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INSTITUTE OF PHYSICS PUBLISHING JOURNAL OF PHYSICS D: APPLIED PHYSICS
J. Phys. D: Appl. Phys. 38 (2005) 555–567 doi:10.1088/0022-3727/38/4/007

The physics and phenomenology of One


Atmosphere Uniform Glow Discharge
Plasma (OAUGDP™) reactors for surface
treatment applications
J Reece Roth1 , Jozef Rahel2 , Xin Dai1 and Daniel M Sherman3
1
University of Tennessee, Knoxville, TN, USA
2
University of Tennessee, and Atmospheric Glow Technologies, Inc., Knoxville, TN, USA
3
Atmospheric Glow Technologies, Inc., Knoxville, TN, USA
E-mail: jrr@utk.edu

Received 15 July 2004, in final form 8 November 2004


Published 3 February 2005
Online at stacks.iop.org/JPhysD/38/555

Abstract
In this paper, we present data on the physics and phenomenology of plasma
reactors based on the One Atmosphere Uniform Glow Discharge Plasma
(OAUGDP™) that are useful in optimizing the conditions for plasma
formation, uniformity and surface treatment applications. It is shown that
the real (as opposed to reactive) power delivered to a reactor is divided
between dielectric heating of the insulating material and power delivered to
the plasma available for ionization and active species production.
A relationship is given for the dielectric heating power input as a function
of the frequency and voltage at which the OAUGDP™ discharge is
operated.
(Some figures in this article are in colour only in the electronic version)

1. Introduction in figure 1, and the One Atmosphere Uniform Glow Discharge


Plasma (OAUGDP™), from F to H in figure 1 [1, section
Many plasma processing applications operate at pressures 12.5.2, 5, 6].
below 10 Torr, where various forms of electrical discharge Compared with other forms of atmospheric pressure
can be easily generated [1], [2, chapter 21]. Because plasma, the uniformity and low-to-moderate areal power
low pressures require expensive vacuum systems and batch density of the glow discharge highly recommend it for
processing of workpieces, interest has grown over the past applications in which it is important to have uniformity of effect
few years in applying atmospheric pressure plasmas to plasma and avoid damaging or heating the surface of the workpiece.
processing. The regimes of the classical dc electrical discharge A recent Internet search identified approximately 122 sites
indicated in the current–voltage diagram of figure 1 provide containing a reference to ‘atmospheric glow discharge’, a topic
a framework within which to discuss plasmas used for that scarcely existed 15 years ago.
processing applications [1]. These plasmas include corona Identification of the OAUGDP™ as a normal glow
discharges, from D to E in figure 1 [2, section 15.2]; discharge through experimental observation and computer
dielectric barrier discharges (DBDs), including filamentary modelling [7–11] is particularly important because it brings
discharges and ozonizers, from C to E in figure 1 [3], into play nearly 200 years of accumulated observations and
[2, section 15.3]; and arcjets, from H to K in figure 1 understanding from electrical discharge research [1, chapter 9].
[2, section 15.5]. More recent developments include the An important example is the knowledge that the OAUGDP™,
atmospheric plasma jet (APJ), from F to K in figure 1 [4], like all normal glow discharges, operates at the Stoletow point.
the atmospheric pressure glow (APG) discharge from D to G This provides assurance that the generation of ion–electron

