IEEE Transactions on Dielectrics and Electrical I n s u l a t i o n Vol. 9 No.

5, O c t o b e r 2 0 0 2 697

Aging and Polarization Phenomena in PE

under High Electric Fields ,
Jean-Pierre Crine
Technology.consultant
Brassard, Qc, Canada

ABSTRACT
The influence of high electrical dc fields (>20 kVlmm) on aging, polarization and on the mor-
phology of polyethylene (PE),isdiscussed. Infrared and positron annihilation spectroscopy
measurements as well as capacitance measurements tend to suggest that the polymermorphol-
ogy is modified by high fields. We show that the accelerated electrical aging characteristics of
PE are linked directly to the morphology changes induced by the field. Below a so-called crit-
ical field, the activation volume of the aging process is dependent on the field-induced strain.
Above the critical field, the amorphous phase is deformed significantly, and weak van der
Waals bonds are broken, leading to another, faster, aging regime. There is an excellent agree-
ment between the proposed model and experimental data obtained with various PE samples.
The possible relation between the submicrocavity formation proposed in our aging model and
various polarization measurements is discussed. It is our contention that strong charge injec-
tion occurs only after submicrocavity formation, Le. after weak bond breakage. As is well
known, the polarization currents obtained under high fields are controlled by space charges. It
seems that the wave packets and the negative resistance observed at >lo0 kV/mm in PE are as-
sociated with a steady state in field-induced defect formation. This suggests that space charges
are related to the formation of submicrocavitiesand, therefore, are a consequence, not a cause,
of high field aging.

1 INTRODUCTION are explored. Polarization by space charges is a phenomenon typical Of

dielectrics occurring above a given high field. It is our contention that
space charges are a consequence of aging, ;.e. charges are injected only
Electrical aging of polymers is still poorly known and often it has
when physical defects [such as submicrocavities) have been formed
been assumed that there is a power law relation between aging time
t and breakdown field F , such as t = CF-", where C and n are by the field-induced strain. The best experimental evidence support-
ing this contention is that indeed there is no charge injection in PE at
constants, characteristicof the dielectric. Acceleratedaging results plot-
fields 4 0 kV/mm, i.e. below the onset of submicrocavity formation.
ted on log field us. log time graphs are expected to fit a straight line.
We have shown elsewhere [l]that, for ac fields, life extrapolations for
crosslinked polyethylene (XLPE) cables made from such graphs are, at
The
-
other evidence is less direct but has many practical implications.
Above 80 to 100 kV/mm at 22T, wave packets have been observed
best dubious, since the linear relation between log field and log time in PE during space charge measurements 161. Interestingly enough,
does not hold. In fact, results fit much better to a semi-log plot be- these packets of charges oscillating through the dielectric occur at fields
tween F and logt, in agreement with our previous aging model ll] where van Roggen [71 and Fallou et ai. [e], long ago, observed a regime
above the same field where the current decreases with increasing field
or with the Dissado-Montanari 131 or the Lewis [4,5] models. In this
paper, we present an improved dc-field aging model partially based on (see Figure 1).We intend to demonstrate that all these phenomena are
associated with the creation of submicrocavities, the precursor step for
Lewis et al. suggestion [4,5] that the field-induced strain deforms the
insulation. The predictions of our new model describe very well actual aging and space charge formation.
accelerated aging data for PE aged under dc fields in air at 22°C. The 2 T H E AGING MODEL FOR DC
model relies on the activation energy and volume parameters, which FIELDS
depend on morphological and structural properties of the dielectric. We
also have investigated some of the influence of high dc fields on these
' 2.1 BASIC CONCEPTS
properties in order to relate aging and polymer morphology The re- The basis of our model based on the rate theory was described in
lations between aging and polarization, especially space charges, also detail elsewhere [I, 21 and it assumed that electricalaging is a thermally

