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Experimental study of radical tesselations of assemblies of discs with size distribution
C. Annic, J. Troadec, A. Gervois, J. Lemaître, M. Ammi, L. Oger
To cite this version:
C. Annic, J. Troadec, A. Gervois, J. Lemaître, M. Ammi, et al.. Experimental study of radical
tesselations of assemblies of discs with size distribution. Journal de Physique I, EDP Sciences, 1994,
4 (1), pp.115-125. �10.1051/jp1:1994124�. �jpa-00246882�
Classification Physics Abstracts
05.40 05.90 64.60C
Experimental study of radical tesselations of assemblies of discs with size distribution
C. Annic
(1),
J. P. Troadec(1),
A. Gervois(2),
J. Lemaître(1),
M. Ammi(1)
and L.Oger (3)
(1)
Groupe
Matière Condensée et Matériaux (*), Université de Rennes 1, 35042 Rennes Cedex, France(2) Service de
Physique Théorique,
Direction des Sciences de la Matière CESaclay,
91191 Gif- sur-Yvette Cedex~ France(3) Laboratoire de Physique et de
Mécanique
des Milieux Hétérogènes (**), ESPCI~ 10 rue Vauquelin, 75231Paris Cedex 5, France(Received
27July
1993, received in finalform
9 September 1993, accepted 20September
1993)Abstract, We had
previously
shown that topological and mettre properties of 2d mosaics obtained from the Voronoi tesselation of monosizepackings
of discs deviate from those of a totally random mosaic. Here, we describe a mosaic obtained from the radical tesselation of a two-size mixture of discs at differentpacking
fractions. Two kinds ofpackings
are considered,expedmental
(discs moving on an air table) and numedcal. The deviations are even morestdking, particularly
atlarge
packing fraction where neither Aboav's nor Lewis' law hold moreover, some distributions, such as the distribution of the number of sides of the cells, or distribution of the oeil area, are splitmto two parts, each of them related to one species of discs.
Finally,
we consider polydisperse packings as to theirtopological properties,
the mosaics obtained from those packings obeyapproximately the laws of random mosaics but this is not so for their mettre
properties,
which are stilllargely
affected by stedc exclusion.1. Introduction.
Binary (or
moregenerally, polydisperse)
assemblies of discs have been less studied than monosize systems, either from theexperimental
or theoreticalpoints
of view. Most of the results deal with compact assemblies which aresupposed
to mimick in thegrain
spaceonly
bi-dimensional
packings
undergravity.
For the densest(disordered) packing
it has been venfiedexperimentally
andjustified
usingtopological
arguments that :the maximal
packing
fractionC~~
does notdepend
much on the percentage of eachspecies and is close to
0.84,
a value a littlehigher
than that found in the monosize case(C
=
0.82) [Ii,
and(*)
URA CNRS 804.(**) URA CNRS 857.
the
physical (contact)
coordination number z is close to 4 and does notdepend
much on the mixture either.Dilute assemblies have been little
studied,
except for numericalexperiments
on randomsequential adsorption (RSA)
assemblies[2].
Thedevelopment
of lowdimensionality
exper-iments
(adsorption
ordeposition
processes,suspensions
ofparticles,
breathfigures..
hasshown the need for an
analysis
of disorder at ailpacking
fractions. The notion of« true
contact » which is not
always
clear even in compactpackings
is nolonger adequate
andmust be
replaced by
the idea of «topological neighbour
». Thesimplest
way fordetermining
the local arrangement around one
grain
isprovided by
the radical tesselationproposed by Gellatly
andFinney
and others[3],
whichgeneralizes
topolydisperse packings
the Voronoïtesselation used for monosize discs or point assemblies
[4].
The main aim of this paper is to
study binary
assemblies of discs with a given size ratio at any concentration and anyproportion
of small andlarge
discsthrough
the arrangement of the Voronoïpolygons. Comparison
with « random » mosaics found in the literature and with the mosaicsgenerated
from monosize assemblies has beenperformed
and because of the existence of two disc sizes whichprovides
two kinds of cells, many differences areexpected.
