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Compact or fractal patterns in diffusion limited growth
Martine Ben Amar
To cite this version:
Martine Ben Amar. Compact or fractal patterns in diffusion limited growth. Journal de Physique I,
EDP Sciences, 1993, 3 (2), pp.353-363. �10.1051/jp1:1993136�. �jpa-00246728�
Classification
Physics
Abstracts61.50C 68.70 47.20
Compact
orfractal patterns in diffusion limited growth
Martine Ben Amar
Laboratoire de
Physique Statistique,
Ecole NormaleSupdrieure.
24 rue Lhomond, 75231 Paris Cedex 5, France(Received
23 June 1992,accepted
22July 1992)
Rdsumd. Des structures fractales ont 4t4 observ4es en
digitations visqueuses
en cellule de Hele-Shaw et aux tempslongs
lorsque les forces capillaires deviennentn4gligeables.
Par opposi- tion, la croissance de monocristaux hpartir
d'un germe ponctuel fait apparaitre des dendritescroissant dans 4 ou 6 directions selon la
sym4trie
cristalline. Unecomparaison
entre des r4sultatsnum4riques
et des donn4esexp4rimentales
expliquel'origine
de l'instabilit4 de d4doublement despointes
en croissance radiale et montrequ'elle
peut Atre supprim4e parl'anisotropie
cristalline.Abstract. Fractal viscous
fingering
patterns are observed in an infinite Hele-Shaw cell atlong
times when thecapillary
forces becomenegligible.
On the contrary,growth
ofmonocrystals
from a
punctual
seed shows dendritesgrowing independently
in 4 or 6directions, according
to thecrystal
symmetry. A closecomparison
of numerical andexperimental
dataexplains
first theorigin
of thetip-splitting instability
in radialgrowth
and shows that it can be inhibitedby
theanisotropy
of surface tension.Among
all hissubjects
ofinterest,
Rammalstudied,
around1984,
the statisticalproperties
of fractal structures and has shown that
they
can be describedby
very fewparameters
such as the fractal and thespectral
dimensions[1, 2].
Ourpoint
of view here will be rather differentmostly geometrical,
since weplan
to understandwhy,
in nature, fractal structures occur ordo not occur. We consider here
growing systems
which aregenerally
believed tosatisfy
theapproximation
relevant to thedynamics
of continuous media but whichreveal,
atlong times,
a fractal
pattern:
a well knownexample
is theinstability
of Saffman andTaylor (S-T)
in the radialgeometry [3].
We will restrict ourstudy
to this situation that we would like to compare toan
analogous
one: solidification from atiny
nucleus in infinite medium. What is ratheramazing
in the viscousfingering instability
in a Hele-Shawcell,
is that the observedstructure,
atlong times, crucially depends
on thegeometry
of theexperimental
cell: it has been known for along time,
since thepioneering
work of Saffman andTaylor
[4], that theinstability
in an infinitelinear cell
gives
a verysteady finger
whose relative width(compared
to the width of thecell)
is very close to
1/2,
a result which hasintrigued
manyphysicists working
in this field[5].
This very stablefinger
proves~ if necessary, that thisgrowth, governed by diffusion,
cangive compact
354 JOURNAL DE
PHYSIQUE
i N°2structures in the presence of
walls, contrary
to whathappens
in infinitegeometry.
Anotherstrange experimental
fact is the difference betweenpatterns
obtained in viscousfingering
[3]and solidification at low
growth
rate[6].
Theequations
which govern both interfaces arequite
the same but not theshape
observed atlong
times(see Fig. i).
Solidification from aunique
nucleus
gives
several dendritesgrowing along
the main axis ofsymmetry
of thecrystal.
Each dendrite growssteadily
witha
tip roughly parabolic
whose size isgiven
in terms ofmacrocospic properties
like theanisotropy
of surface tension[7].
Thisopposition
between observedpatterns
in two different contexts can beexplained by
deterministicequations
without noise. This isthe aim of this paper that we would like to dedicate to Rammal's memory.
1. Position of the
problem:
thetip-splitting instability.
Fractal
growth
occurs when thesystem experiences repeated tip-splitting
events: that is asplitting
in two or threeparts
of aprotuberance
which becomes unstableduring
thegrowth
and recovers some
stability by
asystematic
division of its characteristiclengthscale.
