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Numerical simulation of random composite dielectrics.
II. Simulations including dissipation
S. Stölzle, A. Enders, G. Nimtz
To cite this version:
S. Stölzle, A. Enders, G. Nimtz. Numerical simulation of random composite dielectrics. II. Sim- ulations including dissipation. Journal de Physique I, EDP Sciences, 1992, 2 (9), pp.1765-1777.
�10.1051/jp1:1992243�. �jpa-00246658�
Classification Physics Abstracts
02.60-77.20-77.40
Numerical simulation of random composite dielectrics.
II. Simulations including dissipation
S.
St61zle,
A. Enders and G. NimtzII. Physikalisches Institut der Universitit zu K61n, 5000 K61n 41, Germany
(Received
21 May1992, accepted 29May1992)
Abstract. A simulation model presented earlier for the permittivity of a composite material has now been extended to include the dissipation of energy inside the medium. It is employed to
calculate the complex dielectric function of so-called effective media, I-e- randomly distributed lossy particles in an insulating matrix. A general equation formulated before for lossless media
proves to be valid also for the dissipative mixtures investigated. However, simulations and exper-
imental data show that small deviations from random distribution can induce large deviations in the dielectric function. Experiments are reported that agree with the simulation results.
1. Introduction.
The effective
electromagnetic
parameters ofquasi-homogeneous
mixtures of different materials have beensubject
to alarge
number ofinvestigations
since thebeginning
of this century([1- l8]).
In abinary
mixture forexample,
where a volume fractionf
ofparticles (of permittivity cl
israndomly
distributed in a matrix(of permittivity em),
the effective dielectric function(DF)
T isgenerally
not a linear but acomplicated
sublinear function off,
em and e.There have been many
attempts
for theanalytical development
of a consistenttheory,
whichdescribes the
physical reality
andprovides
a tool for theinterpretation
of measurements on such 'effective media'. But these theories and therespective
formulas fail indescribing experimental
data
jig, 20], although qualitatively they
show a similar sublinear behaviour. Now as computers growbigger
andfaster,
a few authors havedeveloped
computer models for such systems andnumerical simulations of effective media have been carried out,
using
differenttechniques [15- 18].
However, up to now these efforts have not led to aknowledge
thathelps experimentalists
to
interpret
their dataunequivocally.
In [21] we have
presented
a new computer code COSME(Complex
Solution of Maxwell'sEquations),
which wasemployed
in the simulation ofbinary
mixtures. We havecompared
our results to the results calculatedby
several effective medium formulas.Although
thisprocedure
did not even include lossydielectrics,
therespective
formulas failed in most cases. In contrast to them we found a relation betweenf,
e, em and T with a strongsimilarity
toLooyenga's
formula [7], which is valid for
f
< 0.25:1766 JOURNAL DE PHYSIQUE I N°9
p(f)
=
f ~a(f)
+(i fj ea(f) (ij
where
a( Ii
=
(1.60
+0.05)
*f
+(0.265
+0.005)
In this paper we report the continuation of our
investigations,
nowincluding lossy
dielectrics.Apart
fromstudying
the behaviour of thecomplex
effectivepermittivity
in the whole volume fraction range between 0 and 1, we comparedequation (ii
to thecomplex
results andfinally
we carried out
experiments
to prove thevalidity
of the simulation program.2. The
algorithm.
The basis of the simulation is the
following physical
model: a volume of size 20 x 10 x 20mm~
or 20 x 15 x 20 mm~ is surrounded
by ideally conducting walls, forrrdng
acavity
resonator. The solution of Maxwell'sequations
inside this volumeincluding
allboundary
conditions leads toelectromagnetic
resonances characterizedby
certain distributions of the electric andmagnetic
fields
oscillating
with acorresponding
resonancefrequency.
The solution forhomogeneous
materials is
easily
foundanalytically [22].
