Muon Spectroscopy: An Introduction

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 2

Muon
Spectroscopy
An Introduction

St e p h e n J. B lu n d e l l
R o b e rto D e R e n z i
To m L a n c a st e r
F r a n c i s L . P r at t
Muon Spectroscopy - An Introduction
Muon Spectroscopy - An Introduction

Edited by

Stephen J. Blundell
University of Oxford

Roberto De Renzi
University of Parma

Tom Lancaster
University of Durham

Francis L. Pratt
ISIS Neutron and Muon Source
 Great Clarendon Street, Oxford, OX2 6DP,
United Kingdom
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Preface

Muons, radioactive particles that can be produced by accelerators, have

emerged as an important tool to study problems in condensed matter
physics and chemistry. Beams of muons with all their spins polarized
can be prepared and implanted in various types of material. The sub-
sequent precession and relaxation of the spins of these muons can be
used to investigate a variety of static and dynamic effects in a sample
and hence to deduce properties concerning magnetism, superconductiv-
ity, molecular or chemical dynamics, and a bewildering array of other
properties.
The technique has a slightly odd name: µSR. The µ stands, of course,
for the muon and the S is the spin of the muon, because the spin an-
gular momentum of the muon is what provides its magnetic moment,
which is the property from which the muon’s sensitivity to magnetic
fields derives, and this is the key aspect of the interaction between the
muon and the sample. But what about the R? The name was given
to make it look a bit like NMR (nuclear magnetic resonance) and ESR
(electron spin resonance), so you might guess that µSR is muon spin
resonance. However, the muon is a multifaceted probe, and for reasons
we will explain in detail in this book the technique is rarely performed
resonantly, since the dominant effects are rotation (the Larmor preces-
sion of the muon, which we can observe directly) and relaxation. Thus,
sometimes we will be dealing with muon spin rotation, sometimes with
muon spin relaxation, and just occasionally with muon spin resonance.
To avoid this ambiguity, we have called this book Muon spectroscopy:
an introduction, but note that the technique will usually be referred to,
as is conventional, by the name µSR.
The µSR technique was originally the preserve of a few specialists lo-
cated in particle physics laboratories. Today it is used by scientists from
a very wide range of science backgrounds and interests. Although there
are some very good technical monographs and review articles describing
the technique, we felt there was a need for a book designed for begin-
ners of many different types: curious undergraduates, starting graduate
students, or even experts in related fields who want to find out what all
the fuss is about. We hope this is a book that many will be able to learn
from, as well as learning to enjoy the beauty of the physics behind this
wonderful probe.
For those wishing to explore more deeply into the µSR technique, each
chapter is supplemented with further reading. More information is also
available on the websites of the international muon facilities and also
vi Preface

the International Society for Muon Spectroscopy (ISMS). The royalties

of this book are being donated to the ISMS in order to contribute to
the financial support for young scientists, particularly those from less
wealthy countries, to attend the triennial international conference on
muon spectroscopy.
This book grew out of a European workshop held during August 2019
at the Rutherford Appleton Laboratory in which scientists from across
the world gathered for 2 weeks for an advanced school on muon spec-
troscopy. The school was enabled through the major support of ISIS,
PSI and the EU SINE2020 project, along with additional support from
ISMS, TRIUMF, and JPARC. The lecturers from this school consented
to write material for the book based on their lectures. Inevitably, such an
approach produces material using a range of styles and notations, some
overlaps and some omissions. Therefore, the editors of this book resolved
to take the submitted material, mix it up and revise it, reorder and rein-
vent parts, aiming to produce a final result which would look as if it came
from a single author (the one exception being the historical appendix by
Steve Cox; with a relatively new technique, a short history is inevitably a
personal view). We are grateful for the forbearance and generosity of our
team of contributing authors (listed on page vii) for allowing their mate-
rial to be so roughly handled, but we hope that the final result is worth
it. Our thanks are primarily to them, but also to Sönke Adlung and his
team at OUP, our eagle-eyed copy editor Kate Blackham, as well as a
number of kind friends and colleagues who read through the book and
made numerous helpful comments, suggestions, and corrections: Pietro
Bonfà, Stewart Clark, Jonathan Frassineti, Elena Garlatti, George Gill,
Matjaž Gomilšek (who also produced Fig. 16.11), Alberto Hernandez
Melian, Thomas Hicken, Ben Huddart, Gianrico Lamura, Muhammad
Maikudi Isah, Ifeanyi John Onuorah, Giacomo Prando, Samuele Sanna,
Toni Shiroka, Johnny Wilkinson, and Hank Wu, as well as our contribut-
ing authors. The book is better because of their efforts. Finally, we
express our gratitude to the students who attended the school, pressed
us all to think about how to explain the various aspects of µSR, or think
again about what we thought we knew.
Stephen J. Blundell
Roberto De Renzi
Tom Lancaster
Francis L. Pratt
July 7, 2021
List of contributors

