisphere with 2 mm radius (curvature
of electrode tips) has been used to estimate the discharge
current from the calculated current density. In M+D- mode,
the footprint of the discharge at the dielectric covered electrode
spreads widely over the electrode surface whereas in M-D+
mode only a fraction of the surface area is covered by the
discharge [21].
At 2 and 2.5 kV an increase of the discharge current
between subsequent discharge events takes place. It is worth
noting that this effect results from an increase of the plasma
current and is not caused by a growth of the displacement
current ranging between 0.1 and 0.2 mA. The comparison
of experimental and modelling results points out that the
qualitative change in the current form is principally captured
by the model.
In order to exclude effects resulting from noise of the
measured applied voltage, the further analysis of the discharge
characteristics by means of model calculations is performed
by applying the sinusoidal voltage Va = V0 sin(2π t/T ) at
the powered electrode. Modelling results of the periodic
behaviour for V0 = 1.5, 2 and 2.5 kV are represented in
figure 6. In the upper part of this figure the applied voltage
Va , the voltage drop across the gas gap Vg and the memory
6
M M Becker et al
V0 = 2.5 kV
Current [mA]
−20
−40
0 10 20 30 40 50
t [µs]
voltage Vm = Va − Vg , which is the voltage drop across
the dielectric layer caused by the charge accumulated on the
dielectric due to the previous discharge [4], are shown. The
lower part illustrates the temporal evolution of the discharge
current density and the surface charge density accumulated
on the dielectric surface. For all voltage amplitudes, the
modelling results exhibit a reasonable transient behaviour.
The magnitude of the gap voltage increases until the ignition
voltage of approximately 1.5 kV is reached and a discharge
event takes place. The ignition voltage predicted by the
model is in good agreement with the experiment. A single
discharge event per half-period is found which is characterized
by a strong increase of the magnitude of the current density.
Depending on the polarity, positive or negative charges are
accumulated at the dielectric surface and the magnitude of the
gap voltage decreases strongly. These mechanisms lead to an
immediate quenching of the discharge. The further increase
of the magnitude of the applied voltage Va and of the gap
voltage Vg after the discharge event causes the generation of
new charge carriers. Hence the discharge current magnitude
increases between subsequent discharge events for V0
2 kV
in accordance with experimental findings.
The corresponding discharge dynamics in the phase space
of gap voltage and discharge current density is shown in
figure 7. Starting from Vg = 0, at first the transient behaviour
is very similar for all voltage amplitudes. When the discharge
takes place, the magnitude of the discharge current strongly
increases and at the same time the gap voltage decreases.
Thus, the discharge has a negative differential conductivity
and becomes unstable [17, 57]. The small differences in the
ignition voltage for the different applied voltage amplitudes
are caused by memory effects as discussed below.
After the quenching of the first discharge event differences
between the discharge dynamics at V0 = 1.5 kV and the
discharges at higher V0 occur. The insets in figure 7 make
J. Phys. D: Appl. Phys. 46 (2013) 355203 M M Becker et al

V0 = 1.5 kV V0 = 2.0 kV V0 = 2.5 kV

2
Voltage [kV]

1
0
−1
−2
Current density [mA/cm2]

Surface charge [nC/cm2]

200
t0 t0 40
100 20
0 0
−100 −20
−40
−200
0 0.5 1 1.5 0 0.5 1 1.5 0 0.5 1 1.5
t/T t/T t/T
Figure 6. Top: temporal variation of applied voltage (- - - -), gap voltage (——) and memory voltage (— · —) for different amplitudes of
the applied voltage; bottom: corresponding temporal variation of current density (——) and surface charge density (- - - -).

