Liu 2019
Liu 2019
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Jing Liu , Jiancang Su, Liang Zhao, Rui Li, Yuanrong Lu, and Xiaolong Liu
© 2019 Author(s).
Journal of ARTICLE scitation.org/journal/jap
Applied Physics
Jing Liu,1,2,a) Jiancang Su,1 Liang Zhao,1 Rui Li,1 Yuanrong Lu,2 and Xiaolong Liu1
AFFILIATIONS
1
Science and Technology on High Power Microwave Laboratory, Northwest Institute of Nuclear Technology, Xi’an,
Shaanxi 710024, China
2
State Key Laboratory of Nuclear Physics and Technology, Peking University, Beijing 100871, China
a)
Electronic mail: [email protected]
ABSTRACT
Dielectric constant and dielectric strength are two intrinsic electrical parameters of solid insulating materials. In order to finally understand
the relationship between them, the one-sided influence of dielectric constant on dielectric strength is investigated. For theoretical analysis,
we propose that the influence is realized indirectly by two mechanisms: defect discharge in the micro level and molecular polarization in the
nanoscale. The transition phase is composed of the field enhancement related to permittivity and the breakdown of defect molecular bond.
While the local field around the bond is always higher than the cavity interior field, the breakdown field is a competition between the two
mechanisms. According to the simulation model of electrostatic field, the electric field around the cavity is significantly enhanced with a
larger dielectric constant. In view of the simulation result of partial discharge, the discharge intensity of dielectric and gas breakdown in the
cavity is promoted by the increase of material permittivity. To confirm the defect distribution and quantity, several prepared samples are
scanned with the ultrasonic microscope and the cavities are measured via image software. Based on the published experiment data from
oxide films and polymer bulks, a revised relationship is plotted and fitted for the dielectric strength and the dielectric constant. As molecular
polarization is applicable to oxide films with few defects and high permittivities, defect discharge is more effective for polymer bulks with
generous cavities and low permittivities. Since molecular polarization leads to breakdown by enhancing the local electric field, cavity dis-
charge is mainly due to the lower breakdown threshold of defect.
I. INTRODUCTION solid insulation materials, few studies have been published on the
relationship between them.
Solid dielectric is widely used in electrical equipments, elec-
tronic components, pulsed power generators, and other fields for In the classical solid dielectric theory, breakdown is mainly
divided into four forms: electrical, thermal, electromechanical, and
insulation. The dielectric strength of polymers determines the
electrochemical. For the ideal solid dielectric, a proposed model
volume, life, and stability of insulators in the electric power indus-
suggests that the local electric field tends to weaken polar molecular
try and pulsed power technology.1,2 The breakdown strength of bonds and causes breakdown.5,6 To practical insulation materials,
thin oxide films has historically been of great reliability interest in defects such as cavities, impurities, and dislocation are usually
integrated circuit applications.3,4 There are a lot of related studies spread inside, which will obviously reduce the dielectric strength.7,8
on the breakdown characteristics and life evaluation of polymer If the dielectric is subjected to an electric field, a tiny leakage
insulators with a low dielectric constant. Besides, the breakdown current is generated and partial discharge will occur at interior
and the reliability of gate dielectrics with high permittivity in oxide defects.9 Because partial discharge is one of the main reasons for
films have been studied in detail. Although dielectric constant and dielectric deterioration and damage, we believe that defects should
dielectric strength are two intrinsically important parameters of be considered. When an external electric field is applied, all
molecules in the material are polarized synchronously and electrons emission (Fowler-Nordheim tunneling) begins to contribute a signifi-
are ionized, accelerated, or recombined. Since dielectric breakdown cant emission current13
is a phenomenon of electronic instability in the electrical break- pffiffiffiffiffiffiffiffiffiffi 3=2 !
