Peculiarities of atomic oxygen concentration measurement by means of actinometry in negative glow plasma of low pressure discharge in oxygen
This proceeding presents results of investigations of an influence of dissociative excitation and cascading processes on precision of oxygen dissociation degree measurement in negative glow plasma of low pressure discharge by means of actinometry based on emission of O (844.6 nm) and Ar (750.4 nm) w...
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2014
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| Cite this: | Peculiarities of atomic oxygen concentration measurement by means of actinometry in negative glow plasma of low pressure discharge in oxygen / Yu.V. Lavrookevich, S.V. Matsevich, V.Yu. Bazhenov, V.V. Tsiolko // Вопросы атомной науки и техники. — 2014. — № 6. — С. 258-261. — Бібліогр.: 10 назв. — англ. |
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| author | Lavrookevich, Yu.V. Matsevich, S.V. Bazhenov, V.Yu. Tsiolko, V.V. |
| author_facet | Lavrookevich, Yu.V. Matsevich, S.V. Bazhenov, V.Yu. Tsiolko, V.V. |
| citation_txt | Peculiarities of atomic oxygen concentration measurement by means of actinometry in negative glow plasma of low pressure discharge in oxygen / Yu.V. Lavrookevich, S.V. Matsevich, V.Yu. Bazhenov, V.V. Tsiolko // Вопросы атомной науки и техники. — 2014. — № 6. — С. 258-261. — Бібліогр.: 10 назв. — англ. |
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| description | This proceeding presents results of investigations of an influence of dissociative excitation and cascading processes on precision of oxygen dissociation degree measurement in negative glow plasma of low pressure discharge by means of actinometry based on emission of O (844.6 nm) and Ar (750.4 nm) with the use of different model and calculated shapes of electron energy distribution function.
Представлены результаты исследования влияния процессов диссоциативного возбуждения и каскадирования при различных формах модельных и расчетных функций распределений электронов по энергиям на точность определения степени диссоциации кислорода в плазме отрицательного свечения разряда низкого давления методом актинометрии с использованием излучения линий О (844,6 нм) и Ar (750,4 нм).
Представлено результати досліджень впливу процесів дисоціативного збудження та каскадування при різних формах модельних та розрахункових функцій розподілу електронів за енергіями на точність визначення дисоціації кисню в плазмі негативного світіння розряду низького тиску методом актинометрії з використанням випромінювання ліній О (844,6 нм) та Ar (750,4 нм).
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ISSN 1562-6016. ВАНТ. 2014. №6(94)
258 PROBLEMS OF ATOMIC SCIENCE AND TECHNOLOGY. 2014, №6. Series: Plasma Physics (20), p. 258-261.
PECULIARITIES OF ATOMIC OXYGEN CONCENTRATION
MEASUREMENT BY MEANS OF ACTINOMETRY IN NEGATIVE
GLOW PLASMA OF LOW PRESSURE DISCHARGE IN OXYGEN
Yu.V. Lavrookevich, S.V. Matsevich, V.Yu. Bazhenov, V.V. Tsiolko
Institute of Physics NAS of Ukraine, Kyiv, Ukraine
E-mail: digit@meta.ua
This proceeding presents results of investigations of an influence of dissociative excitation and cascading
processes on precision of oxygen dissociation degree measurement in negative glow plasma of low pressure
discharge by means of actinometry based on emission of O (844.6 nm) and Ar (750.4 nm) with the use of different
model and calculated shapes of electron energy distribution function.
PACS: 52.80.-s, 52.25.Ya
INTRODUCTION
Recently oxygen plasma is widely used in different
technological processes [1, 2]. For such plasma it is
important to know atomic oxygen concentration [O],
since namely this species plays dominant role in many
practical applications. The most widely used method of
[O] measurement is actinometry [3] which is simpler in
the use and does not require expensive equipment in
comparison with other plasma optical diagnostics
methods, such as LIF or TALIF. The essence of
actinometry is adding of small amount of pre-
determined gas-actinometer (rare gases are the most
often used ones) to working gas (oxygen in our case),
and determining ratio of their concentrations using ratio
of emission intensities of certain spectrum lines of
actinometer gas and the component of interest for us. In
case of [O] measurement, the most popular is the use of
argon emission line with wavelength = 750.4 nm (2р1
1s2 transition) and oxygen line with = 844.6 nm
(3р
3
Р 3s
3
S transition). Rate of populating the levels
by electron hits is
df
m
e
K
thEe
)()(
2 ,
where Eth is threshold energy of the process, σ(ε) is the
process cross section, f(ε) is electron energy distribution
function (EEDF) with normalizing condition
1)(
0
df .
