1 s2.0 S0001868612000620 Main

Advances in Colloid and Interface Science 176 177 (2012) 1830
Contents lists available at SciVerse ScienceDirect
Advances in Colloid and Interface Science

journal homepage: www.elsevier.com/locate/cis
Soft matter approaches to food structuring

R.G.M. van der Sman
Agrotechnology and Food Sciences Group, Wageningen University & Research, The Netherlands
a r t i c l e
i n f o
Available online 20 April 2012

Keywords:
Food
Soft matter physics
Microstructure
Free volume
Effective temperature
a b s t r a c t
We give an overview of the many opportunities that arise from approaching food structuring from the perspective of soft matter physics. This branch of physics employs concepts that build upon the seminal work
of van der Waals, such as free volume, the mean eld, and effective temperatures. All these concepts aid scientists in understanding and controlling the thermodynamics and (slow) dynamics of structured foods. We
discuss the use of these concepts in four topics, which will also be addressed in a forthcoming Faraday Discussion on food structuring.
2012 Elsevier B.V. All rights reserved.
Contents
1.
Introduction . . . . . . . . . . . . . . . . . . . .
2.
Thermodynamics . . . . . . . . . . . . . . . . .
3.
Concepts for strong driven food materials . . . . . .
4.
Self assembly . . . . . . . . . . . . . . . . . . .
5.
Jamming and slow dynamics . . . . . . . . . . . .
6.
Application of soft matter concepts in food structuring
7.
Conclusions . . . . . . . . . . . . . . . . . . . .
Acknowledgments . . . . . . . . . . . . . . . . . . .
References . . . . . . . . . . . . . . . . . . . . . . .
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1. Introduction
Because of the perceived benets of this approach in understanding
the behavior of complex materials, food researchers are applying the
principles of soft matter physics to food structuring [13]. Their activities receive increasing attention from the eld of soft matter physics,
as indicated by a growing number of food related papers in the highimpact journal Soft Matter. To give this growing eld a good exposure
to food scientists, and also to expose physicists to the rich complexity
of food, a Faraday Discussion will be held at Wageningen University in
2012 (www.rsc.org/FD158). With this review paper we aim to provide
a thorough introduction to concepts from soft matter physics as recently introduced into the eld of food science. Furthermore, we will list the
known applications of these concepts in the food science literature, and
potential future applications. We target this review at scientists from either food science or soft matter physics, who are unaware of the work
from the other eld. We hope that the food scientists are encouraged
E-mail address: ruud.vandersman@wur.nl.

0001-8686/$ see front matter 2012 Elsevier B.V. All rights reserved.
doi:10.1016/j.cis.2012.04.002
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18
19
20
21
22
23
25
26
26
to examine the potential of this relatively novel branch of physics [4],

and that they discover its ability to provide a better understanding of
the thermodynamics and dynamical behavior of complex food materials. Such an understanding will aid them in the design and control of
food structuring processes. Also, we hope this review challenges soft
matter physicist and colloids scientists to delve into the seemingly complex world of food materials. We will show that this complex material is
amendable to the tools of their trade.
Soft matter is a complex uid having dispersed, mesoscopic structures, such as gas bubbles, colloidal particles, emulsion droplets, amphiphiles or polymers. The length scale of these mesoscopic structures is in
the order of microns. It happens that this size is similar to the length
scale that humans can sense with the tongue, and thus often sets the
scale for structured foods. Soft matter physicists approach such diversity and complexity by coarse graining, i.e. they ignore chemical details at
the molecular scale up to the level that similarities in the physical behavior emerge. By doing so, the physicist still keep to the principles of
thermodynamics [4,5]. For a description of these similarities they regularly borrow theories and concepts from other branches of physics, such
as the, quite mature, liquid state theory.
R.G.M. van der Sman / Advances in Colloid and Interface Science 176 177 (2012) 1830
At the mesoscale and beyond, the properties of (edible) soft