This paper is
essentially experimental.
Thelarger
part is devoted to thestudy
ofbinary
mixtures of discs with size ratio 2 index refers to the small discs and index 2 to the
large
ones. Most of the discussion is concerned with the results on
expenmental
assemblies of discsrealized on an air table
already
used forstudying
assemblies of monosize discs[5].
Some numericalpackings
were built forcomparison.
The assemblies are described in section 2. Theanalysis
in ternis of the radicalgeneralization
of Voronoï tesselation is introduced in section 3.Sections 4 and 5 deal with the
experimental
results for the main indicators of the disorder as ansing from the cellanalysis
:topological properties
such as side numberdistribution,
average number ofneighbours
and firstneighbour
correlations(section 4),
metricproperties, typically
average areas
(section 5).
In section6,
we see how theseproperties
are modified when one considerspolydisperse packings
builtnumerically.
2, The assemblies.
2,1 EXPERIMENTAL ASSEMBLIES. The
experimental
device is descnbed in reference[6].
Because of small local
hetereogeneities
in the poroustable,
discs move and rearrangepermanently.
This,together
with the absence offriction,
allows the realization ofhomogeneous
random assemblies at ail densities.
Systematic
measurements have beenperformed
onbinary
mixtures
(2 Ri
= cm and 2R~
=
2
cm) starting
from 2 differentviewpoints
:at fixed numerical
proportions
ni, n~(ni
+ n~ =1)
ofspecies
and2,
we increase thepacking
fraction C(or concentration,
ordensity)
up to the densest disorderedpacking
fraction ; at fixedpacking
fractionC,
wechange
theproportions
ni and n~ of small andlarge
discs.Snapshots
of theassembly
are taken at different times.They
are read using animage
processing
analysis
which determines theposition
of the centers and the radii.Any
newquantity
of interest can be derived from these dataonly.
The number ofsamples
is chosen so that we haveenough
statistics on bothspecies, typically
at least a thousand discs in each category, and the errors have been calculated from thedispersion
found in measurements onindividual
photos.
Due to constant rearrangements, time averages are also ensemble averages.2.2 NUMERICAL ASSEMBLIES. We have tried several kinds of numencal assemblies :
(1) At low
packing fraction,
we havegenerated
RSA[2] binary
assemblies of discs. We recallbriefly
theprocedure
discs areplaced
oneby
one, the centerbeing
chosen at random. Ifthe disc does not
overlap
withalready deposited discs,
it isdefinitely placed
and does not moveanymore ;
otherwise,
it isrejected
and another center istried,
the sizebeing kept.
The process ends when agiven
concentration is reached or when nosupplementary
disc may be added~jamming
limit C~).
Some variations in thebuilding
fuie can be usedaccording
to the choice of thespecies
of the disc to beplaced
: one mayposition
ail thelarge
discs first and then thesmall ones which is easier
-, or
position
the small ones first and then thelarge
ones, which is moredifficult,
or chooserandomly
thespecies
of the disc to bepositioned.
We chose the first alternative.(2)
at theopposite, for
very compactassemblies,
we used a 2dadaptation
of the Powellalgorithm [7]
:grains
areplaced successively
undergravity,
in contact withalready positioned
discs. We get
only
compactassemblies,
withpacking
fraction of the order ofC~ax
= 0.84.For numerical
assemblies,
someexperiments
at alarger
size ratio(R~/Rj
=
4)
and on somepolydisperse packings
wereperformed
both with RSA and Powell fuies. The errors were calculated from thedispersion
of the results obtained on severalsamples
; due to a better statistics(several
thousand discs in a numericalpacking), they
are smaller than in theexperimental
studies.3. The
procedure.
In compact
assemblies,
the relativeposition
of discs iscorrectly
described in terms ofphysical
contact. Contacts are no
longer interesting quantities
in dilute assemblies whereonly
the notionof
«neighbourhood»
has ameaning.
