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CHEMISTRY OF FUNCTIONAL MATERIALS
SURFACES AND INTERFACES
CHEMISTRY OF
FUNCTIONAL
MATERIALS
SURFACES AND
INTERFACES
Fundamentals and Applications

ANDREI HONCIUC
Elsevier
Radarweg 29, PO Box 211, 1000 AE Amsterdam, Netherlands
The Boulevard, Langford Lane, Kidlington, Oxford OX5 1GB, United Kingdom
50 Hampshire Street, 5th Floor, Cambridge, MA 02139, United States
Copyright © 2021 Elsevier Inc. All rights reserved.
No part of this publication may be reproduced or transmitted in any form or by any means, electronic or
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(other than as may be noted herein).

Notices
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understanding, changes in research methods, professional practices, or medical treatment may become
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 Preface

In these times it is undeniable that most industries deal even less so acquire a relevant practical experience. Nav-
increasingly more often than ever with surface and inter- igating through the maze of scientific literature and infor-
facial phenomena. Chemists, physicists, and material sci- mation hard to decipher can be extremely intimidating
entists, with background and training in materials, for the future chemists. The same is true in industry;
surfaces, and interfaces are in great demand. From my working in industry one realizes that time is of the
experience in both industry and academia, I have essence. Chemists and laboratory technicians are
observed that students attending courses of a general expected by the company to be innovative and thrive
chemistry degree program encounter rather late in their in interdisciplinary fields, learn on the go, and become
curriculum courses dealing with interfacial phenomena experts in the shortest amount of time, on the job. There-
and chemistry of interfaces. Some curricula have fore, I feel that this book would be useful as a textbook for
included the chemistry of interfaces under different for- students, chemists working in industry, and laboratory
mats, at the undergraduate level, some only at master’s technicians first encountering the chemistry of interfaces,
level, in specialized modules. This can in part be interfacial phenomena, colloids, nanotechnology, poly-
explained by the fact that Chemistry has become an enor- mer nanoparticle synthesis, etc. I have used myself part
mously vast array of scientific domains, branching into of this material in my teachings both in academia and
biochemistry, organic chemistry, physical chemistry, training of technicians from industry. While this material
catalysis, industrial chemistry, inorganic chemistry, ana- used as a coursework material at master’s level has ini-
lytical chemistry, materials chemistry, nanotechnology, tially included much more theory and formula, I could
polymer chemistry, petroleum chemistry, etc. Due to feel the students had difficulties grasping these, due to
fecund research in the past two decades Chemistry of the pressure, lack of time, and an extremely burdening
functional materials and interfaces covers a multitude curriculum. I thus preferred to make the hard choice of
of intertwined interdisciplinary subjects from the nano- reducing the material only to essential theories and adopt
scale, such as synthesis of polymeric and inorganic nano- a more descriptive and intuitive presentation. One of the
particles, to macroscopic phenomena such as leitmotifs of the book is the emphasis on practical appli-
manufacturing of functional surfaces, food, and con- cations of such theories. After several years in refining
sumer products such as cosmetics, detergents, heteroge- this material I believe it came to a format well received
neous catalysts, etc. The amplitude and the amount of by the students. In addition, to make it more useful for
information in each of these fields put pressure on stu- chemists performing interfacial experiments, in industry
dents, more so than several decades ago; it is now harder or academia, I have tried to add experimental details or
for the students to keep track of the newest advances, hints on data interpretation from my own experience.

vii
 C H A P T E R

1
Introduction

Interfaces are the boundaries separating two phases and define all objects in the three-dimensional world. Depend-
ing on the strength of cohesion forces and binding energies between atoms and molecules, the phases can be gases,
liquids, and solids, defining the physical states of matter. When the cohesion energies between the constituting atoms
and molecules are stronger than randomizing effects of the thermal energy, the physical state changes from gas to a
condensed phase of matter, liquid, or solid. The Boltzmann distribution gives the probability P that a system will be in
a certain state as a function of the state’s energy and temperature:
P
eE=kT
kT factor is often used as a scale energy factor in the molecular interactions. The cohesive energies per atom or molecule
at 298 K can vary from several kT between gas atoms, between
9 and
23 kT in liquid Hg (the liquid with the strongest
cohesive energy, 57.9 kJ/mol [1]), and >50 kT in solids up to 342 kT in W (1 kT  4.05  1021 J), the metal with the high-
est melting point. The kT energy scale factor is introduced and discussed in detail in Chapter 2. Because the most
important interactions between material interfaces take place in the liquid, or between material interfaces and liquids,
the solid-liquid, liquid-liquid, and liquid-air interfaces deserve special attention. The overall balance between the
repulsive and attractive forces between solutes and colloidal objects in liquids must be comparatively equal or larger
than 9–23 kT to have aggregation, adsorption, self-assembly, etc., and below 9 kT to obtain stable dispersions and col-
loids. As mentioned, liquids form at T ¼ 298 K, when the cohesive energy between the constituting atoms and mole-
cules is larger than 9 kT. While in the bulk of a liquid the interaction forces of a molecule or atom are fully symmetric at
interfaces, in contrast, in the topmost layer of molecules or atoms the interaction forces are asymmetric. Due to this
asymmetry, a certain tension/force arises in the plane of the interface. The stronger the interfacial tension, the stronger
the asymmetry. At contact between two phases, the topmost layer of molecules at the phase boundary also interacts
with the molecules from the other phase, this is called adhesion. The adhesion forces and energies counterbalance the
asymmetry of the forces acting on the topmost molecular layer, i.e., the stronger the adhesion force, the smaller the
interfacial tension. If the adhesion force is stronger than the cohesion force, then the interfacial tension disappears,
the interface disappears, and the phases become fully miscible, as discussed in Chapter 3. This interfacial tension
has also the character of an energy density, and for pristine interfaces this is causally related to the cohesion energy
in the bulk material; interfacial energy density is about half the cohesion energy in bulk. Surface and interfacial tension
of liquid-gas and liquid interfaces, as well as interfacial and surface energy of solids-liquid and solid-gas interfaces, are
thoroughly discussed in Chapter 3. The effects of the interface tension can be seen in small liquid droplets or molten
metals, as the shape of the droplet itself is modeled by this interfacial tension. The small world of insects and bugs are
particularly affected by the interfacial tension. Because their size is comparable to the capillary length, when the shape
of the liquids is fully determined by interfacial tension, not by gravitation, they have a different perception of the sur-
rounding world than humans do. Interfacial tension can have a devastating effect on insects; some drown as they can-
not escape the surface tension, but some have adapted to take full advantage of it. For example, small water droplets
can be manipulated and transported by ants without any need for bottles or glasses, and some mosquitos have adapted
on water to straddle along the smooth water surface, etc. (Fig. 1).
Intuitively, the interfacial tension is the 2D equivalent of the cohesion energy in 3D. Interfacial tension is discussed in
detail in Chapter 3.
However, when the surface and the interface are chemically modified, e.g., with surfactant adsorbates, the inter-
facial tension and energy density of interfaces do not reflect anymore the cohesive energy between the molecules
in the bulk phase. Thus, the interface itself can be treated as a thermodynamic system on its own, as discussed in
Chapter 7. The interfacial tension and interfacial energy density between phases are now an exclusive reflection of

Chemistry of Functional Materials Surfaces and Interfaces 1 Copyright © 2021 Elsevier Inc. All rights reserved.
https://doi.org/10.1016/B978-0-12-821059-8.00004-1
2 1. Introduction

FIG. 1 (A) Ant drinking water (https://www.shutterstock.com/image-photo/ant-drinking-water-505718482); (B) mosquito striding on the sur-
face of water (https://www.shutterstock.com/image-photo/water-bug-standing-on-surface-calm-1732352752).

