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The stability of cells in directional solidification
Wouter-Jan Rappel, E. Brener
To cite this version:
Wouter-Jan Rappel, E. Brener. The stability of cells in directional solidification. Journal de Physique
I, EDP Sciences, 1992, 2 (9), pp.1779-1790. �10.1051/jp1:1992244�. �jpa-00246659�
Classification Physics Abstracts
44.30 68.45 81.30F
The stability of cells in directional sofidilication
Wouter-Jan
Rappel
and E.A. Brener(*)
Laboratoire de Physique Statistique
(*°),
24 rue Lhomond, 75231 Paris Cedex 05, France(Received
6 August 1991, revised 27 February 1992, accepted 15 May1992)
Abetract. The stability of numerically obtained cells in the one sided model of directional solidification is investigated, using a numerical approach. In particular, the shapes of the cells
corresponding
to the Saffman-Taylor branch are discussed. The possibility for an oscillatory instability is investigated and the results are compared with a recent approximate analytical stability calculation. For large thermal length we find an instability which is oscillatory forsome parametervalues. The results agree partially with the analytical stability calculation. The
possible limit cycle arising from this instability is discussed.
1. Introduction.
In directional
solidification,
onepulls
abinary alloy through
anexternally imposed
fixed tern~perature
gradient.
Forhigh enough pulling velocities,
theplanar interface, separating
theliquid phase
from the solidphase,
becomes unstable and forms cells with a well definedwavelength ill.
Formetals,
where the diffusion ofimpurities
in the solid can beneglected,
theresulting
cells are
typically
verydeep
[2].The
problem
of the determination of theresulting
cells has receivedconsiderably
attention.Previous work includes numerical calculations
[3-6]
andapproximate
theories [7, 8].Contrary
to the case of the
symmetric
model [9], where one assumesequal dilfusivity
in theliquid
and thesolid,
and to the case ofrapid
solidification[10],
where thepulling velocity
becomes solarge
that theassumption
of localthermodynamic equilibrium
at the interface is violated, a linearstability analysis
of these cells in the one sided model has not beenperformed.
In this paper, we examine the linear
stability
of cells in the one sided model. We focuson the case of small Peclet
numbers,
for which one can make ananalogy
between directional solidification and viscousfingering
[7]. For this case, Karma and Pelcdii Ii
haverecently argued
that the cells should exhibit an
oscillatory instability.
Thegoal
of this paper is to introduce thestability
calculation andapply
this to find anoscillatory instability.
This paper is
organized
as follows: in section 2, the basicequations
of directional solidificationas well as the numerical
techniques
used in this paper are reviewed. Section 3 describes the (*) Pennanent address : Inst. for Solid State Physics, Chemogolovka, U.R.S.S.(**) assoc16 aux universit£s Paris VI, VII et l'Ecole Nomlale Sup6lieure.
shapes arising
from our numerics and compare the results from the numerics withanalytical predictions.
In section4,
thestability
of the obtained cells isinvestigated
and in section 5 we discuss the limitcycle
which results from theinstability
oflarge
thermallength.
2. Basic
equations
and numericaltechnique.
The standard set of
equation
are well described elsewhereiii.
As is oftendone,
we go in the framemoving
with thepulling velocity
vp and measurelengths
in units of half thewavelength A/2
,
the concentration c in units of cn~
(the
concentration far away from theinterface),
and time in units of l~/4D. Then,
for the one sidedmodel,
we havev ~C +
2Pe)
=Ii
(fi
VcL)
"-(I k)(2pefi
§ +vn)cL
c~ =
j
= -7~c
(1)
Here,
D is the diffusion constant in theliquid,
k is thepartition coefficient, f
is the dimensionless thermallength,
7 is the dimensionlesscapillary length
and pe is the Peclet number: pe=
(~.
vn is the contribution from the interface other than the constant
pulling velocity
up which is2pe
in ourunits).
Of course, we have vn= 0 for a
steady
state.To solve the above set of
equations
in a numerical efficient way we rewrite theequations
as aintegrc-differential equation
and solve for the(unknown
andfree) boundary
[3] We will do this for both thequasi-static approximation,
where weneglect
the time derivative term in thediffusion
equation
and for the fullequation.
