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Calculation of the population density in the low pressure
mercury-argon discharge: analysis of the steady state
and sinusoidal operating modes of the positive column
V. Plagnol, Georges Zissis, I. Bernat, J. Damelincourt, J. Bonneval
To cite this version:
V. Plagnol, Georges Zissis, I. Bernat, J. Damelincourt, J. Bonneval. Calculation of the population
density in the low pressure mercury-argon discharge: analysis of the steady state and sinusoidal
operating modes of the positive column. Journal de Physique III, EDP Sciences, 1993, 3 (6),
pp.1167-1180. �10.1051/jp3:1993192�. �jpa-00248990�
J.
Phys.
III Franc-e 3 (1993) l167-l180 JUNE 1993, PAGE l167Classification
Physics
Abstracts52.25 52.80 52.50
Calculation
of
the
population
density
in
the
low
pressure
mercury-argon
discharge
:analysis
of
the
steady
state
and
sinusoidal
operating
modes
of
the
positive
column
V.
Plagnol,
G.Zissis,
I. Bemat, J. J. Damelincourt and J. L. BonnevalLaboratoire des
Ddcharges
dons (es Gaz (U.R.A. 277), Unversit£ Paul Sabatier, l18 rte de Narbonne, 31062 Toulouse, France(Received 26 May 1992, revised 13 January 1993,
accepted
20 January 1993)Abstract. This work deals with the
setting
up of a collisional~radiative model conceming low pressure mercury~argon dischargeoperating
under different powersupplies
(dc and ac). This model allows determination of various characteristicquantities
of thedischarge
using
thepopulation
and electronic energy conservation equations. In view ofoptimisation
of the consumingcomputer time, some
simplifying
but still realistichypotheses
have been assumed. A firststudy
inthe frame of the steady state (dc), allows us to evaluate the «
weight
» of certainphysical
phenomena
in this type ofmodelling.
We assess how much it is ofprime
importance
to considerHg-Hg
collisions as well as the excitation and ionization of argon indischarge
plasmas. The firstpoint,
often discardedby
many authors, has however a quite appreciable influence on the differentdischarge
parameters. Besides, the determination of the escape factors for theHg
resonance linesat 254 nm and 185 nm are not for the least
insignificant.
Introduction.
Lots of
experimental
and theoretical studiesconcerning
low pressure mercury-argondischarge
exist. The main
application
of such studies deals withlighting
domain,
inparticular
with thefluorescent tube that is a
specific
low pressure mercury-argondischarge.
The last few years,important
progresses,conceming
notonly
the increase oflight
efficiency
but moregenerally
better
knowledge
about gasdischarge
behaviour,
have been achieved. These researchesmainly
tum to more and more
complete
models which allow theprediction
ofoptimal
operating
conditions of
lamps.
Thus,
betterunderstanding
ofimportant
mechanismstaking place
in thesystem is
accomplished
as well.This work deals with the
setting
up of a collisional-radiative modelconceming
low pressuremercury-argon
discharges
operating
under different excitation mode(dc
andac).
The present paper discusses results of numerical calculations on the
Hg-Ar positive
column.A first
study
in the frame of thesteady
state(at
constantcurrent),
allows evaluation of theweight
of certainphysical
phenomena
in this type ofdischarge.
We have considered inelasticThe determination of the escape factors for the
Hg
resonance lines at 254 nm and 185 nm havebeen
approached
by
several ways(Holstein's
theory,
Bemat's calculations andexperiment
data).
It is known from
experiments
that theefficiency
of theproduction
of theHg
resonanceradiation goes up with
increasing
supply
frequency
[II.
Many
authors have tried toexplain
thisphenomenon
that is still not soclearly
understood. In the case of ac excitation, we deal with amore
complete
study
on thefrequency
dependence
of the main characteristics of theplasma,
namely
excited statedensity
populations,
electricfield,
electrondensity
and temperature..All the results are obtained under the reference conditions illustrated in table1.
Table I.