Peter J. Baker, STFC-ISIS Rutherford Appleton Laboratory, UK

Adam Berlie, STFC-ISIS Rutherford Appleton Laboratory, UK
Pabitra K. Biswas, STFC-ISIS Rutherford Appleton Laboratory, UK
Stephen J. Blundell, University of Oxford, UK
Pietro Carretta, University of Pavia, Italy
Stephen P. Cottrell, STFC-ISIS Rutherford Appleton Laboratory, UK
Stephen F. J. Cox, STFC-ISIS Rutherford Appleton Laboratory, UK
Pierre Dalmas de Réotier, CEA Grenoble, France
Roberto De Renzi, University of Parma, Italy
Adrian D. Hillier, STFC-ISIS Rutherford Appleton Laboratory, UK
Rustem Khasanov, Paul Scherrer Institute, Switzerland
Tom Lancaster, University of Durham, UK
Leandro Liborio, STFC-SCD Rutherford Appleton Laboratory, UK
James S. Lord, STFC-ISIS Rutherford Appleton Laboratory, UK
Martin Månsson, KTH Stockholm, Sweden
Iain McKenzie, TRIUMF, Vancouver, Canada
Francis L. Pratt, STFC-ISIS Rutherford Appleton Laboratory, UK
Thomas Prokscha, Paul Scherrer Institute, Switzerland
Zaher Salman, Paul Scherrer Institute, Switzerland
Simone Sturniolo, STFC-SCD Rutherford Appleton Laboratory, UK
Jun Sugiyama, CROSS-Tokai, Japan
Andreas Suter, Paul Scherrer Institute, Switzerland
Rui Vilão, University of Coimbra, Portugal
Koji Yokoyama, STFC-ISIS Rutherford Appleton Laboratory, UK

The book website is https://musr.org/muon-spectroscopy-book

Contents

1 The basics of µSR 1

1.1 The key idea 1
1.2 The principles of the experiment 2
1.3 Muon beams and spectrometers 4
1.4 Experimental geometries 6
1.5 What can we do with µSR? 6

I Elements of muon spectroscopy 9

2 Introduction 10
2.1 Discovery of the muon 10
2.2 The first muon application 11
2.3 Muon perspectives 12
2.4 The µSR experiment 17
Exercises 20

3 Muon charge and spin states 21

3.1 State formation 22
3.2 Hydrogen analogues 24
3.3 Measuring the states 26
3.4 Influencing the states 27
Exercises 28

4 The quantum muon 29

4.1 Larmor precession 29
4.2 Density matrices 33
4.3 Mixed states 34
4.4 Two spins: muonium 36
4.5 Multiple spins 44
Exercises 52

5 Polarization functions 54
5.1 Static fields 55
5.2 Dynamical fields 60
5.3 Disordered systems 64
5.4 The stretched exponential 65
Exercises 67
x Contents

II Science with µSR 69

6 Magnetism 70
6.1 The basics 70
6.2 Static magnetic order 72
6.3 The local magnetic field 76
6.4 Static field distributions 81
Exercises 86

7 Dynamic effects in magnetism 87

7.1 Correlation functions 87
7.2 Dynamics in magnets 90
7.3 Dynamics with muons 92
7.4 Relaxation as resonance 95
7.5 Dynamic magnetism 96
7.6 Coupling tensors 101
7.7 Dilute spins 103
Exercises 108

