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Optical and Langmuir Probe Diagnostics in a

Magnetized Hollow Cathode Arc

Article in Plasma Processes and Polymers · June 2009

DOI: 10.1002/ppap.200930804

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 Full Paper

Optical and Langmuir Probe Diagnostics in a

Magnetized Hollow Cathode Arc

Gonzalo Avaria,* Achim Lunk, Attila Schröder, Igor Pavlovitch Vinogradov

The paper presents measurements of the plasma parameters of a hollow cathode arc (HCA)
using Langmuir probes (LPs) as well as optical emission spectroscopy (OES). The plasma of a
HCA is characterized by a high energy beam-like component of electrons which causes a
relatively high ionization degree. Data of LP measurements were evaluated to obtain the
electron energy distribution function (EEDF), which could be approximated by the generalized
Druyvesteyn distribution. The spectroscopic method used is based on the analysis of the
molecular spectra of nitrogen and the atomic spectra of He and Ar. By considering several lines
with different excitation thresholds the EEDF could be obtained in a trial and error procedure
using a regularization routine. Because of the high electron density in HCA, stepwise processes
initiated by metastable states of Ar and He atoms and N2 molecules are taken into account
also. The data evaluated from spectroscopic measurements are compared with those from LP
measurements. The EEDF measured by OES could be approximated by a Maxwellian distri-
bution function.

Introduction low pressure regime (10
3 mbar) ionization degrees of

The increasing application of plasma-technological pro-
cesses in industry demands further development of
plasma sources, which are well adapted to the techno-
logical requirements. Plasmas sources with high electron
density as well as high electron temperature are often
favorable in plasma enhanced physical deposition
(PEPVD) of inorganic materials. Furthermore the produc-
tion cost of the plasma source should be acceptable. The
properties of the hollow cathode arc (HCA) plasma source
agree with many of these requirements. HCA combines
thermo-ionic emission with the hollow cathode effect so
that the plasma production is very effective. Beam-like
electrons with high kinetic energy are detectable near the
exit of the hollow cathode. Thus, the electron energy
distribution function (EEDF) is strongly anisotropic. In the
G. Avaria
Pontificia Universidad Católica de Chile, Chile
Fax: þ49-711-68563102; E-mail: lunk@ipf.uni-stuttgart.de
A. Lunk, A. Schröder, I. P. Vinogradov
Institut für Plasmaforschung, Universität Stuttgart, Pfaffen-
waldring 31, 70569 Stuttgart, Germany
nearly 10% can be obtained. The combination of optical
and Langmuir probe (LP) diagnostics offers a good chance
to compare different measuring methods and to check the
applicability of both methods. The diagnostics of the HCA-
plasma was performed with the back-ground of applica-
tion in PEPVD.
In dc-discharges the measurement of inner plasma
parameters by the LP method is highly developed and
often used.[1] Evaluation of the voltage–current–character-
istics (VCC) of LP gives information about the electron- as
well as the ion-part of the plasma. Data evaluation of the
VCC was carried out by a four step procedure: subtraction
of the ion current from the entire current, fitting of the
electron part of VCC, smoothing of VCC, and derivation of
the VCC to get the first and the second derivatives. The
second derivative was adapted by the generalized
Druyvesteyn distribution.[2] The electron density results
from integration of the EEDF. When measurements are
performed in one-component-gases, the electron density
can be evaluated from ion saturation current because of
quasi-neutrality. In the measurements the OML-theory
was applied for the evaluation of the ion saturation
current at the cylindrical probe.[1]

