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Kinetic dendrite in the boundary-layer model

D. Temkin, J. Géminard, P. Oswald

To cite this version:

D. Temkin, J. Géminard, P. Oswald. Kinetic dendrite in the boundary-layer model. Journal de

Physique I, EDP Sciences, 1994, 4 (3), pp.403-409. �10.1051/jp1:1994147�. �jpa-00246916�

(2)

Classification Physics Abstracts

61.50C 61.50J 81.30F

Kinetic dendrite in the boundary.layer model

D. Temkin

(*),

J. C. Géminard and P. Oswald

Ecole Normale Supérieure de Lyon, Laboratoire de

Physique,

46 Allée d'ltalie~ 69364 Lyon Cedex 07, France

(Received 29

September

J993,

accepted

3 December1993)

Abstract. Within trie

boundary-layer

model and

by taking

into account only interface kinetics

(isotropic

or

anisotropic),

we find a contmuous set of « kinetic » dendrites. This solution exists at

arbitrary supercooling

A in the 2D- and

3D-axisymmetric

cases and reduces to the usual dendrites with

parabolic

tails at A ~ l, and «

angular

» dendrites at A ~ l. In contrast with classical Ivantsov dendrites, there are upper limits for

growth

velocity and tip curvature at each

supercooling

A.

Ivantsov

Ii

was the first to show that there exists a contmuous set of

stationary

needle-like solutions to the

problem

of the free

growth

of a

crystal.

These solutions are obtained

by neglecting capillarity

and interface kinetics and exist

only

at dimensionless

supercoohng

A smaller than 1. To find a

smgle

dendrite

(experimentally, only

one is

observed),

one needs to introduce a

length

in the

problem. Usually,

the

capillary length

d~ is introduced and the solution is found

by disturbing

the Ivantsov

parabolic

solution

using

a

singular perturbation

method. In this case, and in two

dimensions,

the

tip velocity

v is

proportional

to

(D/d~ A~

at A « 1, where the constant of

proportionality depends only

on the

anisotropy

of the surface tension

[2].

D is the diffusion coefficient.

This choice of the

length

is not unique because there is another characteristic

length

connected with interface kinetics : that is, D/w where w is constructed from the interfacial kinetic coefficient

p.

The ratio

d~

= d~ w/D of these two

lengths

determines which of them is

more important. In pure

materials,

D is the thermal

diffusivity

in the

hquid,

whereas m

alloys

it

is the solute diffusion coefficient in the

liquid.

If

d~

» 1, one expects

capillanty

to be more

important

than kinetics. In the opposite case,

dt

« 1, kinetics should dominate surface tension

effects. The parameter d~ is a matenal constant which can be evaluated. For

example,

d~

mû-1 m pure materials as Ni

(by taking

p =160cm/s/1ç

[3])

or succinonitrile

(with

p

=

20cm/s/K [4]).

In contrast, d~ is

usually

much

larger

than m

alloys

because the chemical diffusion coefficient is much smaller than the thermal

diffusivity.

Nevertheless,

(*) Permanent address: I.P.Bardin Institute for Ferrous Metals, 2Baumanskaya Str. 9/23,

107005 Moscow, Russia.

(3)

404 JOURNAL DE PHYSIQUE I N° 3

d~ can also be small in impure materials such as discotic columnar

liquid crystals.

For instance,

we measured

previously

in CBHET p

w 1.3 x 10~ ~ cm/s/K which

gives dt

- 0.5

[5].

In ail

these

examples

we thus expect kinetics to be

significant

even at small

supercooling.

For these reasons, we found it

interesting

to

study

the case

dt

=

0

corresponding

to zero surface tension.

This

problem

has

already

been discussed

by

Lemieux et ai.

[6]

and _by Brener et ai.

[7].

Both calculations are carried out

using

a full non-local

approach

and start from the Ivantsov solution.

This

requires

that kinetic

undercooling

is small. Lemieux et ai. found

analytically

for

isotropic

kinetics a contmuous

family

of solutions m the limit of small A, while Brener et ai. found a discrete set of solutions which are selected

by

kinetic anisotropy for A ~ l. In this article, we

analyze

this

problem

for

arbin-aiy supercooling

A and

arbitrary

kinetic

undercooling.

