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Solutal convection and morphological instability in directional solidification of binary alloys. - II. Effect of
the density difference between the two phases
B. Caroli, C. Caroli, C. Misbah, B. Roulet
To cite this version:
B. Caroli, C. Caroli, C. Misbah, B. Roulet. Solutal convection and morphological instability in direc-
tional solidification of binary alloys. - II. Effect of the density difference between the two phases. Jour-
nal de Physique, 1985, 46 (10), pp.1657-1665. �10.1051/jphys:0198500460100165700�. �jpa-00210114�
Solutal convection and morphological instability
in directional solidification of binary alloys.
II. Effect of the density difference between the two phases
B. Caroli (+), C. Caroli, C. Misbah and B. Roulet
Groupe de Physique des Solides de l’Ecole Normale Supérieure (*), Université Paris VII, 2 place Jussieu, 75251 Paris Cedex 05, France
(Reçu le 11 mars 1985, accepté le 10 juin 1985)
Résumé. 2014 Nous étendons l’analyse de perturbation du couplage entre déformation de front et convection solu- tale présentée dans un article récent [3] pour tenir compte de l’effet de l’« advection », c’est-à-dire de l’écoulement induit par la variation de densité qui accompagne la solidification. Nous étudions le déplacement de la bifurcation à partir du régime stationnaire à front plan. Nous montrons que, le long de la branche convective, l’effet de l’advec-
tion est du même ordre que celui du couplage convection-déformation, alors que, le long de la branche morpho- logique, il est largement dominant.
Abstract
2014We extend the perturbative analysis of the coupling between front deformation and solutal convec-
tion performed in a recent article [3] to include the effect of « advection », i.e. of the flow induced by the density change associated with solidification. We study the resulting shifts of the bifurcation from the stationary planar
front regime. We show that, for the convective branch, the effect of advection is comparable to that of the convec-
tion-deformation coupling, while, for the morphological branch, it is by far dominant Classification
Physics Abstracts
61.50C - 47.20
-64.70D
1. Introduction.
It is well known that when a dilute binary alloy is
submitted to directional solidification (i.e. pulled
at constant velocity V in an external thermal gradient),
the structure of the solid and the morphology of the growth front are primarily controlled, for systems with atomically rough solid-liquid interfaces, by
solute diffusion in the liquid phase. At small pulling velocities, the growth front is planar; beyond a
critical velocity Vc (which depends on the thermal
gradient 6 and on the concentration far from the front in the liquid, C ex)’ the front develops a periodic
cellular structure, associated with the Mullins-Sekerka
instability [1, 2].
However, such a system is never free from hydro- dynamic motion in the liquid phase. This flow is induced by two mechanisms :
(i) the system is submitted to a thermal gradient
(*) Associe au C.N.R.S.
(+) Also : Departement de Physique, UER de Sciences Exactes et Naturelles, Universite de Picardie, 33, rue Saint- Leu, 80000 Amiens, France.
Moreover, solidification of an alloy produces, at the interface, an excess or defect of solute which induces
a concentration gradient in the liquid ahead of the front In the presence of gravity, these gradients give
rise to buoyancy forces and may thus induce a con-
vective flow ;
(ii) the densities of the liquid and solid phases
are different The solidification of a given mass of liquid is therefore associated with a volume change,
which must be compensated for by a hydrodynamic
flow in the liquid In order to make a clear distinc- tion from buoyancy-induced effects, we will conven- tionally call this current an « advective flow ».
Hydrodynamic flows and front deformations are
coupled In a recent article [3] (hereafter referred to
as (I)), we studied the effect of the coupling between
front deformation and solutal convection on the
position of the bifurcation from the regime with pla-
nar front and quiescent liquid in the case where the
solid is pulled vertically, the thermal gradient is stabilizing, and the solid and liquid densities are
assumed to be equal.
We showed that, close to the convective and mor-
phological bifurcation, the effective coupling between
Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphys:0198500460100165700
1658
convection and front deformation is small at usual values of the thermal gradient, and that a first-order
perturbation treatment is well justified We found,
in particular, that the convection-induced shift of the Mullins-Sekerka (MS) bifurcation is, under usual experimental conditions, extremely small.
In this article, we want to study the ways these results are modified when advection effects are taken into account It is clear that advection couples to
front deformation : indeed, the corresponding flow
must be normal to the solid surface. Thus, a defor-
mation of the front distorts the flow, this modifies the transport of solute from (or towards) the inter- face, and that in turn reacts on the front deforma-
bility.
Of course, the relative density changes 8
=(ps - PL)/PL are small (typically, of the order 10-2 to, at
most, 10-’) and so are usually considered as negli- gible. However, advection effects are unavoidable
(even in microgravity experiments). Moreover, since
it is found that the bifurcation shifts due to the convec-
tion-deformation coupling are small, the question
arises of comparing them to those induced by advec-
tion.
In § 2 we write down the equations describing the
solidification problem in the presence of both advec- tion and solutal convection and calculate the solution with a planar stationary solid front We set up the linear stability analysis of this solution and write
down the condition of existence of marginal modes.
In § 3 we study the effect of advection on the decou-
pled MS and convective bifurcations.
In § 4, we include the convection-deformation
coupling and calculate the position of the bifurca- tions in a first-order perturbation approximation.
2. Dynamical equations and planar stationary solu-
tion
We assume that the dilute binary mixture is pulled vertically (in the (- 2) direction) at velocity V, and
that the system is quasi-infinite in the (x, y) directions.
Following (I), we also assume that the thermal gra- dient is stabilizing and neglect thermal expansion (i.e.
thermally-induced convection).
