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THERMOELECTRICS
HANDBOOK
MACRO TO NANO
Edited by D.M. Rowe, Ph.D., D.Sc.
Boca Raton London New York
A CRC title, part of the Taylor & Francis imprint, a member of the
Taylor & Francis Group, the academic division of T&F Informa plc.
© 2006 by Taylor & Francis Group, LLC

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Thermoelectrics handbook : macro to nano / edited by D.M. Rowe.

p. cm.
Includes bibliographical references and index.
ISBN 0-8493-2264-2 (alk. paper)
1. Thermoelectric apparatus and appliances. 2. Microelectronics--Materials. 3. Nanotechnology--
Materials. I. Rowe, David Michael.
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Preface
Thermoelectrics is defined as the science and technology associated with thermoelectric generation and
refrigeration. Ten years ago volume 1 of the CRC Handbook of Thermoelectrics was published. Its
publication brought together the many strands of activities in this scientific field under a unifying cover.
An historical backdrop to thermoelectrics was given in its introductory chapter to which interested
readers are referred.
During the intervening years since its publication, activity in thermoelectrics has increased
substantially. This is primarily due to three major factors: increasing awareness of the deleterious effect
of global warming on the planet’s environment, a renewed requirement for long-life electrical power
sources, including nuclear fueled, and the increasing miniaturization of electronic circuits and sensors.
Thermoelectrics is able to make a contribution to meeting the requirements of all three activities.
Substantial progress has been made in employing thermoelectrics as an environmentally friendly
method of recovering industrial and automobile waste heat, the development of high-performance
functionally graded and segmented thermoelements for power source applications, and in the fabrication
of reliable thin-film generating, cooling, and sensing devices. In addition, the advent of nanotechnology
has had a dramatic effect on thermoelectric material development and has resulted in the syntheses
of nanostructured materials whose thermoelectric properties surpass the best performance of
conventional materials.
This second volume of the Handbook complements volume one. It provides an update of recent
developments and serves both as an authoritative reference text on thermoelectrics for the professional
scientist and engineer, and as a source of general information on thermoelectrics for the well-informed
layman. It comprises 59 chapters, written by 99 internationally acknowledged experts in their field.
The majority of chapters are review type and arranged in five sections I through V, entitled General
Principles and Theoretical Considerations; Material Preparation and Measurements; Thermoelectric
Materials; Thermoelements, Modules, and Devices; and Thermoelectric Systems and Applications. The
theme of this Handbook’s title, macro to nano, is reflected in the order of chapters within each section,
with the subject contents progressing from the large (macro) to micro and nano scale. Two appendices, I,
History of the International Thermoelectric Society and II, Manufacturers and Suppliers of
Thermoelectric Modules, complete the Handbook.
As in the first volume, I have taken the role of an acquisitions editor, rather than a copyeditor and
although I have rephrased on occasion in order to clarify the meaning, every attempt has been made to
preserve the international flavor of the Handbook. I am indebted to my colleagues in the thermoelectric
community who have again unselfishly contributed to this Handbook and to Pat Hyatt, who has assisted
me in responding to the immense volume of e-mail correspondence during the past 18 months and for
retyping many of the chapters. Finally, I thank my wife Barbara for her patience and understanding
during the many hours I spent in collating material and editing this Handbook.
D.M. Rowe
v
Contributors
Robert D. Abelson L.P. Bulat M.S. Dresselhaus

Jet Propulsion Laboratory St. Petersburg State University Massachusetts Institute of
Pasadena, California, USA of Refrigeration Technology (MIT)
St. Petersburg, Russia Cambridge, Massachusetts, USA
L.I. Anatychuk
Institute of Thermoelectricity A.T. Burkov Mohamed S. El-Genk
Chernovtsy, Ukraine Ioffe Physico-Technical Institute of the The University of New Mexico
Russian Academy of Sciences Alberquerque, New Mexico, USA
Alexander A. Balandin St. Petersburg, Russia
University of California N.B. Elsner
Riverside, California, USA Fausto Cargnoni Hi-Z Technology, Inc.
CNR-ISTM, Istituto di Scienze e San Diego, California, USA
Benjamin P. Banney Tecnologie Molecolari
Hydrocool Pty Ltd Milano, Italy David Emin
Rozelle, Australia University of New Mexico
A.I. Casian Alberquerque, New Mexico, USA
J.C. Bass Technical University of Moldova
Hi-Z Technology, Inc. Kishinau, Moldova I.S. Eremin
San Diego, California, USA Ioffe Physico-Technical Institute of the
G. Chen Russian Academy of Sciences
Yury M. Belov Massachusetts Institute of St. Petersburg, Russia
Crystal Ltd. Technology (MIT)
Korolev, Russia Mechanical Engineering M.I. Fedorov
Cambridge, Massachusetts, USA Ioffe Physico-Technical Institute of the
Luca Bertini Russian Academy of Sciences
CNR-ISTM, Istituto di Scienze e Peter T. Clarke St. Petersburg, Russia
Tecnologie Molecolari Hydrocool Pty Ltd
Milano, Italy Rozelle, Australia Ryoji Funahashi
National Institute of Advanced
Chandra Mohan Bhandari B.A. Cook Industrial Science and
University of Allahabad Iowa State University Technology
Allahabad, India Ames, Iowa, USA Osaka, Japan
M. Blumers C. Dames Carlo Gatti

University of Applied Sciences Massachusetts Institute of Technology CNR-ISTM, Istituto di Scienze e
Wiesbaden, Germany (MIT) Tecnologie Molecolari
Cambridge, Massachusetts, USA Milano, Italy
Harald Böttner
Fraunhofer Institute for Physical Montag C. Davis S. Ghamaty
Measurement Techniques Hydrocool Pty Ltd Hi-Z Technology, Inc.
Freiburg, Germany Rozelle, Australia San Diego, California, USA
vii
viii Contributors
H.J. Goldsmid Kunihito Koumoto Igor V. Morgunov

University of New South Wales Nagoya University Crystal Ltd.
Sydney, Australia Nagoya, Japan Korolev, Russia
V.M. Grabov Yan Kucherov Mamoun Muhammed

Ioffe Physico-Technical Institute of the ENECO Inc Royal Institute of Technology
Russian Academy of Sciences Salt Lake City, Utah, USA Stockholm, Sweden
St. Petersburg, Russia
V.A. Kutasov Eckhard Müller
E.A. Gurieva Ioffe Physico-Technical Institute of the German Aerospace Center (DLR)
Ioffe Physico-Technical Institute of the Russian Academy of Sciences Köln, Germany
Russian Academy of Sciences St. Petersburg, Russia
St. Petersburg, Russia George S. Nolas
Peter Hagelstein V.L. Kuznetsov University of South Florida
University of Oxford Tampa, Florida, USA
Massachusetts Institute of
Oxford, Wales, UK
Technology (MIT) Joachim Nurnus
Cambridge, Massachusetts, USA
Armin Lambrecht Fraunhofer Institute for Physical
Measurement Techniques
J.L. Harringa Fraunhofer Institute for Physical
Freiburg, Germany
Iowa State University Measurement Techniques
Ames, Iowa, USA Freiburg, Germany
Michitaka Ohtaki
J.P. Heremans Kyushu University
L.N. Lukyanova
Delphi Research Laboratories Kasuga, Japan
Ioffe Physico-Technical Institute of the
Shelby Township, Michigan, USA Russian Academy of Sciences
St. Petersburg, Russia Brooks O’Quinn
Timothy P. Hogan Center for Thermoelectric
Michigan State University Research
O.J. Luste Research Triangle Park
East Lansing, Michigan, USA
Institute of Thermoelectricity
North Carolina, USA
Chernovtsy, Ukraine
J.-P. Issi
Université Catholique de Louvain S. Paschen
Louvain-la-Neuve, Belgique G.D. Mahan Max Planck Institute for
The Pennsylvania State University Chemical Physics of Solids
Yu.V. Ivanov University Park, Pennsylvania, USA Dresden, Germany
Ioffe Physical-Technical Institute of
the Russian Academy of Sciences Sergei M. Maniakin Kevin Pipe
St. Petersburg, Russia Crystal Ltd. University of Michigan
Korolev, Russia Ann Arbor, Michigan, USA
Bo Brummerstedt
Iversen Brett R. Manners A.A. Pustovalov
Institute of Thermoelectricity
University of Aarhus Hydrocool Pty Ltd
Chernovtsy, Ukraine
Aarhus, Denmark Australia
X.H. Ji Kakuei Matsubara K.R. Rao

Zhejiang University Tokyo University of Science University of Texas
Hangzhou, China Yamaguchi, Japan Arlington, Texas, USA
Takenobu Kajikawa Mitsuru Matsuura P. Rogl

Shonan Institute of Technology Yamaguchi University Universität Wien
Kanagawa, Japan Yamaguchi, Japan Wien, Austria
Tsuyoshi Kajitani A. Meier D.M. Rowe

Tohoku University University of Applied Sciences Cardiff University
Sendai, Japan Wiesbaden, Germany Cardiff, Wales, UK
Dennis D. Klug Gao Min Hamed H. Saber

Steacie Institute for Molecular Science Cardiff University The University of New Mexico
Ottawa, Ontario, Canada Cardiff, Wales, UK Albuquerque, New Mexico, USA

Contributors ix
H. Scherrer Christian Stiewe Rama

Laboratoire de Physique des German Aerospace Center (DLR) Venkatasubramanian
Matériaux Köln, Germany Center for Thermoelectric Research
Nancy, France Research Triangle Park
J. Stockholm North Carolina, USA
S. Scherrer Marvel Thermoelectrics
Laboratoire de Physique des
Matériaux
Vernouillet, France C.B. Vining
ZT Services, Inc.
Nancy, France
Ichiro Terasaki Auburn, Alabama, USA
Axel Schubert Waseda University
Infineon Technologies AG
Tokyo, Japan F. Völklein
München, Germany University of Applied Sciences
Muhammet Toprak Wiesbaden, Germany
J. Schumann Royal Institute of Technology
A. Leibniz Institute of Solid-State Stockholm, Sweden Robert M. Weymouth
and Materials Hydrocool Pty Ltd
Dresden, Germany Terry M. Tritt Rozelle, Australia
Clemson University
V.A. Semenyuk Clemson, South Carolina, USA S.G.K. Williams
Thermion Company
Cardiff University
Odessa, Ukraine
John S. Tse Cardiff, Wales, UK
University of Saskatchewan
Tom Shih
Michigan State University
Saskatoon, Ontario, Canada V.K. Zaitsev
East Lansing, Michigan, USA Ioffe Physico-Technical Institute of the
Ctirad Uher Russian Academy of Sciences
Edward Siivola University of Michigan St. Petersburg, Russia
Center for Thermoelectric Research Ann Arbor, Michigan, USA
Research Triangle Park X.B. Zhao
North Carolina, USA O.N. Uryupin Zhejiang University
Ioffe Physico-Technical Institute of the Hangzhou, China
A.A. Snarskii Russian Academy of Sciences
Kiev Politechnical Institute St. Petersburg, Russia T.J. Zhu
Kiev, Ukraine Zhejiang University
M.V. Vedernikov Hangzhou, China
G. Jeffrey Snyder Ioffe Physico-Technical Institute of the
Jet Propulsion Laboratory Russian Academy of Sciences
Institute of Technology
St. Petersburg, Russia
Pasadena, California, USA

Contents
SECTION I General Principles and Theoretical

Considerations
1 General Principles and Basic Considerations D.M. Rowe .................................................... 1-1

1.1 Introduction ................................................................................................................................ 1-1
1.2 Thermoelectric and Thermomagnetic Effects .......................................................................... 1-2
1.3 Thermoelectric Generation and the Figure-of-Merit .............................................................. 1-3
1.4 Thermoelectric Refrigeration and the Coefficient of Performance ........................................ 1-6
1.5. Thermoelectric Materials ........................................................................................................... 1-7
1.6 Thermocouple Construction and Configurations ................................................................. 1-10
2 Modern Thermodynamic Theory of Thermoelectricity

L.I. Anatychuk and O.J. Luste .................................................................................................................. 2-1
2.1 Introduction ................................................................................................................................ 2-1
2.2 Nonequilibrium Thermodynamics: General Concepts ........................................................... 2-2
2.3 Thermodynamic Theory of Thermoelectricity ........................................................................ 2-5
2.4 Conclusion ................................................................................................................................ 2-13
3 Thermoelectric Phenomena under Large Temperature Gradients

L.I. Anatychuk and L.P. Bulat .................................................................................................................. 3-1
3.1 Introduction ................................................................................................................................ 3-1
3.2 Influence of a Temperature Gradient on Transport Phenomena
in Semiconductors ...................................................................................................................... 3-2
3.3 Calculation of the Influence of a Large Temperature Gradient on
the Properties of Semiconductor Materials ............................................................................. 3-4
3.4 Distribution Function ................................................................................................................ 3-6
3.5 Temperature Fields and Transport Coefficients ....................................................................... 3-6
3.6 New Effects .................................................................................................................................. 3-8
3.7 The Outlook for Practical Applications ................................................................................... 3-8
4 Minority Carriers and Thermoelectric Effects in Bipolar Devices Kevin Pipe .............. 4-1
4.1 Introduction ................................................................................................................................ 4-1
4.2 Conventional Thermoelectric Cooler ....................................................................................... 4-2
4.3 Bipolar Peltier Coefficient .......................................................................................................... 4-2
xi
xii Contents
4.4 Minority Carriers and Quasi-Fermi Levels .............................................................................. 4-4

4.5 Thermoelectric Cooling in Bipolar Devices ............................................................................. 4-4
5 Effects of Charge Carriers’ Interactions on Seebeck Coefficients David Emin ............. 5-1
5.1 Introduction ................................................................................................................................ 5-1
5.2 The Seebeck Coefficient ............................................................................................................. 5-2
5.3 Noninteracting Charge Carriers ................................................................................................ 5-2
5.4 Electron –Electron Interactions ................................................................................................. 5-2
5.5 Electron –Phonon Interactions .................................................................................................. 5-3
5.6 Magnetic Interactions ................................................................................................................ 5-6
5.7 Summary ..................................................................................................................................... 5-6
6 Thermal Conductivity of Semiconductors with