1070-9878/2/ $3.00 0 2002 IEEE

 698 Crine: Aging and Polarization Phenomena in PE

nros the long t i e (low field) regime cannot be well described assuming a
constant value for the activation volume. We have therefore explored
the possibility that AV could vary with F at low field. Note that we
assumed for the sake of simplicity that the field was constant within the
insulation. This could be correct, as long as the sample is not too thick.
2.2 INFLUENCE OF FIELD ON THE

i$ ,
ACTIVATION VOLUME
We propose that aging occurs above a given critical field F, with a
typical value in the 10 to 20 kV/mm range for PE. Its precise value can
be estimated by supposing that above F, submicrocavities are formed.
lw 200 1w cw Lewis et 01. [4,5] have shown that the mechanical stresses induced by
Field (LVimm)
electric field can lead to weak bonds breaking and, thus, to microcrack
Figure 1. Current density of PE samples as a function of dc field at formation. Obviously, the low strains generated by fields in the IO to
22°C by van Roggen [7] and Fallou et RI. [8]showing a 'negative resis- 50 kV/mm range cannot break backbone bonds whose strength is in
tance' &me >SO to 100 kV/mm. The results obtained at lower fields the 1 to 3 eV range. The weaker bonds in a polymer are the van der
by Montanari et nl. [I31on unaged and aged samples are in agreement Waals bonds with strength as low as 0.1 eV (1.6x10~-'@ J). Eyring 191
with [7,8]. and Wunderlich [IO]have shown long ago that a precursor step ~ ~ o u l d
be what Eyring called 'hole' formation, which is equivalent to the 'sub-
activated process. Thus, going from the original (unaged) state to the microcavities' detected by Zhtukov 1111during the mechanical aging of
final (aged) state requires a jump in energy over an activated energy many polymers. In all cases, weak molecular bonds are stretched under
barrier AG = A H - T A S , where A H and A S are the activation the application of a stress up to a point where they are broken, and free
enthalpy and entropy, respectively, and T is the absolute temperature. radicals are formed at the submicrocavity sites, initiating irreversible
We have recently modified the model [2] to include a square-field de- aging of the material. According to Eyring 191 the energy E,, required

-
pendence for AG, in agreement with Lewis et al. [4,5] who proposed to generate a 'hole' is related to the energy of cohesion of the polymer
that the mechanical stress induced by the field may break weak bonds E, 1.6 to 1 . 8 ~ 1 0 - ~J "for PE, to the 'hole' volume
when its value is larger than the Griffith criterion for crack formation. molar volume 1' by
and to its

The term reducing AG is the product of the pressure P induced by the

field F (Maxwell stress) and the activation volume AV (the strained (4)
volume) associated with the process, i.e. Wunderlich [lo] has estimated a hole energy 0f5x10-'~ J for f'E at
P A V = +,EF~AV (1) 237 K, its glass transition temperature T.:
where E,, and E are the permittivity of free space and the static rela- with a slope of 1 . 3 8 ~ 1 0 - * ~ (-T T -
Since E, decreases with T
~ ) ,this means & 4x1WZ1J
tive dielectric permittivity of the polymer, respectively The t i e to go at 295 K. Thus, when the work done by the field (Equation (1))will be
over the barrier being the inverse of the rate, this means that the timet equal to 4xlO-*l J (at room temperature), holes or submicrocavities
needed to reach the aged state is given by (defectsin a general sense) will be formed, because weak bonds would
have been broken or displaced. Assuming that the iictivation volume
for the forward and backward processes of aging have the same value,
where h and-k are the Planck and Boltzmann constants, respectively. this means that the deformation on each site of the energy barrier has
Equation 2 predicts that at zero field, t = -since csch(0) = -=. Thus, only to be equal to half the above work value, in order to induce an en-
there will be some sort of 'tail' at low fields, where t will slowly tend ergy reduction equal to Eh. Substituting P A V by E& into Equation (1
toward =-. At high fields, Equation (2 )reduces to )gives the critical field
AG - ; E , ~ ~ ~ ~ 2
t = -exp
2kT 1 kT 1
which predicts a h e a r relation between F2 and log t. In Figure 2 we
(3)
Below Fc,the activation volume is decreasing with decreasing lield.
have plotted various dry aging results of XLPE cables as F2 us. log t, Since AV is the strained volume, it must be associated with the lield-
and both the linear relation at high fields (Equation (3) and the tail induced strain s given by
(Equation (2)) indeed are observed. Thus, the main features predicted €F'
by the model correspond to actual data. From the slope of the hgh-field s=- (6)
2B
regime and from the intercept in the F 2 us. log t plots it is then possible where B is the bulk modulus of the polymer. Below Fc, no (or very
to determine AV and AG. From a practical point of view, this means little) submicrocavities (or defects) should be created and therefore, the
that the AV and AG values of a given insulation deduced from short- activation volume AVF for F < Fc, is directly varying with 5, i.e.
term accelerated aging tests (high field) and Equation (2 ) can be used with F 2 . At Fc, we may assume that A V F 2 = AVFF2. Thus,
to calculate the long-term (low field) life using Equation (3). However, giving a first order approximation for AVF as
IEEE Transactions on Dielectrics and Electrical Insulation Vol. 9 No. 5, October 2002 699

