USOO544324A

United States Patent (19) 11 Patent Number: 5,414,324

Roth et al. 45 Date of Patent: k May 9, 1995
54) ONE ATMOSPHERE, UNIFORMGLOW Treated With Low Temperature Plasma: Effect Of
DISCHARGE PLASMA Pretreatment With Dimethylformamide Publication:
75 Inventors: John R. Roth; Peter P. Tsai; Chaoyu sen-i gakkaishi, vol. 43, No. 7 (1987).
Liu; Mounir Laroussi; Paul D. Authors: Wakida, T.; Kawamura H.; Song, J. C.; Goto
Spence, all of Knoxville, Tenn. T.; Takagishi, T. Title: Surface Free Energy Poly
73) Assignee: The University of Tennessee Research (Ethylene Terephthalate) And Nylon 6 Films Treated
Corporation, Knoxville, Tenn. With Low Temperature Plasma Publication: Seni-I
Gakkaishi, vol.43, No. 7 (1987).
* Notice: The portion of the term of this patent Authors: Kogoma, M.; Kasai, H.; Takahashi, K.;
subsequent to Feb. 7, 2012 has been Moriwaki, T. & Okazaki, S. Title: Wettability Control
disclaimed. Of A Plastic Surface By CF4 Plasma And Its Etching
21 Appl. No.: 145,786 Effect Publication: J. Phys. D. Appl. Phys, vol. 20
22 Filed: Oct. 29, 1993 (1987).
Authors: Kanazawa, S.; Kogoma, M.; Moriwaki, T., &
Related U.S. Application Data Okazaki, S. Title: Stable Glow Plasma. At Atmospheric
Pressure Publication: J. Physics D. Appl. Phys, vol. 21
63 Continuation-in-part of Ser. No. 68,508, May 28, 1993. (1988) pp. 838-840.
51) int. Cl................................................. HO1, 7/24 Author: Rakowski, W. Title: Plasma Modification Of
52 U.S. C. .......................... 315/111.21; 315/111.51; Wool Under Industrial Conditions Publication: Mell
118/723 E iand Textilberichte, vol. 70 (1989) pp. 780-785.
58) Field of Search ...................... 315/111.21, 111.51; Authors: Yokoyama, T.; Kogoma, M.; Moriwaki, T.; &
118/723 E, 723 I; 313/231.31 Okazaki, S. Title: The Mechanism Of The Stabilisation
56) References Cited Of Glow Plasma. At Atmospheric Pressure Publication:
U.S. PATENT DOCUMENTS J. Physics D. App. Phys, vol. 23 (1990) pp. 1125-1128.
Authors: Naoki Kanda; Masuhiro Kogona; Hiroshi
5,147,493 9/1992 Nishimura ...................... 35/11.51 (List continued on next page.)
5,272,417 12/1993 Ohmi ........... ... 35/11.2
5,309,063 5/1994 Singh .............................. 315/111.51 Primary Examiner-Robert J. Pascal
FOREIGN PATENT DOCUMENTS ASSistant Examiner-Darius Gambino
Attorney, Agent, or Firm-Weiser & Associates
0068775 1/1983 European Pat. Off. .
0117561 9/1984 European Pat. Off. . 57 ABSTRACT
0292582 8/1991 Germany ........................ 315/11.21
0200529 11/1983 Japan .............................. 313/111.21 A steady-state, glow discharge plasma is generated at
1177374 8/1986 Japan ............................... 18/723 E one atmosphere of pressure within the volume between
0002544 1/1987 Japan ............................... 118/723 E a pair of insulated metal plate electrodes spaced up to 5
62-235339 10/1987 Japan . cm apart and R.F. energized with an rms potential of 1
422.5226 8/1992 Japan .............................. 315/11.21
to 5KV at 1 to 100 KHz. Space between the electrodes
OTHER PUBLICATIONS is occupied by air, nitrous oxide, a noble gas such as
Authors: Von Engel, A.; Seeliger, R.; & Steenbeck, M. helium, neon, argon, etc. or mixtures thereof. The elec
Title: On The Glow Discharge At High Pressure Publi trodes are charged by an impedance matching network
cation: Zeit, fur Physik, vol. 85 (1933) pp. 144-160. adjusted to produce the most stable, uniform glow dis
Authors: Wakida, T.; Kawamura, H.; Han, L.; Hwan charge.
Kim, K. Goto, T.; & Takagishi, T. Title: Changes In
Surface Properties Of Poly(Ethylene Terphthalate) 27 Claims, 10 Drawing Sheets
22
per
after
we kHz
0-10kVrns
ska
 5,414,324
Page 2

OTHER PUBLICATIONS lator Symposium, 1992.