We use the

boundary-layer

model

(BLM)

which has been shown to

give quahtatively

correct results in

many situations

[8].

Another

important point

is that we do non use A>antsov's solution as the starting approximation.

In the two-dimensional one-sided model

(no

diffusion in the

sohd)

the BLM

equation

for isothermal and

steady-state

solidification of a dilute

alloy

reads

k( V(1 U)

cos o

~~~

K sm o ~

l~~

[1 +

U(1/k~ -1)]

cos o [1 +

U(1/k~ -1)]

K d KU dU

~

o

(1)

~ V do

cos o [1 +

U(1/k~ 1)]

where V

=

u/w and K

=

J~D/w are

respectively

the dimensionless

velocity

in the z-direction

and the curvature of the interface. The

angle

between the z-axis and the normal to the front is

9 and K is the curvature defined

by

K

=

d9/ds where s is the

arclength along

the interface measured in units of D/w. The dimensionless

undercooling

at the interface U is defined to be U

= (C,~~

C~)/[C~(1/k~-1)]

where C,~~ and

C~

are concentrations of solute at the interface and in the

hquid

far from the interface ;

k~

is the

equilibrium

distribution coefficient.

Equation (1)

is still valid for pure materials and thermal

growth.

In this case, U

= (T~~~

T~)/(L/c)

where L is the latent heat per unit volume and c the heat capacity.

k~

must also be set

equal

to in

equation (1)

which grues the same

equation

as that

previously

used

by Langer

and

Hong [9].

The second

important equation

comes from the Gibbs-Thomson relation. Without anisotropy

effects,

it is

U

=

A

d~

K V cos 9

(2)

with

d~

= d~ w/D. In the chemical case, 4

=

(C~~ C~ )/[C~(1/k~ 1)]

where

C~~

is the

equilibrium

solute concentration m the

liquid

at the temperature chosen. The

capillary length

is d~ =

yT~/L )/ [mC

~

l/k~ )]

and w

=

pmc

~

l/k~

where y is the surface stiffness and

m the

slope

of the

hquidus

fine. In the thermal case A

=

(T~ T~ )/(L/c ),

d~ =

yT~ c/L~

and

w =

pL/c.

One sees

immediately

that in both cases

d~

can be wntten m the

general

form

dt

=

°'~j~ (3)

Equations (1)

and

(2)

can be

generahzed

for 3D axisymmetnc

growth

as follows

[8]

k( V(1 U)

cos 9

