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Organic Ferroelectric Materials
and Applications
Woodhead Publishing Series in Electronic
and Optical Materials
Organic Ferroelectric
Materials and
Applications
Edited by
Kamal Asadi
An imprint of Elsevier
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Contents
Contributors xi
Preface xv
1 Introduction 1
Kamal Asadi
1.1 Piezoelectric phenomena 1
1.2 Pyroelectric phenomena 3
1.3 Ferroelectric phenomena 4
1.4 Conclusion 6
References 6
2 Ferroelectric charge-transfer complexes 7

Sachio Horiuchi, Shoji Ishibashi, and Yoshinori Tokura
2.1 Introduction 7
2.2 Background 10
2.3 Spin-Peierls transition system 15
2.4 Neutral-ionic transition (NIT) system 21
2.5 Miscellaneous approach to ferroelectric CT complexes 34
2.6 Summary and outlook 38
Acknowledgment 39
References 39
3 Hydrogen-bonded organic molecular ferroelectrics/

antiferroelectrics 47
Sachio Horiuchi, Shoji Ishibashi, and Yoshinori Tokura
3.1 Introduction 47
3.2 Prototropic ferroelectrics 49
3.3 Proton-transfer-type binary components 60
3.4 Proton-transfer-type antiferroelectrics 69
3.5 Domain structures 74
Acknowledgement 77
References 77
4 Synthesis of polyvinylidene fluoride and its copolymers 85

Maryam Bozorg, Aldo Altomare, and Katja Loos
4.1 Fluorinated polymers 85
4.2 Poly(vinylidene fluoride) 85
vi Contents
4.3 Homopolymerization of PVDF 86

4.4 Vinylidene fluoride-based copolymers 89
4.5 Well-defined copolymers containing PVDF 91
4.6 Free radical polymerization 91
4.7 Polycondensation 92
4.8 Controlled radical polymerization 93
4.9 Atom transfer radical polymerization (ATRP) 93
4.10 Reversible addition-fragmentation chain transfer
polymerization (RAFT)/macromolecular design via reversible
addition-fragmentation of xanthate (MADIX) 97
4.11 Iodine transfer polymerization 100
4.12 Click chemistry 101
4.13 Grafting 101
4.14 Applications 103
4.15 Conclusion 106
References 107
5 Ferroelectric polymer blends for optoelectronic applications 113

Insung Bae and Cheolmin Park
5.1 Introduction 113
5.2 Thermodynamic preliminaries 114
5.3 Ferroelectric polymer blends: Morphologies, phase separations,
and ferroelectric polarization behaviors 116
5.4 Optoelectronic applications with ferroelectric polymer
blends 126
5.5 Self-assembled ferroelectric block copolymers 142
5.6 Concluding remarks 143
Acknowledgments 145
References 145
6 Nylons 153
Zhongbo Zhang and Lei Zhu
6.2 Ferroelectricity in the crystalline phase of nylons 155
6.3 Ferroelectricity in amorphous phases of nylons 162
6.4 Novel ferroelectric nylons: SHL and DHL 167
References 179
7 Switching dynamics in organic ferroelectrics 185

Tim Cornelissen and Martijn Kemerink
7.2 Dipole switching in organic ferroelectric materials 186
7.3 Analytical models 190
7.4 Monte Carlo models 204
7.5 Molecular dynamics 212
Contents vii
7.6 First-principle theory 217

7.7 Conclusion and outlook 220
References 221
8 Piezoresponse force microscopy for functional imaging of organic

ferroelectrics 233
Haidong Lu and Alexei Gruverman
8.2 Principles of piezoresponse force microscopy 233
8.3 Challenges of PFM characterization in organic
ferroelectrics 236
8.4 Application of PFM technique to organic
ferroelectrics 237
8.5 Conclusion and outlook 259
References 259
9 Dielectric spectroscopy of ferroelectric polymers 263

Valentin V. Kochervinskii and Inna A. Malyshkina
9.2 Methodological aspects 264
9.3 The effect of crystal and supramolecular structure of the
ferroelectric polymers on their dielectric properties 268
9.4 Dielectric properties of textured ferroelectric films 283
9.5 Peculiarities of dielectric relaxation in ultrathin films 305
9.6 Space charge relaxation and phase transitions in heterogeneous
ferroelectric polymers 319
References 343
10 Liquid structuring in fluoropolymer solutions induced by

water 357
Jasper J. Michels, Hamed Sharifi Dehsari,
Mohammad Mahdi Abolhasani, and Kamal Asadi
10.2 Some theoretical ingredients 358
10.3 Water vapor-induced demixing in fluoropolymer
films 362
10.4 Controlled LLPS in electrospun fluoropolymer fibers 366
10.5 Conclusions 372
References 372
11 Solution processing of piezoelectric unconventional structures 375

V.F. Cardoso, C.M. Costa, D.M. Correia, E.O. Carvalho, N. Pe r inka,
P.M. Martins, R.M. Meira, T. Marques-Almeida, T. Rodrigues-Marinho,
and S. Lanceros-Mendez
11.2 Processing and applications of unconventional structures 378
viii Contents
11.3 Final remarks and future trends 419

Acknowledgment 419
References 419
12 Polarization of ferroelectric polymers through electrolytes 441

Negar Sani, Magnus Berggren, and Simone Fabiano
12.2 Ferroelectric/electrolyte interface: The basic concept 442
12.3 Applications 445
References 453
13 Piezoelectric composites 457

Hamideh Khanbareh, Aatif Rasheed, and Jibran Khaliq
13.2 Basic concepts 457
13.3 Critical review 458
Dedication 468
References 468
14 Ferroelectric polymer composites for capacitive energy storage 477

Yao Zhou and Qing Wang
14.2 Dielectric materials for capacitive energy storage 478
14.3 Ferroelectric polymer dielectrics for capacitive energy
storage 479
14.4 Conclusion and perspective 494
References 496
15 Ferroelectric polymers for energy harvesting 503

Zhubing Han and Qing Wang
15.2 Ferroelectric polymers 504
15.3 Piezoelectric nanogenerators 505
15.4 Pyroelectric nanogenerators 512
15.5 Triboelectric nanogenerators 515
15.6 Hybrid nanogenerator 517
15.7 Nanogenerators beyond PVDF 520
15.8 Conclusion 521
References 521
16 Electrocaloric effects in ferroelectric polymers 535

Heng Cui, Wen He, Qibing Pei, and Rujun Ma
16.2 Electrocaloric effect in ferroelectric polymers 545
Contents ix
16.3 Electrocaloric effect in ferroelectric polymer-based

composites 557
16.4 Polymer-based electrocaloric effect devices 563
16.5 Outlook 565
References 565
17 Biomimetic biocompatible ferroelectric polymer materials with an

active response for implantology and regenerative medicine 571
Oleg V. Gradov, Margaret A. Gradova, and Valentin V. Kochervinskii
17.1 Basic criteria for biocompatibility of the implantable materials
and their evolution from passive (since 1970) to active
ones 571
17.2 Surface physics of the implantable material and biointerface as a
prerequisite of biocompatibility 574
17.3 Excitable membrane-mimetic materials with nonstationary
reaction-diffusion properties for development of biocompatible
biomimetic materials 577
17.4 Biocompatibility criteria of ferroelectric polymers as a
consequent of bioferroelectricity 580
17.5 Electrophysical criteria for active biocompatible biomimetic
implants—From energy harvesting toward reactivity 582
17.6 Excitability and multiparametric active response of soft
matter/polymer ferroelectric materials to different external
stimuli 584
17.7 Implantable PVDF-based sensors and actuators within the
framework of “artificial life” and self-organization
concepts 587
17.8 Emergent biomimetic ferroelectric scaffolds as sensors and
actuators for the feedback-controlled tissue
morphogenesis 589
17.9 From PVDF-based sensing to acoustically guided implantable
microfluidics and acoustofluidic micro total analysis
systems 590
17.10 Surface electrocapillary effect and implantable ferroelectric
thread-based microfluidics 592
17.11 Conclusions 593
Acknowledgments 594
References 594
Index 621
Contributors
Mohammad Mahdi Abolhasani Max Planck Institute for Polymer Research, Mainz,
Germany
Aldo Altomare Macromolecular Chemistry and New Polymeric Materials, Zernike

Institute of Advanced Materials, University of Groningen, Groningen, The
Netherlands
Kamal Asadi Department of Physics, University of Bath, Bath, United Kingdom
Insung Bae Department of Advanced Materials, Hannam University, Daejeon, Korea
Magnus Berggren Laboratory of Organic Electronics, Department of Science and

Technology, Link€
oping University, Norrk€
oping, Sweden
Maryam Bozorg Macromolecular Chemistry and New Polymeric Materials, Zernike

Netherlands
V.F. Cardoso CF-UM-UP, Centre of Physics, University of Minho, Braga;

CMEMS-UMinho, University of Minho, Guimarães, Portugal
E.O. Carvalho CF-UM-UP, Centre of Physics; CEB, University of Minho, Braga,

Portugal
Tim Cornelissen Department of Physics, Chemistry and Biology (IFM), Link€oping

University, Link€oping, Sweden; Centre for Advanced Materials, Ruprecht-Karls-
Universit€at Heidelberg, Heidelberg, Germany
D.M. Correia CF-UM-UP, Centre of Physics, University of Minho, Braga; Centre of

Chemistry, University of Trás-os-Montes e Alto Douro, Vila Real, Portugal
C.M. Costa CF-UM-UP, Centre of Physics; Centre of Chemistry, University of

Minho, Braga, Portugal
Heng Cui School of Materials Science and Engineering, National Institute for
Advanced Materials, Tianjin Key Lab for Rare Earth Materials and Applications,
Nankai University, Tianjin, P. R. China
xii Contributors
Simone Fabiano Laboratory of Organic Electronics, Department of Science and

