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'
si si
i
c n =C
(1)
Equation (1) expresses the mass conservation of the elements;
'
si
n is the amount of species i containing
the element s in the plasma,
si
c is the stoichiometric coefficient of the element s appearing in the species i, and
C is the total amount of elements.
Daltons Law:
i h e e
i e
P+P= n kT +n kT
w
=
2
3
1
0
1
P=
24
i
w
i
i
d
Z n
c t =
(2)
Equation (2) represents Daltons Law taking into account the Coulomb field modification; P and P are
respectively the gas pressure and pressure correction resulted from the charged particles interactions
22
. The
latter, which should be taken account of for non-LTE plasmas, was neglected in previous studies
1
.
d
is the
Debye length defined later and w the number of species in the system. k is Boltzmann constant,
0
c the
vacuum permittivity, Z
i
and
i
n respectively the charge number and number density of species i, and T
e
and
T
h
the electron and heavy-particle temperatures respectively.
Electrical quasi-neutrality:
' '
t t e
t
Z n -n =0 (3)
Equation (3) describes electrical quasi-neutrality in the plasma;
t
Z and
'
t
n are respectively the charge
number and number density of the charged species t.
The law of mass action:
int
I,r+1 I,r+1 3/2 e r+1 e e r+1
int 2
r ex r
E -E n n 2m kT Q
=2 ( ) exp(- )
n kT Q h
(
(
(4)
int int
3 2 d A B A B A B h
int 2
AB ex AB AB
E n n Q Q 2m m kT
= ( ) exp(- )
n kT Q m h
(5)
Equations (4) and (5) are respectively the Saha and GulbergWaages equations, which describe ionization
6
(
z+ (z+1)+
A A +e ) and dissociation reactions ( AB A+B ) in the form proposed by the van de Sanden et
al.
22-24
.
int
i
Q and h are the internal partition function of species i and the Planck constant. The subscript
r
indicates r-times ionized species or molecules. AB, A, and B respectively denote the reactant and the two
products of the dissociation chemical reactions, and
ex
T is the excitation temperature of the relevant chemical
reaction. The energies of formation and reaction excitation temperatures relevant to nitrogen plasmas are given
in table I.
It is assumed that translational, rotational and vibrational motions of the heavy species are governed by
h
T ,
but electronic excitation and translational motion of the electrons are described by
e
T . Hence, the partition
functions are as follows
22
:
Monatomic species
int el
i i e
Q Q (T ) = (6)
where
el
i e
Q (T ) is the electron internal partition function of species i .
Diatomic and polyatomic species
int el vib rot
i i e i h i h
Q Q (T ) *Q (T ) *Q (T ) = (7)
where
vib
i h
Q (T ) ,
rot
i h
Q (T ) are, respectively, the vibrational and rotational partition functions of species i .
TABLE I. Chemical reaction energy changes and the reaction excited temperature.
Chemical reaction Energy (kJ/mol) Reaction excited temperature T
ex
2
N N+N
941.6 T
h
+
2 2
N N +e
1509.5 T
h
+
N N +e 1402.3 T
e
+ ++
N N +e 2856.0 T
e
++ +++
N N +e 4578.1 T
e
+++ ++++
N N +e 7475.0 T
e
The lowering of the ionization energy is taken into account using the following expression:
7
2
I,r+1
0 d
e 1
E =(r+1)
4
(8)
where
d
is the Debye length representing the shielding effect of charged particles. It can be seen from Equation
(8) that the ionization potential lowering is inversely proportional to the Debye length. Different methods are
used to calculate
d
in the literature. Aubreton et al.
19
and Colombo et al.
20
both only consider the shielding
effects of electrons, which have much smaller mass and higher velocities than heavy particles. The Debye length
taking into account the shielding effects of both ions and electrons has the form:
d
2 2
-2 e t t
t=1,t e
0 e h
n z n e
= +
k T T
w
=
(
(
(9)
The second term in the brackets is neglected when only the shielding effects of electons is considered.
