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1 Introduction
Non-thermal plasmas at atmospheric pressure are effective sources of radicals and excited species. Therefore,
they have found many technical applications in the plasma chemistry, lighting, and recently also in life-science
[1,2]. In this group the barrier discharges (BDs) have a key position. It is well-known that BDs can be operated in
various discharge modes, namely the lamentary and diffuse mode. In the latter it has to be distinguished between
a Townsend-like and glow-like mode [37]. The appearance of different operation modes depends on the feeding
gas mixture and ow rate, gas pressure, operation frequency and shape of applied voltage, dielectric barrier
material and the reactor geometry (e.g. gap spacing). Especially, for large aspect ratios (ratio of lateral extension
to gap distance) an increased tendency of pattern formation is observed [79]. Finally, the discharge operation
mode (lamentary or diffuse) is related to the ratio of the secondary processes at the electrodes (e.g. exoemission
of electrons) to the ionization in the discharge volume (Townsend mechanism and Penning ionization). Here,
surface charges play an important role, because of the low energy necessary to release electrons from such a
surface. This energy can be provided by metastable species. Many investigation in the past have contributed to
the better understanding of the complex processes. Despite the great progress in this eld of complex plasmas in
the last decade [1013], the diagnostics of these phenomena is still a challenge.
To study the discharge modes and the lateral structuring, a discharge cell conguration has been developed to
combine three high-end diagnostic techniques: The spatio-temporally and spectrally resolved discharge development in the volume was investigated by the well-known cross-correlation spectroscopy (CCS) [3, 1416]. The
temporally resolved detection of surface charges on the dielectric succeeded by the application of the electrooptic
Pockels effect in combination with a CCD camera [1719]. Metastable N2 (A) molecules were determined by the
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M. Bogaczyk et al.: Development of Barrier Discharges: Operation Modes and Structure Formation
laser induced uorescence spectroscopy [11]. This way, it was possible for the rst time to correlate key parameters of the discharge operation modes under identical and well-dened experimental conditions. Additionally,
a separate surface BD conguration was used to investigate the propagation of microdischarges in air along the
interface of the gas and the dielectric surface.
The presented results are an important and extensive source for the comparison with kinetic models to get
a deeper (nally quantitative) understanding of the complex mechanisms in the BD evolution. The modeling
activities - under progress - consider the dominant processes in the discharge volume as well as the interactions
of relevant plasma species with dielectric surfaces [2023].
Fig. 1 Sketch of the principal outline of experimental investigations: Different diagnostic techniques are applied to the same
discharge cell conguration with dielectric BSO crystal as one of the dielectrics.
The developed discharge cell conguration enabled the detailed investigation of the discharge evolution and
processes in the volume as well as the interaction with the dielectric surfaces. As shown in gure 1, it consists of
two parallel electrodes covered with dielectrics. The driven one is a transparent and conductive ITO layer which
covers the topside of a glass plate (glass = 7.6). The grounded electrode is a polished aluminum mirror. On its
top an electro-optic BSO crystal (Bi12 SiO20 , BSO = 56) is placed to permit the measurement of surface charges.
The gap distance between the dielectrics can be varied from 0.5mm to 1 mm. Sidewise orices enable a gas ow
and the application of the optical diagnostics (CCS and LIF). The working gases are pure helium, pure nitrogen,
and mixtures of both. The pressure varies from 200 hPa to 1000 hPa and the frequency is in the range from 2 kHz
to 200 kHz. The applied sinusoidal voltage amounts up to 6 kV depending on the pressure and gas.
The surface charge measurement is based on the electro-optic Pockels effect [24]. The BSO crystal is homogeneously illuminated ( = 634 nm) and the initially linearly polarized light is changed by the optical set-up and
the BSO crystal to elliptic polarization. The ellipticity depends on the voltage drop across the BSO crystal and
thus on the deposited charges on its surface. Via a linear polarization lter, the surface charge distribution (sign
and value) is made visible by means of a high-speed camera (exposure time 10 s).
To investigate the lateral patterns in the luminescence distribution in dependence of the applied voltage an
ICCD camera is directly placed in front of the discharge cell, recording the discharge emission. The exposure
time is typically 200 s. For a driving frequency of 100 kHz, each image is accumulated over several tens of
subsequent periods.
The optical emission evolution can be investigated with the highly sensitive CCS diagnostic technique. It is
based on time-correlated single photon counting from about 106 discharge events. In case of diffuse BDs the
time-information is derived from phase resolved measurements as described in [12]. The spatial resolution is
in the range of 0.05 mm to 0.01 mm. A monochromator provides a spectral resolution of 0.1 nm of the optical
emission signal. The most intensive lines of N2 , namely the N2 second positive system (SPS, 0-0 transition at
= 337 nm) and the rst negative system (FNS, 0-0 transition = 391 nm), as well as the He line at = 706 nm
have been investigated.