Jimmo; Hiroshi Uchiyama & Sachiko Okazaki Title: Author: Rakowski, W. Title: Effect And Cost Of
Atmospheric Pressure Glow Plasma And Its Applica Plasma Treatment Of Polypropylene Melt Blown Webs
tion To Surface Treatment And Film Deposition. Publi Publication: Second Annual TANDEC Conference,
cation: International Symposium on Plasma Chemistry, 13-16 Oct., 1992.
Symposium Proceedings, vol. 3, Bochum, Germany, Authors: Liu, C. Title: Plasma-Related Characteristics
Aug. 4-9, 1991. Of A Steady-State Glow Discharge At Atmospheric
Authors: Liu, C.; Chen, D.; & Roth, J. R. Title: Charac Pressure Publication: Presented at the 1993 Sigma XI
teristics Of A Steady-State, Low Power Glow Dis Graduate Student Paper Competition, The University of
charge At Atmospheric Pressure Publication: APS Bul Tennessee, Knoxville, Tenn. on Mar. 4, 1993.
letin, vol. 37, No. 6 (1992) p. 1563. Authors: Roth, J. R.; Spence, P. D.; Liu, C. Title: Plas
Authors: Roth, J. R.; Liu, C.; & Laroussi, M. Title: ma-Related Characteristics of A Steady-State Glow
Experimental Generation Of A Steady-State Glow Discharge At Atmospheric Pressure Publication: Paper
Discharge At Atmospheric Pressure Publication: Paper 2P-18, Proc. 1993 IEEE International Conference on
Plasma Science, Vancouver, B. C. IEEE Catalog No.
5P-21, Proc. 1992 IEEE International Conference on 93-CH3334-0, ISBN 0-7803-1360-7 (1993), p. 129.
Plasma Science, Tampa, Fla., IEEE Catalog No. Authors: Roth, J. R.; Spence, P. D.; Liu, C. Title: Pre
92-THO460-6, ISBN 0-7803 0716-X (1992), pp. liminary Measurements Of The Plasma Properties. Of A
170-171. One Atmosphere Glow Discharge Plasma Publication:
Authors: Reitz, H.; Schwarz, R.; Salge, J. G. H. Title: Paper Present at 35th Annual Meeting of the APS Divi
Power Modulation For Dielectric Barrier-Discharges sion of Plasma Physics, St. Louis, Mo., Nov. 1-5, 1993;
Publication: Paper presented at Twentieth Power Modu APS Bulletin, Series II, vol. 38, No. 10 (1993), p. 1901.
U.S. Patent May 9, 1995 Sheet 1 of 10 5,414,324

X
S)
O
- c

CX

4:Z :7-Z{) DA,

CN N
CN

A.
N
s

||—|!||31·glZSH/u>d10A

7AJE/MOdI{|c_z/HWX901-6)2/3 Gy07 EN.IXMAJOM

U.S. Patent May 9, 1995 Sheet 3 of 10 5,414,324
U.S. Patent May 9, 1995 Sheet 4 of 10 5,414,324

01AJEM 07 302/17
U.S. Patent May 9, 1995 Sheet 5 of 10 5,414,324

Ima/div
villa
N /N /\ Y REACTIVE CURRENT
VIVA V Ir= 1. 3 mArms
| | | | | | |
Al-AP-1--- PLATE VOLTAGE
1 150 W/div (NAA/NIE VF 1012 Wins

FIG. 7A
ENI IN/
200 pulsec/div
(2kHz)

| | | | | | | |
All All
| | | | IC
Atlall TOTAL CURRENT
It =9. 6mArms

towaiv bj| V | | III| | |

FIG. 7B IIIT III
200 usec/div

|A ||
11.5 WATTS/div AAA IIIEAL 21"
A-L-I-S-N-15P E.
|| || | ID 4 grant
JAL JUUUU -- "rms
// AI? A A PLATE VOLTAGE
AN/NIEN/ Vof 1012 Wins
w V RM
FIG. 7C 200 pusec/div
U.S. Patent May 9, 1995 Sheet 6 of 10 5,414,324

| | | | | | |
1 Oma/div NAZQA
N/I NY | N/
REACTIVE CURRENT
Ir=8. O mArms
| | | | | | | |
Al-RIAP PLATE VOLTAGE
1 150 W/div (MAN (ENE/ V=92O Vrms
by TV/VTV/ (8kHz)
FIG. BA
| | | | |
50 usec/div

TTTTTT
N UW NC US TOTAL CURRENT
MNY/1 it -56 Arms
-In-la
NINNIN PLASA cuRRENT
/ Y| 71 1-52 mArms
50waiver HM II
FIG. BB 50 pulsec/div

| | | | | | | |
115 WATTS/odiv AAA-lear
PLASMA POWER
P = 18.4 WATTS
N YTY
IN NO US PLASMA CURRENT .
M M M I =52 mArms
(NAV (EN/
PTV/ MTV/
PLATE VOLTAGE
VF920 Vs
FIG. BC
U.S. Patent May 9, 1995 Sheet 7 of 10 5,414,324

d= 1. 75cm
m=6 LPM, He

TOTAL POWER

PLASMA POWER
P a v3

NONUNIFOR PLASA INITIATED

f 2 3 4 5
PLATE VOLTAGE k Vs

FIG. 9
U.S. Patent May 9, 1995 Sheet 8 of 10 5,414,324

d= 1. 75cm
m=6 LPM, He

)
ONSET OF
FILAMENTARY
TOTAL POWER - DISCHARGE.