Technology, Link€
oping University, Norrk€
oping, Sweden
Oleg V. Gradov N.N. Semenov Federal Research Center for Chemical Physics,
Russian Academy of Sciences, Moscow, Russia
Margaret A. Gradova N.N. Semenov Federal Research Center for Chemical Physics,
Russian Academy of Sciences, Moscow, Russia
Alexei Gruverman Department of Physics & Astronomy and Nebraska Center for
Materials and Nanoscience, University of Nebraska, Lincoln, NE, United States
Zhubing Han Department of Materials Science and Engineering, The Pennsylvania

State University, University Park, PA, United States
Wen He School of Materials Science and Engineering, National Institute for

Sachio Horiuchi Research Institute for Advanced Electronics and Photonics

(RIAEP), National Institute of Advanced Industrial Science and Technology (AIST),
Tsukuba, Japan
Shoji Ishibashi Research Center for Computational Design of Advanced Functional

Materials (CD-FMat), National Institute of Advanced Industrial Science and
Technology (AIST), Tsukuba, Japan
Martijn Kemerink Department of Physics, Chemistry and Biology (IFM), Link€oping

University, Link€oping, Sweden; Centre for Advanced Materials, Ruprecht-Karls-
Universit€at Heidelberg, Heidelberg, Germany
Jibran Khaliq Department of Mechanical and Construction Engineering,

Northumbria University, Newcastle upon Tyne, United Kingdom
Hamideh Khanbareh Department of Mechanical Engineering, University of Bath,

Bath, United Kingdom
Valentin V. Kochervinskii Karpov Institute of Physical Chemistry, Moscow, Russia
S. Lanceros-Mendez CF-UM-UP, Centre of Physics, University of Minho, Braga,

Portugal; BCMaterials, University of the Basque Country UPV/EHU Science Park,
Leioa; IKERBASQUE, Basque Foundation for Science, Bilbao, Spain
Contributors xiii
Katja Loos Macromolecular Chemistry and New Polymeric Materials, Zernike

Netherlands
Haidong Lu Department of Physics & Astronomy and Nebraska Center for Materials
and Nanoscience, University of Nebraska, Lincoln, NE, United States
Rujun Ma School of Materials Science and Engineering, National Institute for

Inna A. Malyshkina Faculty of Physics, M.V. Lomonosov Moscow State University,

Moscow, Russia
T. Marques-Almeida CF-UM-UP, Centre of Physics; CEB, University of Minho,

Braga, Portugal
P.M. Martins CF-UM-UP, Centre of Physics; IB-S; CBMA, University of Minho,

Braga, Portugal
R.M. Meira CF-UM-UP, Centre of Physics; CEB, University of Minho, Braga,

Portugal
Jasper J. Michels Max Planck Institute for Polymer Research, Mainz, Germany
Cheolmin Park Department of Materials Science and Engineering, Yonsei

University, Seoul, Korea
Qibing Pei Department of Materials Science and Engineering, Henry Samueli School
of Engineering and Applied Science, University of California, Los Angeles, CA,
United States
N. Perinka BCMaterials, University of the Basque Country UPV/EHU Science Park,

Leioa, Spain
Aatif Rasheed Department of Mechanical and Construction Engineering,

Northumbria University, Newcastle upon Tyne, United Kingdom
T. Rodrigues-Marinho CF-UM-UP, Centre of Physics, University of Minho, Braga,

Portugal
Negar Sani Division of Digital Systems, Sensor Systems, RISE Research Institutes of
Sweden, Gothenburg, Sweden
xiv Contributors
Hamed Sharifi-Dehsari Max Planck Institute for Polymer Research, Mainz,

Germany
Yoshinori Tokura Riken Center for Emergent Matter Science (CEMS), Wako;
Tokyo College and Department of Applied Physics, The University of Tokyo, Tokyo,
Japan
Qing Wang Department of Materials Science and Engineering, The Pennsylvania

State University, University Park, PA, United States
Zhongbo Zhang Department of Macromolecular Science and Engineering, Case

Western Reserve University, Cleveland, Ohio, United States
Yao Zhou Department of Materials Science and Engineering, The Pennsylvania State
University, University Park, PA, United States
Lei Zhu Department of Macromolecular Science and Engineering, Case Western

Reserve University, Cleveland, Ohio, United States
Preface
During the past half-century, the field of electronic and electroactive molecular mate-
rials has witnessed a considerable progress due to the great technological promises of
this class of materials. The flexibility in the electronic structure that is offered by
molecular materials, which can be uniquely tailored by design and realized by syn-
thetic chemistry, has been exploited for many applications ranging from flexible elec-
tronics to energy devices. One of the main research focus areas is dielectrics, which
includes piezoelectrics, pyroelectrics, and ferroelectrics. This book focuses on recent
development in pyroelectric, piezoelectric, and ferroelectric phenomena in organic
molecular materials.
Piezoelectricity in organic materials has received a great deal of attention after the
discovery of piezoelectric property in poly(vinylidene fluoride), PVDF, in the 1960s.
During the past decades, there has been a tremendous growth in exploring the material
science, physics, chemistry, and industrial applications (particularly in microelec-
tronic and energy devices) of molecular organic ferroelectric materials. Besides
PVDF and its random copolymer with trifluorethylene, P(VDF-TrFE), other organic
polymers such as polyamides (odd-nylons), cyanopolymers, polyureas, polythioureas,
biopolymers (polypeptides and cellulose), polymer ferroelectric liquid crystals,
polymer-ceramic composites, as well as small organic molecular systems, have been
extensively studied. Nevertheless, due to their relative ease of processing and realiza-
tion of the piezo- and ferroelectric phase, PVDF and P(VDF-TrFE) have contributed
substantially to our understanding of piezo- and ferroelectricity in organic materials
and also to the realization of prototypical devices for various applications.
The field has seen a rapid growth recently in fundamental research as well as in
novel applications of the organic ferroelectric materials, and therefore, it is timely
to consolidate the current knowledge on their science and applications into a single
reference source. This book is a valuable reference for researchers in this field and
collects developments from over the past two decades, in the chemistry, physics,
and technology of the organic ferroelectric materials by experts in the field. This book
is organized in two parts. The first part discusses chemistry, physics, and materials
science of various organic ferroelectric materials. The second part of this book dis-
cusses how these materials can be used in different devices for various applications.
The overview of the chapters is as follows: Chapter 1 provides a general overview of
ferroelectrics and presents a few basics of ferroelectrics. Chapters 2–6 discuss in gen-
eral materials science of various organic ferroelectrics. Chapter 7 presents an account
of the present understanding of dipole switching mechanisms in organic ferroelectrics.
In Chapters 8 and 9, a detailed discussion about two powerful techniques, namely,
piezoelectric force microscopy and broadband dielectric spectroscopy of organic fer-
roelectrics, is made. Chapters 9 and 10 cover issues around processing of organic
xvi Preface
ferroelectrics, in particular polymers. These chapters present guidelines for processing

ferroelectric and piezoelectric polymers into thin films and unconventional structures
such as fibers and spheres. The last part of this book, Chapters 12–17, discuss a
selected list of applications of piezoelectric and ferroelectric polymers.
The aim of putting this volume together is to present an up-to-date account of var-
ious aspects of the field of organic ferroelectrics. Admittedly, the list of topics chosen
for this book is by no means complete to cover the field from all angles. Nevertheless,
one must select, and I hope that the readers will enjoy the selection provided and will
find this book a useful and stimulating source of information to conduct future
research.
I have the greatest appreciation for the contributing authors who laid the foundation
of this book, for their hard work and valuable time particularly during the challenging
period due to pandemic, and I thank them for their dedication. I am also thankful
to Woodhead Publishing and Elsevier for the excellent support in bringing this volume
to reality.
Kamal Asadi
Bath
Introduction
Kamal Asadi
Department of Physics, University of Bath, Bath, United Kingdom
1
1.1 Piezoelectric phenomena
The piezo- in the word piezoelectrics is derived from a Greek word, piezein, meaning
pressure. Piezoelectric materials can generate electricity when mechanical stress is
applied (direct effect). Conversely, when an electric field is applied, the material will
be mechanically stressed. The Curie brothers, Pierre and Jacques, discovered the
interconvertible of the direct and converse piezoelectric effect in 1880 [1].
Crystals that have a non-centrosymmetric structure and are formed by polar mol-
ecules exhibit piezoelectric property, i.e., the material generates a voltage when it is
mechanically stressed (direct piezoelectric effect). Interconvertibility of the piezo-
electric effect means that the application of an electric field (depending on the direc-
tion of the field) generates a mechanical strain, expansion, or contraction in the
piezoelectric material (converse piezoelectric effect) [2].
The application of an electric field always distorts the geometric shape of the
dielectric materials. The materials are constructed of positively charged nuclei sur-
rounded by a compensating negatively charged electron cloud. Applying an electric
field on dielectrics induces polarization, causes changes in charge distribution and,
therefore induces mechanical distortion. The strain resulting from the mechanical dis-
tortion is called electrostriction and is proportional to the square of the field, as shown
in Fig. 1.1. All materials exhibit electrostriction, although in most cases, its effect is
negligible [2].
There are two principal mechanisms for piezoelectricity [3]: (1) The material lacks
a net dipole in the unit cell under the unstrained condition but shows a piezoelectric
response when stressed or strained. A prime example is Quartz. In this case, the elec-
tric field and the mechanical strain have a linear relationship (in the first approxima-
tion), which is also referred to as the linear piezoelectric effect. (2) The unit cell of the
materials has a net dipole moment along its polar axis. If the orientation of the dipole is
changeable with the application of an electric field, then the variation of the mechan-
ical strain with the applied electric field follows the change of polarization in the hys-
teresis loop, as shown in Fig. 1.2. During the poling process, a conventional inorganic
piezoelectric experiences a small expansion along the applied electric field direction
and a contraction in the perpendicular direction, so that the strain along the poling
direction is positive, as schematically shown in Fig. 1.2B. For organic piezoelectrics,
in particular polymers, a reverse relationship occurs, i.e., piezoelectric polymers
contract along the applied electric field direction, as shown in Fig. 1.2C.
Organic Ferroelectric Materials and Applications. https://doi.org/10.1016/B978-0-12-821551-7.00018-X

