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Jonscher Indices for Dielectric Materials

Article  in  Journal of Advanced Dielectrics · December 2019


DOI: 10.1142/S2010135X19500462

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JOURNAL OF ADVANCED DIELECTRICS
Vol. 9, No. 6 (2019) 1950046 (5 pages)
© The Author(s)
DOI: 10.1142/S2010135X19500462

Jonscher indices for dielectric materials


C. L. Wang
School of Physics, Shandong University
Jinan 250100, P. R. China
wangcl@sdu.edu.cn
by SHANDONG UNIVERSITY on 02/12/20. Re-use and distribution is strictly not permitted, except for Open Access articles.

Received 28 November 2019; Revised 20 December 2019; Accepted 20 December 2019; Published 23 January 2020
Two parameters are proposed as Jonscher indices, named after A. K. Jonscher for his pioneering contribution to the universal
dielectric relaxation law. Time domain universal dielectric relaxation law is then obtained from the asymptotic behavior of dielectric
response function and relaxation function by replacing parameters in Mittag–Leffler functions with Jonscher indices. Relaxation
types can be easily determined from experimental data of discharge current in barium stannate titanate after their Jonscher indices
are determined.
Keywords: Jonscher indices; universal dielectric relaxation law; barium stannate titanate.
J. Adv. Dielect. Downloaded from www.worldscientific.com

1. Introduction which are the two parameters in the universal dielectric


relaxation law, are proposed.
Understanding dielectric relaxation has taken more than 100
years if it is counted from the theory proposed by Debye in
1912.1 Since then, many efforts have been devoted to fully
2. Jonscher Indices
understanding the relaxation behavior in dielectric materials.
The physics behind the theory developed by Debye is clear The dielectric relaxation of virtually all solids follows
and mathematics of the theory is concise. The results of the fractional power laws in both time and frequency. That is the
theory have been used to explain experimental findings in a so-called universal dielectric relaxation law, which was pro-
good manner. But they can only fit with experimental data in posed by A K Jonscher in 1980s. To formulate the universal
quantitative scale for quite few materials, for instance, cesium dielectric relaxation law, it is customary to define the di-
dihydrogen phosphate.2,3 Therefore, modifications based electric susceptibility χ as a pure complex number as
upon Debye model have been made, i.e., Cole–Cole (C–C),4 ~χ ðωÞ ¼ χ 0 ðωÞ  iχ 00 ðωÞ; ð1Þ
Davidson–Cole (C–D)5 and Havriliak–Nagami (H–N),6 etc.
These empirical expressions imply that there could be more where ω ¼ 2f is the angular frequency and f is the circular
than one relaxation process in real systems. Distribution frequency in Hertz. For frequency ω lower than the loss peak
functions of relaxation time have been assumed. Until now, frequency ωp, the imaginary part of the dielectric suscepti-
the understanding of these complicated distribution functions bility χ 00 can be expressed as
is still a huge challenge.7 χ 00 ’ ðω=ωp Þ m ; ð2Þ
A milestone in understanding of the dielectric relaxation is
the finding of universal dielectric relaxation law.3 By analysis where 0 < m • 1 is a real number. For convenience of dis-
of numerous experimental data in different materials, cussion, m is called as low Jonscher index in this work. For
Jonscher found that there exists universality in dielectric re- frequency ω higher than the loss peak frequency ωp, the
laxation. Since his pioneering work, much progress has been imaginary susceptibility has the form
made, for example, but not limited to, by Stanislavsky and
χ 00 ’ ðω=ωp Þ n1 ; ð3Þ
Weron,8 Nigmatulin et al.9 and Garrappa et al.,10 etc. Now, it
is well known that the fractional kinetics belongs to the do- where 0 < n • 1 is also a real number, and is called as high
main of influence of universal relaxation law.7 Though this Jonscher index. These Jonscher indices can be served as
law has been found in dielectric relaxations during early material parameters, which characterize the intrinsic property
studies, the relaxation universality can be found in many of the dielectric relaxation behavior. It is plausible that
other materials properties, for instance, luminescence and Jonscher indices strongly related with the microstructure of
photoconductivity, chemical reaction kinetics, as well as the materials. A schematic diagram of the Jonscher indices in
mechanical relaxation.11 In this paper, recent progress on the universal dielectric relaxation law in frequency domain is
dielectric relaxation theory is summarized. Jonscher indices, shown in Fig. 1.

This is an Open Access article published by World Scientific Publishing Company. It is distributed under the terms of the Creative Commons Attribution 4.0
(CC BY) License which permits use, distribution and reproduction in any medium, provided the original work is properly cited.

1950046-1
C. L. Wang J. Adv. Dielect. 9, 1950046 (2019)

Table 1. Jonscher indices and parameters in different models.

