Thin Solid Films 518 (2010) 6705–6713

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Thin Solid Films

j o u r n a l h o m e p a g e : w w w. e l s ev i e r. c o m / l o c a t e / t s f

Special feature

Cold atmospheric plasma: Sources, processes, and applications

L. Bárdos, H. Baránková ⁎
Uppsala University, Ångström Laboratory, Plasma Group, Box 534, SE-751 21 Uppsala, Sweden

a r t i c l e i n f o a b s t r a c t

Available online 14 July 2010 Atmospheric pressure gas discharge plasmas, especially those operated at energy non-equilibrium and
low gas temperatures, have recently become a subject of great interest for a wide variety of
Keywords: technologies including surface treatment and thin-film deposition. A driving force for these
Cold atmospheric plasma developments is the avoidance of expensive equipment required for competing vacuum-based plasma
Non-equilibrium plasma technologies. Although there are many applications where non-equilibrium (cold) plasma at atmo-
Atmospheric plasma sources
spheric and higher pressures represents a substantial advantage, there are also a number of applications
Atmospheric plasma processing
Surface activation
where low-pressure plasmas simply cannot be replaced due to specific properties and limitations of the
Surface treatment and deposition atmospheric plasma and related equipment. In this critical review, the primary principles and
characteristics of the cold atmospheric plasma and differences from vacuum-based plasma processes
are described and discussed to provide a better understanding of the capabilities and limits of emerging
atmospheric plasma technologies.
© 2010 Elsevier B.V. All rights reserved.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6705
2. Generation of non-equilibrium atmospheric and high-pressure plasmas . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6706
2.1. Generation of plasma between electrodes—the Paschen curve . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6707
6706
2.2. Generation of plasma by an electromagnetic field . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6707
2.3. Suppressing arcs and streamers in atmospheric plasmas generated with atomic and molecular gases . . . . . . . . . . . . . . . . . 6708
6707
3. Cold atmospheric plasma sources . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6708
3.1. Corona and dielectric barrier discharges (DBD) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6708
3.2. Microwave discharges and atmospheric pressure plasma jets (APPJ) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6709
6708
3.3. Novel plasma sources for large-area surface treatments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6710
6709
4. Applications of cold atmospheric plasma in surface processing and film deposition. . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6711
6710
4.1. Surface activation and treatment by atmospheric plasmas . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6711
6711
4.2. Deposition of films in atmospheric plasmas . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6712
6711
4.3. Post-treatments of films and particles by atmospheric plasma . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6712
5. Novel and emerging applications of the cold atmospheric plasma . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6712
6. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6713
6712
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6713
6713
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .6713
.

1. Introduction is usually denoted as an electric discharge. The plasma (or more

When delivering power into a neutral gas, a fraction of gas
particles can be converted (ionized) into charged particles to form
plasma. The plasma generated by electric or electromagnetic fields
⁎ Corresponding author.
E-mail address: Hana.Barankova@Angstrom.uu.se (H. Baránková).
correctly, the gas discharge plasma) can be characterized as a
partially ionized gas containing neutral particles as well as an
equivalent number of negative electrons and positive ions. Note
that there are also fully ionized plasmas (primarily at low gas
pressures) where all particles are ionized, and also plasmas with
negative ions (in electronegative gases), but these will not be
discussed here.