8 Measuring dynamic processes 110

8.1 Critical dynamics 110
8.2 Magnetism in metals 113
8.3 BPP relaxation 115
8.4 Mobile excitations 117
8.5 Muon diffusion 125
Exercises 129

9 Superconductors 130
9.1 The discovery 130
9.2 London penetration depth 131
9.3 Ginzburg-Landau model 134
9.4 Type-II superconductors 136
9.5 Measuring the penetration depth 140
9.6 The microscopic model 144
9.7 Example materials 146
9.8 Clean versus dirty 150
9.9 The Uemura plot 151
9.10 Spontaneous fields 154
Exercises 155

10 Semiconductors and dielectrics 157

10.1 Ubiquitous hydrogen impurities 159
10.2 Muonium 160
10.3 Silicon: the foundations 161
10.4 Shallow donor states 165
10.5 Related techniques 166
Exercises 169

11 Ionic motion 170

 Contents xi

11.1 Why use muons? 170

11.2 Science examples 173
11.3 Limitations 175
Exercises 176

12 Chemistry 177
12.1 Chemical environments 177
12.2 Muonium spectroscopy 180
12.3 Reactions of muonium 183
12.4 Muoniated radicals 186
12.5 Structure and dynamics 191
Exercises 198

III Practicalities of muon spectroscopy 199

13 Making muons 200
13.1 Muon production 200
13.2 Surface and decay muons 202
13.3 Beamline components 204
Exercises 209

14 Instrumentation 210
14.1 Spectrometer elements 210
14.2 Pulsed sources 213
14.3 Continuous sources 214
14.4 Small samples 215

15 Doing the experiment 217

15.1 Experimental setup 217
15.2 Calibrations 220
15.3 Data characteristics 221
15.4 Time domain analysis 224
15.5 Frequency domain 230
Exercises 238

IV Further topics in muon spectroscopy 239

16 Calculating muon sites 240
16.1 The site problem 241
16.2 What is DFT? 243
16.3 Methods 246
16.4 Basis sets 248
16.5 Functionals 250
16.6 Mixed methods 251
16.7 Obtaining sites 252
16.8 Quantum effects 257
16.9 Sites via experiment 258
xii Contents

Exercises 261

17 Numerical modelling 263

17.1 Beamline optimization 263
17.2 Muon range profile 265
17.3 Muon spin response 267

18 Low energy µSR 274

18.1 Generating slow muons 274
18.2 LEM facilities 277
18.3 Science examples 280

19 Stimulation methods 283

19.1 Types of stimulation 283
19.2 Case studies 285
19.3 Photoexcitation 288
19.4 Muon-spin resonance 293
Exercises 303

20 High magnetic fields 305

20.1 Why high fields? 305
20.2 Muons and high magnetic fields 307
20.3 Science at high field 310
Exercises 312

21 Muons under pressure 313

21.1 Requirements 313
21.2 The PSI setup 314
21.3 A gas-pressure setup 318
21.4 Science examples 320
21.5 Outlook 321

22 Negative muon techniques 323

22.1 µ− SR spectroscopy 323
22.2 Elemental analysis 328
Exercises 334

V Complementary techniques 335

23 µSR versus other resonance and bulk techniques 336
23.1 Magnetic resonance 336
23.2 When the muon is a plus 340
23.3 Mössbauer spectroscopy 342
23.4 Bulk techniques 344
Exercises 349

24 X-rays, neutrons, and µSR 350

24.1 X-rays 350
 Contents xiii

24.2 Neutrons 352

24.3 Where do muons fit in? 353
Exercises 355

A Fundamental constants 357

B Nuclear moments 358

C Negative muon lifetimes 360

D Answers to selected problems 361

E Muon particle physics 366

E.1 Parity violation 366
E.2 Standard Model and weak interactions 367
E.3 Muon production 368
E.4 Muon decay 369

F Quantum-mechanical polarization functions 373

F.1 Time-dependent perturbations 373
F.2 Evaluating terms 376

G The second moment of a spin distribution 379

G.1 The dipolar interaction 379
G.2 High transverse field 380
G.3 Zero field 384
G.4 Quadrupolar coupling 385

H A short history of µSR 387

Index 406
The basics of µSR 1
This is a book about a set of closely related experiments that use muons
1.1 The key idea 1
to investigate matter. They are known as µSR, which stands for muon-
1.2 The principles of the experi-
spin relaxation, rotation, or resonance. ment 2
1.3 Muon beams and spectrome-
ters 4
1.1 The key idea 1.4 Experimental geometries 6
1.5 What can we do with µSR? 6
The muon is a radioactive particle with a magnetic moment and it Chapter summary 7
can be implanted into a sample.