Model Low Jonscher index m High Jonscher index n

Debye 1 0
C–C α 1α
D–C 1 1γ
H–N α 1  αγ
JWS αγ 1α

1
by SHANDONG UNIVERSITY on 02/12/20. Re-use and distribution is strictly not permitted, except for Open Access articles.

~χ JWS ðωÞ ¼ 1  γ ; ð5Þ


ð1 þ ðiωÞ α Þ
where  is called as relaxation time, α and γ are the model
parameters. The corresponding functions in time domain, i.e.,
relaxation function and response function, have also been
obtained recently.10 The relaxation function, which describes
Fig. 1. Jonscher indices m and n. Solid line is for real part and the decay of polarization, is
dotted dash line for imaginary part of dielectric susceptibility.
γ
HN ðtÞ ¼ 1  ðt=Þ αγ E α;αγþ1 ððt=Þ α Þ; ð6Þ
J. Adv. Dielect. Downloaded from www.worldscientific.com

Jonscher indices diagram is shown in Fig. 2 for different γ


JWS ðtÞ ¼ E α;1 ððt=Þ α Þ; ð7Þ
theoretical models. The standard Debye model is denoted by
Debye, shown as a solid circle. C–D stands for Davidson– γ
where E α; β is called three-parameter Mittag–Leffler function
Cole relaxation, shown as a horizontal line. C–C is for Cole– or Prabhakar function.16 For any z 2 C, this function is
Cole and shown as diagonal line. H–N is for Havriliak– defined as
Negami model, which occupies up-triangle area in Fig. 2. The
lower triangle area is for JWS model, which is a modified γ 1 X 1
Γðγ þ kÞ k
E α; β ðzÞ ¼ z ;
Havriliak–Negami model derived by Jurlewicz et al. in last ΓðγÞ k¼0 k!Γðαk þ βÞ ð8Þ
decade.8,12–15 This model exhibits two-power-law relaxation
α; β; γ 2 C; ReðαÞ > 0;
pattern fairly well in frequency power law with Jonscher
indices m and n satisfying m < 1  n. Generally speaking, where ΓðÞ denotes Euler’s gamma function. For the physical
there are two independent models for dielectric relaxations, acceptability of these models, the complete monotonicity of
i.e., H–N and JWS model. Debye model and C–C model can the response function is essential to ensure the monotone
be regarded as a special case either H–N model or JWS decay of the energy in isolated systems. The Prabhakar
model, and C–D model is a special case of H–N model. function introduced in this paper to describe the response
Then frequency dependence of complex dielectric sus- function that satisfies this property for some range of its
ceptibility for H–N and JWS model is expressed, respec- parameters.17–20 The response function, or the reduced de-
tively, as, polarization current, is
1 1 γ
~χ HN ðωÞ ¼ γ ; ð4Þ HN ðtÞ ¼ ðt=Þ αγ1 E α;αγ ððt=Þ α Þ; ð9Þ
ð1 þ ðiωÞ α Þ 
1 γ
JWS ðtÞ ¼ δðtÞ  ðt=Þ 1 E α;0 ððt=Þ α Þ: ð10Þ

The relation between Jonscher indices [m; n] and model
parameters [α; γ] is summarized in Table 1. This means that
once the Jonscher indices are determined from frequency
function such as dielectric susceptibility, the time dependence
of the polarization and the depolarization current can be
obtained directly.

3. Time Domain Universal Relaxation Law


The universal relaxation law is often presented in form of
frequency domain, such as in Eqs. (1)–(3) and Fig. 1. From
Fig. 2. Jonscher indices diagram for different relaxation models. the asymptotic expansion for short- and long-time scale of

1950046-2
C. L. Wang J. Adv. Dielect. 9, 1950046 (2019)

relaxation function ðtÞ, i.e.,9 Universal relaxation law in time domain of Eq. (16) has
 been obtained by Jonscher11 using Fourier transformation of
ðt=Þ αγ ; t  ;
HN ðtÞ  ð11Þ universal relaxation law in frequency domain, i.e., Eqs. (2)
ðt=Þ α ; t  ;
 and (3). In this work, universal relaxation law in time domain
ðt=Þ α ; t  ; for both discharge current (response function) and polariza-
JWS ðtÞ  ð12Þ
ðt=Þ αγ ; t  ; tion (relaxation function) decay have been obtained from the
asymptotic expansion of these functions. These time domain
both H–N and JWS relaxation can be expressed in a uniform functions have been vigorously proved by Garrapa et al. with
expression when the Jonscher indices defined in Table 1 is fractional calculus technique.9 All of the above results sug-
used, i.e., gest that there could be a unified expression of differential

by SHANDONG UNIVERSITY on 02/12/20. Re-use and distribution is strictly not permitted, except for Open Access articles.

ðt=Þ 1n ; t  ; equation, as well as response and relaxation function, for the
PðtÞ  ðtÞ  ð13Þ
ðt=Þ m ; t  : dielectric relaxation.

