th
THE 8 INTERNATIONAL SYMPOSIUM ON ADVANCED TOPICS IN ELECTRICAL ENGINEERING
May 23-25, 2013
Bucharest, Romania
AC Breakdown Strength and Dielectric Response of
Water-treed Low Density Polyethylene
Florin Ciuprina, Senior Member IEEE, Alexandru Hornea, Laura Andrei,
ELMAT Laboratory, Faculty of Electrical Engineering, University Politehnica of Bucharest,
Bucharest, Romania
florin@elmat.pub.ro
Abstract- Results on AC breakdown strength and on dielectric
behavior of water-treed plane samples of low density
polyethylene (LDPE) are presented in this paper. Water trees
were grown at room temperature, under an electric field of 4
kV/mm, 5 kHz, and having a 0.1 M NaCl solution as electrolyte
in contact with a face of the sample having needle-like defects
created by pressing a sheet of abrasive paper. The breakdown
tests have been carried out under an AC voltage ramp, at 50 Hz.
The dielectric spectroscopy was the tool used to analyze the
dielectric behavior of LDPE samples with and without water
trees, over a frequency range of 10 mHz – 1 MHz, at room
temperature. The results show a good correlation of the
breakdown strength decrease with the increase of water tree
average length and relative volume. The dielectric spectra of
water-treed samples emphasize an increase of the sample
permittivity with the water tree growth, as well as three
relaxation peaks in the loss tangent frequency variation obeying
the Havriliak-Negami law. Possible electrical equivalent circuits
for treed and non-treed samples are also discussed.
Keywords: polyethylene insulation, power cable, water trees,
dielectric spectroscopy, breakdown strength.
I. INTRODUCTION
For over four decades water treeing in polymer cable
insulation has been intensively studied to understand and
control this phenomenon leading to a premature end of
insulation lifetime [1-3]. On the one hand, the researchers
proposed to analyze how different factors, as polymer
structure and morphology, different additives, electric field
strength and/or frequency, electrolyte type and concentration
influence the water tree inception and propagation [4-8]. The
main goal of these studies was to improve the resistance to
water treeing of polymer insulation of power cables. On the
other hand, many studies focused on the relation between the
water trees (WT) grown inside polymer insulation and the
electrical/dielectric behavior of the treed material, aiming to
detect and estimate the degree of water treeing for diagnosing
the state of water-treed insulation. In this sense a good
correlation has been found between water tree length and AC
breakdown strength, while a rather weak influence of water
tree density on breakdown strength was noticed [9-11]. It was
also reported that the breakdown of water tree degraded
polymer insulation depends significantly on the ambient
relative humidity, a rapid drop of the breakdown strength at
high humidity being noticed, while a water tree may extend
up to entire thickness of the sample without causing
breakdown under less humid conditions [12]. As for the
dielectric behavior, a number of studies proposed to correlate
the water tree content with the dielectric response of the
tested polymer samples. Thus, some works focused on the
analysis of the real and imaginary parts of the complex
relative permittivity (εr' and εr'') for different frequency
ranges, test voltages and aging temperatures [13-20], while
other studies have proposed different methods for estimating
water tree permittivity [23]. The main results reported in
these studies have showed an increase of both εr' and εr'' with
aging time and, consequently, with the water tree relative
volume, as well as a change in frequency variation of εr' and
εr'' as a result of water tree growth. Some of these results
were obtained on laboratory samples by performing
accelerated aging, while the others on real cable samples aged
in service conditions [13, 14]. It has to be noticed that the
frequency domain dielectric response of water-treed
polyethylenes was analyzed either at high frequencies (HF),
between 104 and 108 Hz [14], either at low frequencies (LF)
up to medium frequencies (MF), as for example 10-3-101 Hz
[10], 10-1-102 Hz [16], or between 10-2 and 103 Hz [17]. There
are also some studies showing broad range dielectric
spectroscopy results obtained on AC aged polyethylene from
10-5 and 106 Hz [16, 21], but with a gap of missing results
between 10-1 and 101 Hz, and without discussing the possible
water tree presence even if the aging was performed in humid
environment (0.1 M NaCl).
This work presents results from AC breakdown tests and
from broadband dielectric spectroscopy (10-2 to 106 Hz)
performed on LDPE samples water-treed by accelerated
aging. This study proposes first to confirm, on only one type
of samples, the results reported by other authors on different