0022-3727/05/040555+13$30.00 © 2005 IOP Publishing Ltd Printed in the UK 555


J R Roth et al

the transition from the Townsend discharge to the normal glow


(sub-normal glow), where the distortion of the electric field is
present but not great enough to form the cathode layer of a
normal glow discharge.
A comparative study of helium and nitrogen emission
spectra during the afterglow of an atmospheric pressure DBD
and an APG discharge made by Massines et al confirmed the
original statement of Okazaki et al about the important role
of metastables He(23 S1 ) and N2 (A 3 u+ ) in such discharges.
Later numerical simulations [20] suggest that helium atoms
stabilize the APG by the two-step process of Penning
ionization. Fast electrons are effectively removed by exciting
the He (23 S1 ) = 19.8 eV and He (21 S1 ) = 20.6 eV metastable
states. This slows down the ionization process of avalanching
and increases its radial diffusion, making it more difficult to
Figure 1. Regimes of the classical dc electrical discharge. satisfy the streamer formation criterion.
The role of N2 metastables inside the APG is different,
pairs at 1 atm in the OAUGDP™ cannot be done more although initially a model similar to that of the helium APG
efficiently. was introduced [22]. Since the discharge is in the Townsend
Characteristic power fluxes on the electrode surface of discharge regime, the electrons near the anode are more
parallel-plate OAUGDP™ reactors are a few tens of milliwatts energetic and have a higher concentration. This in turn causes
to a few watts per square centimetre, not high enough the maximum density of N2 (A 3 u+ ) metastables to be located
to damage or degrade most materials exposed for surface close to the anode. The flux of metastables is claimed to
treatment, particularly moving webs. Also very important to significantly improve the secondary electron emission, thus
industrial applications is the circumstance that glow discharges helping to initiate the Townsend discharge after the polarity
are energy efficient in maintaining themselves in an ionized of the electrodes is reversed by the next half cycle of the
state. Unobstructed normal glow discharges in the regime from RF. Golubovskii et al [23] showed using a two-dimensional
F to G in figure 1 operate at the Stoletow point [1, p 246], at numerical simulation of a homogeneous N2 discharge that the
which only 81 eV is required to produce an ion–electron pair Townsend discharge is stable to radial perturbations, unlike
in air. In contrast, arcjets and plasma torches typically require the normal glow discharge regime in N2 . The normal glow
an energy input of more than 10 000 eV per ion–electron pair, discharge will inevitably collapse into a streamer ionization
nearly all of which goes into heating the neutral gas instead front, but any time a Townsend discharge is established, the
of producing ionization or active species useful for plasma resulting plasma is expected to be uniform. Due to the rapid
processing. quenching of nitrogen metastables [24] in nitrogen–oxygen
The production of atmospheric glow discharges has a long mixtures, the metastable models described above suggest that
history. In 1933, von Engle et al [12] reported the production it is not possible to generate the uniform glow discharge in air.
of dc and RF normal glow discharges in air and other gases This, as will be shown below, is not the case.
at 1 atm. However, their procedure required initiation of the At the UT Plasma Science Laboratory, a programme to
discharge under vacuum, followed by a gradual increase in produce an atmospheric glow discharge in air was initiated in
pressure to 1 atm. This discharge also required aggressive 1988, and produced a 1.6 litre OAUGDP™ between parallel
cooling of the cathode to suppress the glow-to-arc transition, plates in helium gas in January 1992 [16]. Subsequent
and it found few if any industrial or laboratory applications. development allowed the OAUGDP™ to be generated in a
The later work of Okazaki et al [13–15], Massines et al variety of geometries, including a plane, parallel slab geometry
[8–11] and Roth et al [2, 5, 6, 16–19] between 1988 and 1995 and an aerodynamic plasma actuator in the form of a surface
clearly showed that capacitively coupled, parallel-plate RF layer of plasma on flat panels [2, sections 15.4, 17.1, 25–29].
discharges can, under the proper operating conditions, generate Investigation of physical processes in the OAUGDP™ at UT
a diffuse glow discharge plasma of uniform effect over the identified the ion trapping mechanism and its limitation to
entire gap, and at 1 atm of pressure. The earlier work of a relatively narrow range of audio RF driving frequencies
Okasaki et al [13–15] and Massines et al [8–11] was confined as a requirement for a stable, uniform plasma [1, 5, 6].
to such gases as helium, nitrogen and argon with an admixture Further information on the physics and phenomenology of the
of acetone. The work of the UT group included these gases, OAUGDP™ can be found in [1, sections 15.4, 17.1 and 18.6].
as well as air [5, 6, 17–19].
Fast optical measurements of an APG discharge in He and 2. The charge trapping mechanism
N2 gas revealed a different light distribution in the discharge
gap for the two gases [20, 21]. While the He discharge exhibits The cathode heating responsible for the glow-to-arc instability
the same structure as a glow discharge (positive column, of the von Engle discharge arises from ion bombardment of
Faraday dark space, negative glow, etc), the discharge in the cathode. To avoid this cathode heating, the ion trapping
N2 displays only a luminous layer close to the anode. The mechanism was conceived [5, 6], in which an RF is applied to
presence of luminosity only near the anode instead of the the electrodes at such a frequency that ions, but not electrons,
cathode is characteristic of the Townsend discharge mode, or are trapped between the electrodes [1,2], and a dielectric

556
The One Atmosphere Uniform Glow Discharge Plasma reactor

Figure 2. Normal glow discharge structures in a parallel plate One Figure 3. The Mod VI OAUGDP™ reactor operating in air at 1 atm
Atmosphere Uniform Glow Discharge Plasma™ with of pressure. Recirculating air flows from left to right.
dielectric-coated electrodes.
The qualitative functional dependence of power on
plate is used to further suppress the glow-to-arc transition.
frequency, voltage, gap distance, etc in equations (1) and (2)
This transformation of the von Engle discharge from dc to
has been investigated and found to be generally valid
RF greatly reduces cathode heating, reduces sputtering and
[1, section 12.5.2]. While equations (1) and (2) predict the
erosion of the electrodes, reduces contamination of the plasma,
functional dependence of the critical ion trapping frequency on
stabilizes the plasma against the glow-to-arc transition and
the gap distance d, the rms voltage and the collision frequency,
provides a form of electrodynamic trapping that increases
quantitative predictions based on average electron number
the ion and electron number density available for Lorentzian
densities, electron kinetic temperatures, potentials, electric
collisions, and active species production. In addition to these
fields, etc are not expected to be valid, as a result of the
real or potential advantages, operating at the optimum RF
extreme time and spatial variations that occur during each half
frequency makes it possible to produce a plasma in air and other
gases that is not only visibly uniform and without filamentation cycle of the RF [7–9]. Such quantitative comparisons will
but is also uniform in effect, without the pitting and pin-holing require a detailed comparison with numerical models more
of surfaces characteristic of DBDs. sophisticated than any currently available.
Numerical simulations of the OAUGDP™ by Ben Gadri
[7, 10] and measurements of axial luminous intensity by 3. OAUGDP™ reactor configurations
Massines et al [11], both in helium gas, showed that the
OAUGDP™ has all the classic structures of the dc normal A variety of atmospheric reactor configurations are possible.
glow discharge and that these reverse with each half cycle Here, we give some examples with features that are particularly
of the RF. These structures are indicated schematically in useful for research or industrial surface treatment applications.
figure 2. Later work by Chen addressed the issues of proper
impedance matching of the OAUGDP™ to its power supply The Mod VI parallel plate reactor. A photograph of the Mod VI
[30], and PSPICE simulation of the OAUGDP™ as a circuit OAUGDP™ reactor operating in air at 1 atm is shown in
element [31]. figure 3, and its main features are shown in the schematic
The electric fields employed to create the One Atmosphere of figure 4. This reactor was designed to expose samples
Uniform Glow Discharge Plasma are normally less than to the OAUGDP™ for biological (sterilization) or surface
10 kV cm−1 in air, values too low to achieve dc electrical energy testing in three modes of operation: direct exposure—
breakdown (sparking) of the operating gas. The electrode gap the workpiece is placed on an electrode, and is directly exposed
spacing, electric field and frequency are adjusted so that the to the plasma; single pass remote exposure—the workpiece is
mobility drift of the ions in the oscillating RF electric field located outside the plasma volume on a platform in the exit
traps them between the electrodes during an RF cycle. During manifold, and active species from the plasma are convected
ion trapping, the electrons are free to travel to the electrodes, over its surface only once; and recirculating remote exposure—
where they are collected, recombine or build up a surface the workpiece is located on the platform outside the plasma
charge. volume, and active species from the plasma are convected
In section 12.5.2 of [1], it was shown that the critical over its surface by a gas flow that recirculates through the
frequency, ν0 , above which the uniform glow discharge should OAUGDP™ multiple times.
build up in the plasma volume is given by In our research with this reactor [32, 33], we performed
eUrms paired comparisons of direct exposure and recirculating
ν0 ≈ [Hz]. (1) remote exposure of samples to the OAUGDP™ active
πmνc d 2
species generated by air, and found that direct exposure
The parameters in equation (1) define the operational to the OAUGDP™ is much more effective in increasing
envelope of the uniform discharge regime. It should be the surface energy of materials than single- or multiple-
noted that the product (mνc ) in the denominator is smaller pass remote exposure. We also found, in contrast with
for electrons than for ions. The critical frequency for onset of this trend, that sterilization of surfaces by remote exposure
the uniform discharge (ion trapping) therefore is lower than remains highly effective, nearly as much as direct exposure
the critical frequency for onset of the filamentary discharge to the plasma. In this early work, we also found that
(electron trapping). Thus, for operation in the uniform glow microbial killing/sterilization is more effective for multiple-
discharge regime, the driving frequency should lie between pass recirculating remote exposure than for single-pass remote
limits as follows: exposure [33]. The active species responsible for sterilization
eUrms eUrms appear to build up (or at least become more effective) upon
 ν0  [Hz]. (2)
πmi νci d 2 πme νce d 2 recirculation of the working gas through the plasma.