For the numerical solution for
inhomogeneous fillings
the volume inside the resonator is covered with a 3D cartesian mesh such that every mesh cell containsonly
one kind of material whereas the dielectricproperties
for different mesh cells are uncorrelated. Thus for each cellwe select
randomly
apermittivity
e withprobability f
and a dielectric constant em withprobability
If.
Using
a finite difference method for the fields E and Binterdependent
via Maxwell'sequations
theproblem
is transformed intoa discretized
problem,
whose solution isequivalent
to the solution of the
following eigenvalue equation:
Ae =
qDee
q =
A~
co POw~(2)
Here the matrix A
represents
the discreterotrot-operator,
the vector e the discretized electric field vector, De is adiagonal
matrixcontaining
the differentpermittivities
of all the mesh cells. q is theeigenvalue
to be calculatedcontaining
A = unitlength
of the mesh cells,co, PO "
Permittivity
andpermeability
of vacuum and w= resonance
frequency,
at which thefield distribution e oscillates inside the resonator
(for
details see[21]).
The above
eigenvalue problem
may be solved moreeasily
whenever De is a realmatrix,
because then the
problem
issymmetric
and real. Asreported
in [21] such aproblem,
even if it is of veryhigh
order(here:
>150000),
can be solvedby
aspectral
shift ofeigenvalues
combinedwith inverse iteration
employing
aconjugate gradient (CG)
method for the minimization. For the simulation ofdissipative
mixtures where De iscomplex,
standard CG routines fail asthey
are
only applicable
to Hermitian matrices. So arecently published
CGalgorithm
[23] wasincluded in
COSME,
which worksespecially
well withcomplex-symrnetric
but non-Hermitian minimizationproblems,
hence it is ideal for the solution ofequation (2).
The existence of
complex eigenvalues
q also causes thefrequency
w «@
to becomplex.
Just like the
complex
value of the wave vector k of wavespropagating
inside an infinitesample,
the
complex
value of the oscillationfrequency
w ofstanding
waves insidea resonator may be
used to calculate the
complex
DF of therespective
material. Thecorresponding
relation is~2
0
~ ~2
14
7'
121o 8
70000 140000
li
5
-, ,
~ 4
I
70000 140000
N
Fig-I.
Effective permittivity vs number of nodes in the discretization mesh.e = 50 -120, em
= 1
and f = 0.3.
where wo represents the resonance
frequency
of the empty resonator.For the measurement of w = w' + iw" one would measure the resonance
frequency (w')
and thequality
factorQ,
which isgiven by
w' dividedby
the FWHM(full
width halfmaximum);
w" is then calculated via the
following
relation~,, W' W'
(~j
2Q 2Qofi$
resulting
from the timedependence
of the electric field(and Q
ccvGfi:
E(t)
=Eoe~#e~~"~e~~'~
=
Eoe~%de~~'~
Here
Q
is the measuredquality
factor of the resonatorincluding
a(dissipative)
material andQo,
wo are thequality
factor and resonancefrequency
of the empty resonator. In the ideal case(infinitely conducting walls) Qo
" cc and w"=
w'/(2 Q).
3.
Dissipative
random mixtures with differentfilling
factors.For all the simulations the size of the discretization mesh was chosen 40 x 30 x 40
respectively
40 x 20 x 40
nodes,
so the volume was divided into cells oflength
A= 0.5 mm. This of course
corresponds
to the smallestparticle
size realized in the simulations.For the estimation of discretization errors we carried out several simulations of identical dis- tributions of
particles
oflength
d= 2 mm
varying only
the size of the discretization mesh. Infigure
I theresulting
effectivepermittivities
for meshes of 10 x 6 x10,
20 x 12 x20,
40 x 24 x 40 and 60 x 36 x 60 nodes aredisplayed
vs the number of nodes. In this case e= 50 -120 and
f
= 0.3 werechosen,
the same behaviour was observed for e= 15 I and
f
= 0.4. The
two smaller
grids appeared
to be too coarse toproduce
correct values.Increasing
thegrid length
from 40 to 60obviously
does notchange
the result very muchcompared
to the statis-tical fluctuations, so for standard runs we
always
chose 40 x 30 x 40grids
to save computer time.1768 JOURNAL DE PHYSIQUE I N°9
, >,, i I I I i i i i i ,
, >,, i I I I I I I,, i i , ,
, >, i I, t I I II I, i I I i
, ,
, , t t i i t I ii I I i i t It i
t i i ,
, , , i i i i t I ii I I i t
i, i i i ,
,, i i i i t t I I I I I i Ii t i i t i i i ,
,
I,
, , t t i i I I I it i t t i
, ,
i , i t i t t i I i i i t t i i
i,
, , t i i i i Ii i I i i i i i I I i t,, , ,
, , t t i t t t i t, i i ,
, , t t t t I it I I I I i t t i , t , ,
i i i t I I i t I t t ,, ,,.