Input
datafor
calculations in the dc and ac cases.Parameters
Steady-State
Sinusoidal
Tube radius
(mm)
18Ar pressure
(Torr)
3Filling Temperature
(°C)
24Tube
Cold
spot
Temperature
lo
~60
40Operating Frequency (Hz)
50~20x103
Electric Current 400 400
In this paper the
following
notations are used for the extemaldischarge
parameters :I is the current; w =2grv is the
pulsation
of thesignal
and v thefrequency;
R is the radius of the
discharge
tubeP~~
is the argon pressure T~~ is the cold spottemperature. We note that the cold spot temperature fixes the mercury saturated vapour
pressure in the
discharge.
Theoretical model.
The theoretical
analysis
ofHg-rare
gasdischarges
being
verycomplex,
somesimplifying
butstill realistic
hypotheses
have been assumed in order tooptimize
theconsuming
computer time.The
positive
column is assumed to beaxisymmetric
and therefore all calculations have beenperformed
using
cylindrical
co-ordinates.In this
model,
we consider a six level scheme for mercury as illustrated infigure
I,
wheren~, x e
(g,
m, r, s, p, u,Hg+
),
denotesrespectively
thepopulation
density
of thefollowing
mercury atomic states :6~
So (ground),
6~Po,
1, ~,6~Pi;7~Si
(excited
levels)
and the mercury ion.The excited state densities of the
Hg(6~P)
atomic levels are veTyimportant
for this type ofstudies because the luminous emitted power at 254 nm
depends
directly
on them.In the low pressure
discharges,
a diffusion controlledpositive
column isfrequently
assumed(Schottky's
regime).
The main ion-electron loss process is the diffusion of thesepairs
on thetube wall where recombination takes
place,
rather than the volume recombination. Theformation of molecular ion
Hg(
can beneglected.
Thishypothesis
is confirmedby
the fact thatthis molecular ion is very unstable
(the
corresponding
dissociating
energybeing
0.06eV).
Several authors assume
that,
theargon's
role is limited to that of a buffer gas. This meansthat
only
the mercury can be excited and ionized. However, it seems that argon notonly
N° 6 DC & AC OPERATING
Hg-Ar
LOW PRESSURE ARC MODELLING l169 + i' C~l $U4
(---152
-j
j j jl
ig. I. -rcuryinelastic
lines
correspond to the 2nd kind collisions and the net radiative transitions represented by wavy lines.excitation and ionization are not
negligible.
In this paper we consider a veryiimplified
argonatomic structure which includes an excitation and an ionizatibn state as shown in
figure
2 Ar*is a fictive level which regroups the first two radiative levels and the first two metastable levels
II
s~, I s~,ls~
andls~).
The average energy of these atomic levels is about I1.65 eV. However,direct ionization from the
ground
state is assumednegligible
under the conditions considered inthis
study
(the
mean electron energy is about 1-2eV).
Interactions such as
quenching,
associative ionization.. between argon atoms areneglected
because of its low excited state concentration. We also
neglect
inelastic interactionsbetwqen
excited argon and mercury atoms because of the very small value of
atimic
Ratio
[Ar* II
[Hg]
(about
10~~-10~~).
However,
we consider thefollowing
inelastic reaction :Hg (6~P~)
+Hg
(6~P~)
-Hg(
+ e~(A)
This reaction
corresponds
to an associative ionization process and should be consideredbecause of its destructive contribution to the
population
of theHg
(6~P~)
level,
thusinfluencing
directly
theHg
resonance lineproduction.
Since excitation and ionization characteristic times are lower than the diffusion ones, we
neglect
these terms in the relevantcontinuity
equations.
The electronic temperature is assumed constant over the
discharge
tube radius. This15,76
$~
1,65(Ar*)
4a$
~ l 04.8 nm o (Ar)Fig. 2.
Simplified
argon atomic structure used in this work. We used the same notation as infigure
1.calculations have shown that the radial variation of the
heavy
gastemperature
remains,
in ourcases, less than 20
9b,
therefore we consider a flat radialheavy
gas temperature distribution.Under this last
assumption,
Hg
and Arground
states aresupposed
to beuniformly
distributedwithin the
discharge
tube. We then, deducen~~
and n~~ from theperfect
gas law :n~~
=~~~~~~~
(i)
k~
T~l'Ar(Tg)
~~~k~
T~ ~~~P~~(T~~)
is the mercury saturated vapour pressure and it isonly
a function of the cold spottemperature ;
k~
is the Boltzmann constant and T~ the temperature of neutral atoms, obtainedby
averaging
the radial valuesgiven by
Zissis[3].