Complex Crystal Structures V.K. Zaitsev and M.I. Fedorov ...................................................... 6-1
6.1 Introduction ................................................................................................................................ 6-1
6.2 Boron and Boron-Rich Borides ................................................................................................ 6-1
6.3 Higher Manganese Silicide ........................................................................................................ 6-3
6.4 Argyrodites .................................................................................................................................. 6-4
6.5 Conclusion .................................................................................................................................. 6-6
7 A Chemical Approach to the First-Principles Modeling of Novel

Thermoelectric Materials Luca Bertini, Fausto Cargnoni, and Carlo Gatti .............................. 7-1
7.1 Introduction ................................................................................................................................ 7-1
7.2 Charge Transfer, Charge Donation, and Chemical Bonding
in Type I Inorganic Clathrates .................................................................................................. 7-2
7.3 Theoretical Modeling for Optimal Doping Elements and Doping Level in Co4Sb12 .......... 7-6
7.4 A Combined Theoretical and Experimental Structural Study of b Zn –Sb ........................ 7-10
8 Recent Trends for the Design and Optimization of Thermoelectric

Materials — A Theoretical Perspective John S. Tse and Dennis D. Klug .............................. 8-1
8.1 Introduction ................................................................................................................................ 8-1
8.2 Fundamentals of Band Theory and Thermoelectrics .............................................................. 8-2
8.3 Transport Theory Methods ....................................................................................................... 8-4
8.4 Phonon Glasses ........................................................................................................................... 8-6
8.5 New Materials ........................................................................................................................... 8-16
8.6 Concluding Remarks ................................................................................................................ 8-24
9 Thermoelectric Power Generation: Efficiency and Compatibility G. Jeffrey Snyder ..... 9-1
9.1 Introduction ................................................................................................................................ 9-1
9.2 Reduced Variables ....................................................................................................................... 9-4
9.3 Generator Efficiency and Performance ..................................................................................... 9-8
9.4 Computation of Generator Performance ............................................................................... 9-12
9.5 Thermoelectric Compatibility ................................................................................................. 9-17
9.6 Design Optimization ................................................................................................................ 9-21
10 A New Upper Limit to the Thermoelectric Figure-of-Merit H.J. Goldsmid ................ 10-1
10.1 Introduction .............................................................................................................................. 10-1
10.2 New Materials ........................................................................................................................... 10-2

Contents xiii
10.3 Low-Dimensional Systems ....................................................................................................... 10-3

10.4 The Maximum ZT for Low-Dimensional Structures ............................................................ 10-3
10.5 Solid-State Thermionic Converters ........................................................................................ 10-5
10.6 Possibility of Independent Electron and Phonon Currents .................................................. 10-6
10.7 Vacuum Thermoelements ........................................................................................................ 10-8
10.8 Conclusions ............................................................................................................................... 10-8
11 Thermoelectric Module Design Theories Gao Min ............................................................. 11-1

11.1 Introduction .............................................................................................................................. 11-1
11.2 Power Output and Conversion Efficiency .............................................................................. 11-2
11.3 Design Considerations and Optimization ............................................................................. 11-4
11.4 Coefficient of Performance and Heat Pumping Capacity .................................................... 11-4
11.5 Fabrication Quality Factor ...................................................................................................... 11-7
11.6 Micro/Nano Converters ........................................................................................................... 11-8
11.7 Ring-Structure Module .......................................................................................................... 11-11
11.8 Summary ................................................................................................................................. 11-14
12 Modeling and Characterization of Power Generation Modules Based

on Bulk Materials Timothy P. Hogan and Tom Shih .................................................................. 12-1
12.1 Introduction .............................................................................................................................. 12-1
12.2 Modeling Techniques ............................................................................................................... 12-3
12.3 Multidimensional Analysis ...................................................................................................... 12-9
13 Energy Conversion Using Diode-Like Structures

Yan Kucherov and Peter Hagelstein ....................................................................................................... 13-1
13.1 Introduction .............................................................................................................................. 13-1
13.2 InSb Thermal Diodes ............................................................................................................... 13-2
13.3 HgCdTe Thermal Diodes ......................................................................................................... 13-6
13.4 Multijunction Thermal Diodes ............................................................................................... 13-7
13.5 Modeling Issues ........................................................................................................................ 13-8
14 Size Effects on Thermal Transport Chandra Mohan Bhandari ............................................. 14-1

14.1 Introduction .............................................................................................................................. 14-1
14.2 Phonons and Electrons ............................................................................................................ 14-2
14.3 Electrons and Phonons in Confined Structures .................................................................... 14-4
14.4 Superlattice Structures ............................................................................................................. 14-8
14.5 Graphitic Microtubules .......................................................................................................... 14-10
15 Thermoelectric Aspects of Strongly Correlated Electron Systems S. Paschen ............. 15-1

15.1 Introduction .............................................................................................................................. 15-1
15.2 Kondo Impurity Systems ......................................................................................................... 15-2
15.3 Kondo Lattice Systems ............................................................................................................. 15-6
15.4 Thermoelectric Figure-of-Merit ............................................................................................ 15-10
15.5 New Approaches ..................................................................................................................... 15-13
16 Theory and Modeling in Nanostructured Thermoelectrics Alexander A. Balandin .... 16-1

16.1 Introduction .............................................................................................................................. 16-1
16.2 Electron and Phonon Transport in Quantum Dot Superlattices ......................................... 16-1

xiv Contents
16.3 Optimization of Quantum Dot Structures for ZT Enhancement ....................................... 16-4

16.4 Phonon Engineering Concepts for Thermoelectric Nanostructures .................................... 16-6
17 Thermoelectric Power of Carbon Nanotubes G.D. Mahan ............................................... 17-1

17.1 Experimental Overview ............................................................................................................ 17-1
17.2 Ballistic Transport .................................................................................................................... 17-2
17.3 Nonballistic Transport ............................................................................................................. 17-3
18 Phonon-Drag Thermopower of Low-Dimensional Semiconductor

Structures Yu.V. Ivanov ................................................................................................................... 18-1
18.1 Herring’s Phonon-Drag: Basic Equations .............................................................................. 18-1
18.2 Thermopower of Degenerate 2D Electron Gas at Low Temperatures ................................. 18-4
18.3 Thermopower of Nondegenerate 2D Electron Gas ............................................................... 18-7
18.4 Two-Stage Drag in Low-Dimensional Structures .................................................................. 18-8
18.5 Phonon-Drag Thermoelectric Figure-of-Merit .................................................................... 18-11
Appendix 18A Relaxation Times .......................................................................................... 18-13
SECTION II Material Preparation and Measurements
19 Solid-State Synthesis of Thermoelectric Materials B.A. Cook and J.L. Harringa ............ 19-1
19.1 Introduction .............................................................................................................................. 19-1
19.2 Background ............................................................................................................................... 19-2
19.3 Equipment ................................................................................................................................. 19-5
19.4 Materials .................................................................................................................................... 19-6
19.5 Summary ................................................................................................................................. 19-14
20 Review of Methods of Thermoelectric Materials Mass Production

Yury M. Belov, Sergei M. Maniakin, and Igor V. Morgunov ................................................................ 20-1
20.1 Introduction .............................................................................................................................. 20-1
20.2 The Main Characteristics of the Materials ............................................................................. 20-1
20.3 Material Properties Affecting the Choice of Production Method ........................................ 20-2
20.4 Conventional Material Preparation Methods ........................................................................ 20-2
20.5 Prerequisites for the New Method Development .................................................................. 20-6
21 Structural Studies of Thermoelectric Materials Bo Brummerstedt Iversen ....................... 21-1

21.1 Introduction .............................................................................................................................. 21-1
21.2 Accurate Crystal Structure Investigations .............................................................................. 21-1
21.3 Inorganic Clathrates ................................................................................................................. 21-8
21.4 Concluding Remarks .............................................................................................................. 21-16
22 Measurements of Resistivity and Thermopower: Principles

and Practical Realization A.T. Burkov ....................................................................................... 22-1
22.1 Introduction .............................................................................................................................. 22-1
22.2 Resistivity Measurement .......................................................................................................... 22-1
22.3 Thermopower Measurement ................................................................................................... 22-4
22.4 Resistivity and Thermopower Measurements over the Temperature Range
100 to 1300 K ............................................................................................................................ 22-9

Contents xv
22.5 Thermopower Measurement at Low Temperatures: 3 to 300 K .......................................... 22-9

22.6 Resistivity and Thermopower Measurement at 300 to 2000 K .......................................... 22-12
23 Electrical and Thermal Transport Measurement Techniques for Evaluation

of the Figure-of-Merit of Bulk Thermoelectric Materials Terry M. Tritt ...................... 23-1
23.1 Introduction .............................................................................................................................. 23-2
23.2 Thermoelectric Materials ......................................................................................................... 23-3
23.3 Thermoelectric Measurement Issues ....................................................................................... 23-3
23.4 Electrical Resistivity Measurements (and Electrical Conductivity) ..................................... 23-5
23.5 Seebeck Coefficient or Thermopower Measurements ........................................................... 23-9
23.6 Thermal Conductivity Measurements .................................................................................. 23-11
23.7 Hall Coefficient, Carrier Concentration, and Mobility ....................................................... 23-15
23.8 Z Meters (or Harman Technique) for Thermoelectric Measurements .............................. 23-16
23.9 Summary ................................................................................................................................. 23-17
24 Measurement of the Thermal Conductivity of Thin Films F. Völklein,

A. Meier, and M. Blumers ...................................................................................................................... 24-1
24.1 Introduction .............................................................................................................................. 24-1
24.2 Features and Problems of Measuring Techniques for Thin Films ....................................... 24-2
24.3 Measuring Techniques Using Microstructures Prepared by Micromachining .................... 24-5
25 Solvothermal Synthesis of Nanostructured Thermoelectric Materials X.B. Zhao,

T.J. Zhu, and X.H. Ji .............................................................................................................................. 25-1
25.1 Introduction .............................................................................................................................. 25-1
25.2 Solvothermal Synthesis of Thermoelectric Nanopowders .................................................... 25-2
25.3 Bi2Te3 Nanotubes and Nanocapsules ...................................................................................... 25-3
25.4 Growth Mechanism of Bi2Te3 Nanocrystals ........................................................................... 25-5
25.5 Bi2Te3 Thermoelectric Nanocomposites ................................................................................. 25-7
26 Approaches to Thermoelectric Standardization Eckhard Müller, Christian Stiewe,

D.M. Rowe, and S.G.K. Williams .......................................................................................................... 26-1
26.1 Introduction .............................................................................................................................. 26-1
26.2 Thermoelectric Properties and Their Measurement ............................................................. 26-4
26.3 Strategies toward Standardization ........................................................................................ 26-12
26.4 Conclusions ............................................................................................................................. 26-26
SECTION III Thermoelectric Materials
27 Thermoelectric Properties of Bismuth Antimony Telluride Solid Solutions

H. Scherrer and S. Scherrer .................................................................................................................... 27-1
27.1 Introduction .............................................................................................................................. 27-1
27.2 General Properties of Bi2Te3, Sb2Te3, and Its Solid Solutions .............................................. 27-2
27.3 Growth Methods of Standard Binary Compounds Bi2Te3, Sb2Te3,
and Their Solid Solutions ........................................................................................................ 27-7
27.4 Thermoelectric Properties ..................................................................................................... 27-12
27.5 Technological Production of Materials ................................................................................ 27-16

xvi Contents
28 Bi – Sb Alloys: Thermopower in Magnetic Field V.M. Grabov and O.N. Uryupin .......... 28-1
28.1 Introduction .............................................................................................................................. 28-1
28.2 Magneto-Thermoelectric Power in Undoped Bismuth – Antimony Crystals ..................... 28-3
28.3 Magneto-Thermoelectric Power in Bismuth – Antimony Crystals
Doped with Donor and Acceptor Impurities ........................................................................ 28-9
28.4 Conclusion .............................................................................................................................. 28-18
29 Thermoelectrics on the Base of Solid Solutions of Mg2BIV Compounds

(BIV ¼ Si, Ge, Sn) V.K. Zaitsev, M.I. Fedorov, I.S. Eremin, and E.A. Gurieva ......................... 29-1
29.1 Introduction .............................................................................................................................. 29-1
29.2 Crystal Structure, Physical Properties, and Production of Mg2BIV Compounds
and Their Solid Solutions ........................................................................................................ 29-1
29.3 Solid Solutions of Mg2BIV Compounds ................................................................................. 29-6
29.4 Efficiency of Thermoelectric Energy Conversion .................................................................. 29-8
29.5 Conclusion ................................................................................................................................ 29-9
30 Thermoelectric Properties of the Group V Semimetals J.-P. Issi .................................... 30-1

30.1 Introduction .............................................................................................................................. 30-1
30.2 Semimetallic Behavior and Its Effects on Thermoelectric Transport .................................. 30-2
30.3 Doping and Alloying ................................................................................................................ 30-5
30.4 Diffusive and Ballistic Transport ............................................................................................. 30-9
30.5 Phonon-Drag Effects .............................................................................................................. 30-10
30.6 Size Effects ............................................................................................................................... 30-11
30.7 Summary ................................................................................................................................. 30-12
31 Thermoelectrics of Transition Metal Silicides M.I. Fedorov and V. K. Zaitsev ................ 31-1
31.1 Introduction .............................................................................................................................. 31-1
31.2 Chromium Disilicide ............................................................................................................... 31-1
31.3 Higher Manganese Silicide ...................................................................................................... 31-3
31.4 Iron Disilicide ......................................................................................................................... 31-10
31.5 Ruthenium Sesquisilicide ....................................................................................................... 31-11
31.6 Cobalt Monosilicide ............................................................................................................... 31-12
31.7 Conclusion .............................................................................................................................. 31-14
32 Formation and Crystal Chemistry of Clathrates P. Rogl ................................................... 32-1

32.1 Introduction .............................................................................................................................. 32-1
32.2 Definitions: Clathrates, Zeolites, Clathrasils .......................................................................... 32-1
32.3 Crystal Chemistry of Clathrate Materials (Hydrate Clathrates-Intermetallides) ................ 32-2
32.4 Dual Structures ......................................................................................................................... 32-4
32.5 Classification of Clathrate Structures ..................................................................................... 32-5
32.6 Relation Scheme of Intermetallic Clathrate Compounds ................................................... 32-10
32.7 Zintl Concept and Formation of Clathrates ........................................................................ 32-12
32.8 Rare-Earth Substituted Clathrates ........................................................................................ 32-16
33 Structure, Thermal Conductivity, and Thermoelectric Properties of Clathrate