the lateral interactions between surfactant molecules, polymers, or particles adsorbed at the interface. In fact, under-
standing how to change the interfacial tension and energy density between phases was one of the key enabling ele-
ments in the development of most technological advances in the 20th and 21st centuries, ranging from detergency, oil,
and ore extraction to the advanced manufacturing of processors and advanced electronic devices (see Chapter 15).
Surfactants and amphiphiles are molecules, polymers, and other building blocks of matter that adsorb spontane-
ously at interfaces. Surfactants lower the interfacial tension and energy density between phases (water-oil, water-gas,
solid-water) independently of their cohesion energy. This enables the formation of emulsions and foams and increase
in surface wettability. Earlier, it was mentioned that when the adhesion forces are stronger than the cohesion forces
between two liquids, the interfacial tension vanishes, and the liquids become miscible. The fact that, in the presence of a
surfactant at interfaces, the interfacial tension is not anymore a true reflection of the bulk cohesion energy of the phases
can be understood from the following example. If the interfacial tension between two water and oil phases becomes
vanishingly small due to the addition of a surfactant, then the two phases do not mix, but this time they form emulsions
consisting of very fine oil droplets dispersed into water. Chapter 4 gives an introduction into the vast field of surfactant
chemistry. Emphasis is given on surfactant classification, surfactant design, and structure activity relationship. In sim-
ple words, what makes a surfactant effective and how is this reflected in different physicochemical parameters?
Chapter 4 also introduces other amphiphiles, such as Janus nanoparticles and supra-amphiphiles, noting that amphi-
philicity is a scalable property, being active well beyond the molecular scale, well into the nano- and microscales.
Amphiphiles and surfactants have an important property, which is to self-assemble into suprastructures. This enables
the creation of smart, reconfigurable, or “environmentally aware” materials, bottom up, via self-assembly processes.
Most of the surfaces we interact with on a daily basis are solid, such as the screen of the smartphone, the cup of
coffee, the wheel of the car, etc. The tactile feel, the adhesion, is determined by the interfacial energy between our skin
and these surfaces. In the modern world, the concept of functional surfaces is gaining more popularity and it becomes a
requirement in the consumer products. Functional surfaces can be defined as surfaces that perform a function, such as
self-cleaning windows, or have a superior property, such as antiadherent, omniphobic antifingerprint in smartphone
screens, for example, while others are icephobic, or antifogging, etc. The key concepts in understanding the phenom-
ena behind functional surfaces and interfaces are adhesion and wetting. Surface wetting refers mainly to the interaction
of a liquid with a solid surface. Earlier, it was mentioned that when the adhesion forces are stronger than the cohesion
forces between two liquids, the interfacial tension vanishes, and the liquids become miscible. The interfacial tension or
energy between a solid and a liquid can also be altered, for example, with surfactants; however, when the interfacial
energy between a solid and a liquid becomes vanishingly small, the solid surface becomes fully wetted by the liquid.
The converse is true: when the interfacial energy is large, the surface becomes nonwetted, and the liquid pearls up on
the surface of the solid. Scientists have learned that, in addition to interfacial energy between the solid and liquid, the
geometry of the interface is key to designing functional surfaces. Finding inspiration in nature, scientists found out that
hierarchical structuring of the surface of the solid can lead to a variety of functional surfaces, such as superhydropho-
bic, superhydrophilic, icephobic, omniphobic, self-cleaning, etc. Chapter 5 gives an overview of the phenomena of
 Reference 3
wetting, wettability, and contact angle as the main measurement methods for macroscopic and nanoscale surfaces.
Chapter 5 also introduces the several functional surfaces.
In Chapter 6, a series of equations permitting the calculation of unknown surface tension, energy, work of adhesion,
etc. from known measurable macroscopic parameters have been grouped under the name “fundamental equation of
interfaces.” Their versatility in predicting the values of many interfacial parameters, for example, interfacial tension,
wettability, polarity of the surface, etc. from contact angle makes them extremely useful in practice. In Chapter 7, the
surface and interfacial tension are introduced via thermodynamic treatment of the interfacial layer. Although this
treatment has no direct practical implications, it gives the theoretical background necessary for the interpretation
of interfacial adsorption isotherms and interfacial tension vs concentration curves for surfactants and amphiphiles.
Chapter 8 treats surface functionalization that can be achieved in different ways, by physical methods such as
roughening of the surface, or photolithographic nanopatterning, and by chemical methods, by adsorption of surfactant
molecules. The adsorption of surfactant molecules on solid surfaces involves either chemical or physical bonding,
resulting in the formation of a self-assembled monolayer. Several types of chemical bonding and substrates are
reviewed. In addition, a surfactant monolayer can be prepared first at the water-air interface and then transferred onto
the surface of the solid via the Langmuir-Blodgett and dip-coating methods.
Solid-solid interfaces also have practical relevance, especially in layered electronic devices. Solid-solid interface, in
particular the metal-organic interface, is the locus of another type of phenomena of practical importance, namely the
electron transfer. In the previous chapters, the interfaces were the place where different forces met. In Chapter 9, the
metal-organic interfaces are treated as the contact point between electron energy levels of a metal, material with delo-
calized electron energy levels called bands, and the organic molecules and polymers whose energy levels are discrete
and localized. Understanding electron transfer between metal electrodes and organic conductors is of practical impor-
tance, especially for the manufacturing of organic photovoltaics, organic light emitting diodes, and other organic elec-
tronic devices. Any of these devices requires at least several layers of electroactive organic materials, and knowledge of
adhesion, wettability, and interfaces is required for their development and manufacturing.
Chapters 10 and 11 deal with the interaction forces and energies between interfaces in different media. These inter-
action forces can be repulsive or attractive and they are the same forces governing the molecular interactions. The bal-
ance between the attractive and repulsive interaction forces is of practical importance, controlling the phenomena of
particle aggregation, colloid stability, particle adsorption on surfaces, self-assembly of nanoparticles, etc. Chapter 12
introduces colloids, which are the oldest type of nanomaterials known and are today encountered in the food industry,
pharma, and many other consumer products. Colloids are constituted from finely divided particles, nanoparticles, or
liquid droplets dispersed into a continuous medium. Because their surface-to-volume ratio is very high, their behavior
is governed almost exclusively by their surface and interfacial properties. Synthesis of colloids as well as stability cri-
teria is discussed.
As a continuation on the topic of colloids, but deserving special attention, Chapter 13 introduces the synthesis of
polymeric nanoparticles and polymeric nanostructured interfaces via emulsion polymerizations. As expected, the
interfacial aspects determine the types of emulsions and nature of the nanomaterials that can be synthesized. The types
of emulsions and conditions of formation are briefly reviewed. A case study covers some examples of synthesis of
nanostructured interfaces, polymerization of the emulsions stabilized by amphiphilic particles.
Some nanoparticles, depending on their surface properties, can also spontaneously adsorb at interfaces; they can
form monolayers and stabilize emulsions. The factors responsible for why some particles can adsorb at liquid-liquid,
liquid-gas, and solid-liquid interfaces are discussed in Chapter 14. Once adsorbed at the interfaces the particle-particle
interactions leads to the decrease in the interfacial tension. Responsible for this is their lateral interaction, which is
governed by the same types of forces as in case surfactants, and in addition by particle specific interactions, capillary
floatation, or immersion forces. In fact, in recent times, nanoparticles have been used in the synthesis of photonic crys-
tals via the Langmuir-Blodgett method and other self-assembly structures.
The last chapter of this book discusses the role of interfaces in integrated circuit manufacturing via photolithogra-
phy. Photolithography is the only top-down preparation method of nanomaterials and nanostructured surfaces. In the
past few years, it evolved into the most precise technique to prepare with large machines, structures as small as 7 nm
(the gate of the field-effect transistor). In practice, the photolithographic manufacturing process of chips and processors
requires in-depth knowledge and control of interfacial phenomena such as adhesion, wetting, capillary forces, and
interfaces.

Reference
[1] G. Kaptay, G. Csicsovszki, M.S. Yaghmaee, An absolute scale for the cohesion energy of pure metals, Mater. Sci. Forum. 414–415 (2003) 235–240.
https://doi.org/10.4028/www.scientific.net/MSF.414-415.235.
 C H A P T E R

2
Thermal energy scale kT

At the nanoscale, the interaction energies are generally expressed in multiples of kT, also referred to as the thermal
energy scale. The average kinetic energy of a gas atom with three degrees of freedom is 3/2 kT, is roughly the energy of
thermal fluctuations at a given temperature
1 kT. The thermal energy has a randomizing effect contributing to an
increase in the entropy of the thermodynamic system. By expressing the energy of intermolecular interactions or nano-
particle interactions as multiples of kT, the interaction strength can be compared with the randomizing effect of
temperature.
Next, it is instructive to follow the kT in several different contexts as well as its origin. A thermodynamic system will
tend to move toward a lower energy state when available. When applied to chemical systems, for example, a solute in
a solution or a gas has a chemical potential defined as the rate of change of the Gibbs free energy with the number of
species in the system, at constant temperature and pressure:


δG
μi ¼ (2.1)
δNi T, P
Therefore, the change in chemical potential of a gas or a solute in a solution changes with the change in concentration.
Chemical potentials are important in describing the equilibrium in physicochemical processes such as evaporation,
melting, boiling, solubility, interfacial adsorption, liquid-liquid extraction, etc. The reason why the chemical potentials
are so important in the equilibrium chemistry is that when the two chemical systems are open and can exchange mol-
ecules or atoms, the rate of change of their free energy would be equal when equilibrium is established. Take, for exam-
ple, the molecules in the vapor and the liquid phase at equilibrium; by equating the chemical potentials of the molecule
of type i in two phases at equilibrium, or two regions 1 and 2, we obtain
μ1i + kT ln Xi1 ¼ μ2i + kT ln Xi2 (2.2)
At equilibrium between n different phases, the above equality must be satisfied for all phases:
μni + kT ln Xin ¼ constant (2.3)
where Xni
is the molecular fraction, volume fraction, or concentration of solute in phase n. For pure solution, this is
usually taken as unity. The factor k ln X is known under different names, such as the entropy of mixing, configuration
entropy, entropy of confining the molecules, etc.
Eq. (2.2) gives us the possibility to calculate the distribution of molecules between two phases, or two regions of
space at equilibrium, for example, a liquid in equilibrium with its vapors, or the distribution of the molecules of
gas in the atmosphere due to changes in the gravitational potential with altitude. For example, the number density
ρz of the molecules of gas in the Earth’s atmosphere changes with the altitude z and the mathematical function that
gives us the possibility to predict this change is
μzi + kT ln ρzi ¼ μ0i + kT ln ρ0i (2.4)
where ρzi is the number density of molecule i at altitude z and ρ0i is the number density of molecules of gas i at the
surface of the Earth z ¼ 0. Rearranging the above formula gives us the barometric formula or barometric law that gives
the density at the altitude z as a function of the number density of air molecules at the sea level ρ0i :

