ARTICLE IN PRESS

Radiation Physics and Chemistry 76 (2007) 1684–1687

www.elsevier.com/locate/radphyschem

Effect of crystallinity on electrical properties of electron

beam irradiated LDPE and HDPE
F. Ziaiea,b,, M. Borhanic, G. Mirjalilib, M.A. Bolourizadehc
a
Material Research School, Nuclear Science & Technology Research Institute, P.O. Box 31485 498, Karaj, Iran
b
Radiation Applications Research School, Nuclear Science & Technology Research Institute, P.O. Box 89175 389, Yazd, Iran
c
Physics Department, Shahid Bahonar University, P.O. Box 76169 133, Kerman, Iran
Received 26 December 2006; accepted 28 January 2007

Abstract

Two sets of low-density polyethylene (LDPE) and high-density polyethylene (HDPE) sheets were prepared using warm press system.
Each set consisted of three subsets which were made in different cooling rate procedures: fast cooling with cassette; exposing in open air;
and exposing in 0 1C water, to investigate the crystallinity effects. The samples were irradiated with 10 MeV electron beam in the dose
range of 0–370 kGy using a Rhodotron accelerator system. The variation of electrical properties of all samples such as breakdown
voltage, surface and volume resistivity were measured and graphed against the dose values. The radiation induced cross-linking and
cooling procedure effects were investigated and compared in the obtained results.
r 2007 Elsevier Ltd. All rights reserved.

Keywords: Electrical properties; Breakdown voltage; Surface resistivity; Volume resistivity; Electron beam; Low-density polyethylene; High-density
polyethylene

1. Introduction Eichhorn, 1983; Karasz, 1972). In this work, attention

Solid insulation is usually extruded on to the conductor,
using many different materials including low-density
polyethylene (LDPE), high-density polyethylene (HDPE),
cross-linked polyethylene, or ethylene propylene copoly-
mer (EPR). Polyethylene is used as an insulation material
for wires and cables because of its excellent electrical
properties. The radiation cross-linking of LDPE irradiated
under 5 and 10 MeV electron beams at a wide range of dose
was previously investigated (Mateev et al.,1996; Mateev
and Karageorgiev, 1998). The effects of high-energy
electron beam on mechanical and thermal properties of
LDPE have been reported as well (Gheysari et al., 2001).
Polymers are used in many electrical applications,
often as primary electrical insulation. The electrical
properties of polymers must be understood and taken into
account for many different applications (Von Hippel, 1954,
1966; Whitehead, 1951; Frohlich, 1950; Bartnikas and
has been focused on the study of crystallinity effects on
the electrical properties of LDPE and HDPE irradiated
by 10 MeV electron beam. It could be of industrial
importance to know which cooling rate procedure is most
efficient to develop the electrical properties of an insulator
and what irradiation doses are most suitable in the related
application.
2. Experimental
2.1. Materials
Two sets of low and high-density polyethylenes, LDPE
0075 and HDPE 3840 with densities of 0.92 and 0.94 g/cm3,
respectively, were supplied by Bandar Imam Petrochemical
Company and were used in this investigation.
2.2. Sample preparation and irradiation

Corresponding author. Tel.: +98 261 4411100; fax: +98 261 4464056. The samples were prepared in a sheet form with
E-mail address: fziaie@yahoo.com (F. Ziaie). 270.1 mm thickness using the warm press system. The

0969-806X/$ - see front matter r 2007 Elsevier Ltd. All rights reserved.
doi:10.1016/j.radphyschem.2007.01.011
 ARTICLE IN PRESS
F. Ziaie et al. / Radiation Physics and Chemistry 76 (2007) 1684–1687
samples were irradiated with doses varying from 20 to
370 kGy with a constant dose rate. The irradiation was
performed using the Rhodotron-type electron accelerator
machine, TT200 model, using 10 MeV electron beam with a
maximum of 8 mA beam current.
2.3. Electrical breakdown
Electrical breakdown occurs when the applied voltage
can no longer be maintained across the material in a stable
fashion without excessive flow of current and physical
disruption. Failure of a material, due to the application of
a voltage stress is called voltage breakdown, and the
voltage gradient at failure is called the dielectric strength or
electric strength and is usually expressed in kV/mm. The
type of breakdown investigated in this work was intrinsic
breakdown which is defined by the characteristics of the
material itself in pure and defect-free form under test
conditions which produce breakdown at the highest
voltage. A Dielectric Rigidity system, P/N 6135.053, made
by CEAST Company, Italy, is used for determining the
breakdown voltage of the samples (ASTM D149-97a,
2004).
2.4. Resistance
Insulation resistance is defined as the DC resistance of a
material or device measured between electrodes or con-
ductors. Insulation resistance is a combination of surface
and volume resistance. The unit resistance, volume
resistivity and surface resistivity are calculated from
measurements with electrode arrangements shown in Fig.
1. The guard electrode B minimizes surface resistance in the
measurement of volume resistance (Fig. 1a), and volume
resistance in the measurement of surface resistance (Fig.
1b). A Tera-ohm-meter system, P/N 6148.000, made by
CEAST Company, Italy, is used for determining the
breakdown voltage of the samples (ASTM D257-99, 2005).
3. Results and discussion
3.1. Cooling procedures
The PE sheet preparations were made via three different
cooling rate procedures. In fact, PE is a semi-crystalline
polymer composed of lamellar crystals, which are typically
Fig. 1. Scheme of the electrode arrangements in resistance measurement system: (a) volume and (b) surface.
1685
arranged spherulites when cooled from the melt. When a
polymer is cooled from the melt, the lamellae grow radially
from a central nucleus to form microscopic units called
spherulites whose morphology depends on process vari-
ables such as temperature, cooling rate, pressure and
additives. It means that in slow cooling rate, a high
crystallinity percentage occurs. Therefore, the cooling at
once in 0 1C water, step by step using warm press system
cassette, and naturally in open air at room temperature,
causes the PE samples to have low, medium and high
percentage of crystallinity, respectively.
3.2. Influence on electrical properties
Figs. 2 and 3 show the variations of surface and volume
resistances as a function of irradiation dose for the three
sets of samples prepared in different cooling rate proce-
dures. In all three cases, no considerable variations were
seen due to the radiation dose increase. But, the cooling
rate has a significant role in variation of resistance. The
fluctuations in results are probably due to the sensitivity of
Tera-ohm-meter apparatus which causes a considerable
uncertainty to occur during the resistance measurements.
Numerous studies show that under voltage constraint
the PE is crossed by a low current which could be due to
several origins such as dipole orientation, etc. Although PE
is a non-polar polymer, this situation can be encountered in
the case of oxidation of PE or additives. This current
depends on several factors which relate to morphology. In
fact, cross-linking is a process occurring in the amorphous
region. Therefore, the higher the amorphous ratio, the
more the cross-linking percentage and it leads to an
increase in the molecular weight of the PE. Authors show
that an increase in molecular weight leads to an increase in
resistance (Kolesov, 1980). Moreover, it can be also due to
limiting the orientations of carbonyl dipoles in PE which
were induced by radiation.
Fig. 4 shows the dielectric strength of LDPE and HDPE
versus radiation doses for the samples made in different
cooling rates. In all cases, it is observed that the breakdown
voltage does not vary a lot with increasing absorbed dose.
As it is mentioned, one of the important factors which
affect the electrical properties is the morphological state of
polymers. Another study on PE describes the influence of
molecular weight on morphological properties, and the
consequences on electrical properties (Kolesov, 1980).
 ARTICLE IN PRESS
1686 F. Ziaie et al. / Radiation Physics and Chemistry 76 (2007) 1684–1687

