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The oscillatory instability in rapid solidification
Herbert Levine, Wouter-Jan Rappel
To cite this version:
Herbert Levine, Wouter-Jan Rappel. The oscillatory instability in rapid solidification. Journal de
Physique I, EDP Sciences, 1991, 1 (9), pp.1291-1302. �10.1051/jp1:1991207�. �jpa-00246412�
Classification Physics Abstracts
44.30 68.45 81.30F
The oscillatory instability in rapid solidification
Herbert Levine and Wouter-Jan
Rappel
Department
ofPhysics,
Institute for Nonlinear Science,University
of Califomia, SanDiego,
La Jolla, CA 92093, U-S-A-(Received 4 January 1991, revbed 25
April
1991,accepted
24May 1991)
Rksumk. Les
bquations
habituelles de la solidification directionnelle sont modifibes dans le cas de vitesses detirage
blevdes(solidification rapide).
Apartir
de cesd(uations,
nous ddcrivons une mdthodenumdrique
pouranalyser
la stabilitd des structures cellulaires obtenuesnumdriquement.
Ces cellules
prdsentent
une instabilitd oscillatoire, cequi prddit
l'observation derdgions
en forme de bandes dansl'expbrience.
Lalargeur
de ces bandes, que nous avons estimde, est I peuprds
enaccord avec celle observde
expdrimentalement.
Abstract. We modify the usual directional solidification
equations
for the case oflarge pulling
velocities
(rapid solidification).
Using theseequations
we describea numerical method to analyze the
stability
fornumerically
obtained cellular structures. We find cells which areoscillatory
unstable which will lead to the observation of banded
regions
in theexperiment.
The width of these bands are estimated and found to agreeroughly
with theexperimentally
observed ones.I. Inboduction.
It is well known that the process of
rapid
solidification can lead to variousinteresting
microstructures of the
solidifying
materials. One of thetechniques
consists of thescanning
ofa
high intensity
laser or electron beam over a surfaceof,
forexample,
a metalalloy.
The laser will melt the surface up to a certaindepth
and after thepassing
of the laser the melt will re-solidify.
Thespeed
of the solid-melt frontdepends
on the distance from the surface and is maximal at the surface[I].
One can model this type of solidification with the well-known
equations
of directional solidification[2]. Here,
oneplaces
a bath of a two-componentalloy
in anexternally
fixedtemperature gradient
and moves the bath with a certainpulling velocity
towards the(fixed)
cold contact.
Typically,
thepulling
velocities are of the order of micrometers per second. Ifone assumes that the laser will create a fixed temperature
gradient
we will have a directionalsolidification
experiment
withpulling
velocities close to thescanning velocity
of the laser. Of course, this allows for veryhigh pulling speeds.
The observed microstructures after the melt has solidified
depend
on thevelocity
of the laser and thedepth
of the melt.Typically,
one observes cellular and dendritic structures for small and moderate velocities[I].
Forhigher velocities,
one observes bandedregions
and for9
even
higher
velocities one hasmicrosegregation
free structures. These bandedregions
are theones we are
investigating
in this paper.The
high
velocities will alter the usual set ofequations
for directional solidification since wecan no
longer
assume localthermodynamical equilibrium
at the interface. It can be shown that a linearstability analysis
of the standardequations
of directional solidification modified forhigh pulling
velocities exhibit aHopf bifurcation,
I-e- a bifurcation where theeigenvalue
corresponding
to thegrowth
rate of theperturbation
has a non-zeroimaginary
part when thereal part crosses zero. This will result in the
growth
of anoscillating perturbation
of theinterface and will
give
rise to bandedregions.
In this paper, we will
present
a numericalapproach
to theproblem
ofrapid
solidification.We solve
numerically
the set ofequations
for directional solidification forsteady-state growth,
I-e- weneglect
the timedependent
concentration field.Afterwards,
we use the obtainedsteady
state cellular cells as theinput
for exactstability
calculations.Although
thisapproach
has been used for usual directionalsolidification,
it has never beenapplied
torapid
solidification. Our main result is that the cellular solutions can go unstable to a
Hopf bifurcation, presumably giving
rise to banded cellular structures.Kelly
andUngar [3]
have also found anoscillatory instability,
howeverthey
have used a different model for the interfacetemperature
and the modification of thepartition
coefficient(see
Sect.3)
forhigh pulling velocity.