Such anapproach
wasextensively developed
in monosize assemblies orpoint
systems : it is the well known Voronoi-Dirichlet tesselation[4],
which substitutes thestudy
of the discsby
that of theirsurrounding
cells and may be built at anypacking fraction,
the characteristic cell sizescaling
with C~ ~~~.For
unequal discs,
Voronoï tesselation is not agood
choice as it may intersect thelarge
discs. Several
generalizations
have beenproposed
and thesimplest
one, which takes intoaccount the size of each species is the radical tesselation,
proposed by Gellatly
andFinney [3]
we choose as a
separation
fine between two discs the radicalaxis,
I.e. the fine ofpoints
withequal
tangents(Fig. la).
This fine is outside the two discs andorthogonal
to the cerner fine(for touching discs,
it is thetangent)
; when the discs areequal,
we recover the Voronoiperpendicular
bisector. Whenperforming
this construction for every pair ofdiscs, polygonal
convex cells are
generated.
Each of them contains one disc and one disconly
; two cells with acommon
edge
areneighbour
cells, and the number of sides of agiven
cell issimply
the numberof first
(or nearest) neighbours
for the disc. Thehierarchy
of first, second, etc.neighbours
goesas m the Voronoï case
(Fig. lb). Actually,
similarities between mediator and radical fines aredeeper
: forexample,
as the vertex coordination number is3,
thetopological
constramts on 2dgraphs yield
agam an average number of sides(n)
= 6 as for any tesselation.
In the
followmg,
thepossible
correlations between discs are studiedthrough
the correlations between thepolygons
of the radical tesselation. The sameanalysis
wasperformed
both forexperimental
and numencal assemblies but the results in the paper arequoted mostly
for the air table expenments. Results for numencal assemblies(and eventually
for a size ratio4)
aregiven
in detailonly
whenthey yield supplementary
information.4.
Topological properties.
We
present
here resultsdrealing
with thesimple counting
of the cells and their firstneighbours.
We follow the same fine as in the monosize case and try to see whether the mosaic
generated
inthe radical tesselation is « random » or not. We shall see that many differences anse in the
binary
case, because of the existence of two different classes ofpolygons.
L L i
(a)
,
~b)
o
Fig. l. (a) Pdnciple of constnlction of the radical axes. (b) Tesselation in a binary mixture of discs the striped discs are the neighbours of the black disc.
4,1 DISTRIBUTION OF THE NUMBER OF SIDES OF THE CELLS. The
simplest topological
properties
can be derived from theknowledge
of the distributions p~jjp~
=1 and~
p, ~(
jj
pj~ =
l, i = 1, 2 and p~ = ni Pi
n
+ n~ p~ ~) of the number n of
edges
of the cellsn
when
respectively
ail discs and discs ofspecies
i are considered.Small and
large
discs behavedifferently
asdensity
increases. Atgiven proportions
and low concentration, the total distribution p~ has aunique
maximum near n = 5 or 6 ; then at mcreasingdensity,
itsplits
into two maxima which get more and moreseparated.
Anexample
for an
equal
number of discs of each species on the air table is given mfigure
2. The distribution ispeaked
around two values close to n = 5(for
smalldiscs)
and n= 7
(for large discs).
0.4 Pn
O C = 0.73
o_3 A c = o-m
0.2
o.i
n o
3 5 7 9 11
Fig.
2. Side number distribution p~ forbinary
assemblies of discs at small and largepacking
fractions(ni " 0.5 ).
The
hexagons
which were dominant in the monosize case athigh
compacity are very rare.As a consequence, the
percentage
p~ is nolonger
an order parameter.Although
the totalvariance
q~ =
(n~) (n)~
remains
high,
of the order of1.5,
ii cari be seen that it does flot fit the universal check in termsof p~ which was put into evidence for the classical random mosaics and in the monosize
case
[8].