0 3s
(7)
We have shown elsewhere the good agreement at low fields between
calculations (Equation (7)) and experiments for XLPE cables aged under
ac fields [12]. There is very little data published at low dc fields and
we were unable to verify the validity of Equation (7) under this sort of
electrical stress. However, high dc field results, obtained by Montanari
et ai. (131, Kitani [I41 and Chen and Davies [IS] can be described very
well by the model, as shown in Figure 2. The three different set of re-
sults have nearly identical AG values (from 2.01 to 2 . 0 6 ~ 1 0 - ' J)
~ but e
very different A V values, as can be seen from the slopes in Figure 2. 0 28
The Chen and Davies results must be treated with some care since only 0 2 I B 8 10 12 I4 16

Field (UVImm)
their 100 kV/mm result is an actual data point, the other values being
calculations made as per 1161. Figure 3. Positron annihilation measurements 1161 showing the re-
duction of the amorphous phase fraction of PE as the dc field increases.

In an attempt to get more definitive evidence for the submicrocavity

formation, Meunier and Crine have reported some years ago infrared
(IR) spectroscopy measurements performed on PE subjected to high dc
fields (18). They obsewed that at 40 kV/mm, the intensity of the CHz
rocking doublet (the so-called crystallinity band) at 620 to 630 cm-' had
increased by 15 and 9%, respectively When the field was applied for
long periods of time (>20 h), they also observed that the discharge cur-
rent could suddenly increase by a factor of 2 or 3x, for a duration of l
or 2 h, and then gets back to its former value. This current variation
TIM ( I ) was always associated with an increase in absorption of the IR doublet
at 620 to 630 cm-I. Although the authors were not able at the time to
Figure 2. dc Aging results from 11315Jplotted as F 2 us. log t explain this behavior, it seems now that it was somehow related with
the molecular rearrangement observed by positron annihilation spec-
Note the excellent agreement between experiment and theory (Equa- troscopy 1161. It confirms that the local morphology of PE is affected by
tion (3)). At low fields, we have assumed that A V varies with F fields 2 15 to 20 kV/mm.
according to Equation (7).
2.4 INFLUENCE OF SAMPLE SIZE
2.3 INFLUENCE OF MORPHOLOGY
ON ACTIVATION VOLUME The different AV values deduced from the in F 2 us. log t plots
(Figure 2) may be explained by differenimorphologies, as discussed
Another feature of the proposed model is that below F, the polymer above, but there could be another parameter involved. It is well known
is deformed more or less elastically by the applied field. rE is com- that the electrical breakdown value of dielectrics may increase with de-
posed of a crystalline and an amorphous phase and the latter is much creasing sample thickness 1191. Thus, the insulation thickness may play
more easily deformed by stresses (at least, under low strains). This has
some role but it is not the only geometric parameter. In Figure 4, we
been demonstrated by various morphological measurements, such as have plotted the A V values deduced from the slopes in Figure 2 as
positron annihilation spectroscopy that measures very small changes
a function of the volume of the tested samples. There is a rough rela-
in the free volume (or the development of tiny defects) in polymers. It tion between these A V values and the sample volume. .Recently, Kim

