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18 S. Diaham et al.

: Dielectric Breakdown of Polyimide Films: Area, Thickness and Temperature Dependence

Dielectric Breakdown of Polyimide Films: Area, Thickness


and Temperature Dependence
S. Diaham, S. Zelmat, M.-L. Locatelli, S. Dinculescu, M. Decup and T. Lebey
Université de Toulouse; UPS, INPT; LAPLACE (Laboratoire Plasma et Conversion d'Energie);
118 route de Narbonne, F-31062 Toulouse cedex 9, France.
CNRS; LAPLACE; F-31062 Toulouse, France.

ABSTRACT
Changes in the dielectric breakdown field of polyimide (PI) films have been studied
from 25 to 400 °C under dc ramps. Both the area (from 0.0707 to 19.635 mm2) and
thickness (from 1.4 to 6.7 µm) dependences of the dielectric breakdown field have been
carried out using the Weibull distribution function. The 63%-breakdown field value
(i.e. the -scale parameter) of PI shows a decrease with increasing area, thickness and
temperature but always remains above 2 MV/cm. The -scale parameter of the
distribution shows a typical decrease with increasing area, however, it exhibits an
increase with increasing thickness. This ‘curious’ behavior is discussed on the basis of
the percolation theory. No temperature-dependence is clearly observed. Moreover,
physical interpretations are carried out using the pre-breakdown current analysis.
Index Terms — Polyimide (PI), dielectric breakdown, dielectric strength, area,
thickness, temperature, Weibull distribution.

1 INTRODUCTION geometries. Several studies have reported the area or thickness


dependence of the dielectric breakdown field of PI [10, 11].
THE development of electronic devices operating under Nevertheless, among the large range of values found in the
high temperatures (200-400 °C) involves the use of literature, usually between 1 and 5 MV/cm, it appears as
appropriate thin dielectric materials to achieve the electrical relatively difficult to establish laws where the influence of
insulation of the components [1–3]. Polyimide (PI) materials each parameter is clearly identified when combined to another
are often used for the surface insulation of power electronic one.
devices due to their excellent intrinsic properties such as In a previous study [12], the changes in the electrical
thermal stability (weight losses <1% at 500 °C), high dielectric conductivity of PI up to 400 °C were carried out. In the
breakdown field (EBR>2 MV/cm), relatively low losses, also at present study, the measurements of the dielectric breakdown
higher temperatures (tan <10-2) and thermo-mechanical field across the same temperature range have been performed.
matching with components [4, 5]. They also appear as It corresponds to the highest temperature range of
potential candidates for high temperature power electronic investigation reported up to now for these materials. In
device insulation. addition, the close dielectric breakdown dependence existing
A study of their electrical properties and particularly of their between the area and the thickness combined to the
dielectric breakdown field across a high temperature range has temperature is presented. Finally, a particular analysis is
to be performed. The dielectric breakdown of PI has already done both to the scale and shape Weibull parameters versus
received much attention since their development for electrical the experimental parameters.
insulation and their intensive use in industrial applications [6,
7]; however, for temperatures ranging above 200 °C few has
been investigated and in any case never exceeds 250-300 °C 2 THEORETICAL PART
[8, 9]. Hence, for higher operating temperatures, an extended
study appeared as necessary. 2.1 TEMPERATURE DEPENDENCE OF THE
Moreover, the impact of other parameters usually affecting DIELECTRIC BREAKDOWN OF POLYMERS
the breakdown field of polymers such as geometrical Several studies have already carried out the relationships
parameters (thickness and area) has to be investigated too. The between the high electric field conduction and the
study of their influence is of primary importance since this breakdown processes in polymers [13–15]. Theories on the
allows predicting the dielectric breakdown field for wider breakdown mechanisms are usually divided into three
categories: electronic, thermal and mechanical processes.
However, the measured dielectric breakdown field could
Manuscript received on 14 October 2008, in final form 24 June 2009. sometimes be influenced by secondary effects such as field

1070-9878/10/$25.00 © 2010 IEEE

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IEEE Transactions on Dielectrics and Electrical Insulation Vol. 17, No. 1; February 2010 19

distortion due to space charge, temperature increase due to low critical temperature (T<TC1) and is roughly not
local heating and thickness deformation due to Maxwell depending of the temperature despite in some cases below
stress [15, 16]. room temperature, a slight increase can be observed [16].
The temperature dependence of the dc dielectric The second one is the thermal breakdown process
breakdown field (EBR) of polymers usually shows a appearing for an intermediate temperature range
decreasing behavior with increasing temperature. However, (TC1<T<TC2). It is initiated by the steady state or impulse
this decrease appears as non-linear displaying different slopes thermal processes. Finally, above a high critical
in the EBR thermal dependence, as shown in Figure 1. temperature (T>TC2), an electromechanical mechanism is
preferred due to deformations and softening of polymers
(II) induced by the electrostatic forces between the test
(III)
electrodes.
Dielectric breakdown field EBR

(I)