Plasma Process. Polym. 2009, 6, S352–S356

S352 ß 2009 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim DOI: 10.1002/ppap.200930804
Optical and Langmuir Probe Diagnostics in a Magnetized . . .
Experimental Conditions and Data
Evaluation
Figure 1 shows the experimental set-up. Mainly it consists
of the hollow cathode made from LaB6 with gas feed and
water-cooled anode. At the position of the cathode a
Helmholtz coil is mounted which delivers a magnetic field
of Bmax ¼ 30 mT. The LP can be positioned at two distances
to the cathode: dLP ¼ 25 and 60 cm. At dLP ¼ 25 cm were also
placed windows for OES-measurements. The HCA was
running in a current range from 15 to 110 A in a gas flow
range from 20 to 80 sccm. The upper gas flow rate was
restricted by the pump speed. A butterfly valve was
installed between the plasma volume and the pump so
that the pressure in the chamber could be changed
independently from the gas flow rate. Pressures applied
ranged between 0.3 and 5 Pa.
Measurements discussed in this paper were performed
in Ar and Ar/He, Ar/N2, N2/He mixtures at different
pressures. At discharge currents in the range of 15–110 A,
the discharge voltage ranges from 32 to 42 V. The magnetic
field strength was changed from 0 to 25 mT. For emission
spectroscopy, a spectrometer of 30 cm focal length together
with a CCD-camera and a glass fiber were used. A spectral
resolution of 0.05 nm could be achieved. The spectroscopic
system was calibrated in the region of 350 and
750 nm
with standard tungsten-ribbon-lamp.
Measurements of plasma parameter by OES are often
based on the assumption that the EEDF corresponds to a
Maxwellian distribution.[3] This assumption was checked
for the conditions in the HCA. For this reason, we applied a
collisional radiative model which considers those processes
and quantities that are mainly influenced by the EEDF in the
HCA in mixtures of argon/nitrogen, argon/helium, and
nitrogen/helium. This method used for the determination of
the EEDF without the assumption of a Maxwellian
distribution function was successfully applied in earlier
works in noble gases.[4,5] It can be extended to the analysis of
molecular spectra of nitrogen and atomic spectra of He and
was utilized for the determination of the EEDF in glow- and
ECR-discharges.[6–8] By measuring the relative intensity of
Figure 1. Experimental set-up of the HCA-device.
Plasma Process. Polym. 2009, 6, S352–S356
ß 2009 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
several lines with different excitation thresholds the EEDF is
obtained in a trial and error procedure by a regularization
routine. The EEDF between 1.5 and 4.5 eV was determined
from the vibrational distribution of excited molecular states
of nitrogen.[6–8] The EEDF in the energy range higher than
11 eV was evaluated from the intensities of different
emission lines and bands of He, Ar, and N2, respectively. The
reliability of the EEDF obtained in this way depends on the
systematic errors in the experimental device as well as on
the accuracy of the model and on the reliability of the atomic
and molecular data implemented. An increase in the
number of lines improves the quality of the result. This
spectroscopic method can be applied in a wide range of
plasma parameters and gives at least an educated guess of
the EEDF also at conditions where no other methods are
available.
The recording and evaluation of data in LP- as well as
OES-measurements were carried out in computer-assisted
devices.
Experimental Results and Discussion
Results of LP-measurements of the ion resp. electron
density in dependence on arc current and total pressure in
argon are shown in Figure 2a. The probe was located at a
distance to the cathode dLP ¼ 25 cm, the Ar-gas-flow rate
amounts to 60 sccm. In the figure, the solid lines represent
density measurements calculated from the OML-corrected
ion saturation current. At a pressure of p ¼ 0.5 Pa, data of
this method are compared with results obtained by the
integration of the EEDF (dotted line). Within an error bar of
20% the data of both methods agree well. In the whole
range shown the ion density increases nearly linearly with
increasing current. The ionization degree x remains
constant at x  0.4% between pressure variations of 0.3–
1 Pa and then drops linearly to x ¼ 0.24% at p ¼ 2 Pa
(discharge current I ¼ 100 A, QAr ¼ 60 sccm, B ¼ 0 mT). This
high ionization degree at low pressure recommends the
HCA for the application in PEPVD. The ion density in
dependence on magnetic field, which is localized at
cathode, shows no remarkable effects
at the probe position. This result is in
contradiction to measurements in HCA-
set-ups where the whole arc column was
magnetized.[9,10] In these devices the
charge carrier density could be increased
up to one order of magnitude by
increasing the magnetic field from 0 to
500 mT.
The excitation rate of an atom energy
level from the ground state is propor-
tional to the ground state density n0 and
the electron density ne. Taking into
www.plasma-polymers.org S353