Taking
into account that thedischarge
tubeis a closed
system,
P~~(T~)
can be deduced from thefollowing
equation
:~ T~
~
Ar(Tg)
" P Ar
f
(3)
To is the tube
filling
temperature
andP(~
is the argon pressure at thistemperature.
The radial behaviour of the
charged
and excitedspecies
is morecomplicated
and should beevaluated
by solving
thegoveming
equation
set at each radial node. However, several authorsuse a radial distribution of the type :
nxir)
=
n>(°)
Jo12.4
~
x ~
im,
r, ~, P, u,Hg+,
ei
where
J~
is the zero-order Bessel function. Calculations carried outby
severalauthors,
using
this distribution are in very
good
agreement(within
± 29b)
with theexperimental
measure-ments of Koedam and Kruithof
[5].
This agreement between measurements and calculationscan be
partially
justified
by
the fact that theprevious
distribution is the formal solution of theN° 6 DC & AC OPERATING
Hg-Ar
LOW PRESSURE ARC MODELLING i171this
assumption,
thus thefollowing
radialnormilized
distributions have been tested :r r 2
Pi(r)
= IP~(r)
= I R R r 4 ~ 6P4(r)
= I~R
P~(r)
= I ROur results have shown that the use od
P~
instead of the Besselshape
leads to agood
agreement with the
experiment.
However,
the use ofPi,
P~
andP~ shapes
was averred inconflict with the
experimental
data.Furthermore,
it ispossible
tosimplify
our calculationsby
using only
averaged
valuesalong
thedischarge
radius.Using
a well known radialprofile
(I.e.
Bessel
distribution)
it wasquite
easy to obtain theseaveraged
quantities
by
analytical
integration
over thedischarge
tube cross section.The
previous
assumptions
lead to a set ofcoupled
ordinary
differentialequations
describedbelow :
.
Hg
excited statecontinuity
equations
:dn,
$
~~~
~"~~'
~'~j
'~~
~~"
~~'
~~~ > # (i.Hg~) ' 'where, x e
(m,
r, s, p,u),
y e(g,
m, r, s, p, u,Hg+ )
and n~ is the electrondensity.
The operatorA~
takes into account the contribution of the radiative transitionsincoming
(+
sign)
andoutgoing
(-
sign)
to/from the level x.Consulting
figure
I thefollowing
values arefound for this operator :
X m T S p U J~ ~~ ~~ ~~ ~~ ~~
£
~~ ~ ~ um ~ur ~rg ~ us ~pg ~ ~ ~ ~ ~uy whereT_~ is the effective radiative life-time of the transition x - y,
taking
into account theradiation
trapping
in theplasma.
The operator 3C~ accounts for inelastic collisions between
Hg
atoms. This operator hasnon-zero values
only
in the case of x = s then 3C~ =n)
Z~~~+ where Z~~~+corresponds
to thecollision rate of the reaction
(A),
previously
cited in this paper.. Ar excited state
continuity
equation
:dn~ n~
= n~[n~Z~~
n~(Z_~
+ Z~~~+)]
(5)
at T_~
where x = Ar* and y = Ar.
. Ion
continuity
equations
and localplasma
neutrality
:dn~~+
+ =Df~
V~n~~+ + n~~j
n~Z~~~+ + n~ 2~~~+(6)
dt dn~~+ ~ + ~fi
~a
~ ~ flAr~ + fle fly~y
Ar~?)
n~ =
n~~+
+ n~~+(8)
where x e
(g,
m, r, s, p,u),
y = Ar* and. Electronic energy conservation
equation
:~i
= n~
(-
Kv~~,,iu~
ug)
+ qJ~~E~
+z
nxzxy
uxyj
(9)
~~~
x e
(g,
m, r, s, p, u,Ar,
Ar* and y e(g,
m, r, s, p, u,Hg+,
Ar,
Ar*,
Ar+).