This paper is
organized
as follows. In section 2 we review the basicequations
for directional solidification andmodify
theseequations
for the case ofrapid
solidification. In section3,
wereview the linear
stability analysis
andplot
theregions
ofoscillatory
andnon-oscillatory
instabilities for the system of Sisb. We describe how we can obtain numericalsteady
stateequations
in section 4 and how we cananalyze
theirstability. Finally,
in section 5 we will present and discuss our results.2. Basic
equations
and their modification.The basic
equations
for directional solidification are well known and are described in many papers. In this paper we willonly
consider the one sidedmodel,
where weneglect
the solute diffusion in the solid. In the framemoving
with thepulling velocity
uo we have for theconcentration field
c
~ 3c 3c
~~~~~°fi~&
uofi.y+u~
(fi Vc)~
=
(l k)
c~D
Here,
D is the diffusion constant in theliquid,
k is thepartition coefficient, i~
=
m~/G
is athermal
length (m~
is theslope
of theliquidus
andT~
is themelting temperature
of the puremelt), do
=
«T~/Lm~
is acapillary length («
is the surface free energy and L is the latentheat)
and K is the curvature. The total interfacevelocity
is uofiy
+ u~ where fi is the normal to the interface. Of course, we have u~ =0 for a
steady
state.In
deriving
the aboveequations
we have assumed localthermodynamic equilibrium
at the interface. Thisassumption
is correct for smallpulling
velocities but fails forlarge
velocities. In that case we have tomodify
the aboveequations.
As we will see, these modificationsgive
rise to a different linearstability
behavior and inparticular
there will now exist aHopf
bifurcation forlarge
velocities.Perhaps
the mostimportant change
within theequations
is that thepartition
coefficient k has to be modified forhigh
velocities. It will nowdepend
on thevelocity
and shouldapproach unity
in the limit ofhigh speeds.
In this limit the interface moves soquickly
that the solute can not diffuse out of the solid and will betrapped
inside thesolid,
hence the name« solute
trapping».
Inaddition,
one can introduce the mechanism of attachment kinetics which will describe at which rate the molecules will attach to thecrystal.
There are a number of models for the
velocity dependence
of k. We believe that the actual functionaldependence
of k on v will not mattergreatly
for our purpose,finding
theoscillatory instability.
Infact,
Coriell and Sekerka[4]
have shown that for anoscillatory instability
a non-zero derivative
3k/3u
is sufficient. We have chosen a modelproposed by Boettinger
et al.[5, 6]. They
introduce aparameter flo
which measures thedeparture
of k from itsequilibrium
(u
=
0 value and a parameter
Vo
whichmimici
the effect of kinetic attachment. In this paperwe will
only
consider the caseVo
= tx~, which means that the atoms attachinfinitely
fast and there is no kineticundercooling, although
an extension for different values ofVo
isstraightforward.
For the functionaldependence
of kthey
proposek~+flou
~~~~~
l+flou
~~~where
k~
is theequilibrium
value for u= 0.
Here,
u is the total normalvelocity
of the interface. As we can see, kapproaches unity
as u increases.Boettinger
et al. showed that for a flat interfacemoving
withvelocity
uo thetemperature
at the interface will begiven by
where
m(vo)
= mE
1 ikE k(I
In(k/kE))i (4)
Here, Vo
measures the effect of attachment kinetics. As mentionedbefore,
we will choose Vo = tx~ in the remainder of this paper.Equation (4)
describes thechange
in theliquidus slope
due tonon-equilibrium segregation.
