Influence of negative ions on atomic oxygen production in a hollow cathode discharge in O₂/Ar mixture
The main mechanisms for atomic oxygen generation in a discharge with a hollow cathode in Ar/O₂ mixture were found. It was shown that for different oxygen concentrations the different reactions are responsible atomic oxygen formation. At higher oxygen concentration in the mixture negative ions play a...
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| Опубліковано в: : | Вопросы атомной науки и техники |
|---|---|
| Дата: | 2017 |
| Автори: | , , |
| Формат: | Стаття |
| Мова: | Англійська |
| Опубліковано: |
Національний науковий центр «Харківський фізико-технічний інститут» НАН України
2017
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| Цитувати: | Influence of negative ions on atomic oxygen production in a hollow cathode discharge in O₂/Ar mixture / Yu. Lavrukevich, A. Ryabtsev, V. Tsiolko // Вопросы атомной науки и техники. — 2017. — № 1. — С. 215-218. — Бібліогр.: 14 назв. — англ. |
Репозитарії
Digital Library of Periodicals of National Academy of Sciences of Ukraine| _version_ | 1860082293686665216 |
|---|---|
| author | Lavrukevich, Yu. Ryabtsev, A. Tsiolko, V. |
| author_facet | Lavrukevich, Yu. Ryabtsev, A. Tsiolko, V. |
| citation_txt | Influence of negative ions on atomic oxygen production in a hollow cathode discharge in O₂/Ar mixture / Yu. Lavrukevich, A. Ryabtsev, V. Tsiolko // Вопросы атомной науки и техники. — 2017. — № 1. — С. 215-218. — Бібліогр.: 14 назв. — англ. |
| collection | DSpace DC |
| container_title | Вопросы атомной науки и техники |
| description | The main mechanisms for atomic oxygen generation in a discharge with a hollow cathode in Ar/O₂ mixture were found. It was shown that for different oxygen concentrations the different reactions are responsible atomic oxygen formation. At higher oxygen concentration in the mixture negative ions play a significant role in the formation of atomic oxygen. This property of the discharge is due to the low electric field in the working volume, and consequently low electron temperature.
Выявлены основные механизмы генерации атомарного кислорода в разряде с полым катодом в смеси O₂/Ar. Было показано, что при различных концентрациях кислорода в разряде за образование атомарного кислорода отвечают различные реакции. При высокой концентрации кислорода в смеси в формировании атомарного кислорода играют значительную роль негативные ионы. Это свойство разряда обусловлено низким значением электрического поля в рабочем объёме, а следовательно, низкой электронной температурой.
Виявлено основні механізми генерації атомарного кисню в розряді з порожнистим катодом в суміші O₂/Ar. Було показано, що при різних концентраціях кисню в розряді за утворення атомарного кисню відповідають різні реакції. При високій концентрації кисню в суміші у формуванні атомарного кисню відіграють значну роль негативні іони. Ця властивість розряду зумовлена низьким значенням електричного поля в робочому об'ємі, а отже, низькою електронною температурою.
|
| first_indexed | 2025-12-07T17:17:36Z |
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| fulltext |
ISSN 1562-6016. ВАНТ. 2017. №1(107)
PROBLEMS OF ATOMIC SCIENCE AND TECHNOLOGY. 2017, № 1. Series: Plasma Physics (23), p. 215-218. 215
INFLUENCE OF NEGATIVE IONS ON ATOMIC OXYGEN
PRODUCTION IN A HOLLOW CATHODE DISCHARGE IN O2/Ar
MIXTURE
Yu. Lavrukevich, A. Ryabtsev, V. Tsiolko
Institute of Physics NAS of Ukraine, Kiev, Ukraine
E-mail: rybtsev@iop.kiev.ua
The main mechanisms for atomic oxygen generation in a discharge with a hollow cathode in Ar/O2 mixture were
found. It was shown that for different oxygen concentrations the different reactions are responsible atomic oxygen
formation. At higher oxygen concentration in the mixture negative ions play a significant role in the formation of
atomic oxygen. This property of the discharge is due to the low electric field in the working volume, and
consequently low electron temperature.