Relation of relaxation function ðtÞ being proportional to


the polarization PðtÞ is used in the above equation. This is 4. Discharge in Barium Stannate Titanate
another form of universal dielectric relaxation law in time
domain. It is very interesting to note that n stands for short Dielectric response in time domain or ferroelectric discharge
time or high-frequency response, and m for long time or low- current has been studied in barium stannate titanate (BTS)
frequency response. Similarly, from the asymptotic expansion and lanthanum lead zirconium titanate (PLZT) transparent
J. Adv. Dielect. Downloaded from www.worldscientific.com

of response function ðtÞ as9 ceramic samples.21 A Tikhonov regularization method is


 adopted for derivation of the relaxation time distribution
ðt=Þ αγ1 ; t  ; function from the discharge current. It is found that PLZT
HN ðtÞ  ð14Þ
ðt=Þ α1 ; t  ; discharge current versus time spectra, i.e., the response
 function, exhibit a linear relationship in double logarithm
ðt=Þ α1 ; t  ;
JWS ðtÞ  ð15Þ scale of current and time coordinates. The relation can be
ðt=Þ αγ1 ; t  :
fairly fitted by power law, i.e., IðtÞ ¼ A  t ðmþ1Þ , with m
Also uniform expression for response function, which is between 0.14 and 0.21 at different temperatures. That is the
proportional to the depolarization current IðtÞ, reads experimental evidence of universal relaxation law in long-
 time scale limit.
ðt=Þ n ; t  ;
IðtÞ  ðtÞ  ð16Þ Time domain test is a major experimental mean used to
ðt=Þ m1 ; t  :
study the dielectric relaxation of ferroelectric materials. It is
The universal dielectric relaxation law in time domain is believed that the time domain test has advantage over fre-
schematically shown in Fig. 3 for time-dependent polariza- quency domain test in ultra-low frequency or long-time limit.
tion and depolarization current. A new time domain test system has been developed to in-
vestigate the relaxation phenomena of relaxor ferro-
electrics.22 The electric current span of the signal is up to 10
orders of magnitude that changes from nano-amperes to few
amperes. The time span is up to 12 orders magnitude that
covers from nanoseconds to kilo seconds. The system con-
sists of four segments in accordance with the time range.
The discharge current of BTS has been obtained from the
new system. By fitting the experimental data of current versus
time22 with universal relaxation law in time domain Eq. (16),
Jonscher indices for BTS with different barium/stannate ra-
tios are obtained. The results are listed in Table 2, and the
fitting lines are schematically shown in Fig. 4 for short- and
long-time limits. From the obtained Jonscher indices, it is

Table 2. Jonscher indices for barium stannate titanate.22

Sample Low Jonscher index m High Jonscher index n Relaxation model

BST4 0.27 0.77 H–N


BST8 0.12 0.90 H–N
Fig. 3. Schematic diagram for time domain universal dielectric re- BST225 0.26 0.74 C–C
laxation law. Solid line is for polarization decay and dotted dash line BST275 0.22 0.54 JWS
for depolarization current.

1950046-3
C. L. Wang J. Adv. Dielect. 9, 1950046 (2019)
by SHANDONG UNIVERSITY on 02/12/20. Re-use and distribution is strictly not permitted, except for Open Access articles.

(a) (b)
J. Adv. Dielect. Downloaded from www.worldscientific.com

(c) (d)
Fig. 4. Discharge current in stannate barium titanate samples. Current I in ampere A, and time t in second s. Circles are the experimental data22
and solid lines represent the asymptotic behavior at short- and long-time limits. (a) BTS4, (b) BTS8, (c) BTS225 and (d) BTS275 sample.

easy to identify the relaxation model by checking the position the dielectric materials. The relation between Jonscher indi-
in Fig. 2 of Jonscher indices diagram. These are listed in the ces and parameters in different dielectric relaxation models is
last column in Table 2. It can be seen that dielectric relaxation also given. As an example, Jonscher indices of barium stan-
in BTS4 and BTS8 can be described by H–N model, BTS225 nate titanate are obtained.
by C–C model and BTS275 by JWS model. Also model
parameters [α; γ] in different models can be obtained from
Table 1 with simple algebra work. Hence, dielectric function Acknowledgments
in frequency domain can be obtained with these parameters.
This work is supported by the National Natural Science
Foundation of China (51672159, 51501105, 51611540342).
Author of this work would like to thank Prof. Wei Xiaoyong of
5. Summary Xian Jiaotong University for provide the experimental data.
The two parameters in universal relaxation law are proposed
as Jonscher indices. Low Jonscher index describes the be-
havior at low-frequency or long-time limit, while high References
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1950046-4
C. L. Wang J. Adv. Dielect. 9, 1950046 (2019)

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