0
150 −5
−10
Current density [mA/cm2]

100 −15
−20
50
−0.7 −0.6 −0.5 −0.4 −0.3 −0.2

0
20
−50
15
−100 10
5
−150 0
0.2 0.3 0.4 0.5 0.6 0.7

−1.5 −1 −0.5 0 0.5 1 1.5

Gap voltage [kV]
Figure 7. Calculated current-voltage characteristics in phase space for V0 = 1.5 kV (——), V0 = 2.0 kV (- - - -) and V0 = 2.5 kV (— · —).
Arrows indicate the temporal direction.

clear that during the negative half-period the magnitude a negative differential conductivity between two subsequent
of the current density of the discharges at V0 = 2 and microdischarges. Experimental and theoretical investigations
2.5 kV increases again before a change in polarity takes of similar barrier discharges have pointed out that bifurcation
place. The stability of the discharges is again affected by the and period-doubling are likely to occur in case of a negative
occurrence of negative differential conductivity. Qualitatively differential conductivity [17, 57]. Because of memory
the same behaviour can be observed during the positive effects, the discharge current in a particular period depends
half-period for the discharge at V0 = 2.5 kV. By contrast, strongly on the previous discharge and it is particularly
the current density of the discharge at V0 = 1.5 kV does influenced by the surface charge density and the density of
not increase again in both half-periods before the polarity charge carriers in the discharge volume [58]. Therefore,
changes and no negative differential conductivity occurs. it is not to be expected that the experimental observations
These findings indicate that the instabilities found in the exhibit exactly the same dynamic behaviour as predicted by
experiments at V0
2 kV (see figure 4) are triggered by the model.

7
J. Phys. D: Appl. Phys. 46 (2013) 355203
Figure 8. Temporal variation of the current density (——) and gap voltage (- - - -) (top) and spatiotemporal variation of the electron density
(bottom) at applied voltage amplitudes V0 = 1.5 kV (left) and V0 = 2.5 kV (right) (instantaneous anode at x = 0, cathode at x = 1.5 mm).
In order to analyse the dependence of the observed
mode transition on the thickness of the dielectric, additional
calculations for different thicknesses
were performed. As
expected, it was found that the voltage amplitude at which
the transition to the unstable mode occurs decreases with
decreasing thickness of the dielectric. The decrease of
from
0.5 to 0.25 mm causes the occurrence of negative differential
conductivity already at V0 = 1.5 kV.
Furthermore, in the present study it was found that the
discharge dynamics at amplitudes in the range from 2 to 2.5 kV
is very sensitive with respect to changes in the reaction kinetics
of metastable argon atoms Ar[1s5 ] and Ar[1s3 ]. In [18, 19]
model calculations of DBDs in argon at atmospheric pressure
using a very simple argon model taking into account direct
ionization of ground state atoms only are reported. In these
studies bifurcation and period-doubling phenomena have been
found. A quite similar behaviour has also been obtained by
the present model, if chemo-ionization processes involving the
energetically first metastable state Ar[1s5 ] are considered only,
i.e. if the reactions R75 to R80 in table A2 are neglected [59].
4.2. Spatiotemporal discharge behaviour
In order to understand the differences in the discharge
mechanisms at low and higher amplitudes of the applied
voltage the spatiotemporal discharge behaviour obtained by
the model calculations for V0 = 1.5 kV and V0 = 2.5 kV is
8
M M Becker et al
analysed. Figure 8 represents the spatiotemporal variation of
the electron density ne (x, t) in logarithmic representation in
correlation with the temporal course of the current density and
the gap voltage during positive current peaks. Note that the
instant t0 is set to the maximum of the current. Qualitatively
the same behaviour occurs in the negative half-period. The
particular discharge events investigated here are indicated by
t0 in figure 6.
For both amplitudes of the applied voltage considered here
a similar spatiotemporal variation of the electron density can
be observed from figure 8. With increasing gap voltage the
electron density decreases several orders of magnitude in front
of the momentary cathode located at x = 1.5 mm. When the
gap voltage reaches the ignition voltage the electron density
grows strongly in the cathode-fall region but remains almost
the same at the area close to the instantaneous anode. At the
same time a strong current pulse occurs and at the instant of
maximum current density the spatial profile of the electron
density allows to detect clearly the cathode-fall region and the
positive column, similar to the optical emission observed in the
experiment [21]. Immediately after breakdown, the electron
density in the positive column increases slightly. This effect is
mainly caused by ionization of excited argon states.
Besides the general evolution of the discharge, two
essential differences between the discharge behaviour at
V0 = 1.5 kV and that at V0 = 2.5 kV are pointed out
by figure 8. Firstly, it becomes obvious that the plasma
J. Phys. D: Appl. Phys. 46 (2013) 355203 M M Becker et al