As in[7]
we suppose that the temperature at the interface isgiven by
the aboveexpression
for the flat interfaceplus
a Gibbs-Thomson term :The above modifications will
change
the standardequations
for the directional solidifi- cation. As in[8]
we go into the framemoving
with thepulling velocity
uo and measurelength
in units of A
/2 (the wavelength
of thecell),
concentration in units of c~ and time in units ofA~/4D. Then,
for the one sidedmodel,
we have~ ~ 3c 3c
~~~
~~fi"A
(fi Vc)~
=
(l k(u))(2 pelf y
+u~)
c~~~
k()) f~ "*
~ ~~~where y *
=
2
«Tp/Lm(u)
c~ A, pe=
~~
,
the Peclet number and
f*
=
2 m
(u)
c~Tp/GA.
4 D In our rescaled units the above
equations
readk~
+flu
~~~~
l +
flu
~~~where
p
=po
2Dj> (8)
3. Linear
perturbation theory.
In this section we will review linear
perturbation theory
for the set ofequations (6)
asdescribed
by
Merchant and Davis[7]
andapply
the results to an actual system. As our systemwe will choose the Sisb system described in
[3].
We will see that for this system we will not have anoscillatory instability
if we do notmodify equations (I),
I-e- when we choosepo
=
0.
It is easy to see that
equations (6)
have a solutioncorresponding
to a flat interface~ ~
l
~-2pejy-yoj
°
k
~~~
Yo "
~
k where
k~
+ 2pep
~
l + 2
pep
~~~~We
perturb
the flat solutionc = co + eci e~~~ e~ QY e~~
(I I)
y = yo + eyi e~~~e~~
(12)
where
Q
= Pe +~
(13)
and em I.Substituting
theseexpansions
in the aboveequations
fork(u)
andm(u)
andlinearizing
fore we get
k(u)
=k
+ eAj wyi + o
(e2)
m
(U)
= ni +
8A2
WYI + O(8~) (14)
where
p (I k~) Ai
=
2Pe(1
+fl
~Ai
In(k/k~)
~~
ni
(k~ )
~~~~ni=ni~(1-_~[~ (k~-k(i-in(k/k~)))j.
Next,
we substituteequations (14)
inequations (6)
and we findk~°~~l~i~~'~)~~~~j ~~
+
[~-2pe ~~-2pe ~~ w-2pe(1-k)( +yq~) +4pe~~ ~~=0 (16)
k
k k f k
where
2
«T~
~'
LmC~
A(17)
2
nic~ TM f
"
~>
To find the neutral
stability
curve we set w = 0. This willgive
us a closed curve inparameter (A
vs. u)
space inside which the flat interface is unstable with a pure realeigenvalue.
However,
it is alsopossible
that anw with non-zero
imaginary part
satisfiesequations (16).
If we write
Q
asQ
= pe +
R,
we get a third orderequation
for R from which we can solve forw. For each
wavelength
we get three solutions for w which the determine the nature of theinstability.
If the real part ofw crosses zero and its
imaginary
part is non-zero we will have anoscillatory instability
and we will encounter aHopf
bifurcation. As we can see, a non-zeroAj
orequivalently
an non-zero3k/3u, gives
us a cubicequation
and for realistic parameter values we will find aHopf
bifurcation.As an
example,
we have chosen the Sisb system as described in[3].
The relevant material parameters aregiven
in table I. We haveplotted
the boundaries of thestability regions
for three different values offlo
infigures
1, 2 and 3. Infigure
Ifl
o = 0 and we see that there is no
oscillatory instability.
Theinstability
in the unstableregion
is the Mullins-Sekerekainstability
and we expect to find cells
and/or
dendrites inside thisregion.
Forflo
= I
x10~?
andflo
= I x10~~ however,
we do find an
oscillatory instability
forhigh
velocities(see Figs.
2 and3).
There is a fundamental difference between the
figures
2 and 3. Infigure
2flo
= I x 10~?)
maximum of the neutral
stability
curved lies below the minimum of theoscillatory
unstableregion. Therefore,
if one increases thevelocity,
oneexpects
that the cellular structures which form inside the neutralstability
curve bifurcate back to aplanar
interface. Thisplanar interface,
in turn, willundergo
aHopf
bifurcation if one increases thevelocity
even more.Since the
planar
interface will go unstable for aperturbation
with= tx~, the
planar
interface will oscillate in the direction of thegrowth velocity.