-
was shown by Brandt and Wilkenfeld [16], Figure 3, that the amorphous
phase fraction decreases with field and levels off at 15 to 25 kV/mm,
i.e. for a very moderate strain. When the amorphous phase has been
and Shi [20] have shown that the thickness dependence of the dielectric
strength of TeflonrM(PTFE) is due to a variation of the Young modulus
with samples thickness. Since the Young and bulk moduli are related,
deformed completely, bond breaking will occur because the crystalline
this possibly could explain the thickness (or volume) effect"Kim and
phase is much tougher. Further evidence for the deformation of PE by Shi associated the decrease of the Young modulus with thickness in-
an electric field is provided by the change of capacitance C (ie.change
crease to a change in morphology, especially an increase of the lamellar
of sample thickness). A C measured by Sakamoto and Yahagi 1171, size for thicker samples.
which varies with F 2 . In addition, an hysteresis effect was observed
when fields 2 20 kV/nim where applied, i.e. A C never gets back to However, there is no equivalent data for PE and much more work is
zero when the field is lowered to zero after reaching these high fields. needed to determine the exact cause of the thichess/volume effect on
This implies that permanent deformation of the polymer has occurred aging and on breakdown strength of PE.
under the action of the high field. We may conclude that the proposed model describes very r\rell all
700 Crine: Aging and Polarization Phenomena in J'E

Schottky laws, stating that

- J = Joexp 1- '1.
L
E - aFT
kT
1
(9)

where E is the energy of a barrier, and a is given by

,c
1e.a
.
3-7

S"e8rBd VOl" (In')

2e.7
Figure 4. Activation volume (from the slopes in Figure 2) as a funr
tion of the sample volume.
existing PE aging data obtained in air at 22T, although some improve-
ments are needed to describebetter the morphology and volume effects.
3 POLARIZATION UNDER HIGH
FIELDS
Space charge is one of the main phenomenon observed when a di-
electric is polarized by a high field. It is customary to associate the cur-
rent density J in the space charge limited regime with the well known
Child law
J - 9 EoEpuz
(8)
8 L3
where p is the mobility of the space charge, U the applied voltage
and L the sample thickness. Although this oversimplifying law relies
on several disputable assumptions, it has been used extensively (see
(7.1) for a recent case). We intend to show that it is a very poor tool
to determine the presence of space charge or to evaluate the charge
mobility. Plotting l o g J us. 10g(Ii2/L3)should give a slope of 1,
which obviously is not the case in Figure 5. Thus, evidence for space
charge should not be drawn from Equation (8).
L.7
A straight h e in a log J us. F plot may indicate that injection has
occurred. When the results shown in Figure 5 are plotted in accordance
to Equation (9) in Figure 6, there are indeed straight lines. However,
there is a major problem: the slope should be proportional to the per-
mittivity (Equation (10) and the calculated values assuming a Poole-
Frenkel process, give (Equation (loa)) a permittivity 4, which is phys-
ical nonsense. The calculated permittivity assuming a Schottky process
would be half of these values (Equation (10 )b), which is even worse.
There were several attempts in the past to 'improve' the value of E 1241,
but they all forgot to take into account the basic fact that in his origi-
nal paper Frenkel 1251 clearly stated that the square root parameter in
Equation (9) was not the field but the voltage, because he felt that injec-
tion was a surface effect, dependent on voltage, as in partial discharges,
and not a volume effect (which is more likely to be dependent 011 the
field). Experimental evidence supports the Frenkel assumptions, and
Equation (9) is of no use in determining if space charges are present or
not. In recent years, it has become customary to measure space charge
concentration using sophisticated and expensive setups, such as pulsed
electroacoustic 16,261, pressure wave [27,28] or thermal pulse 1291 tech-
niques. An approximate space charge field can be estimated hom the
experimentally measured current, using complex equations [27], whose
basic assumptions sometimes can be disputed. It is our contention that
the charge concentration in a dielectric can be estimated by a simpler,
faster and less expensive procedure as long as it is assumed that each
submicrocavityformed above F, can accommodate one charge.