PACS: 52.80. Dy, 52.25.Dg, 52.25.Ya
INTRODUCTION
Discharges in oxygen are widely used in plasma
technology, such as etching, deposition of protective
films, surface modification and others [1-3]. In many
industrial gadgets discharges are used not in pure
oxygen but in a mixture of oxygen with an inert gas,
especially argon, which allows to increase the
effectiveness of such devices. One of the most
widespread discharges for generation of active particles
at low pressure is the discharge with a hollow cathode,
which allows obtaining a high yield of such particles at
low power cost. A distinctive feature of this discharge is
a small electric field in the working volume, and as a
consequence, low electron temperature. It was found in
experiments [4] that in such discharges the atomic
oxygen concentration has substantially nonmonotonic
dependence on the composition of the mixture with a
minimum at about equal content of argon and oxygen.
In the current paper, based on the features of the
discharge with the hollow cathode, the main
mechanisms responsible for the formation of atomic
oxygen at different compositions were founded up, and
the influence of other plasma components such as
negative oxygen ions was established.
1. THEORETICAL MODEL
For calculations of dependencies of plasma
component concentrations on the gas mixture content,
averaged model of plasma-chemical processes in hollow
cathode discharge was built. The model was mainly
analogous to one considered in [1]. We assumed that the
component concentrations are uniformly spread over the
whole volume of the chamber represented by cylinder
with radius R = 19 cm and length L = 40 cm.
In the kinetics calculations we considered 18
components. For oxygen, the following species were
considered: molecular oxygen in both ground state
O2(X
3
Σg), and in excited metastable states O2(a
1
g),
O2(b
1
Σg
+
) and O2(A
3
Σu
+
, A
3
Δu, c
1
Σu
-
); atomic oxygen
ground state O(
3
P) and at metastable level O(
1
D); ozone
O3, as well as positive ions O
+
and O2
+
, and negative
ions O
-
, O2
-
and O3
-
. Argon atoms were considered as
the following species: the ground state Ar(3s
2
3p
6
),
metastable levels Ar
m
(mixture of 1s5 and 1s3 levels with
fixed ratio of 5:1), radiation-bounded levels Ar
r
(1s2 and
1s4 levels), all levels Ar(4p), as well as Ar
+
ions. Totally,
in the calculations 131 elementary processes were taken
into consideration. Rate constants for all reactions were
taken the same as in [5], excluding reactions of oxygen
dissociation and ionization, argon ionization in ground
and metastable states, as well as reactions of excitation
of electron levels of molecular oxygen and argon.
Mentioned constants were determined from electron
energy distribution function (EEDF) which was
obtained by solving Boltzmann equation, which was
solved together with the system of kinetic equations.
The EEDF f(ε) was normalized as follows:
. (1)
At solving this equation, electron energy losses to
ionization of molecular oxygen and argon, oxygen
dissociation, excitation of the first seven electron levels
of molecular oxygen, argon levels 1s and 2p (including
stepwise excitation 1s → 2p), and oxygen oscillation
levels were taken into account. Electron heating was
done by electric field, as well as at the expense of
“secondary” electrons formed at the gas ionization by
electrons accelerated in the near-cathode layer. The
dependence of energy distribution of these “secondary”
electrons was considered to be proportional to
1/(ε
2
+ ε0
2
), where ε0 is ionization energy. The density of
these “secondary” electrons was determined from
specific power density introduced into the discharge,
which was supposed to be about 11 mW/cm
3
. Cross
section values for electron processes used for
calculations of rate constants, as well as EEDF
calculation, were taken from [6-11].
To show an influence of a low electric field on the
discharge the calculations were done for two values.
One was produced for E = 20 mV/cm, which is close to
the field which observed at an experiments, and other
for greater value E = 100 mV/cm. Fig. 1 shows the
estimates for the EEDF to these field values, depending
on the Ar contribution to the working mixture.