down theory, polarization is another essential mechanism. 4 2qm* wB
J f ¼ qvR n exp : (2)
In this paper, the influence of dielectric constant on dielectric 3 h E
strength is investigated, while the effect of dielectric strength on
dielectric constant is not mentioned. First, the defects breakdown Here, V a is the applied voltage and V t is the thermal voltage. wB is
mechanism, the cavity partial discharge, and the molecular polari- the barrier height, l is the barrier distance, and the average field E
zation process are discussed for theoretical analysis. Then, the sim- equals wB =l. The Richardson velocity with which the electrons
ulation results of the electrostatic field and the discharge pulse approach the barrier is obtained from
inside the cavity are presented with different material permittivities. rffiffiffiffiffiffiffiffiffi
kT
Finally, the ultrasonic inspection of the polymer and fitting of vR ¼ : (3)
experimental data are carried out to verify the existence of the 2πm
cavity and influence of permittivity. Equations (1) and (2) prove that the current is the product of the
carrier properties (charge q, velocity vR , and available density n) and
the emission probability of the exponential term. These mechanisms
II. THEORETICAL ANALYSIS of electron injection also exist at the interface of cathodes and dielec-
A. Local breakdown of defects trics.14,15 As the discharge of the metal impurity is essentially the
breakdown of the surrounding material, its initial electric field of dis-
Due to the air permeability of material, the cavity in the
charge is also larger than the gas impurity. If the dielectric strength
polymer is always filled with gas. As a result of the preparation
of the gas is considered lower than that of the liquid and solid, then
environment, the cavity in the oxide gate dielectric is vacuum. In
gas impurity is the most vulnerable to breakdown.10
addition to the cavity, there are a little moisture and metal impuri-
ties remaining in the dielectric generally.10 Unlike the cavity which
is difficult to eliminate, drying is effective in removing the moisture, B. Partial discharge of cavity
and metal detritus will be reduced by improved processing technic. Altogether, it is reasonable to use the cavity to represent all
Dislocation is another defect that exists widely in natural and artifi- defects in a quantitative breakdown model. For a typical gas-filled
cial solid dielectrics. Since dislocation changes the local structure of cavity, the initial electric field of partial discharge is determined by
the material, it is regarded as a nonmetallic impurity with different the breakdown threshold of gas. According to Paschen’s curve, the
physical properties from the dielectric.11 Thus, most of the defects breakdown electric field of gas is described by16,17
can be dealt with impurities of gas, liquid, and solid, in order to
make a comparison in a consistent model. Vgas Bp
Egas ¼ ¼ : (4)
The dielectric constant of gas impurities is very small and the d ln (Apd) ln [ ln (1 þ 1=γ)]
increase of a local electric field by molecular polarization is negligi-
ble. But the polarized charges at the interface of the cavity and the Here, V gas is the gas breakdown voltage, d is the gap distance, p is
dielectric result in the electric fields in the gas to be greater than the pressure, γ is the secondary electron emission coefficient, A is
the surrounding material. The dielectric constant of liquid impuri- related to the saturation ionization, and B involves the excitation
ties (generally moisture) is higher than most solid dielectrics except and ionization energies.
for oxides. Although the overall electric field inside the liquid is not In fact, there are various shapes of cavities in materials, but all
apparently enhanced by polarized charges, the local electric field is of them can be approximated as ellipsoidal cavities.7,9 It is natural
greatly improved by molecular polarization. For dislocation which to define the electric potential at the origin of the ellipsoidal cavity
is handled by the nonmetallic solid impurity, its relative permittiv- as zero. The principal axes of the ellipsoidal cavity (a, b, c) are
ity and internal electric field are close to the original dielectric. assumed to lie on the Cartesian axis (x, y, z), respectively. In order
Generally speaking, the qualitative comparison shows that the elec- to analyze the effect of defects separately, the applied electric field
tric fields in the gas and liquid impurities are greater than the non- in the dielectric is supposed to be uniform. Generally, this exter-
