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Dielectrics in

Electric Fields
Gorur G. Raju
University of Windsor-
Windsor, Ontario, Canada

MARCEL

MARCELDEKKER,
INC. NEWYORK BASEL
DEKKER
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POWER ENGINEERING

Series Editor
H. Lee Willis
ABB Inc.
Raleigh, North Carolina

1. Power Distribution Planning Reference Book, H. Lee Willis


2. Transmission Network Protection: Theory and Practice, Y. G. Paithan-
kar
3. Electrical Insulation in Power Systems, N. H. Malik, A. A. AI-Arainy,
and M. I. Qureshi
4. Electrical Power Equipment Maintenance and Testing, Paul Gill
5. Protective Relaying: Principles and Applications, Second Edition, J.
Lewis Blackburn
6. Understanding Electric Utilities and De-Regulation, Lorrin Philipson
and H. Lee Willis
7. Electrical Power Cable Engineering, William A. Thue
8. Electric Systems, Dynamics, and Stability with Artificial Intelligence
Applications, James A. Momoh and Mohamed E. EI-Hawary
9. Insulation Coordination for Power Systems, Andrew R. Hileman
10. Distributed Power Generation: Planning and Evaluation, H. Lee Willis
and Walter G. Scott
11. Electric Power System Applications of Optimization, James A. Momoh
12. Aging Power Delivery Infrastructures, H. Lee Willis, Gregory V. Welch,
and Randall R. Schrieber
13. Restructured Electrical Power Systems: Operation, Trading, and Vola-
tility, Mohammad Shahidehpour and Muwaffaq Alomoush
14. Electric Power Distribution Reliability, Richard E. Brown
15. Computer-Aided Power System Analysis, Ramasamy Natarajan
16. Power System Analysis: Short-Circuit Load Flow and Harmonics, J.
C. Das
17. Power Transformers: Principles and Applications, John J. Winders, Jr.
18. Spatial Electric Load Forecasting: Second Edition, Revised and Ex-
panded, H. Lee Willis
19. Dielectrics in Electric Fields, GorurG. Raju
20. Protection Devices and Systems for High-Voltage Applications,
Vladimir Gurevich

ADDITIONAL VOLUMES IN PREPARATION

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TO MY PARENTS.
MY WIFE, PADMINI,
AND OUR SON, ANAND

WHO GA VE ME ALL I VALUE. SOME DEBTS


ARE NEVER REPAID IN FULL MEASURE.

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SERIES INTRODUCTION

Power engineering is the oldest and most traditional of the various areas within
electrical engineering, yet no other facet of modern technology is currently undergoing a
more dramatic revolution in both technology and industry structure. This addition to
Marcel Dekker's Power Engineering Series addresses a fundamental element of
electrical engineering. Dielectric materials are a key element of electric power
engineering, one of the most challenging aspects of improving reliability and economy
of materials. For an industry pressed hard to increasingly cram more equipment
capacity into ever-tighter spaces, to improve reliability, particularly mean time between
failures, modern dielectric materials and engineering methods provide a valuable tool to
meet these challenges.
Dielectrics in Electric Fields is a well-organized and comprehensive view of both the
theory behind and application of dielectric materials in power equipment, industrial
equipment, and commercial appliances. At both the introductory and advanced levels, it
provides both a solid foundation of theory, fact, nomenclature, and formula, and sound
insight into the philosophies of dielectric engineering techniques and their use. Its
unifying approach, based on both physics and engineering, makes it useful as a day-to-
day reference as well as an excellent tutorial: the book begins with a thorough review of
the basics of dielectric and polymer science and builds upon it a comprehensive and very
broad presentation of all aspects of modern dielectric theory and engineering, including
the lastest analysis and modeling techniques.
As the editor of the Power Engineering Series, I am proud to include Dielectrics in
Electric Fields among this important group of books. Like all the volumes planned for
the series, Professor Raju's book puts modern technology in a context of proven,
practical application; useful as a reference book as well as for self-study and advanced

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classroom use. The series includes books covering the entire field of power engineering,
in all its specialties and sub-genres, all aimed at providing practicing power engineers
with the knowledge and techniques they need to meet the electric industry's challenges
in the 21 st century.