, i i i i it i Ii I i I i i, t ,.
, , , , i I i i, t t i i i i I I i I I t i i t ,
, , , ,, i I I I i i I I ii i i I i
, , ,
, , , ,, t t I i i I I I I Ii t t I I t , i > i i i ,
, , i i I I i i i I I I i t i i , , i ,
<, i i i t I I i i t i i1, ,
Fig.2.
Typical electric field distribution inside a resonator filled with an effective medium(cross section).
Fields calculated by COSME.One can
speak
of an effective medium aslong
as thewavelength
inside everyparticle
con-siderably
exceeds thelength
d of theparticle.
If this conditionW>~
> (41is not
fulfilled,
the wave may be scatteredby
theinhomogeneities
and the mixture does not behavequasi-homogeneously
any more. In this context theproblem
of the skin effect also has to beconsidered,
as thecomplete penetration
of the wave inside theparticle
must be ensured.In the worst case in our simulations
,
Al
(e( was stilllarger
than 7 d. The maximumimaginary
part of e was chosen such that theresulting
skindepth
was still 0.75 mm, I. e.larger
than thelength
of eachparticle.
For
illustration, figure
2 shows atypical
field distribution(electric field)
at resonance insidean effective medium as calculated
by
the COSME program. Thesine-shape
of the fundamental mode of therectangular
resonator isclearly visible, inspite
of local field deformationsas a cause
of the
inhomogeneities (em
= I,e = 102i, f
=0.I,
d= 0.5
mrn).
Mixtures of
particles
with e= 50
-120,
em = I and d= 0.5 mm were
investigated
over the whole range of volume fractions between 0 and I.Looking
at the matrixequation (2)
it is easy to see that anyarbitrary
mixture of two materials may be transformed into aparticle-vacuum
mixture
by normalizing
all thepermittivities
to the DF of the host material.Figure
3 shows the behaviour of the effective DF of the mixtures vs volume fraction. For smallfilling
factors(f
<0.25)
thetypical
sublinear behaviour ofT(f)
isobserved,
belowf
= 0.12 even very close to the line which marksLooyenga's
formula. Forf
>0.25, however, T( ii
shows aperfectly
linearbehaviour,
which reminds of asimple parallel-circuit
relation.In
figure
4 this behaviour becomes even more obvious: the effective loss tangentf'If
= tanchanges dramatically
in the volume fraction range belowf
= 0.25
approximating
theparticles'
loss tangent
e"le'= 0A)
veryrapidly.
Athigher
volume fractions it almost does notchange
any more.
So the loss tangent and the absolute value of the DF of such an effective medium may be influenced
independently
in the different ranges offilling
factors. Belowf
=0.25, ?( ii
is sublinear in both the real and the
imaginary
part, henceiii changes
veryslowly
with the volumefraction,
in contrast to the losstangent.
In thehigh
volume fraction range the two parameters act vice versa: almost nochange
in tan &, linear increase ofiii by adding
a fewparticles
to the mixture.60
E'
50
o
40
.
o
30
20 °
o
IO °
o
-lo
OO O-1 02 03 04 05 06 07 O-B 09 1.O
f
a)
25
E 20
o
5 *
o lo
o
5
o
o
-5
O f b)
Fig.3.
