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Spintronics Handbook:
Spin Transport and
Magnetism,
Second Edition
Metallic Spintronics—Volume One
Spintronics Handbook:
Spin Transport and
Magnetism,
Second Edition
Metallic Spintronics—Volume One

Edited by
Evgeny Y. Tsymbal and Igor Žutić
CRC Press
Taylor & Francis Group
6000 Broken Sound Parkway NW, Suite 300
Boca Raton, FL 33487-2742

© 2019 by Taylor & Francis Group, LLC


CRC Press is an imprint of Taylor & Francis Group, an Informa business

No claim to original U.S. Government works

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International Standard Book Number-13: 978-1-498-76952-5 (Hardback)


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Contents

Foreword . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . vii
Preface . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . xi
About the Editors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . xiii
Contributors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . xv

Section i—introduction

Chapter 1. Historical Overview: From Electron Transport


in Magnetic Materials to Spintronics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3
Albert Fert

Section ii—Magnetic Metallic Multilayers

Chapter 2. Basics of Nanothin Film Magnetism . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 31


Bretislav Heinrich, Pavlo Omelchenko, and Erol Girt
Chapter 3. Micromagnetism as a Prototype for Complexity . . . . . . . . . . . . . . . . . . 95
Anthony S. Arrott
Chapter 4. Giant Magnetoresistance . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 149
Jack Bass
Chapter 5. Spin Injection, Accumulation, and Relaxation in Metals . . . . . . . . . . 199
Mark Johnson

v
vi Contents

Chapter 6. Magnon Spintronics: Fundamentals of


Magnon-Based Computing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 247
Andrii V. Chumak
Chapter 7. Spin Torque Effects in Magnetic Systems: Experiment . . . . . . . . . . . . 303
Maxim Tsoi
Chapter 8. Spin Torque in Magnetic Systems: Theory . . . . . . . . . . . . . . . . . . . . . . . 345
Aurélien Manchon and Shufeng Zhang
Chapter 9. Spin-Orbit Torques: Experiments and Theory . . . . . . . . . . . . . . . . . . . . 387
Aurélien Manchon and Hyunsoo Yang
Chapter 10. All-Optical Switching of Magnetization: From Fundamentals
to Nanoscale Recording . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 421
Andrei Kirilyuk, Alexey V. Kimel, and Theo Rasing

Section iii—Magnetic tunnel Junctions

Chapter 11. Tunneling Magnetoresistance: Experiment (Non-MgO) . . . . . . . . . . 457


Patrick R. LeClair and Jagadeesh S. Moodera
Chapter 12. Tunnel Magnetoresistance in MgO-Based Magnetic
Tunnel Junctions: Experiment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 495
Shinji Yuasa
Chapter 13. Tunneling Magnetoresistance: Theory . . . . . . . . . . . . . . . . . . . . . . . . . . . 525
Kirill D. Belashchenko and Evgeny Y. Tsymbal
Chapter 14. Spin Filter Tunneling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 559
Tiffany S. Santos and Jagadeesh S. Moodera
Chapter 15. Spin Torques in Magnetic Tunnel Junctions . . . . . . . . . . . . . . . . . . . . . . 591
Yoshishige Suzuki and Hitoshi Kubota
Chapter 16. Phase-Sensitive Interface and Proximity Effects in
Superconducting Spintronics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 635
Matthias Eschrig
Chapter 17. Multiferroic Tunnel Junctions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 683
Manuel Bibes and Agnès Barthélémy
Index . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 707
Foreword

S
pintronics is a field of research in which novel properties of materials,
especially atomically engineered magnetic multilayers, are the result of
the manipulation of currents of spin-polarized electrons. Spintronics, in
its most recent incarnation, is a field of research that is almost 30 years old. To
date, its most significant technological impact has been in the development of
a new generation of ultra-sensitive magnetic recording read heads that have
powered magnetic disk drives since late 1997. These magnetoresistive read head
which use spin-valves, that are based on spin-dependent scattering at magnetic/
non-magnetic interfaces, and since 2007, magnetic tunnel junctions (MTJs),
that are based on spin-dependent tunneling across ultra-thin insulating layers,
have a common thin film structure. These structures involve “spin engineer
ing” to eliminate the influence of long-range magneto-dipole fields via the use
of synthetic or artificial antiferromagnets, which are formed from thin mag
netic layers coupled antiferromagnetically via the use of atomically thin layers
of ruthenium. These structures involve the discoveries of spin-dependent tun
neling in 1975, giant magnetoresistance at low temperatures in Fe/Cr in 1988,
oscillatory interlayer coupling in 1989, the synthetic antiferromagnet in 1990,
giant magnetoresistance at room temperature in Co/Cu and related multilay
ers in 1991, and the origin of giant magnetoresistance as being a result of pre
dominant interface scattering in 1991–1993. Together these discoveries led to
the spin-valve recording read head that was introduced by IBM in 1997 and
led, within a few years, to a 1,000 fold increase in the storage capacity of mag
netic disk drives. This rapid pace of improvement has stalled over the past years
as the difficulty of stabilizing tiny magnetic bits against thermal fluctuations,
whilst, at the same time, being able to generate large enough magnetic fields to
write them, has proved intractable. The possibility of creating novel spintronic
magnetic memory-storage devices to rival magnetic disk drives in capacity and
to vastly exceed them in performance has emerged in the form of Racetrack
Memory. This concept and the physics underlying it are discussed in this book