Equation (9) implies that ions play an equally or even more important role in lowering the ionization
potential in a two-temperature plasma. A comparison will be given in section 5 to show the non-negligible
influence of Debye shielding in calculating the thermodynamic and transport properties.
Unless specifically noted, only the shielding effect of the electrons is included in the Debye length
d
, in
order to allow comparison with the work of Aubreton et al.
19
and Colombo et al.
20
.
A. Evaluation of Partition Functions
The partition function of a species, which establishes the link between the coordinates of microscopic
systems and macroscopic thermodynamic properties, is the product of its translational and internal partition
functions. The translation of particles is of a continuous nature while the internal states are of discrete nature.
The translational partition function of species i can be obtained by integration over all spatial and momentum
coordinates to give
tr 3/2 i i
i
2
2m kT
Q =( ) V
h
(10)
where V is the volume of the system and m
i
the mass of species i.
8
The internal partition functions for monatomic species consist of the summation over all possible energy
levels
n
c up to effective ionization energy
ieff
E .
n ieff
n e
<E
- /kT int e
i i e n
n
Q Q (T )= g e =
(11)
Fundamental atomic data on energy levels and degeneracy (statistical weight) are obtained from Moore
25
and the most recent data of NIST
26
. The contribution from energy levels whose data are partially known or
completely unknown has also been taken into account using a method similar to that described by Milone and
Merlo
27
. The contribution of partially-known states was accounted for using information about their
neighboring levels, and that of the completely unknown levels, usually with high principal quantum numbers,
was estimated using the hydrogenic approximation based on the last principal quantum number. The calculation
was performed with an upper limit on the quantum number of n = 1000. The calculation stops when the lowered
ionization energy is reached. The lowering of ionization energy depends strongly on temperature, which
influences the choice of the cut-off value of the quantum numbers used in the calculation of the partition
functions. In order to minimize the discontinuities in the numerical derivatives of the partition functions, the
overlapping of the sub-groups of energy levels characterized by consecutive principal quantum numbers is
taken into account, following Ref. 28. A similar approach was adopted by Colombo et al.
20
. However, they did
not take into account the contribution of the different multiple excited states (core excited electronic states),
which correspond to the different electronic configurations of the corresponding ions. The energy states of the
nitrogen atom, the associated degeneracy, and the ionization limits used in the present work are taken from Ref.
27 and given in table II.
TABLE II. States of the atoms considered in our calculation of the internal partition function of nitrogen atom
atom Elec.
Config.
Ground
State
Excited States Ionization potential
ion
[cm
-1
]
1s
2
2s
2
2p
2
(
3
P)nx(3) 1173450.0
9
N
1s
2
2s
2
2p
3
4
S
o
3/2
(
2
DP
o
) 1s
2
2s
2
2p
2
(
1
D)nx(3) 132660.7
1s
2
2s
2
2p
2
(
1
S)nx(3) 150032.1
1s
2
2s2p
4
4
P
5/2
(
2
DPS)
*
1s
2
2s2p
3
(
5
S
o
)nx(3) 164512.7
1s
2
2s2p
3
(
3
D
o
)nx(3) 209582.9
1s
2
2s2p
3
(
2
P
o
)nx(3) 226563.2
For a diatomic or polyatomic molecule, the internal partition functions can be expressed as follows
max max
el
int *
i e e vib h rot h
e
1
Q = g exp(- /kT ) exp(- ( )/kT ) (2 1)exp(- ( )/kT )
v J
v J c
v J v
u
+
(12)
with the vibration energy of the v-th vibrational state and J-th electronic state computed as
2 3 4
( ) 1 1 1 1
( ) ( ) ( ) ( )
hc 2 2 2 2
vib
e e e e e e e
v
v x v y v z v
c
e e e e = + + + + + +
2
( )
( 1) ( ( 1))
hc
rot
v v
J
B J J D J J
c
= + +
where ( )
vib
v c is the vibrational energy of the th v vibrational state and ( )
rot
J c the rotational energy of the
th J rotational state,
c
u a symmetry factor, v and J the vibrational and rotational quantum number respectively,
and other parameters are spectroscopically-determined constants obtained from Refs. 29 - 30. In equation
(11), the quantity
el
c
-
instead of
el
c is used to represent the energy levels proposed by Bacri et al
28
. This takes
into account that the potential energy of the fundamental level (v = 0, J = 0) of the ground configurations should
be set to zero and this leads to a negative equivalent electronic energy term
0
(1/ 2) (1/ 4)
el e e e
x c e e
-
= + (13)
Note that the difference between
el
c and
el
c
-
can lead to significant modifications to the values of the
internal partition functions of diatomic molecules at low temperatures, as can be seen in figure 1 for the nitrogen
molecular and molecular ion in the LTE state, in which our results are compared with those of Drellishak et al.
