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Rheology
Concept, Methods, and Applications
3rd Edition
Toronto 2017
Published by ChemTec Publishing
38 Earswick Drive, Toronto, Ontario M1E 1C6, Canada
Table of Contents
Preface xi
Preface to the 2nd Edition xiii
Preface to the 3rd Edition xiv
1 Introduction. Rheology: Subject and Goals 1
1 Continuum Mechanics as a Foundation of Rheology 9
1.1 Stresses 9
1.1.1 General theory 9
1.1.2 Law of equality of conjugated stresses 12
1.1.3 Principal stresses 12
1.1.4 Invariants of a stress tensor 14
1.1.5 Hydrostatic pressure - spherical tensor and deviator 16
1.1.6 Equilibrium (balance) equations 19
1.2 Deformations 21
1.2.1 Deformations and displacements 21
1.2.1.1 Deformations 21
1.2.1.2 Displacements 24
1.2.2 Infinitesimal deformations: principal values and invariants 26
1.2.3 Large (finite) deformations 27
1.2.4 Special cases of deformations − uniaxial elongation and simple shear 30
1.2.4.1 Uniaxial elongation and Poisson’s ratio 30
1.2.4.2 Simple shear and pure shear 31
1.3 Kinematics of deformations 34
1.3.1 Rates of deformation and vorticity 34
1.3.2 Deformation rates when deformations are large 35
1.4 Heterogeneity on flow 36
1.4.1 Particle distribution in disperse systems 37
1.4.2 Phase separation 38
1.4.3 Flow of the large-scale structure elements 38
1.5 Summary − continuum mechanics in rheology 39
1.5.1 General principles 39
1.5.2 Objects of continuum as tensors 40
2 Viscoelasticity 45
2.1 Basic experiments 45
2.1.1 Creep (retarded deformation) 45
2.1.2 Relaxation 46
2.1.3 Fading memory 48
2.2 Relaxation and creep − spectral representation. Dynamic functions 49
2.2.1 Retardation and relaxation spectra − definitions 49
2.2.2 Dynamic functions 52
iv Table of Contents
A number of books, devoted to different aspects of both theoretical and applied rheology,
were published in the last 20 years. The keyword in the last sentence is “different aspects”.
Rheology has a unique structure with its own language, fundamental principles, original
concepts, rigorous experimental methods, and a set of well-documented observations with
inherent interrelations between various branches of natural science and numerous practical
applications.
By examining the enormous volume of rheological literature and meeting various
people interested in rheology (university teachers, students, applied scientist, and engi-
neers), the authors felt the need for a systematic presentation of the subject matter in one
book − a book that includes all components of rheology and presents them as an indepen-
dent branch of natural science.
However, it became obvious from the early planning stages that some information
would need to be omitted to provide a clear presentation of the concepts, methods, and
applications which constitute the essence of efforts that created this science. The wish to
present all aspects of rheology will inevitably lead to a book of enormous size. Every
attempt to write a scientific book is personal and objective; objective because science ben-
efits from objective assessments and personal because our experiences make us feel that
certain aspects are more important than others. In our case, we are university teachers and
researchers primarily in the field of applied rheology. An attentive reader will most likely
find some reflections of our personal preferences.
Considering the goals and the tasks of the book, the authors tried to limit the choice
of references to the first publications on a particular subject, also including reviews and
papers providing the most expressive examples and illustrations of the topics under dis-
cussion. Accordingly, a great number of original publications are not mentioned. It is
regrettable because any serious publication is worth mentioning.
The authors hope that the readers of the book will benefit from our presentation of
rheology as an interrelated system of concepts, principal phenomena, experimental meth-
ods, and directions of their application. Our rheology is also a science interwoven with
other branches of theoretical and applied sciences. We take many opportunities to empha-
size these links because they enrich science, make it easier to understand and apply, and
this also helps to fulfil our goals concisely expressed in the book title. To amplify its use-
fulness as a teaching tool, all chapters of the book contain questions to be used by readers
to assess their knowledge of particular subject. Answers to these questions are included as
the last part of the book.