H. Lee Willis

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PREFACE

Materials that do not normally conduct electricity and have the ability to store
electrical charge are known as dielectrics. The behavior of dielectrics in electric fields
continues to be an area of study that has fascinated physicists, chemists, material
scientists, electrical engineers, and, more recently biologists. Ideas that explain aspects of
dielectric behavior in high voltage electrical cables are also applicable to the insulating
barrier in metal oxide semiconductors or interlayer insulation of integrated circuits.
Microwave drying of milk, dielectric properties of agricultural products such as flour and
vegetable oils to determine their moisture content, and the study of curing of cement etc.,
are some nontraditional applications of dielectric studies that show potential promise.
Deeper insight into the interaction between electric fields and molecules has resulted in
many new applications. Power engineers are interested in the study of insulating
materials to prolong the life of insulation and determine the degree of deterioration in
service to plan for future replacements or service maintenance.
Polymer scientists are interested in understanding the role of long chain molecules
in varied applications ranging from heat resistant dielectrics to selfrepairing plastics. The
intensity of research in this area, after a brief respite, has resumed at a furious pace, the
published literature expanding at a rate faster than ever. Advances in instrumentation and
theoretical models have also contributed to this renewed interest.
Organic polymers are considered to be stable materials at high temperatures and
have the ability to withstand radiation, chemical attacks, and high electrical and
mechanical stresses, making them suitable for extreme operating environments as in a
nuclear power plant or in outer space. Polymer materials have the ability to store
electrical charges. Like a diamond-studded sword, this property is wholly undesirable in
applications such as electrical equipment and the petrochemical industry; yet it is a
sought-after property in applications such as photocopying and telephones.

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This book explains the behavior of dielectrics in electric fields in a fundamentally
unifying approach that is based on well-established principles of physics and
engineering. Though excellent monographs exist on specialized topics dealing with a
relatively narrow area of interest, there is a need for a broader approach to understand
dielectrics. It has evolved out of graduate lectures for nearly thirty-five years at the
Indian Institute of Science, Bangalore (1966-1980) and the University of Windsor,
Windsor, Ontario, Canada (1980-2002). The probing questions of students has helped the
author to understand the topics better and to a certain extent dictated the choice of topics.

The book begins with an introductory chapter that explains the ideas that are
developed subsequently. The calculation of forces in electric fields in combinations of
dielectric media is included because it yields analytical results that are used in the study
of the dielectric constant (Ch. 2). The band theory of solids is included because it is
required to understand the energy levels of a dielectric, as in the conduction and
formation of space charge (Ch. 6-11). The energy distribution function is dealt with
because it is a fundamental property that determines the swarm parameters in gaseous
breakdown and partial discharges (Ch. 8-9).
Chapter 2 deals with the mechanisms of electrical polarization and their role in
determining the value of the dielectric constant under direct voltages. Expressions for
the dielectric constant are given in terms of the permanent dipole moment of the
molecule and temperature. Several theories of dielectric constant are explained in detail
and practical applications are demonstrated. Methods of calculating the dielectric
constant of two different media and mixtures of liquids are also demonstrated.
Chapter 3 begins with the definitions of the complex dielectric constant in an
alternating electric field. The Debye equations for the complex dielectric constant are
explained and the influence of frequency and temperature in determining the relaxation
is examined. Functions for representing the complex dielectric constant in the complex
plane are given and their interpretation in terms of relaxation is provided. Several
examples are taken from the published literature to bring out the salient points.
Chapter 4 continues the discussion of dielectric relaxation from chapter 3. The
concept of equivalent circuits is introduced and utilized to derive the set of equations for
both Debye relaxation and interfacial polarization. The absorption and dispersion
phenomena for electronic polarization are considered, both for damped and undamped
situations. These ideas have become very relevant due to developments in fiber optics
technology.
Chapter 5 deals with the application of these ideas to understand the experimental
results in the frequency domain and with temperature as the main parameter in selected
polymers. A brief introduction to polymer science is included to help the reader
understand what follows. The terminology used to designate relaxation peaks is

