J Elasticity (2006) 85: 120

DOI 10.1007/s10659-006-9065-1
Revised Bounds on the Elastic Moduli of
Two-Dimensional Random Polycrystals
Duc Chinh Pham
Received: 26 December 2005 / Accepted: 15 March 2006 /
Published online: 24 May 2006
Springer Science+Business Media B.V. 2006
Abstract Our earlier derived bounds on the elastic moduli of two-dimensional
random polycrystals [1, 2] involve a geometric restriction through an assumption on
the form of an isotropic eight-rank tensor. The general form of the tensor is used
in this study to reconstruct the bounds, which are expected to approach the scatter
range for the moduli of the irregular aggregate.
Mathematics Subject Classications (2000) 74Q20
Key words bounds elastic moduli two-dimensional polycrystals random
aggregate statistical isotropy statistical symmetry
1. Introduction
Macroscopic (effective) properties of randomly inhomogeneous materials, including
random polycrystals, depend upon the properties of their constituents as well as
material microstructure. Because of the irregular nature of the microgeometry of the
random aggregates, generally, there do not exist unique formulae for the effective
properties, which may scatter over some intervals. Hence, the purpose is to nd upper
and lower limits for those possible scatter intervals. General variational approach
has been developed to construct upper and lower bounds on the effective properties
[114] (i.e. to approach the limits from outside). Alternatively, one could also
approach the scatter limits from inside by constructing realizable geometric models,
e.g., as has been done in [15, 16]. In [1, 11, 13] we developed a variational approach
based on minimum energy principles and used polarization trial elds, which are
D. C. Pham (B)
Vietnamese Academy of Science and Technology, Vien Co hoc, 264 Doi Can, Hanoi, Vietnam
e-mail: pdchinh@im01.ac.vn
2 J Elasticity (2006) 85: 120
similar to those of Hashin and Shtrikman [4], to bound the effective properties of the
composites, and the results agree well with those fromthe general perturbation series
expansion approach [510, 17]. The advantage of the former approach is its simplicity
and effectiveness, especially in dealing with random polycrystals. The bounds on the
elastic moduli of two-dimensional random polycrystals derived in Pham [1] based on
the hypothesis that the shape and crystalline orientations of the constituent grains in
a random aggregate are not correlated (consult also [4, 68, 14, 18]). To evaluate the
bounds in Pham [1, 2] we suggested an assumption about an isotropic eighth-rank
tensor. In this work, that geometric restriction is to be substituted by the general
form of the isotropic tensor. In consequence, we obtain the new, more-sophisticated
and less-restricted, but more general bounds on the macroscopic elastic moduli of the
aggregate.
2. Formal Bounds
A representative volume element of the two-dimensional random polycrystal oc-
cupies circular region V of Euclidean space R
2
, the center of which is also the
origin of the Cartesian system of coordinates {x
1
, x
2
}. The representative volume
element V consists of N components occupying regions V

V of volume v

,
= 1, ..., N (the volume of V is assumed to be the unity); each component V

is composed of the grains of the same crystal orientation, the elastic property of
which is described by the fourth-rank tensor C(x) = C

, x V

. In particular, a
random uniphase polycrystal is supposed to be represented by such N-component
conguration when N , v

= v
0
=
1
N
0, with the grains of all possible crystal
orientations allowed to be presented equally. The contact between the grains is
perfect (i.e., without any slip or cleavage during deformation of the aggregate). The
average value of tensor C(x) on V (or of C

over all possible orientations ) is

dened as
C =
_
V
C(x)dx =

=
N

=1
v

. (1)
The effective elastic moduli C
e
of the polycrystal, which relate the average stress
and strain tensors on V, can be determined by the minimum energy principle

0
: C
e
:
0
= inf
=
0
_
V
: C : dx , (2)
where the strain eld (x) expressed through a displacement eld w

ij
=
1
2
(w
i, j
+ w
j,i
) , (3)

0
is a constant strain tensor; a Latin index after comma designates the differentiation
with respect to the respective Cartesian coordinate. Once V is assumed to be
statistically isotropic, the effective elastic tensor C
e
is a fourth-rank isotropic tensor
J Elasticity (2006) 85: 120 3
and can be expressed through the effective elastic bulk (K
e
), shear (
e
) moduli, and
the isotropic fourth-rank tensor function T(K, )
C
e
= T(K
e
,
e
) , (4)
T
ijkl
(k, ) = (K )
ij

kl
+ (
ik

jl
+
il

jk
) , (5)

ij
is usual Kronecker symbol. Instead of nding the exact solution of the difcult
problem (2) and (3) with irregular random geometry of V, one can substitute an
appropriately constructed trial eld into (2) to get upper bounds on the effective
moduli K
e
,
e
that is the approach we follow. In the process we use the Green func-
tion of the elastic equilibrium problem, which involves the harmonic and biharmonic
potentials

(x) =
1
2
_
V

ln | x y | dy ,

(x) =
1
8
_
V

| x y |
2
ln | x y | dy ,

(x) =
4

(x) =

, x V

. (6)
As the shape and crystalline orientations of the constituents in the random aggregate
are supposed to be uncorrelated, statistically isotropic and symmetric hypotheses for
them can be adopted. Statistically isotropic distribution of the components V

in the
circle V implies
1
v

_
V

,ij
dx =
1
2

ij

,
1
v

_
V

,ijkl
dx =
1
8
(
ij

kl
+
il

jk
+
ik

jl
)

. (7)
Let us introduce microgeometrical parameters A

, B

(, , = 1, ..., N):
A

=
_
V

ij


ij
dx ,

ij
=

,ij

1
v

_
V

,ij
dx ,
B

=
_
V

ijkl

ijkl
dx ,

ijkl
=

,ijkl

1
v

_
V

,ijkl
dx . (8)
Clearly, for all x V and all , = 1, ..., N,

ijkk
=

ij
,

ii
= 0 , (9)
where conventional summation on repeating Latin indices is assumed. Statistically
symmetry hypotheses for the aggregate implies [1, 12] ( = = = )
A