This timedependent
process is very hard tohandle,
evennumerically,
for diffusive instabilities due to its non-linear and non-local character. This iswhy
most of the work oncrystal growth
and viscousfingering
has been restricted to thesteady growth regime
of isolated structure[7].
Thiscorresponds
toinvestigate
the stabletip
of along pattern growing
with a constantvelocity,
italso means that the
growth
is unaffectedby
the othergrowing
structuresalways present
ina
real
experiment.
But thisasymptotic regime
is reachedonly
after some time: the dendrites areusually
initiated from apunctual seed,
then growradially
from this seed with a"petal" shape.
Here we want to
study
this intermediategrowth regime
where allfingers
initiated from thesame seed interact. We will mimic this
complicated
interactionby
a suitablegeometry
deduced from theexperimental
observation: we willimagine
that each dendrite grows in a fictitious butwell-defined
sector-shaped
cell. This situation is also met in radial viscousfingering
which has been studied in detail veryrecently [8, 9].
In a Hele-Shawcell,
the air-oil interface is circular and stable up to a criticalradius,
thendevelops fingers
which grow inindependent
fictitious sector. The number offingers
varies from five to seven, itdepends
on the initial conditions andon defects on the
plates.
Thisgrowth
is more or less constrainedby
theneighbours.
It remains self-similar in time aslong
as thetip
radius is less than a critical value. At thispoint,
thetip
becomes toolarge
to be stabilizedby
thecapillary
effects andtip-splitting
occurs. After thetip-splitting,
two or three newfingers
reappear, grow, thentip-split again.
The cascade ofsuccessive
tip-splitting
events leads to a very ramified structure and at verylong
times to the well known fractal structure characteristic of thisgeometry (see
Viscek's book for a detaileddiscussion and
photographs, [10] ). Recently,
much work has beenperformed
in order toexplain
the existence of self-similar
fingers
and toquantify
at least the firsttip-splitting
event [9] which takesplace
when the self-similar solutionsdisappear.
Crystal growth
isgenerally
believed to bequalitatively
similar to viscousfingering,
when theexperiment
is realized at lowsupersaturation
li and in a bidimensionalgeometry. But,
such a cascade oftip-splitting
events has not beenreported
forcrystals
to ourknowledge.
Thegrowth
scenario seems to be the sameexcept
that the number ofpetals
isperfectly
well definedby
theanisotropy
of surface tension: 90 or 60° for a four-fold or six-foldanisotropy.
In earlierexperiments [10],
theimportance
of theanisotropy
on viscouspatterns
has been revealedby engraving
the Hele-Shaw.plates.
At fixedanisotropy,
a transition between ramified and dendriticpatterns
was observed when theapplied
pressure is increased and aphase diagram
of thepatterns
has been sketched. The lower theanisotropy,
thehigher
the pressure necessary toa)
Fig. i. - a)
Long
time behaviour of a gitalized viscous fingering pattern by njecting airinto a ilicon oil. Courtesy of
356 JOURNAL DE
PHYSIQUE
I N°2modify
thedynamics.
These features motivate our numericalinvestigation
for the existence ofgrowing
self-similarfingers,
in theLaplacian regime,
with ananisotropic
surface tensionTic).
2. The
free-boundary problem
ofLaplacian growth
in asector-shaped
cell.Dimensionless
quantities
make moretransparent
thesimilarity
between solidification at low li andLaplacian growth.
In one case, we willmostly speak
of a dimensionlessvelocity potential
# while,
incrystal growth,
we will deal with a dimensionlessimpurity
amount definedby:
u =
~
~°,
,
with
Co
theimpurity
concentration in theliquid
on theinterface,
asgiven [Co (I
Ii)]
by
thebinary phase-diagram
and It thepartition
coefficient(for details,
see[I I]).
Theimpurity
concentration in the
liquid obeys
the diffusionequation
which can be reduced to theLaplace equation (Au
=
0)
for smallgrowth
velocities. Thesimilarity
of thepatterns
has been noticedexperimentally
in[6],
at least for low Peclet numbers.Moreover,
for li <0.2,
the area of the germ increaseslinearly
intime, indicating
a self-similargrowth regime
int~'~
forany
typical length.