V = 1.5 kV V = 2.5 kV
4 0 4 0
x 10 x 10
12 12
4 4
x 10 x 10
10 10

Electric field [V/cm]

Electric field [V/cm]

2 2
8 8
1 1
6 6
0 0
4 4
0 0.5 1 1.5 0 0.5 1 1.5
2 2

0 0

0 0.25 0.5 0.75 1 1.25 1.5 0 0.25 0.5 0.75 1 1.25 1.5
x [mm] a) x [mm] b)
13 13
10 10

Charge carrier density [cm−3]

Charge carrier density [cm ]
−3

12 12
10 10

11 11
10 10

10 10
10 10

9 9
10 10

0 0.25 0.5 0.75 1 1.25 1.5 0 0.25 0.5 0.75 1 1.25 1.5
x [mm] c) x [mm] d)
Figure 9. Electric field (a),(b) and density of electrons (◦), Ar + ions (
) and Ar2+ ions (+) (c),(d) at the times t = t0 –1 µs (- - - -) and t = t0
(——) and applied voltages V0 = 1.5 kV (left) and V0 = 2.5 kV (right) (instantaneous anode at x = 0, cathode at x = 1.5 mm).

recombination between two subsequent discharge events instantaneous anode between subsequent discharge events, the
decreases with increasing voltage amplitude. At V0 = 1.5 kV electric field remains low in that region while the gap voltage
the electron density drops several orders of magnitude in more increases (see results at t0 − 1µs). The insets of figures 9(a)
than half of the discharge region. By contrast, at V0 = 2.5 kV and (b) clearly show that the width of the actual gap where the
the electron density remains high in more than half of the electric field increases becomes smaller with the increase of
gap. The full recombination of charge carriers is prevented the voltage amplitude from 1.5 to 2.5 kV. At time t0 the electric
by a large chemo-ionization rate as discussed below. Because field configuration and the charge carrier densities predicted by
the plasma does not totally recombine between two successive the fluid model show similar behaviour for both amplitudes of
discharges, a memory effect occurs and the characteristics of the applied voltage considered here. The cathode-fall region
each discharge event depends strongly on that of the previous extends to approximately 60 µm in front of the instantaneous
one [60]. Therefore, the ignition voltage is not the same at cathode followed by the negative glow region exhibiting a
V0 = 1.5 kV and V0 = 2.5 kV. reversal of the electric field at x ≈ 1.4 mm. Towards the
Secondly, figure 8 exhibits that at V0 = 2.5 kV the second momentary anode the electric field as well as the charge carrier
increase of the current density after the current pulse is attended densities are spatially modulated but do not exhibit the well
by an increase of the electron density in the cathode-fall region. defined striations observed in the experiment (see figure 1(b)).
The occurrence of a second breakdown is just prevented by the A probable reason for that shortcoming is that kinetic effects
decrease of the sinusoidal applied voltage. At V0 = 1.5 kV no leading to the formation of striated structures are not captured
increase of the electron density in the cathode-fall region takes by the fluid model under consideration.
place before the polarity changes. However, the representation of the ionization rates
Since the plasma recombines only partially between predicted by the calculations at the instant t0 of maximum
subsequent current pulses reignition takes place in a part of current in figure 10 reveals a possible cause for the occurrence
the discharge volume, only, as observed recently in theoretical of striations under certain conditions. Figure 10 shows that
investigations of DBDs in helium [61]. This can readily in the quasi-neutral region in front of the momentary anode
be seen from the representation of the electric field and the the rate of stepwise ionization increases while the rate of
charge carrier densities at the times t0 –1 µs and t0 in figure 9. electron impact ionization of ground state atoms decreases
Because the charge carrier densities remain high in front of the when the voltage amplitude is raised from 1.5 to 2.5 kV.

9
J. Phys. D: Appl. Phys. 46 (2013) 355203 M M Becker et al

V = 1.5 kV V = 2.5 kV
18 0 20 18 0 20
x 10 x 10 x 10 x 10
2.5 2.5
10 10
Ionization rate [cm−3 s−1]

Ionization rate [cm−3 s−1]

2 2
8 8
1.5 1.5
6 6
1 4 1 4

0.5 2 0.5 2

0 0 0 0
0 0.2 0.4 0.6 0.8 1 1.2 1.35 1.5 0 0.2 0.4 0.6 0.8 1 1.2 1.35 1.5
x [mm] x [mm]

Figure 10. Spatial variation of direct ionization (——), stepwise ionization (- - - -) and chemo-ionization (— · —) rates at the instant t0 of
maximum current for applied voltages V0 = 1.5 kV (left) and V0 = 2.5 kV (right) (instantaneous anode at x = 0, cathode at x = 1.5 mm).