= v

( f
1
f
2
) , A

= v

(1 v

)[(1 v

) f
1
+ v

f
2
] ,
A

= v

[(v

1) f
1
v

f
2
] , A

= v

[(1 v

) f
2
+ v

f
1
] ;
B

= v

(g
1
g
2
) , B

= v

(1 v

)[(1 v

)g
1
+ v

g
2
] ,
B

= v

[(v

1)g
1
v

g
2
] , B

= v

[(1 v

)g
2
+ v

g
1
]; (10)
4 J Elasticity (2006) 85: 120
where f
1
, f
2
, g
1
, g
2
are microgeometry-dependent positive parameters, specically
f
1
/f
2
= g
1
/g
2
= 0 for the subclass of circular cell materials. Referring to the uniphase
polycrystal, the statistical symmetry hypothesis reects the observation that an
interchange of the materials between any two sets of the grains of different crystal
orientations (i.e., two components V

and V

) within the random polycrystal (the

representative volume element V) should not alter the overall characteristics of the
aggregate. Circular cell polycrystals are idealistic polydispersed random aggregates
composed exclusively of the grains of circular form. The symmetric cell materials
have been rstly considered by Miller [6], and Williemse and Caspers [8], who
dened them as: The space is completely covered by cells; cells are distributed
in a manner such that the material is statistically homogeneous and isotropic; the
material properties of a cell are statistically independent of those of any other cells;
the material properties are statistically independent of the geometrical distribution
(shape, size, orientation and arrangement) of cells. Examples include Voronoi or
Delaunay tessellations of the space from a set of center-points thrown randomly into
the material space, where the cells are assigned the crystal orientations randomly.
The microgeometry-dependent parameters A

, B

, f
1
, f
2
, g
1
, g
2
correspond to the
respective ones of [6, 8] by the relations specied in [13, 19]. They contain three-point
correlation information about the microgeometry of the aggregate. The geometric
parameters A

, B

dened in (8) are not independent. Here, in particular, we

dene
E

ijkl
=

ijkl
S(

ij

kl
+

kl

ij
+

ik

jl
+

jl

ik
+

il

jk
+

jk

il
), (11)
where S is a scalar parameter. From the obvious inequality
0
_
V

ijkl
E

ijkl
dx = B

12S(1 3S), (12)

taking S =
1
6
, we see B

. Since the positive geometric parameters f

1
,
f
2
, g
1
, g
2
in (10) describe a specic microstructure of the symmetric cell material and
do not depend on the volume fraction v

, we deduce
g
1
f
1
, g
2
f
2
. (13)
We come back to the minimum energy principle (2). Following the procedure of
Pham [1, 11], we make use of Hashin and Shtrikman trial polarization eld (K
0
and

0
any positive values; Greek indices under the sign of sum run on natural numbers
from 1 to N)

ij
=
K
0

0
(K
0
+
0
)

kl

,ijkl

1
2
0

( p

mi

, jm
+ p

mj

,im
) , (14)
where
p

= D

: (C
0
+ C

) :
0
,
D

= E (C

+ C

)
1
:
_

(C

+ C

)
1
_
1
,
E = T(
1
2
,
1
2
) , C
0
= T(K
0
,
0
) ,
C

= T(K

) , K

=
0
,

=
K
0

0
K
0
+ 2
0
, (15)
J Elasticity (2006) 85: 120 5
taking into account the statistical isotropy hypothesis (7), to get from the energy
principle (2) the general formal upper bounds on the effective moduli [1]

0
: C
e
:
0

0
: P
C
(C, K
0
,
0
) :
0
+U

() , (16)
where
P
C
(C, K
0
,
0
) =
_

(C

+ C

)
1
_
1
C

= T
_
P
K
(C, K
0
,
0
), P

(C, K
0
,
0
)
_
,
P
K
(C, K
0
,
0
) =
_
(C + C

)
1
iijj
_
1
K

,
P

(C, K
0
,
0
) =
_
(C + C

)
1
ijij

1
2
(C + C

)
1
iijj
_
1

, (17)
U

() =

_
V

: (C

C
0
) :

dx
=
1

2
0

,,
C
0
ijkl
_

2
p

mn
p

pq
_
V

ijmn

klpq
dx + p

im
p

k n
_
V

jm

ln
dx
2p

mn
p

k p
_
V

ijmn

lp
dx
_
, (18)

=
1
v

_
V

dx , C
0
= C

C
0
, =
K
0
K
0
+
0
.
Similarly, the formal lower bounds on the elastic moduli are constructed from
minimum complementary energy principle [1].
3. Evaluation of the Bounds
To construct the best possible upper bounds we need to evaluate U

in (18), which
contains integral expressions formed with the harmonic and biharmonic potentials,
with the help of statistically isotropic and symmetry hypotheses. These integrals are
certain high rank tensors. According to statistical hypothesis about polycrystalline
random microgeometry, such tensors are the isotropic ones. General forms of the
isotropic tensors are given by the theory of algebraic invariants [2023]. Some low-
rank isotropic tensors have already been given in (7). Consider the isotropic fourth-
rank tensor
_
V

jm

ln
dx, which is symmetric on indices j and m, and on l and n. The
general form of that tensor, involving three isomers, is
_
V

jm

ln
dx = K

1

jm

ln
+ M

1
(
jl

mn
+
jn

ml
) , (19)
6 J Elasticity (2006) 85: 120
where K

1
and M

1
are some scalar invariants, which can be related to the geometric
parameters dened in (8), using (9):
0 =
_
V

jj


ll
dx = 4K

1
+ 4M

1
,
A

=
_
V

jm

jm
dx = 2K

1
+ 6M

1
. (20)
Hence
_
V

jm

ln
dx =
1
4
A

(
jl

mn
+
jn

ml

jm

ln
) . (21)
Next, consider the isotropic sixth-rank tensor
_
V

ijmn

lp
dx, which is symmetric on
indices i, j, m, n, and on l, p. The general form of that tensor, involving 15 isomers, is
_
V

ijmn

lp
dx = K

2

ijmn

lp
+M

2
(
il

jmn p
+
jl

imn p
+
ml

ijn p
+
nl

ijm p
), (22)
where

ijmn
=
ij

mn
+
im

jn
+
in

jm
. (23)
The scalar invariants K

2
and M

2
can be found with the help of (8) and (9):
0 =
_
V

iin n

ll
dx = 16K

2
+ 32M

2
,
A

=
_
V

ijn n

ij
dx = 8K

2
+ 40M

2
. (24)
Hence
_
V

ijmn

lp
dx =
1
12
A

ijmn

lp
+
1
24
A

(
il

jmn p
+
jl

imn p
+
ml

ijn p
+
nl

ijm p
). (25)
Lastly, consider the isotropic eighth-rank tensor
_
V

ijmn

klpq
dx, which is symmetric
on indices i, j, m, n, and on k, l, p, q. The general form of that tensor, involving 105
isomers, is
_
V