557
J R Roth et al

The Mod T transparent electrode reactor. The transparent and held in position by a fifth horizontal bolt. Tap water
electrode parallel plate reactor shown in figure 5 (Mod T) was (specific conductivity 100 µS cm−1 ) served simultaneously as
built at Atmospheric Glow Technologies (AGT) to investigate an electrical conductor and cooling medium. The calculated
the uniformity of the OAUGD plasma. Two parallel water resistive path through the 25 mm thick water electrode was
electrodes are separated by two vertically spaced 1 mm thick 150 , which is negligible compared with the resistivity of
Pyrex™ panes in a closed transparent plastic reactor for gas the discharge plasma (tens of kiloohms). The capacitance of
content control. The active dimensions of the electrodes are the Mod T reactor was measured to be Cp = 110–160 pF,
130 × 128 mm2 . As shown in figure 5, the bottom electrode depending on the width of the discharge gap.
was positioned vertically by four threaded stainless steel bolts A block diagram of the Mod T reactor system is shown
in figure 6. Cooling water was forced to circulate through
(a) the electrodes by two independent water pumps that provided
active cooling. To reduce parasitic electrical currents to ground
through the cooling water to negligible levels, a long (several
metres), small diameter (3 mm) tube was inserted between the
high voltage electrodes and the water pumps. The Mod VI
reactor was also outfitted in this way, and had no significant
leakage currents compared with those needed to energize the
reactor.
Both the Mod VI and Mod T reactors were energized
by a sinusoidal signal from a HP 3310A function generator,
amplified by two RF power amplifiers (Industrial Test
Equipment Co., Inc., Model 1599CN; output 300 V, 1.5 kW)
and four high voltage transformers (Industrial Test Equipment,
model VT-35/RM-109; turns ratio 1 : 40, 5 kV rms).
Two high voltage probes (Tektronix P6015A (1000×))
were used to monitor the potential of the two electrodes, and the
actual inter-electrode voltage was calculated as the difference
between their readings. This approach was necessary to
account for a mutual asymmetry of RF amplifiers and/or
transformers. A Pearson current monitor, Model 2100 (1 : 1),
was employed to measure the electrical current flowing to the
(b)
reactor electrodes. The amplitude of the reactive current for
the Mod T reactor is typically 50% larger than the total current
signal, and was nulled out with the circuit shown in figure 6.
For the Mod VI reactor, a current transformer without biasing
was used.
The time dependence of emitted light was studied with a
Hamamatsu H5773-04 photomultiplier module (185–850 nm).
The optical signal was fed into the photomultiplier module
by 2 m of 400 µm diameter optical cable (250–900 nm). The
visual appearance of the plasma was recorded was a Canon
PowerShot A70 digital camera (3.2 Mpx) signals from the
Figure 4. Structure of the Mod VI OAUGDP™ reactor. (a) Plan HV probes, the current transformer and the photomultiplier
view from top. (b) Elevation view from front, with remote exposure were recorded using a Tektronix TDS 3014B (100 MHz,
platform in plenum on left. Note path of recirculating airflow 1.25 GS s−1 (Gigasamples per second)) and processed using
through the reactor. WaveStar™ software on a PC.

Figure 5. Mod T reactor: (A) water electrodes, (B) discharge gap, (C) adjusting bolts for the bottom electrode positioning. Hollow arrows
indicate direction of gas flow; solid arrows correspond to the flow of cooling water.