Dielectric function of the heterogeneous mixtures vs. the volume fraction (em= 1,e
=
50 -120, d
= 0.5
mm).
Results of the numerical simulations(.)
compared to Looyenga's formula [7](-). a)
Real part of Ib)
Imaginary part of I.In
figure
5 the simulation data and the results calculated fromequation (I)
arecompared.
In the range where
(I)
is claimed to be valid forf
< 0.25 the agreement is excellent. For furtherproof
we carried out simulations withparticles
of evenhigher permittivity (e
= 90145)
and found the same agreement. Soobviously equation (I)
is also valid fordissipative
randommixtures with low volume fractions.
1770 JOURNAL DE PIIYSIQUE I N°9
o.5
tg 6
O.4
~ . .
O.3 O.2
O.
o-o
-o.i
O-O
f
20
6
15
1o
5
-O
f a)
'>
~
-2
-4
-6
-8
O-O
f b)
g.5.
-
equation (-) vs. volume fraction. em, e, d as in figure 3.
calculation
of the
mean polarization, can only up to the sth ntil the limitsof theomputer are
reached
[15].So the interactions between neighboring
particles
roaches and therefore they
can only
bevalid
for very smallfilling
non-random samples.
The
above
sample being higher when the
sth
multipole was included,than
in pure dipole1772 JOURNAL DE PHYSIQUE I N°9
~)
~@~ ~4/
)
a)
C)
Fig.6.
Non-random geometries simulated by COSME.Obviously higher multipole
interactions havea strong influence on the DF of a mixture.
In the simulations
presented
here the interactions between all theparticles
inside thesample
volume are
implicitly considered,
because here Maxwell'sequations
aredirectly
solved in fullgenerality.
This results in the decisive deviations from former well-known effective mediumrelations.
4. Non-random
geometries.
The formation of connected
paths
caneasily
be enhanced orsuppressed
in the computer model.For a
qualitative
evaluation of the influence of geometry on theresulting
effective DF wegenerated
thefollowing
material distributions for five different simulations:I. Several 2D-networks on a stack but
separated by
matrix material. The networks lieperpendicular
to the electric field inside the resonator(Fig. 6a), f
= 0.107.2. 2D-networks as in I. interconnected
by
columns in the directionparallel
to the electric field(Fig. 6b), f
= 0.15.3. 2D-networks and columns as shown in
figure 6c, f
= 0.164.4. As
2.,
withf=0.23.
5. As
3.,
withf=0.28 (due
to closerpacked 2D-networks).
Figure
7 shows the deviation of theresulting
DF'S of such structures from those of random mixtures. From tableI,
which contains thecorresponding
relative deviations forgeometries
1.
5.,
it is obvious howstrongly
the innergeometry
of theinhomogeneities
influences the effectiveDF,
an effect which has also been foundexperimentally [24]. Especially
ahigher proportion
ofpaths parallel
to the electric field increases theresulting
effectivepermittivity
whereas r results to have a lower value when the
inhomogeneities
are locatedperpendicular
to the electric field.20
lo z 4 5
. i
O f
O-O O-i O.2 O.3 O.4
a)
EI,
o
3
~ O
~
_5 .
4
-lo f
0.O O.2 O.4
b)
Fig.7.
Results from the simulations of five different non-random geometries(.) (geometries
1.5., see
text)
compared to the respectiv of random geometries(-),
both displayed vs. the volume fraction.Table I. Relative deviation of the values air calculated for non-random
geometries
from those for mixtures withrandomly
distribu tedparticles (emd ).
Geometries 1. 5. areexplained
in the text. The
corresponding
absolute values are shown infigure
7. In this table 100 ~corresponds
to the effectivepermit tivity
for random mixtures(for
therespective
volume frac-tion).