The concentration left behind in the solidTable I. Parameter values
of
the Sisb system used in the numerical calculation.do
=
7.72 x lo ~~ m G
= 1.33 x
166 K/m T~
=
427 K mt =
452
Klat9b
c~ = I x
10~~
atfb D=
1.5 x lo ~~
m~/s
k
=
0.023
~=0
lo ~
~°
stable
j~
~
(
io 6~/
unstable
>
io 5
lo 4
lo .I lo ° lo I lo 2
~w
(~llll)
Fig. I. The
regions
ofinstability
for po 0.J=lx10~~
lo 8
~° ~
oscillatory unstable
~
E
~ lo 6~
>
lo 5
io 4
10 .1 10 ° 10 10 2 10 3 10 4
~w
(~llll)
Fig. 2. The
regions
of instability for po = I x 10~~depends
on thevelocity (k
is a function ofu)
and we expect to see bandedregions.
Infigure
3 however(po
= I x
lo~~)
the cellular structures should not bifurcate to a stableplanar
interface since thetop
of the neutralstability
curve isalready
in theoscillatory
unstableregion. Instead,
one should find acomposite pattern
of bands of cells.Although
we need aJ=lX10~~
oscillatory unstable
lo ~
~
~s~
~~ ~unstable
>
lo 5
~~/o
'i lo ° lo I lo 2 lo 3 lo 4~w
(~Lm)
Fig.
3. Theregions
ofinstability
forpo
=
I x 10~~
nonlinear
analysis
to examine thesepatterns,
a banded cellular structure seems to be a resonable guess.4. Numerical method.
Next,
we will describe how we can obtain numerical solutions ofequations (6).
Since this has been described elsewhere[9, 10]
in greatdetail,
we will be very brief. Once we have found asteady
statesolution,
weperturb
this solution with a normalshift,
linearize about theamplitude
of this shift and solve theresulting eigenvalue problem.
The trick to solve
(6)
in a numerical efficient way is to rewrite theequations
as aintegro-
differentialequation
and solve for the(unknown
andfree) boundary.
We will do this for both thequasi-static approximation
and for the fullequation.
In thequasi-static approximation
weneglect
the time derivative term in the diffusionequation.
In the
quasi-static approximation
we find(fl+y*K(s))
= i-
@+y*K(s'))(4"v'G)ds'+
+ 2
pek(u @
+ y * K
(s'i nj
G ds'+
I
[k(u) @
+ y * K
(s') (()
+ y * K
(s')
G ds'(18)
where the Green's function G is the solution of
V~G
+ 2 pe ~~= 3
~(x x') (19)
°Y
The
explicit
form of G isgiven
in[8].
For the non
quasi-steady
case we go back to the rest frame and we find(Y(S,
t)
2 Pet)
~ ~ ~ ~~ ~~ ~
j d~,
~
d~i
(Y(S', t')
2Pet')
~ ~ ~ ~~, ~,
f*
'-~
f*
'fi'. V'G
(x(s,
t), x'(s', t')
t,t')
+ ds'~ dt'( (~(~" ~') j ~P~~'~
y * K(s',
t')
x#
-w
where G is a solution of the full diffusion
equation
V~G
~~=
3
~(x x')
3(t t') (21)
To find
steady
state solution weparameterize
the(unknown) boundary
with Npoints
ofequal ardength.
Ourindependent
variables are then the normalangles
at themidpoints
of theequal ardength
sections and theposition
of thetip.
We solve theintegro-differential equation
on the
points
ofequal ardength,
except at theendpoints (x
=
0 and x
=
I)
andrequire
that theslope
vanishes at both thetip
and the tail. Once we have found a solution we can fit aspline through
the solution to obtain a smaller discretizationstep.