Chemistry of Functional Materials Surfaces and Interfaces 5 Copyright © 2021 Elsevier Inc. All rights reserved.
https://doi.org/10.1016/B978-0-12-821059-8.00015-6
6 2. Thermal energy scale kT

 z 

 μi  μ0i ðmgzÞ
ρzi ¼ ρ0i exp ¼ ρi exp
0
(2.5)
kT kT
where m is the molecular mass and g is the gravitational acceleration. Note that the potential energy of the air mol-
ecules mgz is “compared” to the kT at any height above the Earth’s surface. With the increase in the potential energy of
the molecules compared to kT, less molecules are found at higher altitudes (Fig. 2.1). In other words, if mgz is small
compared to kT, then the thermal energy would uniformize the distribution of molecules with the altitude such that
little variation in the number density of air molecules would be registered.
The same distribution applies to ions that, for example, carry a charge e between two different regions that have
different potentials ψ 1 and ψ 2:


eðψ 2  ψ 1 Þ
ρ2i ¼ ρ1i exp (2.6)
kT
and this is known as the Nernst equation. It is nonetheless important to note that interactions are additive; for example,
if the difference in energy between two regions is given by potential, potential energy, and chemical potential, then the
exponent will be the sum of all these contributions.
The above equations also give us the possibility to gauge the strength of interaction between molecules. For exam-
ple, if a liquid is in equilibrium with its vapors at standard conditions of pressure 1 atm and temperature 298 K, then
1 mol of gas will occupy approximately 22.4 m3 and a mole of liquid approximately 0.02 m3. Then the difference in
energy between the liquid and gas states will be [1]:
gas
0 gas 0 liquid Xi 22:4
μi  μi
kT ln liq

kT ln
7kT (2.7)
Xi 0:02

where 1 kT is approximately the energy of the thermal fluctuations. Therefore, it can be said that if the interaction
strength between molecules in a gas phase at temperature T is larger than 7 kT, then it condenses into liquid. Con-
versely, if the cohesion strength between the molecules of a liquid become smaller than 7 kT, then it transforms into
gas as the cohesion energy is simply too low to hold the molecules together. This alludes to what is known as the
Trouton rule, which states that the entropy of vaporization is roughly the same for different kinds of liquids, about
85 J K1 mol1, which is roughly 9.5 kT.

FIG. 2.1 The bottle was capped (left) in the mountain and brought to the ground level (right).
 2. Thermal energy scale kT 7

FIG. 2.2 Various interaction energies on the kT scale.

The kT criterion can be generalized to gauge the interaction strength between molecules; as stated above, if the
interaction between molecules in a medium is larger than 9.5 kT at a given temperature, then this interaction will
dominate over the thermal fluctuations and form a condensed phase, due to aggregation, adsorption, or self-assembly.
For interaction energies, the use of the kT energy scale is convenient, as 1 kT equals the thermally induced 3D Brownian
motion energy of a molecule (surfactant, or solute, or particle), which provides a reference value of interaction energies
for molecules sticking together vs fly apart, binding vs unbinding, etc. (Fig. 2.2). Fig. 2.2 provides a variety of inter-
action energies represented on the kT energy scale.
Similarly, the kT factor is also met in kinetics. For example, the Arrhenius equation per molecule is
Ea
k ¼ Ae kT (2.8)
where Ea is the activation energy barrier and k is the rate constant of the reaction. If, for example, Ea is much larger
than kT, then the reaction rate is also very small. On the other hand, if the energy barrier is comparable to kT, then the
reaction rate is high, and the reaction can be activated by the thermal energy.
The kT factor is also encountered in the Boltzmann distribution, which is a probability distribution that gives the
probability of a state to exist function of the state’s energy and temperature and it is given by


Ei
exp 
kT
P¼ n
 (2.9)
X Ej
exp 
j
kT

where P is the probability of state i, of the energy Ei, and n is the total number of accessible states of corresponding
energies Ej (j¼1 n). The Boltzmann distribution describes the distribution of particles, such as atoms or molecules, over
all accessible energy states. In a system consisting of many particles, the probability of picking a random particle with
the energy Ei is equal to the number of particles in state i divided by the total number of particles in the system, that is,
the fraction of particles occupying the state i:


Ei
exp 
Ni kT
Pi ¼ ¼ n
 (2.10)
Ntotal X Ej
exp 
j
kT
8 2. Thermal energy scale kT

The denominator in the above equation is the partition function 1/Z:

1 1
¼ n
 (2.11)
Z X Ej
exp 
j
kT

Reference
[1] J. Israelachvili, Intermolecular and Surface Forces, third ed., Academic Press, San Diego, CA, 2011.
 C H A P T E R

3
Surfaces and interfaces

An interface is the boundary between two immiscible phases in contact, such as liquid-liquid, liquid-solid, liquid-
air, etc. Immiscibility arises when the constituent molecules interact stronger with the molecules from the same phase
than with the molecules from the other phase, i.e., the “cohesion forces” are stronger than the “adhesion forces.” The
force of cohesion is defined as the sum of the forces that act between the molecules of the superficial layer and the bulk,
while the forces of adhesion are defined as the forces that act between the superficial layer and the molecules of the next
phase.
The interface is characterized by a certain thickness, which is intuitively taken as the thickness of the last layer of
molecules at the surface of the phase that enter in “contact” or “feel” the influence of the molecules in the other phase. It
has been the subject of intense research where exactly lies the borderlines defining the interface between two phases in
contact. This can be simplistically defined as two monolayers thick, one monolayer at the interface belonging to one
phase and the other monolayer to the next phase (Fig. 3.1). This is probably the most satisfactory way to intuitively
understand the interface thickness. However, this not very rigorous, because the molecules from subsequent layers
also feel the presence of molecules from the other phase via “longer ranged” forces that operate and whose intensity
decays with the distance from the interface. Michael C. Petty stated that “if the molecules are electrically neutral, then
the forces between them will be short-range and the surfaces layer will be no more than one or two molecular diam-
eters; in contrast, the Coulombic forces associated with the charged species can extend the transition region over con-
siderable distances” [1].
The experimental studies of the neat liquid-liquid interfacial thickness revealed that the hexadecane-water thickness
is about
6 Å by X-ray reflectivity and
15 Å by neutron reflectivity [2]. The apparent discrepancy comes from the
limitation of the both methods which include two contributions, namely the intrinsic width of the interface “that char-
acterizes the crossover from one bulk composition to the other and a statistical width due to thermally induced cap-
illary wave fluctuations (ripples) of the interface” [2]. This also reflects the difficulty of the experimental methods to
probe the interfaces at molecular length scales. The X-ray reflectivity studies of the thickness of the mercury-water
interface was
5 Å, which is comparable to that of mercury-vapor interface of
5 Å and that of pure water-vapor inter-
face
3 Å [3]. These and other studies have revealed that the liquid-liquid and liquid-vapor interfaces are at least two
monolayers of molecules or atoms.
Recently, combined surface vibrational spectroscopy and molecular dynamics revealed an even more complex
aspect of interfaces; in addition to interfacial thickness variation, molecular structuring by ordering and layering of
molecules near interface were observed [4]. The characteristic molecular vibrations were probed at the water-
chloroform and water-dichloromethane interfaces as a function of interfacial depth. From the concentration profiles
of both water and organic solvent molecules it was observed that both the dichloromethane and water extended dee-
per into the opposite phase forming a thicker interface, while the water-chloroform interface was sharper. Near the
water-chloroform interface water monomers were detected, not associated via H-bonds and the concentration profile
of chloroform deeper into the bulk organic phase is oscillatory suggesting the CCl4 molecules are layered near the
interface, not observed for dichloromethane. Numerous examples of ordering and structuring of molecules near
the interface were reported, as well as the consequences, for example, surface freezing of the top molecular layer
of alkane at alkane-vapor interface is 2–3°C higher than the freezing temperature, while this was not observed at
an alkane-water interface, which suggests an increased ordering of alkane molecules in the former case [2].