vii
viii Foreword

together with a more conventional spintronic memory, magnetic random


access memory (MRAM). MRAM is based on MTJ magnetic memory bits
each one accessed in a two-dimensional cross point array via a transistor.
The fundamental concept of MRAM was proposed in 1995 using local fields
to write the MTJ elements. This basic concept was proven in 1999 with the
subsequent demonstration of large scale fully integrated 64 Mbit memory
chips in the following decade. Writing these same elements using spin
angular momentum from sufficiently large spin-polarized currents passed
through the tunnel junction elements emerged in the 1990s and is now key
to the development of massive scale MRAM chips. The second edition of
this book discusses these emerging spintronic technologies as well as other
breakthroughs and key advances both fundamental and applied, in the field
of spintronics.
Beyond MRAM and Racetrack Memory, this book elucidates other
nascent opportunities in spintronics that do not rely directly on magneto-
resistive effects, such as fault-tolerant quantum computing, non-Boolean
spin-wave logic, and lasers that are enhanced by spin-polarized carriers. It
is interesting that spintronics is a field of research that continues to surprise
even though the fundamental property of spin was realized nearly a century
ago, and the basic concept of spin-dependent scattering in magnetic materi
als was introduced by Neville Mott just shortly after the notion of “spin” was
conceived.
Since the first edition of this book, spintronics has so much evolved
that a new name of “spin-orbitronics” has been coined to describe these new
discoveries and developments. In the first edition of this book spin-orbit
coupling was regarded rather negatively as a property that leads to mix
ing between spin-channels and the loss of spin angular momentum from
spin currents to the lattice, thereby limiting the persistence of these same
spin currents, both temporally and spatially. In this edition several physi
cal phenomena derived from spin-orbit coupling are shown to be key to the
development of several new technologies, such as, in particular, the current
induced motion of a series of magnetic domain walls that underlies Racetrack
Memory. This relies especially on the generation of pure spin currents via
the spin Hall effect (SHE). The magnitude of the SHE was thought for some
time to be very small in conventional metals but over the past few years this
has rather been shown to be incorrect. Significant and useful SHEs have
been discovered in a number of heavy materials where spin-orbit coupling is
large. These spin currents can be used to help move domain walls or to help
switch the magnetization direction of nanoscale magnets. Whether they can
be usefully used for MRAM, however, is still a matter of debate.
Another very interesting development since the first edition of this book
is the explosive increase in our understanding and knowledge of topological
insulators and their cousins including, most recently, Weyl semi-metals. The
number of such materials has increased astronomically and, indeed, it is now
understood that a significant fraction of all extant materials are “topologi
cal”. What this means, in some cases, is that the spin of the carriers is locked
to their momentum leading, for example, to the quantum spin Hall effect.
Foreword ix

The very concept of these materials is derived from band inversion which, is
often due to strong spin-orbit coupling. From a spintronics perspective the
novel properties of these materials can lead to intrinsic spin currents and
spin accumulations that are topologically “protected” to a greater or lesser
degree. The concept of topological protection is itself evolving.
Distinct from electronic topological effects are topological spin tex
tures such as skyrmions and anti-skyrmions. The latter were only experi
mentally found 2 years ago. These spin textures are nano-sized magnetic
objects, related to magnetic bubbles that are also found in magnetic materi
als with perpendicular magnetic anisotropy, but which have boundaries or
walls that are innately chiral. The chirality is determined by a vector mag
netic exchange—a Dzyaloshinskii–Moriya interaction (DMI)—that is often
derived from spin-orbit coupling. The DMI favors orthogonal alignment of
neighboring magnetic moments in contrast to conventional ferromagnetic
or antiferromagnetic exchange interactions that favors collinear magnetic
arrangements. Skyrmion and anti-skyrmion spin textures have very interest
ing properties that could also be useful for Racetrack Memories. Typically,
skyrmions and anti-skyrmions evolve from helical or conical spin textures.
The magnetic phase of such systems can have complex dependences on tem
perature, magnetic field and strain. Some chiral antiferromagnetic spin tex
tures have interesting properties such as an anomalous Hall effect (AHE),
that is derived from their topological chiral spin texture in the absence of
any net magnetization. In practice, however, a small unbalanced moment
is needed to set the material in a magnetic state with domains of the same
chirality in order to evidence the AHE. On the other hand, these same chiral
textures can display an intrinsic spin Hall effect whose sign is independent
of the chirality of the spin texture.
The DMI interaction can also result from interfaces particularly
between heavy metals and magnetic layers. Such interfacial DMIs can give
rise to chiral domain walls as well as magnetic bubbles with chiral domain
walls – somewhat akin to skyrmions. The tunability of the interfacial DMI
via materials engineering makes it of especial interest.
Thus, since the first edition of this book chiral spin phenomena, namely
chiral spin textures and domain walls, and the spin Hall effect itself, which
is innately chiral, have emerged as one of the most interesting developments
in spintronics. The impact of these effects was largely unanticipated. It is not
too strong to say that we are now in the age of “chiraltronics”!
Another topic that has considerably advanced since the first edition of
this book is the field of what is often now termed spin caloritronics, namely
the use of temperature gradients to create spin currents and the use of ther
mal excitations of magnetic systems, i.e. magnons, for magnonic devices.
Indeed, magnons carry spin angular momentum and can propagate over
long distances. Perhaps here it is worth mentioning the extraordinarily long
propagation distances of spin currents via magnons in antiferromagnetic
systems that has recently been realized.
Recently discovered atomically thin ferromagnets reveal how the pres
ence of spin-orbit coupling overcomes the exclusion of two-dimensional
x   Foreword

ferromagnetism expected from the Mermin–Wagner theorem. These two-


dimensional materials which are similar to graphene in that they can readily
be exfoliated from bulk samples, provide a rich platform to study magnetic
proximity effects and transform a rapidly growing class of van der Waals
materials. Through studies of magnetic materials it is possible to reveal their
peculiar quantum manifestations. Topological insulators can become mag-
netic by doping with 3d transition metals: the quantum anomalous Hall
effect has been discovered in such materials and heterostructures that con-
sist of magnetic and non-magnetic topological insulators have been used to
demonstrate current induced control of magnetism.
Spintronics remains a vibrant research field that spans many disciplines
ranging from materials science and chemistry to physics and engineering.
Based on the rich developments and discoveries over the past thirty years
one can anticipate a bountiful future.