sample types, and then to find out the dependences between
AC breakdown strength, frequency dielectric response in the
entire range from LF to HF and water tree content. Equivalent
electrical circuits for unaged and water treed samples are
further imagined starting from our results and from previous
approaches presented in literature.
The material for the present study was chosen a low
density polyethylene (LDPE) to avoid possible influence of
crosslinked polyethylene (XLPE) by-products on dielectric
response, which could mask or dilute the water treeing
influence on dielectric behavior. XLPE behavior in tests such
those presented here will be analyzed in a future study.
 II. EXPERIMENTAL The average length kinetics follows a typical sigmoidal law
A. Water treeing (see also Fig. 2), while average diameter have a sharp
The samples used in this study were disks with a thickness increase at the beginning of water tree growth up to 24 h of
of approximately 0.5 mm and 50 mm diameter made by aging followed by a quasi-constant evolution with small
compression molding from pellets of LDPE from Borealis, as variation around a plateau at about 180 μm. This evolution of
described elsewhere [22]. WT lengths and diameters illustrate the important effect of
Prior to aging small needle-like defects were created on one electric field on WT growth. Thus, at the beginning, the high
face of each sample, as initiation sites for water trees, by electric field all around the tip of needle-like defects created
using the same procedure as in [22]. Water trees were grown by the abrasive paper leads to an initial growth of the water
in cells [22], having the following aging conditions: AC tree channels in several directions spread as a fan which
electric field of 4 kV/mm at 5 kHz, 0.1 M NaCl as electrolyte opens at the needle tip and is centered around the normal to
and different aging times up to 96 h. Three samples were the sample faces. Thus, in the early stage of WT development
tested for each aging time. After aging the water trees were the length and the diameter have similar growth rates. Once
colored with a rhodamine solution in order to facilitate the the tree develop the electric field increases at the WT front
measurements of water tree dimensions. The average water normal to sample faces [23], this leading to a further tree
tree length and diameter for a sample was determined as the growth only in this direction, thus determining a further
average of the water trees lengths Lk and and diameters Dk increase of tree length without a significant change of its
measured on the three slices of 200 μm thickness microtomed diameter. This WT development leads to an evolution of the
from the sample [22]. The water tree relative volume of a relative volume close to that of WT average length, as
sample was determined by considering the trees as ellipsoids remarked from Table 1 and Fig. 2. As for the WT density one
having as semi-axes a = Dk/2 and b = Lk/2 (Fig. 1a) and may notice a step-like increase (in three steps) with aging
summing up the volume of all trees measured and dividing it time, this suggesting different WT inception times at different
with the total volume of the three slices. surface defect sites, related to the needle shapes and thus to
the electric field strength around them.
B. Breakdown tests TABLE I
The breakdown tests were carried out in cells filled with WATER TREE CHARACTERISTICS FOR DIFFERENT AGING TIMES
silicone oil and having plane/plane electrodes with a diameter Water tree
of 10 mm (Fig. 1b). AC voltage (50 Hz) was applied at a rate Aging Relative
time Average Average
of 500 V/s until breakdown. Three untreed samples and three length diameter
Density volume of
treed region
water-treed samples were tested for each aging time. Three
[h] [μm] [μm] [mm-2] [%]
breakdown tests were made on each tested sample and the
average was considered. 14 115 133 5.21 1.11
24 182 181 5.76 3.56
C. Dielectric spectroscopy 38 173 169 6.87 3.47
The real part of the permittivity (εr') and the loss tangent 48 184 193 6.51 4.46
(tan δ) were determined by dielectric spectroscopy (DS) using 66 214 187 8.87 6.79
a Novocontrol ALPHA-A Analyzer in combination with an 96 214 176 9.54 6.60
Active Sample Cell ZGS, over the frequency range 10-2 – 106 Results from breakdown strength analysis with respect to
Hz at a temperature of 300 K. For all tested samples the the water tree growth are presented in Fig. 2, where the
dielectric response was measured before and after water relative breakdown strength variation ΔEb = (Ebwt - Eb0)/Eb0,
treeing. between non-treed Eb0 and water-treed Ebwt values is shown
III. RESULTS AND DISCUSSION in relation with WT average length and relative volume
variation with aging time.
Results of water tree analysis are presented in Table 1.
Relative breakdown strength variation [%]

