intense and energetic atmospheric pressure plasma jet arrays
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Intense and Energetic Atmospheric PressurePlasma Jet Arraysa
Jae Young Kim, John Ballato, Sung-O Kim*
Intense and energetic atmospheric plasma emissions were achieved by direct jet-to-jetcoupling using honeycomb-structured quartz tube arrays. Two plasma modes were foundto exist in the same plasma array structure under a change of gas flow conditions: an intenseplasma mode and the well-collimated plasma mode. In order to describe the direct jet-to-jetcoupling by electrical coupling of charged particles in the plasma, the optical emission of theplasma array was compared with that of a singletube plasma jet. Under identical electrical drivingand gas conditions, the optical intensity from theintense plasma jet was approximately four timeslarger in the coupled array than in the singleplasma jet structure. Additionally, the electronenergy in the intense plasma was larger thanthat of the well-collimated plasma jets in thesame device. This intense and energetic plasmajet, arising through direct jet-to-jet coupling, mayprovide novel applications requiring strong dis-charge processes using simplified structures andaccompanying instrumentation when comparedwith the present vacuum plasma systems.
1. Introduction
The use of an atmospheric pressure plasma jet (APPJ) device,
consisting of a tube with carrier gases and electrodes, is
Dr. J. Y. Kim, Prof. S.-O KimHolcombe Department of Electrical and Computer Engineering,Center for Optical Materials Science and EngineeringTechnologies (COMSET), Clemson University, Clemson,South Carolina 29634, USAE-mail: [email protected]. J. BallatoSchool of Material Science and Engineering, Center for OpticalMaterials Science and Engineering Technologies (COMSET),Clemson University, Clemson, South Carolina 29634, USA
a Supporting Information for this article is available from the WileyOnline Library or from the author.
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perhaps one of the most useful devices for creating non-
thermal atmospheric pressure plasmas.[1–10] These APPJs,
however, are based upon weakly ionized discharge and
their emitting intensities are relatively low in comparison
to low pressure plasmas created using vacuum chambers.
Because such deficiencies can limit the diversity of
applications of these plasma jets, plasma jet focusing has
been undertaken to increase the discharge rate of plasmas
at one atmosphere pressure.[11] Plasmas are gaseous
collections of ionized charged particles that include
electrons, ions, and short-lived free radicals.[12–17] If the
plasma jet from each single plasma jet device is proximate
to each other through an arrayed structure, the collections
of charged particles interact with each other at certain
discharge conditions, thus affecting the discharge beha-
viors in a collective manner. As such, these plasma jets
discharging adjacent to each other ultimately bundle
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Figure 1. Two different plasma plumes from the plasma array device. (A) The concen-trated plasma plume and (B) seven well-collimated plasma plumes between the plasmaarray device and the glass side of the ITO electrode with change in gas velocity.
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J. Y. Kim, J. Ballato, S.-O Kim
together to form a strongly coupled
Coulomb system. Attempts have been
undertaken to develop one- or two-
dimensional array structures to generate
atmospheric plasmas via the extension of
the plasma size for the uniform treat-
ment of a large area.[18–23] There is as yet,
however, little research on the plasma
jet-to-jet coupling to improve plasma
emitting intensity in the plasma jet
arrays at atmospheric pressure.
The emphasis of the effort described
herein was the development of the
intense plasma emission induced by
jet-to-jet coupling in the plasma jet array
device at atmospheric pressure. In order
to investigate the concentration phe-
nomena of the plasma plumes by jet-
to-jet coupled behavior, the optical emis-
sions of the plasma jet array were
observed using the photo sensor amplifier and the fiber
optic spectrometer. The electron energies in the intense and
normal plasma jets were characterized and discussed using
optical emission spectroscopy (OES). Utilizing an intense
plasma jet based on helium gas, plasma etching of glass was
successfully achieved indicating the energetic nature of
these coupled plasma arrays. Lastly, the plasma array with a
large-sized honeycomb structure was investigated to
extend further the conceptual idea of the coupled jet
intense plasma arrays.
2. Experimental Section
Figure 1 shows the plasma jet array device comprising seven quartz
glass (silica) tubes. The shape of the plasma jet array device is a
honeycomb structure with a single tube in the center of the array
with the remaining six tubes surrounding the centered tube. Each
quartz tube, within this array, has an inner diameter length of
1 mm and an outer diameter length of 2 mm, with the center-to-
center distance between the two adjacent quartz tubes at 2.4 mm.