Stuart Parkin
Director at the Max Planck Institute of Microstructure Physics
Halle (Saale), Germany
and
Alexander von Humboldt Professor, Martin‐Luther‐Universität Halle‐
Wittenberg, Germany
Max Planck Institute of Microstructure Physics
Halle (Saale), Germany
Preface

T
he second edition of this book continues the path from the foundations
of spin transport and magnetism to their potential device applications,
usually referred to as spintronics. Spintronics has already left its mark
on several emerging technologies, e.g., in magnetic random access memories
(MRAMs), where the fundamental properties of magnetic tunnel junctions
are key for device performance. Further, many intricate fundamental phenom
ena featured in the first edition have since evolved from an academic curiosity
into the potential basis for future spintronic devices. Often, as in the case of
spin Hall effects, spin-orbit torques, and electrically controlled magnetism, the
research has migrated from the initial low-temperature discovery in semicon
ductors to technologically more suitable room temperature manifestations in
metallic systems. This path from exotic behavior to possible application contin
ues to the present day and is reflected in the modified title of the book, which
now explicitly highlights “spintronics,” as its overarching scope. Exotic topics
of today, for example, pertaining to topological properties, such as skyrmions,
topological insulators, or even elusive Majorana fermions, may become suitable
platforms for the spintronics of tomorrow. Impressive progress has been seen in
the last decade in the field of spin caloritronics, which has evolved from a curi
ous prediction 30 years ago to a vibrant field of research.
Since the first edition, there has been a significant evolution in material sys
tems displaying spin-dependent phenomena, making it difficult to cover even
the key developments in a single volume. The initially featured chapter on gra
phene spintronics is now complemented by a chapter on the spin-dependent
properties of a broad range of two-dimensional materials that can form a myriad
of heterostructures coupled by weak van der Waals forces and support super
conductivity or ferromagnetism even in a single atomic layer. Exciting develop
ments have also been seen in the field of complex oxide heterostuctures, where
the non-trivial properties are driven by the interplay between the electronic,
spin, and structural degrees of freedom. A particular example is the magnetism

xi
xii Preface

emerging in two-dimensional electron gases at oxide interfaces composed


of otherwise non-magnetic constituents. The updated structure of a sig
nificantly expanded book reflects various materials developments and it is
now thematically divided into three volumes, each based on broadly defined
metallic and semiconductor systems or their nanoscale and applied aspects.
Spintronics becomes more and more attractive as a viable platform for
propelling semiconducting technology beyond its current limits. Various
schemes have been proposed to enhance the functionalities of the exist
ing technologies based on the spin degree of freedom. Among them is the
voltage control of magnetism, exploiting the non-volatile performance of
ferromagnet-based devices in conjunction with their low-power operation.
Another approach is utilizing spin currents carried by magnons to trans
port and process information. Magnon spintronics involves interesting fun
damental physics and offers novel spin wave-based computing technologies
and logic circuits. Optical control of magnetism is another approach, which
has attracted a lot of attention due to the recent discovery of the all-optical
switching of magnetization and its realization at the nanoscale. Chapters on
these subjects are included in the new edition of the book.
Nearly nine decades after the discovery of superconducting proximity
effects by Ragnar Holm and Walther Meissner, several new chapters now explore
how a given material can be transformed through proximity effects whereby it
acquires the properties of its neighbors, for example, becoming superconduct
ing, magnetic, topologically non-trivial, or with an enhanced spin-orbit cou
pling. Such proximity effects not only complement the conventional methods of
designing materials by doping or functionalization but can also overcome their
various limitations and enable yet more unexplored spintronic applications.
We are grateful both to the authors who set aside their many priorities
and contributed new chapters, which have significantly expanded the scope
of this book, as well as to those who patiently provided valuable updates to
their original chapters and kept this edition even more timely. The comple
tion of the second edition was again greatly facilitated by Verona Skomski,
who tirelessly collected authors’ contributions and assisted their prepara
tion for the submission to the publisher. We acknowledge the support of
NSF-DMR, NSF-MRSEC, NSF-ECCS, SRC, DOE-BES, US ONR which,
through the support of our research and involvement in spintronics, has also
enabled our editorial work. We are thankful to our families for their sup
port, patience, and understanding during extended periods of time when we
remained focused on the completion of this edition.