ijmn

klpq
dx = K

3

ijmn

klpq
+ M

3

ijmn
klpq
+ L

ijmn
klpq
, (26)
J Elasticity (2006) 85: 120 7
where

ijmn
klpq
=
ik

jmn
lpq
+
il

jmn
k pq
+
ip

jmn
klq
+
iq

jmn
klp
,

jmn
lpq
=
jl

mn
pq
+
jp

mn
l q
+
jq

mn
lp
,

mn
pq
=
m p

nq
+
mq

n p
,

ijmn
klpq
=
ij

mn
klpq
+
im

jn
klpq
+
in

jm
klpq
+
jm

in
klpq
+
jn

im
klpq
+
mn

ij
klpq
,

mn
klpq
=
1
2
(
mnk
lpq
+
mnl
k pq
+
mn p
klq
+
mnq
klp
) . (27)
We put the coefcient 1/2 in the last equality (27), because as one can check every
isomer inside the brackets appear twice. The form (26) and (27) is similar to that of
Weaver [25]. The scalar invariants K

3
, M

3
and L

3
can be found with the help of
(8) and (9):
0 =
_
V

iin n

k k p p
dx = 64K

3
+ 64M

3
+ 288L

3
,
A

=
_
V

ijn n

ijp p
dx = 32K

3
+ 80M

3
+ 300L

3
,
B

=
_
V

ijpq

ijpq
dx = 24K

3
+ 120M

3
+ 264L

3
. (28)
Hence
_
V

ijmn

klpq
dx =
_
5
624
B

23
624
A

ijmn

klpq
+
_
1
48
B

1
48
A

ijmn
klpq
+
_
1
78
A

1
156
B

ijmn
klpq
.
(29)
In Pham [1, 24], to calculate bounds on the effective elastic moduli of the
composites, we presumed a hypothesis about the isotropic eighth-rank tensor, which
is just a specic form of (26) without the last term involving L

3
. That is equivalent
to imposing the restriction B

= 2A

, which has been stated in the mentioned

references, hence should be valid only for the restricted microgeometries. Here we
see that the most general form of the isotropic tensor is (26), which leads to (29).
8 J Elasticity (2006) 85: 120
Substituting (21), (25) and (29) into (18), we obtain
U

=
1

2
0

,,
_
C
0
iik k
p

jj
p

ll
_
5
2
624
B

23
2
624
A

_
+C
0
iik k
p

jl
p

jl
_

2
39
A

2
78
B

_
+C
0
ijij
p

k k
p

ll
_

2
39
A

2
78
B

_
+C
0
ijij
p

kl
p

kl
_

2
12
B

2
12
A

_
+C
0
iikl
p

kl
p

jj
__

6

5
2
52
_
A

+

2
156
B

_
+C
0
iikl
p

k j
p

l j
__
8
2
39


6
_
A

4
2
39
B

_
+C
0
ijkj
p

ik
p

ll
__
8
2
39


6
_
A

4
2
39
B

_
+C
0
ijkj
p

il
p

kl
__
1
4


6

5
2
39
_
A

+
3
2
13
B

_
+C
0
ijkl
p

ij
p

kl
__

3

1
4

3
2
13
_
A

+
3
2
26
B

_
+C
0
ijkl
p

ik
p

jl
__
1
4


3
+
8
2
39
_
A

4
2
39
B

_
. (30)
Making use of (10), one may transform (30) into
U

=
1

2
0

0
: T
_
(K
0
+ K

)
2
U
K
, (
0
+

)
2
U
M
_
:
0
, (31)
where
U
K
= U
Kf 1
f
1
+U
Kf 2
f
2
+U
Kg1
g
1
+U
Kg2
g
2
,
U
M
= U
Mf 1
f
1
+U
Mf 2
f
2
+U
Mg1
g
1
+U
Mg2
g
2
, (32)
Particular expressions of U
Kf 1
, U
Kf 2
, U
Kg1
, U
Kg2
, U
Mf 1
, U
Mf 2
, U
Mg1
, U
Mg2
are given
in Apendix [see (A1A7)].
For specic circular cell polycrystals f
1
= g
1
= 0. Now if we take K
0
= K
V
,
0
=

V
, then from (A6) we get also U
Kf 2
= U
Kg2
= 0, hence from (32) U
K
= 0, and
from(16), (17) and (31) the simple upper bound for K
e
:
K
e
K
u
c
= P
K
(C, K
V
,
V
) . (33)
Similarly, the upper bound on the shear modulus of circular cell polycrystals reads

e

u
c
= P

(C, K
V
,
V
) . (34)
For general shape-unspecied upper bounds, the positive geometric parameters
f
1
, g
1
, f
2
, g
2
are not specied. Using restriction (13) and taking K
0
K
V
,
0

V
,
with (A6) we get
U
Kf 2
f
2
+U
Kg2
g
2
(U
Kf 2
+U
Kg2
) f
2
=
_
_

jjp p
D

llq q
_
_
(K
V
K
0
)
_
1
12

2
39

2
_
+ (
V

0
)
_
6
13

5
6
+
1
2
__
+
_

D
d1
klp p
D
d1
klq q
_
_
(K
V
K
0
)
_
6
13

5
6
+
1
2
_
+(
V

0
)
_
1
3

1
39

2
___
f
2
0,
(35)
J Elasticity (2006) 85: 120 9
keeping in mind that 0 1 as can be seen from (18). Also,
U
Kf 1
f
1
+U
Kg1
g
1
(U
Kf 1
+U
Kg1
) f
1
if U
Kg1
0 . (36)
Hence, if we take any K
0
,
0
such that
K
0
K
V
,
0

V
, U
Kg1
0 , U
Kf 1
+U
Kg1
0 , (37)
then from (32) we get U
K
0, and from (16), (17) and (31) an upper bound K
e

P
K
(C, K
0
,
0
) (by neglecting the negative U
K
to strengthen the inequality). The best
possible shape-unspecied upper bound (for all possible positive microgeometric
parameters f
1
, g
1
, f
2
, g
2
) on the effective bulk modulus is
K
e
K
u
= inf
K
0
,
0
{P
K
(C, K
0
,
0
) | K
0
K
V
,
0