In the
quasi-static approximation
we find-(
+7~t(S))
=/(@
+
7~t(S')) (h'
?'G(S> S'))
dS'+2Pek /(@
+
7~t(S')) niG(S> S')
dS'+
/ vn(S') (k(f
+
7~t(S')) (f
+
~t(S'))j
G(S>
S')
dS'(2)
where the Green's function G is the solution of
V
~G
+2pe )
=
-6~(x x') (3)
The
explicit
form of G can be found in reference [3].For the non
quasi-static
case we go back to the rest frame and we findY~S>t)~~ 2P~t) ~~c(s,i)
= if
ds,f~
di,~Y~S'>t')~- 2P~t') ~c(s,,i,))
-«
A~ v
'G(~(s,1), ~'(/,i,);i,i,)
+f
ds~f~
di'~~~~"~'~j
~~~~'~~(s',i~))
-~
G(~(s,t), ~'(s',t');t,t')(2pen(
+ vn(s',t')) (4)
where G is a solution of the full diffusion
equation
T7
~G ~
=
-6~(x x')6(t t') (5)
To find
steady
state solutions weparameterize
the(unknown) boundary
with Npoints
ofequal arclength.
Ourindependent
variables are then the normalangles
at themidpoints
of theequal ardength
sections and theposition
of thetip.
We solve theintegrc-difLerential equation
on the
points
ofequal arclength,
except at theendpoints (~
= 0 and ~=
l)
andrequire
that theslope
vanishes at both thetip
and the tail. Ingeneral,
we have chosen a discretization rate of l10points.
To examine the
stability
of theresulting cells,
weperturb
thesteady
state solutionby adding
the normal shift:
x(S)
=xo(S)
+iio(S)6(S>t) (6)
where we assume that
6(s, t)
=b(s)e~~
andb(s)
« I. We substitute thisperturbation
in(2)
and linearize in
b,
whichgives
usIds, (7~o
+(° )(6(s')41
v'+ b(s)ho
T7)hl
T7 'G +~(~'~
~(6"(s')
+c(b(s')))
hi
V 'Gf
+
?~to
+
~°) (-b'(S')il
'v 'G+1C0b(S')fit
?G)j
f -2pek /
ds'fly
(71Co +
( )(6(S')fi~
V ' +6(~)~°
?)~
+ ji
~(~'~ 7(b"(s')
+c(6(s')))
G'
~
f
+
7~o
+
(° (-b'(/)iiG
+iy~to6(s')G)j
+
~~~'~ 7(6"(S')
+C(b(S')))
f
= w
/ dsJ(I k)
~° + 7no6(s')G (7)
f
The discretization of the
integrals gives
us a set ofequation
of the formM M
L Aij6j
= w
L B"j
b>
(8)
>=o j=o
where M is the number of discretization
points.
Thisordinary eigenvalue problem
for w can be solved with one of the standard numericalpackages.
For the non
quasi-static approximation
weagain
substitute the normal shift in theintegrc-
difLerential
equation (4).
Thisgives
us:Ids' (7~co
+ ~°)(b(s')fi[
V ' +b(s)fro
V)fi[
V'G(w)
3~~,
+
7(b"(s')
+n(b(s')) hi
V'G(w) f
+
71Co
+() (-6'(S')i~
'V
'G(W) +'~06(S')fi~
'~7G(~°)j
-2pek /
ds'fly
(7~co + ~°
)(6(s')fi[
V'+ 6(s)fro
V)G(w)
f
fi( J)
+
~v (f 7(b"(S') '~(6(S')))
G(~°)
+
7'~o
+
() (-6'(S')I$G + ylCo6(S')G(W))j
+
~~l'~
7(b"(S')
+C(b(S')))
" ~k°~
/
d~'((
+
~0) b(S')G(W) (9)
where an
explicit
form ofG(w)
isgiven
in reference [9].Upon discretizing
theintegrals
we getan
equation
like£
MCjj(W)bj
# 0
(10)
j=0
where C is a function of w. and therefore in
general complex.
To solve the aboveequation,
wehave to vary w until C has a zero
eigenvalue.
This is done with a Newton'salgorithm
which will converge to theright
w after we haveguessed
an initial value for w.The
technique
forfinding
thegrowth
rate of theperturbation
is thefollowing.