Figure 2. (a) Electron density in dependence on discharge current
at different pressures, measured by LP at a distance from cathode
to LP dCP ¼ 25 cm. (b) Electron density in dependence on the
discharge current at different pressures, measured by OES at a
distance to the cathode d ¼ 25 cm.
account the excitation and de-excitation processes of
different atom energy levels, it has been shown that for
different atoms the ratio of different line intensities only
depends on electron density.[11,12] In the experiments
presented here, OES-diagnostics and data evaluation for
electron density measurements were performed with
intensity ratios of the following lines: He-lines ratio
[667.8 nm (31D-21P)]/[728.15 nm (31S-21P)],[5] He-lines
ratio [492.2 nm (41D-21P)]/[504.8 nm (41S-21P)],[11] and Ar-
lines ratio [365 nm (4p1) þ 360.7 nm (4p5)]/[425.9 nm
(3p1)].[12] Figure 2b) shows the dependence of electron
density on current measured by OES in an argon/helium
mixture at a distance of 25 cm from the cathode on the
axis. Note that the minimum electron density which can
be detected by this technique is in the range
of 1016 m
3.[11,12] So the measurements at low discharge
current are characterized by large error bars. Figure 2b
shows that with increasing current the density increases
almost linearly similar to the results of probe measure-
ments. The electron density cannot be evaluated by LP-
Plasma Process. Polym. 2009, 6, S352–S356
S354 ß 2009 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
G. Avaria, A. Lunk, A. Schröder, I. P. Vinogradov
measurements in an Ar/He mixture on the basis of ion
saturation current because the ratio of Arþ-/Heþ-ions is
not known. Evaluation of the electron density based on the
integration of the VCC-second-derivative could not be
performed at these conditions because the high electron
saturation current destroyed the probe due to evaporation.
So a direct comparison of density data of both methods
was not possible.
A better comparison of data received by LP- and OES-
method can be obtained by measuring the EEDF resp. the
mean kinetic energy of the electrons. Here, the restriction
of high electron densities (ne  1016 m
3) is not valid. In
LP-measurements the electron current was fitted by a
Boltzmann-fit after subtraction of the ion current from
the entire current. The fitting procedure performs a
nonlinear fitting of the given signal to a sum of
Boltzmann functions by using nonlinear Marquardt–
Levenberg optimization. After the fitting procedure the
VCC is—if it was necessary—smoothed and the first and
second derivative of the VCC voltage were calculated. The
plasma potential could be derived from the first
derivative. The second derivative was adapted by the
generalized Druyvesteyn distribution function for the
EEDF. The reliability for the fit of the second derivative of
the VCC by a Druyvesteyn EEDF distribution is demon-
strated in Figure 3a. It shows the measured VCC with the
corresponding fitted curve. The second derivative of the
fitted VCC is well fitted by a Druyvesteyn distribution fD
which corresponds to:
  p 
" me 2
fD ¼ Ap "1=2 exp
Bp ; with " ¼ v ;
eTe 2
p ½Gð5=2pÞ3=2 2Gð5=2pÞ p
 
Ap ¼ Bp ¼
h"i3=2
e ½Gð3=2pÞ5=2 3Gð3=2pÞ
Here p is an adaption parameter with p  1. p ¼ 1
denotes Maxwellian- and p ¼ 2 Druyvesteyn-distribution
function. eTe is defined as the mean kinetic energy
according to 32 eTe ¼< " >e . In Figure 3a the coefficient p
corresponds to p ¼ 1.87. Typical results for the dependence
of mean kinetic energy on discharge current are shown in
Figure 3b. The mean kinetic energy does not depend on
current and also not on pressure in a wide range. If we
assume an error bar of 20% for the determination of the
mean kinetic energy the deviations from < " > ¼ 3 eV are
inside of the error bars in Figure 3b.
The data of EEDF measurements by LP were compared
with data from OES. The following assumptions are
implemented in the evaluation of OES-data measured in
the HCA:
(i) Excited states of He atoms (He) can be populated by
direct excitation He(1S0) þ e ! He þ e, and by excita-
tion via the metastable states Hemet [He(1S0), or
DOI: 10.1002/ppap.200930804
Optical and Langmuir Probe Diagnostics in a Magnetized . . .

Figure 3. (a) Fitting of the VCC and adaption of the second

derivative of VCC with generalized Druyvesteyn distribution. Figure 4. (a) Dependence of electron temperature on the dis-
(b) Dependence of the mean kinetic energy on discharge current charge current in the HCA at different mixtures, measured by OES
in the HCA, measured by LP. (d ¼ 25 cm). (b) Mean kinetic energy/electron temperature in
dependence on magnetic field strength; comparison between
LP- and OES-measurements (d ¼ 25 cm).
He(3S1)] He(1S0) þ e ! Hemet þ e, Hemet þ e ! He þ e.
Excitation cross-sections of metastable states are Figure 4a shows the summarized results of EEDF-
5.1  10
18 and 4.5  10
18 cm2 for He(3S1) and measurements by OES. At all measuring conditions the
He(1S0), respectively).[13] form of the EEDF could be approximated by a Maxwell-
2 þ
(ii) Nþ


2 B Su state can be populated by direct excitation, distribution in contradiction to LP-measurements. The
penning ionization [He(3S1, 1
S0) þ N2(X) ! Nþ
2 discharge current was changed from 30 to 60 A and
2 þ [14]