We
perturb
thesteady
solutionby adding
the normal shiftx(s)
=
xo(s)
+ho (s)
3(s,
t(22)
where we assume that 3
(s,
t= 3
(s)
e~~ and 3(s)
« I. We substitute thisperturbation
in(18)
and linearize in 3. This
gives
us the rather messylooking equation
for thequasi steady
stateapproximation
ids'
yKo +~°
(3(s') fi(
V' + 3(s) b0'
Vb~'
V'G +f
+
@
y
(3"(s')
+Kj
3(s')) hi
V'G+
lYKo+1°1(-3(S)to.vG+Ko3(S)no.vG)1
-2pek
ds'b~ yKo+~° (3(s')fi(.V'+3(s)bo.V)G f
+
(yKo +9
(- 3'(s') ijG
+4~
Ko
3(s') G)j
+
j- Y(3"(S')+ K13(s'))j
=w
ids'((I-k)~~°+yKo~ 3(s')G- ~9+yKo) bo.VGA~3(s')
f f
2
Pen)- °
+ YKo GA 3
(S)
+ 2Pekni1 °
+ YKo GA 2 3(S 1 (23)
Once we have chosen M
points
withequal arclength ds,
the discretization of theintegrals gives
us a set ofequation
of the formM M
£
A~j 3j = w
£
B~y 3j.
(24)
j o j o
This is
just
anordinary eigenvalue problem
forw and can be solved with one of the standard numerical
packages.
For the non
quasi-static approximation
weproceed along
the same lines. Substitution of theperturbation
in(20)
andlinearizing gives
usids' ~ yKo+~° (3(s')b(.V'+3(s)fro.V)b(.V'G(w)+
f
+
fi y(3"(s')
+Kj3(s'))j hi V'G(w)
+ yKo +
) (- 3'(s') j
V'G(w)
+ Ko 3
(s') hi
V'G(w ))j
-2pek ds'fi~ yKo+~° f~ (3(s')fi(.V'+3(s)fro.V)G(w)
+
4~( @
y(3"(s')+ Kj3(s'))j G(w)
+
(yKo+9 (- 3'(s') ijG+
fi~ Ko3(s') G(w))j
+
j- Y(3"(s'i
+K13(S'ii)
= W
ids~lkli°+ Kol 3(S~IG(Wi- li°+ Kol no.vG(WiA23(S~i
2
pen(
~° +yKo)
G(w ) Ai
3(s')
+ 2peknj
~° +yKo)
G(w ) A~
3(s')j (25)
f f
where an
explicit
form ofG(w )
isgiven
in[8]. Upon discretizing
theintegrals
we get anequation
like£
MCq(w
3~ = 0(26)
j =o
where C is a function of w and therefore in
general complex.
Tosatisfy
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. Infact,
we can look for theeigenvalues corresponding
to different modes.S. Results and discussion.
The
quasi-static stability
calculation can be checked in several ways. First ofall,
we know from the linearstability analysis exactly
for whichvelocity
andwavelength
the flat interface goes unstable. We have checked that ourstability
program doespredict
theright
onset forinstability
of the flatinterface,
both for small velocities andlarge
velocities.Furthermore, carrying
out theexpansion
described in section 3 to third ordergives
us anequation
for theamplitude
A of the cell of the form~ =aiA+a~A~ (27)
Depending
on thesign
of a~, the so-called Landaucoefficient,
we have a sub- orsupercritical
bifurcation. It can be shown that for the one sided model and for values of k ~ 0.45 we will have a subcritical bifurcation
[11]. Indeed,
we do find a subcritical bifurcation at onset. The lower branch of the subcritical branch has to beunstable, regaining stability
when it bends in the forward directionagain.
We have checked this behavior for the system at hand.The full
stability
program can be checked aswell, using
the flat interface as oursteady
state solution. The linearstability predicts
for which values of u and A the flat solution will losestability
to a cellular structure, willregain stability
and losestability again
to anoscillatory instability.
We are of courseespecially
interested in the lastinstability.
Let us take the case of
po
= I x
10~?
In table IIwe have listed the
predicted eigenvalues
from the linear
stability
calculation of section 3 and the obtained values from our numericalanalysis.
We see that the agreement is excellent. We have also checked the lower branch of the subcritical bifurcation at onset and have found that the lower branch is unstable while theupper branch is
stable,
which is asexpected.
Table II.