31
,
who used
el
c . The deviation at high temperature is due to different numbers of molecular spectral states used in
the calculation.
10
FIG.1. Temperature dependence of internal partition functions of nitrogen molecular and its ion
B. Determination of Plasma Composition
Electrostatic interaction between charged particles affects the equation of state [see Eq. (2)], and the
lowering of the ionization potential in turn influences the generalized Saha equation. This is because the cut-off
of spectral states in the calculation of the partition functions depends on the lowering of the species ionization
potential, which is a function of the Debye length [see Eq. (9)]. This mechanism has been taken into account to
ensure rigorous calculations in an iterative procedure developed in the present work.
11
FIG.2. Numerical computation flow chart
.
The iterative solution for the particle densities at a given temperature, temperature ratio and pressure for
both LTE and non-LTE plasmas is represented by the flow chart in figure 2. The process starts with the
calculation of the first set of plasma composition based on the ground state only. This provides an initial
guessed solution for the iterative computation. The partition function values, the lowered values of the
ionization potential, and the nonlinear equation expression corrections are updated and NewtonRaphson
method is adopted for iterations until convergence of the plasma composition is obtained.
III. DETERMINATION OF THERMODYNAMIC PROPERTIES
After obtaining the partition functions of each nitrogen species, the calculation of the thermodynamic
12
properties proceeds in a straightforward manner, employing the following standard thermodynamic
relationships.
Mass density:
v
i i
i=1
= m n
(14)
where
i
m is the mass of species i.
Internal energy:
int
2 i
i i i i i i
i i i i
lnQ 3 k 1 k
e= n T + n E + n T
2 T
c
c
(15)
where
i
E is the formation energy of species i.
Enthalpy:
int
2 i
i i i i i i
i i i
l nQ 5 k 1 k
h= n T + n E + n T
2 T
i
c
c
(16)
Specific heat at constant pressure:
p
e
h
C
T
c
=
c
(17)
IV. TRANSPORT COEFFICIENTS AND COLLISION INTEGRALS
A. Determination of Transport Coefficients
Transport properties, namely diffusion coefficients, viscosity, thermal conductivities and electrical
conductivity, are calculated approximately using the classical ChapmanEnskog method, which assumes that
the particle distribution function is a first-order perturbation to the Maxwellian distribution
32-34
.
Up to now there are two approaches to deal with the transport properties in plasma. Devoto
35
and
Bonnefoi
36
developed a simplified theory neglecting the collisional coupling between heavy species and
electron. Rat et al.
37-39
proposed a theory to take into account the coupling between heavy species and electron
13
that resulted in a set of new expressions for transport coefficients and coupling terms in the mass, momentum
and energy flux definitions.