2 Organic Ferroelectric Materials and Applications
Fig. 1.1 Schematic

representation of
electrostriction, where the
material expands in the field
direction and contracts in
the perpendicular direction.
Fig. 1.2 Strain versus applied electric field for various materials with (A) a linear piezoelectric
behavior, (B) positive piezoelectric coefficient, and (C) negative piezoelectric coefficient.
Fig. 1.2B and C presents a schematic of poling and strain in different piezoelectric
materials with positive and negative strain responses, which can be defined as piezo-
electric coefficient. The solid lines trace the poling behavior of the material from vir-
gin un-poled state with zero polarization to a saturation polarization. In doing so, most
piezoelectrics expand in the poling direction, yielding the well-known butterfly-
shaped hysteresis-positive strain–field relations (Fig. 1.2B). On the contrary, ferro-
electric polymers such as PVDF and its copolymers exhibit a negative strain–field
relations, as shown in Fig. 1.2C.
The interactions between the electrical and the mechanical variables that describe
the piezoelectric effects can be written as:
D ¼ dX + εX E (1.1)
S ¼ yE X + dE (1.2)
Introduction 3
where D is the dielectric displacement, E is the electric field, X and S are, respectively,
the mechanical stress and strain, y is the elastic stiffness coefficient at a constant elec-
tric field E, and εXis the relative permittivity at constant stress X. The coefficient d is
defined as piezoelectric coefficient and has a unit of coulombs/newton for the direct
piezoelectric effect (Eq. 1.1), and meter/volt for the converse piezoelectric effect
(Eq. 1.2). Since piezoelectric properties are dependent on orientation direction, d,
εX, and y must be described in tensor forms. However, a rigorous mathematical treat-
ment of the subject is beyond the scope of this chapter, as there are numerous books
published on this topic. The ability of a piezoelectric to convert mechanical energy to
electricity (and vice versa) is determined by the electromechanical coupling factor k,
which is defined as:
Electrical energy from converson

k2 ¼ (1.3)
Total input mechanical energy
for the direct piezoelectric effect and
Mechanical energy from conversion

k2 ¼ (1.4)
Total input electrical energy
for the converse piezoelectric effect.
1.2 Pyroelectric phenomena

The prefix pyro- in pyroelectrics means heat in Greek, which implies that pyroelec-
trics generate electricity upon heating. Pyroelectric phenomenon was first discovered
in tourmaline in 314 BCE, but was revisited in modern times in 1824 by Brewster, and
its theory was first formulated in 1878 by Lord Kelvin.
A subclass of piezoelectrics, besides their non-centrosymmetric unit cell, have a
unique polar axis and are spontaneously polarized in their pristine unstrained form.
However, the polarity of the unit cell is sustained only over a certain temperature
range. Such crystals, in addition to their piezoelectric properties, also exhibit pyro-
electric effects, i.e., electric charges will develop on the surface of the pyroelectrics,
when the material is uniformly heated. It should be noted that temperature gradient
caused, for instance, by nonuniform heating will cause a mechanical stress, and there-
fore, the material will have mixed piezoelectric and pyroelectric effects. Therefore,
uniform heating condition is required to decouple piezoelectric effect from the pyro-
electric activity of the material. Since pyroelectricity results from the temperature
dependence of the spontaneous polarization of the polar materials, it occurs also in
single domain crystals or poled polycrystalline ferroelectric materials. A change in
temperature will cause a corresponding change in polarization, which produces a
current if the material is connected to an external circuit.
Pyroelectricity in a material is dependent on the thermal, mechanical, and electrical

constraints on the crystal. The relation between electric displacement, D, and temper-
ature, T, that defines the pyroelectric coefficient is:
dD
pX ¼ (1.5)
dT
where pX is measured at constant mechanical stress and has the unit coulomb cm2 K1.
A change in temperature will cause a change in the polarization of the material. When the
temperature of the material remains constant for a sufficiently long time, the material
reaches an equilibrium and there will be no charge flow. Note the pyroelectric coefficient
under constant mechanical stress condition means that the crystal is not clamped and is
free to expand or contract thermally. When clamping at the interfaces such as electrodes
is considered, the treatment of the pyroelectric becomes more involved and Equation 1.5
cannot be used.
Before ending this section, two considerations should be pointed out. Pyroelectrics
do have a nonzero macroscopic polarization. Therefore, all ferroelectric materials are
also pyroelectric as well. However, only those ferroelectrics with the second-order
transition at the Curie point are suitable for application because materials that exhibit
a steep first-order transition at the Curie point show a thermal hysteresis.
The converse pyroelectric effect is called electrocaloric effect, where an electric
field is applied to the sample to cause a temperature change. The equation of state
for an electrocaloric effect can be written as:
1
dS ¼ αE dX + pX dE + dT (1.6)
T yX,E
Assuming an adiabatic process, hence constant entropy condition where dS ¼ dX ¼ 0,

the electrocaloric coefficient is defined as
dT
qX ¼ ¼ TyX,E pX (1.7)
dE S,X
where the unit of qX is K m V1.
1.3 Ferroelectric phenomena

The term ferroelectrics was coined by analogy with ferromagnetics, mainly because
ferroelectrics show a hysteretic displacement loop under the electric field that looks
like that of magnetization loop of ferromagnetics under magnetic fields. Despite the
prefix ferro, which is derived from ferum meaning iron in Latin, in conventional fer-
roelectrics there are (usually) no iron atoms. Ferroelectricity was discovered much
later than piezo- and pyroelectricity in 1920 in Rochelle salt by Valasek [4]. A ferro-
electric crystal shows a switchable spontaneous electric polarization and a hysteresis
Introduction 5
loop, as shown in Fig. 1.2B and C. The D (or P)-E loop is observed in a certain tem-
perature regime wherein the crystal structure satisfies the non-centrosymmetric con-
dition. The upper temperature limit is called Curie temperature, Tc, above which the
crystal is no longer ferroelectric and exhibits a dielectric behavior. Near Tc, the fer-
roelectrics have an unusually high dielectric constant, which closely follows the
Curie–Weiss relation:
C
ε¼ (1.8)
T TC
where C is called the Curie constant. At Tc, the crystal usually undergoes a phase tran-
sition and a change in its crystal structure, as a result of which besides the dielectric
constant and polarization, also elastic constants and specific heat will also change.
Ferroelectrics are characterized by their switchable spontaneous polarization, PS,
whose direction can be changed by the application of an external electric field. At low
enough electric field, ferroelectrics behave just like all other linear dielectrics and
exhibit a linear behavior in D in response to electric field, E. Once the strength of
the field is above a certain threshold field called the coercive field, EC, the dipoles
begin to align with the electric field and induce a net dipole in the crystal. A typical
hysteresis loop is shown schematically in Fig. 1.2B and C. At high fields, polarization
saturates, and as the field is decreased to zero, the polarization will reduce accord-
ingly, but does not go to zero at zero field. The remaining polarization is called
remanent polarization Pr.
Ferroelectricity is a fascinating property of single crystals or polycrystalline dielec-
tric solids. Ferroelectric materials not only exhibit reversible spontaneous polarization
but also respond to external stimuli in the form of mechanical stress and temperature.
As a result, the ferroelectric materials are employed for a wide range of applications
from microelectronic devices to precision mechanical machinery, and from sonar to
space applications.
Besides conventional ferroelectric crystals, which are mostly based on ceramics,
some synthetic and biological polymers also exhibit piezoelectric, pyroelectric, and
ferroelectric properties. In fact, ferroelectricity was historically discovered in
potassium-sodium tartrate tetrahydrate (KNaC4H4O6 ∙ 4H2O) crystal, a molecular
compound also known as Rochelle salt [4]. Study of the ferroelectric properties of
Rochelle salt, particularly at phase transition temperature, contributed significantly
to shaping our initial understanding of ferroelectrics. Rochelle salt, however, has a
Curie temperature that is below room temperature and rather poor mechanical strength
and low disintegration temperature. Another molecular compound that grabbed
early attention is triglycine sulfate (TGS) with a chemical formula of
(NH2CH2COOH)3 ∙ H2SO4. TGS is a uniaxial ferroelectric and exhibits room-
temperature ferroelectricity, with the Curie temperature that is about 49°C. It was
around the middle of 20th century when piezoelectricity in natural substances,
namely, wood, was discovered [5]. Piezoelectricity in wood originates from a natural
polymer called cellulose. Piezoelectricity in synthetic polymers, namely, poly-
vinylidene fluoride (PVDF), was discovered in 1969 [6] followed by the
demonstration of its pyroelectricity in 1971 [7], and eventually its ferroelectric prop-
erties in the late 1970s and the early 1980s [8]. PVDF, or its copolymer, has been the
subject of active research since the discovery of its piezoelectric property. Molecular
materials, in particular polymers, are suited for many applications because of their
easy processability into thin, and flexible films. With the power of synthetic chemis-
try, it is also possible to change the chemical structure and even introduce further func-
tionality in the molecular systems and to realize multifunctional smart materials. Due
to their molecular nature, the crystalline structure of molecular or polymeric systems
are rather complex. In the microstructure of the molecular system, the ferroelectric
crystalline phase coexists with an amorphous phase and possibly other non-
ferroelectric crystalline phases. Hence, the observation of piezoelectric, pyroelectric,
and ferroelectric activities in molecular systems would require a close attention.
1.4 Conclusion
This book provides an overview of the development in the field of organic and molec-
ular ferroelectrics, with a focus on achievements over the past two decades. There are
already two books [9,10] providing a good summary of early literature and a good
overview of the basic knowledge needed to start in this field. This book therefore brid-
ges the gap between the early and most recent literature by presenting the develop-
ments over the past two decades, which are organized in two parts. The first part
discusses chemistry, physics, and in general the materials science of various poly-
meric and molecular ferroelectric materials. The second part discusses various
applications.
References
J. Curie, P. Curie, Compt. Rend. 91 (1880) 294. and 95 (1881) 1137.
[1]
[2]
K.C. Kao, Dielectric Phenomena in Solid, first ed., Academic Press, 2004.
[3]
I. Bunget, M. Popesco, Physics of Solid Dielectrics, Elsevier, 1984.
[4]
J. Valasek, Phys. Rev. 17 (1921) 475.
[5]
E. Fukada, M. Date, N. Hirai, Nature 211 (1966) 1079.
[6]
H. Kawai, Jpn. J. Appl. Phys. 8 (1969) 975.
[7]
J.G. Bergman Jr., J.H. McFee, G.R. Crane, Appl. Phys. Lett. 18 (1971) 203.
[8]
A.J. Lovinger, G.T. Davis, T. Furukawa, M.G. Broadhurst, Macromolecules 15
(1982) 323.
[9] A.M. Glass, J.M. Herbert, T.T. Wang, The Applications of Ferroelectric Polymers,
Springer, 1988.
[10] H.S. Nalwa (Ed.), Ferroelectric Polymers, CRC Press, 1995.
Ferroelectric charge-transfer
complexes 2
Sachio Horiuchia, Shoji Ishibashib, and Yoshinori Tokurac,d
a
Research Institute for Advanced Electronics and Photonics (RIAEP), National Institute of
Advanced Industrial Science and Technology (AIST), Tsukuba, Japan, bResearch Center
for Computational Design of Advanced Functional Materials (CD-FMat), National Institute
of Advanced Industrial Science and Technology (AIST), Tsukuba, Japan, cRiken Center for
Emergent Matter Science (CEMS), Wako, Japan, dTokyo College and Department of Applied
Physics, The University of Tokyo, Tokyo, Japan
2.1 Introduction
Developing organic molecular ferroelectrics has still been a challenging task, because
only a limited class of polar crystals have some structural flexibilities enough to
reverse the crystal polarities. In this light, one of the straightforward principles to gen-
erate dipoles is a relative displacement of differently charged ions or molecules.
Charge-transfer (CT) complexes are the binary- or multicomponent molecular system
made up by a cohesive force arising from CT interactions (transfer integral, t), i.e., the
orbital hybridization between the highest occupied molecular orbital (HOMO) of elec-
tron donor (D) molecules and the lowest unoccupied molecular orbital (LUMO) of
acceptor (A) molecules. Since the first discovery of ferroelectric signature in permit-
tivity, direct or indirect evidences of ferroelectricity have been found on more than 10
CT complexes until 2020. Many intriguing and exotic behaviors as well as novel func-
tionalities highlighted in these studies are relevant to the charge and spin dynamics
rather than the displacement (dimerization) model of static charges.
CT complexes are roughly classified into three types according to the molecular
arrangements (Fig. 2.1A). In most of the ferroelectric CT complexes, the D and
A molecules are interacting face-to-face with each other, adopting a packing motif
called DA mixed stacks. Mixed stacking of pairwise DA dimers corresponds to the
polar configuration (iv) in Fig. 2.1B. In contrast, DA segregated stacks in the CT com-
plexes or 1D columns or 2D layers in the CT salts are rather suitable for metallic
charge transport. Dimerization (configuration (ii) in Fig. 2.1B) in the chemically
homogenous stack cannot yield the polarity unless it is accompanied by some site
inhomogeneity like charge ordering like the configuration (iv).
Studies on CT complexes started with the Mulliken’s theory [1] describing that
orbital hybridization between the D and A molecules with a CT integral t (Fig. 2.2A),
gives rise to the fractional degree of CT ρ as a key parameter for molecular conductors
and magnets. In 1965, McConnell, Metzger, and Hoffmann theoretically demon-
strated the interface between neutral diamagnetic CT complexes (ρ ¼ 0) and ion
Organic Ferroelectric Materials and Applications. https://doi.org/10.1016/B978-0-12-821551-7.00007-5