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10 3. Surfaces and interfaces

Molecular modeling also helped in gaining insight into the interfacial boundaries. It was found that the water-
hexane interface is very sharp and is about two monolayers thick [5]; the water molecules near the hydrophobic inter-
face are oriented such that the molecular plane and the dipole moment are parallel to the plane of the interface and the
long axis of the hexane molecules is also parallel to the interface [5, 6]. In addition, some of the water molecules at the
hydrophobic interfaces are incapable of hydrogen bonding, about one in four molecules exhibit dangling hydrogen
bonds, which gives rise to a large interfacial energy [7]. On the other hand, water molecules near strongly polar inter-
faces such as quartz are capable of hydrogen bonding and are oriented in an ice-like structure and no dangling bonds
were observed in surface vibrational studies with vibrational sum-frequency spectroscopy [7].
The consequence of the molecular orientational ordering, layering, reduced capability of molecular bonding, and
interfacial mixing lead to a change in the solvent properties near the interface. For example, second-harmonic gener-
ation in combination with solvatochromic surfactants of different lengths known as “molecular rulers” were able to
probe solvent polarity with depth near the weakly and strongly associating water-organic solvent interfaces. For exam-
ple, the solvent polarity near the weakly associating water-cyclohexane interface quickly converges from the aqueous
to the organic limit in less than 9 Å, while the strongly associating water-1-octanol interface revealed a transition region
of ordered octanol molecules at the interface giving rise to a hydrophobic barrier [8]. The chemical structure and the
molecular dimensions greatly affect the thickness of the interface. Further systematic studies performed with
“molecular rulers” revealed that at the water-organic solvent interfaces the interface thickness and polarity strongly
depend on the molecular structure [9, 10].
The conclusion that can be drawn from experimental evidence is that the interface can be visualized as a sheet or as a
thin “membrane” with certain thickness. The thickness of the interface depends on the ability of the phases to interact
given by the balance between the adhesion and cohesion forces. For weakly interacting phases the interface thickness is
nearly two monolayers thick (Fig. 3.1A), while for strongly interacting phases the interface will be thicker than two
molecular monolayers (Fig. 3.1B). In addition, the polarity gradient across the interface can change due to molecular
ordering at the interface, which propagates to a certain depth in bulk, depicted as a color gradient in Fig. 3.1B.
The membrane separating two immiscible phases has therefore boundaries and is an open thermodynamic system
because it can exchange matter and energy with the neighboring phases. Molecules move continuously to and from
interface to bulk. A thermodynamic system is everything that has boundaries, an object constitutes a thermodynamic
system, be that a car, a grain of salt, or an interface, and all possess a certain internal energy, U. The energy of the
interface between the phases, also most commonly referred to as “interfacial energy,” is highest when the cohesion
energy is much larger than the adhesion energy. Interfacial energy decreases to negligible values when the adhesion
forces become comparable to cohesion forces and the phases begin to mix. Water-hexane interface is an example of a
high interfacial energy interface while water-ethanol interface has a zero interfacial energy, i.e., completely miscible.

FIG. 3.1 (A) The ideal sharp inter-

face between two weakly interacting
phases α and β can be imagined as a
thin membrane, two monolayers
thick with a sharp molecular density
profile that separates two phases.
(B) The thicker interface between
two phases that are strongly interact-
ing with diffuse density profile,
thicker than two monolayers. The
oscillation in the β phase indicate
ordering. The solvent polarity near
this interface changes due to order-
ing and loss or gain in bonding
capability.
 3.1 Surface tension of liquids 11
The molecules at the interface have energy higher than those in the bulk because they are not symmetrically sur-
rounded by other “alike” molecules in a perfectly balanced sphere. This imbalance of attraction forces and suppression
in the ability of the molecules to bond lead to more energetic molecules at the interface.

3.1 Surface tension of liquids

In the bulk, a molecule or an atom can be surrounded by a maximum 12 neighboring molecules (6 in the same plane
and 3 on each side of the neighboring planes) and experience a symmetric attraction from all sides in the 3D space. On
the other hand, at the surface of a liquid the molecules are about only half-way surrounded by molecules, thus expe-
rience an asymmetric attraction toward the bulk of the liquid (see Fig. 3.2A). The forces of cohesion act asymmetrically
on the interfacial layer and the topmost layers of molecules of a phase are compressed (Fig. 3.2B).
In addition to the cohesion forces that act perpendicularly on the surface plane, the surface tension forces act in the
plane of the surface and oppose any action to increase the surface area. Surface tension can be intuitively understood as
a unit vector force. To visualize this, an imaginary line can be drawn, of length l, on the surface of the liquid; this imag-
inary line splits the row of two molecules (Fig. 3.3) If it were possible, by pulling apart the two rows of molecules on the
surface of the liquid, a resisting tension force would arise because the molecules from each row attract each other gen-
erating a tension opposing the split (Fig. 3.3A).
If the length of this dividing line is l, then the force with which the pair of molecules in the two rows attracts each
other is.
F¼γl (3.1)
where γ is the unit tension force (N/m), i.e., the surface tension. Therefore, the surface tension γ is the unit force acting
on the surface plane to minimize the surface area.
To better understand the origin of the surface tension, we imagine a cross section through the surface of a liquid
(Fig. 3.3). At equilibrium no net force is acting on this horizontal line (plane) of molecules. If it were possible, the pull of
only one molecule out of this line (plane) would be countered by an opposing tension force trying to minimize the area
of the surface layer. The unit surface tension forces act left and right on the molecule being pulled out of the line and the
sum of these is the cohesion unit force (Fig. 3.3C). It costs energy to bring new molecules from the bulk to surface. When
surface is expanded, more “bonds” from the bulk are “broken” as new molecules are brought to occupy the “holes” in
the newly created surface, represented by the dotted circles in Fig. 3.3B. The energy of the molecules in bulk of the
liquid with maximum of 12 neighbors is lower than the energy of the molecules at the surface with the maximum
6 neighbors. The energy required to bring a molecule from the bulk to increase the area of the surface is the energy
of uncompensated bonds; at the surface, a molecule has about half of the neighbors of a molecule in the bulk, half of its
“physical bonds” remain uncompensated (Fig. 3.3B). Therefore, the surface energy is only a fraction of the cohesion
energy as explained later in more detail.

FIG. 3.2 (A) Molecular interactions in a liquid; (B) compression of the topmost surface layer of molecules due to the force of cohesion.
12 3. Surfaces and interfaces

FIG. 3.3 (A) Surface of a liquid on

which an imaginary line of length l
divides two parallel rows of mole-
cules; when trying to pull sideways
the two rows of molecules by apply-
ing a force F on each side, the surface
tension forces oppose the distancing
of molecules; the surface tension unit
vectors are oriented perpendicular to
the imaginary line. (B) Deformation
of the liquid-gas interface by pulling
only one molecule out of the surface;
in this case two new empty “holes”
(dotted circles) are created by the
expansion of the liquid-gas interface.
Two new molecules must be brought
in from the bulk liquid to occupy the
empty holes, depicted by the green
curved arrows. The total energy of
the interface will increase by an
amount equal to the energy of
uncompensated bonds of the new
molecules occupying the holes.
(C) Same situation as in (B) with the
depiction of the opposing surface ten-
sion forces resisting the deformation.
The vectorial sum of the surface ten-
sion vectors acting on the molecule
being pulled out of the interface is
the cohesion force acting on the
molecule.

FIG. 3.4 Forces acting on a steel needle, with a hydrophobic surface, floating on the surface of water without penetration.

Numerical example 3.1

Draw the surface tension force vectors acting on a steel needle with a hydrophobic surface floating on the surface of water
depicted in Fig. 3.4. The needle does not penetrate the surface. Calculate the maximum radius of a steel needle r, of length
l ¼ 1 cm that can be held on the surface of the water without sinking. The density of steel is 8000 kg/m3, ρwater ¼ 1 kg/dm3,
γ water ¼ 73 mN/m.
Discovering Diverse Content Through
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the following words:—“And when the Ḥayyot went, the Ofannim
went by them; and when the living creatures were lifted up from the
earth, the Ofannim were lifted up” (ver. 19); “and the Ofannim were
lifted up over against them” (ver. 20). And the cause of this is
explained thus:—“The spirit of the Ḥayyah was in the Ofannim”
(ibid.). For the sake of emphasis and further explanation the prophet
adds, “When those went, these went; and when those stood, these
stood; and when those were lifted up from the earth, the Ofannim
were lifted up over against them; for the spirit of the Ḥayyah was in
the Ofannim” (ver. 21). The order of these movements is therefore
as follows:—Whithersoever it is the will of God that the Ḥayyot
should move, thither they move of their own accord. When the
Ḥayyot move the Ofannim necessarily follow them, because they are
tied to them, and not because they move of their own accord in the
direction in which the Ḥayyot move. This order is expressed in the
words, “Whithersoever the spirit was to go, they went, thither was
the spirit to go; and the Ofannim were lifted up over against them;
for the spirit of the Ḥayyah was in the Ofannim” (ver. 20). I have
told you that Jonathan, the son of Uzziel, translates the verse thus,
“to the place whither it was the will that the Ḥayyot should go,” etc.