PLASMA POWER
P a fr2

f 2 3 4 5 6 78
SOURCE FREQUENCY (kHz)

FIG. 10
U.S. Patent May 9, 1995 Sheet 9 of 10 5,414,324

f 2 4 6 8 10 2O 3O 4O 6O 80 100
FREQUENCY, kHz

FIG. 11
U.S. Patent May 9, 1995 Sheet 10 of 10 5,414,324

18O

16O

14O

12O

1OO

8.O
6O

O
O 1 2 3 4 5 6 7 8 9 TO
FREQUENCY V, kHz

FIG. 12
 5,414,324
1 2
supplies since the late 19th century. Filamentary dis
ONE ATMOSPHERE, UNIFORM GLOW charge plasmas are dramatically distinguished from
DISCHARGE PLASMA uniform glow discharge plasmas. Such filamentary dis
LICENSE RIGHTS 5
charges, while useful for ozone production, are of lim
ited utility for the surface treatment of materials, since
The U.S. Government has a paid-up license in this the plasma filaments tend to puncture or treat the sur
invention and the right in limited circumstances to re face unevenly.
quire the patent owner to license others on reasonable It is, therefore, an object of the present invention to
terms as provided for by the terms of contract No. O
teach the construction and operating parameters of a
AFOSR 89-0319 awarded by The U.S. Air Force. continuous glow discharge plasma sustained at a gas
CROSS-REFERENCES TO RELATED pressure of about one atmosphere or slightly greater.
APPLICATIONS INVENTION SUMMARY
This application is a Continuation-In-Part of U.S. 15 This and other objects of the invention to be subse
patent application Ser. No. 08/068,508 filed May 28, quently explained or made apparent are accomplished
1993. with an apparatus based upon a pair of electrically insu
BACKGROUND OF THE INVENTION lated metallic plate electrodes. These plates are
1. Field of Invention
mounted in face-to-face parallel or uniformly spaced
The present invention relates to methods and appara alignment with means for reciprocatory position adjust
tus for generating low power density glow discharge ment up to at least 5 cm of separation. Preferably, the
plasmas at atmospheric pressure. plates are water cooled and covered with a dielectric
insulation.
2. Description of the Prior Art To broaden the range of operating frequency and
In the discipline of physics, the term "plasma' de
scribes a partially ionized gas composed of ions, elec 25 other parameters over which the desirable uniform (as
trons and neutral species. This state of matter may be opposed to filamentary) glow discharge is observed, an
produced by the action of either very high tempera impedance matching network is added to the circuit for
tures, strong constant electric fields or radio frequency charging the electrodes. The parameters of such a
(R.F.) electromagnetic fields. High temperature or matching network are adjusted for the most stable,
“hot” plasmas are represented by celestial light bodies, 30 uniform operation of the glow discharge. This condi
nuclear explosions and electric arcs. Glow discharge tion can occur when the reactive power of the plasma
plasmas are produced by free electrons which are ener reactor is minimized.
gized by imposed direct current (DC) or R.F. electric A radio frequency power amplifier connected to both
fields, and then collide with neutral molecules. These plates delivers up to several hundred watts of power at
neutral molecule collisions transfer energy to the mole 35 a working voltage of 1 to at least 5 KV rms and at 1 to
cules and form a variety of active species which may 100 KHz. To assist the starting of the plasma, the elec
include photons, metastables, atomic species, free radi trical discharge from a standard commercial Tesla coil
cals, molecular fragments, monomers, electrons and may be briefly applied to the volume between the R.F.
ions. These active species are chemically active and/or energized plates. An electric field established between
physically modify the surface of materials and may 40 the metallic plate electrodes must be strong enough to
therefore serve as the basis of new surface properties of electrically break down the gas used, and is much lower
chemical compounds and property modifications of for helium and argon than for atmospheric air. The RF
existing compounds. frequency must be in the right range, discussed below,
Very low power plasmas known as dark discharge since if it is too low, the discharge will not initiate, and
coronas have been widely used in the surface treatment 45 if it is too high, the plasma forms filamentary discharges
of thermally sensitive materials such as paper, wool and between the plates. Only in a relatively limited fre
synthetic polymers such as polyethylene, polypropyl quency band
ene, polyolefin, nylon and poly(ethylene terephthalate). plasma reactor will form
the atmospheric glow discharge
a uniform plasma without filamen
Because of their relatively low energy content, corona
discharge plasmas can alter the properties of a material 50 tary discharges.
To stabilize the plasma and discourage the formation
surface without damaging the surface.
Glow discharge plasmas represent another type of of the
plasma filaments, an inductor may be connected from
median plane to ground.
relatively low power density plasma useful for non
destructive material surface modification. These glow glow least
At in the volume between the plates wherein the
discharge plasma is established, a one atmosphere
