IEEE Transactions on Electrical Insulation Vol. 25 No.

4, August 1990 61 7

A Model for the Simulation of

Relaxation Phenomena in Dielectrics

G. Degli Esposti,
Dept. of Electrical Engineering, University of Pavia

D. Tommasini
Dept. of Electrical Engineering, University of Genova

ABSTRACT
A simulation of the behavior of the complex permittivity in a
polymeric material against the frequency is presented. Starting
from experimental data and taking into account the occurrence
of a distibution function in the relaxation times, an electrical
equivalent circuit for each material can be established. Then
the model is applied to analyze some insulating systems. The
curves are calculated for a stratified insulation and for a single
material subjected to chemical degradation. An experimen-
tal study on ad hoc polypropylene films purposely processed
with different concentration of a particular polar additive is
presented and discussed on the basis of the model. Finally,
several possibilities of applications are considered.

INTRODUCTlON interacting dipoles for which the classical relations of De-

bye and Frohlich [2,3] are assumed. In this first investi-
gation, only the effect of the frequency is considered.
N the study of insulating systems, the analysis of the
I dielectric losses and relaxation phenomena is an inter-
esting instrument to appreciate the status of the material
and the variations on medium composition due to aging
effects [I].

To evaluate the experimental data, a user-friendly com-

puter program of simulation would be very useful. This
work, which is part of a more comprehensive investigation
on aging phenomena in polymeric materials, proposes a Figure 1. Equivalent circuit for polar material
computer model directed toward this aim. This simula-
tion program is especially designed to give information on DESCRIPTION OF THE
the behavior of complex insulations formed by polymeric
materials, starting from the knowledge of experimental MODEL
data concerning each single material composing the ana-
lyzed system.
experimental curves of the real and imaginary
The model is established considering the material as
a continuous medium formed by different kinds of non-
T HE
parts of the complex permittivity vs. frequency gen-
erally show the occurrence of a distribution function in

0018-9307/90/0800-017$1.00 @ 1990 IEEE

618 Esposta and Tommasini: Sim d a t i o n of Relaxation Phenomena in Dielectrics

the relaxation times. To take into account this phenom- 2.30

enon, a distribution function G ( r )can be assumed, with
the normalization condition 2.35 0.012
00

J
0
G ( r ) d r= 1 2.34
0.009

where G ( r ) d rrepresents the fraction of the dipoles with 2.33

+
relaxation times in the range (7, r d r ) . Then the fol- 0.006
lowing expression for the real and imaginary part of E* 2.32
can be derived
0.003
2.31

b 0.000
W (2) 2.30
-3 -1 1 3 5 7
Elr = (E, - &JJwrG(r)dr
1 $-U272 log f- (tlz)
0
Figure 2.
A suitable distribution of relaxation times usually can
be obtained by means of a deconvolution of experimental High viscosity mineral oil. :experimental values
[4]; - : computed values.
data. An appropriate approximation of the above rela-
tions can be obtained considering a finite number of terms
4.0
0.25

3.7 0.20

3.4 0.15
and from these last equations the following equivalent
circuit can be derived where
c, =Em 3.1 0.10
C; = ( E , - E ~ ) G ( T ~ ) A T ;
(4)
R.- 0.05
- ci 2.8

This circuit (Figure 1) represents a polar dielectric ma- 2.5 0.00

-3 -1 1 3 5 7
terial, neglecting the effect of ohmic conductance. With
regard to the choice of the distribution function G ( r ) , log f (112)
many relaxation processes may be described by exact
mathematical distributions, such as the log-Gaussian or Figure 3.
PMMA. a :experimental values [ 9 ] ;- : computed values.
the Poisson's distribution, or by means of the empirical
distributions proposed by different authors [5-81. For our
The occurrence of a log-Gaussian distribution in many
theoretical model, we consider only mathematical distri-
relaxation problems is consistent with the assumption of
butions. Starting from experimental data reported in the
a Gaussian distribution for the activation energy E . In
literature for P M M A [9] and an oil [4] the distribution
function G ( r ) was determined. In both cases, the best fact [2],assuming
fitting to these experimental results was obtained with a T = roexp(E/kT) (6)
log-Gaussian distribution function, which was the first to
be applied to the dielectrics problems by Wagner the variable z becomes
CY
G ( r ) d r= - exp(-a2z2) dt (5) (7)
7r2

where z = ln(r/r") and is normally distributed.

IEEE Transactions on Electrical Insulation Vol. 25 No. 4 , August 1090 619

In Figures 2 and 3 the comparison between the com- n of dipole molecules per unit volume, the distribution
puted values and the experimental data is reported. The function G ( T ) and the values of the static and optical
behavior of a composite material, using a suitable com- permittivity, e.g. n A , G A ( T ) , cool, and n ~ G,B ( T ) ,
bination of different equivalent series or parallel circuits, gag 1 EOOB *

can also be described. Let us consider a continuous me-

0.25
dium formed by N different kind ( j = 1 . . . N ) of dipoles. 1
This material can be simulated with the parallel combi-
nation of N equivalent circuits, with the condition 0.20

E* =Cajc; (8)
j 0.15

where cj is the complex permittivity and aj is a suitable

scale factor depending on the concentration of component 0.10
j. When considering stratified insulation, the system can
be simulated by means of the equivalent series circuits
established for each material. In this case, the condition 0.05

(9)
0.00
where aj is an appropriate scale factor dependi ; on the -3 -1 1 3 7
geometry of the system, must be considered. log f (Hz)
1 .o Figure 5.
E" values for different percentages of B.