After having completed the account of the Ḥayyot, with their form
and motion, and of the Ofannim, which are beneath the Ḥayyot,
connected with them and forced to move when the Ḥayyot move,
the prophet begins to describe a third object which he perceived
prophetically, and gives the account of a new thing, viz., of that
which is above the Ḥayyot. He says that the firmament is above the
four Ḥayyot, above the firmament is the likeness of a throne, and
over the throne the likeness of the appearance of man. This is the
whole account of what the prophet perceived at first at the river
Chebar.
[Contents]
 CHAPTER III
When Ezekiel recalled to memory the form of the Chariot, which he
described in the beginning of the book, the same vision presented
itself to him a second time; in this vision he was borne to Jerusalem.
He explains in describing it things which have not been made clear
at first, e.g., he substitutes the term “cherubim” for Ḥayyot, whereby
he expresses that the [256]Ḥayyot of the first vision are likewise
angels like the cherubim. He says, therefore: “Where the cherubims
went, the Ofannim went by them: and when the cherubims lifted up
their wings to mount up from the earth, the same Ofannim also
turned not from beside them” (x. 16). By these words he shows how
closely connected the two motions are [viz., that of the Ḥayyot and
that of the Ofannim]. The prophet adds, “This is the Ḥayyah that I
saw under the God of Israel by the river of Chebar; and I knew that
they were cherubims” (ver. 20). He thus describes the same forms
and the same motions, and states that the Ḥayyot and the cherubim
are identical. A second point is then made clear in this second
description, namely, that the Ofannim are spherical; for the prophet
says, “As for the Ofannim, it was cried unto them in my hearing, O
sphere” (ver. 13). A third point concerning the Ofannim is illustrated
here in the following words: “To the place whither the head looked
they followed it: they turned not as they went” (ver. 11). The motion
of the Ofannim is thus described as involuntary, and directed “to the
place whither the head looketh”; and of this it is stated that it moves
“whither the spirit is to go” (i. 20). A fourth point is added
concerning the Ofannim, namely, “And the Ofannim were full of eyes
round about, even the Ofannim that they four had” (x. 12). This has
not been mentioned before. In this second description there are
further mentioned “their flesh, and their backs, and their hands, and
their wings” (ibid.), whilst in the first account none of these is
mentioned; and it is only stated that they are bodies. Though they
are endowed in the second account with flesh, hands, and wings, no
form is given to them. In the second account each ofan is attributed
to a cherub, “one ofan by one cherub, and another ofan by another
cherub.” The four Ḥayyot are then described as one Ḥayyah on
account of their interjoining: “This is the Ḥayyah that I saw under
the God of Israel by the river of Chebar” (ver. 20). Also the Ofannim,
though being four in number, as has been mentioned, are called
“one ofan upon the earth” (ver. 15), because they interjoin, and
“they four have one likeness” (ver. 16). This is the additional
explanation which the second vision gives of the form of the Ḥayyot
and the Ofannim.

[Contents]
 CHAPTER IV
It is necessary to call your attention to an idea expressed by
Jonathan, the son of Uzziel. When he saw that the prophet says in
reference to the Ofannim, “It was cried unto them in my hearing, O
gilgal” (“sphere”) (x. 13), he assumed that by Ofannim the heavens
are meant, and rendered ofan by gilgal, “sphere,” and ofannim by
gilgelaya, “spheres.” I have no doubt that he found a confirmation of
his opinion in the words of the prophet that the Ofannim were like
unto the colour of tarshish (ver. 16), a colour ascribed to the
heavens, as is well known. When he, therefore, noticed the passage,
“Now as I beheld the Ḥayyot, behold one Ofan upon the earth” (i.
15), which clearly shows that the Ofannim were upon the earth, he
had a difficulty in explaining it in accordance with his opinion.
Following, however, his interpretation, he explains the terms ereẓ,
employed here as denoting the inner surface of the heavenly sphere,
which may be considered as ereẓ (“earth” or “below”), in relation to
all that is above that surface. He [257]therefore translates the words
ofan eḥad ba-areẓ as follows: “One ofan was below the height of the
heavens.” Consider what his explanation of the passage must be. I
think that he gave this explanation because he thought that gilgal
denotes in its original meaning “heaven.” My opinion is that gilgal
means originally “anything rolling”; comp. “And I will roll thee (ve-
gilgaltika) down from the rocks” (Jer. li. 25); “and rolled (va-yagel)
the stone” (Gen. xxix. 10); the same meaning the word has in the
phrase: “Like a rolling thing (gilgal) before the whirlwind” (Isa. xvii.
13). The poll of the head, being round, is therefore called gulgolet;
and because everything round rolls easily, every spherical thing is
called gilgal; also the heavens are called gilgallim on account of their
spherical form. Thus our Sages use the phrase, “It is a wheel (gilgal)
that moves round the world”; and a wooden ball, whether small or
large, is called gilgal. If so, the prophet merely intended by the
words, “As for the Ofannim, it is cried to them in my hearing, O
sphere” (gilgal), to indicate the shape of the Ofannim, as nothing
has been mentioned before respecting their form and shape; but he
did not mean to say that the Ofannim are the same as the heavens.
The term “like tarshish” is explained in the second account, in which
it is said of the Ofannim: “And the appearance of the ofannim was
like the colour of tarshish.” This latter passage is translated by
Jonathan, the son of Uzziel, “like the colour of a precious stone,”
exactly in the same manner as Onkelos translates the phrase ke-
maʻase libnat ha-sappir, “like the work of the whiteness of sapphire”
(Exod. xxix. 10). Note this. You will not find it strange that I mention
the explanation of Jonathan, son of Uzziel, whilst I gave a different
explanation myself; for you will find many of the wise men and the
commentators differ sometimes from him in the interpretation of
words and in many things respecting the prophets. Why should it be
otherwise in these profound matters? Besides, I do not decide in
favour of my interpretation. It is for you to learn both—the whole of
his explanation, from what I have pointed out to you, and also my
own opinion. God knoweth which of the two explanations is in
accordance with that which the prophet intended to say.

[Contents]
 CHAPTER V
It is necessary to notice that the plural marot elohim, “visions of
God,” is here used, and not the singular mareh, “vision,” for there
were several things, of different kinds, that were perceived by the
prophet. The following three things were perceived by him: the
Ofannim, the Ḥayyot, and the man above the Ḥayyot. The
description of each of these visions is introduced by the word va-
ereh, “and I beheld.” For the account of the Ḥayyot, begins, “And I
looked (va-ereh), and behold a whirlwind,” etc. (Ezek. i. 4). The
account of the Ofannim begins: “Now as I beheld (va-ereh) the
Ḥayyot, behold one Ofan upon the earth” (ver. 15). The vision of
that which is above the Ḥayyot in order and rank begins: “And I saw
(va-ereh) as the colour of the amber, etc., from the appearance of
his loins even upward” (ver. 27). The word va-ereh, “and I beheld,”
only occurs these three times in the description of the Mercabah.
The doctors of the Mishnah have already explained this fact, and my
attention was called to it by their remarks. [258]For they said that
only the two first visions, namely, that of the Ḥayyot and the
Ofannim, might be interpreted to others; but of the third vision, viz.,
that of the ḥashmal and all that is connected with it, only the heads
of the sections may be taught. Rabbi [Jehudah], the Holy, is of
opinion that all the three visions are called maʻaseh mercabah, and
nothing but the heads of the sections could be communicated to
others. The exact words of the discussion are as follows:—Where
does maʻaseh mercabhah end? Rabbi says, with the last va-ereh;
Rabbi Yiẓḥak says it ends at the word ḥashmal (ver. 27). The portion
from va-ereh to ḥashmal may be fully taught; of that which follows,
only the heads of the sections; according to some it is the passage
from va-ereh to ḥashmal, of which the heads of the sections may be
taught, but that which follows may only be studied by those who
possess the capacity, whilst those that cannot study it by themselves
must leave it.—It is clear from the words of our Sages that different
visions are described, as may also be inferred from the repetition of
the word va-ereh, and that these visions are different from each
other in degree; the last and highest of them is the vision
commencing, “And I saw as the colour of ḥashmal”; that is to say,
the divided figure of the man, described as “the appearance of fire,
etc., from the appearance of his loins even upward, and from the
appearance of his loins even downward,” etc. There is a difference of
opinion among our Sages whether it is permitted to give by way of
hints an exposition of any part of this third vision, or whether it is
prohibited even to teach of it the heads of the sections, so that only
the wise can arrive at understanding it by their own studies. You will
also notice a difference of opinion among our Sages in reference to
the two first visions, viz., that of the Ḥayyot and that of the Ofannim
whether these may be taught explicitly or only by way of hints, dark
sayings, and heads of sections. You must also notice the order of
these three visions. First comes the vision of the Ḥayyot, because
they are first in rank and in the causal relation, as it is said, “For the
spirit of the Ḥayyah was in the Ofannim” and also for other reasons.
The vision of the Ofannim [comes next, and] is followed by one
which is higher than the Ḥayyot, as has been shown. The cause of
this arrangement is, that in study the first two must necessarily
precede the third, and in fact they lead to it.