Compounds George S. Nolas .......................................................................................................... 33-1
33.1 Introduction .............................................................................................................................. 33-1
33.2 Crystal Structure ....................................................................................................................... 33-2

Contents xvii
33.3 Transport Properties of Type I and II Clathrates .................................................................. 33-3

33.4 Specimen Purity ....................................................................................................................... 33-5
33.5 Thermoelectric Properties of Clathrates ................................................................................ 33-5
33.6 Summary ................................................................................................................................... 33-6
34 Skutterudite-Based Thermoelectrics Ctirad Uher .................................................................. 34-1

34.1 Introduction .............................................................................................................................. 34-1
34.2 Crystal Structure and Bonding ............................................................................................... 34-2
34.3 Band Structure and Lattice Dynamics .................................................................................... 34-6
34.4 Transport Properties Relevant to Thermoelectricity ........................................................... 34-10
34.5 Approaches toward Further Improvement of Filled Skutterudites .................................... 34-12
34.6 Conclusion .............................................................................................................................. 34-13
35 Oxide Thermoelectrics Kunihito Koumoto, Ichiro Terasaki, Tsuyoshi Kajitani,

Michitaka Ohtaki, and Ryoji Funahashi ............................................................................................... 35-1
35.1 Introduction .............................................................................................................................. 35-1
35.2 Nanoblock Integration ............................................................................................................. 35-2
35.3 NaxCoO2 .................................................................................................................................... 35-2
35.4 Ca – Co – O System .................................................................................................................... 35-4
35.5 SrTiO3 and Layered (SrO)(SrTiO3)m ..................................................................................... 35-6
35.6 ZnO-Based Oxides ................................................................................................................... 35-8
35.7 Fabrication of Thermoelectric Oxide Modules ................................................................... 35-11
35.8 Conclusion .............................................................................................................................. 35-13
36 Thermoelectric Properties of Electrically Conducting Organic Materials

A.I. Casian .............................................................................................................................................. 36-1
36.1 Introduction .............................................................................................................................. 36-1
36.2 Mechanisms of Charge Transport in Organic Materials ....................................................... 36-2
36.3 Quasi-One-Dimensional Organic Crystals — A New Class of
Organic Materials ..................................................................................................................... 36-3
36.4 High Values of the Thermoelectric Figure-of-Merit Expected in
Q1D Organic Crystals .............................................................................................................. 36-4
36.5 Conclusions ............................................................................................................................... 36-7
37 Shifting the Maximum Figure-of-Merit of (Bi, Sb)2(Te, Se)3 Thermoelectrics

to Lower Temperatures V.A. Kutasov, L.N. Lukyanova, and M.V. Vedernikov ........................ 37-1
37.1 Introduction .............................................................................................................................. 37-1
37.2 Review of the Figure-of-Merit Features of Thermoelectrics ................................................ 37-2
37.3 Optimization of Thermoelectric Properties of Thermoelement Legs: Experiment ........... 37-4
37.4 Optimization of Thermoelectric Properties of Thermoelement Legs:
Physical Aspect ......................................................................................................................... 37-8
37.5 The Experimental Cooling Thermoelectric Modules for Low Temperatures ................... 37-14
37.6 Conclusion .............................................................................................................................. 37-15
38 Functionally Graded Materials for Thermoelectric Applications

V.L. Kuznetsov ......................................................................................................................................... 38-1
38.1 Introduction .............................................................................................................................. 38-1
38.2 Modeling of Thermoelectric Properties of Functionally Graded Materials ........................ 38-2

xviii Contents
38.3 Preparation of Functionally Graded Materials ...................................................................... 38-4

38.4 Evaluation of Thermoelectric Properties of Functionally Graded Materials ...................... 38-8
38.5 Conclusions ............................................................................................................................. 38-11
39 Recent Developments in Low-Dimensional Thermoelectric Materials

M.S. Dresselhaus and J.P. Heremans ..................................................................................................... 39-1
39.1 Introduction .............................................................................................................................. 39-1
39.2 Early Work ................................................................................................................................ 39-2
39.3 One-Dimensional Thermoelectric Materials ......................................................................... 39-3
39.4 Quantum Dot Superlattice .................................................................................................... 39-15
39.5 New Research Directions ....................................................................................................... 39-20
40 Thermoelectric Properties of Nanocrystalline Transition Metal Silicides

J. Schumann and A.T. Burkov ............................................................................................................... 40-1
40.1 Introduction .............................................................................................................................. 40-1
40.2 Structure and Thermoelectric Properties of Nanocrystalline Silicides ................................ 40-3
40.3 Conclusion .............................................................................................................................. 40-11
41 Nanostructured Skutterudites Mamoun Muhammed and Muhammet Toprak ..................... 41-1

41.1 Introduction .............................................................................................................................. 41-1
41.2 Methods of Fabrication and Physical Properties ................................................................... 41-3
42 Thermal Conductivity of Nanostructured Thermoelectric Materials

C. Dames and G. Chen .......................................................................................................................... 42-1
42.1 Introduction .............................................................................................................................. 42-1
42.2 Theoretical Framework ............................................................................................................ 42-2
42.3 Estimating Key Length Scales for Bulk Materials .................................................................. 42-5
42.4 Summary and Outlook .......................................................................................................... 42-11
SECTION IV Thermoelements, Modules, and Devices
43 Modeling and Optimization of Segmented Thermoelectric Generators for

Terrestrial and Space Applications Mohamed S. El-Genk and Hamed H. Saber ................. 43-1
43.1 Introduction .............................................................................................................................. 43-1
43.2 Segmented Thermoelectric Model .......................................................................................... 43-1
43.3 Modeling and Optimization of Segmented Thermoelectric Unicouples ............................ 43-3
43.4 Optimum Conversion Efficiency ............................................................................................. 43-6
43.5 Summary ................................................................................................................................. 43-11
44 Thermocouple with a Passive High Temperature Superconductor Leg

V.L. Kuznetsov and M.V. Vedernikov ..................................................................................................... 44-1
44.1 Introduction .............................................................................................................................. 44-1
44.2 Materials for an Active Leg ..................................................................................................... 44-2
44.3 Materials for a Passive Leg ...................................................................................................... 44-3

Contents xix
44.4 Design and Properties of Thermoelements with a Passive Leg ............................................ 44-4
44.5 Conclusion ................................................................................................................................ 44-7
45 Anisotropic Thermoelements A.A. Snarskii and L.P. Bulat .................................................... 45-1

45.1 Introduction .............................................................................................................................. 45-1
45.2 Simple Theory of Anisotropic Thermoelements ................................................................... 45-3
45.3 Rigorous Phenomenological Theory of Anisotropic Thermoelements ............................... 45-4
45.4 Anisotropic Thermoelements of Various Geometry ............................................................. 45-5
45.5 Figure-of-Merit and Efficiency of Anisotropic Thermoelements ......................................... 45-6
45.6 Physical Reasons for an Anisotropic Thermo-Emf ............................................................... 45-7
45.7 Theory of Anisotropic Scattering ............................................................................................ 45-7
45.8 Materials for Anisotropic Thermoelements ........................................................................... 45-8
45.9 Artificial Anisotropic Thermoelements .................................................................................. 45-8
45.10 Optical Anisotropic Thermoelements .................................................................................... 45-9
45.11 Other Applications of Anisotropic Thermoelements ............................................................ 45-9
46 Miniaturized Thermoelectric Converters Harald Böttner, Joachim Nurnus,

and Axel Schubert ................................................................................................................................... 46-1
46.1 Introduction .............................................................................................................................. 46-1
46.2 General Considerations for Miniaturized Thermogenerators .............................................. 46-2
46.3 General Considerations for Miniaturized Peltier Coolers .................................................... 46-3
46.4 Technologies .............................................................................................................................. 46-5
46.5 Conclusion .............................................................................................................................. 46-16
47 Thermoelectric Microelectromechanical Systems

F. Völklein and A. Meier ........................................................................................................................ 47-1
47.1 Introduction .............................................................................................................................. 47-1
47.2 Thermoelectric Microsensors .................................................................................................. 47-2
47.3 Microelectromechanical Thermoelectric Coder and Generator ......................................... 47-11
47.4 Diagnostic Thermoelectric Microstructures ........................................................................ 47-14
47.5 Conclusion .............................................................................................................................. 47-16
48 Nanoscale Thermoelectrics Joachim Nurnus, Harald Böttner, and Armin Lambrecht .......... 48-1
48.1 Introduction .............................................................................................................................. 48-1
48.2 Approaches for Nanoscaled Materials and Devices .............................................................. 48-2
48.3 IV– VI- and V–VI-Based Epitaxial Nanostructures .............................................................. 48-4
48.4 Conclusions ............................................................................................................................. 48-17
49 Superlattice Thin-Film Thermoelectric Material and Device Technologies

Rama Venkatasubramanian, Edward Siivola, and Brooks O’Quinn ................................................... 49-1
49.1 Introduction .............................................................................................................................. 49-1
49.2 Superlattice Approach to ZT Enhancement ........................................................................... 49-2
49.3 Bi2Te3-Based Superlattice Materials and Device Technology ............................................... 49-4
49.4 Advanced Cooling Modules for Laser Thermal Management ............................................. 49-7
49.5 Early Reliability Studies with Cooling Modules .................................................................... 49-9
49.6 Progress in Cooling Modules at Cryogenic Temperatures ................................................. 49-10
49.7 Power Conversion Applications ............................................................................................ 49-12
49.8 Technology Pull for Near-Term Applications and Future Directions ............................... 49-13

xx Contents
SECTION V Thermoelectric Systems and Applications
50 Thermoelectric Power Generation System Recovering Industrial Waste Heat

Takenobu Kajikawa ................................................................................................................................ 50-1
50.1 Introduction .............................................................................................................................. 50-1
50.2 Waste Heat Characteristics as an Energy Resource ............................................................... 50-2
50.3 Thermoelectric Power Generation System for Recovery Waste Heat .................................. 50-6
50.4 Experiments .............................................................................................................................. 50-9
50.5 Technological Problems and Breakthrough Technology ..................................................... 50-23
50.6 Conclusions and Future Prospects ....................................................................................... 50-26
51 The Concept of Thermoelectric Power Generation Topping-Up

Cogeneration System Takenobu Kajikawa .................................................................................. 51-1
51.1 Introduction .............................................................................................................................. 51-1
51.2 Evaluation of Heat Processing System from Available Energy Analysis .............................. 51-2
51.3 Thermoelectric Power Generation Topping-Up Cogeneration ............................................ 51-3
51.4 Estimation of System Effectiveness from the Viewpoint of Increase
in Power Output ....................................................................................................................... 51-4
51.5 Optimum Temperature Allocation ......................................................................................... 51-5
51.6 Extraction of Enthalpy for Topping-Up Thermoelectric Power Generation ...................... 51-7
52 A Thermoelectric Application to Vehicles Kakuei Matsubara and Mitsuru Matsuura ..... 52-1
52.1 Introduction .............................................................................................................................. 52-1
52.2 General Concept of Thermoelectric Generators for Vehicles ............................................... 52-2
52.3 Review of the Exhaust Gas Thermoelectric Generators for Vehicles ................................... 52-3
52.4 Issues to Be Solved from Technological Viewpoints ............................................................. 52-8
52.5 Conclusion .............................................................................................................................. 52-10
53 Thermoelectric Microgenerators with Isotope Heat Sources L.I. Anatychuk

and A.A. Pustovalov ............................................................................................................................... 53-1
53.1 Introduction .............................................................................................................................. 53-1
53.2 Physical Model of Isotope Thermal Generator ...................................................................... 53-2
53.3 Isotope Heat Source ................................................................................................................. 53-4
53.4 Thermopiles .............................................................................................................................. 53-6
53.5 Thermal Insulation ................................................................................................................. 53-14
53.6 Constructions and Applications of Isotope Microgenerators ............................................ 53-15
54 Performance and Mass Estimates of CTM–ARPSs with Four GPHS Bricks

Mohamed S. El-Genk and Hamed H. Saber ......................................................................................... 54-1
54.1 Introduction .............................................................................................................................. 54-1
54.2 CTM– ARPSs for BOM Power of 108 We .............................................................................. 54-3
54.3 Performance Results of CTM – ARPSs .................................................................................... 54-5
54.4 Thermal Analysis of Heat Rejection Radiator ..................................................................... 54-11
54.5 Mass and BOM Specific Power Estimates of CTM –ARPSs ............................................... 54-14
54.6 Summary ................................................................................................................................. 54-14

Contents xxi
55 Parametric and Optimization Analyses of Cascaded Thermoelectric-Advanced

Radioisotope Power Systems with Four GPHS Bricks Mohamed S. El-Genk
and Hamed H. Saber .............................................................................................................................. 55-1
55.1 Introduction .............................................................................................................................. 55-1
55.2 Cascaded Thermoelectric ......................................................................................................... 55-2
55.3 CTM – ARPSs with Four GPHS Bricks ................................................................................... 55-4
55.4 Summary ................................................................................................................................. 55-12
56 Space Missions and Applications Robert D. Abelson .............................................................. 56-1

56.1 Introduction .............................................................................................................................. 56-1
56.2 Radioisotope Heat Sources ...................................................................................................... 56-5
56.3 Thermoelectric Converters ...................................................................................................... 56-5
56.4 Radioisotope Thermoelectric Generator Systems .................................................................. 56-8
56.5 Dynamic Radioisotope Power Systems ................................................................................ 56-20
56.6 Fission Power Systems ........................................................................................................... 56-21
56.7 Russian Space Nuclear Power Systems ................................................................................. 56-24
56.7 Conclusions ............................................................................................................................. 56-26
57 Quantum Well Thermoelectric Devices and Applications

S. Ghamaty, J.C. Bass, and N.B. Elsner ................................................................................................ 57-1
57.1 Introduction .............................................................................................................................. 57-1
57.2 Recent Advances ....................................................................................................................... 57-2
57.3 Thermoelectric Properties ....................................................................................................... 57-5
57.4 Cooling ...................................................................................................................................... 57-8
57.5 Diesel Exhaust Heat Recovery ................................................................................................. 57-9
57.6 Fuel-Efficient and Hybrid Cars ............................................................................................. 57-10
57.7 Cost .......................................................................................................................................... 57-11
57.8 Summary ................................................................................................................................. 57-11
58 Thermoelectric Cooling of Electro-Optic Components V.A. Semenyuk ........................ 58-1