Evgeny Y. Tsymbal
Department of Physics and Astronomy,
Nebraska Center for Materials and Nanoscience, University of Nebraska,
Lincoln, Nebraska 68588, USA

Igor Žutić
Department of Physics, University at Buffalo,
State University of New York, Buffalo, New York 14260, USA
About the Editors

Evgeny Y. Tsymbal is a George Holmes University Distinguished Professor


at the Department of Physics and Astronomy of the University of Nebraska-
Lincoln (UNL), and Director of the UNL’s Materials Research Science and
Engineering Center (MRSEC). He joined UNL in 2002 as an Associate
Professor, was promoted to a Full Professor with Tenure in 2005 and named
a Charles Bessey Professor of Physics in 2009 and George Holmes University
Distinguished Professor in 2013. Prior to his appointment at UNL, he was a
research scientist at University of Oxford, United Kingdom, a research fellow
of the Alexander von Humboldt Foundation at the Research Center-Jülich,
Germany, and a research scientist at the Russian Research Center “Kurchatov
Institute,” Moscow. Evgeny Tsymbal’s research is focused on computational
materials science aiming at the understanding of fundamental properties of
advanced ferromagnetic and ferroelectric nanostructures and materials rel-
evant to nanoelectronics and spintronics. He has published over 230 papers,
review articles, and book chapters and presented over 180 invited presentations
in the areas of spin transport, magnetoresistive phenomena, nanoscale magne-
tism, complex oxide heterostructures, interface magnetoelectric phenomena,
and ferroelectric tunnel junctions. Evgeny Tsymbal is a fellow of the American
Physical Society, a fellow of the Institute of Physics, UK, and a recipient of the
UNL’s College of Arts & Sciences Outstanding Research and Creativity Award
(ORCA). His research has been supported by the National Science Foundation,
Semiconductor Research Corporation, Office of Naval Research, Department of
Energy, Seagate Technology, and the W. M. Keck Foundation.

Igor Žutić received his Ph.D. in theoretical physics at the University of


Minnesota, after undergraduate studies at the University of Zagreb, Croatia.
He was a postdoc at the University of Maryland and the Naval Research Lab.
In 2005 he joined the State University of New York at Buffalo as an Assistant
Professor of Physics and got promoted to an Associate Professor in 2009 and

xiii
xiv   About the Editors

to a Full Professor in 2013. He proposed and chaired Spintronics 2001:


International Conference on Novel Aspects of Spin-Polarized Transport
and Spin Dynamics, at Washington DC. Work with his collaborators spans a
range of topics from high-temperature superconductors, Majorana fermions,
proximity effects, van der Waals materials, and unconventional magnetism,
to the prediction and experimental realization of spin-based devices that are
not limited to magnetoresistance. He has published over 100 refereed articles
and given over 150 invited presentations on spin transport, magnetism, spin-
tronics, and superconductivity. Igor Žutić is a recipient of the 2006 National
Science Foundation CAREER Award, the 2019 State University of New York
Chancellor’s Award for Excellence in Scholarship and Creative Activities,
the 2005 National Research Council/American Society for Engineering
Education Postdoctoral Research Award, and the National Research Council
Fellowship (2003–2005). His research is supported by the National Science
Foundation, the Office of Naval Research, the Department of Energy, Office
of Basic Energy Sciences, the Defense Advanced Research Project Agency,
and the Airforce Office of Scientific Research. He is a fellow of the American
Physical Society.
Contributors

Anthony S. Arrott Andrii V. Chumak


Department of Physics Fachbereich Physik
Simon Fraser University Technische Universität
Burnaby, British Columbia, Canada Kaiserslautern
Kaiserslautern, Germany
Agnès Barthélémy
Unité Mixte de Physique Matthias Eschrig
Centre National de la Recherche Department of Physics, Royal Holloway
Scientifique-Thales University of London
Université Paris-Sud Egham, United Kingdom
Palaiseau, France
Albert Fert
Jack Bass Unité Mixte de Physique
Department of Physics and Astronomy Centre National de la Recherche
Michigan State University Scientifique-Thales
East Lansing, Michigan Université Paris-Sud
Palaiseau, France
Kirill D. Belashchenko
Department of Physics and Astronomy Erol Girt
Nebraska Center for Materials and Department of Physics
Nanoscience Simon Fraser University
University of Nebraska Burnaby, British Columbia, Canada
Lincoln, Nebraska
Bretislav Heinrich
Manuel Bibes Department of Physics
Unité Mixte de Physique Simon Fraser University
Centre National de la Recherche Burnaby, British Columbia, Canada
Scientifique-Thales
Université Paris-Sud
Palaiseau, France
xv
xvi Contributors

Mark Johnson Theo Rasing


Materials Physics Division Radboud University
Naval Research Laboratory Institute for Molecules and Materials
Washington, DC Nijmegen, the Netherlands

Alexey V. Kimel Tiffany S. Santos


Radboud University Western Digital Corporation
Institute for Molecules and San Jose, California
Materials
Nijmegen, the Netherlands Yoshishige Suzuki
Department of Materials
Andrei Kirilyuk Engineering Science
Radboud University Osaka University
Institute for Molecules and Osaka, Japan
Materials
Nijmegen, the Netherlands Maxim Tsoi
Department of Physics
Hitoshi Kubota The University of Texas at Austin
National Institute of Advanced Austin, Texas
Industrial Science and
Technology Evgeny Y. Tsymbal
Spintronics Research Department of Physics and
Tsukuba, Japan Astronomy
Nebraska Center for Materials and
Patrick R. LeClair Nanoscience
Department of Physics and University of Nebraska
Astronomy and MINT Lincoln, Nebraska
The University of Alabama
Tuscaloosa, Alabama Hyunsoo Yang
Department of Electrical and
Aurélien Manchon Computer Engineering, and
Physical Science and Engineering NUSNNI
Division National University of Singapore
King Abdullah University of Science Singapore
and Technology (KAUST)
Thuwal, Saudi Arabia Shinji Yuasa
National Institute of Advanced
Jagadeesh S. Moodera Industrial Science and
Francis Bitter Magnet Laboratory Technology (AIST)
Massachusetts Institute of Tsukuba, Japan
Technology
Cambridge, Massachusetts Shufeng Zhang
Department of Physics
Pavlo Omelchenko University of Arizona
Department of Physics Tucson, Arizona
Simon Fraser University
Burnaby, British Columbia, Canada
Section I
Introduction
Chapter 1 Historical Overview: From Electron Transport
in Magnetic Materials to Spintronics 3
Albert Fert