For the powered electrode within each quartz tube copper tape
6 mm in width was used and placed 10 mm apart from the end of
the tube. The seven tubes were combined through the powered
electrode with the copper tape. An indium tin oxide (ITO)-coated
glass plate of 0.8 mm thickness was placed 10 mm from the ends of
the quartz glass tube array and served as the ground electrode. The
glass side faced the plasma jets. During the discharge process, a
plasma plume was observed between the powered and ground
electrodes, and a high purity helium gas (99.999%) was used as the
discharge gas. In order to observe the input electric energy, the
voltage and current waveforms emanating from the powered
electrode were measured using a high voltage probe (Tektronix
P6015A) and a current monitor (Pearson 4100). An inverter circuit
was used to amplify a low primary voltage to a high secondary
voltage. The driving circuit generated a sinusoidal voltage of
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several tens kilovolts with a frequency of several tens of kilohertz,
and the photo sensor amplifier (Hamamatsu C6386-01) was used to
observe plasma emissions. The wavelength-unresolved optical
emission waveform from the photo sensor amplifier encompassing
the wavelength ranges of 400–1 100 nm was then plotted on the
oscilloscope (Tektronix TDS3014C). In the front of the photo sensor
amplifier, an optical slit of 1 mm in width was used to obviate
external environmental light. A fiber optic spectrometer (Ocean
Optics, USB-4000UV–VIS) was employed to identify the miscellany
of reactive species and to estimate the electron energy in the
plasma plume.
3. Results and Discussion
3.1. Plasma Emission Modes From Honeycomb
Structured Glass Tubes
When the sinusoidal voltage waveform with the peak
voltage of 10 kV and the frequency of 32 kHz (the
corresponding input power of 28 W) was applied to the
powered electrode, the plasma plume between the plasma
jet array device and the glass side of the ITO glass exhibited a
different appearance, due to the change in linear gas
velocity. First, at the linear velocity of He gas of up to
4.6 m � s�1, the corresponding gas flow rate of 1.5 slm
(standard liter per minute), the plasma plume from the
plasma jet array did not reach the ITO glass. At the range of
the He gas velocity from 4.6 to 10.6 m � s�1, and a
corresponding gas flow rate of 1.5–3.5 slm, the plasma
plume was highly concentrated at the center quartz glass
tube. A concentrated plasma plume with a stronger plasma
emission was observed under these conditions. An increase
in the linear velocity of He gas to 10.6 m � s�1 or over, and
an increase in the corresponding gas flow rate above
DOI: 10.1002/ppap.201100190
Intense and Energetic Atmospheric Pressure Plasma Jet Arrays
3.5 slm transformed the plasma into seven well-collimated
plumes (see Supporting Videos 1 and 2). Though the gas
flow became turbulent at extremely large flow rates of He
gas, 15 slm and over, thusly causing unstable discharges,
the plasma plumes are still well aligned and parallel to each
other. Figure 1A and B also show the photographs of two
different plasma jet modes as a change in gas velocities.
Figure 1A shows the intense plasma jet at the gas velocity of
9.1 m � s�1 (the corresponding gas flow rate of 3.0 slm). The
outer quartz glass tubes surrounding the centered quartz
tube, however, did not produce strong individual plumes
but instead reinforced the centered plasma plume, despite
the presence of an equally distributed gas flow. These
results were confirmed through direct observation of a
much more incandescent plasma jet at the center tube of
the array than a well-collimated atmospheric plasma jets.
The six outer plasma plumes were weakened in this
arrangement, however, indicating that an intense plasma
jet is driven by direct jet-to-jet coupling in the air.
Conversely, Figure 1B shows the well-collimated seven
plasma jets at a gas velocity of 15.2 m � s�1 (the gas flow rate
of 5.0 slm). The plasma plumes from seven tubes were well
aligned and parallel to each other under this condition.
The experimental conditions necessary for a successful
plasma jet-to-jet coupling for an intense plasma were
empirically determined; each single plasma jet from the
plasma array must be close enough to each other for easy
interaction; the plasma device must have a single electrode
configuration and a ground electrode several centimeters
apart from the array is needed; and the plasma array must
have an appropriate gas flow rate of around 1–3.5 slm.