58.1 Introduction .............................................................................................................................. 58-1
58.2 Cooling of Intensive Electro-Optic Elements ........................................................................ 58-3
58.3 Cooling of Planar Electro-Optic Elements ............................................................................. 58-9
58.4 Optimal Integration of TE Coolers into an EO Device: A System Approach .................. 58-11
58.5 Conclusion .............................................................................................................................. 58-20
59 Thermoelectric Refrigeration for Mass-Market Applications Montag C. Davis,

Benjamin P. Banney, Peter T. Clarke, Brett R. Manners, and Robert M. Weymouth ......................... 59-1
59.1 Introduction .............................................................................................................................. 59-1
59.2 The Potential of Thermoelectric Cooling .............................................................................. 59-1
59.3 Heat Transfer Systems .............................................................................................................. 59-3
59.4 Thermal Resistance Values ....................................................................................................... 59-5
59.5 Achievable Refrigeration Performance ................................................................................... 59-5
59.6 Mass-Market Applications ....................................................................................................... 59-6
59.7 Other Considerations ............................................................................................................... 59-8
59.8 Conclusion ................................................................................................................................ 59-8

xxii Contents
Appendix I: History of the International Thermoelectric Society C.B. Vining,

D.M. Rowe, J. Stockholm, and K.R. Rao .............................................................................................. AI-1
AI.1 Introduction ............................................................................................................................. AI-1
AI.2 Thermoelectric Activities around the World ........................................................................ AI-2
AI.3 Professor Rao’s Short Course and Founding the ITS .......................................................... AI-4
AI.4 Present Status of the ITS ........................................................................................................ AI-7
Appendix II: Selected Thermoelectric Sources ................................................................................ AII-1

List of Symbols
A sample cross-sectional area e electrical charge of an electron

A cross-sectional area; total area; resonant E electric field
scattering intensity E energy of a charge carrier
A coefficient of T 2 term of electrical E energy of charge carriers, electric field
resistivity of a Kondo lattice system EA activation energy
a coefficient of 2T 2 term of electrical Eb potential barrier height
resistivity of a Kondo impurity Ef electronic energy of the final state of a
system phonon-assisted hop
Å Angstrom unit Ei electronic energy of the initial state of a
Â dimensionless Seebeck tensor phonon-assisted hop
A0 material parameter EF Fermi energy
An, Ap cross-sectional area of the n- and Eg energy band gap
p-legs, respectively Ep energy of a polaron
B magnetic field; elastic constant for hard Evib vibrational energy of a solid
sublattice; magnetic field strength EP “electronic” phonons
B magnetic field F electric-field strength
B0 strength of phonon – electron scattering F function responsible for
C specific heat/unit mass; thermal electron– phonon energy interaction
conductance of thermoelectric F force; pulverizing force
material f fraction of a carrier’s momentum
c ratio of the number of charge carriers that is transferred to sound waves
to the number of available states fi atomic scattering factor
C1(a/d) thin-film correction factor for the f0ð0Þ equilibrium Maxwell function
planar dimensions Fk k-th force field
C2(w/s) thin-film correction factor for the ratio f(k) nonequilibrium part of the electron
of thickness to the contact spacing distribution function
C11 longitudinal elastic constant F(H) structure factor
ck ¼ rk/r component concentration F(H) structure factor
CV specific heat at constant volume F(h) Fermi–Dirac integral
CV specific heat G reciprocal lattice vector
D carrier’s diffusion constant G average temperature gradient
D bandwidth G(q’) form factor of quantum well
D sample density Gi average stiffness constant
d thermal diffusivity (d) and the specific H reciprocal lattice vector
heat (CV) of the sample H reciprocal lattice vector
d/dt ¼ k/kt + ngrad full substantial H(t) heaviside unit step function
time derivative H magnetic field
dS entropy change H magnetic field
e dimensionless electric field h heat transfer rate
xxiii
xxiv List of Symbols
I electrical current L, L Lorenz factor

I electrical current M atomic mass; separation of the chemical
I current in multistage generator potential from the resonant band
I strength of the intra-site exchange center
interaction N number of thermoelements in the
IB Bragg intensity module, degeneracy of spin-orbit
Ii thermodynamic flow level
Io Ioffe criterion N degeneracy of spin-orbit level
Iep, Ipe, Ipp electron – phonon, phonon – electron, n number of charge carriers
and phonon – phonon collision n conduction electron density
integrals n carrier concentration
IB Bragg intensity N number of available states
Ib phonon mean-free path N0 thermal conductance
Ir current ratio Na number of atoms per unit volume
J exchange interaction Ne, Nh equivalent extrema (or valleys) in
J electrical current density conduction or valence bands,
J electrical current density respectively
j total angular momentum nf occupation number of impurity level
!
j current density NÎ impurity density
j0 unit vector of electric current density N0(vq) Planck distribution function
Ji flow of particles or energy Nv number of valleys in conduction or
Ji thermodynamic flow valence band; vacancy
Ji flow of particles or energy concentration
Jk diffusion flow Nq number of phonons of wavevector q
Jq particle current density N(q) nonequilibrium part of the phonon
Jq heat flow distribution function
Jq particle current density N(T) density of acoustic phonons that
Js entropy current density interact with charge carriers at
Js entropy flow density temperature T
K thermal conductance; heat transfer p momentum imparted to sound waves
conductance through a P electrical power, pressure;
thermocouple, thermal conductivity Peltier coefficient
k Boltzmann constant P heating power
k dimensionless heat flow Pba tensor of stresses
K0 kinetic coefficient under small Pc “realistic” power output
temperature gradient P0 electrical power output
Ke electronic thermal conductivity P0 electrical power output of MTEG
KL lattice thermal conductivity Pr power ratio
Kn kinetic coefficient Pmax maximum power output
L length; length of thermoelements P(u) nuclear probability density function
L total length of the sample, P(u) nuclear probability density function
L0 Lorenz number Q heat flow; thermal input
L0 sample distance between the measuring q phonon wavevector
leads or voltage probes q charge of a carrier
Le current carrier cooling length q00 surface heat flux
Le generalized Fermi integral Q` transverse Nernst – Etingshausen
L, Lo Lorenz number coefficient
Lij Onsager coefficient Qc heat pump capacity at cold junction
Lp momentum mean free path of carriers Qh thermal input
Lph thermal phonons mean free path Qh thermal input to MTEG
Lr recombination length Q`
i Nernst– Ettingshausen coefficient
LT characteristic length of temperature Q0 heat rejected
change QP rate of heating or cooling

List of Symbols xxv
R electrical resistance; device resistance; Tav average temperature

electrical resistance of a single TC transition temperature of a
thermocouple; reflectivity superconductor
R MTEG resistance Tc superconducting transition
R^ of dimensionless resistivity temperature
R* effective internal resistance for a Tc cold junction temperature; cold fluid
single thermocouple temperature, superconductivity
RH Hall coefficient transition temperature
Rc electrical contact resistance Tcj cold junction temperature
Rc MTEG contact resistance Te eutectic temperature
Rcc cold temperature contact resistance Th hot junction temperature
Rcc cold temperature MTEG contact Ti atomic temperature factor
resistance Ti atomic temperature factor
Rch hot temperature contact resistance TK Kondo temperature
Rch hot temperature MTEG contact Tk Kondo temperature
resistance T liq liquidus temperature
RC1 contact resistance Tn temperature of n-type leg
RH Hall coefficient Tp temperature of p-type leg
Rl external load resistance TP thermal phonons
ri fractional coordinate TS temperature of the surroundings
Rt total resistance Tw warm fluid temperature
Rt MTEG total resistance Twj warm junction temperature
S entropy DT temperature difference
S entropy, thermic power DTc temperature difference between the
S spin of a magnetic ion electrode at the cold junction and the
S thermopower cold flow
s sound velocity DTteg temperature difference across
s spin quantum number a block of thermoelectric
s elementary volume entropy semiconductor
(local entropy) DTw temperature difference between the
S* transport entropy per particle electrode at the warm junction and
S_ entropy production rate the warm flow
S_ entropy variation rate of unit volume U weighted mobility, Coulomb
S~ e operator combining interaction of interaction energy
electrons with phonons and U Coulomb interaction energy
point defects U internal energy
Sĉ heat exchanging surface area u unit internal energy
corresponding to a single ku2l mean square displacement
thermocouple (cold flow side) Un, Up weighted carrier mobility for electrons
STe thermoelectric Seebeck and holes, respectively
*
coefficient ¼ NBTe STe U(T) phonon energy density
Sw heat exchanging surface area V voltage; terminal voltage; load voltage;
corresponding to a single volume, hybridization energy
thermocouple (warm flow side) between f state and conduction
fT temperature gradient electrons, electrostatic potential
T absolute temperature in Kelvin V electrostatic potential
T absolute temperature V hybridization energy between f state
t modulus of temperature gradient and conduction electrons
T0 temperature of the sample V MTEG load voltage
T0 characteristic temperature (/ TK) v velocity of charged particle
of model v mass transport rate
To magnetic ordering temperature v; u drift velocities of electrons and phonons
t0 unit vector of temperature gradient VA adiabatic voltage

xxvi List of Symbols
Vac critical potential ag phonon-drag thermopower

VE Ettinghausen voltage ai impurity thermoelectric power
VH Hall voltagies due to the Lorentz force an, ap Seebeck coefficient of n- and p-legs
(F ¼ qE ¼ qV/b) aph phonon thermoelectric power
VH Hall voltage apresence Contribution to the Seebeck coefficient
VN Nernst voltage due to a carrier’s presence
VRL Reghi – Leduc voltage atransport Contribution to the Seebeck coefficient
VS Seebeck voltage associated with the mechanism of
Vuc unit cell volume carrier motion
Voc open circuit voltage ar thermoelectric power reference
Voc open circuit voltage electrode
Vopen open terminal voltage as thermoelectric power of the sample
Vr voltage ratio under investigation
VTE Seebeck voltage, VTE ¼ aDT, aTe thermoelectric material Seebeck
plus the resistive or IR voltage, VIR, coefficient
VIR resistive or IR voltage a2T/r power factor (also equal to a2sT)
DV potential difference along a sample b Thomson coefficient nonparabolicity
W ratio of flow of electrical energy, parameter
strength of carrier– phonon x magnetic susceptibility
coupling, energy flux x reduced phonon frequency;
W energy flux thermal conductivity
w thickness of the sample x0 residual magnetic susceptibility
x concentration (number of atoms xb un-enhanced thermoelectric power
in a formula unit) xe electronic thermal conductivity
X(a) electronegativity of element a ximp Impurity contribution to the magnetic
Xi thermodynamic forces susceptibility
Xk thermodynamic force xL lattice thermal conductivity
Xk thermodynamic concentration D energy between ground level and
Xj force giving rise to flows excited spin-orbit level
Xj force giving rise to the flows DC electronic specific heat
DX electronegativity of compounds Dc electronic specific heat
Z thermoelectric figure-of-merit Dg Kondo insulating energy gaps
of material Dg Kondo insulating energy gap
Z reduced phonon frequency DT temperature gradient
Z* optimal Ioffee figure-of-merit d dimensionless Umkehr effect
Ze* Zener criterion d ¼ dc ¼ Rc/R
Zopt optimal figure-of-merit dA elementary work performed
Zc, Znp thermoelectric figure-of-merit of dch ¼ Rch/R
thermocouple di cubic root of atomic volume
ZT dimensionless figure-of-merit 1 electronic energy of an electronic state
1D, 2D, 3D one-, two-, three-dimensional that is shifted by its interaction
a thermoelectric power with phonons
a Seebeck coefficient or thermopower e charge carrier energy, energy
a Seebeck coefficient; thermoelectric e emissivity (0 , e , 1)
power, thermopower, thermal eb potential barrier height
expansion coefficient, coefficient el deformation potential
of T 2 term of electrical resistivity of h reduced energy of charge carrier;
a Kondo impurity system generation efficiency; reduced
a^ seeback coefficient fusion Fermi energy, reduced barrier height
aAB relative Seebeck coefficient or h thermoelectric efficiency
thermopower hc Carnot efficiency
a(E) Seebeck Coefficient for a carrier of hâ
e;p phenomenological coefficients of heat
energy E exchange

List of Symbols xxvii
hintegral integral efficiency ltotal total thermal conductivity

hmax
local maximum local efficiency F ¼ P0/At
hlocal local efficiency F(x) displacement of the soft sublattice atoms
ht thermodynamic efficiency f generator conversion efficiency;
ht MTEG thermodynamic efficiency coefficient of performance
G resonant band width fc ¼ 1+2 dch
Gi effective electron – lattice interaction at P* local Peltier coefficient
the initial state of a phonon- P^ tensor of Peltier coefficients
assisted hop Pab tensor of viscous stresses
Gf effective electron – lattice interaction at Pik Peltier coefficient
the final state of a phonon-assisted p^ dimensionless Peltier tensor
hop m carrier mobility; chemical potential;
Gijk inter-sublattice interaction constant ¼ R0/R
g Carnot efficiency; Thomson coefficient; m* reduced Fermi energy
average anhamonicity of bonds m electrochemical potential
g constant that characterizes thermal ma carrier mobility due to alloy scattering
induced shifts of electronic energy only
levels mc carrier mobility in low carrier
g0 Sommerfeld coefficient of specific heat concentration limit
gG Grüneisen parameter mcl classical Hall mobility
gi impurity contribution to the mH Hall mobility
Sommerfeld coefficient ¼ mn, mp electron and hole mobility, respectively
Ai/li i ¼ n,p mr chemical potential or r-th component
gimp impurity contribution to the V angular frequency
Sommerfeld coefficient V0 average atomic volume
[ Energy w~ electrochemical potential
[F Fermi energy p Peltier coefficient
[f Energy of f level P Peltier coefficient
[j Energy of spin-orbit level c eigenfunction
k total thermal conductivity C ¼ gn/gp
k^ thermal conductivity tensor r electrical resistivity
k* local thermal conductivity coefficient r electrical resistivity; porosity
kE electronic thermal conductivity r^ electric resistivity tensor
contribution r* local resistivity coefficient
kL lattice thermal conductivity r4f 4f density of states
contribution ro residual electrical resistivity
kp lattice thermal conductivity rc electrical contact resistivity
kp lattice thermal conductivity rik components of electric resistivity
kL lattice thermal conductivity tensor
l thermal conductivity; wavelength rn, rp electrical resistivity of n- and p-legs
l0 thermal diffusivity rph phonon contribution to resistivity
l0 virtual crystal thermal conductivity rr “ideal” power output; impurity
lc thermal contact conductivity contribution to the resistivity
le electronic thermal conductivity r(r) electron density distribution
lL lattice thermal conductivity r(r) electron density distribution
lmin minimum lattice thermal conductivity rTe thermoelectric material electrical
of crystals resistivity
ln, lp thermal conductivity of the n- and s electrical conductivity
p-legs s0 electrical conductivity in absence of
ls enhanced thermoelectric power resonant scattering
lst known (standard) thermal conductivity s^ electric conductivity tensor
lTe thermoelectric material thermal sik components of electric conductivity
conductivity tensor