discharge plasmas can produce useful amounts of visible 55
and ultraviolet radiation. Glow discharge plasmas have charge of helium, argon or other gas or mixture of gases
the additional advantage therefore of producing visible is established and maintained.
and UV radiation in the simultaneous presence of active The median plane between two parallel electrodes
species. However, glow discharge plasmas have hereto may or may not contain an insulating or electrically
fore been successfully generated typically in low pres conductive screen or plate which may be used to sup
sure or partial vacuum environments below 10 torr, port exposed materials in the glow discharge plasma
necessitating batch processing and the use of expensive environment. If electrically conductive, the median
vacuum systems. screen or plate may be electrically floating or grounded.
Conversely, the generation of low power density
plasmas at one atmosphere is not entirely new. Filamen 65 BRIEF DESCRIPTION OF THE DRAWINGS
tary discharges between parallel plates in air at one Relative to the drawings wherein like reference char
atmosphere have been used in Europe to generate ozone acters designate like or similar elements throughout the
in large quantities for the treatment of public water several figures of the drawings:
 3
5,414,324
4
FIG. 1 is a schematic of the present invention compo Surrounding the plate assembly is an environmental
nent assembly. isolation barrier 21 such as a structural enclosure suit
FIG. 2 represents a preferred embodiment of the able for maintaining a controlled gas atmosphere in the
electrical circuit, including an impedance matching projected plan volume between the plates 10. Inlet port
network and a grounded midplane screen connected to 22 is provided to receive an appropriate gas such as air,
ground through an inductor. helium or argon, mixtures of either with air or a mixture
FIGS. 3, 4 and 5 represent alternative power supply of argon with helium. Ambient air may also be used. In
output stage circuits. any case, gas pressure within the isolation barrier 21 is
FIG. 6 schematically represents the upper chamber substantially ambient thereby obviating or reducing the
of a one atmosphere glow discharge plasma reactor 10 need for gas tight seals. Normally, it is sufficient to
having a median grid plate. maintain a low flow rate of the modified one atmo
FIG. 7 represents a graph of voltage, current and sphere gas through the inlet port 22 that is sufficient to
power waveforms for a uniform glow discharge plasma. equal the leakage rate. Since the pressure within the
FIG. 8 represents a graph of voltage, current and isolation barrier 21 is essentially the same as that outside
power waveforms for a filamentary discharge plasma. 15 the barrier, no great pressure differential drives the
FIG. 9 is a log-log graph of total and plasma power leakage rate. A vent conduit 28 controlled by valve 29
density in milliwatts per cubic centimeter as a function is provided as an air escape channel during initial flush
of RMS voltage applied to the electrodes. ing of the enclosure. Thereafter, the valve 29 may be
FIG. 10 is a log-log graph of total and plasma power 20 closed for normal operation.
density in milliwatts per cubic centimeter, as a function To broaden the range of operating frequency and
of R.F. frequency. other parameters over which the desirable uniform (as
FIG. 11 is a graph of amplifier frequency and corre opposed to filamentary) glow discharge occurs, an im
sponding breakdown current phase angles respective to pedance matching network, one embodiment of which
is illustrated schematically by FIG. 2, is added to the
a particular operating example of the invention.
FIG. 12 is a graph of amplifier frequency and corre 25 power circuit for charging the electrodes 10. The pa
sponding total reactor power consumption respective to justed rameters of this impedance matching network are ad
a particular operating example of the invention. for the most stable, uniform operation of the
glow discharge. This condition can occur when the
DESCRIPTION OF THE PREFERRED reactive power of the plasma reactor is minimized.
EMBODIMENT 30 FIGS. 3 through 5 represent alternative power sup
Referring to the invention schematic illustrated by sponds ply options having respective attractions. FIG. 3 corre
FIG. 1, the electrodes 10 are fabricated of copper plate terminaltoT1a isconfiguration wherein the bottom electrode
having a representative square plan dimension of 21.6 terminal T2 is charged at ground
connected to
the full
potential and the top
working potential.
cmx21.6 cm. Silver soldered to the plates 10 are closed 35 FIGS. 4 and 5 are electrical equivalents
loops 11 of 0.95 cm copper tubing having hose nipples and T2 voltages are 180 out of phase but wherein at only
the T1
half the
12 and 13 connected therewith on opposite sides of the maximum potential. FIG. 4 represents a grounded cen
closed tubing loop. The edges of the electrode plates ter tap transformer whereas FIG. 5 represents a solid
should have a radius of curvature comparable to the
separation between the electrode plates and median 40 state power circuit embodiment.