0
They show that all determined water tree parameters increase -5
24
22
with aging time but having different evolution laws.
Relative volume of WT region [%]

-10
20
Average WT length [10 μm]

-15
-20 18
ΔEb
-25 16
-30 Vrel 14
-35 12
La
-40
10
-45
8
-50
-55 6
-60 4
-65 2
-70 0
0 20 40 60 80 100
Aging time [h]
a b
Fig. 2. Relative breakdown strength variation ΔEb, water tree average length
Fig. 1. Water tree considered as ellipsoid for volume calculation (a), and La and water tree relative volume Vrel, as a function of aging time.
test cell for AC breakdown (b).
 A good correlation is remarked between the decrease of 2.80
96 h
breakdown strength and the increase of WT length and 2.75

Relative permittivity (real part)

66 h
volume. These results confirm the relation between 2.70 48 h
38 h
breakdown strength and tree lengths found on cable samples 2.65
24 h
[9, 10] or on needle-plane samples [11]. 2.60 14 h
0h
Figures 3 and 4 show the frequency variation of the real 2.55
part of the permittivity (εr') and of the loss tangent (tan δ), 2.50
respectively, for non-treed and water-treed samples at 2.45
different aging times. An increase of εr' values with the aging 2.40
time, and consequently with WT length and volume, is 2.35
remarked for all frequency range from 10-2 to 106 Hz. As for
-3 -2 -1 0 1 2 3 4 5 6 7 8 9
10 10 10 10 10 10 10 10 10 10 10 10 10
Frequency [Hz]
the tan δ variation, the results from Fig. 4 emphasize a
significantly different behavior of LDPE samples in the non- Fig. 3. Frequency variation of εr' for different aging times.
treed state with respect to the water-treed state. To discuss -1
10
this difference we need to account for the two components of
96 h
the loss tangent, which can be written as 66 h
48 h
38 h
tan δ = tan δd + tan δc. (1) 10
-2
24 h
14 h

Tan Delta
0h
In equation (1) tan δd = ε"/ε' is the dielectric loss component
(AC loss) due to different relaxations types, i.e. orientational 10
-3