xxviii List of Symbols
sSB Stephan– Boltzmann constant c atomic concentration of an alloy

sSB ¼ 5.7 £ 1028 W-m22-K24 component
t relaxation time for the relaxation of d density; diameter; potential
sound– wave momentum barrier separation
tp ¼ j0 ðt^ t0 Þ local Thomson coefficient dS area element of a constant energy
t, te relaxation time; conduction electron surface in the wave vector space
relaxation time e electronic charge
t0 energy independent factor of f Fermi– Dirac distribution function
relaxation time fi Atomic scattering factor
tac carrier relaxation time due to f(k) nonequilibrium part of electron
acoustic phonon scattering distribution function
timp carrier relaxation time due to fo(ek) Fermi distribution function
ionized impurity scattering h Planck constant; heat transfer
tn Thomson coefficient of the coefficient
n-type leg hec heat transfer conductance between the
tp phonon relaxation time cold flow and the cold electrode
tp Thomson coefficient of the per unit area
p-type leg hew heat transfer conductance between
tpc phonon relaxation time due to the warm flow and the warm
charge carrier scattering electrode per unit area
tpd phonon relaxation time due to hlec heat transfer coefficient between the
point defect scattering cold flow and the inner surface of
tres carrier relaxation time due to the heat transfer tube
resonance scattering hlew heat transfer coefficient between the
tT Thomson coefficient warm flow and the inner surface of
Q^ of dimensionless thermal conductivity the heat transfer tube
QD Debye temperature h2ec heat transfer conductance through the
QE Einstein temperature insulator and the heat transfer tube
QF Fourier mismatch faced to the cold flow per unit area
QJ Joule mismatch h2ew heat transfer conductance through the
QT Thomson mismatch insulator and the heat transfer tube
uE Einstein temperature faced to the warm flow per unity area
v angular frequency; phonon frequency i electric current density
v0 characteristic frequency of j electron flow, total angular momentum
resonance mode j(k) Heisenberg current operator
vD Debye frequency k wave vector; conduction electron
v(e, T) conductivity of electrons on a constant wave vector
energy surface e(k) ¼ const k Boltzmann constant; absorption
vq frequency of a phonon of wavevector q coefficient
in the absence of charge carriers k0, kB Boltzmann constant
Vq frequency of a phonon of wavevector q kT, kL transverse and longitudinal
in the presence of charge carriers components of the electron (or hole)
J deformation potential constant wave vector
j reduced Fermi energy, dimensionless l length; length of thermoelements;
energy of electron width of soliton wall; phonon
jg reduced band-gap mean-free path
jopt optimum reduced Fermi energy le, lp mean-free path of electron or hole,
z Fermi energy, dimensionless energy of respectively
phonon, chemical potential lpb phonon mean-free path for boundary
z chemical potential scattering
a inter-atomic spacing; mean hopping ls barrier width
distance, quantum well width m* density-of-states effective mass
a0 Bohr constant m0 free electron mass

List of Symbols xxix
mc conductivity (initial) effective mass vs sound (phonon) velocity

md density-of-states effective mass; w weight; thermal current density
density-of-states effective mass in a x fractional content; reduced energy of
single valley charge carriers
m1, m2, m3 effective mass components along z figure-of-merit of single material
principal axes
mpL0 longitudinal component of A coefficient of T 2 term of electrical
effective mass resistivity of a Kondo lattice
mpT0 transverse component of effective mass system
n carrier concentration; reflectivity co- ABaC0 area of cooled base
efficient; number of stages in multistage ABaHe area of heated base
generator, electron density AF in area of fin
nf occupation number of impurity level ATe area of one thermoelectric element
nopt optimum carrier concentration Cxt thermal conductance of seal
q electronic charge; thermal flow; elastic cp.Co.in heat capacity of cooled fluid
constants for the soft sublattice CtTe thermoelectric thermal conductance
q wave vector; quantity of heat ¼ Nb*Te GF* kTe
q00 surface heat flux D bandwidth
qk phonon wave vector component effFin fin efficiency ¼ average t of fin/t at base
parallel to quantum well of fin
q` phonon wave vector component GF geometric factor of thermoelectric
perpendicular to quantum well element
q21 reciprocal of penetration depth hFin convection coefficient of fin
qc heat flux at the cold junction Lte length of thermoelectric element
qw heat flux at the warm junction Nbte number of thermoelectric elements in
r scattering parameter; thermal resistivity the module
rH Hall factor PC0 cooling power
ri fractional coordinate Phe heating power
s scattering parameter, spin quantum QCO mass flow rate of cooled fluid
number RCO electrical resistance of cold-side
sph acoustic phonon-drag effect heat exchanger if in circuit
t time ReCo electrical resistance ReTE/2+RCo
t1/2 half-rise time ReHe electrical resistance ReTE/2+RHe
tav average temperature of thermoelectric ReTe thermoelectric electrical resistance
material ¼ Nb*Te rTe/GF
ku 2l mean square displacement RHe electrical resistance of cold-side heat
u mobility; velocity of longitudinal exchanger if in electrical circuit
sound RtBaCo thermal resistance of cooled base
u drift velocity of phonons RtBaHe thermal resistance of heated base
u0 barrier amplitude RtHyCo thermal hydraulic resistance of
ul velocity of sound for polarization l cooled base
ui displacement vector RtHyHe thermal hydraulic resistance of
uij deformation tensor heated base
v velocity; velocity of sound; conduction tFLCo temperature of cooled fluid
electron velocity; heat pulse tFLCo.ex temperature of cooled fluid at exit of
dissipation function building-block
v elastic constants for the soft sublattice tFLCo.in temperature of cooled fluid at inlet of
v drift velocity of electrons building-block
vL average sound (phonon) velocity tFLHe temperature of heated fluid
vp phonon relaxation rate tTeCo temperature of thermoelectric material
vq constant phonon velocity at the cooled end
npR phonon relaxation rate due to resistive tTeHe temperature of thermoelectric material
scattering processes at the heated end

xxx List of Symbols
ADP atomic displacement factor MEM maximum entropy method

AMD accident model document MTEG multicouple (multi-stage)
ASC absolute Seebeck coefficient thermoelectric generator
ASE absolute Seebeck effect NOAA National Oceanic and Atmosphere
BOL beginning of life Administration
CBCF carbon bonded carbon fiber NPS nuclear-powered source
COP coefficient of performance NRAD Nuclear Risk Analysis Document
CVD chemical vapor deposition NRC Nuclear Regulatory Committee
DoD Department of Defense NSC National Security Council
DOE Department of Energy OSTD Office of Science and Technology
EDD electron density distribution Police
EIS environmental impact statement PGEC phonon glass and an electron
EP “electronic” phonons single crystal
EPA Environmental Protection Agency QID quasi-one-dimensional
FEPF fine weave pressed fabric RDD Reference Design Document
GDS ground demonstration system RSC relative Seebeck coefficient
GIS graphic impact shell RSE relative Seebeck emf.
GPHS general purpose heatsource SAR safety analysis report
HMS higher manganese silicides SER safety evaluation report
HSR heatsink resistance SNAP systems for nuclear auxiliary power
HTSC high temperature superconductor SP space power
IAM independent atom model SQL size quantum limit
ICB ion cluster beam TAGS tellurium – antimony –germanium –
INSRP Interagency Nuclear Safety Review silver
Panel TED thermoelectric device
LEC lower expansion coefficient THM traveling heater method
LPE liquid phase epitaxy TP thermal phonons
LTT low-temperature tetragonal phase TZM traveling zone melted
MA mechanical alloying XRD X-ray diffraction
MBE molecular beam epitaxy ZM zone-melting

SECTION I
General Principles and
Theoretical
Considerations

1
General Principles and
Basic Considerations
1.1 Introduction ....................................................................... 1-1

1.2 Thermoelectric and Thermomagnetic Effects ................. 1-2
Seebeck Effect † Peltier Effect † Thomson Effect † The
Kelvin Relationships † Nernst and Ettinghausen Effects
1.3 Thermoelectric Generation and the Figure-of-Merit ..... 1-3
1.4 Thermoelectric Refrigeration and the Coefficient
of Performance ................................................................... 1-6
1.5. Thermoelectric Materials .................................................. 1-7
D.M. Rowe 1.6 Thermocouple Construction and Configurations .......... 1-10
Cardiff University Modules
1.1 Introduction
This chapter serves as an introduction to thermoelectrics and is intended to provide a readily
comprehensive overview of the range of activities associated with this area of scientific endeavor. The
technology revolves around modern-day thermocouples and their application in power generation
and refrigeration. Specific references are not cited as all topics in this chapter are covered in detail
within the Handbook sections. Suggested texts and review articles for further reading are listed in the
bibliography.
Conventional metallic thermocouples as shown in Figure 1.1(a) are made from metal or metal alloys.
They generate small voltages, typically tens of microvolts per degree temperature difference by the
Seebeck effect, when its junction is located in a hot or cold environment compared to the ambient, and
generate small amounts of electrical power when connected to a resistive load. They are used extensively
in the measurement of temperature or as sensors to operate control systems such as those in domestic air
conditioning equipment, refrigerators and central heating units. The thermocouple also operates in
another way when a voltage source is connected across the open ends so that an electric current is driven
through the couple. It acts as a heat pump and effectively cools the junction by the Peltier effect.
However, probably less familiar to the layman is the use of thermocouples made from modern
semiconductors whose material properties and geometry have been tailored specifically to meet the
intended application requirements and possess Seebeck coefficients of hundreds of microvolts per degree.
In bulk devices for generation or cooling applications, the thermocouples have a typical geometry as
shown in Figure 1.1(b) and consist of two ingot-shaped pellets (thermoelements) of semiconducting
material having dimensions of the order of millimeters connected at one end with an electrically
conducting metal strap. In sensors applications increasing use is made of thin film structures as
1-1

1-2 Thermoelectrics Handbook: Macro to nano
FIGURE 1.1 (a) Conventional metal metal/alloy thermocouple; (b) bulk semiconductor thermocouple; (c)
miniature thin film thermocouples.
shown in Figure 1.1(c). Here, the thermocouples, micrometers wide, are laid down by a variety of
techniques onto a supporting electrically insulating thin film substrate.
1.2 Thermoelectric and Thermomagnetic Effects

1.2.1 Seebeck Effect
The thermometric effects which underlie thermoelectric energy conversion can be conveniently discussed
with reference to the schematic of a thermocouple shown in Figure 1.2. It can be considered as a circuit
formed from two dissimilar conductors, a and b (referred to in thermoelectrics as thermocouple legs,
arms, thermoelements, or simply elements and sometimes as pellets by device manufacturers) which are
connected electrically in series but thermally in parallel. If the junctions at A and B are maintained at
different temperatures T1 and T2 and T1 . T2 an open circuit electromotive force (emf), V is developed
between C and D and given by V ¼ aðT1 2 T2 Þ or a ¼ V=DT, which defines the differential Seebeck
coefficient aab between the elements a and b. For small temperature differences the relationship is linear.
Although by convention a is the symbol for the Seebeck coefficient, S is also sometimes used and the
Seebeck coefficient referred to as the thermal emf or thermopower. The sign of a is positive if the emf
causes a current to flow in a clockwise direction around the circuit and is measured in V=K or more often
in mV=K:
A B
b b
C D
FIGURE 1.2 Schematic basic thermocouple.

General Principles and Basic Considerations 1-3
1.2.2 Peltier Effect

If in Figure 1.2 the reverse situation is considered with an external emf source applied across C and D and
a current I flows in a clockwise sense around the circuit then a rate of heating q occurs at one junction
between a and b and a rate of cooling 2q occurs at the other. The ratio of I to q defines the Peltier
coefficient given by p ¼ I=q, is positive if A is heated and B is cooled, and is measured in watts per ampere
or in volts.
1.2.3 Thomson Effect

The last of the thermoelectric effects, the Thomson effect relates to the rate of generation of reversible
heat q which results from the passage of a current along a portion of a single conductor along which there
is a temperature difference DT. Providing the temperature difference is small, q ¼ bIDT where b is the
Thomson coefficient. The units of b are the same as those of the Seebeck coefficient V=K: Although the
Thomson effect is not of primary importance in thermoelectric devices it should not be neglected in
detailed calculations.
1.2.4 The Kelvin Relationships

The above three thermoelectric coefficients are elated by the Kelvin relationships:
daab b 2 bb
aab ¼ pab =T and ¼ a
dT T
These relationships can be derived using irreversible thermodynamics. Their validity has been
demonstrated for many thermoelectric materials and it is assumed that they hold for all materials used in
thermoelectric applications.
1.2.5 Nernst and Ettinghausen Effects

All the thermoelectric coefficients discussed above are in general dependent on magnetic field B with the
principal parameters used in thermoelectrics, the Seebeck and Peltier effects having corresponding
thermomagnetic coefficients, the Nernst lNl and Ettinghausen lPl effects, respectively. In the Nernst effect
a transverse electric field EY is produced by a longitudinal temperature gradient dT=dx in the presence of
a magnetic field BZ and in the Ettinghausen effect a transverse temperature gradient is produced by a
longitudinal electric current with the thermo magnetic coefficients given by
EY . dT
lNl ¼
BZ dx
1 . dT
lPl ¼
IX BZ dy
1.3 Thermoelectric Generation and the Figure-of-Merit

A thermoelectric converter is a heat engine and like all heat engines it obeys the laws of thermodynamics.
If we first consider the converter operating as an ideal generator in which there are no heat losses, the
efficiency is defined as the ratio of the electrical power delivered to the load to the heat absorbed at the
hot junction. Expressions for the important parameters in thermoelectric generation can readily be
derived by considering the simplest generator consisting of a single thermocouple with thermoelements
fabricated from n- and p-type semiconductors as shown in Figure 1.3(upper).