Finally, the authors are glad to fulfil their pleasing duty to thank Dr. Andrei Andri-
anov (Moscow State University) for his technical assistance in preparing the computer
xii Preface
versions of many figures and realizing the liaison between the authors. The authors are
also grateful to Dr. Sayata Ghose for painstaking proofreading and making corrections for
this book.
Special gratitude goes to Professor J.L. White who read the manuscript of the book
and made many valuable comments, which helped to enrich the presented text.
We express our deep gratitude to publishers of various journals (Advances in Poly-
mer Science, Colloid Journal, European Polymer Journal, International Journal of Poly-
meric Materials, Journal of Applied Polymer Science, Journal of Macromolecular
Science, Journal of Non-Newtonian Fluid Mechanics, Journal of Polymer Science, Journal
of Rheology, Macromolecular Chemie, Polymer, Polymer Engineering and Science, Poly-
mer Science USSR, Reviews of Scientific Instruments, Rheologica Acta) and books (Rhe-
ology of Elastomers by P. Mason and N. Wookey (eds), A Practical Approach to Rheology
and Rheometry by G. Schramm for permission to use figures from their publications.
In preparing the Second Edition of this book, the general structure of the book is main-
tained and some necessary corrections and additions are made. The most important recent
results published in periodicals till the middle of 2011 are added. In particular, Section
2.8.1 of Chapter 2, Section 3.5.2 of Chapter 3 and Subsection 5.8.1.2 of Chapter 5 are
modified. A new Subsection 5.6.2.6 on Capillary breakup in elongational rheometry is
added. Furthermore, Section 3.2.3 on Viscosity of anisotropic liquids and Section 3.6.3 on
Instabilities in flow of elastic fluids of Chapter 3 are completely rewritten. Many other
modifications in the text are made and some new figures are added. Also, all the detected
misprints and errors found by ourselves or pointed out by colleagues are corrected.
After publication of the First Edition of the book, a lot of comments and advice from
our friends and colleagues were received. We are very grateful to all of them for construc-
tive criticism and valuable comments.
We are also grateful to our Editor, Dr. G. Wypych, for his hard work in improving the
manuscript and making it ready for publication.
August 2011
xiv
In the 3rd edition of the book, we updated the material paying special attention to the
issues which have become the hot spots of rheology during last decade. These are such
topics as the rheology of polymeric materials containing fillers, the concept of heterogene-
ity of the flow including the effect of shear-banding, and new ideas in understanding the
visco-plastic media. We have added references to the mosty up-to-date publications in
these fields.
We are grateful to readers who were kind to bring to our attention some misprints
and not quite clear explanations used in the former editions. Necessary corrections have
been implemented.
We hope that this book is continued to be used by students and young researchers
who only start their career in the intriguing world of the rheology of real materials sur-
rounding us in our life.
December 2016
Introduction.
Rheology: Subject and Goals
Rheology, as an independent branch of natural sciences, emerged more than 70 years ago.
It originated from observations of “strange” or abnormal behavior of many well-known
materials and difficulties in answering some “simple” questions. For example:
• paints are evidently liquids because they can be poured into containers, but why
do they remain on vertical walls without sagging down, unlike many other liq-
uids?
• clays look solid but they can be molded into a shape; they may occupy vessels
the way any liquid does; why do clays behave like many liquids?
• yogurt does not flow out of a container (it has high viscosity), but after intensive
mixing its viscosity decreases, and then increases again when left to rest, so
which value of viscosity should be considered?
• concrete mix appears to be solid and rigid, but when subjected to an external
force it changes its shape similar to liquids; what are the reasons for such behav-
ior?
• parts made out of polymeric materials (plastics) look solid and hard, similar to
parts made out of metal, but they are noticeably different: when force is applied
to a metallic part it slightly changes its shape and maintains its new shape for a
long time; this is not the case with plastics which also change their shape after
force is applied but they continue to change shape; if this material is solid, why
does it “creep”?
• pharmaceutical pastes (for example, toothpaste or body lotion) must be “liquids”
when applied and they should immediately become “solids” to remain on skin;
are they liquids or solids?