Typical
experimental curve
2.2 STATE OF THE ART OF THE DIELECTRIC
BREAKDOWN FIELD OF POLYIMIDES
Few papers present a combined study (thickness,
electrode area and temperature) of the dielectric breakdown
field of PI. Table 1 shows a review of the dielectric
TC1 TC2 Temperature
breakdown field values of PI found in the literature,
varying with different experimental parameters [8–11, 17–
(I): T<TC1; Electronic avalanche breakdown 25]. A wide range of EBR values has been reported up to
(II): TC1<T<TC2; Thermal and electro-thermal breakdown now, usually between 1 and 5 MV/cm, but the influence of
(III): T>TC2; Electromechanical breakdown the different parameters is not clearly identified when
combined to another one particularly if extrapolation laws
Figure 1. Typical temperature dependence of the dielectric breakdown are under concerns. Last, a statistical approach of the
field of polymers and the failure processes related (after [15]). dielectric breakdown phenomenon is not always used to
provide accurate and comparable results. It, nevertheless,
Three breakdown processes are usually cited. The first constitutes the state of the art regarding the thickness, area
one is the electronic avalanche breakdown which is a pure and temperature dependence of the dielectric breakdown
electronic breakdown. This phenomenon occurs below a field of PI.

Table 1. State of the art of the dielectric breakdown field of PI varying with different experimental parameters.

Thickness (µm) Electrode area Temperature (°C) Voltage form EBR (MV/cm) Atmosphere Ref.

0.017 – 0.021 0.1 – 0.5 mm2 -243 – 27 dc ~ 0.01 vacuum [17]


2
0.12 – 0.4 5 × 5 mm 30 – 170 ac (10 Hz – 3 kHz) 2–4 vacuum [18]
2
0.4 – 1.6 0.15 – 0.4 cm 20 – 250 dc: 200 V/s 1.2 – 3 SF6, N2 and dry air [9]

0.8 – 2 -100 – 200 dc 1.9 – 5 vacuum [10]

13 – 125 Ø 5 mm 25 ac (50 Hz): 500 V/s 3.1 – 4 transformer oil / dibutyl [19]
DC: 500 V/s 5 – 5.2 phthalate (DBP)

13 – 175 Ø 5 mm 25 ac: 500 V/s 0.8 – 3.75 transformer oil / DBP [20]

25 Ø 0.2 mm 90 dc: 30 V/s 4.7 – 5.2 silicone oil [21]

25 -196 ac: 500 V/s 1.8 – 3.4 liquid N2 [22]

25 – 75 Ø 1.25 – 5 cm 25 dc: 200 V/s 2 – 3.5 air [11]

26 – 78 -196 – 300 dc: 0.5 – 10 kV/s 0.9 – 4.9 liquid N2, silicone oil [8]

125 23 – 160 dc: 5 kV/s 1.5 – 2 [23]

125 90 Pulse: 200 V, 5 ns 3 silicone oil [24]

125 100 – 140 Step: 2 kV for 1 min 1.8 – 2.2 [25]

Ø: diameter.

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20 S. Diaham et al.: Dielectric Breakdown of Polyimide Films: Area, Thickness and Temperature Dependence

performed between 25 and 400 °C (± 1 °C checked with a


3 EXPERIMENTAL thermocouple on the sample surface) thanks to a regulated
Signatone heating chuck in an air-closed cell (i.e. home-
3.1 POLYIMIDE FILM PREPARATION made closed cell with a transparent glass upper face for no
The PI studied here is compound of a biphenyl fresh air exchange with the environment). The heating rise
tetracarboxilic dianhydride and a p–phenylene diamine rate was of 5 °C.min-1. A thermalization of the samples
(BPDA/PDA), as shown in Figure 2. during 10 minutes at the studied temperature was achieved
before the breakdown measurements. Figure 3 shows a
O
schematic representation of the experimental set-up.
Voltage control
O
* N
U U(t)=(U0/t0).t
HV probe GPIB IEEE 488
N * DC voltage
O U0
source
VBR
O t0 t
n
-1 -1
dE/dt=200 kV.cm .s
Figure 2. Chemical structure of the BPDA/PDA polyimide [4]. Probe station
Air-closed cell

Faraday cage
PI films have been obtained from a polyamic acid (PAA) K-type thermocouple

precursor dissolved in N-methyl-2-pyrrolidone (NMP)