V
, U
Kg1
0, U
Kf 1
+U
Kg1
0},
(38)
keeping in mind that P
K
is dened in (17), K
V
,
V
in (A5), and U
Kf 1
, U
Kg1
in (A1)
and (A2). Similarly, the best possible shape-unspecied upper bound on the effective
shear modulus reads

e

u
= inf
K
0
,
0
{P

(C, K
0
,
0
) | K
0
K
V
,
0

V
, U
Mg1
0, U
Mf 1
+U
Mg1
0}.
(39)
Analogously, the shape-unspecied lower bounds on the effective moduli are con-
structed from the minimum complementary energy principle and have the forms
K
e
K
l
= sup
K
0
,
0
{P
K
(C, K
0
,
0
) | K
1
0
K
1
R
,
1
0

1
R
,
U
Kg1
0, U
Kf 1
+U
Kg1
0},

e

l
= sup
K
0
,
0
{P

(C, K
0
,
0
) | K
1
0
K
1
R
,
1
0

1
R
,
U
Mg1
0, U
Mf 1
+U
Mg1
0}, (40)
where
K
R
= [(C

)
1
iijj
]
1
,
R
= [(C

)
1
ijij

1
2
(C

)
1
iijj
]
1
(41)
are Reuss harmonic averages. U
Kf 1
, U
Kg1
, U
Mf 1
, U
Mg1
have similar forms as those
of U
Kf 1
, U
Kg1
, U
Mf 1
, U
Mg1
, with C
0
and D

taking the places of C

0
and D

,
respectively,
C
0
= C
0
: [(C

)
1
(C
0
)
1
] : C
0
,
D

= C
0
:
_
E [(C

)
1
+ (C

)
1
]
1
:

[(C

)
1
+ (C

)
1
]
1

1
_
. (42)
10 J Elasticity (2006) 85: 120
The lower bounds for the specic circular cell polycrystals are
K
e
K
l
c
= P
K
(C, K
R
,
R
) ,

e

l
c
= P

(C, K
R
,
R
) . (43)
The simple bounds for specic circular cell polycrystals (33), (34) and (43) are
identical to those derived in Pham [1], however the general ones (38)(40) are not.
4. Calculation of the Bounds
As all the sums on repeating Latin indices involving C

ijkl
and D

ijkl
in our nal
formulae (A1) and (A2),... are tensor invariants (scalars), they do not depend on
specic orientation ; hence all the constants C

ijkl
and D

ijkl
there can be taken in the
basic crystal reference and denoted as C
ijkl
and D
ijkl
, respectively. In the literature
the convenient two-index notation C
ij
for crystal elastic constants are used. A planar
crystal of general anisotropy has six independent elastic constants, which in two-index
notation are given as C
11
, C
22
, C
33
, C
12
, C
13
, C
23
. The correspondence between the
usual fourth-rank elasticity tensor and those in two-index notation is
C
1111
= C
11
, C
2222
= C
22
, C
1212
= C
33
,
C
1122
= C
12
, C
1112
= C
13
, C
2212
= C
23
. (44)
Voight and Reuss averages are
K
V
=
1
4
(C
11
+C
22
+ 2C
12
) ,
V
=
1
8
(C
11
+C
22
2C
12
+ 4C
33
) ,
K
R
=
C
11
C
22
C
33
+ 2C
12
C
13
C
23
C
2
12
C
33
C
2
23
C
11
C
2
13
C
22
C
11
C
33
+C
22
C
33
C
2
13
C
2
23
+ 2C
13
C
23
2C
12
C
33
,

R
=
2(C
11
C
22
C
33
+ 2C
12
C
13
C
23
C
2
12
C
33
C
2
23
C
11
C
2
13
C
22
)
C
11
C
33
+C
22
C
33
C
2
13
C
2
23
2C
13
C
23
+ 2C
12
C
33
+C
11
C
22
C
2
12
. (45)
The property functions P
K
and P

from (17) take the particular forms

P
K
(C, K
0
,
0
) =
0
+
C
+
11
C
+
22
C
+
33
+ 2C
+
12
C
13
C
23
(C
+
12
)
2
C
+
33
C
2
23
C
+
11
C
2
13
C
+
22
C
+
11
C
+
33
+C
+
22
C
+
33
C
2
13
C
2
23
+ 2C
13
C
23
2C
+
12
C
+
33
,
P

(C, K
0
,
0
) =

+
2[C
+
11
C
+
22
C
+
33
+2C
+
12
C
13
C
23
(C
+
12
)
2
C
+
33
C
2
23
C
+
11
C
2
13
C
+
22
]
C
+
11
C
+
33
+C
+
22
C
+
33
C
2
13
C
2
23
2C
13
C
23
+2C
+
12
C
+
33
+C
+
11
C
+
22
(C
+
12
)
2
,
(46)
J Elasticity (2006) 85: 120 11
Table 1 The elastic constants (in GPa) of some monoclinic crystals in their plane of symmetry
C
11
C
22
C
33
C
12
C
13
C
23
S
K
S

S 20.5 48.3 4.3 15.9 0 0 0.0059 0.0056

U 198.6 267.1 124.4 107.6 0 0 0.0003 0.0013
SiO
2
160.8 231.6 73.3 102.9 36.2 39.3 0.0049 0.0034
SnF
2
47.9 33.6 12.9 5.3 5.1 6.5 0.0007 0.0030
C
14
H
14
9.45 7.20 2.55 4.15 2.4 0.7 0.0112 0.0042
KAl Si
3
O
8
66 122 23.6 26 3 13 0.0020 0.0023
NaFeSi
2
O
6
186 234 51.0 71 10 21 0.0003 0.0004
NaAl Si
3
O
8
74 128 29.6 39.4 6.6 20.00 0.0029 0.0023
C
12
H
10
5.95 14.6 2.26 2.88 0.40 2.02 0.0068 0.0073
KHC
2
O
4
15.6 87.7 3.60 8.24 1.50 3.09 0.0537 0.0889
S
K
= (K
u
K
l
)/(K
u
+ K
l
) and S

= (
u

l
)/(
u
+
l
) are the scatter deviation mea-
sures for the effective bulk and shear moduli of the random polycrystals (K
u
, K
l
,
u
,
l
from
Table 2).
where
C
+
11
= C
11
+
0
+