(dipolar) polarization and/or localized space charge

movement , while tan δc = σDC /(ω ε') is the conduction loss
component (DC loss), where σDC is the conductivity, ω is the
angular frequency, ε' and ε" are, respectively, the real and
imaginary parts of the complex permittivity ε = ε' - j ε" =
ε0 (εr' - j εr"), ε0 being the vacuum permittivity.
Results from Fig. 4, show that the frequency variation of
tan δ for untreed LDPE is dominated for a broad frequency
range, from 10-2 to 105 Hz, by the DC conduction and/or a
quasi-DC (QDC) process [21], showing no dielectric loss
peak and a continuous decrease with frequency. A small peak
of tan δ due to an AC loss contribution can be seen only in
HF region (105 – 106 Hz), and it can be attributed to some
bound water containing ions present even in unaged LDPE
[16]. A completely different tan δ variation is shown in Fig. 4
for water tree aged LDPE. Thus, the major feature to notice is
the appearance of three loss peaks corresponding to three
relaxation mechanisms which become dominant processes in
water-treed LDPE compared to DC conduction for all aging
times. This shape of tan δ variation suggests that the water
tree development leads to an increase of the number of polar
groups and/or localized trapped space charges in the treed
-4
10
-3 -2 -1 0 1 2 3 4 5 6 7 8 9
10 10 10 10 10 10 10 10 10 10 10 10 10
Frequency [Hz]
Fig. 4. Frequency variation of tan δ for different aging times.
where ωp is the peak frequency and the parameters α and β
are in the range (0,1) [21].
LF peak appeared below 10-2 Hz could be due to localized
space charge movements [21] and/or to twists of chains in the
crystal lamellae favored by the disorder of the lamella-
amorphous interface [25] caused by an increase of the free
volume during water treeing [26]. MF peak localized in the
range 10-1 – 1 Hz, may have as causes, the ones for LF peak,
which could also be possible at these frequencies, and an
enhancement of oxidation products including carboxylic
groups. The HF peak may possibly be due to clustered water
containing ions [21] introduced in polymer during water
treeing. While LF and MF could not be correlated with water
tree growth, the HF peak increases with aging times.
10
-1

region [16], especially in WT channels in at the WT front

24 h
[24], being well known that both dipole orientation process HN fitted
and space charge restricted movement usually take a bell 10
-2

shaped curve [21].

Tan Delta

The three relaxation processes has been emphasized in Fig. 5

by fitting the experimental data for an aging time of 24 h with 10
-3

two parameters Havriliak-Negami susceptibility response

function
-4
10
1 (2)
χ ′′(ω ) ∝ . -3 -2 -1 0 1 2 3 4 5 6 7
10 10 10 10 10 10 10 10 10 10 10
(ω / ω p ) + (ω / ω p ) β (1−α )
α −1
Frequency [Hz]

Fig. 5. Frequency variation of tan δ after 24 h of aging and the fitting of

experimental data using Havriliak-Negami function.

R1 R3 R2 R1
C2 C C
G0 C1 G0 C3 C2 C1
water treeing
LF HF LF MF HF
Fig. 6. Equivalent electrical circuits of unaged (left) and water-treed (right)
LDPE samples.
This dielectric behavior with three relaxation loss peaks
was already presented by Das-Gupta et al. [21], but for XLPE
cables AC aged in humid environment, and without any
explicit connection between this behavior and the (possible)
water tree formation in the tested cable insulation.
Fig. 6 presents possible equivalent electrical circuits for the
unaged and water-treed LDPE samples, constructed by
adapting to our results circuits proposed in [21]. The very
high frequency capacitance C∞ and the conductance G0,
which accounts for any DC conduction mechanism, are
present in any equivalent circuit to model a linear dielectric
[15]. Besides C∞ and G0, the equivalent circuit for the
observed dielectric behavior of the unaged LDPE may
comprise a dissipative “universal” capacitance C2 to account
for the QDC relaxation process dominating at LF (and MF)
and by the relaxation R1C1 series network giving the dipolar
peak in HF region. As for the water-treed samples, the
equivalent circuit comprises three relaxation networks: R1C1,
R2C2 and R3C3, accounting for the dipolar peaks in HF, MF
and LF regions, respectively.
IV. CONCLUSIONS
Results from AC (50 Hz) breakdown tests and dielectric
spectroscopy measurements performed in a frequency range
from 10-2 to 106 Hz on LDPE plane samples before and after
water tree growth have been analyzed. A good correlation is
found between the decrease of breakdown strength and the
increase of water tree average length and relative volume.
The dielectric behavior of the water-treed samples show an
increase of εr' values with the aging time and a three loss peak
tan δ variation corresponding to three relaxation mechanisms
which are the dominant processes in water-treed LDPE
compared to DC conduction and QDC relaxation which
dominate the loss tangent variation in the unaged samples.
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