0040-6090/$ – see front matter © 2010 Elsevier B.V. All rights reserved.
doi:10.1016/j.tsf.2010.07.044
6706 L. Bárdos, H. Baránková / Thin Solid Films 518 (2010) 6705–6713
Depending on required applications, there are a wide variety of
plasmas generated under different conditions. One of the most
important characteristics is the gas pressure. At a given gas
temperature, the pressure defines the total density of gas particles
and consequently also the probability of mutual collisions among
particles, i.e. the collision frequency. The higher the gas pressure,
the higher the collision frequency and hence the higher the
probability that with time the particles will reach a steady-state
energy equilibrium. The first ionization potentials of elements are
from several eV up to a maximum of 24.6 eV (for He), where the
equivalent thermal energy kT of 1 eV corresponds to a tempera-
ture T of approximately 11,600 K ≈ 11,300 °C. In thermal equilib-
rium, all particles have the same temperature, including the
neutral gas. Examples are central parts of lightning flashes and the
core of the sun. However, there are also man-made systems
generating hot (thermal) plasma, like arc torches used in waste
incinerators or well-known electric arcs in welding. The thermal
plasma is suitable for pyrolytic processes and applications in
metallurgy, high temperature chemistry, thermal spraying, etc. [1–
3].
In a great number of plasma applications, particularly those in which
the plasma must interact with a solid substrate without damaging it, the
temperature shouldn't exceed roughly 1000 °C; for some applications,
the temperature limit is much lower, close to room temperature. In such
cases, we need relatively “cold” plasma that cannot be in thermal
equilibrium. Non-equilibrium plasmas can be generated at low gas
pressures where collisions are not so frequent. Diverse low-pressure
plasma systems and processes applied to surface processing technolo-
gies are described in many books, e.g. [4–13], and in a large number of
articles and reports. Because low-pressure plasma systems require
expensive vacuum systems and pumps, there has been a growing
interest, mainly over the last two decades, to replace these systems by
non-equilibrium cold atmospheric plasmas.
This article summarizes the primary principles and characteristics of
cold atmospheric plasmas and differences from reduced-pressure
plasmas in order to provide a better understanding of the capabilities
and limits of the non-equilibrium atmospheric plasma. A review of
several cold atmospheric plasma sources, their capabilities, and
achieved results is then discussed with particular focus on coating and
surface processing technologies.
2. Generation of non-equilibrium atmospheric and
high-pressure plasmas
Due to continuous cosmic radiation, there are electron-ion pairs
(ionization) present even in ambient air at normal temperature and
pressure. The ionization rate is affected by radioactive substances both
in the ground and in the air, as well as by cosmic radiation, but is only
approximately 107 ion-electron pairs per s per m3 [14].
Any kind of energy can be used for ionization e.g., electrical, thermal,
optical (e.g., UV light), radioactive (e.g., gamma radiation), X-rays, etc.
However, the most useful ionization tools are electric or electromagnetic
fields. Accounting only for cosmic radiation, the ionization rate in air is of
the order of 106 m− 3 s− 1 ion-electron pairs (1 ion per cm− 3 s− 1). Thus,
dry air is electrically insulating. When applying a voltage of about 30 kV
between electrodes separated by 1 cm in ambient air, i.e. an electric field
of 30 kV/cm, electric breakdown and ignition of an atmospheric air
plasma can occur. Such breakdown can have the form of discrete sparks as
in engine spark plugs, but under certain conditions it is also possible to
create a uniform-looking steady glow-type air discharge.
The properties of plasmas, such as the density of charged particles
(the densities of negative and positive charges are equal) and their
energies, generally depend on the power, type of power (e.g. AC, DC,
pulsed, frequency, etc.), type of gas, etc. The negative electron and
the singly charged positive ion have the same charge (1.6 × 10− 19C),
but different masses. The mass of electrons (9.11 × 10− 31 kg) is
approximately 103–104 times lower than the mass of ions (mass
number × proton [or neutron] mass [1.67 × 10− 27 kg]). Therefore,
light and mobile electrons acquire more energy from the incident
electromagnetic field than the heavier ions. In plasmas generated at
low gas pressures, where the collision frequency is low, electron
energies remain high compared to ion energies (and energies of gas
particles): this represents non-equilibrium in the plasma. Converse-
ly, high gas pressures with correspondingly high collision frequen-
cies lead to equilibrium (hot) plasmas. At atmospheric and higher
pressures, the most feasible way to create non-equilibrium plasmas
is “pumping” of power selectively to electrons. Methods and systems
for this purpose are described in Section 3.
2.1. Generation of plasma between electrodes—the Paschen curve
Almost all textbooks covering gas discharge plasmas describe
Townsend's theory of gas breakdown and current sustainment in an
electric field between negative (cathode) and positive (anode) electro-
des with separation d, see e.g. [15]. The production of electrons in a
simple diode system is described by two Townsend's coefficients, α and
γ. Coefficient α represents the probability that an electron emitted from
the cathode collides along a unit length with a neutral gas particle and
forms an ion and an additional electron. Subtracting the initial electron,
the total number of ions produced along the distance d is [exp(α d)− 1].
The positive ions are attracted to the cathode and upon impact form
secondary electrons with probability γ. Thus γ [exp(α d)− 1] new
electrons can be generated by one initial electron and take part in
subsequent ionizations in an avalanche type process. A simple balance
equation for steady-state ionization is then:
γ ½expðα dÞ – 1 = 1: ð1Þ
In these collision-based ionizations the coefficient α depends
directly on gas pressure p which controls the collision frequency
(α ∝ p) and inversely on the mean free path λe of electrons (α ∝ 1/λe).
As can be seen in Eq. (1), the coefficient γ (production of secondary
electrons) is also very important for ionization and formation of a
steady-state current. γ, often called the secondary electron emission
(SEE) coefficient, depends on a number of factors, e.g. material and
temperature of the cathode, the gas, effects of energetic UV radiation,
etc. It also depends on the cathode surface pretreatment (mechanical,
chemical, thermal, etc.) [16,17]. Note that many ceramic materials have
higher γ coefficients than metals and can generate more electrons
[17,18]. This advantage can be utilized in high frequency AC or pulsed DC
discharges, such as dielectric barrier discharges (DBD) where charge
buildup on insulator surfaces is periodically removed.
Conditions for breakdown at different gas pressures were first
studied by F. Paschen [19]. The result is the well-known Paschen curve
describing the function of the breakdown voltage VB on the distance d
between electrodes and the gas pressure p, i.e. VB = f (pd). For all
gases, the Paschen curve has a concave up form indicating that there is
always an optimal value of the product pd at which the breakdown
voltage has its minimum. On both sides of the minimum, the
breakdown voltage increases. At low pressures, the density of gas
particles available for ionization is low. At high pressures, however,
the collision frequency is high and electrons cannot acquire enough