, C
+
22
= C
22
+
0
+

, C
+
33
= C
33
+

,
C
+
12
= C
12
+
0

=
K
0

0
K
0
+ 2
0
. (47)
The bounds for circular cell polycrystals are calculated according to (33), (34) and
(43). Expansive expressions of the terms U
Kf 1
, U
Kg1
, ... needed for calculations of
the general shape-unspecied bounds in (38)(40) are given in Appendix (A8A19).
For numerical applications, we consider some monoclinic crystals, whose elastic
constants in their plane of symmetry are taken from [26] and collected in Table 1.
In the Table 2, the new general (shape-unspecied) bounds K
u
, K
l
.
u
,
l
from (38)
to (40), the bounds for circular cell polycrystals K
u
c
, K
l
c

u
c
,
l
c
from (33), (34) and
Table 2 The upper and lower bounds on the polycrystalline effective moduli: K
u
, K
l
,
u
,
l
- the
general shape-unspecied bounds; K
u
c
, K
l
c
,
u
c
,
l
c
- the bounds for specic circular cell polycrystals
(all in GPa)
K
u
K
u
c
K
l
c
K
l

u
c

l
c

l
S 21.61 21.61 21.36 21.36 5.750 5.735 5.686 5.686
U 167.5 167.5 167.4 167.4 85.77 85.77 85.54 85.54
SiO
2
132.5 132.5 131.6 131.2 54.56 54.52 54.30 54.19
SnF
2
22.37 22.37 22.34 22.33 13.32 13.32 13.24 13.24
C
14
H
14
5.603 5.603 5.564 5.556 2.001 1.996 1.978 1.956
KAl Si
3
O
8
54.83 54.83 54.65 54.61 26.57 26.53 26.46 26.45
NaFeSi
2
O
6
136.4 136.4 136.4 136.4 58.09 58.08 58.05 58.04
NaAl Si
3
O
8
63.44 63.44 63.18 63.07 27.89 27.87 27.79 27.76
C
12
H
10
5.481 5.481 5.408 5.406 2.527 2.517 2.490 2.490
KHC
2
O
4
18.53 18.53 16.64 16.64 7.035 6.833 5.886 5.886
12 J Elasticity (2006) 85: 120
(43) are presented. The shape-unspecied bounds generally are broader than the
ones derived for restricted geometries in Pham[1, 2], but remain coincide with, or not
far from the much simpler (and tighter) bounds for the subclass of circular cell poly-
crystals, which are supposed to approximate practical equi-axed cell aggregates. The
scatter deviation measures S
K
=(K
u
K
l
)/(K
u
+ K
l
) and S

= (
u

l
)/(
u
+
l
)
are included in Table 1, which indicate that the uncertainty is mainly a few
thousandths.
5. Closure
The bounds derived in Pham [1] are decit because the form of the isotropic eight
rank tensor used there is not correct for the general random polycrystal, which
should have the form (26). As already noted, the assumption in Pham [1] means an
additional geometric restriction on the aggregate microgeometry, hence the bounds
therein should be more restrictive than the ones derived in this new work. Because of
the change, the uctuation terms in the expressions of the bounds here are more
complicated and contain four positive geometric parameters f
1
, g
1
, f
2
, g
2
, which
are subjected to the additional restrictions (13) (in Pham [1], the uctuation terms
contain just two geometric parameters). Allowing these geometric parameters to
take all possible values, we obtain the shape-unspecied bounds given. The bounds
for specic circular cell polycrystals remain simple and exactly as those derived in
Pham [1].
Our bounds on the elastic moduli of random polycrystals do not require a
particular irregular microgeometry be specied, but just overall statistical isotropy
and symmetry assumptions, and are partly third order in expansion series in powers
of the crystal anisotropy contrast, which are denitely tighter than the rst order
VoigtReussHill bounds and second order HashinShtrikman ones. Meanwhile the
general perturbation approach reveals that one cannot go to the third or higher
order bounds without specifying certain shape and arrangement information about
the grains, in addition to the statistical isotropy and symmetry assumptions, but
such information is unlikely to be denite for random polycrystalline materials with
irregular microgeometry. Hence our bounds might be close to the best possible
ones in predicting the scatter ranges for the polycrystals effective moduli. Should
the effective properties of random polycrystals (and more generally randomly
inhomogeneous materials) scatter, or should they be unique as widely assumed?
We do not have mathematical or experimental proofs for either claims. Unique-
ness (in the large volume representative element limit) is generally presumed for
rigorous mathematical treatment of a homogenization problem. Uncertainty of the
macroscopic properties related to the nite size effect of the representative volume
element (relative to the sizes of the constituent inhomogeneities) should decrease
as the size of the representative volume element increases [27, 28]. However the
uncertainty may not decrease to zero, as the size of the representative volume
element increases to innity, but to approach asymptotically certain scatter interval
for a particular random system. There are specic random systems with unique
effective properties, as evidenced analytically or numerically, which include random
hard spheres (circles), random overlapping spheres (circles), multicoated sphere
J Elasticity (2006) 85: 120 13
(circle) assemblages... [29, 30], however our views is that the uncertainty generally
prevails for congurations with irregular microgeometries. It is imperative to perform
numerical simulations to access the possible uniqueness or uncertainty of the elastic
moduli of the Voronoi or Delaunay random aggregates compared to our bounds
established in this study. This is a formidable computing work, however the problem
for two-dimensional random polycrystals is greatly simpler than the respective for
the three-dimensional aggregates. It might be even simpler to treat the conductivity
problem for the two-dimensional polycrystals. However the effective conductivity
of the macroscopically isotropic aggregates has been found analytically and unique
due to the specic mathematical structure of the two-dimensional conductivity
problem [30], hence the case is not typical for the general randomly inhomogeneous
media. Closely related to the problem considered here, the numerical simulations
for random Voronoi cellular solid in [31, 32] reveal that the effective moduli of the
material scatter over an interval as large as about fewpercents of the averaged moduli
in agreement with empirical observations. Still much more efforts are needed to
achieve the convincing quantitative results: Larger representative volume elements,
broader and more systematic procedures are to be developed until a clear asymptotic
tendency toward an uncertainty or uniqueness can be established. Another related
interesting but difcult subject is the random irregular network problem. Up to
the present, in the literature, the numerical simulations have been carried out just
for random regular networks, for which the uniqueness is evidenced, however the
effective properties are distinctly different for different particular kinds of the base
(regular) skeletons (see, e.g., [29] and the references therein).
If the effective moduli of a randomly inhomogeneous material should scatter and
not unique, the homogeneity and isotropy hypotheses for it would not be exact
anymore and could be considered only as approximate. Hence, the macroscopic
moduli tensor C
e
determined for a particular representative polycrystalline sample
may be slightly anisotropic, and the bounds should be given more generally as