These results are characteristic of viscousfingering
in awedge
realized with a constant fluxlo.
A self-similarregime
ofgrowth
exists if oneneglects
thecapillary
effects.Assuming
the
stretching
factor:R(°, t)
=
Ru f(t) r(°)
does not
modify
theLaplace equation
in the bulk:hi
=0(1)
but the
continuity equation
at the interface:R~ fit) @r
n =
nV# j2)
Here,
n is the normal at the interface whileRo,
thetip position
at time t =0,
is ourlength
unit. Atime-independent
freeboundary problem
can be handled if one assumes thatthe
quantity f(t)~ ~~~
isa
constant,
which means agrowth regime
int~'~ [8].
Fora
crystal,
t
the
continuity equation (named
the Stefan-Lamd relation[7])
is identical to(I)
if oneformally replaces # by
-u. Thisfree-boundary problem
has a continuousfamily
ofpetal-shaped
solu-tions,
labelledby
aparameter I,
the relative value of thepetal angle
at the center of the germcompared
to the fictitious sectorangle
go For aphysical
value of this sectorangle
of 90°or
60°,
the whole range of I values 0 < 1 < is accessible
[9].
Let us recall theanalytical expression
of thesefinger shapes
in absence ofcapillarity:
if xi and vi denote the coordinates of apoint
of the
interface, they
read:xi " c
(90) s~°~~~~)l'F ~°~~ ~~, ~~°, j,
Is)
T T
vi "
As~°~~~~)l'(
Is)~/~F ()
+~°~~ ~~, ~~°, ~,
ls)
T '
with-
Y
(1
~ Y(1+ ~(
~ ~ ~~~ ~~~~~~~ ~~~
()
~()
+i~)
~~~ii
-0
(a)
0 0.2 Off O.6 o-B I-o 1.2
Fig.
2. Exact self-similar shapes for adivergent
flowcorresponding
to a sector of So " 60°. The chosen parameters increase from the inner to the outer profile and areequal successively
to o.25, o-s and o.75.r is the Euler
function,
F ahypergeometric function,
c(go)
thesign
of go and s aparameter
between 0 and I. As anexample, figure
2displays
severalshapes
for asector-angle
of 60°.As
usual,
the selection of the Iparameter by
the surface tension isexpected
but the surface tension effectsdestroy
theself-similarity.
For a constant fluxexperiment,
it means that thecapillary parameter
a(defined below)
decreasesduring
thegrowth
as shownby
theLaplace (for
the viscousflow)
or the Gibbs-Thomson relation(for
thecrystal).
a isgiven by:
'~~~ l
2p
~)~UoRj@]
~~~~~'~
Uof~~~]9]
~~~In
(2)
we have introduced thevelocity
of thetip
Uo at time t= 0 and the
capillary length:
do
=7Tm /mLCo(I It),
m is theslope
of theliquidus,
L the latent heat andTm
themelting temperature. Nevertheless,
we willadopt
an adiabaticapproximation, assuming
that atlong times,
thedynamics
is slowenough
so that thefinger
has time toadjust
itself to theslowly varying
surface tensiona(t).
Thisapproximation,
which consists inexamining
the selectionby
a timedependent capillary parameter ail)
is rathergood
for viscousfingering
since Ivaries rather
slowly
when a decreases(for
acomparison
between theoreticalpredictions
andexperimental results,
see[9]).
In this case, the selectionby
a fixed a can beinvestigated numerically.
Theseapproximations
have transformed a rathercomplicated time-dependent
free
boundary problem
into a"steady
one" more suitable to handle at leastnumerically, using
methods which are standard
by
now. Let us recall that one way to handle thisquestion
is to transform the freeboundary problem, taking
into account the threeequations 11, 2, 4)
into aunique
set ofequations
for theinterface,
eitherby
Green's functiontechniques,
orby
conformal map andhodograph
method[4]. Here,
wepresent only
the last method with our numericalresults,
both in viscousfingering
and insolidification,
for two sectorsangles
60 and 90°(for
details,
see[9]).