matter are largely independent of the chemical details of its constituents, which is due to the large separation of the length scales of the
mesoscopic structures and the chemical moieties at the molecular
scale. The results of this makes the interactions at the mesoscale to be
dominated by entropy rather than by chemical bonds. This also makes
the material much more susceptible to externally applied elds, such
as mechanical stress. This gives the materials their soft appearance.
The mesoscopic structures are best characterized by coarse-grained
properties such as size, exibility and amphiphility. Using these properties it is shown that all classical soft matter systems are part of one continuum of systems [5], which is illustrated in Fig. 1. This classication is
one of the examples of how physicists try to nd universality in soft
matter.
A seemingly universal trait of the physicist is to view everything as
a hard sphere. Though, it is often regarded as oversimplistic it has
proven to be a valuable instrument in the quest for universality in
physics. An example of the use of the hard sphere concept is shown
in Fig. 2, where mesoscale structures are disguised as hard spheres.
This illustrates the universality of the jammed state of various kinds
of soft matter [6]. In the jammed state the mesoscale structures
form a percolating network, which is immobilized. In food science,
the jammed states are well studied, but are better known as the glassy
state or the gel state.
Our daily food is extremely rich in types of soft matter [1,2], and
often contains mixtures of various mesoscale building blocks, as
shown in the CSLM images in Fig. 3. Ice cream is an extreme case,
and contains air bubbles, fat crystals, casein micelles, ice crystals, all
embedded in a sugar solution. The multitude of mesoscopic objects
available for foods, offer them seemingly unlimited possibilities for
their structuring [3]. The focus of the coming Faraday discussion will
be food structuring, which we will also take as the guiding line in
the discussion of soft matter concepts.
Food structuring processes can often be divided into 3 steps: 1) destruction of native structures or raw food materials, 2) creation of new
food structures, 3) the arrest of the structured food in a jammed state,
as discussed in detail in our review paper in Soft Matter [3]. For the purpose of this review, we consider that there are two basic, different ways
of organizing food microstructure, via 1) self-assembly of specically
designed building blocks, or 2) non-equilibrium structure formation
by strong external elds [3].
After bringing food materials into the arrested state, they are
thought to be shelf stable. However, frequently they are prone to slow
deterioration of the structure, as evident in the staling of bread crumb
Fig. 1. Various kinds of soft matter can be arranged in a triangle, showing there is a continuum in dispersed phases, which can be characterized by size, exibility, and amphiphility.
The gure is taken from [5], by courtesy of Springer Verlag.
19
(which is arrested in the gel state), and the growth of ice crystals in
ice cream during storage. These processes are examples of what soft
matter physicists call slow dynamics, for which a universal theory is
currently developing [7].
Finally, food structure is broken down again when humans consume their food. The destruction starts in the mouth [8,9], and is completed in the digestive tract, where it is broken down to molecular
building blocks, which can be absorbed by the human intestines
[10,11]. Recently, novel food structures have been created, which are
designed as controlled release vehicles [12], which should be broken
down at certain locations in the human digestive tract. Hence, destruction of food structure is becoming an important research direction, because of its implications for bioavailability of the functional
ingredients present in foods, and also in the more sustainable use of
raw agricultural materials, providing us the building blocks for food
structure [1315].
Below we will discuss concepts and theories from the eld of soft
matter physics, that are relevant to food structuring, of which we especially focus on a) structuring via self-assembly or strong driving
external elds, b) (un)jamming of the food structure, and c) slow
dynamics near or in the arrested state. The destruction of the food
structure as in digestion can be viewed as unjamming or controlled
disassembly, and will be discussed in context of jamming, or self assembly. An overview of the discussed soft matter concepts for the
above mentioned topics is shown in Table 1. To keep this review concise, we have been selective in the number of concepts. The selection
is driven not only by personal experience, but also by whether the
concepts build upon the seminal work of van der Waals. Hence, we
refrain from discussing mechanical and rheological properties of
food matter. The discussed concepts have found wide application in
soft matter physics due to their universal traits, and apply to multiple
topics in the eld of food structuring, as indicated in Table 1.
2. Thermodynamics
While physicists have a quite open mind for coarse-graining out
(irrelevant) details, they are quite rigorous in the application of thermodynamics. It must be said that this rigor is often lacking in current
food science. Van der Waals is one of the early champions for the use
of thermodynamics, and particularly the use of the free energy or,
equivalently, the equation of state. In his famous equation of state,
van der Waals introduced concepts that are still extensively used in
the eld of soft matter, namely: free volume and the mean eld [16].
These concepts are derived by splitting the interaction between molecules into a strong short-range repulsive force, and a weak long-range
attractive force. The repulsive forces determine the free volume,
which is equal to that part of the volume of a system, where new particles can be inserted. Free energy is to be formulated in terms of the
effective volume of the free volume, rather than the total volume. The
effect of attractive forces between particles can be captured with a
(negative) internal pressure, which is added to the actual pressure
eld, to make it an effective pressure or mean eld. With these effective volumes and pressures van der Waals reformulated the equation
of state of an ideal gas as: peffVeff = nRT.
The free volume of a hard sphere suspension is shown schematically in Fig. 4, where the free energy is purely determined by the free volume (in the absence of attractive forces the mean eld is zero). The
free volume of a hard sphere suspension can be computed using the
Widom insertion method or experimentally via confocal microscopy
[18,17]. In Fig. 4 the free volume is indicated by the gray area. Observe
that around each particle there is an excluded volume, where one
cannot insert new particles which is an effect due to the nite size
of particles. The equation of state, obtained for a monodisperse suspension, agrees with the empirical relation by Carnahan and Starling.
Using the free volume concept one can predict the phase behavior of
strong asymmetric bidisperse suspensions, which phase separate via
20
Fig. 2. Various dispersed phases of soft matter can approximated as a hard sphere, and be viewed as a soft glass, having a percolated network in the arrested state.
Figure is taken from [6], by courtesy of RSC.
so-called depletion interaction [19]. Next to thermodynamic properties, free volume also determines transport properties if the system
is near the jammed state [20], as we will discuss below.
After its introduction by van der Waals, other physicists have generalized the concept of the mean eld. A mean eld theory replaces
the interaction between elements in the system by the interaction of
a single element with an effective eld, which is the sum of the external eld and the internal eld. Mean eld theories have been developed for ferri-magnetism by Weiss, for alloys by Bragg and Williams,
and for superconductors by Ginzburg and Landau. Building on these
theories for condensed matter, mean eld theories have been developed also for soft matter, for example by Flory and Huggins for polymers, and by de Gennes for liquid crystals. A detailed discussion of
free energy functionals for various soft matter systems building on
mean eld theory can be found in ref. [21].
Building on the van der Waals picture of a liquid, the liquid state
theory has been further extended [22]. Central to the liquid state theory is the pair distribution function, describing the structure of the
uid. This function is mainly determined by the repulsive part of the
particle interaction. The attractive part of the particle interaction can
be handled as a perturbation of the hard sphere uid. As interactions
between colloidal particles often show similar characteristics as the

interactions between molecules of simple liquids, liquid state theory
is often applied to these colloidal systems [23]. Via generalization of
the van der Waals equation of state, several authors derive the free
volume from the pair distribution function [2426].
3. Concepts for strong driven food materials
Food structuring often requires processing involving intensive
ow, heat and mass transfer [27,28,3]. Hence, in these cases food can
be perceived as strongly driven soft matter. The strong driving is
often combined with phase transitions to induce novel structures.
The driving signicantly modies these phase transitions, and can be
viewed from the framework of non-equilibrium thermodynamics
a eld which is still under active development, even for more common
place soft matter systems [29]. However, in the eld of soft matter
novel concepts have already been deduced, which can be very useful
to food processing.
Studies of driven soft matter may have the strongest link to the
traditional approaches applied to food processing. Food engineers receive a training, which is quite similar as that of chemical engineers.
Fig. 3. Examples of food structures, from left to right: ice cream, yogurt and cheese. Pictures were obtained by CSLM, with uorescent dyes coloring fats (green) and proteins (red).
Figure is taken from [3], by courtesy of RSC.
Table 1
Soft matter concepts used in the discussion topics.
Topic
Driven soft
matter
Self assembly
Directed
assembly
Free energy
Generalized balance eq.
Phase/state diagram
Mean eld theory
Free volume
x
x
x
x
x
x
x
x
x
x
x
Soft glasses
x
x
x
x
Consequently, they tackle problems in food processing via solving the