0
: T(K
l
,
l
) :
0

0
: C
e
:
0

0
: T(K
u
,
u
) :
0
, for all symmetric
0
. (48)
Moreover all the mathematical bounds based on those hypotheses become not
rigorous and should be understood in asymptotic sense (roughly speaking, the bounds
may be violated by amounts asymptotically small compared to the intervals between
the bounds) [33]. In that sense, the scatter measures S in Table 1 should also contain
certain asymptotic error, which is asymptotically small compared to S. Here we do
not consider size effects. If the sizes of the grains become signicant compared to
macroscopic dimensions of interest, the uncertainty of the macroscopic behaviors
should be larger [28, 29]. Here we consider random aggregates where the shape and
crystalline orientations of the grains are uncorrelated. If local texture development
or articial arrangements of the grains are allowed in all possible combinations, the
possible range for the effective properties also should be much larger [15, 34].
High-accuracy numerical simulations (most simple to be performed for the two-
dimensional aggregates) and experiments should test the possible uniqueness or
uncertainty of the effective moduli of random aggregates and practical validity of
our bounds.
14 J Elasticity (2006) 85: 120
Acknowledgements This work is supported by the Program of Basic Research in Natural Science.
Appendix
There are the particular expressions of the terms of (31):
U
Kf 1
=
_

C
0
iik k
D

jjpp
D

llq q
_
_

23
2
624
_
+
_

C
0
iik k
D

jlp p
D

jlq q
_

2
39
+
_

C
0
ijij
D

k kp p
D

llqq
_

2
39
+
_

C
0
ijij
D

klpp
D

klqq
_
_

2
12
_
+
_

C
0
iikl
D

klp p
D

jjqq
_
_

6

5
2
52
_
+
_

C
0
iikl
D

kjp p
D

l jq q
_
_
8
2
39


6
_
+
_

C
0
ijk j
D

ikp p
D

llq q
_
_
8
2
39


6
_
+
_

C
0
ijk j
D

ilp p
D

klqq
_
_
1
4

5
2
39


6
_
+
_

C
0
ijkl
D

ijpp
D

klqq
_
_

3

1
4

3
2
13
_
+
_

C
0
ijkl
D

ik pp
D

jlq q
_
_
1
4


3
+
8
2
39
_
, (A1)
U
Kg1
=
_

C
0
iik k
D

jjp p
D

llqq
_
5
2
624
+
_

C
0
iik k
D

jlp p
D

jlq q
_
_

2
78
_
+
_

C
0
ijij
D

k kpp
D

llqq
_
_

2
78
_
+
_

C
0
ijij
D

klpp
D

klqq
_

2
12
+
_

C
0
iikl
D

klpp
D

jjq q
_

2
156
+
_

C
0
iikl
D

k jpp
D

l jq q
_
_

4
2
39
_
+
_

C
0
ijk j
D

ik pp
D

llq q
_
_

4
2
39
_
+
_

C
0
ijk j
D

ilp p
D

klqq
_
3
2
13
+
_

C
0
ijkl
D

ijp p
D

klqq
_
3
2
26
+
_

C
0
ijkl
D

ikp p
D

jlq q
_
_

4
2
39
_
. (A2)
U
Kf 2
and U
Kg2
have almost the same forms as U
Kf 1
from (A1) and U
Kg1
from
(A2), respectively, with all the sums

C
0
ijkl
D

mnpq
D

rstu
being substituted by

C
0
ijkl

mnpq
D

rstu
(for all possible Latin lower indices). U
Mf 1
, U
Mf 2
, U
Mg1
, U
Mg2
have
the forms similar to those of U
Kf 1
, U
Kf 2
, U
Kg1
, U
Kg2
, respectively, with all tensor-
components D

ijp p
and D

ijqq
being substituted by D
d2
ijpq
(for all possible indices i and
j), where
D
d2
ijpq
= D

ijpq

1
2

pq
D

ijn n
. (A3)
J Elasticity (2006) 85: 120 15
The terms U
Kf 2
, U
Kg2
, U
Mf 2
, U
Mg2
contain the sums of the type

C
0
ijkl
, which
could be calculated beforehand:

C
0
ijkl
= T
ijkl
(K
V
K
0
,
V

0
) , (A4)
where
K
V
=
1
4
C

iijj
,
V
=
1
4
C

ijij

1
8
C

iijj
(A5)
are the Voigts arithmetic averages. Hence, the terms can be simplied considerably:
U
Kf 2
=
_

jjpp
D

llqq
_
_
(K
V
K
0
)
_
1
12

4
39

2
_
+ (
V

0
)
_
11
26

5
6
+
1
2
__
+
_

D
d1
klpp
D
d1
klqq
_
_
(K
V
K
0
)
_
11
26

5
6
+
1
2
_
+ (
V

0
)
_
1
3

41
39

2
__
,
U
Kg2
=
_

jjpp
D

llqq
_
_
(K
V
K
0
)
2
39
+ (
V

0
)
1
26
_

2
+
_

D
d1
klpp
D
d1
klqq
_
_
(K
V
K
0
)
1
26
+ (
V

0
)
40
39
_

2
, (A6)
where
D
d1
klpp
= D

klpp

1
2

kl
D

n npp
. (A7)
Expansive expressions of U
Kf 1
, U
Kg1
in two-index-crystal notation are:
U
Kf 1
=
_
(D
11
+ D
12
)
2
+ (D
31
+ D
32
)
2
_

_
_
C
0
11
+C
0
22
_
_
1
4


3


2
26
_
+C
0
12
_
20
2
39


3
_
C
0
33
_
1
2

23
2
39


3
__
+(D
11
+ D
12
)
2
_
2C
0
33
_

3

1
4

8
2
39
_

_
C
0
11
+C
0
12
_

2
39
2C
0
12
_

3

1
4

3
2
13
__
+(D
31
+ D
32
)
2
_
C
0
33
_
2
3

1
2

20
2
39
_
+2C
0
12
_
1
4


3
+
8
2
39
__
(D
11
+ D
12
)(D
31
+ D
32
)(C
0
13
C
0
23
)
4
2
39
, (A8)
16 J Elasticity (2006) 85: 120
U
Kg1
=
_
(D
11
+ D
12
)
2
+ (D
31
+ D
32
)
2
_
_
(C
0
11
+C
0
22
)
7
26
C
0
12
10
39
+C
0
33
31
39
_