[Contents]
 CHAPTER VI
The sublime and great subject which Ezekiel by prophetic impulse
began to teach us in the description of the Mercabah, is exactly the
same which Isaiah taught us in general outlines, because he did not
require all the detail. Isaiah says, “I saw the Lord sitting upon a
throne, high and lifted up, and his train filled the temple. Above it
stood seraphims,” etc. (Isa. vi. 1 seq.). Our Sages have already
stated all this clearly, and called our attention to it. For they say that
the vision of Ezekiel is the same as that of Isaiah, and illustrate their
view by the following simile:—Two men saw the king riding, the one
a townsman, the other a countryman. The former, seeing that his
neighbours know well how the king rides, simply tells them that he
saw the king; but the villager, wishing to tell his friends things which
they do not know, relates in detail how the king was riding,
describes his followers, and [259]the officers who execute his order
and command. This remark is a most useful hint; it is contained in
the following passage (Ḥagigah, 13 b): “Isaiah saw all that has been
seen by Ezekiel; Isaiah is like a townsman that sees the king, Ezekiel
like a countryman that sees the king.” These words can be explained
in the manner which I have just mentioned, viz., the generation of
Isaiah did not require the detailed description; his account, “I saw
the Lord,” etc., sufficed. The generation of the Babylonian exile
wanted to learn all the details. It is, however, possible that the
author of this saying held Isaiah as more perfect than Ezekiel, so
that the vision might have overawed Ezekiel and appeared fearful to
him; but Isaiah was so familiar with it that he did not consider it
necessary to communicate it to others as a new thing, especially as
it was well known to the intelligent.
[Contents]
 CHAPTER VII
One of the points that require investigation is the connexion
between the vision of the mercabah and the year, month, and day,
and also the place of the vision. A reason must be found for this
connexion, and we must not think that it is an indifferent element in
the vision. We must consider the words, “the heavens were opened”
(Ezek. i. 1); they give the key to the understanding of the whole.
The figure of opening, also that of opening the gates, occurs
frequently in the books of the prophets; e.g., “Open ye the gates
that the righteous nation may enter in” (Isa. xxvi. 2); “He opened
the doors of heaven” (Ps. lxxviii. 23); “Lift them up, ye everlasting
doors” (ibid. xxiv. 9); “Open to me the gates of righteousness, I will
go into them, and I will praise the Lord” (ibid. cxviii. 19). There are
many other instances of this kind. You must further notice that the
whole description refers undoubtedly to a prophetic vision, as it is
said, “And the hand of the Lord was there upon him” (Ezek. i. 3);
and yet there is a very great difference between the various parts of
the description, for in the account of the Ḥayyot the prophet does
not say four Ḥayyot, but “the likeness of the four Ḥayyot” (ibid. ver.
5); similarly he says, “And the likeness of a firmament was over the
heads of the Ḥayyot” (ver. 22); “as the appearance of a sapphire
stone, the likeness of a throne,” and “the likeness of the appearance
of man above it” (ver. 26). In all these instances the word “likeness”
is used, whilst in the account of the Ofannim the phrases, “the
likeness of Ofannim,” the “likeness of an Ofan,” are not employed,
but they are described in a positive manner as beings in actual
existence, with their real properties. The sentence “they four had
one likeness” must not mislead you, for here the word “likeness” is
not used in the same connexion or in the same sense as indicated
above. In the description of the last vision the prophet confirms and
explains this view. When he commences to describe the firmament
in detail, he says, “the firmament,” without adding the words “the
likeness of,” for he says, “And I looked, and behold, in the firmament
that was above the head of the cherubims there appeared over them
as it were a sapphire stone, as the appearance of the likeness of a
throne” (x. 1). Here the prophet speaks of “the firmament” and not
of “the likeness of the firmament,” as he does when he connects the
firmament with the [260]heads of the likeness of the Ḥayyot (i. 22).
But, as regards the throne, he says, “the likeness of a throne
appeared over them,” in order to indicate that the firmament was
first perceived and then the likeness of the throne was seen over it.
Consider this well.

You must further notice that in the description of the first vision the
Ḥayyot have wings and at the same time human hands, whilst in the
second vision, in which the term cherubim is substituted for Ḥayyot,
at first only wings were perceived, and later on human hands were
seen. Comp. “And there appeared in the cherubims the form of a
man’s hand under their wings” (x. 8). Here “form” (tabnit) is used
instead of “likeness” (demut); and the hands are placed under the
wings. Note this.

Consider that in reference to the ofannim, the prophet says, le-

ʻummatam, “over against them,” although he does not ascribe to
them any form.

He further says, “As the appearance of the bow that is in the cloud
in the day of rain, so was the appearance of the brightness round
about. This was the appearance of the likeness of the glory,” etc. (i.
28). The substance and true essence of the bow described here is
well known. The simile and comparison is in this case very
extraordinary, and is undoubtedly part of the prophecy; and note it
well.
It is also noteworthy that the likeness of man above the throne is
divided, the upper part being like the colour of ḥashmal, the lower
part like the appearance of fire. As regards the word ḥashmal, it has
been explained to be a compound of two words ḥash and mal,
including two different notions, viz., ḥash signifying “swiftness,” and
mal denoting “pause.” The two different notions are here joined in
one word in order to indicate figuratively the two different parts,—
the upper part and the lower. We have already given a second
explanation, namely, that ḥashmal includes the two notions of
speech and silence; in accordance with the saying of our Sages, “At
times they are silent, at times they speak,” thus deriving hash of the
same root as heḥeshethi, “I have been silent” (Isa. xlii. 14); the
word ḥashmal thus includes two notions, and indicates “speech
without sound.” There is no doubt that the words, “at times they are
silent, at times they speak,” refer to a created object. Now consider
how they clearly stated that the divided likeness of man over the
throne does not represent God, who is above the whole chariot, but
represents a part of the creation. The prophet likewise says “that is
the likeness of the glory of the Lord”; but “the glory of the Lord” is
different from “the Lord” Himself, as has been shown by us several
times. All the figures in this vision refer to the glory of the Lord, to
the chariot, and not to Him who rides upon the chariot; for God
cannot be compared to anything. Note this. I have thus given you
also in this chapter as much of the heads of the sections as will be
useful to you for the comprehension of this subject, if you fill out
[the sections of] these heads. If you consider all that has been said
in this part up to this chapter, the greater part of this subject or the
whole of it will be clear to you, except a few points and some
repetitions the meaning of which is unknown. Perhaps further study
will help to reveal even these things so that nothing will remain
unintelligible.
Do not expect or hope to hear from me after this chapter a word on
this subject, either explicitly or implicitly, for all that could be said on
it has been [261]said, though with great difficulty and struggle. I will
now begin to treat of some of the other subjects which I hope to
elucidate in this treatise.