energy to ionize along the short path between collisions. The equation
for the breakdown voltage VB is based on fitting experimental data.
According to [20], the Paschen equation can be written as:
VB = B pd=½lnðA =lnð1+1 = γÞÞ+ lnð pdÞ; ð2Þ
where A and B are constants dependent on the type of gas. For air at
room temperature A = 15 cm− 1 Torr− 1, B = 365 V cm− 1 Torr− 1, and
γ = 10− 2 (assuming Cu electrodes). For atmospheric pressure
(0.1 MPa = 760 Torr) and an electrode separation of d = 1 cm, Eq. (2)
 L. Bárdos, H. Baránková / Thin Solid Films 518 (2010) 6705–6713
yields a DC breakdown voltage of VB ≈ 35.5 kV. For an air pressure of
1 Torr (133 Pa), the breakdown is VB ≈ 310 V. Both values agree with
experiment. The experimental DC breakdown values for several gases in
a 1 mm gap are: 3.2 kV in air, 1.5 kV in Ar, and 0.75 kV in He, [21]. Note
that He exhibits the lowest breakdown voltage, while many molecular
gases need very high voltages (e.g., SF6) and can be used as an insulator.
Note also that the breakdown voltage can be decreased in suitable gas
mixtures by the Penning effect (an ionization process resulting from
collisions between excited metastable particles and neutral particles
which have a lower ionization potential than the excitation potential of
the metastable particles) [22,23].
2.2. Generation of plasma by an electromagnetic field
In DC systems, gas breakdown starts in a stationary electric field
between electrodes. Due to high collision frequencies at high gas
pressures, it is nearly impossible to generate a non-equilibrium glow-
type cold plasma by simple DC power. The DC breakdown usually starts
as a transient discharge in the form of a spark and at higher powers it
easily turns into a high-current hot arc.
Gases can also be ionized by oscillating electromagnetic fields having
amplitudes of the electric component high enough for breakdown. Due to
the vastly different mobilities of electrons and ions, at high frequencies the
AC fields enable “pumping” of the power selectively to electrons, thus
enabling a non-equilibrium cold plasma at high gas pressures. The
electromagnetic power (e.g., microwaves) can be radiated into the plasma
without need of electrodes (“electrodeless” discharges). Alternatively, the
electrodes in AC discharges can be covered by dielectrics, preventing
ohmic current and allowing only displacement (convective) current. This
approach is used in DBD systems (see Section 3).
With some simplifications, the principles valid for DC breakdown can
also be applied for AC breakdown between electrodes. Fig. 1 shows
experimental peak-to-peak values Vpp of the minimum breakdown
voltage in an RF powered fused hollow cathode system at atmospheric
pressure (see Section 3.3) plotted as a function of the SEE coefficients of
individual gases for a W cathode, [24]. Once a steady-state current is
sustained, the voltage is considerably lower. In AC breakdown studies,
root mean square voltages Vrms are often used instead of Vpp, but there
pffiffiffi is a
simple relation between these values for sine waveforms, Vpp =2 2Vrms.
It is also seen in Fig. 1 that Vpp for gas breakdown is lower at higher
frequency. Detailed studies reported in [25] show that the breakdown
voltage (given in Vrms values), which depends on the gas, decreases with
AC frequency due to a change in the electron loss mechanism. At high gas
pressures, the electrons make many collisions per oscillation, thus the
motions of electrons and the electron loss are very much controlled by
diffusion. Therefore, the production of secondary electrons at electrode
Fig. 1. Peak-to-peak voltages Vpp for ignition and operation of an RF-powered fused
hollow cathode (FHC) at atmospheric pressure vs. the secondary electron emission
coefficients for air, N2, Ar, and Ne discharges on W [24].
6707
surfaces is also less important. Under these conditions, not only is the
magnitude of the electric field important (voltage and electrode
separation), but also the phase of the electron motion with respect to
the AC electric field has a governing effect [26,27]. The velocity of
oscillating electrons is mobility-controlled, and the mobility is a function
of the gas. The breakdown voltage Vrms is increased considerably when, for
example, Ar, O2, or N2 is added to He, despite the lower ionization
potential of the additives, due to additional electron energy loss channels
(e.g., electronic excitations, for molecules also vibrational and rotational
excitations, or dissociation) [25]. According to recent studies [28], the
dependence of the minimum breakdown voltage Vrms on frequency
between 2 and 100 MHz has a concave up shape which depends on the
distance d between electrodes. At distances exceeding 1 mm, the Vrms
value of the minimum breakdown voltage first decreases with frequency
up to about 15 MHz, and then increases because rapid oscillations prevent
electrons from reaching their maximum kinetic energy. Understanding
the details of breakdown mechanisms, particularly at higher frequencies,
in transient regimes (ns and shorter pulses), with complex organic gas
mixtures (e.g. organosilanes with hydrochlorides or hydrocarbons), for
plasma enhanced chemical vapor deposition (PECVD) of films, etc., will
certainly require further studies.
2.3. Suppressing arcs and streamers in atmospheric plasmas generated
with atomic and molecular gases
A typical feature of atmospheric discharges at high voltages between
electrodes separated by more than several millimeters is formation of
local arc filaments. These filaments are also called streamers. The
streamers are generally more probable in molecular than atomic gases,
because of additional power absorption channels in molecules (rotation,
vibration, excitation, dissociation, and ionization) compared to atoms
(excitation and ionization), [21,29]. A picture of intense arc streamers in
a pulsed DC air plasma (5 kV, 3 kHz) generated in a 1.5 mm gap between
electrodes is shown in Fig. 2.
Properties of streamers, for example the propagation velocity, the
diameter, branching and shape, are primarily affected by the applied
voltage, electrode separation, and content of molecular gas, e.g. O2 in a
He carrier gas [30]. It is interesting to note that streamers can be thought
of as “micro-lightning”. The 30 kA currents in a typical lightning flash
with current channel diameters of about 0.1 m (1–10 m is the light
channel diameter) in thunderstorms compare well with 1 mm diameter
air streamers having a current of 3 A. The current density in both
“flashes” is 1.2 kA/cm2. In addition, streamers often exhibit branching,
similar to lightning flashes, and both are quite noisy.
The streamers make the plasma strongly non-uniform and are not
desirable for surface treatments since hot streamer arcs can damage
surfaces, especially for soft materials such as polymers. There are
several options for avoiding streamers, stabilizing the discharge, and
forming glow-type plasmas at atmospheric pressure. The most useful
approaches are listed below.
i. Using high-frequency AC fields or short-pulsed DC power. An
example is the use of microwave power (2.45 GHz) which has a
stabilizing effect on volume ionization without introducing
electrode-based secondary electrons. Depending on the gas
Fig. 2. Arc streamers in an air plasma generated by a pulsed DC voltage of 5 kV at 3 kHz
in a gap width of 1.5 mm.
6708 L. Bárdos, H. Baránková / Thin Solid Films 518 (2010) 6705–6713
used, atmospheric microwave plasma columns often have a
tendency for axial contractions. However, the radially-contracted
tubular noble gas discharge can be converted into a fully
expanded discharge by admixing another noble gas having a
lower ionization potential [31]. The required content of the
minority gas is below 1% and its optimum value is specific to the