balance equations for mass, momentum and energy [30]. These equations are of course applicable to strongly driven soft materials, as the
conservation of mass, momentum and energy equally holds for them.
However, the balance equations can be generalized to have a proper
coupling to thermodynamics, so that they have the correct driving
forces for transport and phase transitions. The theory of generalized
balance equations is described in Chaikin and Lubensky [31]. The generalized balance equations encompass 1) a generalized NavierStokes
equation, with an osmotic pressure replacing the conventional hydrostatic pressure, describing the evolution of the velocity eld for the
complete mixture, 2) a generalized convectiondiffusion for the evolution of the volume fraction of the dispersed phase with diffusion
driven by a chemical potential, and 3) the energy balance describing
the change of enthalpy of the mixture. The osmotic pressure and
chemical potential are to be derived from a free energy functional,
which describes the thermodynamics of the soft matter system.
A wide variety of driven (soft) condensed matter systems can be described with this framework of generalized balance equations, such as
polymer blends [32,33], surfactant stabilized emulsions [3437], alloys
[38], granular matter [39], or solutions with liquid crystals [40,41]. For
systems with immiscible phases, like emulsions, it is necessary that
the free energy functional is extended with the square gradient term.
This is yet another concept that has been introduced rst by van der
Waals [4244]. The squared gradient term generates a diffuse interface
between immiscible phases, and complex phenomena like droplet
break-up and moving contact lines then emerge naturally from the
generalized balance equations, if they are properly coupled to the free
energy functional [4547]. The framework of generalized balance
21
equations also captures systems undergoing phase transitions via heat

transfer, such as solidifying alloys [48] or polymer melts [49], evaporating liquidgas systems [50], and drying polymer gels [51].
The governing equations of driven soft matter systems are often
solved using mesoscale simulation methods [5255], which are frequently part of a multiscale simulation framework [5658]. In mesoscale
simulations, the dispersed phases of soft matter are fully resolved on the
computational grid. Often they are represented as hard spheres [59], or
represented via a continuous phase eld having surface free energy
modeled by the square gradient term in the free energy functional [42].
Strongly driven systems appear to defy classical thermodynamics, as
shown by the fact that phase transitions are inuenced by strong shear
elds which is not captured by classical thermodynamics. For several
phenomena, it appears that they t into the framework of classical thermodynamics via the denition of an effective temperature [60].
The concept of effective temperature has been introduced rst for
driven (uidized, vibrated or sheared) granular matter. It is taken to
be linear with the kinetic energy of the velocity uctuations of particles
induced by the driving [61]. For sheared granular matter the effective
temperature is quadratic in the shear rate, T eff _ 2 . The governing equations for granular matter have a strong resemblance to those of classical
thermodynamics. The only difference is that the classical temperature
replaced by the effective temperature.
Subsequently, the concept of the effective temperature has been
introduced for shear-induced melting of (colloidal) crystals [62]. For
small departures from equilibrium the effective temperature scales
quadratically with the shear rate [62,63], while at strong driving
the effective temperature scales linearly with the shear rate, T eff _ 1
[62,64,65]. Shear-induced phase transition can be depicted conveniently in a non-equilibrium phase diagram, using volume fraction and
effective temperature as state variables. At high volume fractions and
high effective temperatures the non-equilibrium phase diagram also
shows a re-entrant solid phase probably induced by shear-thickening.
An effective temperature has also been dened for sheared granular
media and emulsions [66], which is probably related to free volume
[6769]. These systems often show shear-banding, as well as having a
yield stress. If sheared, they show coexisting jammed state and owing
states which are governed by both temperature and hydrodynamic
uctuations.
Recently, we have shown the applicability of the effective temperature concept to strongly sheared suspensions conned to small channels,
or concentrated in a boundary layer in the crossow microltration process [65]. Via this denition of the effective temperature, these strongly
sheared suspensions can also be described by the above generalized balance equations.
In pharmacy a frequently used method of manipulation of phase
transitions is ball milling. Recently, it is shown that ball milling is also
amenable to the concept of effective temperature [70]. In food science
ball milling is also occasionally investigated, where it has shown the
change of phase transitions in starchy powders [71,72].
4. Self assembly
Fig. 4. Free volume in a suspension of hard spheres. Black indicated the volume occupied
by the hard spheres, white indicates the excluded volume the center of other hard cannot
enter, and the gray area represents the free volume.
The gure is taken from [17], by courtesy of Nat. Ac. Sci.
Under certain conditions some mesoscopic structures present in