U~ is theaverage electron energy,
U~
is the average thermal energy of the neutral atoms andAU~
=U~
U~ is the energy gap between the levels x and y. If the transition leads to theionization ~y e
(Hg+,
Ar+)
)
then wall losses should be consideredby
means of the relation :AU~
=AU~
5U~/2.
Othersymbols
in the aboveequation
are : v~~,, theelectron-argon
elastic collision
frequency,
p~ the electronmobility
andK the fractional energy loss per
electron per elastic collision. The term
corresponding
toHg
associative ionization(reaction
A),
proportional
ton),
isnegligible
because of the very small rate coefficientcorresponding
to thisreaction
(several
orders ofmagnitude
less than electron-atom collisionrates).
. Ohm's law :
R
1 = 2grqE
n~ p~ r dr(10)
0where E is the axial electric field
strength
and q theelementary
electroncharge
(absolute
value).
In these
equations,
Z~
are thecorresponding
rate coefficients calculated from the relevantQ~
inelastic cross sections. In the case of excitation from theHg(61So)
state we used theRockwood's data
[6].
Excitation cross sections for the excitedHg
levels aregiven
by
Winkler[14]
and cross sections for the ionization from these levels are obtained fromVriens's
[7]
semi-empirical
formula. Dataconceming
argon, have beengiven by
Zissis[3].
All reactions rate for the 2nd kind collisions are determined
by
using
the Klein-Rosseland'srelation based on the
micro-reversibility
principle.
The effective radiativelife-times,
T~, and data
conceming
the two resonance mercqry lines(254
nm and 185nm)
used in thisstudy
aregiven
by
Holstein's[8]
theory,
Bemat's calculations[9]
and Van deWeijer's
experimental
values[10].
The
knowledge
of the ElectronEnergy
Distribution Function is ofprime
importance.
Alltransport coefficients
depend
on the onehand,
on it and the transition rates are very sensitive tothe EEDF choice on the other hand. For
example,
the relative difference between transitionrates calculated
by
using
different EEDFapproximations
can reach 90fb in the case7?~
-
61So
transition[17].
In the present work the Maxwell~Boltzmann classical EEDF hasbeen
mainly
used,
thisassumption
simplifying
considerably
the calculations. However, in thecase of
steady-state
calculations we have examined the influence of a non-Maxwellian EEDFshape.
For thisattempt,
theLagushenko
andMaya's
[4]
semi-empirical
analytical
solution ofthe Boltzmann
equation
has beenimplemented
as EEDF. The results obtainedusing
thisfunction are
clearly
more realistic but the computer time, in the case of acoperating
mode,
becomes
prohibitive
(several
hours of calculations on a HP-9000/330computer).
Results.
STEADY STATE OPERATING MODE
(alai
=
0).
Firstly,
we compare our results withexper-imental data in a dc
discharge
in order to validate our model.Indeed,
such studies are morecommon. We use
experimental
datagiven by
Damelincourt[2]
and Koedam[5]
for theN° 6 DC & AC OPERATING
Hg-Ar
LOW PRESSURE ARC MODELLING l173Our main intention
during
thisphase
is to evaluate thevalidity
of certainassumptions
systematically
adopted by
several authors.Our initial results were not in
good
agreement with thosegiven by
experiments.
This couldbe
explained
by
the fact that in a firstapproach
weneglected Hg
associative ionization as wellas Ar excitation and ionization. Furthermore, we considered the
imprisonment
lifetime gaveby
Holstein's
theory.
As we have shown in theprevious
part
of this paper the radial distribution ofthe
charged
species
couldseverely
influence the emitted power of theHg-254nm
ifT~~ was greater than 40 °C. In view of the overall of the results, we suppose a Bessel
shape
radial distribution for the
charged
and excitedspecies
and a better agreement is obtained.Furthermore,
thecomparison
of our results for theHg
resonance radiation output in the case ofa
typical
low pressuredischarge
with thosegiven
by
morecomplete
radial calculations carriedout
by
Zissis[16]
leads to asatisfactory
agreement.As illustrated in
figure
3,
we demonstrate theimportance
ofHg
associative ionization on theHg(6~Po,,
~)
populations
athigher
cold spot temperature range.Moreover,
thevalidity
ofHolstein's
theory
influences the middletemperature
range.Besides,
argon excitation andionization
weight
is notnegligible
mainly
in the low cold spot temperatures.As far as the influence of the escape factor of the mercury resonance lines are
concemed,
wetested
initially
values deduced from Holstein'stheory [8],
and then those of Bemat[9]
andWeijer
[10]
for theHg-254
nm and 185 nm linesrespectively.