Heating chuck
solvent. PI coatings have been obtained by dispensing
subsequently an adhesion promoter and the PAA solution
on golden stainless steel substrates (16 cm2), followed by a
spin-coating at 4000 rpm during 30 seconds and a RS 232
T +5 °C.min
-1

progressive soft-bake up to 175 °C for 3 minutes on a hot Heating system


t

Temperature
plate in air. For higher film thicknesses, multilayer coatings (25-400 °C) control

have been realized using the same process. The coatings HV

have been finally cured at 400 °C for 1 h in an oven under Voltage


U(t)
Top electrode
source
nitrogen atmosphere in order to drive off the NMP solvent PI film
Substrate Lower electrode
and to complete the imidization chemical reaction of the
films. Three film thicknesses of 1.4, 3.6 and 6.7 µm have Figure 3. Schematic representation of the experimental set-up.
been used and measured thanks to a KLA Tencor
profilometer (accuracy +/- 1 nm).
Circular metal-insulator-metal (MIM) capacitor structures Pre-breakdown current-voltage characteristics have been
have been achieved by the thermal evaporation under measured using a source meter Keithley 2410 (0–1100 V)
vacuum of a gold metallization (150 nm) onto the PI film owning an internal ammeter. Figure 4 shows a typical result
surface followed by the design of circular electrodes using of the measurement of the pre-breakdown current for a
a photolithographic process, as already presented elsewhere linear applied voltage rising.
[26]. Five different diameters have been used from 0.3 to 5
0
mm corresponding respectively to areas from 0.0707 to 10
UBR
19.635 mm2. 10
-1
496

-2
10 397
dE
3.2 MEASUREMENT SET-UP = 200 kV .cm −1 .s −1 ISC=20 mA
-3 dt
10

U (V)
I (A)

298
Dielectric breakdown field measurements have been -4
10
performed using a dc voltage ramp supplied by a 3.5 kV
198
FUG voltage source connected to the sample through a 10
-5

probe station using HV insulated needles fixed to precision -6 99


10
xyz-micropositioners S725 from Microworld. Prior to the
measurements, the needles have been disposed on the top of 10
-7
0
the electrodes with a high precision using a microscope. 0 5 10 15 20 25 30
The equivalent dc electric field rising was controlled Time (sec)
using a software program and was set to 200 kV.cm-1.s-1. Figure 4. Example of the pre-breakdown current measurement versus
The breakdown field was identified when the voltage time for an applied DC voltage ramp.
source switched into current source supplying a short-
circuit current (ISC) set to 20 mA. The maximum voltage
supplied was also recorded using a voltmeter connected to 3.3 SAMPLE POPULATION
the source via a HV probe and was considered as the Due to the stochastic nature of the dielectric breakdown,
breakdown voltage. Measurements followed the D149-97a measurements have been performed on 30-60 samples for
ASTM norm related to the breakdown of solid dielectric each of the parameters under study (electrode area, film
materials [27]. High temperature measurements have been thickness and temperature). During measurements, the

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breakdown craters have rarely been observed near the failure F( )=63.2%, is the shape parameter. A high –
electrode edge (due to their neat circular design using value is related to a low scattering of the data. The location
microelectronic photolithographic masks, and also to the (or threshold) parameter has been set to zero.
small film thicknesses). In almost all cases, the final
location of the irreversible breakdown is near the center of (a)
the structure. A self-healing phenomenon has sometimes
Irreversible
been observed only within the largest area tested electrodes breakdown craters
(diameters Ø = 2.5 and 5 mm). In this case, few healed-
craters (~1 to 3) scattered within the metallization before
the irreversible breakdown were observed, as seen in Figure
5a. The self-healing craters within the metallization (in a Self-healing craters
poor quantity compared to other works [9]) are here
preferably related to a local extrinsic contamination during 2 mm

the coating process. (b)


2
SEM images from Figures 5b to 5d show a typical self-
healing crater at different scales. A central puncture can be
observed in the crater. It corresponds to the breakdown
4
channel through the PI film caused by the arcing (cf. Figure
5b). All around this path, an extended dark carbonized
region (region 3 in Figure 5c) with PI peelings at surface 1 3
film is observed up to the metalized edge of the crater. This
appears as a consequence of a local heating. The main
breakdown channel is around 30 m in diameter. It lets (c)
appear the lower electrode of the MIM structure below the
PI film (cf. Figure 5d). Figure 5e shows the profilometer
scan across the self-healing crater of Figure 5b. It is 4
possible to observe in the regions 4 and 5 the location of
the main breakdown channel through the PI bulk. It is also 3
possible to observe two sharp peaks at the edge of the crater
that correspond to a roll of melted gold (see also in Figure
5b in region 2). The melting temperature of gold (Tm= 1064
(d)
°C) shows the very high local temperature involved during 3
the breakdown process. The huge diameter of the crater 4
(~300 m), ten times wider than the main breakdown
channel, is certainly due to the release of the electrostatic
energy stored in the MIM capacitance strongly associated
with thermo-mechanical constraints involved by the local
heating around an extrinsic defect.

3.4 STATISTICAL ANALYSIS 2,8 (e) 2

Dielectric breakdown field under homogeneous 2,1


conditions has been calculated using the following relation: 2
1,4 crater width
Height (μm)

1 1
U BR
E BR = (1)
0,7
3 3
d 0,0
4

where UBR is the breakdown voltage and d is the film -0,7 5


thickness.
-1,4
Experimental data have been statistically analysed using 0 100 200 300 400
the Weibull distribution law [28]:
Width (μm)
β Figure 5. Breakdown craters observed within the test electrodes (a). SEM
⎛ x −γ ⎞
−⎜ ⎟ images of a self-healing crater (b, c, d). Profilometer scan across a
⎝ α ⎠
F ( x) = 1 − e (2) breakdown crater for a 1.4 m-thick PI film (e). 1: edge of the safe gold
electrode around the crater; 2: roll of melted gold around the crater; 3:
carbonized PI film surface; 4: diameter of the main breakdown channel; 5:
where F(x) is the cumulative probability of failure, is the depth of the main breakdown channel corresponding also to the PI
scale parameter (V/cm) corresponding to a probability of thickness.