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explained and methods for interpreting observed results in terms of physics and
morphology are presented.
Chapter 6 deals with the measurement of absorption and desorption currents in the
time domain in polymers. Though external parameters influence these measurements our
concern is to understand the mechanisms of charge generation and drift. Time domain
currents may be transformed into the frequency domain complex dielectric constant and
the necessary theories are explained. The low frequency, high temperature relaxations
observed in several polymers are explained as complementary to the topics in Chapter 5.
The magnitude of electric fields that are employed to study the behavior in
dielectrics outlined in Chapters 1-6 is low to moderate. However, the response of a
polymer to high electric fields is important from the practical point of view. The
deleterious effects of high electric fields and/or high temperatures occur in the form of
conduction currents and the complex mechanism of conduction is explained in terms of
the band picture of the dielectric. Several examples are selected from the published
literature to demonstrate the methods of deciphering the often overlapping mechanisms.
Factors that influence the conduction currents in experiments are outlined in Chapter 7.
Chapters 8 deals with the fundamental processes in gaseous electronics mainly in
uniform electric fields and again, due to limitation of space, physical principles are
selected for discussion in preference to experimental techniques for measuring the cross
sections and swarm properties. A set of formulas for representing the relevant properties
of several gases, such as the swarm coefficients are provided, from recent published
literature.
Chapter 9 is devoted to studies on nonuniform electric field in general and corona
phenomenon in particular. These aspects of gaseous breakdown are relevant from
practical points of view, for providing better design or to understand the partial discharge
phenomena. Both experimental and theoretical aspects are considered utilizing the
literature published since 1980, as far as possible. Several computational methods, such
as the Boltzmann equation, solutions of continuity equations, and Monte Carlo methods
are included. The results obtained from these studies are presented and discussed.
Chapter 10 deals with thermally stimulated processes, mainly in polymers. The
theory of thermally stimulated discharge currents and techniques employed to identify
the source of charge generation are described to assist in carrying out these experiments
Chapter 11 deals with measurement of the space charges in solids and the different
experimental techniques are explained in detail. These nondestructive techniques have
largely replaced the earlier techniques of charging a dielectric and slicing it for charge
measurements. The Theory necessary to analyze the results of space charge experiments
and results obtained is included with each method presented. The author is not aware of
any book that systematically describes the experimental techniques and the associated
theories in a comprehensive manner.

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The book uses the SI units entirely and published literature since 1980 is cited,
wherever possible, except while discussing the theoretical aspects. The topics chosen for
inclusion has my personal bias, though it includes chapters that interest students and
established researchers in a wide range of disciplines, as noted earlier. Partial discharges,
breakdown mechanisms, liquid dielectrics, Outdoor insulation and nanodielectrics are
not covered mainly due to limitation of space.
I am grateful to a number of graduate students who contributed substantially for a
clearer understanding of the topics covered in this volume, by their probing questions.
Drs. Raja Rao, G. R. Gurumurthy, S. R. Rajapandiyan, A. D. Mokashi, M. S. Dincer,
Jane Liu, M. A. Sussi have contributed in different ways. I am also grateful to Dr.
Bhoraskar for reading the entire manuscript and making helpful suggestions. It is a
pleasure to acknowledge my association with Drs. R. Gorur, S. Jayaram, Ed Churney, S.
Boggs, V. Agarwal, V. Lakdawala, T. Sudarshan and S. Bamji over a number of years.
Dr. R. Hackam has been an associate since my graduate student years and it is
appropriate to recall the many discussions I have held on various aspects of dielectric
phenomena considered in this book. The personal encouragement of Professor Neil Gold,
University of Windsor has contributed in no small measure to complete the present book.
Special thanks are due to Dr. N. Srinivas who provided opportunity to complete
chapters 8 and 9 during sabbatical leave. Prof. C. N. R. Rao, President of the Jawaharlal
Nehru Center for Advanced Scientific Research provided opportunity to spend sabbatical
leave during which time I could work on the manuscript. Mr. N. Nagaraja Rao extended
generous hospitality on campus making it possible to use the library facilities in
Bangalore.
This book would not have been completed without the help of Mr. S. Chowdhury
who showed me how to make software applications cooperate with each other.
Extraordinary help was provided by Alan Johns in keeping the computer system in
working condition throughout. Ms. S. Marchand assisted in checking the manuscript and
Ms. Ramneek Garewal assisted in the compilation of figures and tables. While
acknowledging the help received, I affirm that errors and omissions are entirely my own
responsibility.
I have made sincere attempts to secure copyright permission for reproducing every
figure and table from the published literature, and acknowledge the prompt response
from institutions and individuals. If there are unintentional failures to secure permission
from any source, I render apology for the oversight.
Personal thanks are due to Brian Black and B. J. Clark who have patiently suffered
my seemingly disconnected communications and, provided great assistance in improving
the style and format. Finally the inexhaustible patience of my wife Padmini has been a
source of continuous strength all these years.