plate to discourage electrical breakdown at the edge of form glow fields
Electric employed in a one atmosphere, uni
discharge plasma reactor are only a few
the electrodes. Not shown are fluid flow conduits con
kilovolts per centimeter, values which if D.C. would
nected to the inlet nipples 12 for delivering coolant fluid usually be too low to electrically break down the back
to the loop 11 and to the outlet nipples 13 for recovering ground gas. Gases such as helium and air will break
such coolant fluid. 45 down under such low electric fields, however, if the
The integral metallic units comprising plates 10 and positive ion population is trapped between the two
tubing 11 are covered with a high dielectric insulation parallel or uniformly spaced electrodes, thus greatly
material 14 on all sides to discourage electrical arcing increasing their lifetime in the plasma while at the same
from the edges or back side of the electrode plates. time the electrons are free to travel to the insulated
Preferably, some mechanism should be provided for 50 electrode plates where they recombine or build up a
adjusting the distances between plates. 10 up to at least surface charge. The most desirable uniform one atmo
5 cm separation while maintaining relative parallelism. sphere glow discharge plasma is therefore created when
Such a mechanism is represented schematically in FIG. the applied frequency of the RF electric field is high
1 by the rod adjusters 15 secured to the upper and lower
plates 10. This arrangement anticipates a positionally 55 enough to trap the ions between the median screen and
an electrode plate, but not so high that the electrons are
fixed median screen or plate 30. Although parallelism is also trapped during a half cycle of the R.F. voltage. The
used here in the context of parallel planes, it should be electrons may be trapped by bipolar electrostatic forces.
understood that the term also comprises non-planar If the RF frequency is so low that both the ions and
surfaces that are substantially equidistant. Also included the electrons can reach the boundaries and recombine,
are the geometry characteristics of a cylinder having an the particle lifetimes will be short and the plasma will
axis parallel to another cylinder or to a plate. either not initiate or form a few coarse filamentary
Energizing the plates 10 is a low impedance, high discharges between the plates. If the applied frequency
voltage, R.F. power amplifier 20 having independently is in a narrow band in which the ions oscillate between
variable voltage and frequency capacities over the re the median screen and an electrode plate, they do not
spective ranges of 1 to at least 9 KV and 1 to 100 KHz. 65 have time to reach either boundary during a half period
An impedance matching network 31 is connected be of oscillation and are carried for long times. If the more
tween the R.F. power amplifier and the electrode mobile electrons are still able to leave the plasma vol
plates. ume and impinge on the boundary surfaces, then the
 5,414,324
5 6
desirable uniform plasma is produced. If the applied RF -continued
frequency is still higher so that both electrons and ions C = yce Eo 1 (6)
are trapped in the discharge, then the discharge forms a 2 = -- (o? -- y?)
filamentary plasma.
Without limiting our invention to any particular the The one atmosphere helium glow discharge is oper
ory, we are disposed to a relationship between the elec ated at frequencies between cov27t=1 and 30 KHz,
trode spacing, the RMS electrode voltage, and the ap where, for helium at one atmosphere,
plied frequency which results in trapping ions but not
electrons between the two plates, and produces the 10
ycias 6.8x10°ion collisions/sec., (7a)
desired uniform one atmosphere glow discharge
plasma. On FIG. 6 is a schematic of the upper chamber and
of the one atmosphere glow discharge plasma reactor.
The lower boundary of this space is the midplane screen yeas 1.8x101 electron coll/sec. (7b)
or plate, the floating potential of which should remain 15
near ground if the RF power supply output is con The collision frequency for ions and electrons given by
nected as a push-pull circuit to the two electrodes with Eqs. 7a and 7b is much greater than the RF frequency,
a grounded center tap. In the data reported herein, the Vedd c). The relation ved > co for ions and electrons,
median screen was grounded through an inductive cur implies that C2 is much greater than the constant C1, or
rent choke. In the configuration of FIG. 6, a Cartesian
coordinate system is applied as shown, with the applied
electric field in the x-direction. The maximum ampli 2 2S
eEo
>> Cl
(8)
tude of the electric field between the grounded median nov
screen and the upper electrode is Eo, and the separation
of the screen from the electrodes is the distanced. The 25 The time dependent position of an ion or an electron in
median screen, with an exposed sample on it, is assumed the electric field between the plates is given by substi
not to allow ions through the median plane from the tuting Eq. 8 into Eq. 4, to obtain
upper chamber to the lower, or vice-versa.
The electric field between the electrodes shown on eEo (9)
FIG. 6 is given by 30 x(t) at - r cov
COSC).