Fig. 2.1 Schematic structural representations of CT complexes and CT salts. (A) The typical molecular stacking types. (B) Creation of polar chains
from bond- and charge-ordering. (C) A variety of structural deformations in forming polar stacks.
(a) (d) (f)
(b)
(e)
(g)
(c)
Fig. 2.2 Fundamental properties of DA-mixed stack CT complexes. (A) Energy diagrams of the neutral and ionic states. (B) (Spin-)Peierls transition
and two types of NITs. (C) Band gap opening with the DA dimerization. (D) Charge-transfer processes. (E) CT transition energy. (F) Phase transition
from nonpolar neutral to bipolar ionic states. (G) Spin soliton, charge soliton, and NI domain wall (NIDW) excited in the chain. Arrows and rounded
boxes in (B) and (G) represent the spins and dimerized DA pairs, respectively.
radical salts (ρ ¼ 1) and predicted the corresponding phase transition (Fig. 2.2A) [2].
In 1981, Torrance et al. discovered this neutral-ionic phase transition (NIT) with both
hydrostatic pressures and temperature changes on DA-mixed stack compounds with
findings of drastic changes of optical spectra [3, 4]. It is quite exotic switching
between the two contrastive states of matter in a solid, i.e., van der Waals molecular
assembly and ionic solid. Furthermore, one-dimensionality of electronic systems
along the stacks experiences the so-called (spin-)Peierls instability, which spontane-
ously generates the stack of dipolar DA pairs. This reversible DA dimerization is just
what we want for the switchable polarities. The signatures of one-dimensional ferro-
electricity were first identified by Tokura et al. as a sharp permittivity peak or a cusp
indicative of the phase transition for several CT complexes [5].
Besides the Peierls-type dimerization, several structural strategies have been
proposed in designing dipolar CT complexes for ferroelectricity. Permanent dipoles
parallel or normal to the DA mixed stacks can be switchable if the D or A molecule is
mechanically flexible enough to permit its spontaneous bending or disk rotation, as
shown in Fig. 2.1C. The other case concerns the electron flow between the charge-
disproportionated molecules in CT salts.
This chapter is outlined as below. Section 2.2 introduces the basic background and
pioneering work on the electronic and lattice instabilities as the driving force for
exotic ferroelectricity. Section 2.3 focuses on a ferroelectric spin-Peierls transition
(SPT) in fully ionic CT complexes. Section 2.4 demonstrates a ferroelectric NIT
and many relevant novel dielectric properties such as relaxor, quantum critical behav-
iors, and electronic ferroelectricity. Section 2.5 is a brief overview of ferroelectricity
achieved by a variety of mechanisms other than the Peierls type.
2.2 Background
2.2.1 Valence instability
First, we begin with a D–A dimer with a hopping integral t between two levels. The
electronic ground state is described by a mixture of neutral state jD0A0i and ionic one
j D+ Ai with degree of CT ρ as
pffiffiffiffiffiffiffiffiffiffi 0 0 pffiffiffi +
|Gi ¼ 1 ρ |D A i + ρ |D A i
Energy difference between the neutral (N) and ionic (I) states is 2Γ ¼ ID EA v,
where ID is the ionization potential of D, EA is the electron affinity of A, and v is
the Coulomb interaction between fully ionic D+ and A. The ionicity is expressed with
η ¼ Γ/t as
!
1 η
ρ¼ 1 pffiffiffiffiffiffiffiffiffiffiffi
2 η2 + 2
Ferroelectric charge-transfer complexes 11
In the model by McConnell et al. [2], the ground states of mixed DA molecular stack are
described assuming negligibly small transfer integral √ 2 t ¼ D+ A j Hj D0 A0 ¼ 0,
the ground state is either neutral diamagnetic with ρ ¼ 0 or fully ionic paramagnetic
with ρ ¼ 1 carrying spin S ¼ 1/2 on each molecule (Fig. 2.2A). The N–I phase inter-
face is located where the energy ID–EA required to ionize D and transfer the electron
to the A molecule equals to the Madelung (electrostatic) energy αv per D+ A pair.
Here, v e2/dDA is the nearest neighbor Coulomb interaction, dDA is a D–A separa-
tion, and α > 1 is the Madelung constant. The CT excitation energies are
hνCT ðNÞ ¼ ID EA v
hνCT ðIÞ ¼ ðID EA Þ + ð2α 1Þv
for neutral and ionic CT complexes, respectively (Fig. 2.2D). They are minimized to
(α – 1)v and coincide with each other at the N–I phase interface, where energy required
for ionization, ID–EA, equals the Madelung energy gain, αv (Fig. 2.2E). When the
Madelung energy gain is increased with lattice compression, the N–I phase boundary
sweeps rightward, expanding the I region, and then the neutral CT complexes in close
vicinity of the boundary experience the NIT. Whereas Torrance et al. discovered
pressure-induced NIT (PINIT) in many CT complexes, smaller effects of thermal
expansion restrict the chance to encounter the temperature-induced NIT (TINIT),
as shown by the shaded area in Fig. 2.2E.
2.2.2 Lattice instability

The real DA stack system with a finite t constructs a one-dimensional band. The ionic
DA stacks give rise to a Mott insulator with one electron per site, if their on-site
Coulomb interaction U is large compared with bandwidth 4t. The system behaves
as a 1D Heisenberg antiferromagnet with the kinetic exchange J ¼ t2/2 j Γ j
(J ¼ 2t2/U for U ≫ t limit) and can be a ferroelectric or antiferroelectric when the
electron-lattice interaction induces an SPT at TSP (Fig. 2.2B).
If the electron-lattice coupling causes alternating transfer integrals as t(1 δ)
in the DA mixed stack, the energies of the valence and conduction bands are
expressed by
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
εk ¼ Δ2 + 4t2 cos 2 k + 4δ2 t2 sin 2 k
Here, 2Δ ¼ ID—EA—αv + U is the difference in site energies. Fig. 2.2C exemplifies

the band structure without site energy difference (2Δ ¼ 0) between D and A. In this
special case, the regular DA stacking (δ ¼ 0) realizes the metallic state with half-filled
band structure of bandwidth 4t (red dotted curves). A novel metallic behavior with
high conductivity was actually observed [6]. Note that the band filling is independent
of ionicity. This picture also implies that compounds at the N–I interface have the
maximum energy gain with a Peierls distortion causing the DA dimerization by open-
ing the gap of 4δt at the Fermi level (solid blue curve in Fig. 2.2C). Increment of site
energy difference expands the band gap even with the regular DA stacks and simul-
taneously produces the energy gain with dimerization. This qualitatively explains the
empirical trend [7] that the dimerization increases with decreasing ρ in the ionic com-
plexes (0.5 < ρ < 1). Therefore, approaching to the N–I phase interface is promising
for the enhancement of dimerization in search for ferroelectricity.
The DA-dimerized stacks have two degenerate configurations of opposite polari-
ties. Thereby, NIT accompanied by the dimerization transforms the single minimum
in potential curves into the doubled ones as a function of dimerization (polarization)
(Fig. 2.2F). One-dimensional lattice permits the low-energy excitations creating
the mobile soliton-like topological defects, which correspond to unpaired D or
A molecules at the interface between the oppositely dimerized regions (i.e., domains)
(Fig. 2.2G) [5, 8, 9]. In the ionic DA mixed stacks, there are four kinds of solitons
depending on their molecular valence: spin solitons carrying a spin S ¼ 1/2 on either
D+ or A molecule and charge solitons on either D0 or A0 molecule. These solitons as
well as the N–I domain walls (NIDWs) (Fig. 2.2G) have been found to play important
roles in topological charge transport as well as dielectric responses.
2.2.3 Experimental probes of ionicity