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22 S. Diaham et al.: Dielectric Breakdown of Polyimide Films: Area, Thickness and Temperature Dependence

The experimental data have been ranking using the the material bulk leading to the failure of the insulating
median rank approximation given by [29, 30]: layer. This behaviour has already been reported in organic
materials such as polypropylene [32, 33], aramid paper,
i − 0.3 polyester mylar and Kapton-H films [11], but also in liquids
F (i, n) = (3) [34, 35] and gases [36]. Last, it may be seen that the
n + 0.4 temperature has an effect on the Weibull parameter values
that will be discussed in section IV.3.
where i and n are the rank of a failed sample and the total
number of tested samples, respectively.
For plotting the Weibull distribution law, the Ø 0.3 mm
(a)
0
10 Ø 0.5 mm
transformation of equation (2) into equation (4) has been Ø 1 mm
realized: Ø 2.5 mm
Ø 5 mm
-2

j (A/cm )
10

2
⎡ ⎛ 1 ⎞⎤
log 10 ⎢log e ⎜⎜ ⎟⎟⎥ = β [log 10 ( x) − log 10 (α )] (4)
⎣ ⎝ 1 − F ( x) ⎠⎦
-4
10

The Weibull parameters have been extracted considering


a confidence interval of 90 %. Both the maximum T=25 °C
-6
10
likelihood and least square fit methods have been also 3,0 3,5 4,0 4,5 5,0 5,5 6,0
applied leading to similar – and –parameter values [31]. E (MV/cm)

Ø 0.3 mm
(b)
3.5 PRE-BREAKDOWN CURRENT-VOLTAGE Ø 0.5 mm
-1
CHARACTERISTICS 10 Ø 1 mm
Ø 2.5 mm
Figure 6 shows an example of the conduction current Ø 5 mm
j (A/cm )
2

density in PI films versus the applied electric field at 25 and


300 °C for different electrode diameters. A good
-3
superimposition of the current densities is observed for all 10

the electrode areas investigated. PI films may therefore be


considered of homogeneous quality whatever the
investigated area. Hence, it is also acceptable to assume that T=300 °C
the breakdown current mechanisms are mainly related to 10
-5

2,00 2,25 2,50 2,75 3,00 3,25 3,50


the material bulk and not to edge effects.
E (MV/cm)
Figure 6. Pre-breakdown conduction current density in PI films versus
4 RESULTS AND DISCUSSION applied electric field in the high field region for different electrode
diameters at 25 °C (a) and 300 °C (b). (Film thickness d=1.4 µm).

4.1 ELECTRODE AREA EFFECT ON THE WEIBULL For the lowest breakdown fields (F(x)<10 %), it appears
PARAMETERS that PI displays a deviating behaviour of the distribution of
Figure 7 shows the cumulative probability of failure in PI the breakdown field values. Indeed, another slope of the
films both at room temperature and 300 °C versus the cumulative probability of failure with a lower value can be
dielectric breakdown field for the different electrode distinguished. Trying to fit a non-zero location parameter
diameters. The values of the dielectric breakdown field to the experimental data, a value close to the lowest
ranged from 0.6 to 7 MV/cm depending on the temperature dielectric breakdown field for each electrode area has been
and the electrode area. These orders of magnitude are in found.
agreement with those reported in [9] and [10] for equivalent For the study of polymers, a natural location parameter
PI film thickness ranges. could be the dielectric breakdown field of air (i.e. the
For each temperature, it is possible to observe that the minimum Paschen breakdown voltage ~300 V) due to the
cumulative probability curve shifts slightly towards lower presence of vacuoles in the film. However, the thickness
breakdown fields with increasing the electrode diameter. range investigated here is lower than the minimum vacuole
The scale parameter (F=63.2 %) decreases also with diameter allowing the occurrence of partial discharges (~8
increasing the electrode diameter. In the same way, the µm) and none of this kind of defects has been observed
shape parameter (i.e. the slope of the fitting straight line) even by microscopy. Otherwise, there is no obvious
decreases with increasing the electrode diameter. These two physical or technological reason to take into account a non-
simultaneous observations deal typically with an increase in zero location parameter. It appears more realistic to
the result scattering. They usually are characteristic of an consider that there is another Weibull distribution law for
increase in the probability to find defects or impurities in low electric fields (not investigated here) [14], more

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pronounced with increasing the electrode area. A similar where kA and mA are empirical area coefficients. kA
discussion has been reported by Laihonen et al. on represents the extrapolated dielectric breakdown field for
polypropylene films [33]. The presence of two Weibull an area of 1 m2.
distribution laws across distinct field ranges could be due to
two failure mechanisms of different nature. The first one 7
occurring at low fields and more influent for large electrode 6

areas could be related to the presence of macroscopic 5

impurities in the MIM structure, while the second one 4

α (MV/cm)
appearing across the high field range could be explained by
3
a thermal and/or electromechanical origin.