soft matter can self assemble. Requirements for self assembly are
that the structural elements have sufciently weak (non-covalent)
attractive interactions, and that the interaction leads to more ordered
state [73]. Often the structural elements have some degree of asymmetry, for example in shape or hydrophilic properties, such as hard
rods or amphiphilic molecules, which enables the existence of an ordered, self-assembled state [74]. Often, self assembly can only occur,
if there is a balance between repulsive and attractive forces. The
interaction has to be weak enough such that (thermal) uctuations
allow the elements to adjust their position and orientation, to attain
the more favorable self-assembled conguration. If the uctuations
are too weak, or the interactions too strong (irreversible), it is more
likely that the system ends up in an arrested state. The structural elements can self assemble in the bulk solution like a crystal, or they can
assemble at an interface between immiscible phases. Classical examples of self assembling systems are liquid crystals, surfactants, ber
suspensions, and binary colloid suspensions with strong size asymmetry. The constraint of the reversibility of the interactions sets a
limit to the size of the structural elements.
Self assembly has many similarities with crystallization, and many
tools from (soft) condensed matter physics can be applied; such as the
phase diagram and group theory [73]. Phase diagrams have been
obtained theoretically for liquid crystals, block copolymers and surfactant systems using free energy functionals. These functionals are
based on orientational order parameters, which express the topology
of the system rather than the chemical details similar to other
kinds of soft matter [7578].
For binary suspensions containing hard objects, with strong asymmetry in size or shape, the interactions are purely entropic [79]. Consequently, the free energy functional can be described in terms of free
volume [19]. These theories, developed for classical self assembling
systems, show that the geometry of the structural elements is important. Furthermore, they have provided insight into the universality of
self assembled phases [73], which can be used for more complex self
assembling systems like polysoaps, patchy colloids, synthetic DNA
and proteins [8082]. These modern self assembling systems are
approached theoretically using numerical tools developed earlier for
the classical soft matter systems, such as Brownian Dynamics, Dissipative Particle Dynamics, Self Consistent Field theory or the related
Dynamic Density Functional theory [8386].
In addition to the above described equilibrium self assembly,
ordered states of soft matter can also be obtained via directed (self)
assembly, which is facilitated by external templates and elds such
as a shear ow or electric eld [87]. These dissipative structures are
formed via a constant supply of energy. Therefore, their thermodynamic description closely resembles that of strongly driven soft matter systems, described above. The manufacturing of colloidal particles,
delivery vehicles and emulsion droplets with microuidic devices is
also viewed as an example of directed assembly [88,89].
Directed assembly via templating can be achieved via coacervation. Coacervation is a liquidliquid phase transition in a solution of
polyelectrolytes, where oppositely charged polyelectrolytes undergo
associative interactions [9092]. An example of a system showing
this kind of behavior is a mixture of proteins and pectins. If the protein
is rst absorbed at the interface of emulsion droplets, they function as
a template for pectin which binds to the proteins as in a coacervate.
Pectin can bind proteins again, and consequently multiple layers can
be deposited. Via this multilayer deposition microspheres for controlled release purposes can be created [9395].
For controlled release of functional ingredients in the digestive
tract, directed disassembly is often required [9698]. Via (enzymatic)
cleaving of proteins, the amphiphilic properties can be altered and
the self assembled state is not favored. The conformation of proteins
can also be changed by altering the pH or ionic strength. The size,
shape and surface hydrophobicity of the proteins are changed and
can lead to controlled disassembly.
function. Of course, the concept of caging has strong similarities with

the free volume concept. Via the caging, a jammed system remains
out of equilibrium, and its state cannot be described by a free energy
functional or phase diagram. The jammed state can often be correlated
to a certain temperature for a given composition. Hence, the jammed
state is often represented together with phase transitions in a state
diagram. Liu and Nagel [99] have generalized the jammed state to
various soft matter systems. They have represented this with the
jamming state diagram, which is reproduced in Fig. 5. The jammed
state diagram also shows alternative routes to unjam the soft glasses
[100,101]. If the system is arrested via cooling, it can be unjammed
via shear or dilution. Also gels are viewed as jammed systems, and
they can be unjammed via application of shear or pressure [102]. The
unjamming of gels is often thought of as failure or collapse of the
structure.
The primary relaxation mode is related to translation of the dispersed phase (or molecule/chain in case of hard glasses). The primary
mode determines physical properties like viscosity and mobility,
which is the inverse of diffusivity. These relaxation modes diverge at
the glass transition temperature Tg, meaning that translation of the
disperse phase is immobilized. Many glassy systems also show secondary or beta relaxation modes. They are relatively faster than the
primary (alpha) relaxation mode, and therefore they can persist at
temperatures below the glass transition. In the case of polymers the
secondary relaxations are associated with rotational and vibrational
modes. Key features of the slow dynamics are spatial and dynamical
heterogeneity, and the slow dynamics is driven by stress relaxation.
The slowly (primary) relaxing physical properties often show stretched
(Kohlrausch Williams Watts) exponential behavior [7].
Only a few universal theories exist for describing the slow dynamics
of (soft) glasses, such as free volume theory [103], Gibbs-diMarzio
[104], and Mode Coupling Theory (MCT) [105]. None of them is totally
satisfactory, and they explain only part of the observed phenomena.
All these theories are semi-empirical and they often break down at
temperatures far above the glass transition. For soft glassy materials
the Mode Coupling Theory is most often employed. MCT predicts the
existence of primary and secondary relaxation modes, with the former
showing stretched exponential behavior. However, it predicts the
divergence of primary relaxation at a cross-over temperature Tc. It has
been found that the cross-over temperature is often different from
Liquid
Jammed
max
5. Jamming and slow dynamics

Close to the jammed state many systems of (soft) condensed matter exhibit slow relaxation phenomena with quite universal traits [7].
This universal behavior has been called slow dynamics, and the soft
matter systems showing this behavior are named soft glassy materials.
The systems are in the jammed state because the thermal uctuations are too small to sample the equilibrium state. The dispersed elements of the soft matter cannot escape the cage formed by the other
surrounding dispersed elements. The signature of the occurrence of
caging is the growth of the primary peak in the pair distribution
T / Tg
22
Fig. 5. Jamming state diagram, with axes indicating volume fraction , temperature T,
and stress . Systems get jammed if these state variables crosses a critical value, as indicated on the axes by the random close packing max, the glass transition temperature
Tg, and the yield stress .
The gure is taken from [3], by courtesy of RSC.
experimentally observed glass transition, Tc 1.2Tg. In the regime of