We will first examine thestability
of the pattern in thequasi-static
limit. We will not expect to find theoscillatory instability
in this way but it is a useful first estimate. We then calculate thelargest eigenvalue
fora number of
growth
rates. This willgive
us an indication where theeigenvalue
becomes zero. We then use a Newton's solver to
pin
down the value of thegrowth
rate for which the determinant, or thelargest eigenvalue
is zero. For further details we refer to[10].
3.
Steady
state cellshapes.
In this
section,
we willinvestigate
the cellshapes corresponding
to theregion
in parameter space where one can compare these cells with thefingers
in theSalfman-Taylor (ST) experiments
[7].We have taken the diffusion constant to be D
= 2.5 x 10~~ m~
Is
,
the
capillary length
to bedo " I. x 10~~ m and the
wavelength
= 20. x 10~~ m. For thepartition
coefficient k we havetaken two
values,
k = 0.2corresponding
to a subcriticalbifurcation,
and k=
0.8, corresponding
to a
supercritical
bifurcation. The thermallength
lT is used as the control parameter, but isalways large compared
to the difLusionlength 2D/vp.
This isimportant,
since this enables us to check thestability
program in a non-trivial way(see below).
Depending
on the distance from the neutral curve, we obtain either adeep
cell(see Fig.
la)
or a shallow cell(see Fig-16).
Fromfigure
la we see that the cell is indeed verydeep (notice
the difference in scales on theaxis)
and has a little bubble at its tail. This seems to be characteristic of thesedeep
cells and has beenreported
in earlier numerical work in both the one-sided andsymmetric
model [3, 5]. This bubble is also present for the values oflT
close to the
marginal stability
curve(see Fig. lb).
We think that this bubble does not havea
significant physical meaning,
in the one-sidedmodel,
for two reasons: first ofall,
since the cells arepropagating
into theliquid,
the solidjust
above the bubble will melt first and thenresolidify,
as the cell moves on. This seems to be ratherunphysical
in the one-sidedmodel,
where oneneglects
the diffusion ofimpurities
in the solid. A second argument is the numericalresult
plotted
infigure
2 where we haveplotted
the cellshapes
for fixedvelocity
andwavelength
but different discretization rates. We see that the
tip
of the cells remainessentially unchanged
and that the bubble propagates down as we increase the number of discretization
points.
It therefore seemslikely
that the cellprefers
to be infinitedeep
and that the bubble is an artifact-30300
-30400
1
-30500~
-30600
-30700
O.O 2.O 4.O 6.0 8.O lO.O
x
~m) a)
-450
-soo
-550
-600
O.O 2.O 4.O 6.O 8.O lO.O
x
@m)
~~Fig-I. a)
A typical example of a deep cell(k
= 0.8, ~ = 144
pm/s,
IT= 25300pm; other material parameters as given in
text). b)
An example of a cell close to the marginal stability curve, for a supercritical bifurcation(k
= 0.2, ~ = 134
pm/s,
IT = 400pm).
of our zero
slope
condition at the tail. This result istypica1for
the one-sidedmodel;
in thesymmetric
model we do observe a similar bubble at the tail of thecell,
but itsposition
does notchange
as a function of the discretization rate.Before we discuss the
stability
of thecells,
let usverify
that we are indeed in the STregime.
In
figure
3 we haveplotted
theposition
of thetip
vi vs. thepulling velocity
vp. As we cansee, this curve is non-monotonic. For vp < 600
pm/s
theposition
of thetip
increasesby
increasing velocity.
This part of the curve we will call the STbranch,
while the part on which thetip position
decreases for forincreasing velocity
we will call the second branch(see
also the discussion sectionbelow).
In this paper we will focus on STbranch,
for which we expect-25
[
125/~
~
/ 100 Points
-225
250 points
325
2 4 6 8
x
(~m)
Fig.2.
The cell shapes for fixed material parameters but different discretization rates.-2500
_
-3000
~
<
c
° -3500
aI
+
~ -4000
-4500
O 200 400 600 BOO IOOO
Velocity ~ptn/s)
Fig.3.