No.
f
f T[~d deviation T"f[d
deviationT' from T[~d T" from
f[d
1 0.105 1.3 3.34 -61 iii 0.025 0.76 96 iii
2 0.15 8.9 5.734 + 55 iii 3.84 1.82 + l10 iii
3 0.164 7.6 6.72 + 13 iii 3.19 2.29 + 39 iii
4 0.231 14.5 13.087 + 10 iii 6.74 5.52 + 22 iii
5 0.237 II-1 13.785 19.5 iii 4.86 5.89 17.5 iii
1774 JOURNAL DE PHYSIQUE I N°9
5.
Experiments.
For the verification of the computer simulations several
inhomogeneous samples
wereprepared
and a real resonator was built for the purpose of a direct
comparison
betweenphysical
mea-surements and results obtained from the numerical calculations.
The first
sample
was a block(16
x 7 x16mm~)
ofA1203 (96ili purity),
which wasplaced
in the center(setting A)
and then into the corner(setting B)
of the resonator. Thesegeometries
areeasily reproduced by
the discretization mesh of the computer program and thus serve as verygood
test structures for the simulation results. As a secondsample
a mixture of epoxy resin(em
= 2.98-10.06)
and 8ili small cubes(I
x I x Imm~)
of aTi02
ceramic material(e
= 80I)
was
prepared
to fitexactly
into the resonator andaccording
to a random distributiongenerated by
the computer(setting C).
As a consequence of technicalproblems
whileplacing
thecubes,
the desired random distribution could not be realized. So the distribution for the simulation had to be modified to represent the inner
topology
of thesample correctly.
Inside the
rectangular
resonator(20
x 10 x 20mm~)
constructed for this purpose two currentloops
for H-fieldcoupling
were fixedopposite
to each other in the side walls.They
were realizedby shortening
the end of two coaxial linesby
thin wires in theplane
of the inner resonatorwall. Two PC-7
(7
mmprecision connector)
bulkhead connectors were mounteddirectly
on the resonator sidewalls,
their inner conductorgoing through
holes in the resonator walls thusrealizing
the coaxial lines.Thus the transmission
properties through
the resonator could be determinedusing
a HP 85108 networkanalyzer.
The networkanalyzer
was calibrated with ahigh quality
LRL(two
7 mm air line and one reflect calibration
standards)
calibrationtechnique
in PC-7technique [27]. Consequently
allsystematic
errors up to the resonator PC-7 connector interfaces wereremoved
yielding highest possible
measurement accuracy.First a broad
frequency
range was chosen toidentify
the transmission resonances, then the calibration wasperformed
infrequency
segments around the resonances togive
sufficientfrequency
resolution(down
tofrequency
steps of 200 kHz between each measurementpoint)
for the determination of the resonance
frequencies
and theQ-values. (-3
dBpoints
of theresonance
curves).
The
coupling strength
of the currentloops
was variedby altering
the geometry of the short circuit wires thusyielding
transmissionamplitudes
between -60 and -25 dB at the resonancefrequency
of the empty resonator. In this whole range the resonancefrequency
did notchange by
more than10~~.
Also theQ~value
of the empty resonator did notchange
within measure-ment resolution. This proves that the disturbance of the
coupling
structures on the resonatorproperties
isnegligible.
The resonator was
successively
loaded with thegeometrical settings A,
B and C and for each of them the lowest resonancefrequency
was determined.In table II the results of
experiments
and simulations of the threesettings
aredirectly compared.
Theimaginary
part ofw is related to thequality
factorQ
viaequation (3). However,
in
settings
A and B w" was below the resolution limits and has therefore been omitted.Figure
8 shows the resonance curves of the empty resonator and of the resonator loaded withsample
C.The
good agreement
of cases A and B betweenexperiment
and simulations proves thevalidity
and correctness of the COSME-results.However,
for both these cases there is no effective DF because of the violation of relation(4).
In case C the construction of a random distribution failed as it wasimpossible
tobring
the cubes into closeenough
contact: in the realsample neighboring
cubes were stillseparated by
a resinlayer.