Thus we see that the precision of [O] measurements by
actinometry method is defined by proper selections of
both excitation cross sections of the processes, and the
EEDF shape. Populating Ar level (2p1) can be done both
by the only direct electron hits with cross section e
dir
(Ar, 2p1), and by combined action of electron hits and
cascading processes from upper levels with apparent
cross section e
app
(Ar, 2p1). In case of populating the
level O(3р
3
Р) the situation is somewhat more complex.
Excitation of this state can be performed both by direct
electron hit excitation of oxygen atoms (cross section
e
dir
(O, 3р
3
Р)), and due to dissociative excitation with
cross section de
dir
(O, 3р
3
Р). Similarly to excitation of
Ar atoms, taking into account cascading processes
results in the increase of excitation cross section values
for O(3р
3
Р) state up to e
app
(O, 3р
3
Р) and de
app
(O,
3р
3
Р), respectively.
In case of positive column of direct current
discharges and plasma of low pressure high-frequency
capacitive discharges, the EEDF “tail”, as compared to
Maxwellian distribution, is depleted by fast electrons
(such EEDF in many cases can be expressed as f( ) ~
exp(-k /Te), where k 1.2–1.4). In this case main role
in populating the levels is performed by direct excitation
by electrons with energy of about the excitation
threshold. Cascading processes of the populating from
upper levels play minor role since their excitation
threshold values are in a range where electron quantity
is essentially less. The same considerations essentially
regard contribution of the cascading at dissociative
excitation of O(3р
3
Р) level.
The situation becomes considerably more complex in
case of negative glow plasma (and in some cases plasma
of low pressure inductively coupled discharges). EEDF
in the plasmas of such discharges differs by the
presence of high-energy EEDF “tail” with mean
electron energy being several times higher than mean
energy of major portion of the electrons. In this case
processes of dissociative excitation and cascading can
play considerably more significant role in populating O
and Ar levels under study.
In Fig. 1 one can clearly see such difference in the
excitation processes of O and Ar levels at different
EEDF shapes. Model bi-Maxwellian EEDF with
different values of high-energy electron temperature T2
were built following from the results of experimental
measurements of plasma parameters of the hollow
cathode discharge, and calculated EEDF was obtained
using 0-D model of such discharge [4].
From this figure one can clearly see that, for correct
determining of [O] in the plasmas of discharges with
enhanced (relatively to Maxwellian distribution) content
of high-energy electrons in EEDF, one should take into
consideration all excitation processes for O and Ar
levels used in the actinometry.
Purpose of our work was an investigation of the
influence of populating O(3р
3
Р) and Ar(2р1) levels by
dissociative excitation and cascading processes on the
precision of O2 dissociation degree measurement in
ISSN 1562-6016. ВАНТ. 2014. №6(94) 259
negative glow plasma with different used model and
calculated EEDF.