When the gas flow rate was higher than 3.5 slm in this
experimental set-up, the plasma jets no longer interacted
with each other, but rather transformed into well-
collimated plasma plumes regardless of operating voltage.
The plasma jet-to-jet coupling behavior is caused by not
optical coupling nor chemical coupling, but electrical
coupling of charged particles. The plasma jet-to-jet coupling
behavior is certainly caused by a use of common ground
electrode. When the seven individual plasma jets propel
toward one common ground electrode, the produced
charged particles from the individual plasma jets would
be merged to each other and concentrated along a certain
discharge path between the powered and ground electrodes
where the discharge can be produced easily at certain
experimental condition. In order to investigate the
concentration phenomena of the plasma plumes by the
direct jet-to-jet coupling among the adjacent plasma
plumes, the plasma emission properties of the plasma jet
array device and the single tubing plasma jet device were
examined and compared as a function of linear gas velocity.
When comparing the characteristics of the plasma plume,
the single quartz glass tube plasma jet device was identical
to one element of the plasma jet array. When the applied
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input power was fixed to 28 W, the plasma emissions from
both plasma devices were monitored as an increase of the
linear gas velocity. Under the same power conditions, the
applied sinusoidal voltage waveforms were the peak
value of 10 and 11 kV for the plasma jet array and the
single tubing plasma devices, due respectively to the
impedence difference of two plasma devices. The photo
sensor amplifier with 1 mm-wide optical slit was aligned
with the positions of the centered plasma plume from the
plasma array and the plasma plume of the single tubing
plasma device, respectively. As a result, the optical intensity
of the plasma emission in both plasma devices exhibited
different tendencies with an increase of gas velocity as
shown in Figure 2. Since no jet-to-jet coupling was observed
in the single tubing plasma jet, the optical intensity
increased with a corresponding increase in the linear gas
velocity. The optical intensity of the centered plasma plume
from the plasma jet array abruptly decreased between the
gas velocity of 9.1 and 12.1 m � s�1, however, with a change
of the plasma jet mode in the plasma jet array.
Figure 2 shows the optical intensity of a plasma emission
of a single plasma jet and the array device at linear gas
velocities between 6.1 and 15.2 m � s�1. Regarding the single
tubing plasma jet device, the corresponding gas flow rates
varied from 285 to 715 sccm (standard cubic centimeters
per minute; 1 000 sccm¼ 1 slm), whereas the gas flow rates
of 2.0 to 5.0 slm corresponded with the gas velocities of the
plasma jet array device. The optical intensity of plasma
emission in rising slope of the voltage waveform is shown
to be higher than that in the falling slope in both single
tubing plasma and plasma array in Figure 2. This difference
of the optical intensities is caused by the different shapes
between the powered and ground electrodes. Our proposed
plasma system which consists of the plasma array with a
single electrode configuration and an outside ground
electrode can be classified as a point-to-plane discharge
configuration. The difference of the optical intensities
between rising and falling slopes of the voltage waveform is
a stereotypical discharge property of point-to-plane barrier
discharges driven by ac voltages. The streamer-like
discharge mode in the positive half-period and the
diffuse-like discharge mode in the negative half-per-
iod.[24,25] Therefore, when the powered electrode plays a
role of an anode and the ITO ground electrode play a role of a
cathode, stronger plasmas are generated than vice-versa.
While the optical intensity increased by 85% with an
increase in the gas velocity from 6.1 to 15.2 m � s�1 for the
plasma plume discharged from a single tube, the optical
intensity of the centered plasma plume decreased by 40%
for the plasma plume discharged from the plasma jet array.
At a gas velocity of 9.1 m � s�1, the optical intensity of the
centered plasma plume from the plasma jet array was four
times larger than the plasma plume from the single tube,
despite identical power and gas conditions. Here, the seven
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Figure 2. Optical intensity of plasma plumes from the single tube plasma jet and the intense plasma jet array devices at various gasvelocities from 6.1 to 15.2m/s.