noble gas used. In pulsed DC plasmas, pulse parameters can
strongly affect streamer formation. Streamers were found to
appear after about 100 ns [32]. It is therefore possible to suppress
the streamers by short (≤ 10 ns) pulses, where arcs do not have
sufficient time to develop.
ii. Using dielectric barriers on AC electrodes in Dielectric Barrier
Discharge arrangements (Section 3.1) with displacement currents.
The choice of barrier material is very important due to charging
effects, Penning ionization effects on surfaces, etc. The performance
of the barrier is also dependent on the gas and the field frequency.
For example, it has been observed [33] that propagation of a
discharge is retarded and its channel width is significantly
increased when it moves towards a highly-charged dielectric
surface. In an electronegative gas (air), the propagation velocity is
two orders of magnitude higher than in He. Formation of desirable
uniform diffuse-type discharges in air is based on sufficient
dielectric surface-charge and numerous overlapping partially
diffuse breakdowns. Radially expanding streamers then provide
space-charge necessary for self-stabilization of a glow-like plasma
[34]. As can be expected, an important factor in the performance of
the discharge is the dielectric constant of the barrier [35].
iii. Using high gas flow rates. The gas flow rate controls the
residence time of particles in the plasma and power-per-
particle values. Flowing gas also has a cooling effect [36]; it
affects the length of the flowing plasma [37] and can suppress
or prevent the formation of hot arcs.
iv. Using special electrode shapes with multiple structures having
sharp edges or cones forming high intensity local electric fields
to decrease the breakdown voltage and stabilize a uniform
discharge over the electrode surfaces [38,39]. However, arcs are
likely to form on these sharp parts and the applied power must
therefore be optimized to maintain the plasma in a glow
regime. Alternatively, this very principle can be utilized in
special arc sources (“Glidarc”) for plasma-reactive gas treat-
ments in which pairs of knife-type electrodes generate arc
streamers gliding along the sharp edges [40].
v. Selection of suitable gas. Atmospheric discharges are most
easily sustained in He, due to its small diameter (≈2.8 Å, while
the air molecule has a diameter ≈9.7 Å) and, thus, long mean
free path compared to other gases, as well as a high SEE
coefficient γ enabling a low breakdown voltage.
It is important to note that the efficient suppression of streamers and
the formation of an uniform glow-type atmospheric plasma usually
requires combinations of several of the methods described above.
3. Cold atmospheric plasma sources
A large number of different sources of cold atmospheric plasma
have been designed and developed since the first DBD reactor was
built in the 19th century by W. von Siemens for the production of
ozone [41]. In addition to the wide variety of DBD plasma sources
described in the literature, there are many reports about microwave
plasma systems, microhollow cathode systems, various plasma jets,
plasma arrays, “on-chip” plasmas, etc. Note that for certain applica-
tions, it is also possible to utilize the decaying part of a thermal plasma
where the gas temperature is ≤500 °C [42]. However, thermal plasma
sources usually require considerable power and large gas throughputs
which compromise their efficiency as a cold plasma tool.
Fast ICCD (intensified charge coupled device) camera observations
with 100 ns exposure time and 1000 shots accumulated to form one
picture reveal an interesting feature in atmospheric pressure plasma jets
(APPJ) operated in He and Ar. The homogeneous-looking plasma is
actually not homogeneous. It operates like a “plasma gun”, blowing fast
small “plasma bullets” out of a nozzle [43]. While this feature may not limit
the surface processing abilities of plasma jets, it is certainly important for
the selection of gas inlet positions and gas type. Laminar gas flow is very
important for transport of activated species from the plasma jet to the
surface without substantial mixing with ambient air [43].
Contrary to plasmas at reduced gas pressures available in large
volumes, the short mean free paths at atmospheric pressure limit the
volume and the impact of the plasma. In applications where three-
dimensional objects are to be treated, the decaying and afterglow
regions of the flowing plasma must be used with special jet designs
allowing long plasmas [44]. These systems often require massive gas
throughputs to prolong plasma columns [37,44] and are typically
operated with He, which is expensive. An exception is the hybrid plasma
source (Section 3.2). Treatments of large substrates by jet-type plasmas
require relative motion between the plasma-jet and the substrate. The
plasma source can also be designed as a jet array [45,46].
The plasma density and other parameters of cold atmospheric plasmas
have been reported in a number of articles, e.g. [31,47–51]. Values of
plasma densities depend on the type of source, gas, and power, and range
from 1011 to 1016 cm− 3 which represents up to approximately 0.1% of the
total density of neutral particles (≈ 2.7×1019 cm− 3) at atmospheric
pressure. The highest values of plasma density (≈ 6×1017 cm− 3) have
been reported for the microwave plasma torch operated at 4 kW power in
He [51]; however, at such power the plasma can also be quite hot. The
electron temperatures reported for different plasmas reach up to several
eV [52]. The gas temperature is typically of the order of 103 K [53] and also
depends on the source, gas type, and applied power.
3.1. Corona and dielectric barrier discharges (DBD)
The most popular cold atmospheric plasma sources are based on
DBD, see for example reviews [54,55]. A dielectric barrier at one or both
electrodes can suppress and, in combination with high frequency
power, prevent streamers. There are a large number of different designs,
constructions, electrode shapes, and dielectric barriers used in DBD
sources for different applications. Some of these systems are schemat-
ically shown in Fig. 3. A simple corona (not a DBD) arrangement with
streamers is shown in Fig. 3a for comparison with DBD arrangements in
Fig. 3b. DBD systems for treatments of moving planar substrates are
displayed in Fig. 3c and d. For large-area treatments, a multiple DBD
arrangement can be used with a pair of grid-shaped electrodes covered
by an alumina barrier, Fig. 3e [56]. In all DBD systems, the accumulated
surface charges on dielectric barriers must be neutralized, e.g. by bipolar
pulsed DC power in either static or flowing gas regimes.
3.2. Microwave discharges and atmospheric pressure plasma jets (APPJ)
As discussed in section 2.2, high-frequency fields have a stabilizing
effect on the plasma and can generate streamerless plasmas in
molecular gases. RF power (13.56 MHz and its harmonics) and
microwave power (typical industrial power oscillators operate at
896 MHz, 915 MHz, 922 MHz, 2.45 GHz, and 5.6 GHz) are often used
to generate non-equilibrium plasma columns and jets. Some of these
plasma sources are schematically shown in Fig. 4. The simple microwave
plasma source in Fig. 4a has a tapered waveguide in order to increase the
electric field in the quartz reactor passing through this waveguide [57].
More sophisticated systems utilize waveguide-to-coaxial transitions to
generate plasma jets, see Fig. 4b [58]. The primary disadvantages of the
microwave systems are: (a) high power is often required for plasma
generation and (b) the size of the plasma reactor is limited by
waveguide dimensions. However, the size of the plasma can be enlarged
 L. Bárdos, H. Baránková / Thin Solid Films 518 (2010) 6705–6713 6709