V = 1.5 kV, x = 0.5 mm V = 2.5 kV, x = 0.5 mm

0 0
18 18
10 10
s ]

s ]
−3 −1

−3 −1
17 17
10 10
Rate [cm

Rate [cm

16 16
10 10

15 15
10 10
−2 −1 0 1 2 3 4 −2 −1 0 1 2 3 4
t [µs] t [µs]

Figure 11. Temporal variation of direct ionization (——), stepwise ionization (- - - -), chemo-ionization (— · —) and recombination (◦)
rates at x = 0.5 mm during positive half-period for applied voltages V0 = 1.5 kV (left) and V0 = 2.5 kV (right).

In the cathode-fall region the electron production is mainly 5. Conclusion

driven by direct ionization in both cases. The appreciable role
played by stepwise ionization and chemo-ionization processes The transition between two different discharge modes observed
in the development of striations is well documented in the in filamentary DBDs in argon at atmospheric pressure with an
literature [25, 62, 63] and the interplay of direct ionization and increase of the applied voltage amplitude has been analysed
ionization processes involving excited particles are a possible by means of experimental and theoretical studies. It has been
reason for the stratification of the discharge channel at higher shown that both the experiments and the model calculations
amplitudes of the applied voltage. predict a transition from a stable discharge mode characterized
In order to explain the observed effect that the charge by one current peak per half-period to an unstable discharge
carrier densities remain large in a part of the discharge mode that is characterized by a second increase of the discharge
volume during the entire temporal evolution, the ionization current immediately after breakdown. Mode transition takes
and recombination rates at x = 0.5 mm are displayed in place when the amplitude of the applied voltage exceeds
figure 11. Just before ignition of the discharge recombination approximately 2 kV for the system being considered. The
of charge carriers in collisions of electrons with molecular direct comparison between calculated and measured current-
ions Ar2+ + e −→ Ar[2p] + Ar[1p0 ] (process R68 in table A2) voltage characteristics has pointed out that the spatially
dominates the electron budget. However, due to the long one-dimensional fluid model under consideration is able to
lifetime of metastable argon atoms the chemo-ionization rate reproduce main features of the experimental observations in
remains at a comparatively high level and compensates for the both discharge modes.
loss of charge carriers to a large extent. Instantaneously with The theoretical investigations have revealed that the
the steep increase of the direct and stepwise ionization rates the instabilities observed in the experiment at applied voltages
discharge ignites, while after the discharge event only chemo- largely exceeding the burning voltage are potentially caused
ionization remains the dominant electron generation process. by the occurrence of negative differential conductivity
Again it becomes obvious that the ratio of direct and stepwise immediately after the first breakdown in each half-period.
ionization rates at the instant of maximum current changes with Furthermore, it has been shown that the high rate of chemo-
the increase of the applied voltage amplitude. ionization during the entire temporal evolution prevents the full