558
The One Atmosphere Uniform Glow Discharge Plasma reactor

(a)

(b)

Figure 6. Mod T reactor system: (A) water electrodes, (B) cooling


Figure 8. A 6.3 mm diameter copper rod with annular glass sleeve
system individual for each electrode. HV, high voltage probes;
located 1 cm above an insulating ground plane. (a) Plasma off.
PMT, photomultiplier probe; CT, current transformer; BIAS,
(b) Plasma energized at 4.5 kV rms and a frequency of 10 kHz in
parasitic current elimination tool; Cv , variable capacitor; OSC,
helium gas.
oscilloscope; PC, computer; SIGNL, harmonic signal generator; RF
AMP, radio frequency power amplifier; CCD, digital camera.
Figure 8(a) is an image of a rod-and-plane configuration
(a) containing a 6.3 mm diameter copper tube covered with a glass
sleeve spaced at a gap distance of 1 cm above an insulated
ground plane. Figure 8(b) shows this configuration operating at
1 atm in helium gas at an RF voltage of 4.5 kV and a frequency
of 10 kHz. This plasma also exhibits axial uniformity along
the length of the rod, and greater luminosity near the electrode
surface, due to the greater luminosity of the negative glow that
forms when the electrode is the instantaneous cathode.

4. Uniformity of appearance of the OAUGDP™

For such plasma processing applications as increasing the


surface energy, wettability or sterilization of materials,
particularly thin webs, it is important that the plasma be
sufficiently uniform and free of filamentation not to damage
(b)
the surface by pitting or pin-holing. The latter two forms of
damage are a frequent result of the microdischarges that are
the plasma-generating mechanism of the DBD. As a result of
these forms of damage, it is essential in industrial applications
to distinguish between the uniform OAUGDP™ mode of
operation and the DBD. Both forms of discharge utilize the
same geometry (insulators covering one or both electrodes)
and can operate at the same frequencies and electric fields,
although the DBD usually functions at higher electric fields.
It is an important advantage of the OAUGDP™ that it can
be operated in a mode in which pitting and pin-holing do not
occur, even on a scale down to tens of nanometres. In this
section we discuss the visible uniformity of the OAUGDP™,
Figure 7. Two 6.3 mm diameter copper rods with annular glass and in the next section we discuss its uniformity of effect down
sleeves operating in helium at 1 atm at 4.5 kV rms and a frequency
of 10 kHz. Gap distance is 2.5 cm. (a) Plasma off. (b) Plasma on. to the nanoscale by reference to scanning electron micrographs
(SEMs) of surfaces used as witness plates for filamentary
Two rods and rod-and-plane configurations. In addition to the discharge activity.
above, we developed OAUGDP™ configurations based on
two rods and a rod-and-plane geometry that may be useful Uniformity viewed perpendicular to the electric field. The
in treating webs or flat surfaces. Figure 7 is an image of two visual uniformity of a OAUGDP™ operating with helium gas
6.3 mm diameter copper tubes covered with glass sleeves with a in two dimensions is illustrated by the rod configurations of
gap distance of 2.5 cm operating at 1 atm in helium gas at an RF figures 7(b) and 8(b). Its uniformity in a three-dimensional
voltage of 4.5 kV and a frequency of 10 kHz. Notable features volume is illustrated in figure 9, which shows four images
of this plasma are the axial uniformity along the length of the taken of the Mod I OAUGDP™ reactor operating in helium
rods and the greater luminosity near the electrode surfaces, at 1 atm with an insulating coating on both electrodes, and an
due to the negative glow that forms when the electrode is the applied RF voltage of 4.5 kV rms. As the RF frequency was
instantaneous cathode. raised from below 1 kHz, the discharge first appeared as a few