Instead of v= 5.354 +10.052 GHz a
really
random effective medium with the samefilling
factor would have had its resonance at v = 4.921 +10.047 GHz.S [dB]
resonator
5
dB(
S21
a)
S12
ma'
10[Ge99s9932
adz v
[GHZj
S
sanipie
cs
b)
S12START 5.ZSOOaOOOO G4z
~~
WCP 5.4100@OOOO G4z l' Z
Fig.8.
Measured resonance curves: S21-parameter(I.e.
transmission amplitudeS)
vs. frequency:a)
empty resonatorb)
resonator filled with ceramic-resin mixtureSo the inner
topology
of aheterogeneous
mixture is a veryimportant
parameter for theresulting
effective material parameters, as has beenpointed
out before[14, 9].
Not evenequation (I),
which hasproved
to be correct forcompletely
randommixtures,
can beemployed
on
samples
with unknown inner geometry.1776 JOURNAL DE PHYSIQUE I N°9
Table II. Results of the measurements on different resonator
fillings (vexp, Qexp)
in com-parison
to thecomplex
resonancefrequencies (vsim)
calculatedby
the simulation program. Insettings
A and B theimaginary
parts of e and w were below the limit of resolution and have therefore been omit ted. Theexperimental
data ofset tin g Ccorrespond
to acomplex frequency
of v = 5.354 + 10.052 GHz.Setting
e Ivexp[GHz] Qexp vsim[GHz]
empty I 1. 10.595 2682 10.596
A 8.9 0.448 5.43 1357 5.448
B 8.9 0.448 5.047 1264 5.050
C 80 I 0.08 5.354 50.509 5.311 + 10.053
epoxy 2.98 10.06 1.0 6.2275 47.904
resin
6, Conclusion.
A new computer code has been
presented
which allows the simulation ofinhomogeneous lossy
materials. In this paper it wasemployed
on onespecies
of effective media:randomly
distributeddissipative particles
in an air-like matrix.For the effective
permittivity
a sublineardependence
on thefilling
factorf
was found for the rangef
< 0.25. Theempirical exponential
formula(I),
which had beendeveloped
earlier for losslesscomposite materials,
hasproved
to be valid also for random mixtures ofdissipative
dielectrics. For
f
< 0.25 it fits all the data very well.Mixtures with a
higher
volume fraction showed a linear increase of T withf.
This behaviour may beexplained by
thegradual
formation ofinterconnecting paths by
theparticles.
Itimplies
the losstangent reaching
itslargest
valuealready
at aboutf
=0.25,
whereas the absolute value of T increases much slowlier.The
COSME-program
was testedexperimentally
with measurements carried out on three different resonatorfillings,
which were easy to model on the computer. Two of them were realizedby
amacroscopic A1203-cube
in differentpositions
and the thirdsample
was a mixture of small cubes of ceramic material and a matrix of epoxy resin. Theexperimental
data theresonance
frequency
andquality
factor of a resonator loaded with therespective sample
were in excellent
agreement
with the results of the computer simulations.The measurement on the ceramic-resin-mixture revealed the great
dependence
of the effectivepermittivity
on the inner geometry of anysample. Although
it was a disorderedmixture,
the distribution of theparticles
was notcompletely
random but theparticles
were moreseparated
from each other. For this reason thesample
did not show the behaviourpredicted by
theexponential
formula.In conclusion it must be stated that the
geometrical
correlations have to be taken into ac- count, wheneverexperimental
data are to beinterpreted using
effective medium theories. Thisimplies
thenecessity
of numerical simulations in thegeneral
case. For the case of acompletely
random distribution ofparticles
in amatrix, however,
we havepresented
mathematical rela- tions between the relevant parameters which describe the behaviour of such effective media in the whole range of volume fractions.Acknowledgements.
R. Pelster is
gratefully acknowledged
for the additional lowfrequency
measurements on all the materials used in theexperimental
part. Theinvestigations
weresupported by
the DeutscheForschungsgemeinschaft (SFB 341), by
the Bundesministerium firForschung
und Technolc-gie/Bonn
andby
about 120 hours of NEC SX-3cpu-time
ofCologne University's
computer center.References
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