For the reactions with electrons for which cross-
section are unknown we used dependences of rate
constants on electron temperature. As a temperature we
chose 2/3 of the calculated average electron energy.
Fig. 2 shows dependence of the temperature on the
mixture composition for two values of the electric field.
216 ISSN 1562-6016. ВАНТ. 2017. №1(107)
0 5 10 15 20 25 30
10
-6
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
f(
),
(
e
V
-3
/2
)
, (eV)
0
20
50
80
95
100
b
Fig. 1. EEDF for various compositions of the discharge
mixture, the numbers indicate the percentage of Ar;
a – E = 20 mV/cm; b – E = 100 V/cm
0 10 20 30 40 50 60 70 80 90 100
0.0
0.5
1.0
1.5
2.0
2.5
3.0
3.5
1
2
T
e
,
(e
V
)
Ar, (%)
Fig. 2. The dependence of the electron temperature of
the Ar content in the discharge mixture:
1 E = 20 mV/cm; 2 E = 100 mV/cm
2. RESULTS AND DISCUSSIONS
Fig. 3 shows the dependence of the calculated
concentration of atomic oxygen on the composition of
the discharge mixture for the two values of the electric
field. And Fig. 4 shows the same data obtained by an
experiment for discharge with hollow cathode for which
the value of the electric field was close to 20 V/cm. One
should note the similarity of the shape of experimental
and calculated curves for similar values of the electric
field – the minimum in the atomic oxygen concentration
at about 50 % presence of Ar in the mixture, and
increasing in the atomic concentration while portion of
oxygen in initial mixture both increases and decreases.
0 10 20 30 40 50 60 70 80 90 100
0
1x10
13
2x10
13
3x10
13
4x10
13
1
2
[O], (cm
-3
)
Ar, (%)
Fig. 3. Calculated dependence of the atomic oxygen
concentration on the composition of the mixture:
1 E = 20 mV/cm; 2 E = 100 mV/cm
0 10 20 30 40 50 60 70 80 90 100
0
2x10
13
4x10
13
6x10
13
8x10
13
1x10
14 [O], (cm
-3
)
Ar, (%)
Fig. 4. Experimental dependence of the atomic oxygen
concentration on the mixture composition
The most effective oxygen dissociation mechanism
is the reaction of direct dissociation by electron impacts:
e + O2 e + O + O. (2)
But due to the fact that the threshold energy of
oxygen dissociation (6 eV) is less than the ionization
energy of argon (15.8 eV), there is a "stabilization"
mechanism for the electron impact dissociation rate in
the plasma. This "stabilization" is expressed in the fact
that when more oxygen is present in the discharge, the
portion of electrons with energy greater than 6 eV
becomes smaller, because of effective energy losses in
the dissociation and ionization collisions of electrons
with oxygen molecules. Consequently, the rate constant
of reaction (2) which is defined as
, (3)
will be inversely proportional to the oxygen
concentration (where q and m are charge and mass of an
electron, and d( ) is a cross section of dissociation).
And, therefore, the speed of the reaction (2), which is
equal to kd [O2] ne, will remain nearly constant.
Fig. 5 shows the dependence of the rate constant and
the reaction rate itself on the composition of the
discharge mixture. And indeed, as expected, when the
oxygen concentration changes from 100 to 10 %
0 5 10 15 20 25 30
10
-6
10
-5
10
-4
10
-3
10
-2
10
-1
10
0
f(
),
(
e
V
-3
/2
)
, (eV)
0
20
50
80
95
100
a
ISSN 1562-6016. ВАНТ. 2017. №1(107) 217
Fig. 5. The rate constant for oxygen dissociation (solid
curves, right axis) and the rate of direct dissociation
reaction (dashed lines, left axis); electric field
E = 100 mV/cm
the rate constant increases ten times, but the reaction
rate itself remains substantially constant or, in some
other cases decreases no more than 2…3 times.