We will now unpack the various parts of this sentence in more detail. 1
Real experiments work with either one
muon at a time, or a pulse of 102 –103
(a) The muon is a radioactive particle
muons at a time. Therefore, accumu-
lating 2 × 107 total counts might take
The muon is radioactive and so it does not last very long. It has an ≈ 1 hour, though the time depends a lot
average lifetime of τµ = 2.2 µs, after which it decays into other particles. on the beamline and the experiment, as
The special nature of the particle’s decay allows us to read out the we will discuss in due course.
information that the muon probes.
N (t)/N (0)

Example 1.1
The radioactive decay of the muon means that the number of muons n(t) in the
sample a time t after implantation follows the equation

n(t) = n(0) e−t/τµ . (1.1)

This means that if you were able to implant twenty million muons [n(0) = 2 × 107 ] t (µs)
into the sample at t = 0 (a number of muons which is not uncommon1 in a µSR
experiment), the number remaining at t = 20 µs, is 20 × 106 × e−20/2.2 which is over
Fig. 1.1 The total counts as a func-
22,000. So even though the muon decay time is 2.2 µs, you can measure muons that
tion of time from a µSR experiment,
live a lot longer than that.
illustrating the exponential decay pre-
Note also that the number of muons N (t) dt that decay between t and t + dt is
dicted from eqn 1.2.
given by
dn(t) n(0) −t/τµ 2
N (t) = − = e = N (0) e−t/τµ , (1.2) This is because positive muons are of-
dt τ
ten more effective for investigating the
and N (t) is the quantity that is recorded in a µSR experiment (see Fig. 1.1). collective behaviour of matter, com-
pared to negative muons which, owing
to their resemblance to electrons, are
more useful in investigating the chem-
The muon is a subatomic particle and it can be positively or neg- ical elements in a material. However,
atively charged. We usually employ positively charged muons in µSR negatively charged muons are also used
measurements.2 (see Chapter 22).
2 The basics of µSR
3
Sometimes people mistakenly refer to
this technique as ‘muon scattering’,
which is incorrect.
4
The site of the implanted muon is usu-
ally an interstitial position in a crys-
talline solid. This issue will be dis-
cussed in detail in Chapter 16.
B in Fig. 1.2. Specifically, the Larmor (angular) frequency ω is given by
θ
Sµ
Fig. 1.2 In a magnetic field B the
muon spin S µ precesses around the
field on a cone at an angular frequency
of ω = γµ B.
5
Many facilities use old-fashioned cgs
units, and 2 mT translates to 20 G
(i.e. 20 Gauss, where 104 G = 1 T).
Such a calibration is often known as a
‘T20’, which means a transverse field
of twenty Gauss. For more details on
these units, see Appendix A.
6
It is possible to do this though – see
Chapter 20.
(b) The muon has a magnetic moment
The muon is a spin- 12 particle and has a small magnetic moment. Its
magnetic moment allows it to interact magnetically with its environment
and hence investigate the properties of the sample into which it has been
implanted. A major part of this book will be to explore the nature and
consequences of these magnetic interactions.
(c) The muon is implanted in the sample
Note the word implant. This is not a scattering technique, such as X-
ray scattering or neutron scattering, in which an incoming particle is
directed towards a sample along a particular direction and then a scat-
tered particle detected.3 This is an implantation technique in which
the muon is directed towards the sample to be studied and it comes to
a complete rest somewhere inside the sample.4
1.2 The principles of the experiment
Larmor precession
The positive muons that we implant into materials in these experiments
are always spin polarized, so all start with their spins aligned along a
known direction. If there is a magnetic field at the point where a muon
stops in a material, then the muon spin will undergo Larmor preces-
sion around the direction of the local field, at a frequency determined
by the muon gyromagnetic ratio γµ = 2π × 135.5 MHz T−1 , as shown
ω = γµ B, (1.3)
where B is the magnitude of the field at the muon site. Equation 1.3 is
arguably the most important one in this book.
Example 1.2
Calculate the precession frequency for a muon in (a) the Earth’s magnetic field (≈
50 µT), (b) 2 mT, the magnetic field commonly used to calibrate a µSR experiment,5
and (c) 5 T, a relatively high magnetic field.
Solution: We use the formula for precession frequency ν
ω γµ B
ν= = , (1.4)
2π 2π
and obtain (a) 6.8 kHz, (b) 0.27 MHz, and (c) 0.68 GHz. For experimental purposes,
it is often more useful to write the expressions in terms of frequency (ν) units, rather
than angular frequency (ω) units, although, as we will see later, it is often more
convenient in theoretical work to use angular frequency.
As we have seen, a typical µSR experiment might measure times up to around 20 µs
after muon implantation. Precession in the Earth’s magnetic field [which would have
a period of 1/(6.8 kHz) ≈ 150 µs] is therefore too slow to measure directly and one
would just observe the very beginning of a precession signal. On the other hand,
a 5 T field produces very fast precession, and to measure this one would need very
good timing resolution.6
 1.2 The principles of the experiment 3