E=(Eosin cot, O,O). (1) The RMS displacement of the ion or electron during a
half cycle is given by
It is assumed that the one atmosphere glow discharge
operates in a magnetic field free plasma. The equation of 35 eEo (10)
motion for the ions or electrons between the two plates X Prs - 2.
t
mcovc
letes o

is given by a Lorentzian model, in which the electrons

and ions collide only with the neutral background gas If V is the driving frequency, in Hertz, then the radian
and, on each collision, give up all the energy they ac RF frequency is given by
quired from the RF electric field since the last collision
to the neutral gas. The equation of motion for the ions c)=27Two, (11)
or electrons in the Lorentzian model is given by
and the maximum electric field between the plates can
F=ma= -nvy-eE, (b. 2) be approximated by the maximum voltage Voappearing
45
between them,
where the first term on the right hand side is the Lorent
zian collision term, according to which the momentum Vo (12)
mv is lost with each collision that occurs with a colli Ea -=
sion frequency ve. The x component of Eq. 2 is given by 50
If the charge in question moves across the discharge
width from the median plane to one of the electrode
d2X -- my
in -- = eEsincot,
(3) plates during one full cycle, then we may write
55 arms s d2 (13)
where the electric field E from Eq. 1 has been substi
tuted into the right hand side of Eq. 2. The general
solution to Eq. 3 is Equation 13 states that the RMS displacement of the
particle has to be less than half the clear spacing in order
x= C1 sin ot=C2 cos cot, (4) 60 to have a buildup of charge between the plates. In the
geometry shown in FIG. 6, the distance d is identified
where the constants C1 and C2 are given by with the distance between the grounded median screen
and the energized electrode. Substituting Eqs. 11 to 13
eEa 1.
into Eq. 10 yields the relationship
C s
(5)
(c) + r.) d eVrms (14)
and 27tmvoyd
 7
5,414,324
8
If we now solve for the critical frequency Vo above TABLE I-continued
which charge buildup should occur in the plasma vol OPERATING CHARACTERISTICS OF THE ONE
ume, we have ATMOSPHERE GLOW DISCHARGE PLASMA REACTOR
eV.
voltage = 1.5-9.5 kVrms plate to plate
- Hz.
v, as- -armyd? (15) electrode gap d = 0.8-3.2 cm
pressure = 760 -- i5, -5 torr
RMS power = 10 watts to 150 watts
power density = 4-120 mW/cm
In Eq. 15, the collision frequency ve is approximately plasma volume = 0.7-3.1 liters
given by Eqs. 7a or 7b for ions or electrons, respec 10
tively, at one atmosphere, and the RMS voltage is that
which bounds the upper and lower limit of the uniform ageOnandFIGS. 7 and 8 are shown two waveforms of volt
current taken in helium at the same electrode
discharge regime.
The range of parameters over which we have oper frequencies. FIG. flow
separation and gas conditions, but at two different
7 was taken in the uniform glow
ated a one atmosphere, uniform glow discharge plasma 15 discharge
reactor is given in Table I. The nominal pressure at was taken regime at a frequency of 2.0 kHz, and FIG. 8
in the filamentary discharge regime at a fre
which this discharge has been operated is one atmo quency above the uniform plasma operating band at 8.0
sphere. The variation of several torr shown in Table I is kHz. The high output impedance of our RF power
not intended to represent the day-to-day fluctuations of supply results in a voltage waveform (trace B) that is
barometric pressure, but the pressure differential across 20 very close to sinusoidal.
the midplane screen which is intended to drive active (trace C) is interrupted The by a
reactive current waveform
breakdown of the plasma
species from the upper plasma through the fabric being twice each cycle, once when the voltage is positive, and
exposed. The RMS power shown in Table I is the net once when the voltage is negative.
power delivered to the plasma, less the reactive power reactive current waveform at the Trace same
A shows the
voltage and
which does not appear in the plasma. The total volume 25 operating conditions, but in air, rather than
of plasma between the two electrode plates is given by There was no perceptible plasma present in airhelium. under
S=0.93 d(cm)liters, (16) these conditions, and the power is completely reactive.
This purely reactive current of trace A was subtracted
where d is the separation of a plate from the median 30 from the total plasma current in trace C, to yield trace
D. The instantaneous power deposited in the plasma
screen in centimeters.
The power densities shown in Table I are far below current (trace E) is found by multiplying the excess plasma
those of electrical arcs or plasma torches, but also are voltage above the reactive current (trace D) by the
several orders of magnitude higher than the power found by integrating at that point (trace B). The average power is
densities associated with some other forms of plasma 35 shown, and dividing byover this
the duration of the pulses
duration. It is in this manner
treatment such as corona discharges. The power densi
ties of the one atmosphere glow discharge plasma are that the power and power density into the plasma were