Transformation of electronic state from neutral ρ ¼ 0 to fully ionic ρ ¼ 1 modifies the
molecular structures, especially the geometries of π-bonds, which have significant
contributions to the highest occupied molecular orbital (HOMO) and/or the lowest
unoccupied molecular orbitals (LUMO). Reversely speaking, lengths and stretching
vibration frequencies of these bonds can be a critical function of ρ. These relationships
are well studied for TTF, TCNQ (TTF ¼ tetrathiafulvalene; TCNQ ¼ 7,7,8,8-tetracy-
anoquinodimethane; see Fig. 2.3 for the chemical structures), and their derivatives,
i.e., excellent building blocks of the organic conductors. At the early stage, a linear
relationship between the molecular charge –ρ and infrared active vibrational mode
frequencies was demonstrated as ν(ρ) ¼ ν(0) Δνρ, using the antisymmetric C^N
stretching mode of TCNQ showing the ionization frequency shift Δν of about
40 cm1 at around 2200 cm1 [10]. Since then, this convenient test has been exam-
ined for numerous TCNQ complexes (see the review by Jacobsen [11]), although the
frequency may be often modulated by strongly interacting C^N groups with adjacent
molecules/ions as in the case of hydrogen-bonded complexes or metal-coordinated
TCNQ salts. The use of C]C stretching mode frequencies is recommended to avoid
this problem [12]. Likewise, mode assignments of molecular vibrational spectra and
identification of the diagnostic modes of ionicity have been made for a variety of
donor and acceptor molecules [13–15].
Highly accurate crystal structures can be excellent probes to specify the molecular
ionicity site-by-site. For instance, ρ of the TCNQ molecule has been estimated from
the bond lengths between carbons through the systematic linear interpolations
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world of consciousness, and we are not necessarily opposed to
attempts to reach the physical world from that end. From the point of
view of philosophy it is desirable that this entrance should be
explored, and it is conceivable that it may be fruitful scientifically. If I
have rightly understood Dr. Whitehead’s philosophy, that is the
course which he takes. It involves a certain amount of working
backwards (as we should ordinarily describe it); but his method of
“extensive abstraction” is intended to overcome some of the
difficulties of such a procedure. I am not qualified to form a critical
judgment of this work, but in principle it appears highly interesting.
Although this book may in most respects seem diametrically
opposed to Dr. Whitehead’s widely read philosophy of Nature, I think
it would be truer to regard him as an ally who from the opposite side
of the mountain is tunnelling to meet his less philosophically minded
colleagues. The important thing is not to confuse the two entrances.
Nature of Exact Science. One of the characteristics of physics is that

it is an exact science, and I have generally identified the domain of
physics with the domain of exact science. Strictly speaking the two
are not synonymous. We can imagine a science arising which has
no contact with the usual phenomena and laws of physics, which yet
admits of the same kind of exact treatment. It is conceivable that the
Mendelian theory of heredity may grow into an independent science
of this kind, for it would seem to occupy in biology the same position
that the atomic theory occupied in chemistry a hundred years ago.
The trend of the theory is to analyse complex individuals into “unit
characters”. These are like indivisible atoms with affinities and
repulsions; their matings are governed by the same laws of chance
which play so large a part in chemical thermodynamics; and
numerical statistics of the characters of a population are predictable
in the same way as the results of a chemical reaction.
Now the effect of such a theory on our philosophical views of the
significance of life does not depend on whether the Mendelian atom
admits of a strictly physical explanation or not. The unit character
may be contained in some configuration of the physical molecules of
the carrier, and perhaps even literally correspond to a chemical
compound; or it may be something superadded which is peculiar to
living matter and is not yet comprised in the schedule of physical
entities. That is a side-issue. We are drawing near to the great
question whether there is any domain of activity—of life, of
consciousness, of deity—which will not be engulfed by the advance
of exact science; and our apprehension is not directed against the
particular entities of physics but against all entities of the category to
which exact science can apply. For exact science invokes, or has
seemed to invoke, a type of law inevitable and soulless against
which the human spirit rebels. If science finally declares that man is
no more than a fortuitous concourse of atoms, the blow will not be
softened by the explanation that the atoms in question are the
Mendelian unit characters and not the material atoms of the chemist.
Let us then examine the kind of knowledge which is handled by
exact science. If we search the examination papers in physics and
natural philosophy for the more intelligible questions we may come
across one beginning something like this: “An elephant slides down
a grassy hillside....” The experienced candidate knows that he need
not pay much attention to this; it is only put in to give an impression
of realism. He reads on: “The mass of the elephant is two tons.” Now
we are getting down to business; the elephant fades out of the
problem and a mass of two tons takes its place. What exactly is this
two tons, the real subject-matter of the problem? It refers to some
property or condition which we vaguely describe as “ponderosity”
occurring in a particular region of the external world. But we shall not
get much further that way; the nature of the external world is
inscrutable, and we shall only plunge into a quagmire of
indescribables. Never mind what two tons refers to; what is it? How
has it actually entered in so definite a way into our experience? Two
tons is the reading of the pointer when the elephant was placed on a
weighing-machine. Let us pass on. “The slope of the hill is 60°.” Now
the hillside fades out of the problem and an angle of 60° takes its
place. What is 60°? There is no need to struggle with mystical
conceptions of direction; 60° is the reading of a plumb-line against
the divisions of a protractor. Similarly for the other data of the
problem. The softly yielding turf on which the elephant slid is
replaced by a coefficient of friction, which though perhaps not
directly a pointer reading is of kindred nature. No doubt there are
more roundabout ways used in practice for determining the weights
of elephants and the slopes of hills, but these are justified because it
is known that they give the same results as direct pointer readings.
And so we see that the poetry fades out of the problem, and by
the time the serious application of exact science begins we are left
with only pointer readings. If then only pointer readings or their
equivalents are put into the machine of scientific calculation, how
can we grind out anything but pointer readings? But that is just what
we do grind out. The question presumably was to find the time of
descent of the elephant, and the answer is a pointer reading on the
seconds’ dial of our watch.
The triumph of exact science in the foregoing problem consisted
in establishing a numerical connection between the pointer reading
of the weighing-machine in one experiment on the elephant and the
pointer reading of the watch in another experiment. And when we
examine critically other problems of physics we find that this is
typical. The whole subject-matter of exact science consists of pointer
readings and similar indications. We cannot enter here into the
definition of what are to be classed as similar indications. The
observation of approximate coincidence of the pointer with a scale-
division can generally be extended to include the observation of any
kind of coincidence—or, as it is usually expressed in the language of
the general relativity theory, an intersection of world-lines. The
essential point is that, although we seem to have very definite
conceptions of objects in the external world, those conceptions do
not enter into exact science and are not in any way confirmed by it.
Before exact science can begin to handle the problem they must be
replaced by quantities representing the results of physical
measurement.
Perhaps you will object that although only the pointer readings
enter into the actual calculation it would make nonsense of the
problem to leave out all reference to anything else. The problem
necessarily involves some kind of connecting background. It was not
the pointer reading of the weighing-machine that slid down the hill!
And yet from the point of view of exact science the thing that really
did descend the hill can only be described as a bundle of pointer
readings. (It should be remembered that the hill also has been
replaced by pointer readings, and the sliding down is no longer an
active adventure but a functional relation of space and time
measures.) The word elephant calls up a certain association of
mental impressions, but it is clear that mental impressions as such
cannot be the subject handled in the physical problem. We have, for
example, an impression of bulkiness. To this there is presumably
some direct counterpart in the external world, but that counterpart
must be of a nature beyond our apprehension, and science can
make nothing of it. Bulkiness enters into exact science by yet
another substitution; we replace it by a series of readings of a pair of
calipers. Similarly the greyish black appearance in our mental
impression is replaced in exact science by the readings of a
photometer for various wave-lengths of light. And so on until all the
characteristics of the elephant are exhausted and it has become
reduced to a schedule of measures. There is always the triple
correspondence—
(a) a mental image, which is in our minds and not in the external
world;
(b) some kind of counterpart in the external world, which is of
inscrutable nature;
(c) a set of pointer readings, which exact science can study and
connect with other pointer readings.
And so we have our schedule of pointer readings ready to make
the descent. And if you still think that this substitution has taken
away all reality from the problem, I am not sorry that you should
have a foretaste of the difficulty in store for those who hold that exact
science is all-sufficient for the description of the universe and that
there is nothing in our experience which cannot be brought within its
scope.
I should like to make it clear that the limitation of the scope of
physics to pointer readings and the like is not a philosophical craze
of my own but is essentially the current scientific doctrine. It is the
outcome of a tendency discernible far back in the last century but
only formulated comprehensively with the advent of the relativity
theory. The vocabulary of the physicist comprises a number of words
such as length, angle, velocity, force, potential, current, etc., which
we call “physical quantities”. It is now recognised as essential that
these should be defined according to the way in which we actually
recognise them when confronted with them, and not according to the
metaphysical significance which we may have anticipated for them.
In the old textbooks mass was defined as “quantity of matter”; but
when it came to an actual determination of mass, an experimental
method was prescribed which had no bearing on this definition. The
belief that the quantity determined by the accepted method of
measurement represented the quantity of matter in the object was
merely a pious opinion. At the present day there is no sense in which
the quantity of matter in a pound of lead can be said to be equal to
the quantity in a pound of sugar. Einstein’s theory makes a clean
sweep of these pious opinions, and insists that each physical
quantity should be defined as the result of certain operations of
measurement and calculation. You may if you like think of mass as
something of inscrutable nature to which the pointer reading has a
kind of relevance. But in physics at least there is nothing much to be
gained by this mystification, because it is the pointer reading itself
which is handled in exact science; and if you embed it in something
of a more transcendental nature, you have only the extra trouble of
digging it out again.
It is quite true that when we say the mass is two tons we have not
specially in mind the reading of the particular machine on which the
weighing was carried out. That is because we do not start to tackle
the problem of the elephant’s escapade ab initio as though it were
the first inquiry we had ever made into the phenomena of the
external world. The examiner would have had to be much more
explicit if he had not presumed a general acquaintance with the
elementary laws of physics, i.e. laws which permit us to deduce the
readings of other indicators from the reading of one. It is this
connectivity of pointer readings, expressed by physical laws, which
supplies the continuous background that any realistic problem
demands.
It is obviously one of the conditions of the problem that the same
elephant should be concerned in the weighing experiment and in the
tobogganing experiment. How can this identity be expressed in a
description of the world by pointer readings only? Two readings may
be equal, but it is meaningless to inquire if they are identical; if then
the elephant is a bundle of pointer readings, how can we ask
whether it is continually the identical bundle? The examiner does not
confide to us how the identity of the elephant was ensured; we have
only his personal guarantee that there was no substitution. Perhaps
the creature answered to its name on both occasions; if so the test of
identity is clearly outside the present domain of physics. The only
test lying purely in the domain of physics is that of continuity; the
elephant must be watched all the way from the scales to the hillside.
The elephant, we must remember, is a tube in the four-dimensional
world demarcated from the rest of space-time by a more or less
abrupt boundary. Using the retina of his eye as an indicator and
making frequent readings of the outline of the image, the observer
satisfied himself that he was following one continuous and isolated
world-tube from beginning to end. If his vigilance was intermittent he
took a risk of substitution, and consequently a risk of the observed
time of descent failing to agree with the time calculated.[41] Note that
we do not infer that there is any identity of the contents of the
isolated world-tube throughout its length; such identity would be
meaningless in physics. We use instead the law of conservation of
mass (either as an empirical law or deduced from the law of
gravitation) which assures us that, provided the tube is isolated, the
pointer reading on the schedule derived from the weighing-machine
type of experiment has a constant value along the tube. For the
purpose of exact science “the same object” becomes replaced by
“isolated world-tube”. The constancy of certain properties of the
elephant is not assumed as self-evident from its sameness, but is an
inference from experimental and theoretical laws relating to world-
tubes which are accepted as well established.
Limitations of Physical Knowledge. Whenever we state the