Asymmetric emission of positrons

When a muon decays, a positron e+ and two neutrinos (ν) are emitted
via the reaction
µ+ → e+ + ν̄µ + νe . (1.5)

A property of this decay (which we will describe in more detail later)

is that the positron is not emitted isotropically, with equal chance of it Sµ
emerging in any direction. Instead it is emitted preferentially along the
direction of the muon spin at the moment of decay. (The distribution
is shown in Fig. 1.3.) Detecting the direction along which the positron
is emitted allows us to work out in which direction the muon spin was
pointing at the moment of its decay. Each muon lives for a different
amount of time (according to the radioactive decay law in eqn 1.1) and
so each muon decay gives rise to a positron whose detection contributes
to a data point at a particular time t. If we make many such positron Fig. 1.3 The probability of positron
detections, taken over many million muon decays, we can build up a emission in the direction of each grey
arrow is indicated by its length. (for
histogram. This histogram then tells us the average spin polarization of a particular value of emitted positron
the large ensemble of muons as a function of time. The data set which we energy; see Appendix E.4 for more
obtain from the experiment is simply the collection of measured average details). Positrons are preferentially
spin polarization values as a function of time after implantation. emitted along the muon spin direction
(shown in a black arrow). The figure
is axially symmetric about the muon-
spin direction (and so looks a bit like
the surface of a cherry in three dimen-
sions).
Example 1.3
A stopped spin-polarized ensemble of muons sits close to the origin of a set of Carte-
sian coordinates. Its spin initially lies along a unique direction (conventionally we
call this z) and a B-field is applied along x. Assuming no other interactions, the
muon spins will precess, undergoing circular motion in the y-z plane at an angular
frequency ω = γµ B. We place positron detectors in front of (i.e. at some value of
positive z) and behind (negative z) the origin. The average polarization P (t) of the
muon ensemble at a particular time t can be found by computing the normalized
difference in the number NF (t) of positrons counted in the forward detector and the
number NB (t) in the backward detector, both measured in a small interval centred
on t, which is to say
P (t)

NF (t) − NB (t)
P (t) ∝ . (1.6)
NF (t) + NB (t)
The polarization in this case is proportional to a cosine function P (t) ∝ cos γµ Bt,
which is simply the circular precessing motion projected along the z direction. If we
did not know the magnitude of the magnetic field we applied, we could measure it
very accurately from the frequency of the oscillations in P (t). An example of some
data showing this effect can be seen in Fig. 1.4. t (µs)

Fig. 1.4 Muon precession in a field of

2 mT.
The polarization P (t) as a function of time t can be used to tell us
about the magnetic field at the muon stopping site. If the magnetic
field at the muon site fluctuates as a function of time, then we can also
obtain information about the nature of those fluctuations. Much of this
book describes how this and other electronic and chemical properties of
matter can be extracted from the data.
4 The basics of µSR

1.3 Muon beams and spectrometers

In order to obtain enough muons to carry out one of these experiments we
must create them in a high-intensity beam of particles. For this reason
the experiments are carried out at facilities where such beams are made
using particle accelerators. Muons are born 100% spin polarized because
of the way they are produced from the decay of pions via a reaction, as
described in the following example.