~~~ ~

~~~

~

Kj

sin 9 ~

~~

[l +

U(1/k~ )]

d9 cos 9[1 +

U(1/k~

1)]

K d

~~i

~ dU

1=

o

(1~)

~ VR d9

cos 9 [1 +

U(1/kE 1)]

d9 '

(4)

U

= A

d~(Ki

+

K~)

V cos 9

(2~)

where

Kj(9)=d9/ds

and

K~(o)

=

(sin9(/R(9)

are the two

principal

curvatures and

R(9

=

o dt(cos

t

)/Kj (t)

is the radius of the circular section normal to the z-axis

(growth

direction).

Let us now discuss the solutions to

equations (1)

and

(2)

in the

limiting

case

dt

=

0

corresponding

to zero surface tension

(2D case).

To

simplify,

we further assume that

à « and k~ =

1. In this

limit,

the BLM is not

stnctly

vahd but it

gives qualitatively

the

right physics

as shown

by Langer [10].

We can now substitute U

by

A in ail terms of

equation (1)

besides

dU/d0=V

sm 9 in the last term of

equation (1).

We thus obtain

ÎÎ

~

k

~n 9111~

~ ~~~

where k

= K/A, v

=

V/A~.

The

problem

now is to determine whether this

equation

has

symmetric

needle-like solutions

corresponding

to an even function

k(9)

which starts at o

=

0 with a fimte curvature ko and which tends to k

=

0 when 9

- gr/2.

Equation (4)

has a

singular point

at o

=

0.

Thus,

for any

physical solution,

the numerator of the r-h-s- of equation

(4)

must also vanish at 9

=

0. This

regulanty

condition gives a relation between

velocity

v and tip curvature ko:

v =

ko k(. (5)

We can

expand

the curvature

k(9)

close to o

= 0 in the

followmg

form :

k(o

=

jj ~

C,~

,~(o~)~~+~

for a # (or

ko

#

IN) (6a)

n o m o

k o

=

IN +

~ ~ Ci

~

o~'~

(In

o

)~

for ko = Il

(6b)

n i m o

with

Co

o =

ko. Inserting (6a)

into

(4)

and equatmg coefficients of

(o~)""

+"', we find

a =

1/2ko

-1

(7)

and recursion relations which define coefficients C,~,

~

in ternis of

Co

= 3 VI

[2 (4 ko )]

and of the

arbitrary

coefficient C

m C

o. Constant C must be evaluated

by integratmg equation (4)

with

boundary

condition k = 0 at o

=

gr/2. For

example,

for a

= 1/2

(or

ko

=

1/3),

we find

C - 0.39. The same

procedure

can be used when ko =

Il for

calculating C,[~

m terms of C j*1 =

3 v/2

ko

= 9/8 and of the

arbitrary

constant C *

m C i*

o which agam must be calculated

by integration.

Relations

(5-7)

define a contmuous set of needle-like solutions which can be

parametrized

by

a. The

only

limitation is a>0

(to

avoid

divergence

of the curvature

k(o)

at

o

=

0).

Note that for 0

~ a ~

l/2,

we have

k'(o

= 0

)

= m, whereas for

a > 1/2, we have

k~(o

=

0)

=

0.

The main difference between these solutions and lvantsov's solutions

[Ii

is that the

tip

curvature and

velocity

now have upper limits which came from the

k(

term m

equation (5)

(lvantsov's

solution

corresponds

to v =

ko

m the BLM

approximation), Indeed, equation (5)

imposes ko ~ l and v

~ Il while condition a

gives

and additional stronger limitation

ko ~ l/2 and v ~ Il. The dimensional

velocity

and

tip

curvature are given

by

v =

ko(1 ko) wA~, J~o

=

ko(w/D

4

,

ko

~ l/2

(8)

JO~RNAL DE PHYSIQUE T 4 N' 1 &IARCH 19g4 Ii

(5)

406 JOURNAL DE PHYSIQUE I N° 3

The

problem

now is to understand what

happens

when surface tension and

anisotropy

are

mcluded. In this case

equations (2)

and

(4)

are

generalized

as follows

U

= A

Kdt(1

y,~ cos mo V cos o

(1 p

~

cos m o

) (9)

v COS~ ~ k COS~ ~

ù

~ol

~

ù ikô (i

Ym COS m~ +

+ v cos o

(1 p~

cos m9

= 0

(10)

where à

=

d~/A~.

y~ is the surface stiffness

anisotropy

while

p~

is the amsotropy of the kinetic coefficient

p

for m-fold symmetry. We also assume that directions of minimal surface stiffness and of maximal kinetic coefficient coincide with the

growth