Surface Resistance (1012 ohm)

50

Surface Resistance (1012 ohm)

40
40
30
30
20
20
0°C Water
10 Cst 10 0°C Water
Air Cst
Air
0 0
0 100 200 300 400 0 100 200 300 400
Dose (kGy) Dose (kGy)

Fig. 2. Surface resistance variation versus absorbed dose, (a) for LDPE and (b) for HDPE. (the error bars are close to each other for all the three sets
of results).

Volume Resistance (1012ohm)

Volume Resistance (1012ohm)

250 250
0°C Water 0°C Water
Cst Cst
200 Air 200 Air

150 150

100 100

50 50

0 0
0 100 200 300 400 0 100 200 300 400
Dose (kGy) Dose (kGy)

Fig. 3. Volume resistance variation versus absorbed dose, (a) for LDPE and (b) for HDPE. (the error bars are close to each other for all the three sets
of results).

a b
Dielectric Strength (KV/mm)

Dielectric Strength (KV/mm)

40 40
35 35
30 30
25 25
20 20 W
W
15 15 CASS
CASS
10 10 A
A
5 5
0 0
0 50 100 150 200 250 300 350 400 0 50 100 150 200 250 300 350 400
Dose(KGy) Dose (KGy)

Fig. 4. Dielectric strength variation versus absorbed dose, (a) for LDPE and (b) for HDPE (the error bars are close to each other for all the three sets
of results).

Since the irradiation changes the polymer network, it of the charge carriers and finally decreases the breakdown
changes the morphological state of the polymer. An increase (Chen et al., 1995). Our assumption is that the above
in the radiation dose leads to an increase in the degree of discussion shows opposite behaviors, so that, it may be
cross-linking in amorphous area which may barrels to prevent concluded that the irradiation dose does not have much of an
the electric breakdown path and thus increases breakdown effect on the breakdown voltage variation.
stress (Okashita et al., 1998). On the other hand, the increase The assumption about the crystallinity ratio is that
in radiation dose increases the chain scission of PE that leads an increase in the crystallinity decreases the dielectric
to decrease in the breakdown, and it increases the oxidation strength due to increase in the amorphous–crystalline
degree of PE which leads to an increase in the carbonyl boundary regions, but it also is parallel to decreasing the
groups and trap centers. So, it causes to increase the mobility amorphous ratio and decreasing the dielectric strength due
 ARTICLE IN PRESS
F. Ziaie et al. / Radiation Physics and Chemistry 76 (2007) 1684–1687
to increasing the density (Kolesov, 1980). Thus, overall the
dielectric strength variations are not considerable.
4. Conclusion
Measurement of the surface and volume resistance and the
dielectric strength in different crystallinity ratios and different
electron beam radiation doses were carried out for LDPE and
HDPE materials and led to the following conclusions:
1. Increasing the irradiation dose does not change the
surface and volume resistance of the 10 MeV electron
beam irradiated LDPE and HDPE samples.
2. Increasing the crystallinity ratio leads to a decrease in
the surface and volume resistance of the 10 MeV
electron beam irradiated LDPE and HDPE samples.
3. Increasing the radiation dose does not change the
dielectric strength considerably.
4. Variation of crystallinity ratio does not affect the
dielectric strength.
Acknowledgments
The authors would like to thank Mr. A. Shamekhi and
other experts of polymer and dosimetry laboratories of the
Yazd Center.
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