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J. Y. Kim, J. Ballato, S.-O Kim
plasma jets from the plasma jet array begin to interact with
each other under this precise condition to reinforce the
centered plasma plume by this coupling effect among the
seven plasma jets when the six outer plasma plumes were
weakened. The three pairs of outer quartz glass tubes facing
each other that surround the centered quartz tube plus the
center tube comprising the four jet-to-jet couplings yield an
optical intensity four times greater than in previous
experimentation. Interestingly, at the gas velocity of
15.2 m � s�1 in the well-collimated plasma mode, the optical
intensity of the centered plasma plume from the plasma
array is also 1.4 times greater than the plasma plume from
the single tube, despite identical power and gas conditions.
Though this increase does not occur in the jet-to-jet
coupling phenomenon in the well-collimated mode within
the seven plasma plumes, there is electrical coulping of
charged particles between closed adjacent plasma plumes,
thusly enhancing slightly the plasma emission. There are
increases in the amplitudes of the produced plasma
emission at not only the rising slope but also the falling
slope of the input voltage in the intense plasma mode as
shown in Figure 2. Since the operating voltage condition
(Vp ¼ 10 kV and Freq.¼ 32 kHz) is not changed with the
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plasma mode transition, this higher emission in the intense
plasma mode is indicative of both a greater maximum
intensity, and an improved average discharge rate than the
well-collimated plasma mode.
3.2. Optical and Plasma Emitting Behaviors of Intense
Plasma Jet at Atmospheric Pressure
OES is a non-invasive method for investigating atoms, ions,
and molecules in a plasma media.[26–28] Its diagnostic use
for emitting media has yielded a greater understanding of
very complex phenomena such as high gas pressure
plasmas.[29] In order to verify the reactive species generated
by the intense helium APPJ in the ambient air, the emission
spectra of two different plasma jet modes were monitored
and compared using the fiber optic spectrometer in which
the distance between the end of the device and the
spectrometer was fixed at 10 mm. Figure 3A and B show the
emission spectra from 300 to 800 nm of two different
plasma modes, further indicating that the excited N2, Nþ2 ,
He, H, and O exist in the plasma plumes. As is observed in
these figures, the optical emission spectra of the intense
plasma jet mode exhibited strong intensity levels of
DOI: 10.1002/ppap.201100190
Figure 3. Comparison of optical emission spectra of two different plasma plumes: The optical emission spectra of plasma plumes between(A) the intense plasma mode and (B) the well-collimated plasma mode under identical input driving conditions; (C) and (D) Magnifiedemission spectra of second positive systems of nitrogen.
Intense and Energetic Atmospheric Pressure Plasma Jet Arrays
nitrogen and oxygen species that are highly reactive
radicals compared to the spectra of the well-collimated
plasma jet. Note also that the emission spectra of the
intense plasma jet only exhibits the oxygen atomic lines at
533 nm and 615 nm, and the hydrogen atomic line at
656 nm, which is likely due to humidity from the air. These
results imply that the higher emission of the intense
plasma jet is indicative of not only stronger atomic
intensity levels, but also an improved discharge rate. The
emission spectra observations are well matched with the
results of the optical emission intensity.
In order to determine if the proposed intense plasma
exhibited higher electron energy than the well-collimated
plasma, the properties of electron energy of two different
plasma modes were characterized and compared by peaks
of both first negative and second positive systems of
nitrogen using OES. Figure 3C and D show the magnified
emission spectra of the second positive systems and the
first negative system of nitrogen. Note that the nitrogen
molecule is transferrable from the ground state N2(X1Pþg )
into an excited state N2(C3Pu) by the impact of electrons
with an energy >11.0 eV. Subsequently, the excited
N2(C3Pu) molecules transferred into the N2(B3Pg) state
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by emitting a proton of 337.1 nm in wavelength. If electrons
exhibit energy >18.7 eV, nitrogen ions Nþ2 (B2Pþ
u ) will be
produced that release photons of 391.4 nm in wavelength
via transfer into the Nþ2 (X2Pþ
g ) state. Based on these
different emitting procedures of nitrogen, the relative
changes in the concentration of active species N2(C3Pu) and
Nþ2 (B2Pþ
u ) in two different plasma modes can be monitored
by measuring the emission intensities at 391.4 nm and
337.1 nm.[30–32] The normalized emission intensity at
391.1 nm (an emission intensity at 391.4 nm divided by
an emission intensity at 337.1 nm) of the intense plasma
mode is revealed to be 1.5 times greater than that of the
well-collimated plasma mode (i.e., the normalized emission
intensities at 391.1 nm indicate that the electron energy of
the intense plasma mode is relatively greater than that of
the well-collimated plasma mode).