The same holds
qualitatively
for other concentration ratios on the air table(and
for numericalassemblies),
1-e- theheight
and theposition
of eachpeak depend
on the mixture. For a size ratio4,
and a Powellpacking (ni
= n~ =
0.5,
maximumcompacity)
theseparation
of the cells into 2 classes is still morestriking
: 70 fb of thepolygons
around a small disc arequadrilaterals
and
nearly
the same percentage of cells aroundlarge
discs have n= 7 and 8 sides while the total
proportion
ofhexagons
isonly
7 fà.4.2 ABOAV-WEAIRE LAW. In classical mosaics, the average number of sides
m(n)
of thefirst
neighbours
of a cell with nedges
is well fittedby
theempirical
law[9]
6a+q~
m(n)
=
6 -a +
(1)
n
where a is a parameter which is believed to be universal if cells can divide or
disappear,
andequal
to[loi.
The Aboav-Weaire law is a first attempt tostudy
the correlations betweenneighbounng
cells : the lineardependence
on 1/n means that cells with a small number ofedges
are surroundedby
cells with alanger
number of sides andconversely. Actually,
parameter a is of the order of 0.5 in the Poisson Voronoï tesselations
[1Il
and was found to bean
increasing
function of thepacking
fraction m our monosize assemblies[5] (it
goesapproximately
from 0.5 to1.5).
Othercounterexamples
to the value a= were found in breath
figures [12] (a
=
2 and in some evolutive numerical mosaics
[13] (where
a can benegative !).
In these cases, cell
disappearance
may or may not occur.In
fact,
the law(1)
appearsonly
as anapproximation
and some(weak)
deviations from thelinear
dependence
ofnm(n)
on n have been observednumerically[14].
In ourbinary
assemblies, at least at medium or
high packing
fraction, when the twospecies
aredifferenciated,
the result is morestriking
: Aboav-Weaire law does non hold at ail. The variations ofnm(n)
with n areS-shaped (Fig. 3)
; for n w5,
mostpolygons
anse from small discs and for n m 7 fromlarge
ones ; a breakclearly
occurs at n = 6 because of the differentsurroundings
of the two classes. Let us note that for 4 w n w8,
the values ofm(n )
come froman average on several hundred
cells,
and thenon-linearity
cannot be attributed to a too small statistics.It is
possible
tostudy
small andlarge
discsseparately.
For each species, one gets a lineardependence
ofnm~(n)
(1 = 1, 2 with n and ai = a~approximately.
Thea~'s
areincreasing
functions of the
packing
fraction and may belarge,
of the order of 2 or more(when
ni " 0.75
they
may reach the value2.5). However,
it is notpossible
to consider it as aprecise
result as the linear fit is
performed
with 3 values of nonly
for eachspecies.
5. Metric
properties.
A
study
similar to that for monosizepackings
wasperformed
for metricproperties
andparticularly
for the cell areas. In the monosize case, some distortions to theempincal
lawswere observed because of stenc exclusion : for instance the Lewis law does not hold.
so
nm(n)
,
A
D suldloniy
~ Ô largeonly
~
° global
30
OEl
n
3 4 5 6 7 8 9 10
Fig. 3. Aboav's law is not verified in dense binary packings (here C
=
0.73 and ni 0.5).
Nevertheless,
the behaviour of the total area distribution remains ratherregular
and follows a gamma distribution[5, 15].
In
binary mixtures,
the differences are morestriking
: as the radical axis is closer to thecenter of the small
disc,
the area of thepolygons
isdirectly
related to the size of the discsthey
contain
(this
is one of the reasons forhaving
chosen such atesselation).
The different behaviour of the 2 classes is more accentuated thon in thetopological properties.
5,1 DISTRIBUTION OF THE AREAS.- In
figure 4,
we haveplotted
thehistogram
of thenormahzed areas for an
equal
number of small andlarge
discs and for the monosizepacking
at the samedensity (medium compacity,
C0.45)
: for thebinary assembly,
the twopopulations
are
already
wellseparated.