0 10 20 30 40 50
1E-6
1E-4
0,01
1
1E-19
1E-18
1E-17
Energy , eV
e
dir
(Ar, 2p
1
)
e
dir
(O, 3p
3
)
e
dir
(O, 3p
3
)
C
ro
s
s
s
e
c
ti
o
n
i,
c
m
2
E
E
D
F
f
(
),
e
V
-3
/2
Fig. 1. Model bi-Maxwellian EEDF f(ε): - - T2 =
2.9 eV; - - T2 = 2.1 eV; calculated EEDF with T2 ≈
14 eV [4]; calculated EEDF of positive column
(PC) plasma in low pressure discharge [5] Direct
excitation cross sections of Ar(2p1) and O(3p
3
P) states
1. METHODS AND TECHNIQUES
Ratio of emission intensities IAr(2p1) and IO(3P) of
spectrum lines Ar(2р1) and O(3р
3
Р) enables
determining relative concentration of atomic oxygen
[5]:
P
e
P
de
pAr
POp
P
K
K
I
I
C
O
O
3
3
)12(
)3(12
3
2 ][
][
, (1)
where
]
2
[
1212
]
2
[
33
3
12
3
12
844
750
]
2
[
][12
3
O
q
p
q
K
j
p
ij
A
O
q
P
q
K
j
P
ij
A
P
e
k
p
e
k
P
A
p
A
h
h
O
Arp
P
C ,(2)
and Ke, Kde are rates of populating by direct electron hits
and dissociative populating, respectively; hνij is energy
of actinometry line emission quantum; Aij is Einstein
coefficient for respective transition; KQ is rate of
collisional quenching of excited states.
An analysis of existing up to now literature on
the cross section values was accomplished, and
selection of actual and recommended excitation cross
sections of Ar(2р1) and O(3p
3
P) levels was done which
are presented in Fig. 2 [6-10].
Apparent cross section of dissociative excitation
of O(3p
3
P) level by electron hit was taken from [7].
Direct cross section of dissociative excitation of
O(3p
3
P) level by electron hit was estimated by
subtracting the cross sections of upper state from
apparent cross section value at 100 eV energy using the
method described and applied for O(3p
5
P) level in
mentioned work.
10 20 30 40 50
1E-19
1E-18
1E-17
C
ro
ss
s
ec
tio
n
i, c
m
2
Energy , eV
Fig. 2. Excitation cross sections: -○- e (Ar 2p1), -□-
e (O, 3р
3
Р),- ∆- de (O, 3р
3
Р). Open points – direct
cross section, close points – apparent one
Direct and apparent cross sections of excitation
by electron hits for Ar(2p1) level were taken from [8].
Contribution of cascading to Ar(2p1) level population is
minimum one, as compared to the other Ar(2pх) levels,
that is why it is most often used in OES methods.
Direct cross section of O(3p
3
P) excitation by
electron hit of oxygen atom was taken from [9].
Apparent cross section of excitation of this level was
obtained by summing its direct excitation cross sections
and direct electron hit excitation cross sections of upper
levels using approach described in [7].
The quenching rates Kq
2p1
and Kq
3P
were taken
from [5].
Model EEDF used in the calculations were
created on a basis of experimental EEDF in energy
range 0…12 eV [4]. As it has been shown there, EEDF
of hollow cathode discharge plasma has bi-Maxwellian
behavior, at that temperature of “hot” ( 2 eV)
electrons T2 significantly exceeds that of “cold”
electrons T1. At 4 Pa T2 temperature increases towards
the chamber center from 2.3 eV up to 3.0 eV, and,
on the contrary, at 12 Pa decreases towards the center
from 2.1 eV down to 1.7 eV. Since it is difficult to
obtain the data on T2 at energy 12 eV by probe
technique, model EEDF were obtained by
approximation of high-energy “tails” of experimental
EEDF for T2 temperature up to 50 eV energy.
Calculated EEDF for both pressure values had
similar profiles, and temperature of electrons with
energies higher than excitation thresholds of used argon
and atomic oxygen levels T2 14 eV.
2. RESULTS AND DISCUSSIONS
From Fig.3 one can see, that ratios of rates Ke
2p1
/Ke
3P
and Kde
3P
/Ke
3P
grow up monotonously with Т2
temperature increase at the use of both direct and
apparent cross section. It should be also noted that, due
to the difference in absolute values of cross sections, the
growth of Ke
2p1
/Ke
3P
ratio does not exceed (1.5…2),
whereas Kde
3P
/Ke
3P
increases by about 10 times. At
that, use of apparent cross section decreases these ratios
by about 1.5…2 times in the whole range of T2
variations. (Smaller values of these ratios in case of use
of apparent cross sections is due to fact that e
app
(O,
260 ISSN 1562-6016. ВАНТ. 2014. №6(94)
3р
3
Р) is (2…3) times larger than e
dir
(O, 3р
3
Р)
practically in the whole range of energy , whereas the
difference between e
dir
(Ar, 2p1) and e
app
(Ar 2p1), as
well as de
dir
(O, 3р
3
Р) and de
app
(O, 3р
3
Р), is practically
absent).