2
+(D
11
+ D
12
)
2
_
(C
0
11
+C
0
12
)
1
78
C
0
12
3
13
+C
0
33
8
39
_

2
+(D
31
+ D
32
)
2
_
C
0
33
10
39
C
0
12
8
39
_

2
+(D
11
+ D
12
)(D
31
+ D
32
)(C
0
13
C
0
23
)
2
2
39
, (A9)
where
D
11
= D
1111
= 1 K
+
(S
+
12
+ S
+
11
) +
+
(S
+
12
S
+
11
) ,
D
22
= D
2222
= 1 K
+
(S
+
12
+ S
+
22
) +
+
(S
+
12
S
+
22
) ,
D
12
= D
1122
= K
+
(S
+
12
+ S
+
11
)
+
(S
+
12
S
+
11
) ,
D
21
= D
2211
= K
+
(S
+
12
+ S
+
22
)
+
(S
+
12
S
+
22
) ,
D
33
= D
1212
=
1
2
2
+
S
+
33
, D
13
= D
1112
= 2
+
S
+
13
,
D
31
= D
1211
= K
+
(S
+
13
+ S
+
23
)
+
(S
+
13
S
+
23
) ,
D
23
= D
2212
= 2
+
S
+
23
,
D
32
= D
1222
= K
+
(S
+
13
+ S
+
23
) +
+
(S
+
13
S
+
23
) , (A10)
K
+
= P
K
(C, K
0
,
0
) +
0
,
+
= P

(C, K
0
,
0
) +

, (A11)
S
+
11
=
C
+
22
C
+
33
C
2
23

+
c
, S
+
22
=
C
+
11
C
+
33
C
2
13

+
c
,
S
+
12
=
C
13
C
23
C
+
12
C
+
33

+
c
, S
+
33
=
C
+
11
C
+
22
(C
+
12
)
2
4
+
c
,
S
+
13
=
C
+
12
C
23
C
+
22
C
13
2
+
c
, S
+
23
=
C
+
12
C
13
C
+
11
C
23
2
+
c
,

+
c
= C
+
11
C
+
22
C
+
33
+ 2C
+
12
C
13
C
23
(C
+
12
)
2
C
+
33
C
2
23
C
+
11
C
2
13
C
+
22
; (A12)
and
C
0
11
= C
0
1111
= C
11
K
0

0
, C
0
22
= C
0
2222
= C
22
K
0

0
,
C
0
12
= C
0
1122
= C
12
K
0
+
0
, C
0
33
= C
0
1212
= C
33

0
,
C
0
13
= C
0
1112
= C
13
, C
0
23
= C
0
2212
= C
23
. (A13)
J Elasticity (2006) 85: 120 17
For calculations of U
Mf 1
, U
Mg1
we need
C
0
iikk
D

jjpq
D

llpq
=(C
0
11
+C
0
22
+2C
0
12
)
_
(D
11
+D
21
)
2
+ (D
12
+D
22
)
2
+ 2(D
13
+D
23
)
2
_
,
C
0
iik k
D

jlpq
D

jlpq
= (C
0
11
+C
0
22
+ 2C
0
12
)
_
D
2
11
+ D
2
22
+ D
2
12
+ D
2
21
+ 2D
2
13
+ 2D
2
23
+ 2D
2
31
+ 2D
2
32
+ 4D
2
33
_
,
C
0
ijij
D

k kpq
D

llpq
= (C
0
11
+C
0
22
+ 2C
0
33
)
_
(D
11
+ D
21
)
2
+ (D
13
+ D
23
)
2
_
2,
C
0
ijij
D

klpq
D

klpq
= (C
0
11
+C
0
22
+ 2C
0
33
)
_
D
2
11
+ D
2
22
+ D
2
12
+ D
2
21
+ 2D
2
13
+ 2D
2
23
+ 2D
2
31
+ 2D
2
32
+ 4D
2
33
_
,
C
0
iikl
D

klpq
D

jjpq
= (C
0
11
+C
0
12
)
_
D
11
(D
11
+D
21
)+D
12
(D
12
+D
22
)+2D
13
(D
13
+D
23
)
_
+(C
0
12
+C
0
22
)
_
D
21
(D
11
+D
21
)+D
22
(D
12
+D
22
)+2D
23
(D
13
+D
23
)
_
+2(C
0
13
+C
0
23
)
_
D
31
(D
11
+D
21
)+D
32
(D
12
+D
22
)+2D
33
(D
13
+D
23
)
_
,
C
0
iikl
D

kjpq
D

l jpq
= (C
0
11
+C
0
12
)
_
D
2
11
+ D
2
12
+ 2D
2
13
+ D
2
31
+ D
2
32
+ 2D
2
33
_
+(C
0
12
+C
0
22
)
_
D
2
21
+ D
2
22
+ 2D
2
23
+ D
2
31
+ D
2
32
+ 2D
2
33
_
+2(C
0
13
+C
0
23
)
_
D
11
D
31
+D
12
D
32
+2D
13
D
33
+D
31
D
21
+D
32
D
22
+2D
33
D
23
_
,
C
0
ijk j
D

ikpq
D

llpq
= (C
0
11
+C
0
33
)
_
D
11
(D
11
+D
21
)+D
12
(D
12
+D
22
)+2D
13
(D
13
+D
23
)
_
+(C
0
22
+C
0
33
)
_
D
21
(D
11
+ D
21
) + D
22
(D
12
+ D
22
) + 2D
23
(D
13
+ D
23
)
_
+2(C
0
13
+C
0
23
)
_
D
31
(D
11
+ D
21
) + D
32
(D
12
+ D
22
) + 2D
33
(D
13
+ D
23
)
_
,
C
0
ijk j
D

ilpq
D

klpq
= (C
0
11
+C
0
33
)
_
D
2
11
+ D
2
12
+ 2D
2
13
+ D
2
31
+ D
2
32
+ 2D
2
33
_
+(C
0
22
+C
0
33
)
_
D
2
21
+ D
2
22
+ 2D
2
23
+ D
2
31
+ D
2
32
+ 2D
2
33
_
+2(C
0
13
+C
0
23
)
_
D
11
D
31
+D
12
D
32
+2D
13
D
33
+D
31
D
21
+D
32
D
22
+2D
33
D
23
_
,
C
0
ijkl
D