Tc b T b Tg MCT often fails to explain experimental relaxation phenomena [7], as observed in viscosity and diffusivity for example. Various
extensions of MCT have been proposed to explain the phenomena in
this range [106]. In this regime free volume theory also offers semiempirical explanations for the observed behavior of viscosity and diffusion [103,107].
Slow dynamics is also shown for soft glassy systems under shear,
which is described by Soft Glassy Rheology [108]. The shear eld provides hydrodynamic uctuations via which the system can sample
states with a lower free energy. An effective temperature is taken as
a measure for these uctuations. The concept of effective temperature
is expected to describe quantitatively the slow dynamics and aging of
soft glassy materials [7]. However, experimentally it is still difcult to
determine the effective temperature, and often experiments yield
contradictory results. The effective temperature is related to the local
stress [109]. A similar statement is found above for strongly driven
soft matter. The fact, that slow dynamics is dominated by stress relaxation, strengthens the plausibility of the hypothesis that the effective
temperature is linear with the local stress.
Via combining Soft Glassy Rheology with effective medium theory,
it has been shown that the viscosity of soft glassy materials shows similar behavior to hard glasses [110]. For glasses, the viscosity diverges at
the glass transition Tg, as follows from the free volume theory [103]. Effective medium theory is a kind of mean eld theory, which states that
physical properties of a mixture can be obtained from theories considering a single particle immersed in a uid. In the effective medium theory the uid obtains properties equal to those of the mixture. Often, the
problem has to be solved in a self-consistent way. Effective medium
theory has been applied successfully to predict the viscosity of hard
sphere suspensions, using the Einstein theory of dilute suspensions
[111]. The celebrated KriegerDoghourty relation for suspension viscosity is derived via effective medium theory, which states that the viscosity diverges at random close packing volume fraction [112114]. Both
free volume theory and the KriegerDoghourty relation for viscosity
of hard sphere suspension are also related to free volume [115]. Both
theories state that the viscosity diverges if the free volume reaches a
critical value.
Recently, slow dynamics has been observed in living matter, namely
the cytoskeleton commonly referred to as active gels [116,117]. As
these active gels constantly require input of energy (ATP), the distinction between directed self assembling systems, strongly driven systems
and soft glassy systems becomes somewhat blurred [118]. Also, for active gels, the effective temperature concept has been proposed [119].
Other phenomena illustrate the fuzziness of the boundaries between soft glassy materials and strongly driven soft matter systems.
These are for example, viscoelastic phase separation [120] and shear
induced migration [65].
Viscoelastic phase separation occurs in mixtures having strong
asymmetry in viscoelastic properties of the mixed components, which
is satised by many soft matter systems. Viscoelastic phase separation
leads to the formation of a transient network (gel) of the dispersed
phase, under the constraints of sufciently strong attractive interactions, and sufcient concentration of the dispersed phase. The transient
network exhibits quite slow dynamics. In the case of asymmetric polymer blends, viscoelastic phase separation is described by the generalized balance equations as used for strongly driven soft matter systems
[121].
Shear induced migration occurs in pressure driven hard sphere
suspensions, conned in narrow ow channels [122]. Hydrodynamic
interactions between particles give rise to an osmotic pressure [123],
which is linear with the local shear stress, and which can be viewed
as an effective temperature [65]. In narrow ow channels there are
gradients in the shear stress, which lead to gradients in the osmotic
pressure. These gradients are relaxed via particle migration towards
the center of the ow channel. Shear induced migration is solved
23
using generalized balance equations, as with other driven soft matter

systems. The particle migration is shown to be a kind of diffusive behavior [124], which takes place at much slower time scales as hydrodynamics. Hence, shear induced migration might also be termed as
slow dynamics. This slow dynamics is also described by an effective
temperature, which is linear with the local stress. The local stress is
linear with the suspension viscosity, for which expressions derived
via effective medium theory show best correspondence with empirical relations for shear induced diffusivity [65].
6. Application of soft matter concepts in food structuring
In the above topics in food structuring processes, we have discussed
repeatedly various soft matter concepts, which have been found useful
in the theoretical description of relevant physical phenomena. These recurring concepts we have listed in Table 1. Below, we discuss in how far
these concepts have been used already in the eld of food science. Furthermore, we indicate novel problems for which the soft matter concepts are expected to have a large added value.
As an indication of the use of soft matter concepts in food science,
we have classied the papers, published by food scientists in the Soft
Matter journal, in Table 2. This shows that the most investigated
topic is self-assembly, which is driven by 1) the interest in the correct
delivery of functional ingredients in the digestive tract, and 2) the
quest for food structures having less fat, but with similar functionality.
Thermodynamics and jammed systems receive moderate interest,
while driven systems and directed assembly are the least investigated
topics. Furthermore, observing the list of principal investigators following the soft matter approach in Table 3, one nds that they are not
evenly spread over the globe. We nd they are concentrated in a small
number of sites, namely Wageningen University and Research, ETH in
Zurich, Birmingham and Leeds in England, Guelph University, the research institutes NIZO and IFR, and the multinationals Unilever and
Nestle. Most sites are specialized in certain topics, while Wageningen
and the multinationals are more diverse, which is likely due to their size.
Due to the specic drivers for the above mentioned food research,
the physics of many food systems under investigation is quite novel to
the main-stream research in Soft Matter physics. Below, we will discuss the typical nature of various food systems, with the objective of
raising the interest of these main-stream physicists in food materials.
Under the topic of self-assembly, food scientists are trying to create
microspheres that are able to function as controlled delivery vehicles
[139]. These microspheres are self-assembled via absorption of foodgrade colloids onto the interface of emulsion droplets. Controlled delivery can then happen in the digestive tract, via the disassembly of the
colloid layer on the interface [10]. This can be done via change in pH
(changing conformation of proteins), enzyme activity or displacement
of colloids by (bile) surfactants. Another major theme in self-assembly
is organogels, whose primary function is to replace gels formed by fat
crystal networks as present in fatty food products like butter, margarine and bakery doughs [138].
The topic of thermodynamics is found typically in studies investigating biopolymer mixtures, which are also termed water-in-water
emulsions. These systems consist of solutions of proteins with polysaccharides, that are phase separated [178]. The driver for these studies is again the quest for low-fat food materials, but now having a
Table 2
Food studies taking soft matter approach, sorted according to topics.
Topic
References
Thermodynamics
Self assembly
Directed (Dis)assembly
Driven systems
Jammed systems
[94,125129]
[130,10,131139]
[140,11,141,142]
[143,65,144,145]
[146151,6,152]
24
Table 3
Principal investigators taking a soft matter approach to Food.
Name
Address
Topics
Ref.
Aken
Bakalis
Boom
NIZO/Wageningen, Food
Birmingham, Food
Wageningen, Food
[126]
[143]
[141]
Bot
Brady
Callaghan
Cohen-Stuart
Unilever, Food
Cornell
MacDiarmid, Physics
Wageningen, Food
de Kruif
Dickinson
Utrecht, Physics/NIZO
Food
Leeds, Food
Disassembly/emulsions
CFD, driven systems
Driven systems/directed
assembly
Organogels/self assembly
MD sugars
NMR/MRI/rheology
physical chemistry
proteins
Dairy colloids
[94]
Dutcher
Ettelaie
Euston
Fisher
Foegeding
Frith
Fryer
Garti
Guelph, Physics
Leeds, Food
Edinburgh, Food
ETH, Food
North-Carolina, Food
Unilever, Food
Birmingham, Food
Hebrew
Groot
Gunning
Hartel
Hermansson
Unilever, Food
IFR, Food
Wisconsin
SIK/Food
Horne
Leermakers
Leser
Limbach
Livney
Marangoni
Mayama
McClements
Meinders
Mezzenga
Michel
Mitchell
Moldenaers
Hannah Research Inst.,