10
J. Phys. D: Appl. Phys. 46 (2013) 355203 M M Becker et al

Table A1. Electron–neutral particle collision processes considered in the reaction kinetic model. The third column gives the energy range in
eV for which data of the given references were used. The cross sections for deexcitation have been obtained according to the principle of
detailed balancing.
Index Process Energy range Data source
Elastic electron collision
1 Ar[1p0 ] + e −→ Ar[1p0 ] + e 0–10000 [64]
Electron-collision excitation and deexcitation
2, 3 Ar[1p0 ] + e ←→ Ar[1s5 ] + e 11.54–30; 35–1000 [65]; [40, 64]
4, 5 Ar[1p0 ] + e ←→ Ar[1s4 ] + e 11.62–30; 50–1000 [65]; [40, 64]
6, 7 Ar[1p0 ] + e ←→ Ar[1s3 ] + e 11.72–30; 35–400 [65]; [40, 64]
8, 9 Ar[1p0 ] + e ←→ Ar[1s2 ] + e 11.82–30; 35–1000 [65]; [40, 64]
10, 11 Ar[1p0 ] + e ←→ Ar[2p] + e 12.9–30; 30–1000 [65]; [40, 64]
12, 13 Ar[1p0 ] + e ←→ Ar[2p
] + e 13.28–30; 30–1000 [65]; [40, 64]
14, 15 Ar[1p0 ] + e ←→ Ar ∗ [hl] + e 13.84–1000 [40, 64]
16, 17 Ar[1s5 ] + e ←→ Ar[1s4 ] + e 0.07–18; >18 [65, 66]; [67]
18, 19 Ar[1s5 ] + e ←→ Ar[1s3 ] + e 0.17–18; >18 [65, 66]; [67]
20, 21 Ar[1s5 ] + e ←→ Ar[1s2 ] + e 0.28–18; >18 [65, 66]; [67]
22, 23 Ar[1s5 ] + e ←→ Ar[2p] + e 1.36–18; >18 [65, 68]; [67]
24, 25 Ar[1s5 ] + e ←→ Ar[2p
] + e 1.73–18; >18 [65, 68]; [67]
26, 27 Ar[1s5 ] + e ←→ Ar ∗ [hl] + e
2.91 [67]
28, 29 Ar[1s4 ] + e ←→ Ar[1s3 ] + e 0.1–18; >18 [65]; [67]
30, 31 Ar[1s4 ] + e ←→ Ar[1s2 ] + e 0.2–18; >18 [65]; [67]
32, 33 Ar[1s4 ] + e ←→ Ar[2p] + e 1.28–18; >18 [65]; [67]
34, 35 Ar[1s4 ] + e ←→ Ar[2p
] + e 1.66–18; >18 [65]; [67]
36, 37 Ar[1s4 ] + e ←→ Ar ∗ [hl] + e
2.84 [67]
38, 39 Ar[1s3 ] + e ←→ Ar[1s2 ] + e 0.1–18; >18 [65]; [67]
40, 41 Ar[1s3 ] + e ←→ Ar[2p] + e 1.18–18; >18 [65]; [67]
42, 43 Ar[1s3 ] + e ←→ Ar[2p
] + e 1.56–18; >18 [65]; [67]
44, 45 Ar[1s3 ] + e ←→ Ar ∗ [hl] + e
2.74 [67]
46, 47 Ar[1s2 ] + e ←→ Ar[2p] + e 1.08–18; >18 [65]; [67]
48, 49 Ar[1s2 ] + e ←→ Ar[2p
] + e 1.45–18; >18 [65]; [67]
50, 51 Ar[1s2 ] + e ←→ Ar ∗ [hl] + e
2.63 [67]
52, 53 Ar[2p] + e ←→ Ar[2p
] + e 0.38–18; >18 [65]; [67]
54, 55 Ar[2p] + e ←→ Ar ∗ [hl] + e
0.94 [67]
56, 57 Ar[2p
] + e ←→ Ar ∗ [hl] + e
0.56 [67]
Electron-collision ionization
58 Ar[1p0 ] + e −→ Ar + + 2e 15.75–1000 [69]
59 Ar[1s5 ] + e −→ Ar + + 2e
4.21 [67]
60 Ar[1s4 ] + e −→ Ar + + 2e
4.13 [67]
61 Ar[1s3 ] + e −→ Ar + + 2e
4.21 [67]
62 Ar[1s2 ] + e −→ Ar + + 2e
4.1 [67]
63 Ar[2p] + e −→ Ar + + 2e
2.49 [67]
64 Ar[2p
] + e −→ Ar + + 2e
2.46 [67]
65 Ar ∗ [hl] + e −→ Ar + + 2e
1.6 [67]
66 Ar2∗ [3 u+ , v  0] + e −→ Ar2+ + 2e 3.23–50; >50 [70]; [67]
67 Ar2∗ [1 u+ , v  0] + e −→ Ar2+ + 2e 3.15–50; >50 [70]; [67]