[Contents]
 CHAPTER VIII
Transient bodies are only subject to destruction through their
substance and not through their form, nor can the essence of their
form be destroyed; in this respect they are permanent. The generic
forms, as you know, are all permanent and stable. Form can only be
destroyed accidentally, i.e., on account of its connexion with
substance, the true nature of which consists in the property of never
being without a disposition to receive form. This is the reason why
no form remains permanently in a substance; a constant change
takes place, one form is taken off and another is put on. How
wonderfully wise is the simile of King Solomon, in which he
compares matter to a faithless wife; for matter is never found
without form, and is therefore always like such a wife who is never
without a husband, never single; and yet, though being wedded,
constantly seeks another man in the place of her husband; she
entices and attracts him in every possible manner till he obtains from
her what her husband has obtained. The same is the case with
matter. Whatever form it has, it is disposed to receive another form;
it never leaves off moving and casting off the form which it has in
order to receive another. The same takes place when this second
form is received. It is therefore clear that all corruption, destruction,
or defect comes from matter. Take, e.g., man; his deformities and
unnatural shape of limbs; all weakness, interruption, or disorder of
his actions, whether innate or not, originate in the transient
substance, not in the form. All other living beings likewise die or
become ill through the substance of the body and not through its
form. Man’s shortcomings and sins are all due to the substance of
the body and not to its form; while all his merits are exclusively due
to his form. Thus the knowledge of God, the formation of ideas, the
mastery of desire and passion, the distinction between that which is
to be chosen and that which is to be rejected, all these man owes to
his form; but eating, drinking, sexual intercourse, excessive lust,
passion, and all vices, have their origin in the substance of his body.
Now it was clear that this was the case,—it was impossible,
according to the wisdom of God, that substance should exist without
form, or any of the forms of the bodies without substance, and it
was necessary that the very noble form of man, which is the image
and likeness of God, as has been shown by us, should be joined to
the substance of dust and darkness, the source of all defect and
loss. For these reasons the Creator gave to the form of man power,
rule, and dominion over the substance;—the form can subdue the
substance, refuse the fulfilment of its desires, and reduce them, as
far as possible, to a just and proper measure. The station of man
varies according to the exercise of this power. Some persons
constantly strive to choose that which is noble, and to seek
perpetuation in accordance with the direction of their nobler part,—
their form; their thoughts are engaged in the formation of ideas, the
acquisition of true knowledge about everything, and the union with
the divine intellect which flows down upon them, and which is the
source of man’s form. Whenever they are led by the wants of the
body to that which is low and avowedly disgraceful, they are grieved
at their [262]position, they feel ashamed and confounded at their
situation. They try with all their might to diminish this disgrace, and
to guard against it in every possible way. They feel like a person
whom the king in his anger ordered to remove refuse from one place
to another in order to put him to shame; that person tries as much
as possible to hide himself during the time of his disgrace; he
perhaps removes a small quantity a short distance in such a manner
that his hands and garments remain clean, and he himself be
unnoticed by his fellow-men. Such would be the conduct of a free
man, whilst a slave would find pleasure in such work;—he would not
consider it a great burden, but throw himself into the refuse, smear
his face and his hands, carry the refuse openly, laughing and
singing. This is exactly the difference in the conduct of different
men. Some consider, as we just said, all wants of the body as
shame, disgrace, and defect to which they are compelled to attend;
this is chiefly the case with the sense of touch, which is a disgrace to
us according to Aristotle, and which is the cause of our desire for
eating, drinking, and sensuality. Intelligent persons must, as much
as possible, reduce these wants, guard against them, feel grieved
when satisfying them, abstain from speaking of them, discussing
them, and attending to them in company with others. Man must
have control over all these desires, reduce them as much as
possible, and only retain of them as much as is indispensable. His
aim must be the aim of man as man, viz., the formation of ideas,
and nothing else. The best and sublimest among them is the idea
which man forms of God, angels, and the rest of the creation
according to his capacity. Such men are always with God, and of
them it is said, “Ye are princes, and all of you are children of the
Most High” (Ps. lxxxii. 6). This is man’s task and purpose. Others,
however, that are separated from God form the multitude of fools,
and do just the opposite. They neglect all thought and all reflection
on ideas, and consider as their task the cultivation of the sense of
touch,—that sense which is the greatest disgrace; they only think
and reason about eating and love. Thus it is said of the wicked who
are drowned in eating, drinking, and love, “They also have erred
through wine, and through strong drink are out of the way,” etc.
(Isa. xxviii. 7), “for all tables are full of vomit and filthiness, so that
there is no place clean” (ver. 8); again, “And women rule over them”
(ibid. iii. 2),—the opposite of that which man was told in the
beginning of the creation, “And for thy husband shall thy desire be,
and he shall rule over thee” (Gen. iii. 16). The intensity of their lust
is then described thus, “Every one neighed after his neighbour’s
wife,” etc. (Jer. v. 8); “they are all adulterers, an assembly of
treacherous men” (ibid. ix. 2). The whole book of the Proverbs of
Solomon treats of this subject, and exhorts to abstain from lust and
intemperance. These two vices ruin those that hate God and keep
far from Him; to them the following passages may be applied, “They
are not the Lord’s” (ibid. v. 10); “Cast them out of my sight, and let
them go forth” (ibid. xv. 1). As regards the portion beginning, “Who
can find a virtuous woman?” it is clear what is meant by the
figurative expression, “a virtuous woman.” When man possesses a
good sound body that does not overpower him nor disturb the
equilibrium in him, he possesses a divine gift. In short, a good
constitution facilitates the rule of the soul over the body, but it is not
impossible to conquer a bad constitution by training. For this reason
King [263]Solomon and others wrote the moral lessons; also all the
commandments and exhortations in the Pentateuch aim at
conquering the desires of the body. Those who desire to be men in
truth, and not brutes, having only the appearance and shape of
men, must constantly endeavour to reduce the wants of the body,
such as eating, love, drinking, anger, and all vices originating in lust
and passion; they must feel ashamed of them and set limits to them
for themselves. As for eating and drinking in so far as it is
indispensable, they will eat and drink only as much as is useful and
necessary as food, and not for the purpose of pleasure. They will
also speak little of these things, and rarely congregate for such
purposes. Thus our Sages, as is well known, kept aloof from a
banquet that was not part of a religious act, and pious men followed
the example of R. Phineḥas, son of Jair, who never dined with other
persons, and even refused to accept an invitation of R. Jehudah, the
Holy. Wine may be treated as food, if taken as such, but to form
parties for the purpose of drinking wine together must be considered
more disgraceful than the unrestrained conduct of persons who in
daylight meet in the same house undressed and naked. For the
natural action of the digestive organ is indispensable to man, he
cannot do without it; whilst drunkenness depends on the free will of
an evil man. To appear naked in the presence of other people is
misconduct only according to public opinion, not according to the
dictates of reason, whilst drunkenness, which ruins the mind and the
body of man, reason stamps as a vice. You, therefore, who desire to
act as human beings must keep away from it, and even from
speaking of it. On sexual intercourse, I need not add anything after I
have pointed out in the commentary on Abot (i. 17) how it is treated
by our Law, which is the teaching of pure wisdom—no excuse
whatever should induce us to mention it or to speak of it. Thus our
Sages said, that Elisha the prophet is called holy, because he did not
think of it, and consequently never found himself polluted with
semen. In a similar manner they say that Jacob had the first issue of
semen for the conception of Reuben. All these traditional stories
have the object of teaching the nation humane conduct. There is a
well-known saying of our Sages, “The thoughts about the sin are
more dangerous than the sin itself.” I can offer a good explanation of
this saying: When a person is disobedient, this is due to certain
accidents connected with the corporeal element in his constitution;
for man sins only by his animal nature, whereas thinking is a faculty
of man connected with his form,—a person who thinks sinfully sins
therefore by means of the nobler portion of his self; and he who
wrongly causes a foolish slave to work does not sin as much as he
who wrongly causes a noble and free man to do the work of a slave.
For this specifically human element, with all its properties and
powers, should only be employed in suitable work, in attempts to
join higher beings, and not in attempts to go down and reach the
lower creatures. You know how we condemn lowness of speech, and
justly so, for speech is likewise peculiar to man and a boon which
God granted to him that he may be distinguished from the rest of
living creatures. Thus God says, “Who gave a mouth to man?”
(Exod. iv. 11); and the prophet declares, “The Lord God hath given
me a learned tongue” (Isa. l. 4). This gift, therefore, which God gave
us in order to enable us to perfect ourselves, to learn and to teach,
must not be employed in doing that which is for us most
[264]degrading and perfectly disgraceful; we must not imitate the
songs and tales of ignorant and lascivious people. It may be suitable
to them, but is not fit for those who are told, “And ye shall be unto
me a kingdom of priests and a holy nation” (Exod. xix. 6). Those
who employ the faculty of thinking and speaking in the service of
that sense which is no honour to us, who think more than necessary
of drink and love, or even sing of these things; they employ and use
the divine gift in acts of rebellion against the Giver, and in the
transgression of His commandments. To them the following words
may be applied: “And I multiplied her silver and gold, which they
prepared for Baal” (Hos. ii. 10). I have also a reason and cause for
calling our language the holy language—do not think it is
exaggeration or error on my part, it is perfectly correct—the Hebrew
language has no special name for the organ of generation in females
or in males, nor for the act of generation itself, nor for semen, nor
for secretion. The Hebrew has no original expressions for these
things, and only describes them in figurative language and by way of
hints, as if to indicate thereby that these things should not be
mentioned, and should therefore have no names; we ought to be
silent about them, and when we are compelled to mention them, we
must manage to employ for that purpose some suitable expressions,
although these are generally used in a different sense. Thus the
organ of generation in males is called in Hebrew gid, which is a
figurative term, reminding of the words, “And thy neck is an iron
sinew” (gid) (Isa. xlviii. 4). It is also called shupka, “pouring out”
(Deut. xxiii. 2), on account of its function. The female organ is called
kobah (Num. xxv. 8), from kebah (Deut. xviii. 3), which denotes
“stomach”; reḥem, “womb,” is the inner organ in which the fœtus
develops; ẓoah (Isa. xxviii. 8), “refuse,” is derived from the verb
yaẓa, “he went out”; for “urine” the phrase meme raglayim, “the
water of the feet” (2 Kings. xviii. 17), is used; semen is expressed by
shikbat zeraʻ, “a layer of seed.” For the act of generation there is no
expression whatever in Hebrew; it is described by the following
words only: baʻal, “he was master”; shakab, “he lay”; laḳaḥ, “he
took”; gillah ʻervah, “he uncovered the nakedness.” Be not misled by
the word yishgalennah (Deut. xxviii. 30), to take it as denoting that
act; this is not the case, for shegal denotes a female ready for
cohabitation. Comp. “Upon thy right hand did stand the maiden”
(shegal) “in gold of Ophir” (Ps. xlv. 10). Yishgalennah, according to
the Kethib, denotes therefore “he will take the female for the
purpose of cohabitation.”

We have made in the greater part of this chapter a digression from

the theme of this treatise, and introduced some moral and religious
matter, although they do not entirely belong to the subject of this
treatise, but the course of the discussion has led to it.

[Contents]
 CHAPTER IX
The corporeal element in man is a large screen and partition that
prevents him from perfectly perceiving abstract ideals; this would be
the case even if the corporeal element were as pure and superior as
the substance of the spheres; how much more must this be the case
with our dark and opaque body. However great the exertion of our
mind may be to comprehend the Divine Being or any of the ideals,
we find a screen and partition between Him [265]and ourselves. Thus
the prophets frequently hint at the existence of a partition between
God and us. They say He is concealed from us in vapours, in
darkness, in mist, or in a thick cloud; or use similar figures to
express that on account of our bodies we are unable to comprehend
His essence. This is the meaning of the words, “Clouds and darkness
are round about Him” (Ps. xcvii. 2). The prophets tell us that the
difficulty consists in the grossness of our substance; they do not
imply, as might be gathered from the literal meaning of their words,
that God is corporeal, and is invisible because He is surrounded by
thick clouds, vapours, darkness, or mist. This figure is also expressed
in the passage, “He made darkness His secret place” (Ps. xviii. 12).
The object of God revealing Himself in thick clouds, darkness,
vapours, and mist was to teach this lesson; for every prophetic
vision contains some lesson by means of allegory; that mighty
vision, therefore, though the greatest of all visions, and above all
comparison, viz., His revelation in a thick cloud, did not take place
without any purpose, it was intended to indicate that we cannot
comprehend Him on account of the dark body that surrounds us. It
does not surround God, because He is incorporeal. A tradition is
current among our people that the day of the revelation on Mount
Sinai was misty, cloudy, and a little rainy. Comp. “Lord, when thou
wentest forth from Seir, when thou marchedst out of the field of
Edom, the earth trembled, and the heavens dropped water” (Judges
v. 4). The same idea is expressed by the words “darkness, clouds,
and thick darkness” (Deut. iv. 11). The phrase does not denote that
darkness surrounds God, for with Him there is no darkness, but the
great, strong, and permanent light, which, emanating from Him,
illuminates all darkness, as is expressed by the prophetic simile,
“And the earth shined with His glory” (Ezek. xliii. 2).