metallic solid impurity and the dielectric. nally applied field ~ E0 equals the electrodes voltage U 0 divided by
But the influence of metal impurity is quite different from the the dielectric thickness d0 . Therefore, the electric potential distribu-
above types as it brings partial discharge around the impurity rather tion of a single cavity inside the dielectric is derived with Laplace
than its interior. On the one hand, the metal impurity distorts the equation and boundary conditions as
electric field nearby, and on the other hand, its free electrons ε2 E0x x ε2 E0y y ε2 E0z z
are injected into the dielectric. When strengths of the electric field are wcav ¼ ,
ε2 þ (ε1 ε2 )na ε2 þ (ε1 ε2 )nb ε2 þ (ε1 ε2 )nc
lower than about 100 kV=mm1 , thermal emission (the Richardson-
(5)
Dushman effect) is relatively accurate with a current of 12
ð1
w Va abc dμ
Jt ¼ qvR n exp B exp 1 : (1) nv ¼ pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi (v ¼ a, b, c),
Vt Vt 2 0 ( μ þ a ) þ ( μ þ b2 ) þ (μ þ c2 )(μ þ v2 )
2
1
For electric field strengths higher than 100 kV=mm , field electron (6)
where ε1 and ε2 are the dielectric constants of the cavity and mate- In the study of breakdown characteristics of polymer speci-
rial, E0x , E0y , and E0z are the components of uniform electric field mens, another breakdown criterion related to hole capture is pro-
~
E0 . Besides, nv (v = a, b, c) is the shape factor of the ellipsoidal posed.20 The free electron in the dielectric is accelerated by the
cavity, which is determined only by the length of three principal externally applied electric field within a distance of the mean free
axes. In particular, the shape factor equals 1/3 for a spherical cavity path λ. If the electron is captured by a hole and its obtained kinetic
(a ¼ b ¼ c), which happens to coincide with the common L ¼ 1=3 energy satisfies ΔH 0 , the molecular bond will break off. The differ-
for a Lorentz spherical cavity. For convenience, the applied electric ence between these two criteria is that p0 in Eq. (11) is replaced by
field ~ E0 is supposed to follow the direction of x axis and eλ. Hence, the dielectric strength decreases with the increase of the
E0y ¼ E0z ¼ 0. As the dielectric constants of the cavity and vacuum dielectric constant, which is verified in several polymer materials
are about the same, the electric field distribution inside the cavity is including PTFE, PMMA, Nylon, and PE.21
solved as9
~ 1 ~ D. Comparison of two mechanisms
Ecav ¼ rwcav ¼ E0 : (7)
1 þ (ε1
r 1)na
Based on Eqs. (7) and (9), two field enhancement factors are
However, Eq. (7) is solved for a single cavity which is located in an defined as f cav ¼ Ecav =E0 and f loc ¼ Eloc =E0 , which are indepen-
infinite uniform electric field. Then, the details of the cavity size dent of the uniform applied electric field ~ E0 . As the factors are
and the dielectric thickness are lost. When the relative size of the expressed as functions of the relative permittivity εr , they are
cavity and dielectric is introduced later, Eq. (7) will be applicable to plotted with na ¼ L ¼ 1=3 in Fig. 1(a). Along with the increasing
both the cavity shape and size. Based on Eqs. (4) and (7), the crite- of relative dielectric constant εr , f cav gradually approaches the limit
rion for cavity partial discharge in a dielectric is given by of 1.5, while f loc grows continuously and linearly. Only if εr equals
1, the field enhancement factors f cav and f loc are the same. But it
Ebd ¼ [1 þ (ε1
r 1)na ]Egas : (8) is unpractical for the natural and artificial solid insulation material.
The occurrence of cavity discharge is usually accompanied by the Thus f loc of molecular polarization is always beyond f cav of cavity
formation of small channels. Once the electrical tree structure ulti- discharge at any relative dielectric constant εr . When applied with
mately bridges the electrodes, the material loses its insulation the same external field ~ E0 , the electric field around polar molecular
capability. bond ~ Eloc in the nanoscale is much larger than the interior of the
cavity ~ Ecav in the micrometer level. It should be pointed out that
f cav in the actual cavity is directly related to the cavity size. Because
C. Polarization process of molecules no infinite dielectric really exists as the hypothesis in Eq. (7). Due
According to the Lorentz relation or the Mossotti field, the to the boundary conditions of dielectric, f cav is affected by the rela-
local electric field ~
Eloc in homogeneous and isotropic dielectrics is a tive size of the cavity and dielectric.