plasma recombination between subsequent discharge events. found to be a possible reason for the striations observed in
Therefore, the characteristics of each breakdown is largely the experiment under certain conditions.
affected by the previous one and reignition takes place in
a part of the discharge volume, only. The analysis of the
Acknowledgments
spatiotemporal variation of the charge carriers and the electric
field for different amplitudes of the applied voltage has pointed
This work was supported by the German Research Foundation
out that the extent of plasma recombination decreases when the
within the Transregional Collaborative Research Centre
voltage amplitude is increased.
Transregio 24 Fundamentals of complex plasmas.
It has been shown that the role of stepwise ionization
during discharge events increases and the importance of direct
ionization decreases with the transition from the low voltage Appendix A. Reaction kinetic processes for argon
mode to the high voltage mode. Even though the striations
observed in the experiment cannot be reproduced by the The coefficients for radiative transitions R95 and R96
fluid model considered, the interplay of direct ionization and (see table A2) of resonant argon states Ar[1s4 ] and
ionization processes involving excited particles have been Ar[1s2 ] are determined using the approximation of effective

11
J. Phys. D: Appl. Phys. 46 (2013) 355203 M M Becker et al

Table A2. Recombination, heavy particle collision and radiative processes considered in the reaction kinetic model. The rate coefficients of
two-body collisions are given in units of cm3 s−1 and those of three-body collisions in units of cm6 s−1 . Rates of emission are given in units
of s−1 ; d denotes the gap width in cm and kB Te = 2ε̄/(3e0 ).
Index Process Rate coefficient Data source
Electron–ion recombination
68 Ar2+ + e −→ Ar[2p] + Ar[1p0 ] 5.9 × 10−8 (Te )−2/3 [71]
69 Ar + + 2e −→ Ar ∗ [hl] + e 8.7 × 10−27 (Te )−9/2 [46]
70 Ar + + e −→ Ar ∗ [hl] + hν 2.7 × 10−13 (Te )−3/4 [46]
Chemo-ionization processes
71 Ar[1s5 ] + Ar[1s5 ] −→ Ar + + e + Ar[1p0 ] 1.3 × 10−9 [72]
72 Ar[1s5 ] + Ar[1s4 ] −→ Ar + + e + Ar[1p0 ] 4.5 × 10−10 [72]
73 Ar[1s5 ] + Ar[1s3 ] −→ Ar + + e + Ar[1p0 ] 1.3 × 10−9 [72]
74 Ar[1s5 ] + Ar[1s2 ] −→ Ar + + e + Ar[1p0 ] 4.5 × 10−10 [72]
75 Ar[1s4 ] + Ar[1s4 ] −→ Ar + + e + Ar[1p0 ] 4.5 × 10−10 [72]
76 Ar[1s4 ] + Ar[1s3 ] −→ Ar + + e + Ar[1p0 ] 4.5 × 10−10 [72]
77 Ar[1s4 ] + Ar[1s2 ] −→ Ar + + e + Ar[1p0 ] 4.5 × 10−10 [72]
78 Ar[1s3 ] + Ar[1s3 ] −→ Ar + + e + Ar[1p0 ] 1.3 × 10−9 [72]