It should, however, be noted that a recent study of non-LTE transport properties based on a comparison of
the approaches of Devoto and Rat et al. shows that coupling between electrons and heavy species does not lead
to significant changes in the predicted non-equilibrium plasma transport properties, except for certain ordinary
diffusion coefficients
40
. No significant discrepancies occur in the total thermal conductivity (including the
reactive contribution), viscosity or electrical conductivity, even when they depend on the ordinary diffusion
coefficients. Besides, at high temperatures when ionization processes dominate in the mixture, the third-order
approximation for thermal conductivity and second-order approximation for viscosity are required to provide
calculation accuracy of 1%. Consequently, we have used the simplified approach of Devoto with a third-order
approximation for transport properties, except for viscosity for which the second-order approximation has been
adopted.
Thermal conductivity depends not only on the translation of the particles. but also is affected by processes
related to the internal energy changes and chemical reactions. Chemical reactions (namely dissociation,
ionization and recombination) lead to an additional heat flux. This introduces an additional reactive thermal
conductivity component
re
. An expression for the reactive thermal conductivity of high temperature gases and
their mixtures
42
, which follows the Vant Hoff equations modified to reflect the nature of two-temperature
plasmas
41
for monatomic gases, is used in this work.
The presence of internal degrees of freedom can affect the heat flux vector, and gives rise to an internal
thermal conductivity
in
, which has been derived using the HirschfelderEucken approximation as follows
43
:
1
int
/ ( 2.5 ) ( )
w w
j
ii
ii h pi
i e j e i ij
x
D
PD RT C R
x D
= =
=
(18)
14
where C
pi
is the specific heat at constant pressure of the species i, D
ii
and D
ij
respectively the self-diffusion
coefficient and the binary diffusion coefficient between species i and species j. R, Px
i
, and w respectively
denote the molar gas constant, pressure , mole fraction of species i, and the total number of species.
B. Evaluation of collision integrals
The complicated combinations of bracket integrals, which appear in the expressions for the transport
coefficients, can be represented as linear combinations of the collision integrals, which are defined as follows
32-34
:
( , ) 2 2 3
0
exp( ) ( )
2
ij l s s l
ij ij ij ij ij
ij
kT
Q g d
t
-
+
O =
}
(19)
The transport cross sections ( )
l
ij
Q g [see Eq. (19)] are defined by
0
( ) 2 (1 cos )
l l
ij
Q g bdb t _
=
}
(20)
where b is the impact parameter.
ij
and
ij
T
-
are the reduced mass and the reduced temperature of the
colliding molecules i and j , respectively given by
1 1 1
ij i j
m m
= + (21)
i j j i
ij
i j
mT m T
T
m m
-
+
=
+
(22)
Here
ij
is the reduced initial speed of the colliding molecules i and j , given by
2
ij
ij ij
g
kT
=
(23)
where
ij
g is the initial relative speed of the colliding molecules i and j . _ , the angle by which the molecules
are deflected in the centre of gravity coordinate system, is given by
15
( )
2
2 2 2
1
2
/
2
1 ( )
m
ij ij ij
r
dr r
b
r g b r
_ t
(
(
(
(
(
]
=
(
(24)
where the term
m
r is the outermost root of the equation
(25) and ( )
ij
r is the potential energy of interaction
between the colliding particles.
2
2
2
( )
1 0
1
2
ij
m
ij ij
r
b
r
g
=
(25)
In this paper, reliable collision integrals were obtained as described in the following sub-sections.
1. Neutralneutral interactions
For the N
2
N
2
and N
2
N interactions, the tabulated collision integrals determined by recent ab-initio
calculations from quantum-mechanically derived potential energy surfaces were used in view of the fact the
data were consolidated by extensive benchmark comparisons to previous theoretical and experimental results
44-45
.
In the case of the NN interactions, collision integrals were obtained by averaging the contributions of the
bound and repulsive states of the N
2
molecular system. The Morse potential and exponential repulsive potential
were used to fit the relevant interaction potentials. The parameters used for the potentials were those compiled
by Capitelli et al.