Forhigher compacity,
theseparation
is even moremarked,
thehistogram
issplit
into twocompletely separated
parts. Of course,larger
size ratios lead to stilllarger
separations.5.2 LEWIS LAW. -Lewis
[16]
has shown that inbiological tissues,
the average areaA~
of the cells with n sides is anincreasing (linear)
function of n.A~ =
Ao(n no)
where
Ao
and no are parameters of the tissue. This law was venfied later for most randommosaics in the
literature, though
a similar law for the penmeter P,~ is sometimes a better fit(Desch
law[17]).
We have shown that the Lewis law and the Desch law do not hold incompact (C
m 0.45 monosize assemblies of discs[5],
asA~ (and P~)
exhibits a minimum forn = 5 : stenc exclusion is
responsible
for thehigh
value of the area of low orderpolygons
(triangles including
a disc need moreplace
thanquadrilaterals
and so on..),
while the average size of the cells increases again forpolygons
with 6, 7, etc. sides as ailneighbour
discs cannot betouching.
In
binary
mixtures, the strongdiscrepancy
in the disc cell size induces a strongnon-hnearity
of the Lewis law with a
rapid change
at n =6
(see Fig.
5 for C=
0.48,
as above ; for 4 w n w8,
the values ofA~
come from an average over several hundredcells).
For a size ratio(a)
o-i
A o
0~ 1 U 2 2~
(b)
o-i
o-s i i-s 2
Fig.
4.Histogram
of normabzed areas(a)
for a monosizepacking
at C=
0.46 (b) for a
binaly packing
at C
= 0.48 with ni = 0.5.
of 4 and medium concentration small cells have on average areas of 4 to 10 times smaller than the
large
ones and thechange
at n = 6 is verysharp.
One may wonder whether some linear behaviour may existseparately
for small andlarge
discs.Actually
this is not so for compactassemblies;
ifA~
behavesroughly
hke anincreasing (more
or lesslinear)
function ofn for both sizes at low
packing
fraction as small andlarge
discs are not verydifferentiated,
mthe compact case, the 2 classes behave
differently
: for smalldiscs, A~
is a function ofn similar to that in the monosize case, with a minimum (at n
=
4)
due to the steric exclusion.For
large discs, A~
isnearly
constant or can evenslowly
decrease withincreasing
n : this is because in this case a
langer
value of ncorresponds
to alanger
number of small discs around alarge
one and a better spacefilling.
JOURNAL DE PHYSIQUEt T 4, N' JANUARY 1994
12
An
~~
i
s
6
~
i
'n 2
3 4 5 6 7 8 9 10
Fig. 5. Average area A~ as a function of n in a binary
packing
at C=
0.48 with ni =
0.5 the Lewis law is not verified.
6.
Polydisperse packings.
As seen above, at
large packing
fraction, abinary
mixture leads to bimodal distributions andthen appears as the more
diametricallf opposed
to the monosizepacking.
One may thenwonder how results are modified when more radius sizes are mvolved which allow one to get a
wide range of cell dimensions. In order to see that, we have built numerical
polydisperse packings (6
sizes ofdiscs),
either dilute(RSA,
C0.5)
or dense(Powell,
C 0.85) packings,
with the same values of radii
(6, 10, 14, 18, 22, 26)
but differentproportions
of the disc species :uniform,
mcreasing anddecreasmg
linear distributions of the radii.6.1 TOPOLOGICAL PROPERTIES. For ail these
packings,
the distribution p~ of the number of sides of thepolygons
is ummodal with a maximum for n=
6
(Fig. 6).
Of course, theshape
of0.3 Pn
.
a
o
002
a
a Powell
. WA
a
a
o-i °
o
a
n 0
2 4 6 8 10 12
Fig. 6. Side number distribution p~ m a dense (Powell, C 0.85) and a dilute (RSA~ C 0.5)
polydisperse packing for a uniforrn distribution of radii.
the distribution
depends
on thecomposition
of the mixture : the more numerous the smallest discs, the wider the distribution forlarge
values of n. At agiven packing fraction,
thedistribution is wider than for a monosize
packing
and the value of q~ islanger. However,
the umversal law q~ =f~p~)
is well followedby
thepolydisperse packings.