We define the following dimensionless variables :
where the tilded variables are the physical ones.
f, ti, dr ,, C are the temperature, liquid velocity,
front velocity, and solute concentration in the liquid
is the relative density change at solidification (for
most materials, s > 0). D is the solute diffusion coef-
ficient in the liquid, TM the melting temperature of the pure solvent, Coo the solute concentration in the
liquid far from the front, and K the equilibrium solute
distribution coefficient
Following (I), we neglect, in the non-dimensionaliz- ed equations of the problem, all terms proportional
to D/Dth and to D/v (where Dth is a heat diffusion coef- ficient and v the kinematic viscosity of the liquid).
We also neglect diffusion in the solid phase, treat the liquid as incompressible, and assume quasi-instan-
taneous local thermodynamic equilibrium on the
front
The system is then described by the following equa- tions :
(i) In the solid phase :
Heat diffusion :
(ii) In the liquid phase:
Heat diffusion :
Solute diffusion, :
(z is the unit vector along Oz)
Mass conservation :
Momentum conservation :
a PL TC- is the solutal expansion coefficient;
PL
the gravity g is positive.
(iii) At the interface (z
=zs(x, y, t)) : No-slip condition :
where n is the unit vector along the normal to the front pointing into the liquid.
Mass conservation :
Continuity of temperature :
Heat balance :
where n
=ks/kL is the ratio of the thermal conducti-
vities.
Concentration balance :
Curvature-induced local interface temperature shift :
M
=ML CwIKTm, where mL is the slope of the liquid-
us curve of the mixture at (T
=T M, C
=0).
r
=y VIED, where y is the solid-liquid surface tension, C the specific latent heat of fusion, and X
the curvature of the front, defined as positive for a
convex solid
Moreover, we assume that the hydrodynamic flow
is free at infinity in the liquid (z -+ oo), where the
pressure is fixed.
When comparing equations (1-12) with the corres- ponding equations of (I), it is seen that taking advec-
tion into account results in the following :
-
a redefinition of the non-dimensional variables that is, a rescaling of the diffusion length and time of the system which become, respectively, D/(1 + 8) V and D/(1 + 8)2 V2 ;
-
a factor (1 + s)- 3 in the coefficient of the second term of the hydrodynamic equation (7). As shown in
(I), this coefficient is directly related to the Rayleigh
number for our problem
where
and the (1 + E)-3 factor naturally accounts for the rescaling of the diffusion length;
-
the presence of a term proportional to 8 in equation (9), which describes how the volume defect
resulting from solidification must be fed by advection.
We first look for a stationary solution of the above
equations corresponding to a planar front Choosing
the origin of the z-coordinate at the front position,
one finds that this solution is described by
GL is the positive dimensionless temperature gradient
in the liquid :
with 6 the physical thermal gradient
We are interested in the thresholds of instability
of this solution, so we want to study its linear stability.
That is, we assume that the planar front undergoes
a small deformation of wavevector a (chosen along the arbitrary x-direction)
This induces variations of wavevector a and growth
rate a of the various fields. One then standardly expands equations (3.12) to first order in these varia- tions. The corresponding equations, which are written
and solved in the Appendix, provide the « dispersion
relation » a
=f (a). We assume that the bifurcations
we study are not oscillating. As shown in (I) and
confirmed by numerical results [4], this is indeed true in the absence of advection, except at unrealistically
small thermal gradients or for very small values of the distribution coefficient K. Since the parameter e, which measures the strength of advection effects, is
small (s 10-1), one may reasonably expect that the introduction of these effects does not alter the character of the bifurcations. This can be proved explicitely [5], to first order in 8, with the help of a perturbation expansion.
The equation determining the neutral modes of the system then reads (see Appendix) :
where
with
The functions A and B which appear in equation (19)
are the same as those appearing in (I) ; the presence of advection changes their argument from R,, into ,k.
The new quantity C(.,k, a) is defined in the Appendix.
3. The uncoupled bifurcations.
Following the analysis performed in (I), we first
define the « pure » or uncoupled bifurcations from the planar solution, namely :
- the pure morphological one, i.e. the MS bifur- cation at zero gravity, and
- the pure convective one, Le. the onset of convec-
tion in the liquid ahead of a planar non-deformable solid front.
In this section, we study how these uncoupled
bifurcations are shifted by advection.
1660
3.1 ADVECTION-INDUCED SHIFT OF THE MS BIFUR- CATION.
-The equation for the corresponding
neutral modes is obtained by taking the l§’ -+ 0
limit of equation (19). In this limit (see Appendix)
where
The neutral mode equation (19) then becomes
The determination of the bifurcation proceeds
in the standard way : one looks, at fixed p, for the position CbMS, aMS) of the minimum of the neutral
curve 1Jc(a).
The critical wavevector is the solution of
Equations (24) and (25) provide a parametrization
of the bifurcation curve -Gms(P).
Since E 1, they can be, to a good approximation,
solved to first order in £. One obtains :
where the critical wavevector is, to the first order, unshifted It is given by
With the help of equations (20), (21), and (27),
we obtain from equation (26) the relative shift of the bifurcation at constant G, V :
As discussed in (I), for not-too-small thermal gra- dients (typically 6 > 1 K/cm) and not-too-large pulling velocities (V 1 cm/s)
and
That is, on the small velocity side of the bifurcation
curve CII(V), which corresponds to usual directional solidification conditions,
-
if 8 > 0 (ps > PL) the effect of advection is
destabilizing : the MS bifurcation for given Coo occurs
at smaller velocities,
-