79 Ar[1s3 ] + Ar[1s2 ] −→ Ar + + e + Ar[1p0 ] 4.5 × 10−10 [72]
80 Ar[1s2 ] + Ar[1s2 ] −→ Ar + + e + Ar[1p0 ] 4.5 × 10−10 [72]
Charge-transfer reaction
81 Ar + + 2Ar[1p0 ] −→ Ar2+ + Ar[1p0 ] 2.5 × 10−31 [73]
Quenching
82 Ar ∗ [hl] + Ar[1p0 ] −→ Ar[2p
] + Ar[1p0 ] 1.0 × 10−11 estimated
83 Ar[2p
] + Ar[1p0 ] −→ Ar[2p] + Ar[1p0 ] 1.7 × 10−11 [74]
84 Ar[2p
] + Ar[1p0 ] −→ Ar[1s2 ] + Ar[1p0 ] 4.3 × 10−11 [74]
85 Ar[2p] + Ar[1p0 ] −→ Ar[1s2 ] + Ar[1p0 ] 2.7 × 10−11 [74]
86 Ar[1s2 ] + Ar[1p0 ] −→ Ar[1s3 ] + Ar[1p0 ] 1.5 × 10−14 estimated
87 Ar[1s3 ] + Ar[1p0 ] −→ Ar[1s4 ] + Ar[1p0 ] 5.3 × 10−15 [75]
88 Ar[1s4 ] + Ar[1p0 ] −→ Ar[1s5 ] + Ar[1p0 ] 1.5 × 10−14 [76]
89 Ar[1s4 ] + 2Ar[1p0 ]
−→ Ar2∗ [1 u+ , v  0] + Ar[1p0 ] 1.5 × 10−33 [76]
90 Ar[1s5 ] + Ar[1p0 ] −→ Ar[1s4 ] + Ar[1p0 ] 2.5 × 10−15 [76]
91 Ar[1s5 ] + Ar[1p0 ] −→ Ar[1p0 ] + Ar[1p0 ] 1.5 × 10−14 [76]
92 Ar[1s5 ] + 2Ar[1p0 ]
−→ Ar2∗ [3 S+u , v  0] + Ar[1p0 ] 1.3 × 10−32 [76]
93 Ar2∗ [1 u+ , v  0] + Ar[1p0 ]
−→ Ar2∗ [1 u+ , v = 0] + Ar[1p0 ] 1.7 × 10−11 [77]
94 Ar2∗ [3 u+ , v  0] + Ar[1p0 ]
−→ Ar2∗ [3 u+ , v = 0] + Ar[1p0 ] 1.7 × 10−11 [77]
Radiative processes √
95 Ar[1s4 ] −→ Ar[1p0 ] + hν 6.2/√d × 104 [78]
96 Ar[1s2 ] −→ Ar[1p0 ] + hν 2.8/ d × 105 [78]
97 Ar[2p] −→ Ar[1s5 ] + hν 2.0 × 107 [79]
98 Ar[2p] −→ Ar[1s4 ] + hν 1.1 × 107 [79]
99 Ar[2p] −→ Ar[1s3 ] + hν 4.0 × 105 [79]
100 Ar[2p] −→ Ar[1s2 ] + hν 1.5 × 106 [79]
101 Ar[2p
] −→ Ar[1s5 ] + hν 3.3 × 106 [79]
102 Ar[2p
] −→ Ar[1s4 ] + hν 4.0 × 106 [79]
103 Ar[2p
] −→ Ar[1s3 ] + hν 7.6 × 106 [79]
104 Ar[2p
] −→ Ar[1s2 ] + hν 2.0 × 107 [79]
105 Ar ∗ [hl] −→ Ar[1s5 ] + hν 1.5 × 105 [80]
106 Ar ∗ [hl] −→ Ar[1s4 ] + hν 8.7 × 104 [80]
107 Ar ∗ [hl] −→ Ar[1s3 ] + hν 3.2 × 104 [80]
108 Ar ∗ [hl] −→ Ar[1s2 ] + hν 9.1 × 104 [80]
109 Ar ∗ [hl] −→ Ar[2p] + hν 9.2 × 105 [80]
110 Ar ∗ [hl] −→ Ar[2p
] + hν 8.6 × 105 [80]
111 Ar2∗ [1 u+ , v  0] −→ 2Ar[1p0 ] + hν 2.4 × 108 [76]
112 Ar2∗ [3 u+ , v  0] −→ 2Ar[1p0 ] + hν 6.2 × 106 [76]
113 Ar2∗ [1 u+ , v = 0] −→ 2Ar[1p0 ] + hν 2.4 × 108 [76]
114 Ar2∗ [3 u+ , v = 0] −→ 2Ar[1p0 ] + hν 3.5 × 105 [76]

12
J. Phys. D: Appl. Phys. 46 (2013) 355203
space-independent lifetimes [78, 81]
 √ −1
2 2 τl−1
τl =
eff
, l = 2, 4 (A.1)
3 πk0,l d
with natural lifetimes τ4 = 8.6 ns and τ2 = 2.15 ns according
to [82]. The absorption coefficients k0,l , l = 2, 4 are
determined as [78]
 
2λ0 g2 3/2 ε0 me c
k0,l = , (A.2)
2.1τl g1 e02 f21
where λ0 is the vacuum wavelength, g1 and g2 denote the
statistical weights, f21 is the oscillator strength and c the speed
of light.
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