1
1
Historical Overview
From Electron Transport
in Magnetic Materials
to Spintronics
Albert Fert

1.1 
Introduction 4
1.2 
Spin-Dependent Conduction in Ferromagnets and
Early Examples of Spin Transport Experiments 4
1.3 
Concept of GMR in Experiments on Ternary Magnetic
Alloys 8
1.4 
Discovery of the GMR 8
1.5 
Golden Age of GMR 10
1.6 
TMR Relays GMR 12
1.7 
Spin Accumulation and Spin Currents 14
1.8 
Spin Transfer 19

3
4   Chapter 1. From Electron Transport in Magnetic Materials to Spintronics

1.9 Spintronics Today and Tomorrow 21


1.10 
Conclusion 23
References 23

1.1 
INTRODUCTION
Spintronics is now an important field of research with major applications
in several technologies. Its development has been triggered by the discov-
ery [1, 2] of giant magnetoresistance (GMR) in 1988. The basic concept of
spintronics is the manipulation of spin-polarized currents, in contrast to
mainstream electronics in which the spin of the electron is ignored. Adding
the spin degree of freedom provides new effects, new capabilities, and new
functionalities. Spin-polarized currents can be generated by exploiting the
influence of the spin on the transport properties of the electrons in ferro-
magnetic conductors. This influence, first suggested by Mott [3], had been
experimentally demonstrated and theoretically described in early works
[4, 5] more than 10 years before the discovery of the GMR. The GMR was the
first step on the road of the utilization of the spin degree of freedom in mag-
netic nanostructures. Its application to the read heads of hard disks greatly
contributed to the fast rise in the density of stored information and led to
the extension of hard disk technology to consumer electronics. Then, more
development and intensive research revealed many other phenomena related
to the control and manipulation of spin-polarized currents. Today, the field
of spintronics is expanding considerably, with very promising new axes, such
as the manipulation of magnetic moments and the generation of microwaves
by spin transfer, spintronics with semiconductors, molecular spintronics,
the spin Hall effect (SHE), the quantum spin Hall effect (QSHE), and single-
electron spintronics for quantum computing. In this chapter, I will tell the
story of this development from the early experiments on spin-dependent
conduction in ferromagnets to the emerging directions of today.

1.2 
SPIN-DEPENDENT CONDUCTION IN
FERROMAGNETS AND EARLY EXAMPLES
OF SPIN TRANSPORT EXPERIMENTS
GMR and spintronics take their roots from previous research on the influ-
ence of spin on electrical conduction in ferromagnetic metals [3–5]. The
spin dependence of the conduction can be understood from the typical
band structure of a ferromagnetic metal, which is shown in Figure 1.1a. Due
to the splitting between the energies of the “majority spin” and “minority
spin” directions (spin up and spin down in the usual notation), the elec-
trons at the Fermi level, which carry the electrical current, are in different
states and exhibit different conduction properties for opposite spin direc-
tions. This spin-dependent conduction was proposed by Mott [3] in 1936 to
explain some features of the resistivity of ferromagnetic metals at the Curie
temperature. However, in 1966, when I started my Ph.D. thesis, the subject
1.2 Spin-Dependent Conduction in Ferromagnets 5

FIGURE 1.1 The basics of spintronics. (a) Schematic band structure of a ferro-
magnetic metal. (b) Schematic for spin-dependent conduction through indepen-
dent spin-up and spin-down channels in the limit of negligible spin mixing (ρ↑↓ = 0
in the formalism of Ref. [4]). (c) Resistivities of the spin-up and spin-down conduc-
tion channels for nickel doped with 1% of several types of impurity (measurements
at 4.2 K) [4]. The ratio α between the resistivities ρ0↓ and ρ0↑ can be as large as 20
(Co impurities) or smaller than 1 (Cr or V impurities). (After Fert, A. et al., J. Phys. F
Met. Phys. 6, 849, 1976. With permission.)

was still almost completely unexplored. My supervisor, Ian Campbell, and


I investigated the transport properties of Ni- and Fe-based alloys and, from
the analysis of the temperature dependence of the resistivity and also from
experiments on ternary alloys I describe in Section 1.3, we demonstrated the
spin dependence of conduction in various metals and alloys. In particular,
we showed that the resistivities of the two channels can be very different in
metals doped with impurities presenting a strongly spin-dependent scatter-
ing cross-section [4]. In Figure 1.1c, I show the example of the spin-up and
spin-down resistivities of nickel doped with 1% of different impurities. It can
be seen that ratio α of the spin-down to spin-up resistivity can be as large as
20 for Co impurities or smaller than 1 for Cr or V impurities. This was con-
sistent with the theoretical models developed at this time by Jacques Friedel
for the electronic structures of impurities in metals. The two-current con-
duction was rapidly confirmed in other groups and, for example, extended to
Co-based alloys by Loegel and Gautier [5].
The so-called two-current model [4] for conduction in ferromagnetic
metals was worked out for the quantitative interpretation of the experiments
described in the preceding paragraph. This model is based on a picture
of spin-up and spin-down currents coupled with spin mixing, that is, by
exchange of current between the spin-up and spin-down channels. Spin
mixing comes from spin-flip scattering, mainly from electron-magnon
scattering, which conserves the total spin of the electronic system but is a
mechanism of current transfer between the two channels. It increases with
temperature and tends to equalize partly the spin-up and spin-down cur-
rents at room temperature in most ferromagnetic metals [4]. The two-current
model is the basis of spintronics today, but, except in very few publications
6   Chapter 1. From Electron Transport in Magnetic Materials to Spintronics