TH I TC
n-type
HEAT input
p-type
Electrical
power
output
The Seebeck effect (Thermoelectric generation)
TC I TH
n-type
+
HEAT absorbed HEAT rejected
p-type
Electrical
power
input
The Peltier effect (Thermoelectric cooling)
FIGURE 1.3 Thermoelectric generator (upper); thermoelectric refrigerator (lower).
The efficiency of the generator is given by

energy supplied to the load
f¼
heat energy absorbed at hot junction
If it is assumed that the electrical conductivities, thermal conductivities, and Seebeck coefficients of a
and b are constant within an arm, and that the contact resistances at the hot and cold junctions are
negligible compared with the sum of the arm resistance, then the efficiency can be expressed as
I2R
f¼
1 2
aab ITH ¼ l0 ðTH 2 TC Þ 2 I R
2
where l0 is the thermal conductance of a and b in parallel and R is the series resistance of a and b. In
thermoelectric materials s; l0 ; and a change with temperature, and in both, generation and
refrigeration should be taken into account. However, the simple expression obtained for the
efficiency can still be employed with an acceptable degree of accuracy if approximate averages of
values are adopted for these parameters over the temperature range of interest. Appropriate allowances
can also be made for contact resistance.
Efficiency is clearly a function of the ratio of the load resistance to the sum of the generator arm
resistances, and at maximum power output it can be shown that
TH 2 TC
fp ¼ 1
3TH TC 4
þ þ
2 2 Zc
while the maximum efficiency
fmax ¼ hc g
where
TH 2 TC
hc ¼
TH

qffiffiffiffiffiffiffiffiffiffi
1 þ Zc T 2 1
g ¼ qffiffiffiffiffiffiffiffiffiffi
T
1 þ Zc T þ C
TH
and
TH þ TC
T¼
2
and
a2ab
Zc ðthe figure-of -merit of the coupleÞ ¼
Rl0
The maximum efficiency is thus the product of the Carnot efficiency, which is clearly less than
unity, and g, which embodies the parameters of the materials.
If the geometries of a and b are matched to minimize heat absorption, then
a2ab
Zc ¼ " 1 1
#2
la 2 l 2
þ b
sa sb
In practice, the two arms of the junction have similar material constants, in which case the concept of a
figure-of-merit for a material is employed and given by
a2 s
Z¼
l
where a2 s is referred to as the electrical power factor.
The above relationships have been derived assuming that the thermoelectric parameters which occur
in the figure-of-merit are independent to temperature. Although generally this is not the case, assuming
an average value provides results which are within 10% of the true value.
The conversion efficiency as a function of operating temperature difference and for a range of values of
the material’s figure-of-merit is displayed in Figure 1.4. Evidently an increase in temperature difference
provides a corresponding increase in available heat for conversion as dictated by the Carnot efficiency, so
large temperature differences are desirable. As a ballpark figure a thermocouple fabricated from
Conversion efficiency %
Cold junction at 300K Z × 10 − 3
40 4
3
30 2
20 1
10
0
300 450 600 750 900 1050 1200 1350 1500 Temperature (K)
0 33% 50% 60% 66% 71% 75% 77% 80% Carnot efficiency
FIGURE 1.4 Generating efficiency as a function of temperature and thermocouple material figure-of-merit.

thermoelement materials with an average figure-of-merit of 3 £ 1023/K would have an efficiency of 20%
when operated over a temperature difference of 500 K.
1.4 Thermoelectric Refrigeration and the Coefficient

of Performance
The performance of any refrigerator is in general expressed by its coefficient of performance. This is given
by the cooling power produced divided by the rate at which electrical energy is supplied. In Figure 1.3
(lower) is illustrated an ideal thermoelectric circuit upon which the operation of a thermoelectric cooling
device is based as is the case of a generation (Section 1.3). The circuit is identical to that of a generator
discussed above, but in this case a direct current is passed through the thermocouple circuit and heat is
pumped from TC to TH. If TH . TC the device operates as a refrigerator.
As a result of the Peltier effect the rate of heat pumping at the junction TC is given by pabI.
Using the Kelvin relationship
aab ¼ pab =TC
where aab is the Seebeck coefficient of the junction we can write
pab I ¼ aab ðTM 2 DT=2ÞI
TM is the mean absolute temperature and DT the temperature difference TH –TC.

The cooling effect at the source junction is opposed by Joule heating in the thermoelements and by
heat conducted from the hot junctions. Half the overall Joule heating travels to each of the junctions.
Thus neglecting the Thomson effect, the rate of absorption of heat from the source is given by
1 2
Qab ¼ aab TC I 2 I R 2 KðTH 2 TC Þ
2
An input power by
P ¼ aab DTI þ I 2 R
where the potential difference applied to the thermocouple is used in part to overcome the
electrical resistance of the thermoelements and to balance the Seebeck voltage which results from the
temperature difference between the junctions.
The energy efficiency of a refrigerator is measured by its coefficient of performance, COP, defined as
1
heat absorbed aab ITC 2 I 2 R 2 KDT
COP ¼ ¼ 2
electrical power input aab IDT þ I 2 R
K is the thermal conductance of the thermoelements in parallel, and R is the electrical resistance of
the thermoelements in series. Evidently the coefficient of performance for a given temperature difference
is dependent on the current I.
The current I 0 for maximum cooling power is given by
ðaab ÞTC
I0 ¼
R
with the corresponding COP
1 2
ZTC 2 DT
f ¼ 2
0
ZTH TC

2.0
1.5
1.25
4×
0.5
3 × 10 −30
2 × 10 −3 k −1
10 − 3
2=
10
−3
0
0 20 40 60 80 100
∆T °C
FIGURE 1.5 Theoretical coefficient of performance of a thermoelectric module plotted against temperature
difference for different Z values, mean temperature.
The maximum temperature difference is given by

1 2
ðTH 2 TC Þ ¼ ZT and the current I for maximum coefficient of performance
2 C
aDT
I 00 ¼ 1
Rð1 þ ZTM Þ 2 2 1
with the maximum coefficient of performance
1 TH
TC ð1 þ ZTM Þ 2 2
TC
fmax ¼
1
ðTH 2 TC Þ ð1 þ ZTM Þ 2 þ 1
Evidently the figure-of-merit Z determines both the maximum temperature difference that can be
achieved and also the maximum coefficient of performance. The dependence of fmax with Z value
for different temperature differences is shown in Figure 1.5 and the dependence of the maximum
temperature difference with Z in Figure 1.6.
1.5. Thermoelectric Materials

One of the parameters that is used in the classification of materials is the electrical conductivity. Metals
have a high electrical conductivity while in insulators the conductivity is very low and under normal
conditions is taken as zero with semiconductors occupying an intermediate position between the two.
The electrical conductivity is a reflection of the charge carrier concentration and all three parameters
which occur in the figure-of-merit are functions of carrier concentration. The electrical conductivity
increases with increase in carrier concentration as shown in Figure 1.7 while the Seebeck coefficient
decreases, with the electrical power factor maximizing at a carrier concentration of around 1025/cm. The
electronic contribution to the thermal conductivity le, which in thermoelectric materials is generally
around 1/3 of the total thermal conductivity, also increases with carrier concentration. Evidently the
figure-of-merit optimizes at carrier concentrations which corresponds to semiconductor materials.
Consequently, semiconductors are the materials most researched for thermoelectric applications.
Thermoelectric phenomena are exhibited in almost all conducting materials (except for supercon-
ductors below Tc ). Because the figure-of-merit varies with temperature a more meaningful measure of

100
80
Max DT=75°C
60
∆Tmax
40
20
Best available Z value
0
0 1 2 3 4 5
Z (10−3 K−1)
FIGURE 1.6 Theoretical maximum temperature difference of a thermoelectric module plotted against Z at a
hot-side temperature of 298 K (258C).
performance is the dimensionless figure-of-merit ZT where T is absolute temperature However, only

those materials which possess a ZT . 0:5 are usually regarded as thermoelectric materials.
Established thermoelectric materials (those which are employed in commercial applications) can be
conveniently divided into three groupings with each dependent upon the temperature range of operation
(Figure 1.8). Alloys based on bismuth in combinations with antimony, tellurium, and selenium are
referred to as low-temperature materials and can be used at temperatures up to around 450 K. These are
the materials universally employed in thermoelectric refrigeration and have no serious contenders for
Electrical
a power factor s s
a Electrical
Seebeck a s2 conductivity
coefficient
In carrier concentration(n)
1 × 1019 cm−3
l Electronic thermal
Thermal le conductivity
conductivity
Loffice thermal
lL conductivity
In carrier concentration(n)
Insulators Semiconductors Metals
FIGURE 1.7 Schematic dependence of electrical conductivity, Seebeck coefficient, power factor, and thermal
conductivity on concentration of free carriers.

4.0
Sb-BiTe-Se
Bi2Te3-75Sb2Te3
(p-TYPE)
Z (K−1 × 103 ) 3.0
Bi2Te3-25Bi2Se3
2.0 (n-TYPE)
4N-PbTe
3N-PbTe ZT = 1
1.0
SiGe (n-TYPE)
SiGe (p-TYPE)
0
0 200 400 600 800
Temperature (°C)
FIGURE 1.8 Performance of the established thermoelectric materials.
applications over this temperature regime. The intermediate temperature range up to around 850 K is
the regime of materials based on lead telluride while thermoelements employed at the highest
temperatures are fabricated from silicon germanium alloys and operate up to 1300 K.
Although the abovementioned materials still remain the cornerstone for commercial applications in
thermoelectric generation and refrigeration, significant advances have been made in synthesizing new
materials and fabricating material structures with improved thermoelectric performance. Efforts have
focused on improving the figure-of-merit by reducing the lattice thermal conductivity. Two research
avenues are currently being pursued. One is a search for so-called ‘phonon glass-electronic crystals’ in
which it is proposed that crystal structures containing weakly bound atoms or molecules that “rattle”
within an atomic cage should conduct heat like a glass, but conduct electricity like a crystal. Candidate
materials receiving considerable attention are the filled skutterudites and the clathrates.
During the past decade material scientists have been optimistic in their belief that low-dimensional
structures such as quantum wells (materials which are so thin as to be essentially of two dimensions (2D),
quantum wires (extremely small cross-section and considered to be of one dimension (1D), and referred
to as nanowires) quantum dots which are quantum confined in all directions and superlattices (a
multiple-layered structure of quantum wells) will provide a route for achieving significantly improved
thermoelectric figures-of-merit. The expectation is that the reduced dimensions of these structures will
result in an increase in phonon interface scattering and a consequent reduction in lattice thermal
conductivity.
Although low-dimensional structures would find immediate application in microelectronics, at
present the technology is expensive and applying it to bulk devices problematic. In some respects
nanowires appear a more attractive proposition for thermoelectric applications than quantum well
superlattices because the geometry of the current flow is more favorable and the fabrication process more
compatible with integrated technology than MBE.
Attempts are also being made to improve the competitiveness of thermoelectric material in directions
other than the figure-of-merit. Efforts have focused for example on increasing the electrical power factor,
decreasing cost, and developing environmentally friendly materials. As examples, when the fuel cost is
low or essentially free, as in waste heat recovery, then the cost per watt is mainly determined by the power
per unit area and the operating period. The rare-earth compounds YbAl3, although possessing a relatively

low figure-of-merit, has a power factor almost three times that of bismuth telluride while MgSn has
almost the same performance but costs less than a quarter of the price.
1.6 Thermocouple Construction and Configurations

In parallel with efforts to identify and syntheses materials and fabricate structures with increased
thermoelectric figures-of-merit, there has been a sustained effort to improve the conversion performance
of thermocouples in generation application by optimizing their performance over the temperature range
of operation. A thermoelectric material operates at its maximum figure-of-merit at a specific
temperature. Consequently when operating over a wide temperature range the majority of the
thermoelement material is operating below its potential maximum performance. Materials can be
prepared in which the carrier concentration along the thermoelement length is tailored to match the
required value for optimizing the figure-of-merit at each position along the operating temperature
gradient. This functionally graded thermoelectric material (FGTM) can be prepared using the Bridgman
technique. This has been successful in low-temperature materials for example in p-type bismuth telluride
materials using a double doping technique. However in n-type crystals the gradient of thermoelectric
properties along the pulled ingot length is in general insufficient to use the material as a FGTM. In this
case, the thermoelectric performance of the n-type thermoelement can be improved by segmentation. In
this arrangement two materials are joined or segmented together, each with its figure-of-merit optimized
for a different temperature range. In Figure 1.9 is displayed a thermocouple arrangement fabricated from
a functionally graded p-type leg and a segmented n-type leg. In principle this technique can be extended
to higher-temperature materials.
An example of a multisegmented generator is shown schematically in Figure 1.10. Under development
for applications recovering automobile waste exhaust heat, the cold-side sections of both elements are
comprised of established materials based on bismuth telluride. The hot-side sections of the p- and n-type
elements consist of high-performance materials under development, a cobalt-filled skutterudite and a
cobalt antimonide clathrate, respectively, with zinc antimonide segmented into the p-type leg to operate
over the intermediate temperature range. A 15% conversion efficiency has been obtained in prototype
generators when operated over a temperature difference of around 700 K.
FIGURE 1.9 Functionally graded and segmented thermoelements.

T (°C) HOT-SIDE T (°C)
700°C 700°C
p-type n-type
Ce filled CoSb3
skutterudite
400°C
p-type Zn4Sb3
150°C 250°C
p-type Bi0.25Sb0.75Te3 n-type Bi2Te2.7Se0.3
Room Room
temperature COLD-SIDE temperature
LOAD
FIGURE 1.10 High-performance multisegmented thermoelectric generator.
1.6.1 Modules
The voltage output from semiconductor thermocouples remains relatively low, hundreds of microvolts
per degree, and in practice a large number of thermocouples are connected electrically in series and
thermally in parallel by sandwiching them between two high thermal conductivity but low electrical
conductivity ceramic plates to form a module (Figure 1.10). The module is the building-block of a
thermoelectric conversion system and its general construction is very similar for both generator and
refrigerating applications. Ideally the geometry of the thermoelements should be wire-like (long and
thin) for generation and squat (short and fat) for refrigeration.
A cutaway of a typical refrigerating (Peltier) module is shown in Figure 1.11.
Sizes can vary from 1.5 mm2 for a single thermocouple module to more than 50 mm2 for a multi-
element module. The maximum temperature difference hat can be achieved with single-stage module is
given by 12 ZT 2 : However it is possible to increase this temperature difference by operating the coolers in
cascade with the modules arranged in pick-a-back with the first stage of the cascade serving as a low-
temperature heat-sink for the second stage and so on. A selection of modules including a two- and five-
stage one are shown in Figure 1.12. The pyramidal appearance reflects the requirement that the cooling
FIGURE 1.11 Cutaway of a typical Peltier cooler.