46
2. Ionneutral interactions
For interactions between neutral species and ions, two kinds of processes should be taken into account,
purely elastic collisions and the resonant charge-exchange process which is of inelastic nature. For l odd (l=1
and 3) [see Eq. (20)], the latter carries a heavy weighting in determining the collision integrals. Considering the
16
elastic and inelastic processes, we follow the previous work of Murphy
47
and estimate the total collision
integrals by the empirical mixing rule:
( , ) (l,s)
( , ) 2 2
in el
( ) ( )
l s
l s
O = O + O
(26)
where the subscripts in and el denote the collision integrals derived from the inelastic and the elastic interactions,
respectively.
In the case of the elastic interaction, collision integrals for N
+
N have been calculated using Morse and
repulsive potentials averaged with statistical weights considering interactions through 12 potential curves. The
relevant potential parameters were given in Ref.46, and the values of the collision integrals
(1,1)
ij
O ,
(1,2)
ij
O ,
(1,3)
ij
O
and
(2,2)
ij
O that were tabulated there were extended in the presented work to include
(2,3)
ij
O ,
(2,4)
ij
O and
(2,5)
ij
O , as required for the third-order approximation.
For the N
+
N
2
, N
2
+
N
2
and N
2
+
N interactions, the phenomenological potential (an improvement of the
LennardJones potential) developed by Capitelli and co-workers
48-50
has been used. The potential parameters
were defined in and taken from Ref.49 and are given in table III.
TABLE III Parameters for ion-neutral interaction potentials
49
Interaction
|
( )
0
eV c
e
r ()
m
+
2
N N
7.3650 0.12679 3.071 4
2 2
N N
+
8.0746 0.09657 3.454 4
2
N N
+
6.9373 0.06871 3.358 4
2
N N
+
6.9373 0.06871 3.358 4
For other ionneutral interactions involving multiply-charged species, collision integrals have been
derived using the polarization potential
51
:
17
2
2
4
0
( ) 1
( ) ( )
4
2
i n
in
Z e
r
r
o
tc
=
(27)
with
i
Z being the ion charge and
n
o the polarizability of neutral species. The values of polarizability of N
2
and
N are 1.76
3
and 1.13
3
respectively.
It should be noted that the use of this potential can lead to an underestimation of the collision integrals;
however, since the neutral species will have very low concentration when the concentration of multiply-charged
species is significant, and vice versa, the interactions have only a minor influence on the transport coefficients in
the situations under consideration.
For interactions between a parent atom or molecule X and its ion X
+
or X
(32)
The collision integral
(1,1)
, e j
O varies as a function of reduced temperature of electron and heavy particles,
which is approximately equal to the heavy-particle temperature. The temperature dependence of the electrical
conductivity is shown in figure 17. For each value of , the electrical conductivity first increases and then
slightly decreases, mainly due to the variation of the electron density.
Dissociation of nitrogen molecules, which is related to the heavy-particle temperature, does not occur until
the corresponding electron temperature is reached. This shifts the electrical conductivity curves towards higher
electron temperatures as increases.
The degree of non-equilibrium and the ions shielding influence the electrical conductivities through their
influence on the electron density. Further, the Debye length definition influences the Coulomb collision
integrals as discussed above, which makes a large contribution to the deviations shown in figure 17.
36
The electrical conductivity values presented here are in good agreement with those reported by Colombo et
al.
20
when the same Debye length definition including only the contributions of electrons is used. The slight
discrepancy is attributed to the different electronneutral interactions potentials and the method of
determination of the species composition.
D. The influence of pressure on properties
(a)
(b)
37
(c)
(d)
(e)
38
(f)
FIG. 18. Influence of pressure on electron mole fraction (a), specific heat at constant pressure (b), electron
thermal diffusion coefficients (c), viscosity (d), thermal conductivity (e) and electrical conductivityfof
nitrogen plasmas under different pressures 0.1atm, 1atm, 2atm, 3atm, 5atm, 10atm for =3; Symbols are as in
Fig. 5.