[6, 7] discussing the temperature dependence of the GMR, the interpretation


of the spintronics phenomena is surprisingly based on a simplified version
of the model neglecting spin mixing and assuming that conduction occurs
through two independent channels in parallel, as in the sketch of Figure 1.1c.
It should certainly be useful to revisit the interpretation of many recent
experiments by considering the spin mixing contributions (note that the
spin mixing mechanism by spin-flips should not be confused with the spin
relaxation mechanism transferring spin accumulation to the lattice and due
mainly to spin–orbit scattering).
The research on spin transport developed before the discovery of GMR
has not only worked out the basic physics of spin transport in ferromagnetic
conductors but also explored some topics that came into fashion only recently
in spintronics. I take the example of the SHE. When an electrical current flows
in a nonmagnetic conductor, the electrons of opposite spins are deflected in
opposite transverse directions by spin–orbit interactions. With equal spin-up
and spin-down currents, there is no charge accumulation and consequently
no Hall voltage between edge contacts, but the deflections induce opposite
spin accumulations on the edges of the conductor, as illustrated in Figure
1.2a. This is the SHE, already described in 1971 by D’yakonov and Perel’ [8].
As spin accumulation by the SHE can be used to generate spin currents,
the SHE is nowadays presented as a possible method for carrying out spintron-
ics without magnetic materials, which explains the intense current research
on this topic. In most recent experiments, the SHE is detected by breaking the
symmetry between the opposite spin directions to obtain a transverse voltage,
either by using a ferromagnetic metal for one of the Hall probes or by locally
injecting a spin-polarized current (or even a pure spin current) from a ferro-
magnetic contact, the so-called inverse SHE detection. This can be done only
in nanodevices fabricated by lithographic techniques [9–11]. Thirty years ago,
it was not technically possible to fabricate such nanodevices, but, neverthe-
less, a precise determination of the SHE could be performed in other ways. In
Figure 1.2b, we show the results published in 1981 [12] on the SHE induced
by 5d impurities (Lu, Ta, Ir, Au) in Cu. The SHE is detected by adding 0.01%
of Mn impurities and applying a magnetic field. It had previously been shown
that applying a field with only Mn impurities in Cu does not give any signifi-
cant contribution to the Hall effect but induces (by exchange scattering) a spin
polarization of the current, which can be seen through the associated negative
magnetoresistance (GMR-like effect). In brief, the spin polarization induced
by exchange with dilute impurities of Mn replaces the spin injection of mod-
ern experiments. As the current polarization follows the polarization of the
paramagnetic Mn impurities and is inversely proportional to the temperature
(T), one obtains the variations of the Hall constant as 1/T seen in Figure 1.2b
for different types of nonmagnetic impurities. The amplitude of the SHE can
be characterized by the Hall angle, ΦH = ρxy/ρxx. From the results of Figure 1.2b,
Fert et al. [12] derived Hall angles varying from −2.4 × 10−2 for CuLu to +5.2 ×
10−2 for CuIr, with the typical change of sign between the beginning and the
end of the 5d series predicted by a model of resonant scattering on impurity 5d
states split by a spin–orbit interaction [12, 13]. Similar values of the SHE angle
1.2 Spin-Dependent Conduction in Ferromagnets 7

FIGURE 1.2 (a) Sketch illustrating the SHE in a nonmagnetic conductor.


(b) Experimental results [12] on the SHE induced by resonant scattering on 5d levels
(split by spin–orbit coupling) of nonmagnetic impurities in Cu (open triangles =
Lu 0.013%, circles = Ta 0.023%, black triangle = Ir 0.19%). The inverse SHE of the Cu
alloys is revealed by adding ≈0.01% of Mn impurities and applying a field H to spin-
polarize the current by exchange scattering on the spin-polarized Mn impurities.
With a paramagnetic-like spin polarization proportional to H/T, the SHE is revealed
through a contribution to the Hall constant proportional to T−1 with different slopes
for different impurities (the squares represent measurement on Cu with only 0.015%
of Mn and without 5d impurities, which shows the quasi-absence of 1/T contribu-
tion to the Hall effect from Mn alone). Note the characteristic change of sign of the
SHE between the beginning (Lu) and the end (Ir) of the 5d series.

in Cu doped with Ir have again been found in “modern” SHE experiments with
spin injection from lateral spin valves [13].
The SHE is not the only effect that had been already observed in the
“prehistory” of spintronics before beginning the object of intense attention
in the very recent years of the developments of spintronics. For example,
the Dzyaloshinskii-Moriya Interactions (DMI) have been introduced for
non-centrosymmetric magnetic compounds [14, 15], metallic spin glasses
[16], and at the interface of magnetic films with heavy metals [17] well
8   Chapter 1. From Electron Transport in Magnetic Materials to Spintronics

before being extensively exploited in the last years to generate magnetic


skyrmions [18–19] or chiral domain wall [20]. Another example is the very
early observation of current-induced domain wall motion by Berger [21],
as it will be discussed later in this chapter.