3.3. Temperature Variation on the Surface of ITO
Glass by Plasma Jet Emissions From a Seven Tube
Honeycomb Array and a Single Tube
Figure 4 shows the temperature variation of the surface of
ITO glass as a function of time when the plasma plume
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Figure 4. Temperature variation of the ITO glass as a function oftime when the plume from single tube plasma jet and plasma jetarray devices reaches the glass side of the ITO glass.
258
J. Y. Kim, J. Ballato, S.-O Kim
makes contact with the glass side of the ITO glass electrode.
The applied input power was also fixed to 28 W with
frequency of 32 kHz.
The ITO glass temperatures were measured using the
infrared thermometer (Extech IR Thermometer 42545) with
the measuring point being the center of the plasma plume
on the glass surface of the ITO glass. The initial ITO glass
temperature is 25 8C. Regarding the plasma jet emissions
from the single tube, the ITO glass temperatures became
saturated at 150 s. When the gas velocities through the
single tube were 9.1 and 15.2 m � s�1, the saturated
temperatures of the ITO glass via plasma jet from the
single tube were 37 and 32 8C, respectively. This tempera-
ture difference likely is due to neutral He gas flows. An
acceleration of the gas velocity also resulted in a rapid
increase of neutral He gas flow that quickly cooled the
surface of the ITO glass. Regarding the plasma jet array
device, the ITO glass temperature becomes saturated at
approximately 150 s at a gas velocity of 15.2 m � s�1, and at
240 s at a gas velocity of 9.1 m � s�1, respectively. Gas
velocities through the plasma jet array device at 9.1 m � s�1
and 15.2 m � s�1 yield saturated temperatures of 81 and
67 8C, respectively. Though the input power and the
distance between the powered and ground electrodes are
identical, the saturated temperature on the ITO glass caused
by plasma jet arrays is more two times greater than that
with a single plasma jet, regardless of the plasma jet modes.
3.4. Glass Etching by Intense Helium Atmospheric
Pressure Plasma
It can be concluded from these experimental results that an
intense and energetic plasma process occurs in the
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concentrated plasma jet; i.e., this jet-to-jet coupling
behavior exhibits greater electron energy than either the
single plasma jet or the seven well-collimated plasma jets.
The observation of plasma etching on the glass confirms
that the proposed plasma jet is an energetic plasma. Despite
the use of the helium gas at atmospheric pressure, the
etching by the concentrated plasma jet strongly and quickly
occurs on the glass as shown in Figure 5. When the
concentrated plasma plume begins to etch a glass, the
plasma plume is no longer reflected upon the glass surface,
but instead penetrates the spot as shown in Figure 5A. No
etching occurs, despite an increase in input powers and
treated times of the single plasma jet and the well-
collimated plasma mode. Figure 5B shows the resultant
etched spots on the glass surface of ITO-coated glass from
the concentrated plasma plume, in which a total of 30 (6 by
5) etched spots on the glass with an area of 10 cm� 10 cm
were created. Figure 5C and D show SEM images of one
etched spot from the intense and energetic plasma jet on
the glass. As shown in the SEM images, many-ion
bombardments on the glass are observed in a single etched
spot, which caused a physical etching of the glass during the
plasma processes. As shown in Figure 5C, the non-
uniformity of the etching process was observed inside
the spot. The intense plasma jet driven by sinusoidal
voltage with several kilohertz temporally consists of a large
number of micro-discharges with a short duration (in
microseconds), which are spatially randomly distributed
between powered and ground electrodes. The micro-
discharges are produced along a certain discharge path
where the discharge can be produced easily, resulting in
filamentary discharge, which is represented as ‘‘plasma
concentration’’. Since the filamentary discharge character-
istics show not only non-uniformity but also spatial
randomness, the non-uniformity of the etching process
can be observed inside the etched spot. This physical
etching in turn reveals substantial evidence of the energetic
plasma process involving the charged particle transport in
the concentrated plasma jet channel by direct jet-to-jet
coupling.