direction.

In the

simplest

case, we include

only

kinetic

anisotropy (with

zero surface tension, à

=

0). Thus,

for

sufficiently

small

anisotropy p~,

there exists a continuous set of solutions given

by

v =

ko k(/B

,

a =

(B/2 ko

1) > 0

(11)

with B

=

Il

[1- p~(m~ +1)]

and

hmiting

values of

velocity

and

tip

curvature given

by

v ~ BM and ko ~B/2. The solutions

disappear

when

p~(m~

+

1)

m1

(Fig. I).

> OE=

~

fi,=0.03 fi,=

0.15

4£j £~4

,~ ~~~

0 X~ 0

X~

'

0.10 0.15

fi4

Fig.

l. Dimensionless

velocity

as a function of kinetic

anisotropy.

Trie sobd line grues trie maximal

velocity

of « kinetic dendrites

>>. Dots correspond to velocities v~ of dendrites selected by anisotropy (see

also mset m

Fig.

2). Two dendrite

profiles

(with trie unit of length D/(w. A. v)) corresponding to two different values of P4 and à

=

10~ ~ are given m trie insets. Trie profiles are compared with trie parabolic

profiles havmg

trie same

tip

curvature (dashed lines; m trie nght mset trie two profiles are

indistinguishable

on trie choosen scale).

When we include

isotropic

surface tension without any

anisotropy (y~

=

p~

=

0)

all

solutions

disappear

as usual

[10].

This result is obtained from numerics and reflects the

impossibility

of

finding physical

solutions

k(

9

) starting

from 9

=

gr/2 with k

=

0 and

arriving

at 9

=

0 with

k'(0)

=

0

iii (in

all cases,

k'(0)

is found to be

negative).

(6)

When amsotropy is

included,

we find

numerically

some values of v which

provide k'(0)

=

0,

thus

giving

a discrete spectrum of solutions for each

given

value of à

[12].

In

figure 2,

we

plot

maximum selected

velocity

v as a function of dimensionless parameter à

=

d~/A~.

These curves have been

numerically

calculated for different values of

p~

and

y~. Two different cases can be considered

depending

on the existence or not of surface

stiffness amsotropy :

if y~ #

0,

there are two

asymptotic regimes

: in the

capillary regime,

at à

- m, the

dimensionless

velocity

v scales hke

y/'~/ô

in agreement with the calculations of

Langer

and

Hong

for the BLM

[9].

In the kinetic

regime,

at à

- 0

(or d~

-

0), velocity

v tends to a limit vo

(which

is obtained

by extrapolation) depending only

on

p~ (see

mset in

Fig. 2).

At small

anisotropy

vo

PI

~~, in agreement with

a

previous analytical prediction [7].

This selected

velocity

is

plotted again

m

figure1

in order to compare it with the maximal

velocity

of

« kinetic » dendrites

corresponding

to

d~

= 0. Two

points

must be

emphasized

:

first,

the selected dendrite still exists when

p~

>1/17 and « kinetic » dendrites

disappear.

Second,

when

p4

m

(0.02-0,04 ),

the selected

velocity

is close to the maximal

velocity

of « kinetic » dendrite.

~

o , p4"0.01,

o

v

=

x. ,,v=150 m

~

' ~

> ',, ',

»

O

>

v~ =

1 ~ j

j

> j

i

j (

jj

4

°'°~

Fig.

2. -

v

VIA

stiffness and

kinetic

P~. Trie

velocity v~ found by

to

à = 0 are given m

trie

mset.

-

Wheny~ =

0

two symptotic regimes

at à

-

0 is

independent of

y~ and thus

coincides

with the inetic regime discussed just

before, while the second ne, at

à

- m, is haracterized by v ~ p ('~ ô

~

m agreement with the

analytical of

Brener. We can agam phasize

that esult

is easier to find

with the

BLM than by solvmg the

full

nonlocal problem [14].

SO far, we have assumed that AM 1 and

k~

= 1. We

now

discuss

rbitrary

4

and k~ without

amsotropy and tension. sing the ame procedure as that

(7)

408 JOURNAL DE PHYSIQUE I N° 3

used

previously

to denve

equations (4)-(7),

we find :

k(V(1-A+V) [1+ (A-V)(1/k~-1)]-Ko(A-V)~+K((A-V)=0 (12)

