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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)
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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)
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J R Roth et al
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.
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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.
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J R Roth et al
(a) (a)
(b) (b)
(c)
(a)
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
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.
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]
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