properties of a body in terms of physical quantities we are imparting
knowledge as to the response of various metrical indicators to its
presence, and nothing more. After all, knowledge of this kind is fairly
comprehensive. A knowledge of the response of all kinds of objects
—weighing-machines and other indicators—would determine
completely its relation to its environment, leaving only its inner un-
get-atable nature undetermined. In the relativity theory we accept
this as full knowledge, the nature of an object in so far as it is
ascertainable by scientific inquiry being the abstraction of its
relations to all surrounding objects. The progress of the relativity
theory has been largely due to the development of a powerful
mathematical calculus for dealing compendiously with an infinite
scheme of pointer readings, and the technical term tensor used so
largely in treatises on Einstein’s theory may be translated schedule
of pointer readings. It is part of the aesthetic appeal of the
mathematical theory of relativity that the mathematics is so closely
adapted to the physical conceptions. It is not so in all subjects. For
example, we may admire the triumph of patience of the
mathematician in predicting so closely the positions of the moon, but
aesthetically the lunar theory is atrocious; it is obvious that the moon
and the mathematician use different methods of finding the lunar
orbit. But by the use of tensors the mathematical physicist precisely
describes the nature of his subject-matter as a schedule of indicator
readings; and those accretions of images and conceptions which
have no place in physical science are automatically dismissed.
The recognition that our knowledge of the objects treated in
physics consists solely of readings of pointers and other indicators
transforms our view of the status of physical knowledge in a
fundamental way. Until recently it was taken for granted that we had
knowledge of a much more intimate kind of the entities of the
external world. Let me give an illustration which takes us to the root
of the great problem of the relations of matter and spirit. Take the
living human brain endowed with mind and thought. Thought is one
of the indisputable facts of the world. I know that I think, with a
certainty which I cannot attribute to any of my physical knowledge of
the world. More hypothetically, but on fairly plausible evidence, I am
convinced that you have minds which think. Here then is a world fact
to be investigated. The physicist brings his tools and commences
systematic exploration. All that he discovers is a collection of atoms
and electrons and fields of force arranged in space and time,
apparently similar to those found in inorganic objects. He may trace
other physical characteristics, energy, temperature, entropy. None of
these is identical with thought. He might set down thought as an
illusion—some perverse interpretation of the interplay of the physical
entities that he has found. Or if he sees the folly of calling the most
undoubted element of our experience an illusion, he will have to face
the tremendous question, How can this collection of ordinary atoms
be a thinking machine? But what knowledge have we of the nature of
atoms which renders it at all incongruous that they should constitute
a thinking object? The Victorian physicist felt that he knew just what
he was talking about when he used such terms as matter and atoms.
Atoms were tiny billiard balls, a crisp statement that was supposed to
tell you all about their nature in a way which could never be achieved
for transcendental things like consciousness, beauty or humour. But
now we realise that science has nothing to say as to the intrinsic
nature of the atom. The physical atom is, like everything else in
physics, a schedule of pointer readings. The schedule is, we agree,
attached to some unknown background. Why not then attach it to
something of spiritual nature of which a prominent characteristic is
thought. It seems rather silly to prefer to attach it to something of a
so-called “concrete” nature inconsistent with thought, and then to
wonder where the thought comes from. We have dismissed all
preconception as to the background of our pointer readings, and for
the most part we can discover nothing as to its nature. But in one
case—namely, for the pointer readings of my own brain—I have an
insight which is not limited to the evidence of the pointer readings.
That insight shows that they are attached to a background of
consciousness. Although I may expect that the background of other
pointer readings in physics is of a nature continuous with that
revealed to me in this particular case, I do not suppose that it always
has the more specialised attributes of consciousness.[42] But in
regard to my one piece of insight into the background no problem of
irreconcilability arises; I have no other knowledge of the background
with which to reconcile it.
In science we study the linkage of pointer readings with pointer
readings. The terms link together in endless cycle with the same
inscrutable nature running through the whole. There is nothing to
prevent the assemblage of atoms constituting a brain from being of
itself a thinking object in virtue of that nature which physics leaves
undetermined and undeterminable. If we must embed our schedule
of indicator readings in some kind of background, at least let us
accept the only hint we have received as to the significance of the
background—namely that it has a nature capable of manifesting
itself as mental activity.
Cyclic Method of Physics. I must explain this reference to an endless

cycle of physical terms. I will refer again to Einstein’s law of
gravitation. I have already expounded it to you more than once and I
hope you gained some idea of it from the explanation. This time I am
going to expound it in a way so complete that there is not much
likelihood that anyone will understand it. Never mind. We are not
now seeking further light on the cause of gravitation; we are
interested in seeing what would really be involved in a complete
explanation of anything physical.
Einstein’s law in its analytical form is a statement that in empty
space certain quantities called potentials obey certain lengthy
differential equations. We make a memorandum of the word
“potential” to remind us that we must later on explain what it means.
We might conceive a world in which the potentials at every moment
and every place had quite arbitrary values. The actual world is not so
unlimited, the potentials being restricted to those values which
conform to Einstein’s equations. The next question is, What are
potentials? They can be defined as quantities derived by quite
simple mathematical calculations from certain fundamental quantities
called intervals. (MEM. Explain “interval”.) If we know the values of
the various intervals throughout the world definite rules can be given
for deriving the values of the potentials. What are intervals? They are
relations between pairs of events which can be measured with a
scale or a clock or with both. (MEM. Explain “scale” and “clock”.)
Instructions can be given for the correct use of the scale and clock
so that the interval is given by a prescribed combination of their
readings. What are scales and clocks? A scale is a graduated strip
of matter which.... (MEM. Explain “matter”.) On second thoughts I will
leave the rest of the description as “an exercise to the reader” since
it would take rather a long time to enumerate all the properties and
niceties of behaviour of the material standard which a physicist
would accept as a perfect scale or a perfect clock. We pass on to the
next question, What is matter? We have dismissed the metaphysical
conception of substance. We might perhaps here describe the
atomic and electrical structure of matter, but that leads to the
microscopic aspects of the world, whereas we are here taking the
macroscopic outlook. Confining ourselves to mechanics, which is the
subject in which the law of gravitation arises, matter may be defined
as the embodiment of three related physical quantities, mass (or
energy), momentum and stress. What are “mass”, “momentum” and
“stress”? It is one of the most far-reaching achievements of
Einstein’s theory that it has given an exact answer to this question.
They are rather formidable looking expressions containing the
potentials and their first and second derivatives with respect to the
co-ordinates. What are the potentials? Why, that is just what I have
been explaining to you!
The definitions of physics proceed according to the method
immortalised in “The House that Jack built”: This is the potential, that
was derived from the interval, that was measured by the scale, that
was made from the matter, that embodied the stress, that.... But
instead of finishing with Jack, whom of course every youngster must
know without need for an introduction, we make a circuit back to the
beginning of the rhyme: ... that worried the cat, that killed the rat, that
ate the malt, that lay in the house, that was built by the priest all
shaven and shorn, that married the man.... Now we can go round
and round for ever.
But perhaps you have already cut short my explanation of
gravitation. When we reached matter you had had enough of it.
“Please do not explain any more, I happen to know what matter is.”
Very well; matter is something that Mr. X knows. Let us see how it
goes: This is the potential that was derived from the interval that was
measured by the scale that was made from the matter that Mr. X
knows. Next question, What is Mr. X?
Well, it happens that physics is not at all anxious to pursue the
question, What is Mr. X? It is not disposed to admit that its elaborate
structure of a physical universe is “The House that Mr. X built”.
Fig. 8
It looks upon Mr. X—and more particularly the part of Mr. X that
knows—as a rather troublesome tenant who at a late stage of the
world’s history has come to inhabit a structure which inorganic
Nature has by slow evolutionary progress contrived to build. And so
it turns aside from the avenue leading to Mr. X—and beyond—and
closes up its cycle leaving him out in the cold.
From its own point of view physics is entirely justified. That matter
in some indirect way comes within the purview of Mr. X’s mind is not
a fact of any utility for a theoretical scheme of physics. We cannot
embody it in a differential equation. It is ignored; and the physical
properties of matter and other entities are expressed by their
linkages in the cycle. And you can see how by the ingenious device
of the cycle physics secures for itself a self-contained domain for
study with no loose ends projecting into the unknown. All other
physical definitions have the same kind of interlocking. Electric force
is defined as something which causes motion of an electric charge;
an electric charge is something which exerts electric force. So that
an electric charge is something that exerts something that produces
motion of something that exerts something that produces ... ad
infinitum.
But I am not now writing of pure physics, and from a broader
standpoint I do not see how we can leave out Mr. X. The fact that
matter is “knowable to Mr. X” must be set down as one of the
fundamental attributes of matter. I do not say that it is very
distinctive, since other entities of physics are also knowable to him;
but the potentiality of the whole physical world for awaking
impressions in consciousness is an attribute not to be ignored when
we compare the actual world with worlds which, we fancy, might
have been created. There seems to be a prevalent disposition to
minimise the importance of this. The attitude is that “knowableness
to Mr. X” is a negligible attribute, because Mr. X is so clever that he
could know pretty much anything that there was to know. I have
already urged the contrary view—that there is a definitely selective
action of the mind; and since physics treats of what is knowable to
mind[43] its subject-matter has undergone, and indeed retains
evidences of, this process of selection.
Actuality. “Knowableness to mind” is moreover a property which