Food
Wageningen, Food
Nestle, Food
Nestle, Food
Technion, Food
Guelph, Food
Japan
UMass
Wageningen, Food
ETH, Food
Nestle, Food
Nottingham, Food
Leuven, Physics
Morris
Nicolai
Normand
Norton
IFR, Food
Lemans, Physics
Firmenich, Food
Birmingham, Food
Opheusden
Parker
Rogers
Rousseau
Stokes
Stoyanov
Schurtenberger
Terentjev
Tromp
Tuinier
Turgeon
Wageningen, Food
IFR, Food
Saskatchewan, Food
Toronto, Food
Queensland, Food
Unilever, Food
Friburg, Physics
Cambridge, Physics
NIZO, Food
IFF Juelich, Physics
Lafayette, Food
Ubbink
van der Linden
van der Sman
(formerly) Nestle
Wageningen, Food
Wageningen, Food
Velikov
Vilgis
Wilde
Unilever, Food
MPI Mainz, Physics
IFR, Food
SCF/Brownian dynamics/
scattering
AFM, proteins
Brownian dynamics/SCF
MD proteins
Food rheology
Oral processing
Rheology/soft glasses
Driven systems
Thermodynamics liquid
crystals
Mesoscale simulation
Disassembly/digestion
Crystallization/thermo
Biopolymer mixtures/
driven
Protein molecular
dynamics
SCF
Liquid crystals
Molecular dynamics
Self-assembly
Organogels/fat crystals
Fat crystals
Controlled delivery
Emulsions/foams
SCF simulations
Liquid crystals
Starch
Rheology/biopolymer
mixtures
Polymers/glasses
Protein gels
Glassy dynamics
Oral processing/
destructuring
Brownian dynamics/gels
Polysaccharides
Organogels/fat crystals
Fat crystals
Rheology/soft glasses
Self-assembly/delivery
Scattering techniques
theory, thermodynamics
Driven biopolymers
Soft matter/scattering
Thermodynamics
biopolymers
Glassy systems
Protein self-assembly
Mesoscale simulations/
driven systems
Self-assembly/delivery
Polymers
Digestion
[153]
[154]
[155]
[126]
[156]
[132]
[157]
[158]
[159]
[160]
[161]
[143]
[162]
[163]
[10]
[164]
[149]
[165]
[85]
[166]
[146]
[167]
[168,133]
[125]
[169]
[170]
[1]
[166]
[171]
[172]
[10]
[173]
[174]
[175]
[176]
[140]
[177,133]
[147]
[6]
[128]
[178]
[179]
[180]
[156]
[90]
[2,146]
[181]
[3,58]
[139]
[182]
[11]
creamy texture. The construction of phase/state diagrams has already

a long-standing tradition in food science, but it is often done using
only experimental input [192]. The phase/state diagram is acclaimed
to be a convenient tool for depicting the processing path during food
processing, where phase transitions are used to induce structuring of
the food material [3]. Recently, we have shown that these phase/
state diagrams can be constructed using the thermodynamic theory