1.3 
CONCEPT OF GMR IN EXPERIMENTS
ON TERNARY MAGNETIC ALLOYS
Twenty years before the discovery of GMR, some experiments with ferromag-
netic metals doped with two types of impurities [4] were already anticipating
the GMR. This is illustrated in Figure 1.3. Suppose, for example, that nickel is
doped with impurities A (Co, for example), which strongly scatter the electrons
of the spin-down channel with impurities B (Rh, for example), which strongly
scatter the spin-up electrons. In the ternary alloy Ni(Co + Rh), that I call type
1, the electrons of both channels are strongly scattered, either by Co in one of
the channels or by Rh in the other, so that there is no shorting by one of the
channels and the resistivity is strongly enhanced, as illustrated in Figure 1.3a.
In contrast, there is no such enhancement in alloys of type 2 doped with impu-
rities A and B (Co and Au, for example) strongly scattering the electrons in the
same channel and leaving the second channel open, as in Figure 1.3b.
GMR occurs with the replacement of impurities A and B in the ternary
alloy with the successive layers A and B of the same magnetic metal in a
multilayer. If the magnetizations of the layers A and B are antiparallel, this
corresponds to the situation of strong scattering in both channels in alloys
of type 1, while the configuration with parallel magnetizations corresponds
to the situation with a relatively free channel in alloys of type 2. What is new
with respect to the ternary alloys is the possibility of switching between high
and low resistivity states applying a magnetic field and by simply changing
the relative orientation of the magnetizations of layers A and B from anti-
parallel to parallel. However, the transport equations tell us that the relative
orientation of layers A and B can be felt by the electrons only if their distance
is smaller than the electron mean free path, that is, practically, if they are
spaced by only a few nanometers. Unfortunately, in the 1970s, it was not
technically possible to make multilayers with layers as thin as a few nano-
meters, and the discovery of the GMR had to wait until the development of
sophisticated deposition techniques.

1.4 
DISCOVERY OF THE GMR
In the mid-1980s, with the development of techniques such as molecular
beam epitaxy (MBE), it became possible to fabricate multilayers composed
of very thin individual layers and one could consider trying to extend the
experiments on ternary alloys to multilayers. In addition, in 1986, I saw
the beautiful Brillouin scattering experiments of Grünberg and cowork-
ers [22] revealing the existence of antiferromagnetic interlayer exchange
couplings in Fe/Cr multilayers. Fe/Cr appeared as a magnetic multilayered
system in which it was possible to switch the relative orientation of the
1.4 Discovery of the GMR    9

FIGURE 1.3 Experiments on ternary alloys based on the same concept as that of
GMR [4]. The sketches illustrate the conduction by two channels in a ferromagnet
doped with impurities A (black) and B (gray), the circles are at the scale of the scat-
tering cross-sections of impurities A and B. (a) Schematic for the spin-dependent
conduction in alloys with impurities of opposite scattering spin asymmetries (αA =
ρA↓/ρA↑ > 1, αB = ρB↓/ρB↑ < 1, ρAB ≫ ρA + ρB) and experimental results for Ni(Co1–xRhx)
alloys. (b) Same for alloys with impurities of similar scattering spin asymmetries (αA
= ρA↓/ρA↑ > 1, αB = ρB↓/ρB↑ > 1, ρAB ≈ ρA + ρB) and experimental results for Ni(Au1–x Cox)
alloys. In GMR, the impurities A and B are replaced by multilayers, the situation of
(a) corresponding to the antiparallel magnetic configurations of adjacent magnetic
layers and (b) corresponding to parallel.

magnetization in adjacent magnetic layers from antiparallel to parallel by


applying a magnetic field. In collaboration with the group headed by Alain
Friederich at the Thomson-CSF company, I started the fabrication and
investigation of Fe/Cr multilayers. In 1988, this led us to the discovery [1]
of very large magnetoresistance effects that we called GMR (Figure 1.4a).
Effects of the same type in Fe/Cr/Fe trilayers were obtained practically at
the same time by Grünberg at Jülich [2] (Figure 1.4b). The interpretation of
GMR is similar to that described above for the ternary alloys and is illus-
trated in Figure 1.4c. The first classical model of GMR was published in
1989 by Camley and Barnas [23], and I collaborated with Levy and Zhang
on the first quantum model [24] in 1991.
I am often asked if I was expecting such large MR effects. My answer is
yes and no: on one hand, a very large magnetoresistance could be expected
from an extrapolation of the preceding results on ternary alloys, on the other
hand, one could fear that the unavoidable structural defects of the multi-
layers, interface roughness, for example, might introduce spin-independent
scatterings canceling the spin-dependent scattering inside the magnetic layers.
10   Chapter 1. From Electron Transport in Magnetic Materials to Spintronics

FIGURE 1.4 The first observations of giant magnetoresistance. (a) Fe/Cr(001)


multilayers [1] (with the current definition of the magnetoresistance ratio, MR =
100[RAP – RP]/Rp, MR = 85% for the Fe 3 nm/Cr 0.9 nm multilayer). (b) Fe/Cr/Fe trilay-
ers [2]. (c) Schematic of the mechanism of GMR. In the parallel magnetic configura-
tion (bottom), the electrons of one of the spin directions can easily go through
all the magnetic layers, and the short circuit through this channel leads to a small
resistance. In the antiparallel configuration (top), the electrons of each channel
are slowed down on every second magnetic layer and the resistance is high. (After
Chappert, C. et al., Nat. Mater. 6, 813, 2007. With permission.)

Fortunately, the scattering by the roughness of the interfaces was also spin
dependent and added its contribution to the “bulk” (the “bulk” and interface
contributions can be separately derived from GMR experiments with the
current perpendicular to the layers).