Gorur G. Raju

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CONTENTS

Series Introduction
Preface

Chapter 1
Introductory Concepts
1.1 A dipole
1.2 The potential due to a dipole
1.3 Dipole moment of a spherical charge
1.4 Laplace's equation
1.4.1 A dielectric sphere immersed in a different medium
1.4.2 A rigid dipole in a cavity within a dielectric
1.4.3 Field in a dielectric due to a conducting inclusion
1.5 The tunneling phenomenon
1.6 Band theory of solids
1.6.1 Energy bands in solids
1.6.2 The Fermi level
1.6.3 Electron emission from a metal
1.6.4 Field intensification factor
1.7 Energy distribution function
1.8 The Boltzmann factor
1.9 A comparison of distribution functions
1.10 References

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Chapter 2
Polarization and Static Dielectric Constant
2.1 Polarization and dielectric constant
2.2 Electronic polarization
2.3 The internal field
2.4 Orientational polarization
2.5 Debye equations
2.6 Experimental verification of Debye equation
2.7 Spontaneous polarization
2.8 Onsager's theory
2.9 Theory of Kirkwood
2.10 Dielectric constant of two media
2.10.1 Raleigh's formula
2.10.2 Wiener's formula
2.10.3 Formula of Lichtenecker and Rother
2.10.4 Goldschmidt's Equation
2.11 The dissipation factor
2.12 Dielectric constant of liquid mixtures
2.12.1 Raleigh's formula
2.12.2 Formula of Meredith and Tobias
2.12.3 Bruggeman' s formula
2.12.4 Looyenga's formula
2.12.5 Bottcher's formula
2.13 Effect of high electric fields
2.14 Atomic polarizability
2.15 References

Chapter 3
Dielectric Loss and Relaxation-!
3.1 Complex permittivity
3.2 Polarization build up
3.3 Debye equations
3.4 Bi-stablemodelofadipole
3.5 Complex plane diagram
3.6 Cole-Cole relaxation
3.7 Dielectric properties of water
3.8 Davidson-Cole equation
3.9 Macroscopic relaxation time
3.10 Molecular relaxation time
3.11 Straight line relationships

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3.12 Frohlich's analysis
3.13 Fuoss-Kirkwood equation
3.14 Havriliak and Negami dispersion
3.15 Dielectric susceptibility
3.16 Distribution of relaxation times
3.17 Kramer-Kronig relations
3.18 Loss factor and conductivity
3.19 References

Chapter 4
Dielectric Loss and Relaxation-ll
4.1 Jonscher' s universal law
4.2 Cluster approach of Dissado-Hill
4.3 Equivalent circuits
4.3.1 A series equivalent circuit
4.3.2 Parallel equivalent circuit
4.3.3 Series-parallel circuit
4.3.4 Summary of simple equivalent circuits
4.4 Interfacial polarization
4.5 The Absorption phenomenon
4.6 Frequency dependence of s*
4.7 References

Chapter 5
Experimental Data (Frequency Domain)
5.1 Introduction to polymer science
5.1.1 Classification of polymers
5.1.2 Molecular weight and size
5.1.3 Glass transition temperature
5.1.4 Crystallinity of polymers
5.1.5 Thermally stable groups
5.1.6 Polymer degradation and defects
5.1.7 Dipole moment of polymers
5.1.8 Molecular structure
5.2 Nomenclature of Relaxation Processes
5.3 Non-Polar Polymers
5.3.1 Polyethylene
5.3.2 Poly(tetrafluoroethylene)
5.4 Polar Polymers

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5.4.1 Polypropylene
5.4.2 Poly(vinyl chloride)
5.4.3 Polychlorotrifluoroethylene
5.4.4 Polycarbonate
5.4.5 Poly(methyl methacrylate)
5.4.6 Poly(vinyl acetate)
5.4.7 Polystyrene
5.4.8 Polyethylene terephthalate)
5.4.9 Polyisoprene
5.4.10 Epoxy Resins
5.4.11 Polyamides
5.4.12 Polyimides
5.5 Scaling methods
5.6 Concluding Remarks
5.7 References

Chapter 6
Absorption and Desorption Currents
6.1 Absorption current in a dielectric
6.2 Ramon's approximation
6.3 Distribution of relaxation time and dielectric function
6.3.1 Cole-Cole function
6.3.2 Davidson-Cole function
6.3.3 Fuoss-Kirkwood function
6.3.4 Havriliak-Negami function
6.4 The Williams-Watts function
6.5 The G(i) function for William-Watt curent decay
6.6 Experimental measurements
6.6.1 Poly(vinyl acetate)
6.7 Commercial dielectrics
6.7.1 Aramid paper
6.7.2 Composite polyamide
6.7.3 Polyethylene terephthalate)
6.7.4 Fluoropolymer
6.7.5 Polyimide
6.8 References