Figure 18 presents the influence of pressure on the chemical equilibrium composition, specific heat and
transport coefficients for pressures 0.1atm, 1atm, 2atm, 3atm, 5atm, 10atm for =3. Once again, results are
presented for the two Debye length definitions, whose influence on the properties has been discussed in
previous sections. According to Le Chateliers law, the increase of the pressure opposes changes to the
original state of equilibrium, so that dissociation and ionization at a given temperature are suppressed;
therefore, the relevant properties curves are shifted to a higher electron temperature as the pressure increases.
For viscosity [see Fig. 18 d], the temperature position of the maxima (T
max
) can be taken as the boundary
between a weakly-ionized gas and a plasma controlled by interaction between charged particles, and also the
point at which deviations in the properties begin to occur as a result of the differences in the charged particle
collision integrals caused by the different Debye length definitions.
For specific heat at constant pressure and thermal conductivity [see Fig. 18 b, e], the peaks that are related
to particular chemical reactions move towards higher electron temperature. The electron thermal diffusion
coefficients and electrical conductivity are directly dependent on the electron density, i.e. the ionization degree
of the plasma. Their values decrease as the pressure increases at electron temperatures below around 17 000 K,
39
as shown in figure 18 (c), (f). This is because the ionization temperature increases with pressure, so the
ionization degree is lower at a given temperature. Above around 17 000 K, the electron density, and thus the
electron thermal diffusion coefficients together with electrical conductivity, increase with pressure.
VI. CONCLUSIONS
In this paper, a considerable effort has been devoted to the calculation of partition functions, species
composition, thermodynamic properties and transport coefficients of nitrogen plasmas in and out of thermal
equilibrium over a wide temperature range (300 to 40 000 K) and pressure range (0.1-10atm), assuming
chemical equilibrium. These data are required for the computational modelling of many plasma applications.
The plasma composition was determined by iterative numerical solution of the nonlinear equation system
based on fundamental principles taking into account the lowering of ionization potential and contributions
corresponding to different core excited electronic states, and using partition functions derived from the most
recent spectroscopic data. The thermodynamic properties, obtained from the composition and internal partition
functions, have been presented in detail. For the calculation of transport coefficients, collision integrals obtained
from recent intermolecular interaction studies were used. Results obtained using two different shielding
distances (i.e. Debye length definitions), considering only electrons or all charged species, were compared.
Comparisons with data from the literature have also been carried out, and generally good agreement has been
found with the recent data.
It was found that with the increasing degree of non-LTE, it is possible to arrive at a situation where the
electron number density is much higher than that in LTE. An important finding is that the ionization potential
reduction due to the Coulomb interaction of charged species cannot be ignored for a non-LTE degree of = 3
or above for nitrogen plasmas. This was obtained by comparing the composition taking into account and
neglecting the influence of the ion shielding effect on the lowering of the ionization potential., The changes in
40
the chemical equilibrium composition can also lead to particular features in the thermophysical properties, such
as peaks in the viscosity and reactive thermal conductivity and the rapid increase in electrical conductivity,
being shifted to higher electron temperature. Properties became sensitive to the choice of Debye length
definition in the case of large . This is partly due to the differences in plasma composition as a consequence of
the altered internal partition functions, but predominantly due to the different collision integrals for interactions
between charged species, which are affected by the different screening distance used in evaluating the Coulomb
potential.
The results presented here are expected to be more accurate than those previously published. They will
serve as reliable reference data for computational simulation of the behaviour of nitrogen plasmas.
ACKNOWLEDGMENTS
This work was supported by the Chinese Government Scholarship program for postgraduates and Dual
Collaborative PhD Degree Program between Xian Jiaotong University and University of Liverpool.
41
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