I
arc 4w 6.w ax,* todo'
10'. 10'4 10.' IO" IO'D ?e
Square Ron of Field (Whnm)'"
VInl IVInl~l
Figure 5. Current density as a function of U21L3 (Equation (8)). Figure 6. log J us. fi,according to Equation (9) for the results
The expected slope of 1 is not respected for three different measure- shown in Figure 5 (22-231
ments ([U]for the unaged and aged samples, and [231).
Below Fc, there are few (if any) submicrocavitiesgenerated by the
If there is space charge, there must have been strong injection. Other field, but defects are already present, which means that the concentra-
models used to validate this assumption are the Poole-Frenkel and the tion N of 'polaiizable defects' is independent of F . For the sake of
IEEE Transactions on Dielectrics and Electrical Insulation VOl. 9 No. 5,OctoberZOOZ 701

simp1icity;we assume that it is constant and its value is then equal to with the measured values in Figure 9. The agreement is excellent in-
the N value at F,. This value may be empirically determined from the dicating that it is possible to estimate the polarization properties of PE
charge measurements performed by Montanari et d. (22) on the same from the aging results (and vice versa), provided we take into account
samples used for the current measuements shown in Figures 5 and 6. the capacitance and volume of the sample. It should be stressed that we
-
The low-field measurements gave a charge of 0.2 to 0.25 Cnr3, which did not need any space-charge field to attain these results, and we only
seems fairly typical of the residual charges always detected in PE, what- assumed that the density of injected charges was equal to thenumber of
ever the measurement technique [26-291. If we compare the measured free radicals (broken bonds) associated with submicrocavity formation.
charge to the maximum static charge.Q,,,
15kV/mm, the ratio of the measured Q over Q, is in the 2.5xlO-.'
-
= CU, we see that at 10 to This supports our contention that space charges are a consequence of
aging (they appear after bond breaking), and not a cause.
range (Figure 7). We have assumed that the concentration of defects per
10,
unit volume N , present at F, in PE at 22°C is then
N, - 2.5~10-'-
V3
cu
(11)
where V, is the stressed volume, C the sample capacitance, and U the
applied voltage.
008 ,

. . 0

.
0

0 Figure 8. lime evolution of charge measured after 2 h in PE with

various techiuqucs by Suh 1261, Chen [28] and Abou Dakka.1291.

L----
J 0
0.m
. 10 100

Field (kVlolm)

Figure 7. Ratio of measuredover maximum static charge for the w-

aged and aged samples of [22]. The minimum value occurs at the
critical field.

It is quite obvious that the high field results shown in Figures 5 and 6
are somehow associated with space charges, and we intend to show that
they are associated with submicrocavity formation. Above Fc, submi-
crocavities are formed and their concentration increases exponentially
with the square ofthe field and with time t according to J
101 ' (0' 1Y
Field IkVlmm)