of FloryHuggins, complemented with the free volume extension by
Vrentas and Vrentas [189,188].
Also, the investigation of jammed systems, such as glasses of carbohydrates or biopolymers, and gels of proteins, already has considerable
history in food science [227]. These are subjects addressed by food scientists having a background in colloid science. Such systems are also
regularly addressed by soft matter physicists [99]. Also for a long time,
food researchers have been investigating slow dynamics in these systems [236]. However, the theories of soft matter physics are not yet
widely applied but their potential has been appreciated [6]. Food
materials are very rich in phenomena having slow dynamics, which
are hardly investigated by soft matter physicists. Examples of these
slow dynamics are blooming of chocolate [125], retrogradation (recrystallization) of starch [241], and swelling of starch granules [145]. Furthermore, it is expected that many food systems exhibit visco-elastic
phase separation (VPS) [120]. This is a phenomenon quite unknown
to the food science community, given a few exceptions [1,239]. In
some food systems VPS is conned to the two-dimensions of the interface. This happens in self-assembled delivery vehicles, which are disassembled via displacement of proteins by surfactants. The displaced
protein network displays similar characteristics to a transient gel network, a typical signature of VPS [94].
As stated in Table 2 directed assembly or structuring via strong
driving is still minor subjects of investigation. However, the investigated
systems are quite non-conventional to the soft matter community. Several directed (dis)-assembly studies involve enzymes, which assemble
via making crosslinks [242], or disassemble via incisions in biopolymers
[11], thereby imparting their stabilizing functionality. Several studies
investigate food structuring using the conning walls of microuidic
devices [141]. Connement can also be used for destructuring, as in
the mouth during eating or in microuidic devices, via which raw food
materials are separated into various functional ingredients [175].
From Tables 2 and 3 we conclude that food research, taking a soft
matter perspective, is gaining momentum. This research addresses
topics that are shared with the mainstream research in soft matter
physics, albeit that their main focus is on systems near equilibrium.
Systems driven far from equilibrium are still a challenge, but highly relevant for food structuring processes. From the literature one also observes that various soft matter concepts, as summarized in Table 1,
are used in the analysis of the phenomena occurring in food structuring
processes. This we have made more explicit in Table 4, where we have
listed in which reference these concepts are used, together with the
food system under investigation and the principal investigator. As already discussed partly above, the use of some concepts has already
some history in food science, like the phase/state diagram, slow dynamics and the generalized balance equations. The concepts of the
state diagram and slow dynamics are in use already for two decades,
due to the early recognition that shelf-stable foods are in the glassy
state [227]. However, it must be said that the analysis of slow dynamics
is largely empirical. The use of the generalized balance equation is due
to the rooting of food engineering in chemical engineering approaches,
where these balance equations are heavily used in the description of
momentum, heat and mass transfer. To make this a proper soft matter
approach, the driven forces in the description of these transport processes have to be linked to a proper description of the thermodynamics
of the food material, as we have done in our recent papers [37,211,65].
The thermodynamics of various food systems is investigated theoretically. However, the community performing this research is quite
different from the one investigating transport phenomena food systems, using balance equations of conserved physical quantities. This
can be seen from the principal investigators listed in Table 4. It is obvious that understanding of food structuring is enhanced if exchange
between these communities is stimulated. Recognizing that the food
material being structured is an example of strongly driven soft matter, the use of soft matter concepts like mean eld theory, free volume
Table 4 (continued)
Table 4
Soft matter concepts applied to food systems.
Topic
System
PI
Ref.
Free energy
Calciumproteins
Microchannel emulsication
Protein solutions
Casein micelles
Casein micelles and
polysaccharides
Protein/polysaccharide
mixtures
Proteins/starch at high
pressure
Meat proteins
Starch
Milk
Proteins
Baking
Waterwater emulsion
Casein/thickener
Microemulsions
High pressure freezing
Liquid crystals/lipids
Starch-based foods
Watersugar solution
Organogels
Surfactant/biopolymer mixture
Gelatin
Starch lms
Maltodextrins glasses
Starch thermodynamics
Water diffusion
Penfold
Nakajima
McClements
Kruif
Tuinier
[183]
[184]
[185]
[156]
[186]
Turgeon
[90]
Heeremans
[187]
van der Sman

van der Sman
Vuataz
Kokini
Guilbert
Tuinier/deKruif
deKruif
Garti
LeBail
Mezzenga
Mitchell
Blond
Bot
McClements
Sobral
Benczedi
Ubbink
van der Sman
Karel/van der
Sman
Seow
Kokini
Kasapis/Mitchell
[188]
[189,190]
[191]
[192]
[193]
[194,195,93]
[196]
[197]
[198]
[199]
[200]
[201]
[202]
[203]
[204]
[205]
[146]
[189]
[206,152]
van der Sman

van der Sman
van der Sman
Datta
Bakalis/Fryer
Saguy
Mizrahi
Fito
LeBail
Dincov
Trystram
Andrieu
Vorobiev
McClements
van der Goot/
Boom
van der Linden
Dickinson
Roos
[65]
[211]
[212]
[28]
[143]
[213]
[214]
[215]
[216]
[217]
[218]
[219]
[220]
[221]
[222]
Slade/Levine
[227]
van der Sman

Agterof
Robins
Vorobiev
Sutton
Rotstein
van der Sman
Frith
[65]
[228]
[229]
[220]
[230]
[231]
[65]
[161]
Sutton
Hemminga
Parker/Noel
Nicolai
Dickinson/
Ettalaie
Ludescher
Noel/Parker
Johari
Dickinson
[230]
[232]
[233]
[173]
[234]
Thermodynamic
theory
Phase/state
diagram
Free volume
Generalized
balance eq.
Non-equil. phase
diagram
Mean eld
theory
Effective
temperature
Slow dynamics
Anti-plasticizing
Biopolymer rheology
Rheology sugar/biopolymer
mixture
Sheared suspensions
Heated meat
Emulsion
Intensively heated food
Heated chocolate
Rehydrated foods
Hydrogels
Osmotic dehydration
Frozen foods
Microwave heating
Baking
Baking
PEF/electroporation tissue
Emulsion/thickener
Directed assembly
high-protein
Gels of protein bers
Gels at high pressure
Polysaccharide/carbohydrate
glasses
Polysaccharide/carbohydrate
glasses
Sheared suspensions
Sheared emulsions
Creaming emulsions
Electroporation
Ice recrystallization
Thermal conductivity
Sheared suspension
Sheared waterwater
emulsions
Ice recrystallization
Maltodextrins
Protein aggregation
Protein gelation/aggregation
Foam disproportionation
Sugar glassy dynamics
Sugar glassy dynamics
Beta-relaxation meat
Viscoelastic phase separation
25
[207]
[208]
[209,210]
[223]
[224]
[225,226]
[235]
[236]
[237]
[238,239]
Topic
System
PI
Ref.
Slow dynamics
Fat crystallization
Starch retrogradation
Dense emulsions
Starov
Blanshard
Wilde
[240]
[241]
[229]
and effective temperature can be advantageous for describing the