358 JOURNAL DE
PHYSIQUE
i N°23 Numerical result s.
3. I THE METHOD. Let us
briefly
recall the details of thehodograph
method and the cor-responding algorithm
which have beenpublished
elsewhere[9]. First,
the sectorgeometry
is transformed into the more familiar infinite linear cellby
a conformal map:z =
~
ln
(zi), (z
go
describes the
complex plane). Then,
we haveadapted
thehodograph
method of McLean and Saffman[12] since,
forgo
"0,
it appearsremarkably
efficient. Somewhatunfortunately,
this method introduces ratherunphysical quantities
such as the derivative q e~~~ of acomplex
pc-tential which transforms the interface into a streamline
[9]. Originally,
for the S Tinstability,
thisquantity
was thecomplex velocity
of the fluid in thefinger
framebut,
in our case, it has lost thisphysical meaning. Nevertheless,
let usgive
theequation:
« q s
tag
q =
~i
~>~
,.
i~/>
P P.£~
dt~~l'°il~- l~~~
15)
with
Ho
= exp(- ~°~ )[l
c cos(m(T
+x/2
+90v/2)] q
s
~~
+
~° (l I) in(T)j
(6)
2 as 2'
and
~
'~
(l -~2 ~jo
IA
~~~ ~ ~and the
following boundary
conditions:r(0)
=
0, r(I)
=-x/2, q(0)
= 1,
q(1)
= 0. As
usual,
P P means the
principal
value of theintegral.
A second conformal transformation maps the
finger
over thesegment
s E[0,
1], which is very convenient for the numerical calculations. Note that theposition
ofM,
thepoint
of the interface entersequation (5)
via both the curvature and theintegral.
This is due to themodification of the Stefan-Lamd and Gibbs-Thomson law via the first conformal
mapping
transformation.
Equation (5)
which relates three unknowns functions q, r and zrequires
two otherequations
in order to be solved.They
are deduced fromanalyticity
of q and z[12].
Here,
in order to also treat the solidification at low Picletnumber,
we have introduced akey ingredient,
thatis,
theanisotropy
of surface tension. Itrequires
tomodify
a inequation (5)
asfollows: a
ii
ccos(m9)] (with
m= 4 or
6)
with c theanisotropy
of the surface free energy:Tiff)
+7"1°).
The numerical
procedure
consists inwriting
a discretized version of these threeequations
at every
point
so of anadequate
mesh. Theresulting
non-linearalgebraic
system for the three unknowns q, r, z is solvedby
Newton's method. The iterativealgorithm requires
astarting
function and we
always
use the S -T solution at 0° because itsexpression
is muchsimpler
than the zero-surface tensionprofile
atarbitrary
sector value. infact,
to obtainquick
convergence,a
good
guess of the initialeigenvalue
isrequired
once the surface tension a is fixed. Beforegoing further,
we willbriefly
recall the main resultsconcerning
the lineargeometry
which is well understood now. Note that in this case, thefinger
issteady
andespecially
stableagainst
perturbations.
3. 2 SELECTION BY AN ISOTROPIC SURFACE TENSION.
Perhaps,
it is useful to recallbriefly
the main resultsconcerning
the viscousfingering instability
in a linear cell. It concerns the selection of the relative widthii)
of thefinger by
thecapillary
effects(a),
in both theisotropic
Although
years manywe will refer to them for our discussion.
isotropic
surface tension selects an infinite discrete set ofprofiles
among the zero-surface-tension set of Saffman andTaylor.
At fixed surface tensiona or «, there exists a discrete set of
eigenvalues
labelledby
n,l~,
all of themmerging
from the 0.5 1-limit atvanishing
a or «[12].
The 0.5 1-limit for all theeigenvalues
was known from thepioneering
work of Saffman andTaylor
[4] and since hassuggested
a lot of numerical[12]
and
analytical
works[5].
Thispuzzle
has been solvedonly recently by singular perturbation
theories
(W.K.B, [5]).
When a
increases,
so doesl~,
anotheramazing
result is that the discrete setl~ collapses
to I for a finite value of the
capillary
parameter amax m 0.35.Any eigenvalue
goes from 0.5 up to I when a increases from 0 up to 0.35[13].