Example 1.4
In a muon facility, a beam of protons is fired into a target and this makes pions. The
experiment is usually carried out using pions which are at rest in the surface of the
target and which decay quickly into muons via the reaction
π + → µ+ + νµ . (1.7)
Since this reaction must conserve linear and angular momentum, and since the pion
is initially at rest and has no spin or orbital angular momentum, we deduce that
both the muon (µ+ ) and the neutrino (νµ ) must have opposite linear and angular
momenta. Having opposite linear momenta just means the two particles head off in
opposite direction. Because neutrinos always have a negative helicity (i.e. their spin
is always observed to be antiparallel to their momentum) then the muon must also
have negative helicity (so that its spin is also antiparallel to its momentum). For this
reason, we are able to obtain a beam of fully spin-polarized muons.

cryostat

As mentioned in Section 1.1, µSR measurements are not scattering ex-

periments: the muons are always stopped in the material under inves-
tigation. The beam must therefore be of a low enough energy that the
muon can be stopped in (typically) a few hundred milligrams of solid
µ+ matter. The sample under investigation is placed in the beam, where the
muon beam muons stop in the bulk of the material without any appreciable change
sample in their spin orientation nor damage to the material. This is where the
experiment begins, with a muon at rest in the sample in a known spin
state. Muons are introduced into the sample one at a time or in a pulse.
In either case, the number of muons in the sample is so small that there
detector detector
is effectively no possibility of muons interacting with each other: they
are an ultra-dilute probe of matter.
The sample is usually mounted on a sample stick and placed in a
Fig. 1.5 A schematic of a µSR exper-
iment.
cryostat so that its temperature can be varied. The cryostat has a win-
dow to allow the muon beam to enter. The positrons that emerge after
muon decay are very energetic, travelling at a large fraction of the speed
of light, and easily exit the sample and cryostat. They are detected in
particle detectors placed around the cryostat. The apparatus comprising
this array of detectors is known as a spectrometer. The output from
these detectors is connected to the data acquisition system (which has to
receive signals at a very high rate) and then to the analysis computers.
Because the timing of the signals has to be measured to better than a
nanosecond (and sometimes to a few picoseconds) it is worth remember-
ing that the speed of light is around 0.3 m per nanosecond, so the lengths
 1.3 Muon beams and spectrometers 5

of cables and other paths for electrical signals have to be adjusted very
carefully. A very simple schematic of the experiment, showing the main
features of the spectrometer, is shown in Fig. 1.5 (we will discuss many
more details of the experimental arrangement in Chapters 14 and 15).

Example 1.5
An example of a real muon spectrometer is the HiFi instrument at ISIS, as shown
in Fig. 1.6 and Fig. 1.7. The sample is placed in a cryostat at the centre of the
spectrometer, where it stops muons from the particle beam. The sample is surrounded
by positron detectors, each of which consists of a piece of scintillator material linked
optically through a plastic light guide to a photomultiplier.

Fig. 1.6 An exterior view of the HiFi

Fig. 1.7 A cutaway drawing of the HiFi spectrometer. instrument at ISIS.

Muon spectrometers can be used at various user facilities around the

world and the main ones are shown in Fig. 1.8. Two of these have
pulsed muon beams (ISIS, based at the Rutherford Appleton Labora-
tory in Oxfordshire in the UK and J-PARC, located in Tokai, Japan)
while the other two provide continuous muon beams (PSI, in Villigen,
Switzerland and TRIUMF, in Vancouver, Canada). All four operate as
user facilities and beamtime is available through competitive applica-
tions. There is also a continuous muon beam source MuSIC in Osaka,
Japan, and further proposed muon facilities in Korea, China, and the Fig. 1.8 User facilities where µSR ex-
US are at various stages of planning and/or building. periments can be performed.
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