superposition of the externally applied field ~E0 and the dipolar field However, the breakdown electric fields of these two mechanisms
due to the polarization ~ P. In general, the local electric field is exhibit another trend as Fig. 1(b) shows. From Eqs. (8) and (11), it is
expressed as obvious that the breakdown field (dielectric strength) is influenced by
the dielectric constant. Besides, the breakdown criteria of cavity dis-
Eloc ¼ ~
~ E0 þ L(~
P=ε0 ) ¼ [1 þ (εr 1)L]~
E0 , (9) charge and molecular polarization are very similar in the mathemati-
cal form. With Egas ¼ 43:6 kV=mm at the inflexion of Paschen’s
where εr is the relative dielectric constant and L is the Lorentz
curve and ΔH 0 = p0 ¼ 2000 kV=mm for Pr2 O3 , the breakdown crite-
factor.18 Since the factor is initially calculated by a Lorentz spheri-
ria are compared. Because the increase of f cav is little when εr
cal cavity, L ¼ 1=3 has long been used for both cubic-symmetry
exceeds 10, the breakdown electric field stays near 30 kV/mm. The
and amorphous dielectrics. As the local electric field increases with
influence of εr on Ebd mainly operates at a low dielectric constant
the dielectric constant, the polar molecular bonds will be distorted
(,10) by the cavity discharge mechanism. Since f loc is proportional
and weakened in high permittivity materials, then becomes very
to εr , the breakdown electric field decreases sharply with the increase
susceptible to breakage by standard Boltzmann process.5 While the
of the dielectric constant. Then, εr owns an important effect on Ebd
bond strength in the absence of field is ΔH 0 , the enthalpy of activa-
via the molecular polarization mechanism to all dielectric constants.
tion (activation energy) ΔH in the presence of field is reduced by
A specific relative dielectric constant is defined as εc , where
ΔH ¼ ΔH0 p0 Eloc , (10) the influences of both mechanisms on breakdown field are the
same. Although ~ Eloc is far higher than ~ Ecav , the cavity is more easier
where p0 is the molecular dipole moment component opposite to to breakdown than the molecular bond if εr , εc . The reason is
~
Eloc . Bond breakage is expected when the activation energy ΔH that Egas is just about 1/40 of ΔH 0 = p0 , which counteracts the
tends to zero, which is one of the criteria for breakdown advantage of polarization over discharge in the electric field. The
ΔH0 breakdown threshold of the cavity and the molecular bond is more
Ebd ¼ [1 þ (εr 1)L]1 , (11) decisive in this low permittivity region. When εr is over εc , Ebd of
p0
the molecular polarization process is smaller than cavity partial
where Ebd is the dielectric strength (breakdown field).19 Once the discharge. The mechanism of molecular polarization and the
molecular bond breaks, an associated defective site is thought to be influence of field enhancement begin to play a leading role. The
formed and a conductive percolation path of defect grows with time. factor f loc is strong enough to overcome the impact of low
FIG. 2. Geometry and mesh of electrostatic field model via the CST EM Studio:
(a) polymer sample and Bruce electrodes, (b) section view from y direction, and
(c) meshed spherical cavity.
compared with the calculation result in Fig. 1(a). During the elec-
trostatic field simulation, the physical parameters of dielectrics
(conductivity, inductivity, loss angle, etc.) are consistent except per-
mittivity. But the molecular polarization of the nanoscale is too
small to be simulated with current electromagnetic software.
Moreover, the influence of permittivity on the breakdown field is
analyzed experimentally in Sec. IV, which corresponds to the theo-
retical calculation in Fig. 1(b).