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+
For the detection of the metastable N2 (A3 u ) state a LIF set-up is used. The laser excites the transition from
+
the A3 u , v = 0 state to the B 3 g , v = 3 state at the wavelength of = 687.44 nm. The uorescence band of
+
the following transition to the A3 u , v = 1 state at about 762 nm is measured perpendicularly to the laser beam
via a monochromator and a photomultiplier tube. For the absolute density calibration the Rayleigh scattering at
carbon dioxide has been measured for equal conditions [25, 26].
All diagnostics are completed by the measurement of applied voltage, discharge current, and transferred
charge.
Fig. 2 Spatio-temporally resolved discharge developments of the SPS and FNS in pure helium and nitrogen. 500 hPa, 2 kHz,
0.45 kV in pure helium, and 3.7 kV in pure nitrogen.
In gure 3 a) the discharge net current (solid line) and surface charge development (circle) over one period are
shown for pure nitrogen. The low current and its long pulse duration corresponds to the Townsend-like mode.
During the appearance of a current pulse, the surface charge changes its sign. After that, it remains constant on
the BSO crystal until the next current pulse in the next half period occurs. The temporally integrated net current
(dashed line) shows an excellent agreement with the measured surface charges. One reason for the generation of a
diffuse discharge mode in pure nitrogen is the effective secondary emission of electrons by plasma species. Here,
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M. Bogaczyk et al.: Development of Barrier Discharges: Operation Modes and Structure Formation
metastable nitrogen molecules (in competition with energetic ions) play an important role [12, 13]. Therefore,
+
the time dependence of the N2 (A3 u , v = 0) density is measured and plotted with the applied voltage and the
discharge current in gure 3 b). The averaged density is about 21013 cm3 in the center of the gap which is in
the same order of magnitude as in [11]. The N2 (A) density increases during the discharge pulses and is clearly
larger in the positive half period than in the negative one. This is reasonable because of the asymmetric discharge
cell set-up due to the different dielectrics (glass, BSO).
Fig. 3 a): Phase resolved surface charge from the electro-optic measurement (circles) with the corresponding net current
(solid line) and the temporally integration of the net current (dashed line). b): Time dependence of metastable N2 (A3 +
u,
v = 0) density in the center of the discharge gap. 500 hPa, 2 kHz, 4 kV.
For small admixtures of nitrogen to helium in percent range a lamentary BD is observed [28]. The spatial
resolved surface charge density for a 9:1 He/N2 mixture is shown in gure 4 a) for both half periods after the
discharge breakdown. Both images show deposited surface charge spots which are caused by previous microdischarges [29]. Negative surface charges are electrons deposited on the dielectric. Positive surface charges result
most probably from the recombination of ions with electrons from the bulk material. Notably, the negative surface charges are more extended than the positive ones due to the higher electron mobility in the volume in front
of the electrodes compared to the ions [30, 31]. Their radial proles can be tted well by a Gaussian function
as shown in gure 4 b). Also, the discharge re-ignition is preferred on deposited surface charges, the so-called
+
memory effect. In gure 4 c) the N2 (A3 u , v = 0) metastable density is shown after one microdischarge in
pure nitrogen. It has its maximum several microseconds after the few nanoseconds lasting discharge pulse.
Fig. 4 a) Charge distribution in the lamentary mode (90% He and 10% N2 mixture) of positive and negative surface charges
in the positive and negative half-period, respectively. b) Radial
prole of positive and negative surface charges, FWHM: + =
0.9 mm and = 1.6 mm, respectively. c) Density of N2 (A3 +
u , v = 0) metastables in the afterglow of one microdischarge
in pure nitrogen. 500 hPa, 2 kHz, a)-b) 0.91 kV, and c) 5.5 kV.
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+
Hence, the production of N2 (A3 u , v = 0) is dominated by depletion of energetically higher states instead
of electron impact excitation. This corresponds to the delay of the metastable production with respect to the
discharge current in the diffuse mode as shown in gure 3 and in literature [11, 32].
350V, d) U = 342V.
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Fig. 7 Analysis of the transition from the hexagonal pattern to the stochastic arrangement of the laments. Evaluated are the ratios of the 60 -peak at nearest neighbor distance to the mean background in angular and radial direction, Hang = y60 / < y(d0 , ) > and Hrad = y60 / <
y(r, 60 ) >r , respectively.
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M. Bogaczyk et al.: Development of Barrier Discharges: Operation Modes and Structure Formation
It evaluates the positions of any triple of discharge spots and returns a probability distribution y(r, ) of nding
a second spot in a distance r and an angle with respect to an arbitrarily selected nearest neighbor, see gure 6
[33]. Qualitatively, the degradation of the hexagonal order starts with a blurring of order in angular direction.
A decay of the radial order follows. However, whereas the angular order is entirely removed at the end of the
transition, a small modulation in the radial order remains because two discharge spots can not move arbitrarily
close as they inhibit each other [18, 34].
In order to characterize the transition quantitatively, convenient measures for the hexagonal order are chosen.