Figure 9. Comparison of the charge measured (symbols)by 1221 and

where T is the time to breakdown in agmg as given by Equation (3),
calculated (lines) with Equation (13) in waged and aged PE samples
AV is the activation volume determined in aging tests, and Nc is given as a function of field.
by Equation (11). Figure 8 shows that our assumption of linear rela-
tion between log N and t seems correct for a wide variety of results Assuming that our approach also could be applied to other aging
obtained with different techniques [26,28-291. At short time (1.e. in the results, we have calculated the radicals (submicrocavities) concentra-
hour range), we may assume that the exp(-t/T) term will be % 1, tion using Equation (13), i.e. considering the charge density equal to
and as a first auuroximation. N is then the submicrocavity concentration. Figure 10 shows the results of these
calculations based on the AV, C a n d V , values (13-151. Note that Ki-
tani ef 01. (141 did not report the size of their electrodes and thus we
We have calculated N for the imaged and aged samples of (221 us- map have assumed wrong values for C and V,. This may explain the
ing Equation (12) for N,and assuming that the F, value corresponded relatively large residual charges at fields below F,. For the two other
to the limit of the Ohmic regime in the J us. F plots. The activa- cases, the low charge concentration is between 0.25 and 0.5 Cm3, which
tion volume was then calculated from Equation (5)and substituted into agrees well with experimental data. Obviously, the very high concentra-
Equation (13) to give N. The results shown as charge Q are compared tions at high fields, shown in Figure 10, are unrealistic since the current
 702 Cnne: Aging and Polarization Phenomena in PE

levels off (see Figure 1) in the 100 kV/mm range. In addition, maxi-
mum charge concentration near breakdown are in the 200 to 400 Cni3
range 1301, which means that at very high fields Equation (13) should
be modified. Our assumption is that the current saturation shown in
Figure 1 occurs when the energy spent by the field is equal to the c o h e z
sion energy E, of the polymer ( 1 . 5 ~ 1 0 -J ~for~ PE at 22T),i.e. for a
saturation field F, given by
\\ ./" z-
,/'

I - 1

The expected saturation above Fsfor the samples used by [13-15]
is represented on Figure 10 by dashed lines. This has to be confirmed
by more experimental work. We have applied Equation (14) to Fallou's
results [SI by assuming that a AV value of Z X ~ O -m3 ~ could
~ be de-
duced from Figure 4 and the experimental [8] V' value of Z X ~ O -m3~
The calculated saturation field is then 87 kV/mm, which is very close
-
to the experimental value of 90 kV/mm (Figure 1).
0 100 zoo 300 Iw
>I m am ua
FlWid ,*"A"
Figure 11. Positronium yield [31]and current density [8] in PE as a
function of electric field.
temperature although the influence of sample size on the activation
volume is still unclear.
The detection of submicrocavities under various fields and after var-
ious times would be extremely helpful to validate the fundamental as-
pects of the model.
The influence of morphology on XLPE aging and its evolution with
time, field and temperature requires much more work.
There is no need to calculate and use a so-called space charge field;
the applied field combined with our model gives an excellent agreement
to the existing experimental data.
Polarization seems to be related to the same physical processes than
those describing aging and at fields above the critical field the concen-
tration of charges appears to be directly related to the concentration of

F8eId (kVlmm)
submicrocavities.
Polarization and aging are sensitive to the sample size via the re-
Figure 10. Concentrationof radicals (or submicrocavities or charges)
lation between the activation energy and the sample size. This may
calculated as a function of field for samples used in [1?-15]. The
dashed lines represent the estimated saturation concentration value possibly explain the thickness effect on breakdown strength.
for each case. Our model predicts that the wave packets and current saturation
observed at very high fields occur when the energy spent by the field is
The assumption that no more defects are created above F, is sup- equal to the cohesion energy of the polymer.
ported by the positron annihilation spectroscopy performed on PE un- The relation between charges and defect concentration (formed be-
der high fields [31], which also indicates a saturation in the positronium fore injection) suggests that space charges are more a consequence than
yield (i.e. a saturation in the formation of defects) in the 100 kV/mm a cause of aging under high fields.
range (Figure 11). The saturation of the positronium yield corresponds
very well with the current saturation measured by Fallou and also with ACKNOWLEDGMENT
the~wavepackets observed in space charge measurements [6]. Hence,
This work was partially funded by EPRI, and we thank W. Zenger
we suggest that wave packets and 'negative resistance' occur in the 60 for his support,
to 100 kV/mm ranee. because there are no more defects created. which
Y .

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Manuscript was received on 2 December 2001