The simulation for a different percentage of product B

0.8 in the medium, given by

B=- nL? x 100

0.6
nA +nB (10)

is performed. In Figure 4 the obtained curves of ~ ' ( w )

0.4 for different percentage of B, and in Figure 5 the relevant
curves of &"(U) are plotted. Subsequently the behavior of
a stratified insulating system, formed by two materials C
0.2
and D is considered. The calculation is executed for a uni-
form field, that is a very simple geometry (plane-parallel
electrodes), but often used in measuring cells. The same
0.0
-3 -1 1 3 5 7 calculation can be made for any different voltage distri-
bution subject to an analytical formulation.
log f (Hz)
Figure 4. Assuming as data n, G ( T ) ,cl, E ~ the, equivalent cir-
e' values for different percentages of B. cuit for the two materials is established. Then, putting in
series the equivalent circuits, the variation of E with the
frequency for the whole system is analyzed. In Figure 6
G ENERA L APPLICATION S and 7 the computed results are reported, for different val-
+
ues of the parameter (Y = d z / ( d l dz) where d l and dz
o show the possibilities offered by the proposed model, are the thickness of the considered layers.
T some general examples of applications are described.
First the model can be applied to study the influence on
the complex permittivity of a variation in the composi- EXPERI MENTAL
tion due, for instance, to chemical reactions connected
with aging phenomena. The case referring to a degrada-
tion of a material A in a final product B is considered. HE polymers used in this study are a pure isotactic
Both materials A and B are characterized by the number T polypropylene and polypropylene with two different
620 Esposta and Tommasini: Simulation of Relaxa tion Phenomena in Dielectrics

1 .o o=c- (CH2)6 -C 0
! I
0 0
0.8 I I

0.6

0.4
I I
H H
0.2 Figure 8. Tinuvin 770

RESULTS
0.0
-3 -1 1 3 5 7
HE curves of loss angle as a function of frequency over
log f (Hz) T the range 30 Hs to 100 kHz are given in Figure 9 for
the films. Starting from the experimental data obtained
Figure 6.
Stratified insulation: E' values for different cy.
for pure polypropylene and for the film with 0.25% ad-
ditive, the model was applied to describe the behavior
of polypropylene with 1% additive. The results of the
computation are shown also in Figure 9.

0.20 At the moment, only measurement a t ambient temper-

ature have been performed, and therefore the experimen-
tal data cannot show the whole relaxation phenomenon.
0.15 Nevertheless, the results obtained seem to indicate that
the model is suitable to describe some composite systems
0.10 formed by a pure polymer with an additive.
0.12
0.11 3
E". 10
0.05
0.10

0.09
0.00 0.03
-3 -1 1 3 5 7
0.Q7
log f (Hz) O.OG
0.05
Figure 7.
Stratified insulation: e" values for different a. 0.04

0.03
contents of additive, 0.25% and 1%. The additive is Tin- 0.02
uvin 770, a hindered amine stabilizer (Figure 8). 0.01
0.00

The permittivity and loss have been measured as a I 2 3 4 5

function of frequency at room temperature. A General log f (Hz)
Radio transformer ratio arm type 1615 A capacitance
Figure 9.
bridge was used, in conjunction with a Hewlett Packard
oscillator with a frequency range from 20 Hz to 200 kHz, Loss data vs. frequency for polypropylene films.
and the General Radio detector type 1232 A tunable from
* :pure film, experimental values.
a :film with 0.25% additive, experimental values.
20 Hz to 100 kHz. A three-terminal guarded cell and
@ :film with 1% additive, experimental values.
graphite electrodes has been used. The temperature was - :film with 1%additive, computed values.
21 k 1°C during the period of the tests.
IEEE Transactions on Electrical Insulation Vol. 25 No. 4, August lQQ0
CONCLUSIONS
HE approach utilized in this work, which leads to the
T simulation of a polymeric material by means of an
electrical circuit is useful in studying relaxation phenom-
ena in complex situations. The model can be applied to
investigate the variations of &‘(U) and of &”(U) caused
by modifications due to chemical reactions, the presence
of additives or plasticizers, the degree of crystallinity or
crosslinking. Moreover, it is possible to analyze stratified
insulating systems and the interaction of the specimen
under test with external systems such as the measuring
apparatus.
The available CAD programs allow the study of the be-
havior of the material, not only with alternating voltage,
but also during different electrical transients. Neverthe-
less in some applications several phenomena not yet con-
sidered in the present model can be significant. Work is
in progress to consider the influence of the conductivity
and temperature on some polymer films whose chemical
composition and additives content has been carefully con-
trolled.
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131 I. I. Perepechko, An Introduction to Polymer Physics,
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621
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This manuscript is based on a paper given at the 2nd Interna-
tional Conference on Properties and Applications ofDielectric
Materials, Beijing, China, 12-1 6 September 1988.
Manuscript was received on 28 Feb 1989, in final form 25 Jan
1990.