The position of the tip Vt as a function of the pulling velocity ~p, for IT" 1100 pm and
k
= 0.2. The circles represent the numerical data points, with the solid line as a guide to the eye.
the
tip position
to increase forincreasing velocity ill].
We can also
directly
compare thesteady
state cells with a STfinger.
We know that in the limit oflarge
ITcompared
to the diffusionlength,
the cell should have a width A ofill]:
i
A= ~~
(II)
I-(I-k))
T
where
§
is theposition
of thetip
of the cell relative to theposition
of theplanar
interface.We have verified the above relation with our numerics. We find that the width of the
finger
agrees within 5$lo of the value
given
above.Furthermore,
the width remainsroughly
constant for thermallengths typically
an order ofmagnitude larger
than the difLusionlength.
We cantherefore conclude that we are on the ST branch. In other
words,
the results of Karma and Pelcd shouldapply
to our cells.There are some checks on our
stability
calculation. First ofall,
we can check that theplanar stability
calculationgives
theright
answer. The other check uses the fact that the nature of the bifurcation of theplanar
interface can be either super- or subcritical. Formetals,
with smallk,
the onset to cells from theplanar interface,
istypically through
a subcritical bifurcation.Indeed,
as we decrease thewavelength
for fixedvelocity
for k=
0.2,
we encounter a saddle- node bifurcation. Fromelementary
bifurcationtheory,
we know thestability assignments
of the tworesulting branches;
the upper branch should bestable,
while the lower branch should be unstable. Our numerics also agree with thisstability picture, although
in thevicinity
of thesaddle node we need more
points
on the interface to resolve thestability.
The last check of the program, is a
highly
non-trivial one. If we take the thermallength
to be muchbigger
than the diffusionlength,
weapproximate
the case of a dendrite ina channel.
There,
we have asingle
cellgrowing
in a narrow channel, in the absence of a temperaturegradient (I.e. lT
"
oo).
As has beenshown,
bothanalytically
[12] andnumerically [13],
in thecase of a dendrite in a channel the ST branch is unstable. This
provides
us with an excellent check for ourstability
program: the cell should become unstable for verylarge lT.
We haveindeed found that this is the case, as will be discussed in detail below.
4. The
oscillatory instability.
As mentioned
before,
Karma and Pelcdill]
haverecently argued
that in the limit of small Pecletnumbers,
the cells canundergo
aHopf
bifurcation.Using
anapproximate
interfaceformalism, they
showed that thegrowth
rate can have apositive
real part with a non-zeroimaginary
part, which would mean anoscillatory instability.
If one would increase the thermallength,
one will encounter a first critical thermallength
for which the real part of thegrowth
part becomespositive.
If one increases the thermallength
even more, thecomplex conjugate
root
pair
willcollapse
into two pure realpositive
roots at a second critical thermallength.
One of the roots is
going
to a finitevalue, corresponding
to theinstability
of the dendrite in achannel,
and one isgoing
to zero,corresponding
to the zero mode which is present in the caseof zero temperature
gradient.
To
verify
the result of Karma andPelcd,
Kessler and Levineperformed
a linearstability analysis
like we havepresented
in this paper, for thesymmetric
model [9]. Thatis, they
obtained
steady
state solutions with theintegrc-difLerential method, perturbed
this solution with a normal shift and solved theresulting eigenvalue problem
for thegrowth
rate of theperturbation.
Their conclusion was that there was no evidence for anoscillatory instability.
These
contradictory
results have been controversial ever since. There are a fewpossibilities
for the
disagreement,
apart from the fact that one of the two groupsmight
have made a mistake.One
possible
difference between the twoapproaches
is that Karma and Pelcdanalyzed
the one sided model while Kessler and Levine used thesymmetric
model.However,
we will argue below that we don't believe that there will be an essential difference between the models.Nevertheless,
we haveperformed
all our calculations in the one sided model.For the parameter values of Kessler and
Levine,
we have not been able to find aninstability.
All the cells are
linearly stable,
consistent with the results of Kessler and Levine.However,
as we have
pointed
outabove,
forlarge
IT theproblem
of directional solidificationapproaches
JOURNAL DE PHYSIOUEI T 2, N'9. SEPTEMBER 1992 64
O.3
O.2
o-1 5
j
o-o-o.i
-O.2
SOD 1000 1500 2000 2500
~~wn)
FigA.