1.5 
GOLDEN AGE OF GMR
Rapidly, the papers reporting the discovery of GMR attracted attention for
their fundamental interest, as well as for the many possibilities for appli-
cation, and research on magnetic multilayers and GMR became a very hot
topic. In my team, as well as in the small but rapidly increasing community
working in the field, we had the exalting impression of exploring a wide vir-
gin country, with so many amazing surprises in store. On the experimental
1.5 Golden Age of GMR    11

FIGURE 1.5 Oscillatory variation of the GMR ratio of Fe/Cr multilayers as a function
of the thickness of the Cr layers. (After Parkin, S.S.P. et al., Phys. Rev. Lett. 64, 2304,
1990. With permission.)

side, two important results were published in 1990. Parkin et al. [25] dem-
onstrated the existence of GMR in multilayers made by the simpler and
faster technique of sputtering (Fe/Cr, Co/Ru, and Co/Cr) and found that the
oscillatory behavior of the GMR was due to the oscillations of the inter-
layer exchange as a function of the thickness of the nonmagnetic layers
(see Figure 1.5). Also in 1990, Shinjo and Yamamoto [26], as well as Dupas
et al. [27], demonstrated that GMR effects can be found in multilayers with-
out antiferromagnetic interlayer coupling but composed of magnetic layers of
different coercivities. Another important result, in 1991, was the observation
of large and oscillatory GMR effects in Co/Cu, which became an archetypical
GMR system. The first observations were obtained at Orsay [28] with multilay-
ers prepared by sputtering at Michigan State University and at about the same
time at IBM [29].
Also in 1991, Dieny et al. [30] reported the first observation of GMR in
spin valves, that is, trilayered structures in which the magnetization of one
of the two magnetic layers is pinned by coupling with an antiferromagnetic
layer, while the magnetization of the second one is free. The magnetization of
the free layer can be reversed by very small magnetic fields, so the concept is
now used in many devices. The various applications of GMR are described in
other chapters of this book. Its application to the read heads of hard disks is
certainly the most important [31, 32]. The GMR, by providing a sensitive and
scalable read technique, has led to an increase of the areal recording density
by more than two orders of magnitude (from ≈1 to ≈600 Gbit/in.2 in 2009).
This increase opened the way both to unprecedented drive capacities (up to 1
terabyte) for video recording or backup and to smaller hard disk drive (HDD)
sizes (down to 0.85 inch disk diameter) for mobile appliances like ultra-light
laptops or portable multimedia players. GMR sensors are also used in many
other types of application, mainly in the automotive industry and biomedical
technology [33].
12   Chapter 1. From Electron Transport in Magnetic Materials to Spintronics

1.6 
TMR RELAYS GMR
An important stage in the development of spintronics has been the research
on the tunneling magnetoresistance (TMR) of the magnetic tunnel junc-
tions (MTJs). The MTJs are tunnel junctions with ferromagnetic electrodes,
and their resistance is different for the parallel and antiparallel magnetic
configurations of their electrodes. Some early observations of small TMR
effects had been already reported by Jullière [34] in 1975 and Maekawa and
Gäfvert [35] in 1982, but they were found to be hardly reproducible and
actually could not be really reproduced until 1995. It was at this time only
that large (≈20%) and reproducible effects were obtained by Moodera’s and
Miyasaki’s groups on MTJ with a tunnel barrier of amorphous alumina [36].
After 1995, the research on TMR became very active, and the most
important step was the transition from MTJ with an amorphous tunnel
barrier (alumina) to single-crystal MTJ and especially MTJ with an MgO
barrier. In the first results with MgO, the TMR ratio was only slightly larger
than that found with alumina barriers and similar electrodes [37]. The impor-
tant breakthrough came in 2004 at Tsukuba [38] and IBM [39] where it was
found that very large TMR ratios, up to 200% at room temperature, could be
obtained with MgO MTJ of a very high structural quality, as illustrated in
Figure 1.6. Since 2004, these results have been progressively improved [40],
and TMR ratios up to 1000% have been now reached [41].
The large TMR of MTJ with single-crystal tunnel barriers, such as
MgO(001), come from symmetry selection [42–45]. This is illustrated in
Figure 1.6c where one sees the calculated density of states (DOS) of eva-
nescent wave functions of different symmetries, Δ1, Δ5, etc., and the much
slower decay of the symmetry Δ1 in an MgO(001) barrier between Co elec-
trodes [45]. The key point is that, at least for interfaces of high quality, an
evanescent wave function of a given symmetry is connected to the Bloch
functions of the same symmetry and same spin direction at the Fermi level
of the electrodes. For Co electrodes, the Δ1 symmetry is well represented
at the Fermi level in the majority spin direction sub-band and not in the
minority one. Consequently, a good connection between the majority spin
direction sub-bands of the Co electrodes by the slowly decaying channel
Δ1 can be obtained only in their parallel magnetic configuration, which
explains the very high TMR. Other types of barriers can select symmetries
other than the symmetry Δ1 selected by MgO(001). For example, a SrTiO3
barrier predominantly selects evanescent wave functions of Δ5 symmetry,
which are well connected to minority spin states of cobalt [46]. This explains
the negative effective spin polarization of cobalt observed in SrTiO3-based
MTJ [47].
The high spin polarization obtained by symmetry selection gives a very
good illustration of what is under the word “spin polarization” in a spintronic
experiment. There is no intrinsic spin polarization of a magnetic conductor.
In an MTJ, the effective polarization is related to the symmetry selected by
the barrier and, depending on the barrier, can be positive or negative, large or
small. In the same way, as we have seen in Section 1.2, the spin polarization
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