559
J R Roth et al

(a) long-term (approximately 10 s) start-up transients affecting the


plasma uniformity and the nature of the active species (as
determined by their ability to sterilize remote samples).
We have also seen a similar slow initial change in plasma
uniformity on our Mod T transparent electrode parallel plate
reactor when operating in air and nitrogen. Images of this
phenomenon are illustrated in figure 10. The first image of
(b) figure 10 at 0 s shows the reactor volume before the RF voltage
is turned on. In the image 3 s after turn-on, the plasma is
filamentary, particularly near the edges. After a few additional
seconds have elapsed, a uniform region of high luminosity
spreads from the interior to fill the reactor cross section, and
this process is virtually complete after 15 s.
The time required—15 s—is too long for a plasma
instability based on Maxwell’s equations and the equations of
continuity, momentum, etc. It does not appear to be a thermal
(c) time constant associated with heating of the electrode surface
or with a change of chemistry associated with such heating,
as a temperature rise of the electrode surface induced with
a heat gun of up to 20 ˚C—far greater than the temperature
rise associated with plasma contact—had no effect on the
uniformity. Removal of adsorbed monolayers or contaminants
by plasma cleaning also had no relation to this phenomenon, as
was confirmed by paired comparison studies with and without
(d) deliberately introduced surface contamination.
The uniformity of appearance is associated with the shift
of breakdown voltage to lower values, which is believed to be
due to the alteration of existing memory voltage, i.e. the slow
accumulation of surface charge on the dielectric. Moreover,
after turning the plasma off and restarting it a few seconds
later, a uniform plasma appears instantaneously at the same
location it occupied when it was interrupted, proving again the
Figure 9. Appearance of the Mod I parallel plate OAUGDP™ importance of surface conditioning. This effect is observed
reactor operating at 1 atm of helium at 4.5 kV rms and a gap spacing for up to a 30 s plasma-off period for the dielectric material
d = 2.5 cm at frequencies of (a) 30 kHz; (b) 40 kHz; (c) 60 kHz; and (Pyrex™) used in the Mod T reactor.
(d) 80 kHz. Experiments for N2 , He and air confirmed that a uniform
OAUGDP™ can be easily obtained in the Mod T reactor by
coarse filaments, and then became brighter and more uniform, flowing N2 and He gases, at a 5 lpm flow rate, through the
to the point where it was uniform to the eye at about 2–3 kHz. discharge volume. The gap distance and frequency domain
As the frequency was further raised, it remained uniform to the required to produce a uniform He plasma are 1–5 mm and
eye until 30 kHz, as shown in figure 9(a). Above this frequency, 0.5–37 kHz, respectively. Above 20 kHz, our power supply
however, the appearance of the discharge became progressively had to be operated out of its resonant frequency with the Mod T
less uniform, with increasing gaps and coarse filaments, as reactor (3.7 kHz), and was therefore not able to energize the
shown in figures 9(b)–(d). These filaments were as much plasma sufficiently to cover the entire electrode area.
as 2 mm in diameter, larger than the sub-micrometre scale Only a uniform plasma was obtained in helium up to a
filaments normally associated with avalanching in the DBD. 3 mm gap distance. Above 3 mm, three modes of He discharge
Under uniform conditions, a slight increase in luminosity near were identified. Immediately after breakdown, as shown in
the electrodes was evident, consistent with the presence of the figure 11(a), a plasma spot several centimetres in diameter
negative glow near the instantaneous cathode. In helium gas, formed, and this was associated with a single current pulse
the luminosity appeared to be greatest circa 10 kHz. In helium and continuous light emission lasting for 10 µs. An increase
and argon, the plasma was initiated at electric fields from 2 to in voltage changes this uniform region into a microfilament
3 kV cm−1 ; in air, an electric field of at least 8.5 kV cm−1 was DBD mode, as shown in figure 11(b), with multiple current
required, and the frequency range over which the plasma was pulses of the same time duration as the primary uniform mode.
uniform was much more restricted. Increasing the voltage further enhances the number density of
the discharge filaments in the reactor until it is not possible
Uniformity viewed along the electric field. Figure 9 shows the to identify individual filaments, as illustrated in figure 11(c).
luminosity in helium perpendicular to the electric field. We For frequencies below 7 kHz, a ‘primary uniform mode’ with
used the Mod T transparent electrode reactor of figure 5 to study a single current peak is not present.
the uniformity of the OAUGDP™ along the electric field lines. The gap distance and frequency domain for a nitrogen
Previous research on OAUGDP™ reactors revealed significant uniform plasma were 1–3 mm and 1–12 kHz, respectively.

560
The One Atmosphere Uniform Glow Discharge Plasma reactor

0s 3s 6s

9s 12 s 15 s

Figure 10. Plan view images of the Mod T transparent electrode reactor, showing intensification and propagation of the uniform glow
discharge mode from the centre to fill the reactor cross section. Images taken with 1 s exposure time, artificially enhanced contrast and
plasma operating conditions of 3.5 kHz and 12 kV rms.

The current waveform exhibits a characteristic single hump the Mod VI reactor of figures 3 and 4 for various durations,
free of any streamer pulse component. Unlike the situation for various arrangements of recirculating gas flow, for visibly
in helium, the nitrogen OAUGDP™ in the Mod T reactor uniform OAUGDP™ conditions and under conditions for
always operated in the primary uniform mode. Above 12 kHz which the reactor was filamentary and functioning as a DBD.
the power supply used was not able to initiate electrical During these tests, the lower electrode of the Mod VI
breakdown. reactor (15 cm in diameter) was covered by a 20 cm diameter
When a gap distance of 3 mm is exceeded, a nitrogen silicon wafer, with the photoresist directly exposed to the
plasma begins to operate in the gas stream-line coupled mode plasma. After adjustment of the flow velocity, flow geometry,
illustrated in figure 12(a). This appears to be the mode referred RF frequency and rms voltage, we obtained the result shown in
to by Gherardi et al [22]. The associated current waveform figure 13, a topographical representation of the average depth
was, however, the same as that of the uniform mode, i.e. free of photoresist removed over 5 min of OAUGDP™ exposure.
of streamer pulses. The macroscopic uniformity of stripping across the 15 cm
For dry air and discharge gaps larger than 1.5 mm, the diameter of the plasma was a commercially acceptable 5%,
plasma generated is in the DBD mode when operated in still and the stripping rate was 270 nm min−1 .
air. In flowing air, it operates in a stream-line coupled mode, An additional requirement for microelectronic stripping
as shown in figure 12(b). The presence of gas flow makes is that the process not deposit dust or contaminants on the
the transition from the DBD to the uniform mode much faster wafer, and this is normally assured by maintaining clean room
(<2 s). A bistable oscillation between the DBD and uniform conditions. Our lab is not a clean room, and this requirement
modes was not observed in the flowing gas. was not met. Figure 14 is an SEM of the etched surface
depicted in figure 13, under uniform OAUGDP™ conditions,
5. Uniformity of effect of OAUGD plasmas which reveals small ≈50 nm grains of dust that settled on the
surface of the photoresist. The corrugated, parallel structures
The type of data represented by figures 9–12 refer only to at the bottom of the etch are aligned with the gas flow in the
the apparent, visible luminosity of the plasma. For industrial Mod VI reactor (see figure 4). It should be noted that under
applications, one would like to have, in addition, data showing these uniform OAUGDP™ conditions, the surface of the wafer
that the OAUGDP™ is uniform in its effect on workpieces at is free of the pitting associated with filamentation and/or DBD
the microscopic scale. Such data were produced in the course operation.
of research programmes conducted with other objectives. SEMs of the surface obtained when the Mod VI reactor
was operating in a visibly filamentary/DBD mode revealed the
Uniformity of effect in etching of photoresist. In one such features shown in the images of figure 15. These features are
programme, we exposed several 20 cm diameter silicon wafers, consistent with surface damage at the root of microfilaments
coated with a proprietary photoresist, to an air OAUGDP™ in in the DBD, where the local energy flux is highest.