1 10
0,01
0,1
T2, eV
R
at
io
K
de
3P
/K
e
3P
,
K
e
2p
1
/K
e
3P
Fig. 3. Dependencies of ratios Ke
2p1
/Ke
3P
(-□-) and
Kde
3P
/Ke
3
(-○-) on temperature T2 at the use of direct
(open points) and apparent (close points) cross sections
In calculations of dissociation degree [O]/[O2] the
dependencies of intensity ratio IO(3P)/IAr(2p1)
experimentally measured in [4] were used (Fig. 4). One
can see that at working gas pressure P = 4 Pa ratio of
spectrum line intensities IO(3P)/IAr(2p1) is higher than that
at 12 Pa pressure and slightly (about 1.3 times)
decreases with radius R increase, whereas at 12 Pa
pressure this ratio is practically independent on R.
Calculation of dissociation degree by formulas (1,2)
has shown, that at the use of model EEDF taking into
account process of dissociative excitation of O(3p
3
P)
state results in variation of dissociation degree by no
more than 5 %, and in case of calculated EEDF – no
more than 20 %. The results of [O]/[O2] calculations
presented below are obtained without taking mentioned
process into account.
Results of oxygen dissociation degree calculations
are presented in form of [O]/[O2] dependency on the
system radius in Figs. 5,a,b. In case of model EEDF,
each R value was corresponded by certain T2 value
used in the calculations of rates of the processes and
IO(3P) /IAr(2p1) ratio. In case of calculated EEDF, T2 radial
dependence was absent because of the use of 0-D
model, due to that [O]/[O2] dependencies on R are
approximate ones.
From Figs. 5a,b one can see that with the use of
model EEDF, [O]/[O2] dependencies on R for both Р
values well correlate with IO(3P) /IAr(2p1) behavior at the
use in calculation of both direct, and apparent cross
sections. In other words, in our case T2 radial
dependencies weakly influence the [O]/[O2] dependence
on R.
More interesting is an influence of used cross
sections of the processses on [O]/[O2] value.
Comparison of Fig. 5,a and Fig. 5,b shows that
substitution of direct cross section by apparent one
decreases [O]/[O2] value by about 1.5 times. Besides,
difference between [O]/[O2] values, obtained with the
0 2 4 6 8 10 12
10
12
14
16
18
R
at
io
in
te
ns
iti
es
I
O
(3
P
)
/I
A
r(
2p
1)
Radius R, cm
P = 4 Pa
P = 12 Pa
Fig. 4. Experimentally obtained dependencies of
emission intensity ratio IO(3P) /IAr(2p1) on the system
radius for two oxygen pressure values
0 2 4 6 8 10 12
0.00
0.04
0.08
0.12
0.16
0.20
0.24 a)
[O
]/
[O
2
]
R, cm
0 2 4 6 8 10 12
0,00
0,04
0,08
0,12
b)
[O
]/[
O
2]
R, cm
Fig. 5 . Dependencies of oxygen dissociation degree
[O]/[O2] on radius R for two O2 pressure values with
different EEDF. a – with the use of direct cross-section;
b – with the use of apparent cross section.
(-□-) – model EEDF with T2 = (2.3…2.9) eV,
corresponding to P = 4 Pa; (-○-) – model EEDF with
T2 = 2.1 eV, corresponding to Р = 12 Pa;
(-■-) – calculated EEDF for Р = 4 Pa;
(-● -) – calculated EEDF for Р = 12 Pa
use of model and calculated EEDF essentially decreases
at that. As it follows from expression (2) and figure 3,
main role in this effect is performed by essential (in
comparison with the other
ISSN 1562-6016. ВАНТ. 2014. №6(94) 261
processes) difference in the values of direct and
apparent excitation cross sections of O( 3р
3
Р) state.