3.3. Novel plasma sources for large-area surface treatments

Many atmospheric plasma sources are based on micro-discharges.

Small atmospheric plasma units are multiplexed to form arrays,
integrated in-line systems, or area-distributed systems. An example is
an array of RF-powered DBD jets [66]. Very special systems for
generation of large area plasmas are based on multiple hollow cathodes
integrated to form a fused hollow cathode (FHC) system. Fig. 6a
schematically shows a FHC with integrated open structure and flowing
gas. Many hollow cathodes, powered by a common RF, or a pulsed-DC,
generator, are positioned close to each other so that individual plasmas
can interact [67]. Such an arrangement enables the use of very low RF
power densities (≥ 0.2 W/cm2 for Ne) and low RF breakdown voltages
while maintaining the plasma over the entire electrode surface. The
fused hollow cathodes can be of different shapes. Fig. 6b shows an
example of a rectangular FHC system operated at an RF power of 40 W
with Ne plasma in open air over an electrode area of 115 mm× 18 mm.

Fig. 3. Corona and dielectric barrier discharge (DBD) arrangements. (a) Corona with
streamers; (b) dielectric barriers on electrodes; (c) DBD arrangement for treatment of
large-area planar substrates; (d) DBD arrangement for two-sided treatments; and (e)
multiple grid-type DBD arrangement (200 μm × 200 μm windows). The arrows in (c),
(d), and (e) indicate the direction of substrate motion.