• sealants widely used in construction must be fluid-like to seal all spaces and to
fill cavities, but then sealant must rapidly “solidify” to prevent sagging; is sealant
liquid or solid?
• metals are definitely solids, but how is it possible to change their initial form by
punching and stamping as if metal was liquid?
These are just few examples. It is common for them that they represent properties of
many real materials and that they exhibit a mixture of liquid-like and solid-like properties.
This shows that commonly used words “liquid” and “solid” are insufficient to describe
their properties, and new concepts are need to understand properties of many real materi-
als. A new terminology emerges from discoveries and description of new features of mate-
2 Introduction. Rheology: Subject and Goals
rials. New methods are needed to characterize and measure their properties. New fields of
application can be expected from the application of new concepts and the results of stud-
ies. All these are the essence of rheology.
Superposition of liquid-like and solid-like features in behavior of technological
materials is directly regarded as the consequence of time effects, i.e., the results of obser-
vations depend on a time scale. Possibly, this is the most common feature of the materials,
which were listed above. Time by itself has no meaning, but time is a reflection of changes
in material structure taking place during the period of observation (or experiment).
The main method of rheology consists of constructing models, which are useful in
qualitative or (better) quantitative description of experimental results of mechanical
behavior of different materials. Any natural science pretends to deal with reality and does
so by means of phenomenological models. Any model is created not to reflect all, but the
most important, characteristic features of an object. The concepts of liquids and solids are
also models and their formal (mathematical) representation originated from the classical
works by Isaac Newton and Robert Hooke.
Newton (1687) reflected upon a resistance of liquids to a cylinder rotating in a ves-
sel. His ideas were converted to a more accurate form by Stokes, who formulated a general
law of liquid-like behavior, known as the Newton-Stokes law. According to this concept,
the deformation rate is expected to be proportional to stress and the constant coefficient of
proportionality is called viscosity, which is a material parameter of liquid. This law
assumes that, in flow of liquids, a force (or resistance to flow) is proportional to a velocity
(of movement).
Hooke (1676) formulated a similar proposal concerning properties of solids. The
law, named after him, was translated to modern form by Bernoulli and then by Euler.
Hooke’s law states that in deformation of solids, stress is proportional to deformation. The
coefficient of proportionality is called Young’s modulus.
Both models represent properties of many real materials and work well in describing
their behavior with a considerably high degree of accuracy. However, there are many other
materials which are not described by the Newton-Stokes and the Hooke laws. Rheology
relies on the concept that non-Newtonian and non-Hookean materials exist in reality.
These materials are interesting from both theoretical and applied aspects, and that is why
such materials must be the objects of investigation.
It is important to emphasize that every model describes properties of real materials
with a different degree of approximation. The Newton-Stokes and Hooke laws are not
exceptions, and more strict and complex laws and equations give much better approxima-
tion of reality than the classical Newton-Stokes and Hooke laws known from school years.
Both basic phenomenological (i.e., taken as probable assumptions, but only assump-
tions) relationships (the Newton-Stokes and Hooke laws) do not include inherent structure
of matter. Because matter consists of molecules and intermolecular empty spaces, every
material is heterogeneous. At the same time, an observer sees a body as a homogeneous
continuous mass without holes and empty spaces. The obvious way out of these contradic-
tory evidences lies in the idea of the space scale of observation. This scale can be small
enough to distinguish individual molecules or their parts. Then, molecules can be com-
bined in regular arrangements, such as crystals, and then crystals can be organized in
super-crystalline (or super-molecular) arrangements. All this leads to the concept of mate-
14 Continuum Mechanics as a Foundation of Rheology
and principal stresses, denoted as σ1, σ2, and σ3 appear to be the three roots of this equa-
tion. These roots are evidently expressed through coefficients of Eq. 1.1.7 − I1, I2, and I3.