For refining the influence of EEDF shape and
used excitation cross sections on the precision of
dissociation degree [O]/[O2] measurement in the plasma
of hollow cathode discharge, in subsequent it is planned
to perform similar researches with the use of another
pair of lines involving Ar(2p1) and O(3p
5
P) states.
REFERENCES
1. T. Gokus, R.R. Nair, et al. Making Graphene
Luminescent by Oxygen Plasma Treatment // ACS
Nano. 2009, v. 3, p. 3963-3968.
2. D.B. Graves. The emerging role of reactive oxygen
and nitrogen species in redox biology and some
implications for plasma applications to medicine and
biology // J. Phys. D: Appl. Phys. 2012, v. 45,
p. 263001.
3. J.W. Coburn and M. Chen. Optical emission
spectroscopy of reactive plasmas: A method for
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density // J. Appl. Phys. 1980, v. 51, p. 3134.
4. V.V. Tsiolko, S.V. Matsevich, et al. Kinetic processes
in negative glow plasma of low pressure discharge in
oxygen // Problems of Atomic Science and Technology.
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5. D. Pagnon, J. Amorim, et al. On the use of the use of
actinometry to measure the dissociation in 02 DC glow
discharges: determination of the wall recombination
probability // J. Phys.D: Appl. Phys. 1995, v. 28,
p. 1856-1868.
6. Y. Itikawa, A. Ichimura, et al. Cross-sections for
collisions of electron and photons with oxygen
molecules // J. Phys. Chem. Ref. Data. 1989, v. 18, № 1,
p. 23-42.
7. M.B. Schulman, F.A. Sharpton, et al. Emission from
oxygen atoms produced by electron-impact dissociative
excitation of oxygen molecules // Phys. Rev. A. 1985,
v. 32, p. 2100.
8. J.E. Chilton, J.B. Boffard, et al. Measurement of
electron-impact excitation into the 3p5 4p levels of
argon using Fourier-transform spectroscopy// Phys. Rev.
A. 1998, v. 57, p. 267-277.
9. R.R. Laher and F.R. Gilmore. Updated excitation and
ionization cross sections for electron impact on atomic
oxygen // J. Phys. Chem. Ref. Data. 1990, v. 19, p. 277.
10. M. Hayashi. Bibliography of electron and photon
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Article received 26.10.2014
ОСОБЕННОСТИ ИЗМЕРЕНИЯ КОНЦЕНТРАЦИИ АТОМАРНОГО КИСЛОРОДА В ПЛАЗМЕ
ОТРИЦАТЕЛЬНОГО СВЕЧЕНИЯ РАЗРЯДА НИЗКОГО ДАВЛЕНИЯ В КИСЛОРОДЕ МЕТОДОМ
АКТИНОМЕТРИИ
Ю.В. Лаврукевич, С.В. Мацевич, В.Ю. Баженов, В.В. Циолко
Представлены результаты исследования влияния процессов диссоциативного возбуждения и
каскадирования при различных формах модельных и расчетных функций распределений электронов по
энергиям на точность определения степени диссоциации кислорода в плазме отрицательного свечения
разряда низкого давления методом актинометрии с использованием излучения линий О (844,6 нм) и Ar
(750,4 нм).
ОСОБЛИВОСТІ ВИМІРЮВАННЯ КОНЦЕНТРАЦІЇ АТОМАРНОГО КИСНЮ В ПЛАЗМІ
НЕГАТИВНОГО СВІТІННЯ РОЗРЯДУ НИЗЬКОГО ТИСКУ В КИСНІ МЕТОДОМ АКТИНОМЕТРІЇ
Ю.В. Лаврукевич, С.В. Мацевич, В.Ю. Баженов, В.В. Ціолко
Представлено результати досліджень впливу процесів дисоціативного збудження та каскадування при
різних формах модельних та розрахункових функцій розподілу електронів за енергіями на точність
визначення дисоціації кисню в плазмі негативного світіння розряду низького тиску методом актинометрії з
використанням випромінювання ліній О (844,6 нм) та Ar (750,4 нм).