FIGURE 1.12 Selection of cooling (Peltier) modules.
capacity of the higher-temperature stages should be greater than those which operate at lower
temperatures. Also shown in Figure 1.13 is the cold-side temperature as a function of number of stages.
A practical limiting factor to the number of stages is the interstage thermal resistance although six-stage
thermoelectric coolers are commercially available.
Until relatively recently commercially available thermoelectric modules were designed for operation in
the refrigerating (Peltier) mode and it is only in the last 5 to 10 years or so that thermoelectric power
generating modules have become commercially available with their thermoelement geometry and
material composition tailored for this application. Previously, thermoelectric generating modules were
an integral component of a custom-built thermoelectric generating system designed for a specific
application and they could not be obtained separately. A typical example is the multicouple shown in
Figure 1.14 which was developed specifically for application on U.S. space missions. It consists of 40
thermoelectric elements, with silicon germanium gallium phosphide forming the n-leg and fine grained
silicon germanium the p-leg. The extremely advanced level of material technology achieved in
thermoelectrics enables this device to operate unattended for decades at temperatures around 1300 K.
The worldwide concern about the harmful effect of global warming and the recognition that
thermoelectric technology offers an environmentally friendly method of converting waste heat into
electrical power has resulted in the commercial availability of modules designed for generation.
10
Vacuum 0.13 Pa
9
Dry nitrogen
8 Hot-side temperature = 300 K
7
Number of Stages
293 273 253 233 213 193 173 153

T(K)
Cold-side temperature
FIGURE 1.13 Dependence of cold-side temperature on number of stages.

FIGURE 1.14 Modular-RTG multicouple.
Although not exhaustive, a list of module manufacturers/suppliers is given in Appendix II.
Bibliography
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Cadoff I.B. and Miller E., eds., Thermoelectric Materials and Devices, Reinhold, New York, 1959.
Bateman, P.J., Thermoelectric power generation, Contemporary Physics, 2, 302 –311, 1960.
Goldsmid, H.J., Applications of Thermoelectricity, Methuen Monograph, London, 1960.
Putley, E.H., The Hall Effect and Related Phenomena, Butterworths, Sevenoaks, Kent, 1960.
Ure R.W. and Heikes R.R., eds., Thermoelectricity; Science and Engineering, Interscience, London, 1961.
Beer, A.C., Galvanomagnetic Effects in Semiconductors, Academic Press, New York, 1963.
Burshteyn, A.J., Semiconductor Thermoelectric Devices, Temple Press, London, 1964.
Harman, T.C., Honig, J.M., Thermoelectric and Thermomagnetic Effects and Applications, McGraw-Hill,
New York, 1967.
Rosi, F.D., Thermoelectricity and thermoelectric power generation, Solid-State Electronics, 11, 833 –868,
1968.
Wright, D.A., Materials for direct conversion thermoelectric generators, Metallurgical Reviews, 15,
147– 160, 1970.
Rowe, D.M., Thermoelectric power generation, Proc. IEE, Vol. 125, 11R, November 1978.
Rowe, D.M., and Bhandari, C.M., Modern thermoelectrics, Holt Technology, 1983.
Goldsmid, H.J., Electronic Refrigeration, Pion Limited, London, UK, 1986.
Rowe D.M., ed., Handbook of Thermoelectrics, CRC Press, Boca Raton, FL, 1994.
Nolas, G.H., Sharp, G.J., and Goldsmid, H.J., Thermoelectrics, Springer, Berlin, 2001.
Proceedings of Thermoelectric Conferences

Proceedings of International Thermoelectric conference 1976 to present. Available from IEEE at
http://www.its.org/proceedings/.

Proceedings of European Conferences/Workshops on Thermoelectrics 1987–present. Information

available from Prof. D.M. Rowe, e-mail: RoweDMI@Cardiff.ac.uk or Prof. H. Scherrer, e-mail:
scherrer@mines.u-nancy.fr.
Proceedings of the International Forum on Thermoelectrics, published in the J. Thermoelect. 1994 –
present. Available from Prof. L Anatychuk, e-mail: anatych@inst.cv.ua.
Proceedings of Japanese Symposium on Thermoelectrics (in Japanese) 1997– present. Information
available from Prof. T. Kajikawa, e-mail: kajikawa@elec.shonan-it.ac.jp.

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Parameter Name Restriction Remark
Io ¼ ZT Ioffe criterion 0 # ZT , 1 For isotropic medium
Ze Zener criterion 0 # Ze p , 1
Ze
; a p Generalized Zener criterion Generalized

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5 Chapter 5 Effects of Charge
Carriers'Interactions on Seebeck
Coefficients
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motion, Phys. Rev. Lett., 35, 882, 1975.
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6 Chapter 6 Thermal Conductivity of
Semiconductors with Complex Crystal
Structures
1. Golikova, O.A., Zaitsev, V.K., Orlov, V.M., Petrov,

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2. Zaitsev, V.K., Thermoelectric properties of anisotropic

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3. Cohn, J.L., Nolas, G.S., Fessatidis, V., Metcalf, T.H.,

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14. Zaitsev, V.K., Fedorov, M.I., Rakhimov, K.A.,

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15. Hahn, H., Schulze, H., and Secher, L.,

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19. Leibfried, G. and Schlomann, E., Nachr. Akad. Wiss.

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20. Roufosse, M. and Klemens, P.G., Thermal conductivity of

complex dielectric crystals, Phys. Rev. B, 7, 5379, 1973.
21. Ioffe, A.F., Semiconductors in Modern Physics,

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22. Kittel, C., Introduction to Solid State Physics, 2nd

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23. Anderson, O.L., In Physical Acoustics: Principles

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7 Chapter 7 A Chemical Approacht o the
First-Principles Modeling of Novel
Thermoelectric Materials
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Harrison, N.M., Orlando, R., and ZicovichWilson, C.M.,
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2. Elliott, S., The Physics and Chemistry of Solids, Wiley,

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3. Bertini, L. and Gatti, C., ELTRAP, CNR-ISTM, Milan, 2003.
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5. Gatti, C., TOPOND98 User’s Manual, CNR-ISTM, Milan, 1999.
6. Slack, G.A., New materials and performance limits for

thermoelectric cooling. In CRC Handbook of Thermoelectrics,
D.M. Rowe, ed. CRC Press, Boca Raton, FL, chap. 34, 1995.
7. Bryan, J.D., Blake, N.P., Metiu, H., Iversen, B.B.,

Poulsen, R.D., and Bentien, A., Nonstoichiometry and
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8. Blake, N.P., Bryan, D., Latturner, S., Møllnitz, L.,

Stucky, G.D., and Metiu, H., Structure and stability of the
clathrates Ba 8 Ga 16 Ge 30 , Sr 8 Ga 16 Ge 30 , Ba 8 Ga 16
Si 30 and Ba 8 In 16 Sn 30 , J. Chem. Phys., 114, 10063,
2001. 0 0 200 400 600 600 A 12 Sb 10 A 11 BCSb 10 A 10
BCDSb 10 0.5 α 2 σ ( m W / K 2 c m ) Doping level
(e/formula unit) 1 1.5 2
FIGURE 7.10 Power factor a 2 s at 700 K as a function of

the doping level in the b-ZnSb crystal. Zero doping level
corresponds to a crystal cell with stoichiometry Zn 12 Sb

10 ; the insertion of 2 e/cell corresponds to a 13-Zn atoms
cell.
The power factor is computed applying the frozen band

approximation to the band structures of A 12 Sb 10 , A 11
BCSb 10 ,
and A 10 BCDSb 10 .
9. Bentien, A., Palmqvist, A.E.C., Bryan, J.D., Latturner,
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10. Bentien, A., Nishibori, E., Paschen, S., and Iversen,

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Guest-framework interaction in type I inorganic clathrates
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12. Sales, B.C., Mandrus, D., Chakoumakos, B.C., Keppens,

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Holmgren, L., Iversen, B.B., Mueller, E., Muhammed, M.,
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D bandwidth
H magnetic field
J exchange interaction
n kinetic coefficients
0 Lorenz number
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S thermopower
T absolute temperature
0 characteristic temperature (/ T K ) of model in Ref. [12]
c superconducting transition temperature
T
K Kondo temperature
U Coulomb interaction energy
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electrons
ZT dimensionless thermoelectric figure-of-merit
a coefficient of 2T 2 term of electrical resistivity of a

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j total angular momentum
B Boltzmann constant
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Appendix 18A
Relaxation Times
Consider t ep ð1 k Þ and k t p l for the system of 2D

electrons, scattered by deformation potential of 3D
phonons. Suppose the quantum well width is small enough,

i.e. T k =T ’ ,, 1: In this case, in the
form factor Gðq ’ Þ the component q ’ can be replaced by q

and integration over angles is performed
analytically: t 21 ep ðkÞ ¼ 2m J 2 p 2 " 2 u r I 1 ; kt p l

¼ I 2 I 1 ð18:A1Þ
where I 1 I 2 { ! ¼ ð 1 QðkÞ 1 t p ðqÞ { ! {N 0 ð v q Þ þ f

0 ð1 k þ " v q Þ}G 2 ðqÞDðq; kÞqdq ð18:A2Þ
Dðq; kÞ ¼ lql 4k 2 p 2 1 2 bq ffiffiffiffiffiffiffiffiffi p 2 1 2 p 2 2 p K

ffiffiffiffiffiffiffiffiffiffi q 2 2 p 2 2 p 2 1 2 p 2 2 s 0 @ 1 A 2 ffiffiffiffiffiffiffiffiffi
p 2 1 2 p 2 2 q E ffiffiffiffiffiffiffiffiffiffi q 2 2 p 2 2 p 2 1 2 p 2 2 s 0
@ 1 A for q 2 , p 2 1 q 2 2 bq ffiffiffiffiffiffiffiffiffi q 2 2 p 2 2 p K
ffiffiffiffiffiffiffiffiffiffi p 2 1 2 p 2 2 q 2 2 p 2 2 s 0 @ 1 A 2 ffiffiffiffiffiffiffiffiffi
q 2 2 p 2 2 q E ffiffiffiffiffiffiffiffiffiffi p 2 1 2 p 2 2 q 2 2 p 2 2 s 0 @
1 A for q 2 . p 2 1 8 > > > > > > < > > > > > > : ð18:A3Þ
QðkÞ ¼ b2 2k for k , b; 2k 2 = b for k $ b; ( p 1 ¼
ffiffiffiffiffiffiffiffiffiffi k 2 þ bq q þ k; p 2 ¼ ffiffiffiffiffiffiffiffiffiffi k 2 þ bq q 2 k
KðxÞ and EðxÞ are the complete elliptic integrals of the

first and second kind, and b ¼ 2um=" is
the abscissa of the point of intersection of phonon and

electron spectrums. The function Dðq; kÞ
logarithmically diverges at q 2 ! p 2 1 and tends to p=4 at

q 2 .. p 2 1 : In most cases, the values k .. b are of
interest. In this region, Dðq; kÞ can be approximated by

the function Dð hÞ ¼ h½KðhÞ2 EðhÞ for h , 1 h 2 ½Kð1= hÞ2
Eð1=hÞ for h . 1 ( ð18:A4Þ
where h ¼ lql=2k: In the region lql ,, 2k function DðhÞ <

ph 3 =4: For a large h the dependence DðhÞ; as
well as Dðq; kÞ; tends to p=4:

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FIGURE 25.6 Transport properties of the Bi 2 Te 3

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Sb
Te 3’ p 575 21 3.2 244 92 1.6 1.6
Sb
Te 3// p 605 10 1.9 313 83 5.6 0.6
Bi
Sb 32 Te 60 p 540 4.8 10 176 194 1.3 3.0
Bi
10
Sb 30 Te 60 p 540 3.5 13 177 225 1.4 2.9
Bi
Sb 31 Te 60 p 530 3.9 8.89 190 206 1.5 3.2
Bi
40
Sb 57 Te 3 n 580 4.0 11 140 223 1.6 2.8
Bi
40
Te 58.5 Se 1.5 n 580 4.3 11 150 230 1.7 2.9
Column n-p, type of conduction; T (8C), saturation

temperature in 8C; C p ; carrier concentration 10 19 cm 23
; r, resistivity
mVm; mH, mobility of carriers cm 2 v 21 sec 21 ; a,

absolute Seebeck coefficient mV K 21 ; l, thermal
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28 Chapter 28 Bi – Sb Alloys
1. Smith, G.E. and Wolfe, R., Thermoelectric properties of

bismuth–antimony alloys, J. Appl. Phys., 33(3), 841–846,
1962.
2. Wolfe, R. and Smith, G.E., Effects of a magnetic field on

the thermoelectric properties of a bismuth–antimony alloys,
Appl. Phys. Lett., 1(1), 5, 1962.
3. Ivanov, G.A., Kulikov, V.A., Naletov, V.L., Panarin,

A.F., and Regel, A.R., Figure-of-merit undoped and doped
Bi–Sb alloys in magnetic field, Fizika and tehknika
poluprovodnikov, 6(7), 1296–1299, (in Russian), 1972.
4. Yim, W.M. and Amith, A., Bi–Sb alloys for

magnetothermoelectric and thermomagnetic cooling, Solid
State Electron., 15(10), 1141–1165, 1972.
5. Zemskov, V.S., Belaya, A.D., and Borodin, P.G.,

Thermoelectric and magnetothermoelectric figure-of-merit Bi
and Bi–Sb alloys, Izvestia Akademia Nauk SSSR
Neorganicheskie Materially, 18(6), 1154–1157, (in Russian),
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6. Hansen, O.P. and Nielsen, H., Magneto-thermoelectric

power of bismuth in weak magnetic fields, Phys. Status
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7. Uher, C. and Goldsmid, H.J., The magneto-Seebeck

coefficient of bismuth single crystls, Phys. Status Solidi
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8. Hansen, O.P., Cheruvier, E., Michenaud, J.-P., and Issi,

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7, 1–44, 1963.
11. Cohen, M.H., Falicov, L.M., and Golin, S., Crystal

chemistry and band structures of the group V semimetals and
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12. Goldsmid, H.J., Bismuth–antimony alloys, Phys. Status