These coefficients are constructed by means of all components of a stress tensor for arbi-
trary orthogonal orientations in space as:
I 1 = σ 11 + σ 22 + σ 33 [1.1.7a]
2 2 2
I 2 = σ 11 σ 22 + σ 11 σ 33 + σ 22 σ 33 – ( σ 12 + σ 13 + σ 23 ) [1.1.8a]
2 2 2
I 3 = σ 11 σ 22 σ 33 + 2σ 12 σ 13 σ 23 – ( σ 11 σ 23 + σ 22 σ 13 + σ 33 σ 12 ) [1.1.9a]
The principal stresses σ1, σ2, and σ3 do not depend on orientation of axes of a unit
cube (at a point) in space but they are expressed by values of I1, I2, and I3. This leads to the
conclusion that I1, I2, and I3 are also invariant with respect to the choice of directions of
orientation and that is why they are usually called invariants of a stress tensor at a point.
According to its structure (the power of the components), I1 is the first (linear), I2 is the
second (quadratic), and I3 is the third (cubic) invariant. The invariants can also be
expressed via the principal stresses only. These formulas are easily written based on Eqs.
1.1.7a -1.1.9a.
I1 = σ1 + σ2 + σ3 [1.1.7b]
I2 = σ1 σ2 + σ1 σ3 + σ2 σ3 [1.1.8b]
I3 = σ1 σ2 σ3 [1.1.9b]
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a prayer but chiefly ecstatic description of his power, the worshipper
is really endeavouring to charge himself with higher religious magic
by this outpouring. In fact, here and elsewhere, a magic origin for the
practice of theologic exegesis may be obscurely traced; narrative
might acquire an apotropaeic effect; thus tablets containing the
narrative of the achievements of the plague-god, hung up before the
houses, could avert pestilence,296.2 or, again, the reading aloud the
tablet narrating the victory of Shamash and Ramman over the seven
demons who attacked the moon-god Sin served to defeat the seven
demons by the same sympathetic magic as would be worked by a
dramatic representation of that event.296.3
There is no record or hint that the Hellenes recited hymns to
Demeter or wrote up passages of Homer to avert demons.
It belongs to the magic use of formulae that minute exactness in
respect of every syllable is necessary to the power of the spell or the
spell-prayer. An Assyrian king who is consulting the sun-god
concerning success in a war with which he is threatened, prays that
the ritual which the enemy may be employing may go wrong and fail;
and in this context occurs the curious petition, “May the lips of the
priest’s son hurry and stumble over a word.”297.1 The idea seems to
be that a single slip in the ritual-formulae destroyed their whole
value; and such a view belongs to magic rather than to religion.
Now it is probable that in his earliest mental stage the Hellene had
been in bondage to the religious magic of sacred formulae and
sacred names; and as a tradition of that stage, the divine epithet
whereby he appealed to his deities according to his needs retained
always for him a mysterious potency; but otherwise we have no
proof that he worked word-magic by means of his sacred texts.
Babylonian sorcery, whether legitimate or illegitimate, was
intended to work upon or through demons; and its familiarity with the
names and special qualities of demons is its peculiar mark. In the
ritual of exorcism of the demons, idols play a prominent and often
singular rôle. The following performance is probably unique: in the
exorcism of disease two idols, male and female, were set up before
the sick man, then the evil spirits of sickness are invited thus: “Oh ye
all wicked, all evil, who pursue so-and-so, if thou art male, here is thy
wife; if thou art female, here is thy husband.”297.2 The intent of the
exorciser seems to be to attract the demon of disease, of whose sex
he is not sure, into one or the other of these images, and he lures it
by amorous enticement into the figure of opposite sex to its own;
having got the demon into the image, he doubtless takes it out and
burns or buries it. Or the evil spirit may be attracted from the patient
by means of its own image placed near him. One document
prescribes various images of bestial form, all of which are to be
taken by night to the bank of the river, probably that they may be
thrown in and carry the impurity of sickness away.298.1 Another
shows us how to deal with Labartu, the daughter of Anu;298.2 her
image, made of clay, is placed above the head of the sick man, so as
to draw her or her power out from him; it is then taken out, slain, and
buried. And this exorcism is all the more notable because Labartu is
rather an evil goddess than a mere demon, being styled in another
text “August lady,” “Mistress of the dark-haired men.”298.3 Such
magical drama, in which the demon-image might be slain to annul its
potency, seems characteristically Babylonian: it entered also into the
ritual of the high gods. For, at the feast of the New Year, when Nebo
arrived from Borsippa, two images are brought before him and in his
presence decapitated with the sword. Dr. Langdon interprets
them298.4 as representing probably “the demons who aided the
dragon in her fight with Marduk; they are the captive gods of
darkness which ends with the Equinox.” This is dramatic magic
helpful to the gods.