a =

[(A-V)/2Ko-1]>0. (13)

Similar

equations

con be obtained for 3D

axisymmetnc

dendrites

using equations (1')

and

(2~)1

k(V(1-4+V) [1+ (A-V)(1/k~-1)]-2Ko(A-V)~+2K((A-V)=0 (14)

and the same relation for a as that

given by equation (13).

In this case, the two curvatures at the

tip

of the dendrite are

equal (Kj(0)

=

K~(0)

=

Ko)

and the

tip

radius

equals 1/Ko.

Equations (12-14) only

grue the relation between

growth velocity

and

tip

curvature as well as their upper limits

(Fig. 3).

On the other hand, to find dendrite

profiles (see

msets in

Fig. 3),

we need to solve

numerically

the

corresponding

differential

equations (1)

or

(1')

in

K(9)

with

condition

K(gr/2)

=

0 at A~1

(usual

dendrite with a

parabolic tait)

and with condition

K(90)=0

at ~ ml

(angular dendrite[15, 16]).

In the latter case,

90

is

given by

V cas

90

=

(A 1).

à = o.5 3D

>

à = 1.5

2D

o-s à

Fig. 3.

Tip

velocity V (in unit of w) and tip curvature Ko (in unit w/D) versus supercoolmg for two and three-dimensional dendrites (k~

=

1). Solid lines correspond to « kinetic » dendrites of maximal velocity (d~ = 0 and a

- 0). Trie thick sohd lines V

=

0 at A ~ l, V

= (A 1) for A ~ l, and K~ = 0

correspond

to

steady-state growth

of trie

planar

front.

They

also

correspond

to kinetic dendrites m trie hmit a

- co. Two

profiles

for 2D « kinetic

» dendrites (d~ = 0 and a - 0) are shown m trie msets.

In

conclusion,

we have found a new basic continuous

family

of solutions which takes mto

account interface kinetics but not surface tension. This solution descnbes a needle-like

dendrite at

arbitiaiy supercoolmg

A smaller or

larger

than 1.

Consequently,

it should be more

appropnate

for

describing

dendrites at

large supercoohng

than the usual Ivantsov solution

only

vahd at A

~ l. It could also serve as a startmg

approximation

m a more

complete theory.

Acknowledgments.

This work was

supported by

CNES contract No. 93.0215. D. Temkin is

grateful

for the Poste

Rouge provided by

the CNRS.

(8)

References

Ii Ivantsov G. P., Dokl. Akad. Nauk SSSR 58 (1947) 467.

[2] For a review see Brener E. A., Mel'nikov V. I., Adv. Phys. 40 (1991) 53.

[3] Willnecker R., Herlach D. M., Feuerbacher B., Phys. Rev. Lent. 62 (1989) 2707.

[4] Glicksman M. E., Schaefer R. J., Ayers J. D., Menai Tians. A 7A (1976) 1747.

[5] Géminard J. C., Oswald P., Temkin D., Malthête J., Europhys. Lent. 22 (1993) 69.

[6] Lemieux M.-A., Liu J. and Kothar G., Phys. Rev. A 36 (1987) 1849.

[7] Brener E. A., Geilikman M. B., Temkin D. E., Sov. Phys. JETA 67 (1988) 1002.

[ii Ben-Jacob E., Goldenfeld N.,

Langer

J. S., Schôn G., Phys. Rev. A 29 (1984) 330.

[9] Langer J. S., Hong D. C., Phys. Rev. A 34 (1986) 1462.

[10] Langer J. S., Phys. Rev. A 33 (1986) 435 and also Ref. [ii.

l Ii Condition k'(0 0 comes from symmetry and from trie fact that trie differential equation is now of second order (see Refs. [8-10]).

[12] Ben-Jacob E., Garik P., Mueller T. and Grier D.,

Pliys.

Rev. A 38 (1988) 1370.

[13] Brener E. A., J. Ciyst. Growth 99 (1990) 165.

[14] There is nevertheless a restriction to this conclusion concemmg trie scalmg with A. Indeed, m the limit A

- 0, exact scaling for dimensional velocity and tip curvature reads u

yÎ'~(D/d~)

A~

and Ko

yl'~(1/d~)

A~ [2] whereas BLM grues v

yÎ"(D/d~)

~~ and Ko

yÎ~~(1/d~)

A~. We suggest that this difference in trie power of A exists in ail trie asymptotic regimes we have

discussed.

[15] Brener E. A., Temkin D. E., Europhys. Lent. 10 (1989) 171.

[16] Classen A., Misbah C., Müller-Krumbhaar H., Saito Y., Phys. Rev. A 43 (1991) 6920.

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