using different resonators with systems of slots distributed, for example,

outside the reactor and radiating the power toward the reactor axis [59].
Fig. 4c shows a typical RF plasma jet source [60,61]. Such sources
can also be arranged with a dielectric barrier on one or both electrode
surfaces [62,63]. The operating frequency of coaxial plasma sources
can be extended up to the microwave range to suppress streamers
and generate glow-type plasmas in molecular gases.
The hybrid plasma source in Fig. 4d combines a microwave
antenna with a hollow cathode powered by an RF, or a pulsed DC,
generator [64]. This source is termed an H-HEAD (hybrid hollow
electrode activated discharge). The microwave plasma is produced
by surface waves and the particle energies can be controlled both
by the microwave power and by the hollow cathode parameters.
Such a source is capable of producing very long plasma columns
(up to 18 cm) at very low gas flows (≤ 250 sccm) and it works
with both monoatomic and molecular gases [65]. Recent results
demonstrate the possibility of operating the source with water Fig. 4. Microwave and radio frequency (RF) plasma sources. (a) Simple rectangular
waveguide arrangement; (b) plasma jets arranged in the waveguide; (c) coaxial RF
vapor or even submerged in water [13]. The plasma generated by plasma jet arranged as a DBD; and (d) hybrid plasma source with surface-wave antenna
an H-HEAD source, with air flowing through the antenna, serving as a pulsed DC hollow cathode. The longer arrows in (b), (c), and (d) indicate
immersed in water contained in an Al vessel, is shown in Fig. 5. the direction of substrate motion.
6710 L. Bárdos, H. Baránková / Thin Solid Films 518 (2010) 6705–6713
Fig. 5. Plasma generated by an H-HEAD source, with 300 sccm air flowing through the
antenna, immersed in water contained in an Al vessel.
Fig. 6. Fused hollow cathode (FHC) plasma source. (a) Schematic arrangement of an
integrated RF hollow cathode system. (b) Rectangular 120-mm-long FHC source, with
Ne plasma in open air, generated at 40 W.
Employing the methods used in microelectronics and microme-
chanics, it is possible to construct special plasma systems using
multiple small “on-chip” plasma sources distributed over printed-
circuit-board plates [68]. Examples of such small-size sources are an
RF powered inductively-coupled plasma (ICP) chip [69] and a small
resonator-based microwave source [70].
Fig. 7. Low-temperature plasma, incident on human skin, generated in Ar at 50 W
microwave power.
4. Applications of cold atmospheric plasma in surface processing
and film deposition
Surface processing and coating by cold atmospheric plasmas
are among the most intensively studied technologies during the
last decade. Primary applications include: (i) surface pretreatment,
cleaning, and activation or passivation; (ii) deposition of films;
and (iii) post-treatment of coated surfaces in order to change the
chemical composition or crystallinity of the coating. Application
capabilities of non-equilibrium atmospheric plasmas are quite
broad due to their gas temperatures ranging from roughly room
temperature to 1000 °C. An example of a low-temperature non-
equilibrium plasma (gas temperature ≤ 50 °C) is the microwave Ar
H-HEAD (2.4 GHz, 50 W) plasma shown touching human skin in
Fig. 7. Low-temperature plasmas have been tested in the
treatment of living tissues, including human tissue sterilization
and blood coagulation [71], as well as in dental applications [72].
They are also suitable for surface treatments of other kinds of
temperature-sensitive surfaces, such as polyethylene (Section 4.2).
Typical cold atmospheric plasmas are suitable for rapid
production of reactive radicals and for plasma-activated reactions
based on radical chemistry. However, there are no ion-assisted
processes such as those in low-pressure plasma processing of
surfaces. Thus, for some applications, an additional post-treatment
(e.g. annealing or plasma aftertreatment) of cold-plasma treated
surfaces is necessary. Film deposition regimes in cold atmospheric
plasma are generally based on plasma-enhanced chemical vapor
depositions (PECVD). High voltages applied in the plasma at
atmospheric pressure can enhance UV radiation, which can lead to
surface and film activation, gas activation, and the production of
radicals. However, average ion energies are too low for sputtering,
and evaporation processes can be applied only in special
arrangements, for example in an H-HEAD source with an
overheated hollow cathode [64,73].
 L. Bárdos, H. Baránková / Thin Solid Films 518 (2010) 6705–6713
4.1. Surface activation and treatment by atmospheric plasmas
Activation of substrate surfaces, particularly webs, is perhaps the
oldest surface processing application of cold atmospheric plasma. An
increased surface energy (decreased contact angle) after plasma
treatment results in improved adhesion of coatings. For example, the
adhesion of polyethylene terephthalate (PET) and other polymers to
an epoxy can be increased by a factor of 2× to 10× in peel tests after
treatment in the afterglow region of a microwave plasma [74]. In this
arrangement, the process rate has been found to be comparable with
low-pressure plasma treatment [75].
Processing rates depend, however, on the plasma equipment used.
A dramatic increase in the surface tension of polyethylene (PE) and
polyethylene terephtalate (PET) via processing in a Fused Hollow
Cathode plasma can be detected in less than 1 s [24,76]. Measurements
using wetting inks (from Softal Electronic GmbH) according to the
standardized procedure DIN 53364 (ISO 8296) [77] show that the
surface tension of PE increases from ≤34 mN/m (approx. 36 mN/m
for PET) to values ≥56 mN/m after plasma treatment. Fig. 8 shows a
comparison of results on a PE surface (a) before and (b) after a 5 s
exposure to a Ne FHC plasma treatment. A more precise evaluation has
been carried out by dynamic measurements of the contact angle. A
pendant drop of a precisely defined volume is released after triggering
and the shape of the sessile drop is scanned very fast, within fractions of
a second (e.g., 40 scans in 8 s). An increase in the surface tension from
33.5 mN/m to 57.5 mN/m was measured on PE after a 3 s treatment in
Ne+ air FHC plasma [78].
Treatment by DBD plasma can be up to 10 times faster than with
low-pressure plasmas. The plasma treatment can be safely used on
polymers before ink printing without any backside damage or
pin-holing. Detailed studies show that the wetting of a surface is
not determined only by the magnitude of its surface energy, but also
by the free energy of adhesion between the solid and liquid as well as
the surface tension of the liquid [79]. Plasma parameters for surface
treatments must therefore always be carefully optimized.
Due to production of active oxygen species, air atmospheric plasmas
can be used for surface oxidation of, for example Si. Such processes could
replace thermal oxidation, particularly for complex substrate geome-
tries. Early attempts to replace thermal oxidation by low-pressure
microwave plasma oxidation and anodization were reported in the mid
1960s [80–82]. The atmospheric plasma could be a better solution. An
example of rapid Si oxidation by the H-HEAD source (200 sccm Ar,
2.4 GHz/250 W, 1 kV/0.2 A/0.5 μs/250 kHz) is presented in Fig. 9. The
Fig. 8. Effect of FHC plasma activation on PE web surface. Testing ink balls up and forms
drops on an untreated surface (surface energy b 34 mN/m), while on the plasma-
treated surface (surface energy ≥ 56 mN/m) the ink forms a continuous film.
6711
interference colors show that the oxide thickness reaches approximate-
ly 500 nm after 4 min processing of the Si surface (2 cm from the source)
with an Ar plasma jet in ambient air. In these experiments, traces of TiO2
were deposited near the axis of the oxide spot from the Ti hollow
cathode [64]. Another example is the rapid surface oxidation of Mo
substrates performed using a hybrid atmospheric plasma in air [83]. At a
substrate temperature close to 500 °C, polycrystalline MoO3 is formed
after several tens of minutes by plasma treatment over much larger
areas than the diameter of the interacting plasma column on the Mo
substrate. Surprisingly, MoO3 is also formed at the opposite side of the
substrate placed on a stainless steel holder.
4.2. Deposition of films in atmospheric plasmas
Because of the low ion energies in cold atmospheric plasmas, all
coating regimes reported so far are based on PECVD using precursors
diluted primarily in He carrier gas. Most of the results reported so far are
for oxides. For example, amorphous SiO2 films have been grown from
N2 + SiH4 + N2O mixtures on polypropylene substrates [84], and from
tetramethyldisiloxane (TMDSO), hexamethyldisiloxane (HMDSO), and
tetraethylorthosilicate (TEOS) precursors on polycarbonate and poly-
ethylene terephthalate substrates [85] by DBD-based plasma devices.
An RF plasma jet has been used to deposit SiO2 with rates up to 300 nm/
min from tetraethoxysilane/He [61]. A large-area commercial coater for
2-m-wide polyamide webs using a DBD arrangement with multiple
open-perimeter flat conductive liquid-based electrodes in a He plasma
with aerosol sprayed liquid precursors (e.g. alkenes, acrylates) has been
reported in reference [86]. By mixing precursors that have multiple
polymerizable functional groups, different co-polymer coatings with
highly cross-linked networks have been deposited [86].
Table 1 summarizes examples of as-deposited films and
corresponding atmospheric plasma deposition parameters from refer-
ences [83,84,87–99]. As can be seen, in addition to electrically-insulating
oxides, transparent conductive oxides such as Al-doped ZnO, SnOx, and
InOx have been grown. ZnO:Al films deposited at 225 °C have a
resistivity of 3 × 10−2 Ω cm with transparency of 95% over the spectral
range from 375 nm to 2500 nm [90]. Comparable properties were also
reported for SnOx and InOx films [91,92]. An elevated substrate
temperature (up to an optimum near 200 °C) was found to be very
important. Similar to vacuum deposition, film properties can be
modified further by post-deposition annealing.
Several groups have reported using atmospheric plasma PECVD to
grow C-based films. It is noteworthy that film deposition can proceed at
very high rates, 40 μm/min was reported in [93]. However, depending
on intended applications, it is desirable to optimize the growth rate with
Fig. 9. Circular SiO2 region formed in ambient atmosphere on a Si(001) wafer during 4
minutes of interaction with an H-HEAD plasma jet in Ar. Parameters: 200 sccm Ar,
2.4 GHz/250 W, 1 kV/0.2 A/250 kHz.
6712 L. Bárdos, H. Baránková / Thin Solid Films 518 (2010) 6705–6713