differentiates the actual world of our experience from imaginary
worlds in which the same general laws of Nature are supposed to
hold true. Consider a world—Utopia, let us say—governed by all the
laws of Nature known and unknown which govern our own world, but
containing better stars, planets, cities, animals, etc.—a world which
might exist, but it just happens that it doesn’t. How can the physicist
test that Utopia is not the actual world? We refer to a piece of matter
in it; it is not real matter but it attracts any other piece of (unreal)
matter in Utopia according to the law of gravitation. Scales and
clocks constructed of this unreal matter will measure wrong intervals,
but the physicist cannot detect that they are wrong unless he has
first shown the unreality of the matter. As soon as any element in it
has been shown to be unreal Utopia collapses; but so long as we
keep to the cycles of physics we can never find the vulnerable point,
for each element is correctly linked to the rest of the cycle, all our
laws of Nature expressed by the cycle being obeyed in Utopia by
hypothesis. The unreal stars emit unreal light which falls on unreal
retinas and ultimately reaches unreal brains. The next step takes it
outside the cycle and gives the opportunity of exposing "the whole
deception. Is the brain disturbance translated into consciousness?
That will test whether the brain is real or unreal. There is no question
about consciousness being real or not; consciousness is self-
knowing and the epithet real adds nothing to that. Of the infinite
number of worlds which are examples of what might be possible
under the laws of Nature, there is one which does something more
than fulfil those laws of Nature. This property, which is evidently not
definable with respect to any of the laws of Nature, we describe as
“actuality”—generally using the word as a kind of halo of indefinite
import. We have seen that the trend of modern physics is to reject
these indefinite attributions and to define its terms according to the
way in which we recognise the properties when confronted by them.
We recognise the actuality of a particular world because it is that
world alone with which consciousness interacts. However much the
theoretical physicist may dislike a reference to consciousness, the
experimental physicist uses freely this touchstone of actuality. He
would perhaps prefer to believe that his instruments and
observations are certified as actual by his material sense organs; but
the final guarantor is the mind that comes to know the indications of
the material organs. Each of us is armed with this touchstone of
actuality; by applying it we decide that this sorry world of ours is
actual and Utopia is a dream. As our individual consciousnesses are
different, so our touchstones are different; but fortunately they all
agree in their indication of actuality—or at any rate those which
agree are in sufficient majority to shut the others up in lunatic
asylums.
It is natural that theoretical physics in its formulation of a general
scheme of law should leave out of account actuality and the
guarantor of actuality. For it is just this omission which makes the
difference between a law of Nature and a particular sequence of
events. That which is possible (or not “too improbable”) is the
domain of natural science; that which is actual is the domain of
natural history. We need scarcely add that the contemplation in
natural science of a wider domain than the actual leads to a far
better understanding of the actual.
From a broader point of view than that of elaborating the physical
scheme of law we cannot treat the connection with mind as merely
an incident in a self-existent inorganic world. In saying that the
differentiation of the actual from the non-actual is only expressible by
reference to mind I do not mean to imply that a universe without
conscious mind would have no more status than Utopia. But its
property of actuality would be indefinable since the one approach to
a definition is cut off. The actuality of Nature is like the beauty of
Nature. We can scarcely describe the beauty of a landscape as non-
existent when there is no conscious being to witness it; but it is
through consciousness that we can attribute a meaning to it. And so
it is with the actuality of the world. If actuality means “known to mind”
then it is a purely subjective character of the world; to make it
objective we must substitute “knowable to mind”. The less stress we
lay on the accident of parts of the world being known at the present
era to particular minds, the more stress we must lay on the
potentiality of being known to mind as a fundamental objective
property of matter, giving it the status of actuality whether individual
consciousness is taking note of it or not.
In the diagram Mr. X has been linked to the cycle at a particular
point in deference to his supposed claim that he knows matter; but a
little reflection will show that the point of contact of mind with the
physical universe is not very definite. Mr. X knows a table; but the
point of contact with his mind is not in the material of the table. Light
waves are propagated from the table to the eye; chemical changes
occur in the retina; propagation of some kind occurs in the optic
nerves; atomic changes follow in the brain. Just where the final leap
into consciousness occurs is not clear. We do not know the last
stage of the message in the physical world before it became a
sensation in consciousness. This makes no difference. The physical
entities have a cyclic connection, and whatever intrinsic nature we
attribute to one of them runs as a background through the whole
cycle. It is not a question whether matter or electricity or potential is
the direct stimulus to the mind; in their physical aspects these are
equally represented as pointer readings or schedules of pointer
readings. According to our discussion of world building they are the
measures of structure arising from the comparability of certain
aspects of the basal relations—measures which by no means
exhaust the significance of those relations. I do not believe that the
activity of matter at a certain point of the brain stimulates an activity
of mind; my view is that in the activity of matter there is a metrical
description of certain aspects of the activity of mind. The activity of
the matter is our way of recognising a combination of the measures
of structure; the activity of the mind is our insight into the complex of
relations whose comparability gives the foundation of those
measures.
“What is Mr. X?” In the light of these considerations let us now see
what we can make of the question, What is Mr. X? I must undertake
the inquiry single-handed; I cannot avail myself of your collaboration
without first answering or assuming an answer to the equally difficult
question, What are you? Accordingly the whole inquiry must take
place in the domain of my own consciousness. I find there certain
data purporting to relate to this unknown X; and I can (by using
powers which respond to my volition) extend the data, i.e. I can
perform experiments on X. For example I can make a chemical
analysis. The immediate result of these experiments is the
occurrence of certain visual or olfactory sensations in my
consciousness. Clearly it is a long stride from these sensations to
any rational inference about Mr. X. For example, I learn that Mr. X
has carbon in his brain, but the immediate knowledge was of
something (not carbon) in my own mind. The reason why I, on
becoming aware of something in my mind, can proceed to assert
knowledge of something elsewhere, is because there is a systematic
scheme of inference which can be traced from the one item of
knowledge to the other. Leaving aside instinctive or commonsense
inference—the crude precursor of scientific inference—the inference
follows a linkage, which can only be described symbolically,
extending from the point in the symbolic world where I locate myself
to the point where I locate Mr. X.
One feature of this inference is that I never discover what carbon
really is. It remains a symbol. There is carbon in my own brain-mind;
but the self-knowledge of my mind does not reveal this to me. I can
only know that the symbol for carbon must be placed there by
following a route of inference through the external world similar to
that used in discovering it in Mr. X; and however closely associated
this carbon may be with my thinking powers, it is as a symbol
divorced from any thinking capacity that I learn of its existence.
Carbon is a symbol definable only in terms of the other symbols
belonging to the cyclic scheme of physics. What I have discovered is
that, in order that the symbols describing the physical world may
conform to the mathematical formulae which they are designed to
obey, it is necessary to place the symbol for carbon (amongst others)
in the locality of Mr. X. By similar means I can make an exhaustive
physical examination of Mr. X and discover the whole array of
symbols to be assigned to his locality.
Will this array of symbols give me the whole of Mr. X? There is
not the least reason to think so. The voice that comes to us over the
telephone wire is not the whole of what is at the end of the wire. The
scientific linkage is like the telephone wire; it can transmit just what it
is constructed to transmit and no more.
It will be seen that the line of communication has two aspects. It
is a chain of inference stretching from the symbols immediately
associated with the sensations in my mind to the symbols descriptive
of Mr. X; and it is a chain of stimuli in the external world starting from
Mr. X and reaching my brain. Ideally the steps of the inference
exactly reverse the steps of the physical transmission which brought
the information. (Naturally we make many short cuts in inference by
applying accumulated experience and knowledge.) Commonly we
think of it only in its second aspect as a physical transmission; but
because it is also a line of inference it is subject to limitations which
we should not necessarily expect a physical transmission to conform
to.
The system of inference employed in physical investigation
reduces to mathematical equations governing the symbols, and so
long as we adhere to this procedure we are limited to symbols of
arithmetical character appropriate to such mathematical equations.
[44] Thus there is no opportunity for acquiring by any physical
investigation a knowledge of Mr. X other than that which can be
expressed in numerical form so as to be passed through a
succession of mathematical equations.
Mathematics is the model of exact inference; and in physics we
have endeavoured to replace all cruder inference by this rigorous
type. Where we cannot complete the mathematical chain we confess
that we are wandering in the dark and are unable to assert real
knowledge. Small wonder then that physical science should have
evolved a conception of the world consisting of entities rigorously
bound to one another by mathematical equations forming a
deterministic scheme. This knowledge has all been inferred and it
was bound therefore to conform to the system of inference that was
used. The determinism of the physical laws simply reflects the
determinism of the method of inference. This soulless nature of the
scientific world need not worry those who are persuaded that the
main significances of our environment are of a more spiritual
character. Anyone who studied the method of inference employed by
the physicist could predict the general characteristics of the world
that he must necessarily find. What he could not have predicted is
the great success of the method—the submission of so large a
proportion of natural phenomena to be brought into the prejudged
scheme. But making all allowance for future progress in developing
the scheme, it seems to be flying in the face of obvious facts to
pretend that it is all comprehensive. Mr. X is one of the recalcitrants.
When sound-waves impinge on his ear he moves, not in accordance
with a mathematical equation involving the physical measure
numbers of the waves, but in accordance with the meaning that
those sound-waves are used to convey. To know what there is about
Mr. X which makes him behave in this strange way, we must look not
to a physical system of inference, but to that insight beneath the
symbols which in our own minds we possess. It is by this insight that
we can finally reach an answer to our question, What is Mr. X?
[41] A good illustration of such substitution is afforded by
astronomical observations of a certain double star with two
components of equal brightness. After an intermission of
observation the two components were inadvertently interchanged,
and the substitution was not detected until the increasing
discrepancy between the actual and predicted orbits was inquired
into.
[42] For example, we should most of us assume (hypothetically)
that the dynamical quality of the world referred to in chapter V is
characteristic of the whole background. Apparently it is not to be
found in the pointer readings, and our only insight into it is in the
feeling of “becoming” in our consciousness. “Becoming” like
“reasoning” is known to us only through its occurrence in our own
minds; but whereas it would be absurd to suppose that the latter
extends to inorganic aggregations of atoms, the former may be
(and commonly is) extended to the inorganic world, so that it is
not a matter of indifference whether the progress of the inorganic
world is viewed from past to future or from future to past.
[43] This is obviously true of all experimental physics, and must
be true of theoretical physics if it is (as it professes to be) based
on experiment.
[44] The solitary exception is, I believe, Dirac’s generalisation
which introduces -numbers (p. 210). There is as yet no approach
to a general system of inference on a non-numerical basis.
Chapter XIII
REALITY
The Real and the Concrete. One of our ancestors, taking arboreal
exercise in the forest, failed to reach the bough intended and his
hand closed on nothingness. The accident might well occasion
philosophical reflections on the distinctions of substance and void—
to say nothing of the phenomenon of gravity. However that may be,
his descendants down to this day have come to be endowed with an
immense respect for substance arising we know not how or why. So
far as familiar experience is concerned, substance occupies the
centre of the stage, rigged out with the attributes of form, colour,
hardness, etc., which appeal to our several senses. Behind it is a
subordinate background of space and time permeated by forces and
unconcrete agencies to minister to the star performer.
Our conception of substance is only vivid so long as we do not
face it. It begins to fade when we analyse it. We may dismiss many
of its supposed attributes which are evidently projections of our
sense-impressions outwards into the external world. Thus the colour
which is so vivid to us is in our minds and cannot be embodied in a
legitimate conception of the substantial object itself. But in any case
colour is no part of the essential nature of substance. Its supposed
nature is that which we try to call to mind by the word “concrete”,
which is perhaps an outward projection of our sense of touch. When
I try to abstract from the bough everything but its substance or
concreteness and concentrate on an effort to apprehend this, all
ideas elude me; but the effort brings with it an instinctive tightening
of the fingers—from which perhaps I might infer that my conception
of substance is not very different from my arboreal ancestor’s.
So strongly has substance held the place of leading actor on the
stage of experience that in common usage concrete and real are
almost synonymous. Ask any man who is not a philosopher or a
mystic to name something typically real; he is almost sure to choose
a concrete thing. Put the question to him whether Time is real; he will
probably decide with some hesitation that it must be classed as real,
but he has an inner feeling that the question is in some way
inappropriate and that he is being cross-examined unfairly.
In the scientific world the conception of substance is wholly
lacking, and that which most nearly replaces it, viz. electric charge, is
not exalted as star-performer above the other entities of physics. For
this reason the scientific world often shocks us by its appearance of
unreality. It offers nothing to satisfy our demand for the concrete.
How should it, when we cannot formulate that demand? I tried to
formulate it; but nothing resulted save a tightening of the fingers.
Science does not overlook the provision for tactual and muscular
sensation. In leading us away from the concrete, science is
reminding us that our contact with the real is more varied than was
apparent to the ape-mind, to whom the bough which supported him
typified the beginning and end of reality.
It is not solely the scientific world that will now occupy our
attention. In accordance with the last chapter we are taking a larger
view in which the cyclical schemes of physics are embraced with
much besides. But before venturing on this more risky ground I have
to emphasise one conclusion which is definitely scientific. The
modern scientific theories have broken away from the common
standpoint which identifies the real with the concrete. I think we
might go so far as to say that time is more typical of physical reality
than matter, because it is freer from those metaphysical associations
which physics disallows. It would not be fair, being given an inch, to
take an ell, and say that having gone so far physics may as well
admit at once that reality is spiritual. We must go more warily. But in
approaching such questions we are no longer tempted to take up the
attitude that everything which lacks concreteness is thereby self-
condemned.
The cleavage between the scientific and the extra-scientific
domain of experience is, I believe, not a cleavage between the
concrete and the transcendental but between the metrical and the