|
| id | nasplib_isofts_kiev_ua-123456789-81966 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 1562-6016 |
| language | English |
| last_indexed | 2025-12-07T17:17:53Z |
| publishDate | 2014 |
| publisher | Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
| record_format | dspace |
| spelling | Lavrookevich, Yu.V. Matsevich, S.V. Bazhenov, V.Yu. Tsiolko, V.V. 2015-05-22T20:18:00Z 2015-05-22T20:18:00Z 2014 Peculiarities of atomic oxygen concentration measurement by means of actinometry in negative glow plasma of low pressure discharge in oxygen / Yu.V. Lavrookevich, S.V. Matsevich, V.Yu. Bazhenov, V.V. Tsiolko // Вопросы атомной науки и техники. — 2014. — № 6. — С. 258-261. — Бібліогр.: 10 назв. — англ. 1562-6016 PACS: 52.80.-s, 52.25.Ya https://nasplib.isofts.kiev.ua/handle/123456789/81966 This proceeding presents results of investigations of an influence of dissociative excitation and cascading processes on precision of oxygen dissociation degree measurement in negative glow plasma of low pressure discharge by means of actinometry based on emission of O (844.6 nm) and Ar (750.4 nm) with the use of different model and calculated shapes of electron energy distribution function. Представлены результаты исследования влияния процессов диссоциативного возбуждения и каскадирования при различных формах модельных и расчетных функций распределений электронов по энергиям на точность определения степени диссоциации кислорода в плазме отрицательного свечения разряда низкого давления методом актинометрии с использованием излучения линий О (844,6 нм) и Ar (750,4 нм). Представлено результати досліджень впливу процесів дисоціативного збудження та каскадування при різних формах модельних та розрахункових функцій розподілу електронів за енергіями на точність визначення дисоціації кисню в плазмі негативного світіння розряду низького тиску методом актинометрії з використанням випромінювання ліній О (844,6 нм) та Ar (750,4 нм). en Національний науковий центр «Харківський фізико-технічний інститут» НАН України Вопросы атомной науки и техники Диагностика плазмы Peculiarities of atomic oxygen concentration measurement by means of actinometry in negative glow plasma of low pressure discharge in oxygen Особенности измерения концентрации атомарного кислорода в плазме отрицательного свечения разряда низкого давления в кислороде методом актинометрии Особливості вимірювання концентрації атомарного кисню в плазмі негативного світіння розряду низького тиску в кисні методом актинометрії Article published earlier |
| spellingShingle | Peculiarities of atomic oxygen concentration measurement by means of actinometry in negative glow plasma of low pressure discharge in oxygen Lavrookevich, Yu.V. Matsevich, S.V. Bazhenov, V.Yu. Tsiolko, V.V. Диагностика плазмы |
| title | Peculiarities of atomic oxygen concentration measurement by means of actinometry in negative glow plasma of low pressure discharge in oxygen |
| title_alt | Особенности измерения концентрации атомарного кислорода в плазме отрицательного свечения разряда низкого давления в кислороде методом актинометрии Особливості вимірювання концентрації атомарного кисню в плазмі негативного світіння розряду низького тиску в кисні методом актинометрії |
| title_full | Peculiarities of atomic oxygen concentration measurement by means of actinometry in negative glow plasma of low pressure discharge in oxygen |
| title_fullStr | Peculiarities of atomic oxygen concentration measurement by means of actinometry in negative glow plasma of low pressure discharge in oxygen |
| title_full_unstemmed | Peculiarities of atomic oxygen concentration measurement by means of actinometry in negative glow plasma of low pressure discharge in oxygen |
| title_short | Peculiarities of atomic oxygen concentration measurement by means of actinometry in negative glow plasma of low pressure discharge in oxygen |
| title_sort | peculiarities of atomic oxygen concentration measurement by means of actinometry in negative glow plasma of low pressure discharge in oxygen |
| topic | Диагностика плазмы |
| topic_facet | Диагностика плазмы |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/81966 |
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