[Contents]
 CHAPTER X
The Mutakallemim, as I have already told you, apply the term non-
existence only to absolute non-existence, and not to the absence of
properties. A property and the absence of that property are
considered by them as two opposites, they treat, e.g., blindness and
sight, death and life, in the same way as heat and cold. Therefore
they say, without any qualification, non-existence does not require
any agent, an agent is required when something is produced. From
a certain point of view this is correct. Although they hold that non-
existence does not require an agent, they say in accordance with
their principle that God causes blindness and deafness, and gives
rest to anything that moves, for they consider these negative
conditions as positive properties. We must now state our opinion in
accordance with the results of philosophical research. You know that
he who removes the obstacle of motion is to some extent the cause
of the motion, e.g., if one removes the pillar which supports the
beam he causes the beam to move, as has been stated by Aristotle
in his Physics (VIII., chap. iv.); in this sense we say of him who
removed a certain property that he produced the absence of that
property, although absence of a property is nothing positive. Just as
we say of him who puts out the light at night that he has produced
darkness, so we say of him who destroyed the sight of any being
that he produced blindness, although darkness and blindness are
negative properties, and require no agent. [266]In accordance with
this view we explain the following passage of Isaiah: “I form the
light and create (bore) darkness: I make peace, and create (bore)
evil” (Isa. xlv. 7), for darkness and evil are non-existing things.
Consider that the prophet does not say, I make (ʻoseh) darkness, I
make (ʻoseh) evil, because darkness and evil are not things in
positive existence to which the verb “to make” would apply; the verb
bara “he created” is used, because in Hebrew this verb is applied to
non-existing things, e.g., “In the beginning God created” (bara),
etc.; here the creation took place from nothing. Only in this sense
can non-existence be said to be produced by a certain action of an
agent. In the same way we must explain the following passage:
“Who hath made man’s mouth? or who maketh the dumb, or the
deaf, or the seeing,” etc. (Exod. iv. 11). The passage can also be
explained as follows: Who has made man able to speak? or can
create him without the capacity of speaking, i.e., create a substance
that is incapable of acquiring this property? for he who produces a
substance that cannot acquire a certain property may be called the
producer of that privation. Thus we say, if any one abstains from
delivering a fellow-man from death, although he is able to do so,
that he killed him. It is now clear that according to all these different
views the action of an agent cannot be directly connected with a
thing that does not exist; only indirectly is non-existence described
as the result of the action of an agent, whilst in a direct manner an
action can only influence a thing really in existence; accordingly,
whoever the agent may be, he can only act upon an existing thing.

After this explanation you must recall to memory that, as has been
proved, the [so-called] evils are evils only in relation to a certain
thing, and that which is evil in reference to a certain existing thing,
either includes the non-existence of that thing or the non-existence
of some of its good conditions. The proposition has therefore been
laid down in the most general terms, “All evils are negations.” Thus
for man death is evil; death is his non-existence. Illness, poverty,
and ignorance are evils for man; all these are privations of
properties. If you examine all single cases to which this general
proposition applies, you will find that there is not one case in which
the proposition is wrong except in the opinion of those who do not
make any distinction between negative and positive properties, or
between two opposites, or do not know the nature of things,—who,
e.g., do not know that health in general denotes a certain
equilibrium, and is a relative term. The absence of that relation is
illness in general, and death is the absence of life in the case of any
animal. The destruction of other things is likewise nothing but the
absence of their form.

After these propositions, it must be admitted as a fact that it cannot

be said of God that He directly creates evil, or He has the direct
intention to produce evil; this is impossible. His works are all
perfectly good. He only produces existence, and all existence is
good; whilst evils are of a negative character, and cannot be acted
upon. Evil can only be attributed to Him in the way we have
mentioned. He creates evil only in so far as He produces the
corporeal element such as it actually is; it is always connected with
negatives, and is on that account the source of all destruction and all
evil. Those beings that do not possess this corporeal element are not
subject to destruction or evil; consequently the true work of God is
all good, since it [267]is existence. The book which enlightened the
darkness of the world says therefore, “And God saw everything that
He had made, and, behold, it was very good” (Gen. i. 31). Even the
existence of this corporeal element, low as it in reality is, because it
is the source of death and all evils, is likewise good for the
permanence of the Universe and the continuation of the order of
things, so that one thing departs and the other succeeds. Rabbi Meir
therefore explains the words “and behold it was very good” (tob
me’od); that even death was good in accordance with what we have
observed in this chapter. Remember what I said in this chapter,
consider it, and you will understand all that the prophets and our
Sages remarked about the perfect goodness of all the direct works
of God. In Bereshit Rabba (chap. i.) the same idea is expressed thus:
“No evil comes down from above.”
[Contents]
 CHAPTER XI
All the great evils which men cause to each other because of certain
intentions, desires, opinions, or religious principles, are likewise due
to non-existence, because they originate in ignorance, which is
absence of wisdom. A blind man, for example, who has no guide,
stumbles constantly, because he cannot see, and causes injury and
harm to himself and others. In the same manner various classes of
men, each man in proportion to his ignorance, bring great evils upon
themselves and upon other individual members of the species. If
men possessed wisdom, which stands in the same relation to the
form of man as the sight to the eye, they would not cause any injury
to themselves or to others; for the knowledge of truth removes
hatred and quarrels, and prevents mutual injuries. This state of
society is promised to us by the prophet in the words: “And the wolf
shall dwell with the lamb,” etc.; “and the cow and the bear shall feed
together,” etc.; and “the sucking child shall play on the hole of the
asp,” etc. (Isa. xi. 6 seq.). The prophet also points out what will be
the cause of this change; for he says that hatred, quarrel, and
fighting will come to an end, because men will then have a true
knowledge of God. “They shall not hurt nor destroy in all my holy
mountain: for the earth shall be full of the knowledge of the Lord, as
the waters cover the sea” (ibid. ver. 9). Note it.

[Contents]
 CHAPTER XII
Men frequently think that the evils in the world are more numerous
than the good things; many savings and songs of the nations dwell
on this idea. They say that a good thing is found only exceptionally,
whilst evil things are numerous and lasting. Not only common people
make this mistake, but even many who believe that they are wise.
Al-Razi wrote a well-known book On Metaphysics [or Theology].
Among other mad and foolish things, it contains also the idea,
discovered by him, that there exists more evil than good. For if the
happiness of man and his pleasure in the times of prosperity be
compared with the mishaps that befall him,—such as grief, acute
pain, defects, paralysis of the limbs, fears, anxieties, and troubles,—
it would seem as if the existence of man is a punishment and a
great evil for him. This author commenced to verify his opinion by
counting all the evils one by one; by [268]this means he opposed
those who hold the correct view of the benefits bestowed by God
and His evident kindness, viz., that God is perfect goodness, and
that all that comes from Him is absolutely good. The origin of the
error is to be found in the circumstance that this ignorant man, and
his party among the common people, judge the whole universe by
examining one single person. For an ignorant man believes that the
whole universe only exists for him; as if nothing else required any
consideration. If, therefore, anything happens to him contrary to his
expectation, he at once concludes that the whole universe is evil. If,
however, he would take into consideration the whole universe, form
an idea of it, and comprehend what a small portion he is of the
Universe, he will find the truth. For it is clear that persons who have
fallen into this widespread error as regards the multitude of evils in
the world, do not find the evils among the angels, the spheres and
stars, the elements, and that which is formed of them, viz., minerals
and plants, or in the various species of living beings, but only in
some individual instances of mankind. They wonder that a person,
who became leprous in consequence of bad food, should be afflicted
with so great an illness and suffer such a misfortune; or that he who
indulges so much in sensuality as to weaken his sight, should be
struck with blindness! and the like. What we have, in truth, to
consider is this:—The whole mankind at present in existence, and a
fortiori, every other species of animals, form an infinitesimal portion
of the permanent universe. Comp. “Man is like to vanity” (Ps. cxliv.
4); “How much less man, that is a worm; and the son of man, which
is a worm” (Job xxv. 6); “How much less in them who dwell in
houses of clay” (ibid. iv. 19); “Behold, the nations are as a drop of
the bucket” (Isa. xl. 15). There are many other passages in the
books of the prophets expressing the same idea. It is of great
advantage that man should know his station, and not erroneously
imagine that the whole universe exists only for him. We hold that
the universe exists because the Creator wills it so; that mankind is
low in rank as compared with the uppermost portion of the universe,
viz., with the spheres and the stars; but, as regards the angels,
there cannot be any real comparison between man and angels,
although man is the highest of all beings on earth; i.e., of all beings
formed of the four elements. Man’s existence is nevertheless a great
boon to him, and his distinction and perfection is a divine gift. The
numerous evils to which individual persons are exposed are due to
the defects existing in the persons themselves. We complain and
seek relief from our own faults; we suffer from the evils which we,
by our own free will, inflict on ourselves and ascribe them to God,
who is far from being connected with them! Comp. “Is destruction
his [work]? No. Ye [who call yourselves] wrongly his sons, you who
are a perverse and crooked generation” (Deut. xxxii. 5). This is
explained by Solomon, who says, “The foolishness of man perverteth
his way, and his heart fretteth against the Lord” (Prov. xix. 3).
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