2
25 °C
1
F (%) 200 °C
T=25 °C 300 °C
95.7
340 °C
400 °C (a)
log10[loge(1/1-F)]

0 63.2
1
27.1 0,01 0,1 1 10 100
2
Electrode area (mm )
-1 9.5
Ø 0.3 mm
Ø 0.5 mm 0.95
Ø 1 mm 25°C
-2 Ø 2.5 mm 200°C
Ø 5 mm
10 300°C
(a)
340°C
0,1 1 10 400°C
EBR (MV/cm)

1 β
F (%)
T=300 °C
95.7

(b)
log10[loge(1/1-F)]

0 63.2
1
27.1 0,01 0,1 1 10 100
2
Electrode area (mm )
-1 9.5
Ø 0.3 mm Figure 8. Changes in the scale (a) and shape (b) parameters versus the
Ø 0.5 mm 0.95
electrode area and for different temperatures (film thickness d=1.4 µm).
Ø 1 mm
-2 Ø 2.5 mm
Solid lines represent the best fits given by equation (6).
Ø 5 mm
(b)
Transformation of equation (5) into equation (6) allows
0,1 1 10
obtaining kA and mA fitting linearly data in Figure 8a:
EBR (MV/cm)

1
Figure 7. Cumulative probability of failure in PI films versus the
dielectric breakdown field at 25 °C (a) and 300 °C (b) and for different log 10 (α ) = log 10 ( k A ) − log 10 ( A) (6)
electrode diameters (film thickness d=1.4 µm). Solid lines represent the
mA
best fits given by equation (4) considering a confidence interval of 90%.
Table 2 lists the changes in kA and mA versus
temperature. These parameters allow extrapolating the –
Figure 8 shows the changes in the scale and shape parameter whatever the electrode area. It also appears that
parameters versus the electrode area for different the dielectric breakdown field of PI remains high (above 1
temperatures. Both the – and –parameters present a linear MV/cm) even for large areas and high temperatures.
decrease in a bi-logarithmic plot with increasing the
Table 2. Evolution of the kA and mA coefficients from equation (6) versus
electrode area. Assuming that the weak points present in the temperature for a PI film thickness of 1.4 µm.
material leading to a breakdown are randomly and Temperature (°C) kA (MV/cm) mA
uniformly scattered, it is known that the scale parameters
used to decrease with increasing the electrode area 25 2.33 18.64
following the area extrapolation law given by [31, 34, 36]: 200 2.02 20.92
300 1.88 24.06
1 340 1.14 15.05

α ( A) = k A A mA
(5) 400 0.61 9.87

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24 S. Diaham et al.: Dielectric Breakdown of Polyimide Films: Area, Thickness and Temperature Dependence

The decrease in with increasing the electrode area (cf. 1


Figure 8b) shows also the widening of the Weibull log 10 (α ) = log 10 ( k d ) − log 10 (d ) (8)
distribution law related to a higher dispersion of the md
breakdown measurements for large electrodes. The slopes
of the area extrapolation law for the –parameter range Values of md in the range from 0.16 to 0.25 have been
between 0.18 and 0.32. obtained between 300 and 400 °C. This result is in good
agreement with typical values found in the literature for
polymers and for such a little variation of the thickness.
4.2 THICKNESS EFFECT ON THE WEIBULL Usually, the md coefficient tends towards 0.5 for higher
PARAMETERS changes in the thickness [38].
The influence of the thickness on the Weibull parameters
has also been investigated. The impact of the PI film 5
thickness has only been studied for the lowest electrode
4
area (diameter Ø = 0.3 mm) to avoid the occurrence of two
Weibull distribution laws. It is also assumed that the
3
breakdown is intrinsic.

α (MV/cm)
Figure 9 shows the cumulative probability of failure in PI
versus the dielectric breakdown field for the different 2
thicknesses investigated. As expected, a unique Weibull
distribution law is observed.
300 °C
1 400 °C
F (%)
T=300 °C 1
95.7 1 2 3 4 5 6 7 8
Thickness (µm)
log10[loge(1/1-F)]

0 63.2
Figure 10. Changes in the scale parameter versus the PI film thickness
27.1 (electrode Ø 0.3 mm). Solid lines represent the best fits given by equation
(8).
-1 9.5