Therefore, we need additional mechanisms of atomic
oxygen formation, different for different mixture
compositions. In the case of small oxygen
concentrations and, consequently relative high electron
temperature, such mechanisms may be the dissociation
of metastable levels of oxygen
c
1
u
-
) The cross
sections for the excitation of these states are the order of
magnitude smaller than for the reaction of dissociation.
Also electron energy loss in such collisions (0.98, 1.64
and 4.5 eV, respectively) are smaller than for
dissociation and ionization, so these processes do not
have a significant influence on the EEDF. Thus, with
decreasing of [O2] concentration the rate constants of
these reactions grow slower than 1/[O2], and the
concentrations of metastable oxygen molecules have
maximum, the positions of which depend on the electric
field in the discharge (Fig. 6). As a result dissociations
of metastable molecules are responsible for an increase
in the degree of dissociation of oxygen while reducing
its portion in the discharge.
As mentioned above, a discharge with a hollow
cathode is characterized by low electric field in the main
discharge volume and therefore low average electron
energy. At high oxygen concentrations, the electron
temperature may have a value less than 1 eV (see
Fig. 2). These conditions are favorable for the formation
and preservation of negative oxygen ions, as the
electron affinity of oxygen molecule is 0.87 eV.
Fig. 7 shows the rate of atomic oxygen formation for
the mane reactions. Since loss of atomic oxygen is
proportional to its concentration, the result of
summation of these curves represents, up to a factor, the
desired concentration. It can be seen that the
contribution of the dissociation of oxygen molecules in
the ground state is weakly dependent on the oxygen
content in the mixture. Because recombination rate of
the positive and negative ions is proportional to their
concentrations, which in turn are proportional to the
concentration of neutral molecules, as a result, the rate
of this reaction has the quadratic dependence. The
contribution to the overall atomic oxygen formation
from the recombination reaction decreases with
increasing of electric field. On the contrary, the value of
the metastable atom concentration increases with the
electric field, but the maximum production rate of the
respective reactions becomes broader and shifts toward
higher concentrations of oxygen.
From our point of view, the discrepancy between the
results of numerical simulation and experiment can be
explained by shortcomings in consideration of processes
at walls. First of all, a great variation of a value for
recombination coefficient of oxygen at walls exists in
the literature [12-14]. These values vary from 0.05 to
0.001 (we have used value 0.05). Moreover, all these
values relate to cold walls, but under conditions of a
discharge with a hollow cathode when a wall being
bombarded by ions, this coefficient may be even less.
Since recombination at walls is one of the main
mechanisms of atomic oxygen departure, the decrease in
this constant may result in a corresponding increase in
the atomic concentration in the discharge. Secondly, we
do not have confidence in the accuracy of accounting of
negative ions departure from the discharge volume.
However, these corrections may only affect the specific
value, but not the general form of dependency.
0 10 20 30 40 50 60 70 80 90 100
0.0
5.0x10
12
1.0x10
13
1.5x10
13
2.0x10
13
2.5x10
13
3.0x10
13
3.5x10
13
4.0x10
13
N, (cm
-3
)
Ar, (%)
1
2
3
4
0 10 20 30 40 50 60 70 80 90 100
0.0
1.0x10
13
2.0x10
13
3.0x10
13
4.0x10
13
5.0x10
13
6.0x10
13 N, (cm
-3
)
Ar, (%)
1
2
3
4
Fig. 6. The dependence of concentration of metastable
oxygen molecules and negative ions on the mixture
composition: a – electric field E = 20 mV/cm;
b – E = 100 mV/cm; 1 – O2(a
1
g); 2 – O2(b
1
g
+) multiplied
by 10; 3 – O2(A
3
u
+, A3
u, c
1
u
-) multiplied by 10;
4 – O2
- multiplied by 200
0 10 20 30 40 50 60 70 80 90 100
0.0
2.0x10
-10
4.0x10
-10
6.0x10
-10
8.0x10
-10
1.0x10
-9
1.2x10
-9
1.4x10
-9
k
d
, (cm
3
/s)
Ar, (%)
0.0
5.0x10
13
1.0x10
14
1.5x10
14
2.0x10
14
2.5x10
14
k
d
[O
2
] n
e
, (cm
-3
s
-1
)
a
b
218 ISSN 1562-6016. ВАНТ. 2017. №1(107)
0 10 20 30 40 50 60 70 80 90 100
0
1x10
14
2x10
14
3x10
14
4x10
14
5x10
14
6x10
14
Ar, (%)
1
2
3
4
5
Rates, (cm
-3
s
-1
)
0 10 20 30 40 50 60 70 80 90 100
0
1x10
14
2x10
14
3x10
14
4x10
14
5x10
14
6x10
14
Ar, (%)
1
2
3
4
5
Rates, (cm
-3
s
-1
)
Fig. 7. The rate of formation of atomic oxygen in a
variety of reactions: a – E =20 mV/cm;
b – E = 100 mV/cm.