The second set ofvalues,
30 9bor 40 9b lower than Holstein's is in better
agreerqent
with the valuesgiven by
experiments.
Figure
3 shows that this choice leads to a sensitive decrease of thedensity
populations.
A very common
hypothesis
is tonegglect
the inelasticscattering
between excitedHg
atoms.In
fact,
forHg
partial
pressures less than 10 mTorr, the atomic ratio[Hg*]/[Hg]
remains lessthan
19b,
thus theprobability
ofHg*/Hg*
inelasticscattering
seems to benegligible.
However,
it isquite
hazardous toneglect
these collisions whenHg partial
pressure becomesimportant.
Asshown,
the reaction(A)
leads to a decrease of theHg(63P2)
density.
However,
we do not
dispose
precise
information on the nature of these interactions and thepublished
cross section data are very uncertain. These cross section values find in the literature vary
between I
h~
and 100h~.
As shown infigure
3,
agood
agreement between calculation andexperimental
data is obtained when this cross sectionapproaches
50h2.
For lower values of T~~, when mercury
partial
pressure becomes very low(some
l00~LTorrs),
withoutincluding
Ar excitation and ionization in our model,significant
deviations between calculation and
experimental
data have been observed.By
including
thesephenomena
andchoosing
a suitable Ar resonance radiationtrapping
factor our results, asshown in
figure
3, fit well the excited statespopulation.
Furthermore, as has been shownelsewhere
[18]
the influence of the Ar is of aprime
importance
notonly
forpopulation
calculations but also for the determination of the axial electric field
strength
and the electrontemperature in the
discharge
plasma.
As shown in
figures
4 and 5 the agreement between our calculations andexperimental
datafor the
Hg-254
nm resonance line emissionintensity
and the axial excited state densities of theHg(6~Po,1,
~)
excited levels as function of the cold spottemperature
isquite
satisfactory.
Thediscrepancies
observed in the other author's results[13-15]
can beexplained
by
the fact thatthey
do not account forHg
associativeionization,
andbesides,
most of them use the Holstein'stheory
for the determination of the escape factors. Moreover,they
do not consider argon as anactive
species.
The above considerations validate our model in
steady-state
operating
mode. The betteragreement has been obtained
by
using
thefollowing
combination of parameters :.
Escape
factors :30
(C)
E r~ Q 15 7 ~ Z o 40~~
(b)
E r~~''~
20 ~ Z e m a w 0 20(a)
E r~~~
10 7 E 0 0 20 40 50 60 ~CS~~~~
Fig. 3. Influence of different physical processes on the mercury excited state
populations
(curve aHg-63Pu1
b :Hg-6~Pj
cHg-6~P2)
as function of the cold spot tube temperature. Shadowed areascorrespond to the influence domain of the
following
processes:@
Hg associative ionizationreaction a) with cross section « varying from 0 to 50
12
;fill
Ar excitation and ionization with excitedstate effective life time, r~~
varying
from 0 (excitation and ionization excluded) to 5 times theexperimental
valuegiven by
[I I]fill
Hg
resonance radiation escape factors, r,~ and r~~varying
fromthe Holstein's theory to experimental values given by [9] and [10]
respectively.
-m-. our finalcalculations with « = 50
l~,
r,~ from [9], r~~ from [10], r~, from [I I],
including
AT excitation and ionization. Experimental data (?) are from reference [2].N° 6 DC & AC OPERATING
Hg~Ar
LOW PRESSURE ARC MODELLING l175 25$@
--~f
f~
° o o o ,, ,, IS '',~
, ', , , = ,' ', o z , , m e',,
$~ # o n~)
J
o Expe1inlent mfl131 ~efj14] this work10
20 30 40 50 60 70 TCS(°c)
Fig.
4.Comparison
between several calculated values (lines) of the emitted power at 254 nm (Hgresonance line) per unit of positive column
length
and the experimental data(symbols).