0.95 The second observation was unexpected. Indeed, the


1.4 µm shape parameter shows an increase with increasing PI
-2 3.6 µm
6.7 µm
thickness (cf. Figure 11). It could be a priori supposed that
when the probability to find defects into the bulk increases,
1 10 an increase in the scattering of the breakdown and a
EBR (MV/cm) decrease in the shape parameter value ought to be observed.
This atypical behavior has already been discussed in the
Figure 9. Cumulative probability of failure of PI versus the dielectric
literature for thin oxides and seems to be related to
breakdown field for different film thicknesses (T=300 °C; electrode Ø 0.3
mm). percolation theories [39–41].
2
10
As for the electrode area dependence, the –parameter
shifts towards lower field when the film thickness
increases. However, unlike the area case, the slope of the
Weibull distribution law (i.e. the –parameter) increases
with increasing the film thickness. The first observation
leads to show that the dielectric breakdown field is affected 1
β

10
300 °C
by the thickness increase due to the increase in the 320 °C
probability to find defects or impurities in the bulk of the 340 °C
insulating layer leading to the failure. Such a behavior has 360 °C
380 °C
already been observed in PI films [8, 10, 19, 20]. Reporting 400 °C
the –parameter values in a plot versus the PI film 10
0

thickness (cf. Figure 10), it seems that the scale parameter 1 2 3 4 5 6 7 8


obeys to the following thickness extrapolation law [36, 37]: Thickness (µm)
Figure 11. Changes in the shape parameter versus the PI film thickness
α (d ) = k d d − m d
(7) (electrode Ø 0.3 mm).

It has been shown that the shape parameter decreases as


where kd and md are empirical thickness coefficients. a result of scaling-down of oxide thickness. The reduction
Transformation of equation (7) into equation (8) allows of the shape parameter with decreasing oxide thickness
obtaining kd and md fitting linearly data in Figure 10: has been attributed to the decrease in the critical defect

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IEEE Transactions on Dielectrics and Electrical Insulation Vol. 17, No. 1; February 2010 25

density required to form a breakdown path. It is evident that the dielectric breakdown field shows a slight decrease when
such a behavior may have a physical origin that cannot be the film thickness increases with values of the –parameter
resolved experimentally with the statistical accuracy even from 3.7 to 2.9 MV/cm and from 3.3 to 2.3 MV/cm,
with large experimental data, as seen in Figure 9. However, respectively at 300 and 400 °C.
the values obtained here from 8 to 30 are of the same order
and show the same tendency than those reported by 7
Laihonen et al on polypropylene films across the similar
thickness range [33]. Up to now, no clear interpretation has 6

been proposed for explaining such an increase. On-going 5

α (MV/cm)
works have recently started in order to explain this
behavior. 4

3
Ø 0.3 mm
4.3 TEMPERATURE EFFECT ON THE WEIBULL 2 Ø 0.5 mm
Ø 1 mm
PARAMETERS 1 Ø 2.5 mm
As presented in section 2.1, the typical change in the Ø 5 mm
0
dielectric breakdown field of polymers usually decreases 0 50 100 150 200 250 300 350 400
with increasing temperature even if, in some cases below Temperature (°C)
room temperature, a slight increase can be observed [15, Figure 12. Changes in the scale parameter versus temperature for
16]. This decrease is usually due to thermal and/or different electrode diameters (film thickness d=1.4 µm).
electromechanical processes. In PI materials, the widest and
highest temperature region of investigation found in the
literature up to now has been reported by Nagao et al in Figure 13 shows the high temperature dependence of the
PMDA/ODA from -196 to 300 °C using a dc electric field –parameter versus geometrical changes. Contrary to the –
rising rate of 200 kV.cm-1.s-1 [8]. These authors observed a parameter, the –parameter is independent with increasing
slight increase in the dielectric breakdown field from -196 temperature.
to 25 °C, before measuring an exponential decrease up to
300 °C. A higher temperature range of investigation has 10
2

been studied here (up to 400 °C) as long as the dielectric


Ø 0.3 mm Ø 2.5 mm
breakdown field remained high (≥2 MV/cm) even above Ø 0.5 mm Ø 5 mm
300 °C. This high temperature range was also motivated by Ø 1 mm
both theoretical and application interests. The observed
behavior corresponds exclusively to values of EBR 1
10
β

measured before the beginning of thermal ageing


phenomena that can occur usually at long-term above 300
°C (usually over several hours). So, it can be considered
here that ageing phenomena have no time to occur due to
the fastness of measurements. (a)
Figure 12 shows the changes in the scale parameter 10
0

300 320 340 360 380 400


versus temperature from 25 to 400 °C and for the different
electrode diameters under study. Exponential decreases in Temperature (°C)
the dielectric breakdown field appear with increasing 10
2

temperature except for electrodes of 0.3 mm in diameter


(linear behavior). Even if the dielectric breakdown field
decreases with increasing temperature, no dramatic drop
has been observed at a critical temperature. This is certainly
due to the absence of a glass transition phenomenon across 1
β

10
the whole temperature range of investigation, as shown in
[42]. The dielectric breakdown field of PI shows also a
behavior close to the one of the region II of the Figure 1, 1.4 µm
just between the two critical temperatures (TC1<T<TC2) and 3.6 µm
where TC2 often corresponds to the glass transition 6.7 µm (b)
0
temperature. So, a thermal origin of the breakdown process 10
300 320 340 360 380 400
is maybe supposed as the most probable failure mechanism.
PI films with various electrode areas have shown a Temperature (°C)
dielectric breakdown field from 4.3 to 6 MV/cm and from Figure 13. Changes in the shape parameter versus temperature for
1.9 to 3.3 MV/cm, respectively at 25 and 400 °C. For a different (a) electrode diameters (film thickness d=1.4 µm) and (b) PI
given electrode diameter of 0.3 mm (as seen in Figure 10), thicknesses (electrode diameter Ø = 0.3 mm).