1 dissociation of the ground state; 2 recombination
of positive and negative molecular ions;
3 dissociation of the metastable level of O2(a
1
g);
4 dissociation of the metastable level of O2(b
1
g
+);
5 dissociation of metastable levels
of O2(A
3
u
+, A3
u, c
1
u
-)
CONCLUSIONS
It was shown that at low argon content in the
working mixture of a hollow cathode discharge, the
negative oxygen ions play a significant role in the
atomic oxygen formation.
It was found that this feature of a hollow cathode
discharge is obliged to lower value of the electric field
in the volume and hence a low electron temperature.
The calculated dependences are in the good agreement
with the experimental data.
This work was supported in part by the program of
NASU "Prospective research in plasma physics, nuclear
fusion and plasma technologies" in the 2014-2016 years.
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Article received 12.10.201
ВЛИЯНИЕ ОТРИЦАТЕЛЬНЫХ ИОНОВ НА ПРОИЗВОДСТВО АТОМАРНОГО КИСЛОРОДА
В РАЗРЯДЕ С ПОЛЫМ КАТОДОМ НА СМЕСИ O2/Ar
Ю. Лаврукевич, А. Рябцев, В. Циолко
Выявлены основные механизмы генерации атомарного кислорода в разряде с полым катодом в смеси O2/Ar.
Было показано, что при различных концентрациях кислорода в разряде за образование атомарного кислорода
отвечают различные реакции. При высокой концентрации кислорода в смеси в формировании атомарного
кислорода играют значительную роль негативные ионы. Это свойство разряда обусловлено низким значением
электрического поля в рабочем объёме, а следовательно, низкой электронной температурой.
ВПЛИВ НЕГАТИВНИХ ІОНІВ НА ВИРОБНИЦТВО АТОМАРНОГО КИСНЮ В РОЗРЯДІ
З ПОРОЖНИСТИМ КАТОДОМ НА СУМІШІ O2/Ar
Ю. Лаврукевич, А. Рябцев, В. Циолко
Виявлено основні механізми генерації атомарного кисню в розряді з порожнистим катодом в суміші
O2/Ar. Було показано, що при різних концентраціях кисню в розряді за утворення атомарного кисню
відповідають різні реакції. При високій концентрації кисню в суміші у формуванні атомарного кисню
відіграють значну роль негативні іони. Ця властивість розряду зумовлена низьким значенням електричного
поля в робочому об'ємі, а отже, низькою електронною температурою.