Table 1
Examples of films deposited using cold atmospheric plasma.

Film Plasma Power Gases, precursors Rate[nm/min] Year Reference

SiOx 20–50 kHz DBD 10–20 kV Ar + O2 + 0.1% tetramethylsilane (Si[CH3]4) b300 1997 [87] R. Thyen et al.
SiO2 DBD 10 W/cm2 N2 + SiH4 + N2O 12 2000 [84] N. Gherardi et al.
CeOx RF jet in He 360 W (CH3COOH)3Ce in H2O spray 8.33 2003 [88] L. Soukup et al.
TiO2 100 kHz DBD PI 600 W Ti (IV) oxide acetylacetonate (TiO[CH 3COCH = C(O–)CH3]2) in 7.5 2007 [89] C. Jiménez et al.
MOCVD butanol at 0.02–0.1 mol/l
Al:ZnO RF Atomflo™ 40–75 W [diethylzinc (C2H5)2Zn + trimethylaluminum C3H9Al] + O2 in He ≤200 2007 [90] M.D. Barankin et al.
SnOx HV AC DBD ≈ 250 W Mono- or Tetrabutyltin (C16H36Sn) in air at 130 °C ≤ 140 2008 [91] R.Y. Korotkov et al
InOx RF Atomflo™ 110 W Sublimed (185 °C) solid Indium (III) acetylacetonate In(acac)3 in Not given 2008 [92] R.A. Sailer et al
C-polymer Pulse 1:10 DBD 1 ms 10 kV Acetylene (C2H2) b40,000? 1996 [93] J. Salge
F–C polymer 40 kHz DBD 3–18 kV Argon + CF4, C2F6, C2H2F4, C3F8, C3HF7, c-C4F8 “Low” for F/C b 3 2005 [94] I.P. Vinogradov et al.
Teflon-like Surface DBD ≤1 W/cm2 ≈ 95% N2 + 5% C4F8 Not given 2006 [95] P. Kloc et al.
Poly-pyrrole 2 kHz DBD N 0.1 W/cm2 Pyrrole C4H5N monomer in He 30–100 2007 [96] P. Heyse et al.
C n-tubes μW 2.4 GHz 300 W He/H2/CH4&He/H2/CF4(600 °C) 400 2004 [97] A. Matsushita et al.
a-C:H 1 kHz pulse DBD 18 kV 95% H2 + 5% C2H2 ≤1830 2007 [98] S.P. Bugaev et al.
Diamond H-HEAD ≤300 W + pulsed DC Air + C2H2OH (≤500 °C) ≈3 2007 [83] L. Bardos et al.
Si n-cones RF jet 700 nm Unspecified Ar jet + CH4 etching of Fe/Si 30–400 2007 [99] Z. Yang et al.