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26 S. Diaham et al.: Dielectric Breakdown of Polyimide Films: Area, Thickness and Temperature Dependence

The only changes are induced by the geometrical [5] C. P. Wong, Polymers for Electronic and Photonic Applications,
London: Academic Press. Inc, 1993.
parameters of the MIM structures with a main effect caused
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[9] Y. Muramoto, M. Nagao, F. Mizuno, and M. Kosaki, “Self-Healing
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The dielectric breakdown field of polyimide (PI) thin Proc. 30th Intern. Sympos. Electr. Insulating Materials, pp. 173-176,
1998.
films has been studied across the temperature range from 25 [10] K. Iida, S. Nakamura, and G. Sawa, “Dielectric Breakdown and
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temperature range ever investigated up to now for this Pyromellitimide)”, Japanese J. Appl. Phys., Vol. 33, pp. 6235-6239,
material. This study has mainly been motivated by both 1994.
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characteristic of an increase in the probability to find [14] L. A. Dissado and J. C. Fothergill, Electrical Degradation and
Breakdown in Polymers, IEE Materials and Devices Series 9, Peter
defects or impurities underneath the electrode leading to a Peregrinus Ltd, London, UK, 1992.
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electrode area, only the –parameter shows a decrease with Breakdown in Insulating Polymers: Present Situation and Future
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unexpected increase with increasing the thickness.
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The authors are grateful to B. Schlegel and B. Lantin for [22] E. Tuncer, I. Sauers, D. Randy James, A. R. Ellis and M. 0. Pace,
“Breakdown Statistics of Polyimide at Low Temperatures”, IEEE
their technical contribution to this work.
Conf. Electr. Insul. Dielectr. Phenomena (CEIDP), pp. 561-564,
2002.
[23] G. R. Govinda Raju, A. Katebian, and S. Z. Jafri, “Breakdown
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IEEE Transactions on Dielectrics and Electrical Insulation Vol. 17, No. 1; February 2010 27
[27] ASTM D149-97a, “Standard Test Method for Dielectric Breakdown Samir Zelmat was born in Sidi Bel Abbes,
Voltage and Dielectric Strength of Solid Electrical Insulating Algeria in 1978. He received the Engineer degree
Materials at Commercial Power Frequencies”, 1983. in electrical engineering from Djilali Liabes
[28] W. Weibull, “A Statistical Distribution of Wide Applicability”, J. University, Sidi Bel Abbes, Algeria in 2000, the
Appl. Mechanics, Vol. 18, pp. 293-297, 1951. M’Res degree and the Ph.D. degree in electrical
[29] J. C. Fothergill, “Estimating the Cumulative Probability of Failure engineering, respectively in 2002 and 2006 from
Data Points to Be Plotted on Weibull and Other Probability Paper”, Paul Sabatier University, Toulouse, France. From
IEEE Trans. Electr. Insul., Vol. 25, pp. 489-492, 1990. 2002 to 2007, he worked as an Assistant
[30] C. Chauvet and C. Laurent, “Weibull Statistics in Short-term Professor at Paul Sabatier University, and the
Dielectric Breakdown of Thin Polyethylene Films”, IEEE Trans. University of Poitiers, France. He currently works
Electr. Insul., Vol. 28, pp. 18-29, 1993. at LAPLACE Laboratory in Toulouse as a
[31] S. J. Laihonen, “Polypropylene: Morphology, Defects and Electrical Research Associate Fellow. His research interests include dielectric
Breakdown”, Ph.D. thesis, Royal Institute of Technology of materials and high temperature power electronic packaging.
Stockholm, Sweden, p. 84, 2005.
[32] S. J. Laihonen, A. Gustafsson, U. Gäfvert, T. Schütte, and U. W. Marie-Laure Locatelli was born in Nantua,
Gedde, “Area Dependence of Breakdown Strength of Polymer Films: France, in 1965. She received the engineering
Automatic Measurement Method”, IEEE Trans. Dielectr. Electr. degree in electrical engineering in 1988 and the
Insul., Vol. 14, pp. 263-274, 2007. Ph.D. degree in integrated electron devices in
[33] S. J. Laihonen, U. Gäfvert, T. Schütte, and U. W. Gedde, “DC 1993 from the INSA of Lyon (France). As a
Breakdown Strength of Polypropylene Films: Area Dependence and Research Associate of the National Center of
Statistical Behavior”, IEEE Trans. Dielectr. Electr. Insul., Vol. 14, Scientific Research (CNRS) since 1993, she had
pp. 275-286, 2007. been working at CEGELY Laboratory in Lyon for
[34] H. Goshima, N. Hayakawa, M. Hikita, H. Okubo, and K. Uchida, 8 years, on the study of silicon power device high