Hrad and Hang are the ratios of y60 = y(d0 , 60 ) to the TCF mean background along a line in radial and angular
direction, respectively. d0 is the nearest neighbour distance. Figure 7 shows the previously observed transition
using Hrad and Hang . Both plots show principally the same behavior: at higher voltages, the measures of order
remain nearly constant. At decreasing voltages occurs a sudden change of the measures slope, and the measure
of order decreases. This abrupt transition is a supercritical bifurcation. At the smallest used voltages, the peak
y60 vanishes in the background noise due to the low order and low lament number. Hence, Hang and Hrad are
b,rad occurs at lower
not meaningful anymore. In all measurements, the bifurcation point for the radial order U
voltages than the bifurcation point for the angular order Ub,ang , which is consistent with the previous qualitative
observations.
3.3 Surface discharges
The propagation of microdischarges along the interface between the gas and dielectric surface can be investigated by the discharge cell shown in gure 8. The proposed electrode arrangement was carried out after testing
different surface BD arrangements for the investigation of single repetitive microdischarges in air [35, 36]. The
discharge cell consists of two needle electrodes (syringe hollow needles made of chrome-nickel-steel alloy, 0.4
mm diameter) placed on the opposite sites of a 0.6 mm thick Al2 O3 ceramic plate (96% purity, p = 10). The
tips of the electrodes faced each other with a gap of g = 1.15 mm. To prevent parasitic discharges, the driven
electrode was covered by additional isolating material. The discharge was driven in dry air (gas ow 300 sccm)
by means of sinusoidal voltage with several kV amplitude at a frequency of about 60 kHz.
In gure 8 results of ICCD-photography are shown. There is a higher discharge activity if the exposed electrode is the anode. Only these results are presented in the following. The side-on ICCD photos (upper right
pictures) show that in the chosen electrode conguration the discharge channel develops directly on the dielectric
surface. The discharge channel is about 100 m thick and its length increases with the amplitude of the applied
voltage. At 3.2 kV the transferred charge of a single channel was about 1.5 nC. The increase of the voltage amplitude leads to the generation of further discharge pulses in the same half period. Four to six individual current
pulses could be detected [37]. The top-view ICCD camera photo (left lower part of gure 8) at 3.2 kV shows that
the rst microdischarge in the half period develops on the direct path between the electrode positions. At 3.75 kV
two microdischarges per half period are observed. The corresponding ICCD-photo was taken with gate setting
only recording the second microdischarge event (20 accumulations). The second discharge channel evades the
region of the preceding breakdown taking a curved and thus longer path resulting in larger current amplitude and
transferred charge by trend. This result demonstrates that charge carriers are deposited on the dielectric surface
leading to specic discharge pattern.
The gure 9 presents the result of CCS measurement for the 0-0 transition of SPS, the most intensive band in
the emission spectrum. The microdischarge starts with a short Townsend prephase at the tip of the anode, similar
as observed in volume BD and coplanar discharges [16]. A positive space charge accumulates in front of the
anode up to a level incepting the propagation of a cathode directed ionization front or streamer. The maximum
velocity of the ionization front is about 2.8105 m/s [36] at the distance of 0.2mm in front of the the anode. With
increasing distance from the anode, the velocity decreases to 1.5105 m/s at the cathode region. This behavior
is quite different from volume BDs where the velocity increases towards the cathode. The presented surface BD
conguration is a good object for the detailed and quantitative investigation of surface effects on the breakdown
and discharge development since the channel propagates along the interface between gas and dielectric. Similarly
as the discharge re-ignition or uniformity described in the previous subsections, the propagation of discharge
channels is determined by the elementary interaction with the charged dielectric surface. Surface ionization due
to detrapping, ion impact and photo effect or surface attachment of charge carriers may have a strong inuence
[38, 39] which should be investigated in more detail.
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M. Bogaczyk et al.: Development of Barrier Discharges: Operation Modes and Structure Formation
effect, an inuence of the propagation of repetitive microdischarge channels along the interface of the gas volume
and the dielectric surface has been investigated.
In the case of patterned discharges the voltage amplitude controls the number and the order of the discharge
spots. The breakdown of the hexagonal order is a supercritical bifurcation appearing with decreasing voltage
amplitude.
The presented experimental results are an extensive source for the comparison with kinetic models to get
a deeper (nally quantitative) understanding of the complex mechanisms in the BD evolution. The modelling
activities - under progress - consider the dominant processes in the discharge volume as well as the interactions
of relevant plasma species with dielectric surfaces [2023, 40].
In order to gain more information about the elementary processes of plasma-dielectric interaction further
experiments in discharge arrangements with the breakdown appearing directly on and along the surface are proposed. The application of the surface BD geometry described in this contribution to a BSO as the dielectric would
enable the measurement of surface charges in correlation with the plasma propagation along the surface. In order
to control the microdischarge the implementation of a third electrode is foreseen, a so-called sliding discharge
[41]. In particular, it is planned to investigate the role of negative ions by the laser photodetachment technique
[42].
Acknowledgements This work was supported by the Deutsche Forschungsgemeinschaft (DFG) through the transregional
collaborative research center SFB/TRR 24. The authors are grateful to Tomas Hoder (INP Greifswald) and Helge Grosch
(DTU Risoe, formerly INP) for supporting surface BD investigations.
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