The elaboration of exorcism must have led to a minuter articulation
of the demon-world; the exorciser is most anxious to know and
discover all about his unseen foes: he gives them a name, a sex if
possible, and a number: he says of the powerful storm-demons Utuk
“they are seven, they are seven, they are neither male nor female,
they take no wife and beget no children;”299.1 for knowledge of the
name or nature of the personality gives magic power.
Many of these examples, which might easily be multiplied, show
us magic applied to private but beneficent purposes, the healing of
disease, the exorcism of spirits of moral and physical evil. It was also
in vogue for national purposes—for instance, for the destruction of
the enemies of the king; one of our documents describes such a
process as the making of a tallow-image of the enemy of the king
and binding his face with a cord, so as to render the living foe
impotent of will and speech.299.2
We have already noticed that the Babylonian gods themselves
work magic, and that it was also worked on behalf of the gods.299.3
And in the ritual-records much that might be interpreted as religion
may find its truer account from the other point of view; for instance,
the ritual of placing by the bedside of a sick man the image of Nergal
or those of the “twins who overthrow the wicked Gallu”299.4 might
appear at first sight as a religious appeal to the deities to come to his
aid; but as in form it is exactly similar to the use made on the same
occasion, as noted above, of the images of demons, we may rather
suppose that the intention was magical in this act also, and that the
divine idols were supposed to combat the demon of sickness by their
magical influence. Or, again, in part of the ritual of exorcism we find
acts that bear the semblance of sacrifice, such as throwing onions
and dates into the fire; but they were charged with a curse before
thrown, and the act is more naturally interpreted as a magic
transference of evil.300.1
For the purpose of the exorcism, to deliver a “banned” person, the
high god, Marduk or another, might be called in; but Marduk also
works the effect by magic: a rope is woven by Ishtar’s maidens,
which Marduk (or his priest) turns round the head of the sufferer,
then breaks it through and throws it out into the desert.300.2 This
looks like symbolic magic; the knotted rope represents the ban,
which is then broken and thrown away.
There are many features in these methods of exorcism, such as
the apotropaeic use of idols, that are common to other peoples at a
certain stage of culture; there remains much also that seems
peculiar to Babylon.
But what is uniquely characteristic of this Mesopotamian people,
and at the same time most un-Hellenic, is the all-pervading
atmosphere of magic, which colours their view of life and their theory
of the visible and invisible world. Babylonia, at least, was the one
salient exception to the historic induction that a distinguished
writer300.3 has recently sanctioned—“religion once firmly established
invariably seeks to exclude magic; and the priest does his best to
discredit the magician.” The psalmody of Babylon, with its occasional
outbursts of inspiration and its gleams of spiritual insight, would have
appealed to an Isaiah; its magic would have appealed to many a
modern African. The Babylonian prophet does not frown on it; the
high gods accept it, the priest is its skilled and beneficent
practitioner. And at no other point, perhaps, is the contrast between
the Hellenic and the Mesopotamian religions so glaring as at this.
This comparison of Eastern and Western ritual may close with
some observations on another religious function that may be of
some value for the question of early ethnic influence.