B Su þ He] with a rate constant k ¼ different gas mixtures (Ar/He, Ar/N2, and He/N2) were
7.1  10
11 cm3s
1 for He(3S1), k ¼ 17  10
11 cm3 applied. The electron temperature does not depend on the
s
1 for He(1S0), and by a two step excitation process discharge current similar to the results of LP-measure-
through the ground state of Nþ 2 ðXÞ. ments and it does also not depend on the species of gas
(iii) In the mixture of Ar/N2 are considered[15] the followin- mixture. The averaged value is about eTe ¼ 4.0  0.5 eV in
genergy transfer processes for the additional popu- contrast to hei ¼ 3 eV measured by LP. The electron
lation of nitrogen molecule in excited states: Ar(3P2) þ temperature measured by OES showed a similar behavior
N2(X) ! N2(C3Pu) þ Ar with k ¼ 2.9  10
11 cm3s
1; by applying the longitudinal magnetic field at the cathode.
Ar(3P2) þ N2(X) ! N2(B3Pg) þ Ar with k ¼ 0.6 10
11 cm3 Measurements indicate no dependence on the discharge
s
1. Because of the relatively high electron density the current in the range of 20–70 A as well as on the species in
stepwise processes via metastable states of Ar and He gas mixture at a constant magnetic field strength of 20 mT.
atoms as well as N2(A) molecules must be taken into However, the electron temperature is increased up to the
account. value eTe ¼ 7.8  0.8 eV.

Plasma Process. Polym. 2009, 6, S352–S356

ß 2009 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.plasma-polymers.org S355

The application of a longitudinal magnetic field located
at the cathode changes the electron density and electron
temperature close to as well as faraway from the cathode.
The magnetic field influences the processes in the cathode
range two-fold. First: the longitudinal magnetic field
bundles the beam-like electrons which leave the cathode.
These bundled electrons increase the density far from the
cathode on the axis. The second influence refers to the
processes inside cathode. We can assume that the energy
of the electrons which are accelerated in the cathode drop
inside the cathode-hole is in the range of 15 eV in
argon.[16,17] Then the gyro radius of electrons results in
1.3 mm at 10 mT—comparable to the radius of cathode.
The gyration of electrons can only influence processes
inside the cathode if the ratio of gyro frequency

over electron collision frequency vg ne > 1. In argon

with a magnet field strength of 25 mT results vg ne  1
for p 3 mbar (elastic collisions are taken into account
as the main processes). In former measurements in
static systems it was shown that the HCA effect is
working if the product pressure  cathode-diameter
( p  d)  1.3 mbarcm. The pressure inside the cathode
cannot be measured in the flow regime. Otherwise, it is
known from previous experiments that at very low gas
flow rates the HCA becomes instable, probably because of
the pressure is to low inside the cathode. Hence, we
conclude that at very low gas flow rates the longitudinal
magnetic field influences the discharge processes inside
the cathode by inducing a gyration movement of the
electrons. However, this effect disappears at higher gas

flow rates because in this case one obtains vg ne < 1 and
only the first effect mentioned is efficient.
Spectroscopic measurements were compared with
probe measurements with and without magnetic field.
The results of both methods agree within the limits of the
experimental errors at measurements if the magnetic field
is equal to zero. But probe measurements strongly disagree
from spectroscopic data if the magnetic field is applied.
Figure 4b shows the dependencies of mean kinetic energy
on applied magnetic field strength (distance cathode—
measuring position d ¼ 25 cm). Data obtained from probe
measurements are compared to spectroscopic ones for
different values of HCA discharge current. While hei
measured by LP decreases or remains nearly constant
with increasing magnetic field the spectroscopic measure-
ments show a strong increase. This disagreement could be
caused by the different measuring methods applied. The
cylindrical LP is not sensitive to the high energy tail of the
EEDF in contrast to the spectroscopic method where the
Plasma Process. Polym. 2009, 6, S352–S356
S356 ß 2009 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
View publication stats
G. Avaria, A. Lunk, A. Schröder, I. P. Vinogradov
high energy tail contributes strongly to the excitation of
atoms. Further experiments with plane LPs are in
preparation.
Conclusion
The EEDFs evaluated from LP measurements differ from
Maxwellian ones and can be approximated by the
generalized Dryvesteyn-distribution. The mean kinetic
energy of the electrons in dependence on current remains
constant and shows no significant dependence on
current. The application of a longitudinal magnetic field
to the cathode of HCA seems to change the electron
temperature of the electrons drastically. At higher
magnetic fields (B > 10 mT) results of the spectroscopic
measurements of the electron temperature deviate from
those received by cylindrical LP.
Received: September 25, 2008; Accepted: January 23, 2009; DOI:
10.1002/ppap.200930804
Keywords: DC discharge; electron-energy distribution function;
hollow cathode arc; Langmuir probe; optical emission spectro-
scopy
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DOI: 10.1002/ppap.200930804