561
J R Roth et al

(a)

(b)

(c)

Figure 11. Current (——) and PMT (· · · · · ·) waveforms and corresponding photographs for three different modes of helium OAUGDP™ at
a fixed frequency f = 8 kHz, gap width D = 3 mm: (a) primary uniform mode, (b) DBD mode, (c) secondary uniform mode.

Uniformity of effect in etching PET. In the course of research embedded in the surface. Figure 16(b) shows an SEM of a
aimed at increasing the surface energy of polymeric films piece of the same white PET film made after direct exposure
[34], we saw unmistakable evidence of vertical etching in a for 5 min to an air OAUGDP™ operating in the Mod IV reactor
poly(ethylene terephthalate) (PET) film that was exposed to [34] at 5 kHz and 12 kV rms, with single-pass airflow. Close
a uniform OAUGDP™ operating in air. This film is made inspection of figure 16 reveals numerous spires that feature a
commercially for the white plastic covering of baby diapers, grain of titanium dioxide at their top, some with diameters less
and the white colour is imparted by fine grains of titanium than 200 nm and length/diameter ratios as high as 20.
dioxide (TiO2 ) pigment. The titanium dioxide is much harder The etching rate of PET implied by the tallest spires (those
and more resistant to etching than the PET that surrounds it. with the TiO2 grains originally nearest the surface) over the
Figure 16(a) shows an SEM of an untreated sample of 5 min exposure period is about 500 nm min−1 . There is no
this white PET film. A few grains of the TiO2 pigment are indication in the field of view of the SEM of pitting or melt

562
The One Atmosphere Uniform Glow Discharge Plasma reactor

(a) (b)

Figure 12. OAUGDP™ in flowing gas at 3.5 mm discharge gap; f = 3.5 kHz; 0.6 s exposure time; diameter of figures corresponds to
120 mm: (a) nitrogen, (b) dry air.

a simple method involving a Pearson current monitor and a


variable high voltage capacitor was used, as shown in figure 10.
The OAUGDP™ reactor is represented as a parallel connection
of a parasitic capacitance Cp and a real reactance Z. A Pearson
current monitor is placed between the compensating variable
capacitor, Ck , and the reactor. It measures Ip and Iz , which
represent the parasitic current and real current, respectively.
The wire carrying the compensating current, Ik , is wound
around the body of the Pearson current monitor, forming nk
loops. The sense of winding is such that Ik is opposite to
I = Ip + Iz (figure 17).
The voltage induced on the Pearson current monitor is
Figure 13. Isometric contour plot of etching depth across a 20 cm R R R
diameter silicon wafer with a uniform coating of photoresist (outer U = − (Ip + Iz − Ik nk ) = − Iz − j U0 ω(Cp − nk Ck ),
n n n
circle) directly exposed to a visibly uniform air OAUGDP™, 15 cm
in diameter, for 5 min (wafer and topographic analysis courtesy of (3)
Eaton Corporation). where R and n are parameters of the Pearson current monitor
itself. When Ck = Cp /nk , the imaginary term is equal to zero,
damage similar to that of figure 15. It is also likely that the and the Pearson current monitor senses only the real current,
spire structures would have served as ‘lightning rods’ for the Iz , through the plasma:
formation of avalanches and filamentation, and would have R
been destroyed. The fact that no such damage is evident is U = − Iz . (4)
n
another indication that the OAUGDP™ can be made uniform
in effect. The physical process(es) responsible for vertical The power dissipated in the reactance Z by the harmonic
etching have not been identified at this time. current can then be expressed as

P = 21 Umax Imax , (5)


6. Parasitic heating of reactor components
where Umax and Imax are the maxima of the applied voltage and
In the course of our research, we noticed that the input power Pearson current monitor reading, respectively.
into our OAUGDP™ reactors appeared to be greater than could The general formula describing the dielectric power losses
be accounted for by the power needed to create the OAUGDP™ is [35]
plasma itself. We then took measurements to determine the 2 2πf A
P = Umax εr ε0 tan δ. (6)
role of dielectric heating of the insulating plates (3 mm thick d
Pyrex) and other forms of parasitic losses in the Mod VI parallel Substituting typical values for our experiment, Umax = 1 kV;
plate reactor, and the dielectric heating losses to the 1 mm thick f = 5 kHz; A = 13 × 13 cm2 ; d = 1 mm; tan δ = 0.04
Pyrex pane in the Mod T transparent electrode parallel plate and εr = 5, we obtain 0.9 W of absorbed power. The values of
reactor. tan δ and εr correspond to Pyrex 7740, the Pyrex glass with the
highest loss factor (based on CRC Handbook of Chemistry and
Direct measurement of the real dissipated power below the Physics 84th edn, pp 12–59). This gives us an upper estimate
plasma onset voltage. To measure directly the real current of the expected power losses in the Pyrex material of typical
flowing in our capacitively coupled OAUGDP™ reactor, parallel plate reactors.