Experimental data are from reference [2].~~ ~~ , E 15
'~
E1'
~ ~ ~ / ~ ~ ~ / / * W o w /d
~ o £ / _/ I,./
o / Q ° ° o o o o 20 40 6l &J ~20 40 6l 80 0 20 40 6l 80 Tcs(°C~ T~(°C) Tcs(°C)Fig.
5.Comparison
between several calculated values of excited~state densities of theHg(6~Po
j
2)
atomic levels and
experimental
data as a function of the cold spot temperature. lo)experimental
data [5] ;T~~(Hg-185
nm)
: asgiven by Weijer
[10]
T~~(Ar-105
nm)
: asgiven by
data in reference[I1]
.
Hg
associative ionization cross section(reaction
Al
« =
50
A2
SI.NUSOIDAL OPERATING MODE
(alat
#0).
Experimental
works carried outby
Damelin-court
[2]
and Bemat[9]
demonstrate thegreat
difficulties tointerpret
excited statepopulations
leading
from measurements of theHg-254
nmabsorption
in thedischarge
plasma.
When thefrequency
is about 0, I kHz andlower,
the wave form of the current is not a true sine curve(Fig.
6).
For the above reasons we use theexperimental
data of the relative flux of theHg-254 nm resonance line in order to validate our calculations. These measurements are direct and
do not need any
interpretation
calculations. Thegood
agreement between data and calculationsshown in
figure
6.However,
there is aproblem
at lowfrequency.
At the verybeginning
of thehalf
period
of the current, theexperimental
values present animportant
increase followedby
asensible decrease.
For the other
quantities
such asdensities,
electric field, electron temperature, ourcalculations do not
reproduce
experimental
resultsquantitatively.
However,
they
fit theexperimental
dataqualitatively
well.Figure
7gives
the calculation results and thecorrespond-ing
experimental
values. Thesequantitative
discrepancies
could beexplained
asfollowing.
The
rapid
increase of n~, E and T~ observed at thebeginning
of thehalf-period
due to the factthat there is an « extinction » of the
discharge
corresponding
to a very low electrondensity.
The field
strength
E must increase in order to maintain the current in thedischarge.
This« heats » the electrons and T~ increases as well. At the
beginning
of the halfperiod,
there arenot
enough
excitedspecies
and electrons,Only
inelastic collisions between electrons andHg
ground
state atoms takeplace
andthey
populate
directly
thehigher
excited levels. Whilen~ remains
low,
Hg(63Po)
andHg(63P~)
cannotdepopulate
becausethey
canonly
decay by
2nd kind collisions with electrons. In
opposition,
because of itsrapid
decay
by
radiativetransitions,
thepopulation
of theHg(63Pi)
resonant level does not increasesignificantly
at thebeginning
of the halfperiod.
As shown in
figures
8 and9,
representing
thetime-average
values of the electric field andthe electron
density
population
over aperiod,
there is agood
agreement between calculatedvalues and
experimental
data.Conclusion.
A first
study
in the frame of thesteady
state, allows us to evaluate the «weight
» of certainphysical
phenomena
in thistype
ofmodelling.
We assess how much it is ofprime
importance
to consider
Hg~Hg
inelasticscattering
as well as the excitation and ionization of argon in ourdischarge
plasma.
The firstpoint,
often discardedby
manyauthors,
hasquite
anappreciable
influence on the different
discharge
parameters.
Besides,
the determination of the escapefactors for the
Hg-254
nm and 185 nm resonance lines are not at leastinconsequential.
In the case of sinusoidal
excitation,
we deal with a morecomplete
study
aboutfrequency
dependence
of excited state and iondensities,
electronic temperature and axial electric field.We use the
experimental
data of the relative flux of theHg-254
nm resonance line in order tovalidate our calculations. A
good
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bU fly (W'/A)3 I ~ "Acknowledgments.
The authors are
greatly
indebted to Professor J. J. Damelincourt for hisextremely
usefulremarks and the
unflagging
supervision
of this work. We would also like to thank K. Charradaand L. S6vier for their contribution
through
many discussions and N.Sewraj
for his assistancein the realisation of this paper.
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