The real and the imaginary part of the eigenvalue as a function of the thermal length IT Here, k= 0.2 and pe
= 0.268.
that of the dendrite in a channel.
There,
as has been shown before[12],
the cellcorresponding
to the ST branch is unstable. It is therefore
logical
to extend the range of parameters tolarger
IT. Note that the ST branch in a channel is also unstable in the two sided model, and wetherefore expect to see the same
qualitative
behavior in that case [14].We have
performed
the calculation for two different values of thepartition
coefficient: k= 0.2
and k
= 0.8. For a fixed Peclet number pe we have varied the thermal
length
IT and have examined thestability
of theresulting
cells.For all Peclet numbers we found that if we increased the thermal
length
above a criticalvalue,
saylT,c
the cells become unstable. Forlarge
values of lT(I.e.
lT »lD),
thisinstability
isalways
pure real. This is inagreement
with thestability
calculation for a dendrite in achannel,
as well as Karma and Pelcd.The results of the
eigenvalues
for k= 0.2 and pe = 0.268 are
presented
infigure
4.Here,
the solid linecorrespond
to the real part of thelargest eigenvalue,
and the dotted linecorrespond
to the
imaginary
part of thiseigenvalue.
We see that the cell becomes unstable with for lT ~' l125 ~tm, and that theinstability
has a non-zeroimaginary
part. In otherwords,
we dohave an
oscillatory instability
here.Our numerics
show, however,
that anoscillatory instability
occursonly
forlarger
Peclet number(I.e,
pe >0.I).
For small Peclet numberwe have
never found an
oscillatory instability.
There,
theeigenvalue
becomes pure real so close thelT,c
that we are not able to observe anon-zero
imaginary
part forpositive
real part. Note however that theimaginary
part of thegrowth
rate at the critical thermallength
in Karma and Pelc6'stheory
goes to zero as pe goesto zero. It is
possible
that our numerics cannot handle such a smallimaginary
part.In
figures
5a and 5b we have summarized our results for the two values of k. The solid linecorrespond
to thepredicted
value oflT,c.
We see that of the two curves the one for k= 0.8
agrees better with the
prediction
of Karma and Pelc4. For this value of k, our numerics agree better with the solid curve for small values of pe. This isexpected
since theiranalysis
is valid for small Peclet numbers. Forhigher
values of pe theanalytical lT,c
becomes constant, while thenumerically
obtained value increasesagain.
This can beexplained by noting
that3500
2500
soo
SOD
~~
a)
isoo
iooo
soo
O
0.OO O.05 O.lO O,15 O.20
pe ~~
Fig.5. a)
Our numerical results for lT,c(circles)
and the prediction Irom the analytical theory(solid line).
Here k= 0.8,
b)
Same asfigure
5a but now for k= 0.2.
for
increasing
Peclet number we will move towards the stable secondbranch,
which will be discussed in more detail in thefollowing
discussion(see
alsoFig. 6).
As one moves toward the transitionpoint
between the two brancheslT,c
- oo since the second branch is stable.The
analysis
of Karma and Pelcd is of courseonly
valid for the ST branch.Also, according
to Karma and
Pelcd,
the thermallength
for which theinstability
becomes pure real is muchlarger
thanlT,c.
Our numericshowever,
find no second critical thermallength,
or one which is much closer tolT,c.
~t
limit CST Second
branch branch
~ V
P
Fig.6.
A schematic drawing of the limit cycle arising Irom the instabfiity for large thermal length.The solid line corresponds to the steady state solution branch while the dashed curve corresponds to the limit cycle. The ST branch
(or
at least the part on which point A islocated)
is unstable while the second branch,corresponding
to the decreasing part of the non-monotonic curve is stable(compare Fig.3)
The limit cycle will consist ofthe trajectory D - E- C - D. For
a detailed explanation see the text.
5. Discussion.
To summarize our numerical
results,
we can say that in the ST limit the cells will become unstable forlarge
IT- If we are in the unstableregion
theinstability might
ormight
not beoscillatory
of nature,depending
on theparametervalues
of the system. The agreement with thetheory
of Karma and Pelcd is at mostpartially.