563
J R Roth et al

(a) (a)

(b) (b)

(c)

Figure 15. SEMs of photoresist etched in the Mod VI reactor


operating in the DBD mode with airflow from left to right. The
approximate distance across the width of the above images is
(a) 25.8 µm and (b) 2.4 µm. Note the pits formed by the roots of
microdischarges and/or filaments.

(a)

Figure 14. SEMs of photoresist etched in the presence of surface


dust in the Mod VI reactor (see figures 3 and 4) operating in the
OAUGDP™ mode with airflow from left to right. The approximate
distance across the width of the above images is (a) 7.9 µm,
(b) 3.1 µm and (c) 1.1 µm. Note the absence of microdischarge pits
and the presence of vertical etching.

Dielectric heating power in the Mod T reactor. Figures 18


and 19 show our results for the dissipated power as a function
(b)
of the applied rms voltage and the parameter f (Urms )2 ,
respectively. Data were obtained for two discharge gaps,
d = 1 mm, 3 mm.
The frequencies were within the range 3–15 kHz, and the
applied voltage, Urms , between 600 and 9400 V. The linear
dependence between the dissipated power and the f (Urms )2
product from figure 19 enables us to identify the dissipated
power as pure dielectric losses. The lower value of the
linear slope for the data at the d = 3 mm gap suggests the
contribution of the discharge volume to dielectric losses as
well, by increasing the value of d in equation (6). Figure 16. SEMs of PET film before (a) and after (b) a 5 min
exposure to an air OAUGDP™. Both images are approximately
Dielectric heating power in the Mod VI reactor. The power 20 µm wide [37]. (a) Unexposed film with scattered grains of
titanium dioxide pigment. (b) PET film after direct exposure to an
input to the parallel plate Mod VI OAUGDP™ reactor was air OAUGDP for 5 min at operating conditions of 5 kHz and
calculated using a programmable oscilloscope that multiplied 12 kV rms. Note the sub-micrometre spires under titanium dioxide
the instantaneous voltage and current flowing to the reactor grains and the absence of pitting due to filamentation.

564
The One Atmosphere Uniform Glow Discharge Plasma reactor

d=1mm
(a) 100
3 kHz
5 kHz Plasma ON
7 kHz
15 kHz
-11 2
6.0x10 *U f
10

Power [W]
1 Plasma OFF

Figure 17. Schematic of the method.

d 0.1
(a)

0.01
9 10 11 12
10 10 10 10
2 2 -1
f (Urms)[V s ]

d=3 mm
(b) 100
3 kHz
5 kHz Plasma ON
7 kHz
15 kHz
-11 2
4.1x10 *U f
10
Power [W]

1 Plasma OFF

Voltage RMS
0.1

d
(b)
0.01
9 10 11 12
10 10 10 10
2 2 -1
f (Urms)[V s ]

Figure 19. Mod T reactor power versus f (Urms )2 for (a) d = 1 mm,
(b) d = 3 mm.

us to determine the functional relation corresponding to


equation (6).

P = KU 2 f = 0.05U 2 f [W, kV, kHz]. (7)

This formula has been used to plot the dielectric heating


power alone as a dashed line in figure 20. At a given frequency
and voltage, the dielectric heating power can be as much as
5–30% of the power deposited in the plasma.
Figure 18. Mod T reactor (transparent electrode configuration)
power versus voltage for various frequencies: (a) d = 1 mm, 7. Conclusions
(b) d = 3 mm.
The formation of a uniform plasma at 1 atm was demonstrated
in various gases, including dry air. In a manner similar to
and integrated over an RF cycle. This removed the reactive that in helium, atmospheric pressure air could operate in both
power, leaving only the power delivered to the plasma and a spatially uniform and a filamentary DBD mode. At the
the power used by dielectric heating of the panel material. The macroscopic level, the uniform mode is characterized by
latter two inputs were resolved by operating the Mod VI reactor the absence of localized highly luminous hot filaments. At
below the point of plasma initiation, so that all input power was the microscopic level, their absence was confirmed by SEM
consumed by heating the dielectric material. images of OAUGDP™ treated polymer samples. Surface
The total power to the reactor is shown in figure 20. In charge appears to play an important role in the growth and
these data, the plasma was initiated above 4 kV. The data stabilization of the uniform mode of plasma operation in air,
below 5 kV are due to dielectric heating only and allow and is currently being studied intensively.

565
J R Roth et al

150 References
8 kV Total power
100 Dielectric heating
50 Hard copies of many of the references by University of
0 Tennessee authors may be downloaded in their entirety
100 from the website http://plasma.ece.utk.edu by clicking on
7 kV ‘publications’ on the homepage and then clicking on the ti-
50 tle of the desired reference.
0
50 [1] Roth J R 1995 Industrial Plasma Engineering
6 kV Vol I—Principles (Bristol: Institute of Physics Publishing)
25 see section 12.5.2
[2] Roth J R 2001 Industrial Plasma Engineering
0 Vol II—Applications to Non-Thermal Plasma
Power [Watt]