Astability criterion,
shownnumerically
andanalytically [14],
proves thatonly
the firsteigenvalue ii
isexperimentally relevant, although,
at
extremely
low surface tension orlarge pulling speed,
thefinger
becomes unstable. This ismainly
due to the common limit 0.5 for all theeigenvalues
Ithey
are very close to each other and thefinger
cannot fix itselfon one of them.
Adding
four-foldanisotropy
in the same way as thecrystalline
one,destroys
the 0.5 common limit which now goes to zero andgives
narrowfingers [15].
This fact shows off the closesimilarity
between solidification at low Pdcletnumber,
and viscousfingering
since thevanishing
I limit
(which
means that the walls of the Hele-Shaw cell arerejected
atinfinity) corresponds
to the
needle-crystal growth.
What isprobably
less known is the range of thisanisotropic
effect when the surface tension increases.
Figure
3displays
acomparison
between the(c
=0) )-spectrum
and(c
=0.2)
one versus a. We have chosen thisanisotropy
value which can appear ratherlarge compared
to thecrystalline
one, because if fits rather well theexperimental
data(Couder, private communication).
o
,o
$
Fig.
3.Eigenvalue
spectrum of the viscousfingering
pattern in the linear geometry: the relative width versus a:(-)
withisotropic
surface tension,(o o)
withanisotropic
surface tension(e
=
o.2),
(+ +) experimental
data of Couder and collaborators.360 JOURNAL DE
PHYSIQUE
I N°2As
predicted by
the W.K.Bapproach [15],
the firstanisotropic eigenvalue ii
is lowered butonly
on a rather restricted range of a values(a
is less than5~
of its extremumamax).
As for thehighest levels,
theanisotropy
does not affectthem,
at least in the numerical accessiblerange. This is the reason
why anisotropic fingers
appear more stable: at low surface tension the characteristiclength
scaleii
issmaller,
and the stabilizationby
the surface tension is increased.Moreover,
the first and secondeigenvalues
are more distant than in theisotropic
case and noise cannot induce a transition between two levels.Nevertheless,
fromfigure 3,
we conclude that theefficiency
of theanisotropy
in the Hele-Shaw cell is limited to very low surface tension orhigh finger speed.
This is not an intuitive result. Theanisotropy
coefficient is a dimensionlessparameter, independent
of the surface tension. It is difficult toexplain why
it does not affect theeigenvalues
as soon as a increases. We wellkeep
in mind that theanisotropy
of surfacetension stabilizes the viscous
fingering pattern
at lowcapillary
number when it appears less stableagainst perturbations.
3.3 SELECTION IN THE SECTOR SHAPED GEOMETRY. The
isotropic capillary parameter
a(t),
which istime-dependent
in this case, selectsa
unique
relativeangular
widthI(t),
at least when it is not too small.However,
asurprising phenomenon
occurs at low values.By opposition
to the lineargeometry
where all theeigenvalues
merge at 0.5 atvanishing
a[12],
the levelsl~
andl~+i (n
isodd)
mergeby pair
above anon-vanishing
surface tension threshold~~, ~+i and
disappear
below(this labelling
of theeigenvalues
is deduced from their order atlarge a).
The threshold a~, n+i decreases when nincreases,
and the first and second levelsdisappear
first(see Figs.
4 and5).
This isimportant because,
when itexists,
thecomputed
valueii
agreesquite
well with theexperimental data,
measured at different times[9].
When itdisappears
a closecomparison
withexperimental
data shows thattip-splitting
occurs. This isthe reason
why
we have claimed thattip-splitting
occurs in radialgrowth
because a self-similargrowing pattern
cannot exist atlong time,
when a is less than ai, ~.~.
+.
+m Woo
+
+
o,8 ~l
~ ~
~ m
~+
~~$ +,
~
(
m '
0.COO .O02 0006 DOOB
O
0010Fig.
5. -The
relativeangular A
the
apillaryarameter a for a ixfoldisotropy
Figure
4(resp. 5) displays
our resultsconcerning
the 90degree geometry (resp.