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2 Ferroelectric charge-transfer complexes 7

3 Hydrogen-bonded organic molecular ferroelectrics/

4 Synthesis of polyvinylidene fluoride and its copolymers 85

4.3 Homopolymerization of PVDF 86

5 Ferroelectric polymer blends for optoelectronic applications 113

7 Switching dynamics in organic ferroelectrics 185

7.6 First-principle theory 217

8 Piezoresponse force microscopy for functional imaging of organic

9 Dielectric spectroscopy of ferroelectric polymers 263

10 Liquid structuring in fluoropolymer solutions induced by

11 Solution processing of piezoelectric unconventional structures 375

11.3 Final remarks and future trends 419

12 Polarization of ferroelectric polymers through electrolytes 441

13 Piezoelectric composites 457

14 Ferroelectric polymer composites for capacitive energy storage 477

15 Ferroelectric polymers for energy harvesting 503

16 Electrocaloric effects in ferroelectric polymers 535

16.3 Electrocaloric effect in ferroelectric polymer-based

17 Biomimetic biocompatible ferroelectric polymer materials with an

Aldo Altomare Macromolecular Chemistry and New Polymeric Materials, Zernike

Kamal Asadi Department of Physics, University of Bath, Bath, United Kingdom

Insung Bae Department of Advanced Materials, Hannam University, Daejeon, Korea

Magnus Berggren Laboratory of Organic Electronics, Department of Science and

Maryam Bozorg Macromolecular Chemistry and New Polymeric Materials, Zernike

V.F. Cardoso CF-UM-UP, Centre of Physics, University of Minho, Braga;

E.O. Carvalho CF-UM-UP, Centre of Physics; CEB, University of Minho, Braga,

Tim Cornelissen Department of Physics, Chemistry and Biology (IFM), Link€oping

D.M. Correia CF-UM-UP, Centre of Physics, University of Minho, Braga; Centre of

C.M. Costa CF-UM-UP, Centre of Physics; Centre of Chemistry, University of

Simone Fabiano Laboratory of Organic Electronics, Department of Science and

Zhubing Han Department of Materials Science and Engineering, The Pennsylvania

Wen He School of Materials Science and Engineering, National Institute for

Sachio Horiuchi Research Institute for Advanced Electronics and Photonics

Shoji Ishibashi Research Center for Computational Design of Advanced Functional

Martijn Kemerink Department of Physics, Chemistry and Biology (IFM), Link€oping

Jibran Khaliq Department of Mechanical and Construction Engineering,

Hamideh Khanbareh Department of Mechanical Engineering, University of Bath,

Valentin V. Kochervinskii Karpov Institute of Physical Chemistry, Moscow, Russia

S. Lanceros-Mendez CF-UM-UP, Centre of Physics, University of Minho, Braga,

Katja Loos Macromolecular Chemistry and New Polymeric Materials, Zernike

Rujun Ma School of Materials Science and Engineering, National Institute for

Inna A. Malyshkina Faculty of Physics, M.V. Lomonosov Moscow State University,

T. Marques-Almeida CF-UM-UP, Centre of Physics; CEB, University of Minho,

P.M. Martins CF-UM-UP, Centre of Physics; IB-S; CBMA, University of Minho,

R.M. Meira CF-UM-UP, Centre of Physics; CEB, University of Minho, Braga,

Cheolmin Park Department of Materials Science and Engineering, Yonsei

N. Perinka BCMaterials, University of the Basque Country UPV/EHU Science Park,

Aatif Rasheed Department of Mechanical and Construction Engineering,

T. Rodrigues-Marinho CF-UM-UP, Centre of Physics, University of Minho, Braga,

Hamed Sharifi-Dehsari Max Planck Institute for Polymer Research, Mainz,

Qing Wang Department of Materials Science and Engineering, The Pennsylvania