20 Processing (Bristol: Institute of Physics Publishing) see


5 kV section 18.6
10 [3] Eliasson B and Kogelschatz U 1988 Appl. Phys. B 46
299–303
0
[4] Schutze A, Jeong J Y, Babayan S E, Park J, Selwyn G S
10 and Hicks R F 1998 IEEE Trans. Plasma Sci. 26
4 kV
5
1685–94
[5] Roth J R, Tsai P P and Liu C 1995 US Patent No 5,387,842
0 [6] Roth J R, Tsai P P, Liu C, Laroussi M and Spence P D 1995
10 US Patent No 5,414,324
3 kV [7] Ben Gadri R 1999 IEEE Trans. Plasma Sci. 27 36–7
5 [8] Rabehi A, Ben Gadri R, Segur P, Massines F and Decomps Ph
1994 Proc. Conf. on Electrical Insulation and Dielectric
0 Phenomena (CEIDP 94) (Arlington, TX) pp 840–5
5 [9] Ben Gadri R, Rabéhi A, Massines F and Ségur P 1994 Proc.
2 kV
12th European Sectional Conf. on the Atomic and
Molecular Physics of Ionized Gases (Noordwijkkerhout,
0
The Netherlands) pp 228–9
[10] Ben Gadri R 1997 Numerical simulation of an atmospheric
2 4 6 8 10 12 pressure and dielectric barrier controlled glow discharge
f [kHz] PhD Thesis Order No 2644, University Paul Sabatier,
Toulouse III, France
Figure 20. Total reactor input power as a function of RF frequency [11] Massines F, Rabehi A, Decomps Ph, Ben Gadri R, Segur P and
and RF voltage in the Mod VI parallel plate OAUGDP™ plasma Mayoux C 1998 J. Appl. Phys. 83 2950–7
reactor. Calculated dielectric heating for K = 0.04 W kHz−1 kV−2 [12] Von Engle A, Seeliger A and Steenback M 1933 Z. Phys 85
is represented by the dashed line. 144–60
[13] Kanazawa S, Kogoma M, Moriwaki T and Okazaki S 1988
J. Phys. D: Appl. Phys. 21 838–40
We have shown that the real power input to an OAUGDP™ [14] Yokoyama T, Kogoma M, Moriwaki T and Okazaki S 1990
parallel plate reactor is dissipated both by heating of the J. Phys. D: Appl. Phys. 23 1125–8
dielectric material covering the electrodes and by power input [15] Kanda N, Kogoma M, Jinno H, Ychiyama H and Okazaki S
1991 Proc. 10th Int. Symp. on Plasma Chemistry vol 3,
to maintain the plasma. The fraction of the total input power
pp 3.2-201–3.2-204
dissipated as dielectric heating ranged over 16–100% for the [16] Roth J R, Laroussi M and Liu C 1992 Paper No 5P21 Proc.
Mod VI parallel plate reactor, and over 10–100% for the Mod T 19th IEEE Int. Conf. on Plasma Science (Tampa, FL)
reactor. These power fractions are significant and imply that pp 170–1
care should be taken to select dielectric materials with low [17] Liu C and Roth J R 1992 APS Bull. 37 1563
[18] Roth J R, Tsai P P, Wadsworth L C, Liu C and Spence P D
losses. The importance of dielectric heating power loss is 1995 Method and apparatus for glow discharge plasma
likely to extend to other atmospheric pressure plasma reactors, treatment of polymer materials at atmospheric pressure
including DBDs. US Patent No 5,403,453
[19] Roth J R, Tsai P P, Liu C and Wadsworth L C 1995 Method
and apparatus for glow discharge plasma treatment of
polymer materials at atmospheric pressure US Patent
Acknowledgments No 5,456,972
[20] Massines F et al 2003 Surf. Coat. Technol. 174–175
This work was supported in part by the National Science 8–14
Foundation (NSF) Nanoscale Exploratory Research (NER) [21] Wagner H E et al 2003 Vacuum 71 417–36
[22] Gherardi N et al 2001 IEEE Trans. Plasma Sci. 29
grant, NSF-NER DMI-0210554, in part by the University of
536–44
Tennessee Center for Materials Processing (Director Dr Carl [23] Golubovskii Yu B et al 2003 J. Phys. D: Appl. Phys. 36
McHargue), in part by Atmospheric Glow Technologies, Inc. 975–81
(President Thomas W Reddoch) and in part by AFOSR [24] DeBenedictis S et al 1997 J. Chem. Phys. 107 6219–29
Contract AF F49620-01-1-0425 (Roth) (Program Manager [25] Liu C and Roth J R 1994 Proc. 21st IEEE Int. Conf. on Plasma
Sci. (Santa Fe, NM) pp 97–8
John Schmisseur). The Eaton Corporation provided silicon [26] Roth J R 1997 Method and apparatus for covering bodies with
wafers and performed SEM analysis for the topographic a uniform glow discharge plasma and applications thereof
studies. US Patent No 5,669,583

566
The One Atmosphere Uniform Glow Discharge Plasma reactor

[27] Sherman D M, Wilkinson S P and Roth J R 2001 Paraelectric [33] Roth J R, Sherman D M, Gadri R B, Karakaya F, Chen Z,
gas flow accelerator US Patent No 6,200,539 B1 Montie T C, Kelly-Wintenberg K and Tsai P P 2000 IEEE
[28] Roth J R, Sherman D M and Wilkinson S 1998 Proc. 36th Trans. Plasma Sci. 28 56–63
AIAA Aerospace Sciences Meeting & Exhibit (Reno, NV) [34] Carr A K 1997 Increase in the surface energy of metal and
Paper AIAA 98-0328 polymeric surfaces using the one atmosphere uniform glow
[29] Roth J R 2003 Phys. Plasmas 10 2117–26 discharge plasma, MS in EE Thesis University of Tennessee,
[30] Chen Z 2002 IEEE Trans. Plasma Sci. 30 1922–30 Knoxville
[31] Chen Z 2003 IEEE Trans. Plasma Sci. 31 511–20 [35] John D Kraus 1991 Electromagnetics 4th edn (New York:
[32] Montie T C, Kelly-Wintenberg K and Roth J R 2000 IEEE McGraw-Hill) Sec ‘10–14 Dielectric Hysteresis’,
Trans. Plasma Sci 28 41–50 p 445

567

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