It has been remarked that divination played an important, perhaps
a dominant part in the Babylonian ritual of sacrifice, divination, that
is, by inspection of the victim’s entrails, especially the liver; and that
this method was adopted in Greece only in the later centuries.301.1
But there are other salient differences between the Babylonian and
the more ancient mantic art of Hellas.301.2 Another method much in
vogue in the former was a curious mode of divining by mixing oil and
water and watching the movements and behaviour of the two
liquids.301.3 The first and only indication of a similar practice in Hellas
is a passage in the Agamemnon of Æschylus, of which the true
meaning has hitherto escaped the interpreters.301.4 And here, as
usual, an obvious example of Mesopotamian influence on Hellenic
custom belongs only to a late epoch. It is also true that the ancient
divination of the two peoples agreed in certain respects, namely, in
that both used, like most communities at a certain stage of culture,
the auguries of birds and the revelations of dreams. As regards the
facts relating to the former, we know more about Greece than at
present about Babylon. But in the matter of dream-oracles, it is
manifest that the Hellenic phenomena are entirely independent of
Mesopotamian fashion. The Assyrian and Babylonian documents
reveal the fashion of dream-prophecy in its simplest and highest
form: the high deity of his own pleasure sends a dream, and the
divining priest or skilled interpreter interprets it. No hint has so far
been detected of that artificial method of provoking prophetic dreams
by “incubation” or ἐγκοίμησις, the fashion of laying oneself down in
some sacred shrine and sleeping with one’s ear to the ground, that
was much in vogue in ancient Hellas and still survives in parts of the
modern Greek world and which may be regarded as an immemorial
tradition. In this divination, the divine spokesman was the power of
the underworld. And this was the most important difference between
the Western and the Eastern society in respect of the divine agency.
In an early period of Hellenic history that may be called pre-Apolline,
the earth-mother was conspicuously oracular by the vehicle of
dreams; and this power of hers was generally shared by the nether
god and buried heroes. Nor could the religion of Apollo suppress this
“chthonian” divination. But in Mesopotamia the earth-powers and the
nether world have no part or lot in this matter. It is almost the
prerogative of Shamash, the sun-god, though Adad is sometimes
associated with him;302.1 both being designated as “Bēlē-Biri” or
“Lords of Oracles.”303.1
Another remarkable distinction is the fact that the ecstatic or
enthusiastic form of prophecy, that of the Shaman or Pythoness
possessed and maddened by the inworking spirit of god, is not found
in the Babylonian record, which only attests the cool and scientific
method of interpreting by signs and dreams and the stars. Perhaps
Mesopotamia from the third millennium onward was too civilised to
admit the mad prophet and prophetess to its counsels. But such
characters were attached to certain Anatolian cults, especially to
those of Kybele,303.2 and also to the Syrian goddess at
Hierapolis;303.3 we have evidence of them also in a record of the
Cretan Phaistos in the service of the Great Mother.303.4 Some
scholars have supposed that prophetic ecstasy was only a late
phenomenon in Hellas, because Homer is silent about it. But there
are reasons for suspecting that demoniac possession was
occasionally found in the pre-Homeric divination of Hellas,303.5 an
inheritance perhaps from the pre-Hellenic period.
In any case, the theory that primitive Hellas was indebted to
Babylonia for its divination-system is strongly repugnant to the facts.
CHAPTER XIV.
Summary of Results.
CHAPTER I NOTES
11.1 I am aware that there are exceptions to this principle, which I
propose to consider in a future course; no single formula can ever
sum up all the phenomena of a complex religion.
14.1 Vide Langdon, in Transactions of Congress of the History of
Religions, 1908, vol. i. p. 251.
15.1 P. 382, C.
15.2 Vide Petrie, in Transactions of Congress of the History of
Religions, 1908, vol. i. p. 192.
17.1 Archiv für Religionswissenschaft, 1904.
17.2 Vide Jastrow, Religion Babyloniens u. Assyriens, vol. i. p. 545.
20.1 Vide my Evolution of Religion, pp. 139-152.
21.1 1. 132.
25.1 Transactions of Congress of History of Religions, 1908, vol. i.
p. 192.
25.2 Hibbert Journal, 1904, “Sacrificial Communion in Greek
Religion.”
CHAPTER II NOTES
31.1 Vide the critical remarks on such a view by Prof. Jastrow in
Transactions of the Third International Congress of the History of
Religions, vol. i. pp. 234-237.
34.1 Vide Annual of the British School, 1909, 1910.
35.1 Vide Zimmern, Die Keilinschriften und das alte Testament