generally low enough not to damage exposed fabrics, calculated for these highly nonsinusoidal current wave
but are also enough higher than coronal plasmas used forms. FIGS. 8 for the uniform discharge and 8 for the
for surface treatment that they should provide far more filamentary
power
discharge show characteristically different
waveforms in trace E; this is a method of distin
active species than the latter. The plasma parameters, guishing the uniform from the filamentary discharge.
such as electron kinetic temperature and number den The plasma power is of interest because it is propor
sity are somewhat speculative at this early stage in the tional
development of our invention. A few results from prob plasma;tothethereactive production rate of active species in the
power is significant because it de
ing the plasma midplane with a floating Langmuir 45 termines the required power handling rating of the
probe indicates that the plasma, without grounding the plasma power supply and associated equipment. The
midplane screen, will float to positive potentials of sev total power is the sum of plasma and reactive power. On
eral hundred volts. The ion kinetic temperatures are FIG. 9 is shown a log-log plot of the plasma and total
very likely close to that of the room temperature atoms power
with which they frequently collide at these high pres 50 functions of the RMS voltage applied tocentimeter,
density in milliwatts per cubic as
the parallel
sures; the electrons apparently remain numerous and plates. The active plasma volume in FIG. 9 was 1.63
energetic enough to excite the neutral background liters, with
atoms, hence making this a glow discharge. The exis each plate ofa separationd=1.75
between the median screen and
centimeters in a plasma of helium
tence of excited states which emit visible photons im gas. On FIG. 10 is a similar presentation
plies that the electron population has a kinetic tempera 55 density plotted on log-log coordinates as of a
the power
function of
ture of at least an electron volt. The diagnostic difficul the frequency. The approximate bound of the uniform
ties of measuring plasma parameters at this high pres plasma discharge regime is shown by the arrow. These
sure are very severe, since ordinary Langmuir probing data were taken in helium gas for the same plasma vol
technique cannot be applied due to the short mean free
paths of the electrons compared to a Debye distance. 60 ume and electrode separation as FIG. 10.
Electron number densities, however, may be measured EXAMPLE 1
by microwave interferometric techniques. In a first operational example of the invention, the
TABLE I above described physical apparatus sustained a glow
OPERATING CHARACTERISTICS OF THE ONE discharge plasma in one atmosphere of helium at stan
ATMOSPHERE GLOW DISCHARGE PLASMA REACTOR 65 dard temperature with a separation distances of 3.0 cm
working gas = He, He + 1-7% O2, Ar, Ar - He between plates 10. The plates were charged with a 4.4
Ar + 1-7% O2, N2O and atmospheric air KV working potential. Holding these parameters con
frequency = 1 KHz to 100 KHz stant, the R.F. frequency was increased as an indepen
 9
5,414,324
10
dent variable. As the dependent variable, FIG. 11 charts been sustained by the FIG. 1 apparatus with a one atmo
the corresponding breakdown current phase angle. Sim sphere ambient air environment and 8 KV/cm R.F.
ilarly, FIG. 12 charts the total power, reactive and electric field.
plasma, used to sustain the plasma at the respective R.F. Having fully disclosed our invention, the presently
frequencies. 5 preferred embodiments and best modes of practice,
EXAMPLE 2 We claim:
1. Apparatus to generate and maintain a glow dis
In a second operational example of the invention, the charge plasma at a pressure of about 1 atmosphere, the
above described physical apparatus is used to sustain a apparatus comprising
glow discharge plasma in one atmosphere of helium at 10 a pair of electrically insulated electrodes aligned and
standard temperature with a separation distances of 1.0 secured in equidistant opposition,
cm between plates 10. In this example, the R.F. fre means for supplying and maintaining a glow dis
quency was held constant at 30 KHz while plate poten charge plasma sustaining gas at a pressure of about
tial was manipulated as the independent variable and
current breakdown phase angle, 6, (Table 2) and total 15 one atmosphere in the volumetric space between
power, P, (Table 3) measured as dependent variables. said electrodes, and
TABLE 2
radio frequency (RF) amplifier means for generating
and maintaining a glow discharge plasma by ener
V(KV)
8(deg) 28
1.5
40
2
61
2.5
46
3
65
3.5
76.5
gizing said electrodes with a potential of 1 to at
2O least 5 kV rims at 1 to 100 kHz, wherein said radio
frequency amplifier means includes an impedance
TABLE 3 matching network.
V(KV) 1.5 2 2.5 3 3.5
2. An apparatus as described in claim 1 wherein said
P(W) 7 13 22 57 50 44.9 radio frequency amplifier means for generating and
25 maintaining a glow discharge plasma comprises means
for providing an applied frequency of the RF electric
EXAMPLE 3 field which is high enough to trap the positive ions of