Let us now
discuss,
what we think thisinstability
will lead to. Weemphasize
that the scenariowe are
giving
here isonly
valid for the case whenwavelength
selection is not available. In otherwords,
we envision a situation where the cell cannotadjust
itswavelength. Experimentally,
this wouldcorrespond
to directional solidification in a channel. If thewavelength
can be selected it is very wellpossible
that theinstability
described in this paper can be avoidedaltogether.
The limit
cycle
which will arise is sketched infigure
6. We assume alarge
but not infinite thermallength (I.e.
the temperaturegradient
is small butnon-zero).
Here we havesketched,
as a solid
line,
the twoexisting steady
statebranches,
as infigure
3. Note that thedependence
of vi on up is non
monotonic,
andcorresponds,
in the limit oflarge lT,
to the one discussed in reference[14].
To avoid anypossible
confusion we note that in theproblem
of a dendrite in a channel onetypically plots
thevelocity
as a function of theundercooling, resulting
in a double valued curve.Here,
weplot
thetip position
as a function of thevelocity resulting
in a non- monotonic function. In reference[14],
it was shown that the ST branch(where
yt increases forincreasing
vp, compareFig. 3)
is unstable while the second branch is stable(we
have verified that the cellscorresponding
to the second branch ofFig.3
are indeedstable). Thus,
thesteady
state solution we start with
(point
A inFig. 6)
is unstable. If we start from this unstable solution on the STbranch,
it ispossible
tojump
topoint
B on the second branch. The time for thisjump
isquite
small:2jump
-~1/Re
w where w is thegrowth
rate of theperturbation.
At B, the
tip position
of the cell will beessentially unchanged
but thetip velocity
vtip islarger
than the
pulling velocity
vp.Next,
thetip
of the cell will advance in the channel towards a hotterregion,
while thevelocity
of thetip
decreases(B
-C,~following
the dashedcurve).
Atpoint C,
thevelocity
of thetip
isequal
to thepulling velocity:
vtip " vp. There is no stablesteady
state solutionhowever,
so that the
velocity
continues to decrease and becomes smaller than thepulling velocity.
Asa result, the
tip position
decreases as well and the cell will follow thetrajectory
indicatedby
the arrow in
figure
6 on the dashed curve(C
-D).
The time for this process is of the orderof
lT/vtip,
which isquite large.
Once vi has decreased so much that thetip position
is smaller than thelargest possible
vi on thebranches,
we haveagain
thepossibility
of ajump
to the second branch(D
-E).
This will
finally give
us alimiting cycle
D - E - C -D,
as sketched infigure
6by
the dashed curve. The averagevelocity
of the cellduring
this limitcycle
should be thepulling velocity
vp and theperiod
of thecycle
will of the order oflT/@.
The selection of thepoints
D and E on the solution branches are not known at the moment
(one
should solve the full non-linearproblem),
butperhaps they
will be selectedby
the condition = vp. Notethat,
since yt is related toit,
the width of the cell will(slowly)
oscillate.Let us conclude with a final word on
sidebranching
in dendrites. Karma and Pelc6 have ar-gued
that theiroscillatory instability
could be a mechanism for the sidebranching
in dendrites.This idea of a linear
Hopf instability
from cells to dendrites which leads tosidebranching
does not agree,however,
with thegeneral accepted phenomena
of free space dendrites. First ofall,
one has found that the free space needle islinearly
stable. Sidebranchgeneration
can beexplained
if one introduces a noise-driven mechanism.Secondly,
unlike the case of cellular structures, dendritesdepend
verystrongly
on theanisotropy
of thecrystal.
We therefore do not believe that theoscillatory instability
could lead tosidebranching.
In
conclusion,
we havepresented
numerical results on thestability
of cells in the one-sided model of directional solidification. We show that our programproduces
aninstability
forlarge
values of the thermal
length.
We also showthat,
for some values of the parameter, we find anoscillatory instability.
Acknowledgements.
One of us
(E.A.B.)
has beensupported by
the Minist4re de la Recherche et de laTechnologie.
Part of the work of E.A.B. was done
during
a visit at IFF-KFA Jiilich. We would like toacknowledge
useful discussions with H. Levine.References
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