3.5. Plasma Jet Emissions From Honeycomb
Structured Nineteen Tube Arrays
In order to extend the conceptual idea of the intense plasma
jet with direct jet-to-jet coupling, the honeycomb struc-
tured and triplely-coupled nineteen tube array was
developed as is shown in Figure 6A. The 19-array is
constructed such that the central tube protrudes 1 mm from
other tubes for an easier ignition of the plasma. The
discharge gas was high purity helium, flowing at a rate of
4.0 slm. The intense plasma plume generated from this
configuration is illustrated in Figure 6B. Note the direct jet-
to-jet coupling behavior. Despite an equally distributed gas
DOI: 10.1002/ppap.201100190
Figure 5. Plasma etching from the intense plasma jet generated from the plasma array device: (A) A photograph of concentrated plasmaplume focused on the etched spot; the plasma starts to etch the glass within 10 s, (B) etched spots from a concentrated plasma jet on theglass side: (C) and (D) SEM images of one etched spot by a concentrated He plasma jet on the glass.
Intense and Energetic Atmospheric Pressure Plasma Jet Arrays
flow, the outermost tubes do not produce strong individual
plumes. Rather, the plasma flow from these tubes is drawn
into the central plume, which is in turn amplified. Using a
photo sensor amplifier, the plasma emission properties
among 19- and 7-array plasma jet devices and the single
tubing plasma jet device were quantified and compared.
While the input power of the applied sinusoidal voltage
waveform was fixed to 28 W at 30 kHz, the gas flow rates of
19- and 7-arrays and a single jet were varied to 4.0, 2.5, and
1.0 slm, respectively, which are the experimentally opti-
mized flow conditions for the maximum optical intensity
of each plume under the same input power. As seen in
Figure 6C under these experimental conditions, the optical
intensity of plasma plumes created by jet arrays increases
with the number of tubes in the array. The 19-array yields a
much greater optical intensity compared to either the 7-
array or single tube. Compared to a solitary tube, a seven-jet
array possesses approximately triple the optical intensity,
while the 19-array possessed almost five times the optical
intensity. The discharge delays of coupling effect, observed
among the three devices, indicates that the coupling effect
requires time for mutual interaction as shown in Figure 6C.
That is to say the coupling effect can be controlled by
changing parameters and structural design according to
their purpose and applications.
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4. Conclusion
Described in this work was the initial development of an
intense and energetic plasma jet mode from a honeycomb
structural APPJ array. The discharge modes between the
intense plasma and well-collimated plasma jets were
observed to transform to a linear gas velocity. At
identical conditions of input power and linear velocity
of the helium gas condition, the optical intensity from
the centered plasma jet of the plasma jet array with
seven tubes was four times greater than a single plasma
jet. Compared to the well-collimated jet spectra, the
emission spectra of the intense plasma jet also
exhibited both strong intensity levels of nitrogen and
oxygen species and more reactive oxygen and hydrogen
species. In addition, the normalized emission intensities at
391.1 nm indicate that the electron energy of the intense
plasma jet was greater than that of the well-collimated
plasma jet. The triple coupled 19-array exhibited a
fivefold greater optical intensity compared to the single
tube and double larger than the 7-array. The intense and
energetic plasma jet by the direct jet-to-jet coupling is
useful for determining the accuracy of applications
requiring the high energetic plasmas, using only a very
elemental apparatus.
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Figure 6. 19-array APPJ array device: (A) 19-array APPJ array struc-ture and (B) intense plasma plume from this plasma jet arraydevice: (C) Comparison of optical intensity of plasma plumesamong 19- and 7-APPJ arrays and a single jet at maximum plasmaemission conditions.
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J. Y. Kim, J. Ballato, S.-O Kim
Acknowledgements: The authors wish to acknowledge thefinancial assistance of the Center for Optical Materials Scienceand Engineering Technologies (COMSET) at Clemson Universityand the editorial assistance of Mr. Godfrey Kimball, also atClemson University.
Received: October 20, 2011; Revised: December 19, 2011;Accepted: January 6, 2012; DOI: 10.1002/ppap.201100190
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Keywords: atmospheric pressure plasma jet; concentrated plasmaplume; jet-to-jet coupling; plasma array
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DOI: 10.1002/ppap.201100190