The Aboav-Weaire law is
quite
well verified in thepolydisperse packings (Fig. 7)
with aparameter
a close to 1.3.However,
thelinearity
is not asperfect
as in monosizepackings.
70
nm(n)
6o
. Rs~
° Powefl
30
n 2o
3 5 7 9 11
Fig. 7. Aboav-Weaire law is quite well verified in dense and dilute
polydisperse packings
(here the radius distribution islinearly decreasmg).
The errors bars are of the order of magnitude of the symbols.6.2 METRIC PROPERTIES. The above results show that the defects appearing m a two-size
distribution of discs are to a
large
part eliminated for a muchlarger
distribution of radii, at least for thetopological properties.
This is nolonger
true for the metricproperties. Figure
8 shows thehistogram
of the normalized areas A of the cells for a densepacking
with linear mcreasing0.12
P(A)
o-io
0.08 m Powell
11 WA
0.06
o-m
0.02
A 0
0~ 1 1.S 2
Fig.
8.Histogram
of the area A of the cells, norrnahzed to its average value, for a dense and a dilutepacking,
m the case of a linearly increasmg distribution of radii.distribution of radii. One can see that the size of the
polygons
isdirectely
related to the size of the discs : the area distribution issplit
into 6separated
distributions : each of these comes fromone
species
of discs and itsheight
is reminiscent of the radius distribution. The same is true atlarge packing
fraction for the othercompositions.
For RSApackings,
thehistogram
of theareas is no
Ionger
multimodal as also shown infigure
8, because steric exclusion is lessimportant here.
As can be seen in
figure 9,
the Lewis law is not verified the behaviour ofA~
withn is
qualitatively
the same as in densebinary
mixtures(here again,
for 4 w n w8,
the values ofA~
come from an average on several hundredcells,
and thenon-linearity
cannot be attributed toa too weak
statistics).
Trienon-linearity
is less strong but is still evident in the dilutepackings.
The values of
A~ depend
on the disc size distribution : of course, for agiven packing fraction,
alarger
number of small discs leads to cells with smaller size. Thatexplains
the relativepositions
of the curvescorresponding
to the three radius distributions.3ww
An
o o
o ~
2000 A
+ a
A a
~~
. A
o A ~
A ~
° ~
3 5 7 9
4000
An
~~ A
o A
a
a
~ A
~~~
A a
a n
3
Fig. 9. Average area A~ as a function of n for dense (a) and dilute (b)
polydisperse
packings with respectively umform (6), hnearly increasmg (+) andlinearly
decreasmg (U) distribution of radii. The Lewis law is not vedfied.7. Conclusion.
We have
reported
hereexperimental
results on the statistics of cells obtained from the radical Voronoï tesselation ofbinary
mixtures of discs.Mosaics behave very
differently
from the « random » mosaics in the literature and from the mosaics of the monosizepackings.
The existence of 2 classes ofcells, depending strongly
onthe size of the central disc
(even
at mediumdensity)
leads to strongnon-regulanties
both in thetopological
and the metricproperties.
This holds both for theexperimental
and numerical assemblies and the effect is more and more accentuated as thepacking
fraction increases and when the size ratio islarge.
Finally,
inpolydisperse packings,
the distribution of the number of sides of the cells is moreequilibrated.
Moregenerally,
as to theirtopological properties,
the mosaicsgenerated
from the tesselation of thosepackings obey approximately
the laws of random mosaics. This is not so for their metricproperties,
which are stilllargely
affectedby
steric exclusion.We
awaiting
with the interest thegeneralisation
tobinary
andpolydisperse
assemblies of the argumentsleading
to the linear Aboav[9, 13]
and Lewis[10]
laws in random mosaics.Acknowledgments.
We would like to thank D. Bideau for useful discussions. This work was
partly supported by
the GDR CNRS «
Physique
des MilieuxHétérogènes Complexes
».References
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(1983)
Bideau D., Gervois A.,
Oger
L. and Troadec J. P., J.Phys.
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Viot P. and
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