|
| id | nasplib_isofts_kiev_ua-123456789-122154 |
| institution | Digital Library of Periodicals of National Academy of Sciences of Ukraine |
| issn | 1562-6016 |
| language | English |
| last_indexed | 2025-12-07T17:17:36Z |
| publishDate | 2017 |
| publisher | Національний науковий центр «Харківський фізико-технічний інститут» НАН України |
| record_format | dspace |
| spelling | Lavrukevich, Yu. Ryabtsev, A. Tsiolko, V. 2017-06-28T05:34:16Z 2017-06-28T05:34:16Z 2017 Influence of negative ions on atomic oxygen production in a hollow cathode discharge in O₂/Ar mixture / Yu. Lavrukevich, A. Ryabtsev, V. Tsiolko // Вопросы атомной науки и техники. — 2017. — № 1. — С. 215-218. — Бібліогр.: 14 назв. — англ. 1562-6016 PACS: 52.80. Dy, 52.25.Dg, 52.25.Ya https://nasplib.isofts.kiev.ua/handle/123456789/122154 The main mechanisms for atomic oxygen generation in a discharge with a hollow cathode in Ar/O₂ mixture were found. It was shown that for different oxygen concentrations the different reactions are responsible atomic oxygen formation. At higher oxygen concentration in the mixture negative ions play a significant role in the formation of atomic oxygen. This property of the discharge is due to the low electric field in the working volume, and consequently low electron temperature. Выявлены основные механизмы генерации атомарного кислорода в разряде с полым катодом в смеси O₂/Ar. Было показано, что при различных концентрациях кислорода в разряде за образование атомарного кислорода отвечают различные реакции. При высокой концентрации кислорода в смеси в формировании атомарного кислорода играют значительную роль негативные ионы. Это свойство разряда обусловлено низким значением электрического поля в рабочем объёме, а следовательно, низкой электронной температурой. Виявлено основні механізми генерації атомарного кисню в розряді з порожнистим катодом в суміші O₂/Ar. Було показано, що при різних концентраціях кисню в розряді за утворення атомарного кисню відповідають різні реакції. При високій концентрації кисню в суміші у формуванні атомарного кисню відіграють значну роль негативні іони. Ця властивість розряду зумовлена низьким значенням електричного поля в робочому об'ємі, а отже, низькою електронною температурою. This work was supported in part by the program of NASU "Prospective research in plasma physics, nuclear fusion and plasma technologies" in the 2014-2016 years. en Національний науковий центр «Харківський фізико-технічний інститут» НАН України Вопросы атомной науки и техники Низкотемпературная плазма и плазменные технологии Influence of negative ions on atomic oxygen production in a hollow cathode discharge in O₂/Ar mixture Влияние отрицательных ионов на производство атомарного кислорода в разряде с полым катодом на смеси O₂/Ar Вплив негативних іонів на виробництво атомарного кисню в розряді з порожнистим катодом на суміші O₂/Ar Article published earlier |
| spellingShingle | Influence of negative ions on atomic oxygen production in a hollow cathode discharge in O₂/Ar mixture Lavrukevich, Yu. Ryabtsev, A. Tsiolko, V. Низкотемпературная плазма и плазменные технологии |
| title | Influence of negative ions on atomic oxygen production in a hollow cathode discharge in O₂/Ar mixture |
| title_alt | Влияние отрицательных ионов на производство атомарного кислорода в разряде с полым катодом на смеси O₂/Ar Вплив негативних іонів на виробництво атомарного кисню в розряді з порожнистим катодом на суміші O₂/Ar |
| title_full | Influence of negative ions on atomic oxygen production in a hollow cathode discharge in O₂/Ar mixture |
| title_fullStr | Influence of negative ions on atomic oxygen production in a hollow cathode discharge in O₂/Ar mixture |
| title_full_unstemmed | Influence of negative ions on atomic oxygen production in a hollow cathode discharge in O₂/Ar mixture |
| title_short | Influence of negative ions on atomic oxygen production in a hollow cathode discharge in O₂/Ar mixture |
| title_sort | influence of negative ions on atomic oxygen production in a hollow cathode discharge in o₂/ar mixture |
| topic | Низкотемпературная плазма и плазменные технологии |
| topic_facet | Низкотемпературная плазма и плазменные технологии |
| url | https://nasplib.isofts.kiev.ua/handle/123456789/122154 |
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