ijpq
D

klpq
= C
0
11
_
D
2
11
+ D
2
12
+ 2D
2
13
_
+C
0
22
_
D
2
21
+ D
2
22
+ 2D
2
23
_
+2C
0
12
_
D
11
D
21
+D
12
D
22
+2D
13
D
23
_
+ 4C
0
33
_
D
2
31
+D
2
32
+ 2D
2
33
_
+4C
0
13
_
D
11
D
31
+D
12
D
32
+2D
13
D
33
_
+4C
0
23
_
D
21
D
31
+D
22
D
32
+2D
23
D
33
_
,
C
0
ijkl
D

i kpq
D

jlpq
= C
0
11
_
D
2
11
+ D
2
12
+ 2D
2
13
_
+C
0
22
_
D
2
21
+ D
2
22
+ 2D
2
23
_
+2C
0
12
_
D
2
31
+ D
2
32
+ 2D
2
33
_
+2C
0
33
_
D
11
D
21
+ D
12
D
22
+ 2D
13
D
23
+D
2
31
+ D
2
32
+ 2D
2
33
_
+ 4C
0
13
_
D
11
D
31
+ D
12
D
32
+ 2D
13
D
33
_
+4C
0
23
_
D
21
D
31
+ D
22
D
32
+ 2D
23
D
33
_
, (A14)
18 J Elasticity (2006) 85: 120
As already said after Eq. (41), U
Kf 1
, U
Kg1
, U
Mf 1
, U
Mg1
have similar forms as those
of U
Kf 1
, U
Kg1
, U
Mf 1
, U
Mg1
, with
D
11
= (K
0
+
0
) K
+
_
(K
0
+
0
)C
+
11
+ 2K
0
C
+
12
+ (K
0

0
)C
+
22
_
+
+
_
(K
0
+
0
)C
+
11
+ 2
0
C
+
12
+ (K
0

0
)C
+
22
_
,
D
22
= (K
0
+
0
) K
+
_
(K
0
+
0
)C
+
22
+ 2K
0
C
+
12
+ (K
0

0
)C
+
11
_
+
+
_
(K
0
+
0
)C
+
22
+ 2
0
C
+
12
+ (K
0

0
)C
+
11
_
,
D
12
= (K
0

0
) K
+
_
(K
0
+
0
)C
+
11
+ 2K
0
C
+
12
+ (K
0

0
)C
+
22
_
+
+
_
(K
0
+
0
)C
+
11
2
0
C
+
12
(K
0

0
)C
+
22
_
,
D
21
= (K
0

0
) K
+
_
(K
0
+
0
)C
+
22
+ 2K
0
C
+
12
+ (K
0

0
)C
+
11
_
+
+
_
(K
0
+
0
)C
+
22
2
0
C
+
12
(K
0

0
)C
+
11
_
,
D
33
=
0
4
0

+
C
+
33
,
D
13
= 2
+
_
(K
0
+
0
)C
+
13
+ (K
0

0
)C
+
23
_
,
D
23
= 2
+
_
(K
0
+
0
)C
+
23
+ (K
0

0
)C
+
13
_
,
D
31
= 2
0
K
+
(C
+
13
+C
+
23
) 2
0

+
(C
+
13
C
+
23
),
D
32
= 2
0
K
+
(C
+
13
+C
+
23
) 2
0

+
(C
+
23
C
+
13
), (A15)
where
C
+
11
=
S
+
22
S
+
33
S
2
23

+
c
, C
+
22
=
S
+
11
S
+
33
S
2
13

+
c
,
C
+
12
=
S
13
S
23
S
+
12
S
+
33

+
c
, C
+
33
=
S
+
11
S
+
22
(S
+
12
)
2
4
+
c
,
C
+
13
=
S
+
12
S
23
S
+
22
S
13
2
+
c
, C
+
23
=
S
+
12
S
13
S
+
11
S
23
2
+
c
,

+
c
= S
+
11
S
+
22
S
+
33
+ 2S
+
12
S
13
S
23
(S
+
12
)
2
S
+
33
S
2
23
S
+
11
S
2
13
S
+
22
, (A16)
K
+
= (C
+
11
+C
+
22
+ 2C
+
12
)
1
,

+
= 2(C
+
11
+C
+
22
2C
+
12
+ 4C
+
33
)
1
, (A17)
J Elasticity (2006) 85: 120 19
S
+
11
=
C
22
C
33
C
2
23

c
+
1
4
0
+
1
4

, S
+
22
=
C
11
C
33
C
2
13

c
+
1
4
0
+
1
4

,
S
+
12
=
C
13
C
23
C
12
C
33

c
+
1
4
0

1
4

, S
+
33
=
C
11
C
22
C
2
12
4
c
+
1
2

,
S
13
=
C
12
C
23
C
22
C
13
2
c
, S
23
=
C
12
C
13
C
11
C
23
2
c
,

c
= C
11
C
22
C
33
+ 2C
12
C
13
C
23
C
33
C
2
12
C
11
C
2
23
C
22
C
2
13
; (A18)
and
C
0
11
=
1

c
_
(K
0
r
0
)
2
(C
11
C
33
C
2
13
+C
22
C
33
C
2
23
+ 2C
13
C
23
2C
12
C
33
) + 4
2
0
(C
22
C
33
C
2
23
)+4
0
(K
0

0
)(C
22
C
33
C
2
23
+C
13
C
23
C
12
C
33
)
_
K
0

0
,
C
0
22
=
1

c
_
(K
0

0
)
2
(C
11
C
33
C
2
13
+C
22
C
33
C
2
23
+ 2C
13
C
23
2C
12
C
33
) + 4
2
0
(C
11
C
33
C
2
13
)+4
0
(K
0

0
)(C
11
C
33
C
2
13
+C
13
C
23
C
12
C
33
)
_
K
0

0
,
C
0
12
=
1

c
_
(K
2
0

2
0
)(C
11
C
33
C
2
13
+C
22
C
33
C
2
23
+ 2C
13
C
23
2C
12
C
33
)
+4
2
0
(C
13
C
23
C
12
C
33
)
_
K
0
+
0
,
C
0
33
=
1

2
0
(C
11
C
22
C
2
12
)
0
,
C
0
13
=
1

c
K
0

0
(C
12
C
23
C
22
C
13
) +
0
(K
0

0
)(C
12
C
13
C
11
C
23
)],
C
0
23
=
1

c
K
0

0
(C
12
C
13
C
11
C
23
) +
0
(K
0

0
)(C
12
C
23
C
22
C
13
)]. (A19)
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