Chapter 7
Field Enhanced Conduction
7.1 Some general comments

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7.2 Motion of charge carriers in dielectrics
7.3 Ionic conduction
7.4 Charge injection into dielectrics
7.4.1 The tunneling phenomenon
7.4.2 Schottky emission
7.4.3 Hopping mechanism
7.4.4 Poole-Frenkel Mechanism
7.4.5 Space charge limited current (trap free)
7.4.6 Space charge limited current (with traps)
7.5 Space charge phenomenon in non-uniform fields
7.6 Conduction in selected polymers
7.6.1 Conduction in polyethylene
7.6.2 Conduction in fluoropolymers
7.6.3 Aromatic polyimide
7.6.4 Aromatic polyamide
7.7 Numerical computation
7.8 Closing remarks
7.9 References

Chapter 8
Fundamental Aspects of Gaseous Breakdown-l
8.1 Collision phenomena
8.1.1 Elastic collision
8.1.2 Collision cross section
8.1.3 Probability of collision
8.1.4 Inelastic collisions
8.1.5 Mean free path
8.1.6 lonization by collision
8.1.7 Direct ionization
8.1.8 Dissociative ionization
8.1.9 Excitation
8.1.10 Dissociative excitation
8.1.11 Photoexcitation
8.1.12 Electron attachment
8.1.13 Electron detachment
8.1.14 Recombination
8.1.15 Secondary ionization coefficient
8.1.16 Photo-ionization
8.1.17 Electron swarm coefficients
8.2 Electron Growth in an Avalanche

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8.3 Criteria for Breakdown
8.4 Paschen's Law
8.5 Breakdown time lags
8.5.1 The statistical time lag
8.5.2 Formative time lags in uniform fields
8.5.3 Formative time lags in cylindrical geometry
8.6 The streamer mechanism
8.6.1 The leader mechanism
8.7 Field distortion due to space charge
8.8 Sparkover characteristics of uniform field gaps in SF6
8.9 Sparkover characteristics of long gaps
8.10 Breakdown voltages in air with alternating voltages
8.11 Concluding remarks
8.12 References

Chapter 9
Fundamental Aspects of Electrical Breakdown-ll
9.1 Electron energy distribution functions (EEDF)
9.1.1 EEDF: The Boltzmann equation
9.1.2 EEDF: The Monte Carlo method
9.2 Streamer formation in uniform fields
9.3 The corona discharge
9.4 Basic mechanisms: Negative corona
9.5 Basic Mechanisms: Positive corona
9.6 Modeling of corona discharge: Continuity equations
9.7 Non-equilibrium considerations
9.8 Monte Carlo simulation: Negative corona in SF6
9.9 Monte Carlo Simulation: Positive corona in SF6
9.10 Concluding Remarks
9.11 References

Chapter 10
Thermally Stimulated Processes
10.1 Traps in insulators
10.2 Current due to thermally stimulated depolarization (TSDC)
10.3 TSD currents for distribution of activation energy
10.4 TSD currents for universal relaxation mechanism
10.5 TSD currents with ionic space charge
10.6 TSD currents with electronic conduction
10.7 TSD currents with corona charging

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10.8 Compensation temperature
10.9 Methods and analyses
10.10 TSD and AC dielectric properties
10.11 References

Chapter 11
Space Charge in Solids Dielectrics
11.1 The meaning of space charge
11.2 Polarons and traps
11.3 A conceptual approach
11.4 The thermal pulse method of Collins
11.5 DeReggi's analysis
11.6 Laser intensity modulation method (LIPP)
11.7 The pressure pulse method
11.7.1 Laser induced pressure pulse method
11.7.2 Thermoelastic stress waves
11.7.3 Pressure wave propagation (PWP) method
11.7.4 Nonstructured acoustic probe method
11.7.5 Laser generated acoustic pulse method
11.7.6 Acoustic pulse generated by mechanical excitation
11.7.7 Piezo-Electric Pressure Step Method (PPS)
11.7.8 Pulsed Electro-Acoustic Stress Method
11.7.9 Electron Beam Method
11.7.10 Special Techniques
11.8 Experimental Results
11.9 Closing Remarks
11.10 References

Appendix 1: Trade Names of Polymers


Appendix 2: General Classification of Polymer Dielectrics
Appendix 3: Selected Properties of Insulating Materials
Appendix 4: Relative Ranking of Thermoplastic Polymers
Appendix 5: Selected Propertiers of Polymer Insulating Materials

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