“Area and Volume Effects on Breakdown Strength in Liquid temperature limitations, and on the study of new
Nitrogen”, IEEE Trans. Dielectr. Electr. Insul., Vol. 2, pp. 376-384, SiC power devices. Since 2001, she has been working at the LAPLACE
1995. laboratory in Toulouse. She studies dielectric materials suitable for the
[35] H. Goshima, N. Hayakawa, M. Hikita, H. Okubo, and K. Uchida, insulating environment of high temperature and/or high voltage wide band
“Weibull Statistical Analysis of Area and Volume Effects on the gap semiconductor dies (SiC, GaN and Diamond). She is co-author of 43
Breakdown Strength in Liquid Nitrogen”, IEEE Trans. Dielectr. communications in international scientific reviews, and 50 papers in
Electr. Insul., Vol. 2, pp. 385-393, 1995. international conferences.
[36] K. Kato, X. Han, and H. Okubo, “Insulation Optimization by
Electrode Contour Modification Based on Breakdown Area/Volume Sorin Dinculescu was born in 1971 and obtained
Effects”, IEEE Trans. Dielectr. Electr. Insul., Vol. 8, pp. 162-167, his electrical engineer degree in 1996 from the
2001. "Politehnica" University of Bucharest (Romania).
[37] H. K. Kim and F. G. Shi, “Thickness Dependent Dielectric Strength He joined the Plasma and Energy Conversion
of a Low-permittivity Dielectric Film”, IEEE Trans. Dielectr. Electr. Laboratory at the "Paul Sabatier" University of
Insul., Vol. 8, pp. 248-252, 2001. Toulouse in 1999 as a Research Engineer. His
[38] B. Helgee and P. Bjellheim, “Electric Breakdown Strength of main fields of interest are in power electronics,
Aromatic Polymers: Dependence on Film Thickness and Chemical from both an active devices point of view and
Structure”, IEEE Trans. Electr. Insul., Vol. 26, pp. 1147-1152, 1991. their dielectric environnement. He is particularly
[39] J. H. Stathis, “Percolation Models for Gate Oxide Breakdown”, J. dealing with different high power and/or high
Appl. Phys., Vol. 86, pp. 5757-5766, 1999. voltage characterisation and diagnostic setups and methods.
[40] J. Suñé, “New Physics-Based Analytic Approach to the Thin-Oxide
Breakdown Statistics”, IEEE Electron Device Letters, Vol. 22, pp. Michaël Decup was born at Albi, France in 1982.
296-298, 2001. He received the M.Sc degree in electrical
[41] E. Y. Wu, J. Suñé, and W. Lai, “On the Weibull Shape Factor of engineering from Paul Sabatier Toulouse France
Intrinsic Breakdown of Dielectric Films and Its Accurate University in 2007. At present, he is working at
Experimental Determination—Part II: Experimental Results and the the Plasma and Energy Conversion Laboratory in
Effects of Stress Conditions”, IEEE Trans. Electron Devices, Vol. 49, order to obtain the Ph.D. degree in electrical
pp. 2141-2150, 2002. engineering. He belongs to the Dielectric
[42] S. Diaham, M. L. Locatelli, and T. Lebey, “High Temperature Materials and Energy Conversion team. His main
Dielectric Behavior of Al/Polyimide/Al Capacitor Structures”, IEEE research interest is to analyze the impact of
Vonf. Electr. Insul. Dielectr. Phenomena (CEIDP), pp. 97-100, 2006. fabrication and assembly technologies on the dielectric properties of
ceramic substrates used in power electronic applications.

Sombel Diaham was born in Montauban, France, Thierry Lebey (M’98) received the M.Sc. degree
in 1982. He received the M.Sc. and Ph.D. degrees in solid state physics in 1984, his Ph.D. in
in electrical engineering, respectively in 2005 and electrical engineering in 1989, both from
2007, both from the Paul Sabatier University of University Paul Sabatier in Toulouse. Since 1990,
Toulouse, France. In 2005, he joined the he is engaged with the French National Scientific
LAPLACE laboratory in Toulouse where he has Research Center (CNRS) where he is now Senior
been since 2008 an Associate-Professor. His Research Scientist. He is the author of more than
current research fields focus on the study of 60 journal and 100 conference papers and holds 8
dielectric materials for the insulating international patents.
environment (passivation and encapsulation) of high temperature and/or
high voltage wide band gap semiconductor power devices (SiC, GaN and
Diamond). His fields of interest cover from both the study of the physical
properties of insulating materials and their reliability in high temperature,
up to the study of their impact on the electrical characteristics of the
devices. He is co-author of 6 communications in international scientific
reviews and 8 papers in international conferences.

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