60° for two different values of theanisotropy
coefficient c =0.1, 0.2, compared
to theisotropic
case which isalways
our reference.Qualitatively,
theeigenvalue spectrum
is the same for the twoangles
but differs
depending
upon the values of c. For a small cvalue,
say c =0.I,
oneonly
noticesa small shift
compared
to the reference(c
=0)
for the levelsii
and12.
Let us recall thatonly ii
is believed to be relevant for theexperiments.
Since these two levelsonly
exist fora =
0.004, they
arepoorly
affectedby
theanisotropy.
On thecontrary,
it affects the upperlevels,
which merge at lower a. As anexample, 13
seems to fall at zero when a vanishes and theloop 13,4
hasdisappeared.
For this range of cvalues,
ourprediction
is that thedynamics might
be dominatedby tip-splitting
events. This is inagreement
with theexperimental
resultson
anisotropic
radiallaplacian growth [10].
At lowanisotropy,
when theapplied
pressure is not toolarge,
severaltip-splitting
events are observedgiving
a ramifiedpattern. But,
for anyanisotropy value,
when theapplied
pressure islarge enough,
six needles can beobserved,
without
tip-splitting
events.According
toequation (4),
alarge applied
pressure means a small initial value for a, whichnevertheless,
will decreaseduring
theexperiment.
So, by comparing
the numerical and theexperimental data,
we canimagine
thefollowing
scenario: at low
applied
pressure, theexperiment
starts on the levelii,
andduring
thegrowth,
since a
decreases, ii
describes the lower level up to theloop
and at thispoint
thefinger tip- splits
as in theisotropic
case. When theapplied
pressure islarger,
theexperiment
starts on level three so as time runs, a decreases and alsoI, continuously.
Narrowfingers
are observed which in the limit ofvanishing
I look like needles. Due to the lack ofquantitative data,
thisinterpretation
is audacious since this third level isgenerally
believed to be unstable. This is true for the linear cell buthere,
thespectrum
is rather different and theoreticalpredictions concerning stability
aremissing.
For
greater
values of c, say c =0.2,
theeigenvalue spectrum
is rather differentas shown
by
figures
4 and 5. Theii eigenvalue
decreasesmonotonously
from the reference value down to zero as adecreases,
so as time increases. Ourprediction
here is that thecrystal shape
modifies362 JOURNAL DE
PHYSIQUE
I N°2itself
continuously
from thepetal shape
for short times to the dendriticshape
forlong
times.There are never
tip-splitting
events.Although
measurement of c isimpossible
forengraved plates,
the absence oftip-splitting
events athigh anisotropy
issuggested by
thephase diagram
of
[10]. Ordinary crystal anisotropy
values c4 varies from 0.075 forsuccinonitrile,
up to 0.016 forpivalic acid,
and it reaches 0.2 for helium.Concerning thermotropic
columnarmesophase,
c6 has been measured to be around 0.I.
Ordinary transparent
materials areexpected
to havea different
dynamics
in radialgrowth.
Oswald et al. do not mention anytip-splitting
events but we think that theirpetal-shaped regime (A
<0.2) corresponds probably
toii
while thedendritic
regime (observed
when 0.2 < A < 0.6 that is smaller initial values fora) corresponds
to
l~.
in the dendriticregime,
due to thesharp
variation of I with a, when both go to zero, the selected solution labelledby
I(as
well as thefinger shape)
varies veryquickly
and theself-similarity
is nolonger
verified. This canexplain
thechange
in thedynamics
from at~/2 regime
to a constantvelocity
one, as indicatedby
theexperiment [6].
In summary,
anisotropic laplacian growth
in the circulargeometry
has been examined. Weshowed that the
anisotropy
of surface tension is akey ingredient
to describe thegrowth dynam-
ics from one seed. It
explains why crystal growth patterns
do notdisplay
the fractal structure characteristic of viscousfingering
atlong
times.But,
to beoperative,
this stabilizationby anisotropy requires
a sufficientsupersaturation.
Acknowledgements.
would like to -thank the
Organizers:
J.C.Angles d'Auriac,.B. Dougot
and J.M.Maillard,
for this
moving,
sober and sinceremeeting
on condensed matterphysics
dedicated to our friend Rammal. I would like to thank them forparticipating
to thisspecial
issue dedicated toRammal.
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