The simulation model is reconstructed in equal proportion
according to our improved system for the cavity experiment. The
geometry of the electrostatic field model is composed of two Bruce
εr 1 2 3 4 5
f acav 1 1.2 1.28571 1.33333 1.36364
f bcav 1 1.18087 1.25664 1.29830 1.32465
f ccav 1 1.1998 1.2855 1.3330 1.3633
f dcav 1 1.1999 1.2855 1.3331 1.3634
a
Calculated by Eq. (7).
b
Simulated by CST EMS for electrostatic field model.
c
Simulated by Comsol for partial discharge model (AC).
d
Simulated by Comsol for partial discharge model (pulse).
which accumulated on the cavity surface. Since Einc is the initial elec-
tric field of gas in the cavity like Egas , the change is not obviously
compared with other parameters. In particular, the factor fcav
obtained by Ecav0 =E0 in the partial discharge model is identical to
the electrostatic field model as Table I shows. Meanwhile, the dis-
charge quantity parameters (total for 10 cycles Qcharge and mean for
per cycle Qmax , Qmin ) are also increased gradually. Besides, the max
and mean cavity temperature T cav shows a similar trend for both AC
and pulse voltage. As a result, cavity partial discharge becomes more
intense if the relative permittivity increases. While cavity is the main
source of material partial discharge, the dielectric is more likely to
breakdown when the dielectric constant gets larger.
TABLE III. Dielectric constant and dielectric strength of some polymers from
Ref. 24.
εr Ebd
Material Type (106 Hz) (kV/mm)
Polyethylene Low density 2.3 22.8
Polypropylene Pure 2.3 30
Polymethyl Pure 2.95 19.65
methacrylate
Polymethyl α-Methylstyrene 3.03 18.7
methacrylate
Polymethyl ACS 3.01 21.7
methacrylate
Polyvinyl chloride Hard 2.325 26.5
Polystyrene General 2.525 23.6
Polycarbonate Pure 2.54 19.5
Polycarbonate 25% glass fiber 3.17 22
Polyformaldehyde Pure 3.56 18.6
Chlorinated Pure 3.1 18.3
polyether
Polyamide resin Nylon 1010 3.1 20
Polyamide resin Nylon 6 3.4 20
Polyamide resin Nylon 610 2.98 20
Polyamide resin MC-Nylon 3.7 19.1
Polyamide resin 40% glass fiber 3.1 23
Fluorinated resin Polytetrafluoroethylene 2.1 32.5
Fluorinated resin Polytrifluorochloroethylene 2.5 19.7
Phenolic resin Wood powder filling 9 12.95
Urea α-cellulose filling 8.25 13.75
formaldehyde
resin
Alkyd resin Inorganic filling 6.3 15.7
Alkyd resin Glass fiber filling 6.6 15.3
Diallyl phthalate Inorganic filling 5.2 16
Diallyl phthalate Glass fiber filling 4.45 16.6
Unsaturated Casted and hard 3.65 17.25
polyester FIG. 7. Variation of the dielectric strength on relative dielectric constant for
Unsaturated Glass fiber filling 4.85 16.65 different solid materials: (a) polymer bulks and (b) oxide films.
polyester
Unsaturated Glass cloth filling 4.8 16.65
polyester
Polyimide Glass fiber filling 3.8 19.6
Polyurethane Pure 5.75 15.7 While the correlations of three fitting methods are matched,
the coefficient of cavity discharge is 0.76 for polymer bulks. In
nearly two decades of dielectric constant, the fitting correlation
coefficients of oxide films are all over 0.83. Theoretical dielectric
strength is the intrinsic property of solid insulation materials. In
only 7%. This consistency demonstrates that the cavity is an impor- practice, the breakdown electric field is related to field, electrode,
tant factor of the breakdown process and dielectric strength for environment, etc. The insulation performance decreases with the
polymers. Because the cavity electric field is related to relative per- increase of sample size, working temperature, AC frequency, and
mittivity, the dielectric constant determines the dielectric strength ambient humidity. Therefore, the breakdown of the solid material
of polymers indirectly. Meanwhile, the practical ΔH 0 = p0 of oxide is such a complex physical phenomenon. There are numerous
films coincides with the fitted one at a difference of 15%. Since concepts, theories, and experimental studies. As cavity discharge
ΔH 0 = p0 is also obtained from two irrelevant ways, molecular polari- and molecular polarization play a part in dielectric strength, the
zation contributes to the dielectric strength of oxides. As the polariza- correlation coefficients are reasonable. Since the dielectric cons-
tion degree is determined with the dielectric constant, the dielectric tant stands out from many factors as Fig. 7 shows, it has an
strength of oxides is indirectly affected by relative permittivity. important influence on dielectric strength.