Solidi (a), 1(1), 7–28, 1970.
13. Dresselhaus, M.S., Electronic properties of the group V

semimetals, J. Phys. Chem. Solids, 32(Suppl. 1), 3–33,
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14. Issi, J.-P., Low temperature transport properties of

the group V semimetals, Aust. J. Phys., 32(6), 585–628,
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15. Holl, I.J. and Koenig, S.H., Transport Properties and

Band Structure in Bi, Sb and Bi–Sb Alloys, IBM J. Res.
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16. Golin, S., Band model for bismuth–antimony alloys,

Phys. Rev., 176(3), 830–832, 1968.
17. McClure, J.M. and Choi, K.H., Energy band model and
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Transport phenomena peculiarities caused of intervalley and
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effect in an extrinsic Bi–Sb alloys, Phys. Lett., 27A(6),
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28. Zemskov, V.S., Belaya, A.D., and Kojemyakin, G.N.,

Thermoand magnetothermoelectrics properties of the Bi–Sb
alloys with 9 at.% and 15 at.% antimony, doped and undoped
tellurium. Dep. v VINITI, N4905-80, p. 52, (in Russian),
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29 Chapter 29 Thermoelectrics on the Base
of Solid Solutions of Mg2BIV Compounds
(BIV = Si, Ge, Sn)
1. Nikitin, E.N., Bazanov, V.G., and Tarasov, V.I., The

thermoelectric properties of solid solution Mg 2 Si–Mg 2
Sn, Sov. Phys. Sol. State, 3, 2648, 1961.
2. Labotz, R.J., Mason, D.R., and O’Kane, D.F., The

thermoelectric properties of mixed crystals Mg 2 Ge x Si
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3. Nicolau, M.C., Material for direct thermoelectric energy

conversion with a high figure of merit, Proceedings of the
2nd International Conference on Thermoelectric Energy
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1976.
4. Noda, Y., Kon, H., Furukawa, Y., Nishida, I.A., and

Masumoto, K., Temperature dependence of thermoelectric
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851, 1992.
5. Hansen, M., Anderko, K., and Elliot, R., The structures

of binary alloys, M. Metallurgia, 1970.
6. Sacklowski, A., Ann. Physik., 77, 241, 1925.
7. Grosch, G.H. and Range, K.J., Studies on AB 2 -type

intermetallic compounds. I.Mg 2 Ge andMg 2 Sn:
single-crystal structure refinement and ab inito
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8. Busch, G. and Winkler, U., Electrische Leitfa ¨ higkeit

von Mischkristallen intermetallisher Verbindungen, Helv.
Phys. Acta, 26, 578, 1953. 0.8 1 2 3 4 5 0.6 0.4 Z T 0.2
0.0 300 400 500 600 700 800 T, K
FIGURE 29.12 Thermoelectric figure-of-merit for someMg 2 Si

12x Sn x solid solutions. 1 to 3, Mg 2 Si 0.7 Sn 0.3
(samples
of various electron concentration); 4, Mg 2 Si 0.8 Sn 0.2 ;

5, Mg 2 Si 0.6 Sn 0.4 .
9. Bolshakov, K.A., Buljonkov, N.A., Fedorov, P.I., Bull

izobr. N45. Patent of U.S.S.R. N 150495, 1962.
10. Clark, C.R., Wright, C., Suryanarayana, C., Baburaj,

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11. Xiaoping, Niu. and Li, Lu., Formation of magnesium

silicide by mechanical alloying, Adv. Perform. Mater., 4,
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12. Riffel, M. and Schilz, J., Influence of production

parameters on the thermoelectric properties of Mg 2 Si.
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13. Schilz, J., Muller, E., Kaysser, W.A., Langer, G.,

Lugscheider, E., Schiller, G., and Henue, R., Graded
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14. Ewald, P.P. and Hermann, C. Strukturbericht 1913-28.

Akad. Verlagsges. m.b.H., Leipzig, 1931.
15. Winkler, U., Die electrischen eigenschaften der

intermetallisher verbindungen Mg 2 Si, Mg 2 Ge, Mg 2 Sn und
Mg 2 P, Helv. Phys. Acta, 28, 633, 1955.
16. Muntjanu, Sh., Sokolov, E.B., and Makarov, E.S., The

study of system Mg 2 Sn–Mg 2 Si, Izv. AN SSSR, Neorg.
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17. Klemm, W. and Westlinning, H., Untersuchungen u ¨ ber

die Verbindungen des Magnesiums mit den Elementen der
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18. Makarov, E.S., Muntjanu, Sh., Sokolov, E.B., and

Slesareva, G.A., The study of system Mg 2 Pb– Mg 2 Ge, Izv.
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19. Gottfried, C. and Schossberger, F. Strukturbericht.

Akad. Verlagsges. m.b.H., Leipzig, 1937.
20. Zintl, E. and Kaiser, H., U ¨ ber die Fa ¨ higkeit der

Elemente zur Bildung negativer Ionen, Z. Anorg. Allg.
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21. Makarov, E.S., Muntjanu, Sh., Sokolov, E.B., and

Slesareva, G.A., The study of system Mg 2 Sn– Mg 2 Ge, Izv
AN U.S.S.R. Neorg. Mater., 2, 2116, 1966.
22. Heller, M.W. and Danielson, G.C., Seebeck effect in Mg

2 Si single crystals, J. Phys. Chem. Sol., 23, 265, 1962.
23. Redin, R.D., Morris, R.G., and Danielson, G.C.,
Semiconducting properties of Mg 2 Ge single crystals, Phys.
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24. Blunt, R.F., Frederikse, H.P.R., and Hosler, W.R.,

Electrical and optical properties of intermetallic
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1955.
25. Stella, A. and Lynch, D.W., Photoconductivity in Mg 2

Si and Mg 2 Ge, J. Phys. Chem. Sol., 25, 1253, 1964.
26. Koenig, P., Lynch, D.W., and Danielson, G.C., Infrared

absorption in magnesium silicide and magnesium germanide,
J. Phys. Chem. Sol., 20, 122, 1961.
27. Lipson, H.G. and Kahan, A., Infrared absorption of Mg 2

Sn, Phys. Rev., 133A, 800, 1964.
28. Lott, L.A. and Lynch, D.W., Infrared absorption in Mg 2

Ge, Phys. Rev., 141, 681, 1966.
29. Mead, C.A., Photothresholds in Mg 2 Ge, J. Appl. Phys.,

35, 2460, 1964.
30. Zaitsev, V.K. and Nikitin, E.N., Electrical properties,

thermal conductivity and forbidden-band width of Mg 2 Sn at
high temperatures, Soviet Physics of Solid State, 12, 289,
1970.
31. Au-Yang, M.Y. and Cohen, M.L., Electronic structure and

optical properties of Mg 2 Si, Mg 2 Ge, and Mg 2 Sn, Phys.
Rev., 178, 1358, 1969.
32. Baranek, P., Schamps, J., and Noiret, I., Ab initio

studies of electronic structure, phonon modes, and elastic
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33. Arnaud, B. and Alouani, M., Electron-hole excitations

in Mg 2 Si and Mg 2 Ge compounds, Phys. Rev. B, 64, 33202,
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I electrical current (A)
J electrical current density (A m 22 )
k thermal conductivity (Wm 21 K 21 )
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L total length of the STU
N number of segments in p-leg (1 to 5)
M number of segments in n-leg (1 to 5)
P power (W e )
PD electrical power density (W e m 22 )
Q thermal power (W th )
q heat flux (W th m 22 )
000 volumetric heat generation (Wm 23 )
r contact resistance (V-m 2 )
R electrical resistance (V)
0 resistance ð r‘Þ (V-m 2 )
T temperature (K)
x coordinate from heat junction
Z FOM (K 21 )
ZT dimensionless FOM
Greek Symbols
a Seebeck coefficient (V K 21 )
0 effective Seebeck coefficient (V K 21 )
g area ratio (A n /A p ) Symbol Quantity t Thomson h

conversion efficiency (%) h C Carnot efficiency (1 2 T c /T h
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Symbol Quantity
FPS fission power system
FWPF fine-weaved pierced fabrice
GPHS general-purpose heat source
GPHS-RTG general-purpose heat source radioisotope

thermoelectric generator
GRC Glenn Research Center
JHU Johns Hopkins University
JPL Jet Propulsion Laboratory
LES Lincoln experimental satellite
LGA low gain antenna

MHW-RTG multihundred watt radioisotope thermoelectric
generator
MMRTG multimission radioisotope thermoelectric generator
MSL Mars Science Lab
NASA National Aeronautics and Space Administration
NPS nuclear power system
PbTe lead telluride
PG pyrolytic graphite
RHU radioisotope heater unit Symbol Quantity RORSAT radar

ocean reconnaissance satellite RPS radioisotope power
system SiGe silicon germanium SNAP systems for nuclear
auxiliary power SRG Stirling radioisotope generator T amb
ambient temperature TAGS Tellurides of antimony, germanium,
and silver TCM thermoelectric converter module TE
thermoelectric TEM thermoelectric electromagnetic module
TFE thermionic fuel element UHF ultra high frequency U.S.
United States USAEC United States Atomic Energy Commission
USAF United States Air Force We watts (electric) Wt watts
(thermal)
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Thermoelectric Workshop, Coronado, CA, 2002.
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Electro-Optic Components
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microdevices, Proceedings of the 18th International
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and cooling micro/nanodevices for distributed system
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thermoelectric micro coolers with diamond substrates,
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August, 1997.

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spot cooling high power electronic components, Proceedings
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detectors, pp. 633–640. In CRC Handbook on Thermoelectrics.
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on single crystals of solid solutions of bismuth and
antimony chalcogenides, Inorg. Mater., 28(9), 1856–1859,
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modules for cooling electro-optic components, Proceedings
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0.5 1.0 1.5 2.0 TE leg length (mm) 1.5 2.0 2.5 3.0 3.5 I n
p u t p o w e r ( W ) A = 16mm 2 Power necessary to
maintain detector at 253 K FIGURE 58.20 Effect of deviation
from the optimal TE leg length.
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for semiconductor lasers, Proceedings of the 13th
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Appendix I History of the International
Thermoelectric Society
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the origin of modern semiconductor thermoelectric energy
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THERMOELECTRICS

Boca Raton London New York

© 2006 by Taylor & Francis Group, LLC

© 2006 by Taylor & Francis Group, LLC

No claim to original U.S. Government works

International Standard Book Number-10: 0-8493-2264-2 (Hardcover)

Library of Congress Cataloging-in-Publication Data

Thermoelectrics handbook : macro to nano / edited by D.M. Rowe.

Visit the Taylor & Francis Web site at

© 2006 by Taylor & Francis Group, LLC

Robert D. Abelson L.P. Bulat M.S. Dresselhaus

M. Blumers C. Dames Carlo Gatti

H.J. Goldsmid Kunihito Koumoto Igor V. Morgunov

V.M. Grabov Yan Kucherov Mamoun Muhammed

X.H. Ji Kakuei Matsubara K.R. Rao

Takenobu Kajikawa Mitsuru Matsuura P. Rogl

Tsuyoshi Kajitani A. Meier D.M. Rowe

Dennis D. Klug Gao Min Hamed H. Saber

© 2006 by Taylor & Francis Group, LLC

H. Scherrer Christian Stiewe Rama

© 2006 by Taylor & Francis Group, LLC

SECTION I General Principles and Theoretical

1 General Principles and Basic Considerations D.M. Rowe .................................................... 1-1

2 Modern Thermodynamic Theory of Thermoelectricity

3 Thermoelectric Phenomena under Large Temperature Gradients

4.4 Minority Carriers and Quasi-Fermi Levels .............................................................................. 4-4

6 Thermal Conductivity of Semiconductors with

7 A Chemical Approach to the First-Principles Modeling of Novel

8 Recent Trends for the Design and Optimization of Thermoelectric

© 2006 by Taylor & Francis Group, LLC

10.3 Low-Dimensional Systems ....................................................................................................... 10-3

11 Thermoelectric Module Design Theories Gao Min ............................................................. 11-1

12 Modeling and Characterization of Power Generation Modules Based

13 Energy Conversion Using Diode-Like Structures

14 Size Effects on Thermal Transport Chandra Mohan Bhandari ............................................. 14-1

15 Thermoelectric Aspects of Strongly Correlated Electron Systems S. Paschen ............. 15-1

16 Theory and Modeling in Nanostructured Thermoelectrics Alexander A. Balandin .... 16-1

© 2006 by Taylor & Francis Group, LLC

16.3 Optimization of Quantum Dot Structures for ZT Enhancement ....................................... 16-4

17 Thermoelectric Power of Carbon Nanotubes G.D. Mahan ............................................... 17-1

18 Phonon-Drag Thermopower of Low-Dimensional Semiconductor

SECTION II Material Preparation and Measurements

20 Review of Methods of Thermoelectric Materials Mass Production

21 Structural Studies of Thermoelectric Materials Bo Brummerstedt Iversen ....................... 21-1

22 Measurements of Resistivity and Thermopower: Principles

© 2006 by Taylor & Francis Group, LLC

22.5 Thermopower Measurement at Low Temperatures: 3 to 300 K .......................................... 22-9

23 Electrical and Thermal Transport Measurement Techniques for Evaluation

24 Measurement of the Thermal Conductivity of Thin Films F. Völklein,

25 Solvothermal Synthesis of Nanostructured Thermoelectric Materials X.B. Zhao,

26 Approaches to Thermoelectric Standardization Eckhard Müller, Christian Stiewe,

SECTION III Thermoelectric Materials

27 Thermoelectric Properties of Bismuth Antimony Telluride Solid Solutions

© 2006 by Taylor & Francis Group, LLC

29 Thermoelectrics on the Base of Solid Solutions of Mg2BIV Compounds

30 Thermoelectric Properties of the Group V Semimetals J.-P. Issi .................................... 30-1

32 Formation and Crystal Chemistry of Clathrates P. Rogl ................................................... 32-1

33 Structure, Thermal Conductivity, and Thermoelectric Properties of Clathrate

© 2006 by Taylor & Francis Group, LLC

33.3 Transport Properties of Type I and II Clathrates .................................................................. 33-3

34 Skutterudite-Based Thermoelectrics Ctirad Uher .................................................................. 34-1

35 Oxide Thermoelectrics Kunihito Koumoto, Ichiro Terasaki, Tsuyoshi Kajitani,

36 Thermoelectric Properties of Electrically Conducting Organic Materials