the plasma between the electrodes, but not so high that
A third operational example of the invention included the electrons of the plasma are also trapped during a
a one atmosphere environment of helium between a 1 half cycle of the RF voltage.
cm separation distance s between plate electrodes 10 3O 3. An apparatus as described by claim 2 which com
charged at 1.5 KV rms potential. R.F. frequency was prises means for establishing and maintaining a gas bar
manipulated as the independent variable. As a measured rier envelope surrounding said plates and the volumet
dependent variable, Table 4 reports the corresponding ric space therebetween.
phase angle e of breakdown current. The measured
dependent variable of Table 5 reports the correspond- 35 meansAnforapparatus
4. as described by claim 2 wherein said
supplying and maintaining the gas comprises
ing total power consumption data, both reactive and gas supply means to provide a substantially steady sup
plasma. ply flow of said gas.
TABLE 4 5. An apparatus as described by claim 2 wherein said
f(KHz) 10 20 30 40 50 60 70 80 90 100 40 gas is helium.
8(deg) 43 32 43 52 54 61 60 56 45 22.5 6. An apparatus as described by claim 2 wherein said
gas is a mixture of helium and air.
TABLE 5
7. An apparatus as described by claim 2 wherein said
gas is argon.
f(KHz) 10 20 30 40 50 60 70 80 90 100 45 8. An apparatus as described by claim 2 wherein said
P(W) 5 8 11 19 35 43 47 57 89 124 gas is a mixture of argon and air.
9. An apparatus as described by claim 2 wherein said
EXAMPLE 4 gas is a mixture of argon and helium.
10. An apparatus as described by claim 2 wherein said
The largest volume helium plasma of 3.1 liters was 50 gas is atmospheric air.
achieved with the above described apparatus at a 3.2 cm 11. An apparatus as described by claim 2 wherein said
plate separation having a 5KV potential charged at 4 gas is nitrous oxide.
KHZ. 12. An apparatus as described by claim 2 wherein said
It will be understood by those of ordinary skill in the electrodes are fluid cooled.
art that the present invention is capable of numerous 55 13. An apparatus as described by claim 12 wherein
arrangements, modifications and substitutions of parts fluid flow conduits are bonded to said electrodes to
without departing from the scope of the invention. In extract heat from said electrodes.
particular, FIGS. 3, 4 and 5 represent respective power 14. A method of generating and maintaining a uni
supply options having respective attractions. form glow discharge plasma at a pressure of about 1
FIGS. 3, 4 and 5 are electrical equivalents wherein atmosphere within a volumetric space between two
the T1 and T2 voltages are 180° out of phase but at only electrodes energized by radio frequency amplifier
half the maximum potential. FIG. 4 represents a means having an impedance matching network, said
grounded center top transformer whereas FIG. 5 repre method comprising the steps of operating said amplifier
sents a solid state power circuit embodiment with or means to energize said electrodes with a potential of 1
without a provision for a grounded center tap of the 65 to at least 5 kV rms at 1 to 100 kHz frequency while
output. charging and maintaining the volumetric space between
Although expansive data is not presently available, it said electrodes with a glow discharge plasma sustaining
is to be noted that a uniform glow discharge plasma has gas at approximately 1 atmosphere of pressure.
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15. The method as described in claim 14 wherein the 21. A method as described by claim 16 wherein said
uniform glow discharge plasma is generated and main gas is a mixture comprising helium and argon.
tained by using an applied frequency of the RF electric 22. A method as described by claim 15 wherein said
field which is high enough to trap the positive ions of gas is atmospheric air.
the plasma between the electrodes, but not so high that 5 23. A method as described by claim 14 wherein said
the electrons of the plasma are also trapped during a gas is nitrous oxide.
half cycle of the RF voltage. 24. A method as described by claim 15 wherein said
16. A method as described by claim 15 wherein said electrodes are positioned at a separation distance there
electrodes are enclosed by an environmental gas barrier between of 5 cm or less.
internally charged by a substantially continuous flow of 10 25. A method as described by claim 24 wherein at
said gas. least one of said electrodes is positionally adjustable
17. A method as described by claim 16 wherein said relative to the other.
gas is helium. 26. A method as described by claim 15 wherein said
18. A method as described by claim 16 wherein said amplifier frequency is variable over the range of 1 to
gas is a mixture of helium and air. 15 100 KHZ.
19. A method as described by claim 16 wherein said 27. A method as described by claim 15 wherein said
gas is argon. amplifier potential is variable over the range of 1 to at
20. A method as described by claim 16 wherein said least 5 kV rims.
gas is a mixture of argon and air. 2k xk k k k
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