Eigenvalues for d#ferent flat interfaces (flo
=
I x
10~?).
~
(Jll/Sl
A(iLJlll
t°numencal t°linearstabil,ty
0.023 5 3.51 3.52
0.32 5 89.8 + I 54.3 89.9 + I 56.0
0.9 5 15.3 + I 1673.7 9.I + I 1681.6
Next, we have examined the
stability
of the cellular structures forhigh velocities,
I-e- at thetop
of the neutralstability region.
Forflo
=
I
x10~~
we have indeed found an
oscillatory instability
for the cellular solution. Infigure
4 we haveplotted
twosteady
state solution withu =
2.3m/s
and u=2.32m/s.
Here x and y are theposition
of the solution in thecomputational
box(the wavelength
of the solution is thus 0.15 ~Lm). We can search for the value of wcorresponding
to any mode. We expect the « zero mode whichcorresponds
to a translation of the interface in the direction of thegrowth velocity
to be the first mode to go unstable. The results of our numerics for this mode arepresented
in table III and the modesare
plotted
infigure
5. We have calculated w for different number of discretizationpoints
of the interface to check that the answer converges. We see that the real part of thegrowth
ratew crosses zero somewhere between u
=2.3m/s
and u=2.32m/s. Thus,
the solutioncorresponding
to an u = 2.3m/s
is stable while the solutioncorresponding
to an u = 2.32m/s
is unstable with aneigenvalue having
a non-zeroimaginary
part. This solution is thusoscillatory
unstable The other modes were found to stable.The cellular structures with
flo
= I x 10~ ? however are found to be
stable,
even at thetop
of the unstableregime. This,
of course, is related to the fact that in the case oflarger
flo
theplanar
interface can restabilize before itundergoes
theHopf
bifurcation.1.34
v=2.32x10~
v=2.3x10~
~
/s~
-l.35 i'>~~'~~.00
1.50 3.00 4:50 6.00 7.50x10.2X
(~m)
Fig. 4. The steady state solutions for v
=
2.3 m/s and u = 2.32 m/s
(po
=
I x
10~~).
Table III.
Eigenvalues for
the cells infigure
4for
ad%ferent
numberof
discretizationpoints of
theinterface (A
= 0.15 ~Lm,fl
=
I
x10~~).
v
(m/s)
w(50 points)
w(100 points)
w(150 points)
2.3 0.I I + I 1.46 0.15 + I 1.41 0.15 + I 1.40
2.32 + 0.041 + I 1.43 + 0.036 + I 1.44 + 0.035 + I 1.44
We can also estimate the width of the
resulting
bands. This isjust
thegrowth velocity
times theperiod
of oscillation. Forw we take the value
corresponding
to themarginal
stable mode(I.e.
where the realpart
isequal
tozero).
Since we measure time in units of ~/4 D we havearuo A~ W
=
(28)
In the above case we have
u=2.32m/s,
A=0.l5~Lm
and w~l.5. Thus we findW 3 ~Lm which is close to the
expeRmentally
observed bandwidths. Of course this isjust
arough
estimate since we have chosen aquite arbitrary
value offlo. Nevertheless,
the resultmakes sense in a
physical
way.In
conclusion,
we havedeveloped
a numerical way to examine thestability
ofsteady
state cellular structures for the one-sided model. We have found that modifications due tolarge pulling
velocities can result inoscillatory
unstablecells, depending
on our modificationparameter
flo. Also,
theresulting
bandwidths agreeroughly
with theexperimentally
observedones. Of course this
approach
cannotexplain
thealternating
bands with and without structureas observed in the
experiment.
For the exactdynamics
of the cells we have toperform
anonlinear
analysis.
xlo.I -o.70
0.80
o.90
-1,oo
V=2.32X10~
~ v=2.3x10~
i>~ ~'~°
-l.20
1.30
-1.40
0.00 1.50 3.00 4.50 6.00 7.50x10.2
X
(~m)
Fig.
5. The modes corresponding to the tigenvalues in table III.Acknowledgments.
This work was
supported
inpart by
DARPA Grant No. N00011-86-K-0758.References
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