respect to film properties. Among examples shown in Table 1, carbon
nanotubes are of particular interest because of their applications in
catalysts, filters, functional coatings, microelectronics, etc. In addition to
atmospheric microwave plasma PECVD results [97] in Table 1, where
SiO2 substrates were patterned with a Ni catalyst and held at 600 °C,
there have also been successful attempts to grow C nanotubes on anodic
alumina substrates held at temperature ≤200 °C by a simple DC corona
discharge (pin-to-plate) in a closed reactor using 10% CH4 in H2 [100].
An array of RF plasma jets in He with C2H2 admixed at the outlet end of
the nozzles have been used recently to achieve high-rate nanotube
growth (89 μm/min at a power of 40 W) on oxidized p-type silicon
wafers pre-heated to 780 °C, with 10-nm-thick sputtered Fe films acting
as catalysts [101].
Superconductive films were deposited by atmospheric plasma as
early as 20 years ago [102,103]. For example, Bi2Sr2Ca2Cu3Ox layers with
a critical temperature of 100 K were grown on heated MgO substrates
(730 °C) at rates of 10–20 nm/min from aqueous aerosol solutions of
the nitrates of Bi, Sr, Ca, and Cu in O2 carrier gas. The films were
deposited in the decaying part of the 5 kW RF plasma torch, where the
additional heating of the substrate by the plasma was estimated to be
not more than 150 °C.
4.3. Post-treatments of films and particles by atmospheric plasma
Post-treatments of as-deposited solid films, enhancement of the
thermal stability of polymer matrices, and plasma treatments of solid
particles represent newer applications of atmospheric plasma processing.
For example, an atmospheric Ar microplasma jet generated by an RF
(13.56 MHz, 35 W) hollow needle electrode (700 μm inner diameter) was
used to crystallize up to 3-μm-thick a-Si films on Al-coated glass in several
milliseconds due to rapid local surface heating to temperatures
1000–1200 °C in less than 1 ms [104]. A DBD air plasma treatment of
indium–tin–oxide (ITO) surfaces has been shown to remove carbon
contamination and increase the work function of ITO as an alternative to
the conventional oxygen vacuum plasma process [105]. Similar results
have been obtained using the FHC system [24]. This kind of treatment
seems to require somewhat higher plasma temperature; therefore, the
decaying parts of the thermal plasma can be more efficient than the cold
plasma. However, a recent comparison of microporous polyvinyl chloride
(PVC) composites after surface treatments by CO2 laser (thermal effect)
and helium DBD plasma revealed [106] that the cold He plasma has better
ability to penetrate into the PVC microstructure and affect a larger
material thickness. Moreover, the plasma causes no significant modifica-
tions in the microstructure, such as redistribution of Cl atoms under the
surface, formation of cracks, etc. and clearly has less destructive effects on
composite surfaces than the laser. It is therefore always important to
optimize plasma parameters, i.e. selection of the plasma gas, power and
power mode (pulsed, continuous, frequency, duty cycle), etc. with respect
to the substrate and the desired application.
5. Novel and emerging applications of the cold atmospheric plasma
Cold atmospheric plasmas have many new and promising applica-
tions other than surface treatment and film growth. For example, DBD
plasmas can induce chemiluminescence and serve as a small gas
chromatographic detector sensitive to a broad range of volatile organic
compounds [107]. Examples of other emerging applications of cold
atmospheric plasma are in environmental processes, such as conversion
of exhaust gas and plasma catalysis, applications in health care and
therapy (also called “plasma medicine”), chemical treatments of liquids
and processes with, at, and under water, etc. [13,108].
6. Conclusions
Non-equilibrium (cold) atmospheric pressure plasma systems pro-
duce higher plasma densities (1011–1016 cm− 3) than typical densities in
low-pressure plasmas (109–1013 cm− 3), but this still represents not more
than 0.1% of the total density of neutral particles (≈ 2.7×1019 cm− 3)
available at atmospheric pressure. Due to high collision frequencies, the
ion energy in atmospheric plasmas is too low for sputter-based physical
vapor deposition (PVD) of films or other ion-beam treatments similar to
those in low-pressure plasmas. Therefore, the cold atmospheric plasma
serves rather as a radical-chemistry based system capable of performing
fast surface activation treatments or PECVD film growth. Without
substrate heating, the growing films are mostly amorphous. Because of
a high concentration of reactive oxygen in the plasma, the films deposited
outside hermetic reactors are mostly oxides.
Cold atmospheric plasmas have many new interesting applications
such as the generation of nano-sized (≈ 100 nm) plasma jets for etching
ultrafine trenches [109], or forming special composites of micro-plasmas
and metal wires showing extraordinary properties for electromagnetic
waves, including a negative-refractive index (metamaterial effects),
which are not available in nature [110]. Because of the relatively short
extension of atmospheric plasmas, large-area surface processing applica-
tions require multiple plasma sources (e.g. plasma arrays) with
considerable gas consumption. However, these systems can be scaled-
up without limitations, contrary to low-pressure systems limited by the
size of vacuum chambers. At the moment, however, cold atmospheric
plasmas cannot replace low-pressure plasmas, especially when hard,
dense, crystalline films with controlled texture are required. Thus, the cold
atmospheric plasma offers a complimentary option to well-established
low-pressure plasma systems.
 L. Bárdos, H. Baránková / Thin Solid Films 518 (2010) 6705–6713
Acknowledgements
Financial supports by the Foundation for Strategic Environmental
Research (MISTRA) and by the J. Gust. Richert Foundation are gratefully
acknowledged. The authors are thankful to Professor Joe Greene for his
stimulating comments.
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