thermodynamics and transport coefcients. There are a few examples
of the use of these concepts within food science, which are listed in
Table 4.
Often the complexity of food materials is so rich that the application
of the concepts of soft matter implies the use of advanced simulation
techniques which are also commonly applied in soft matter physics.
The simulation techniques used range from molecular dynamics (MD)
at the molecular microscale, Lattice Boltzmann techniques at the mesoscale of the food structure, to macroscale approaches based on the (generalized) balance equations. These advanced methods often require
quite expert knowledge. Consequently, this implies again a different
community with little exchange with other communities. Again, to
stimulate communication we have listed illustrative examples of the
use of such simulation techniques in Table 5. On occasion multiple
lengthscales present in structured foods are addressed in multiscale
approaches [251].
We believe that there is a huge potential for the soft matter approach in various other problems concerning food structuring. To give
the reader an idea of these potential applications, we have listed them
in Table 6. There we have indicated to which systems several soft matter
concepts might be applied. The listed references indicate studies where
these systems have been investigated or reviewed. As one can observe,
we foresee much potential for concepts from the eld of strongly driven
soft matter. In several food systems shear banding has been observed,
but it has not yet been analyzed using theories for these systems, such
as Soft Glassy Rheology (SGR) or Shear Transition Zones. Mesoscale
simulations with phase eld theory can be used to describe foods
being structured via crystallization, such as chocolate and ice cream.
Protein assembly/aggregation can be described via patchy colloids,
which is an enhancement of the often applied hard sphere representation of colloids. Here, the hard sphere is sticky of several patches on the
surface. These augmented hard spheres can easily be included in mesoscale simulation techniques such as Brownian Dynamics or Lattice
Boltzmann. After having applied free volume theory for describing
moisture sorption in polysaccharides, we have recently investigated
the application of this theory to moisture sorption in proteins [188]
and to moisture diffusion in polysaccharides [20]. Free volume theory
can also be applied to mixtures exhibiting depletion interactions. In
food structuring processes the matter is frequently driven by elds,
which are not commonly applied in soft matter physics, such as electrical elds and high pressure elds. This would make the problems very
attractive for physicists. Theoretical work has yet to be performed, but
analysis by means of qualitative tools as non-equilibrium phase diagram has great potential. Of course, these tools also have potential in
food structuring processes, where material is driven in a more conventional way, namely by shear ow. For shear-driven systems theory is
more developed, where such concepts as effective temperature and effective medium theory can be very helpful.
7. Conclusions
In this review we have shown that the soft matter approach to food
materials is denitely gaining ground in food science, and it also receives
recognition from the eld of soft matter physics. In the different phases
of the food structuring process a multitude of concepts from soft matter
physics can be applied. Surprisingly, many of these universal concepts
build upon the original work of van der Waals. Their universality offers
26
Table 5
Advanced simulation techniques used in the Soft Matter approach to Food.
Scale
Technique
Micro
Molecular
dynamics
SCF
System
Carbohydrates
Protein/Polysaccharide mix
Casein at interfaces
Liquid crystals
Protein/polysaccharide mix
at interface
MonteCarlo
Proteins absorption at
interfaces
Surfactants at interfaces
Bulk protein/polysaccharide
mixtures
Mesoscale Brownian dynamics
Colloids at interfaces
Food gels
Colloids displacement at
interface
Lattice Boltzmann
Emulsions
Suspensions
Macro
Porous media approach Intensively heated foods
Multiscale Cell model + macro
Expanded snacks
Ref.
[154,243,146]
[149]
[244]
[245]
[157]
[246,247]
[158]
[158]
[248]
[176]
[249]
[212]
[250]
[28]
[251]
Table 6
Potential applications of soft matter concepts in food structuring.
Topic
System
Ref.
Shear banding/SGR
Slow dynamics
High protein foods

Yogurt
Fruit pulp
Waterwater emulsions
Foams
Emulsions
Fat/ice crystals
Protein phase diagram
Colloidpolymer systems
Moisture sorption proteins
Moisture diffusion
Electric elds
High-pressure
Sheared rod/colloid suspension
Foams
Shear-induced melting of fat crystals
Starch gelatinization/
Fragmentation in extruders
Shear thinning emulsions
Thermal properties complex uids
[242]
[252]
[253]
[180]
[254]
[255]
[256]
[257,258]
[19]
[259]
[260]
[261]
[262]
[161]
[263265]
[266]
[161]
[267,168,268]
[269271]
[272,273]
[274]
[275,276]
Phase eld simulations

Patchy colloids
Free volume
Driven soft matter

Non-equil. phase diagram
Effective medium theory
good opportunity for improved understanding of the complexity of the

food materials and their structuring processes.
Researchers are performing food research taking a soft matter approach, but they do not form a united community, as they come from
starkly differing disciplines, like soft matter physics, computational
physics, food colloidal science and food engineering. Hence, it is timely to form such a community, which is stimulated via this review, and
the upcoming Faraday Discussion.
Acknowledgments
Hereby, we acknowledge the fruitful discussions with Job Ubbink
on this review. Furthermore, we appreciate the careful reading of the
manuscript by Bill Frith.
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Advances in Colloid and Interface Science 176 177 (2012) 1830

Contents lists available at SciVerse ScienceDirect

Advances in Colloid and Interface Science

Soft matter approaches to food structuring

Available online 20 April 2012

E-mail address: ruud.vandersman@wur.nl.

to examine the potential of this relatively novel branch of physics [4],

At the mesoscale and beyond, the properties of (edible) soft

between colloidal particles often show similar characteristics as the

Consequently, they tackle problems in food processing via solving the

equations also captures systems undergoing phase transitions via heat

Under certain conditions some mesoscopic structures present in

function. Of course, the concept of caging has strong similarities with

5. Jamming and slow dynamics

experimentally observed glass transition, Tc 1.2Tg. In the regime of

using generalized balance equations, as with other driven soft matter

Hannah Research Inst.,

creamy texture. The construction of phase/state diagrams has already

state diagrams can be constructed using the thermodynamic theory

van der Sman

van der Sman

van der Sman

and effective temperature can be advantageous for describing the

High protein foods

Phase eld simulations

Driven soft matter

Effective medium theory

good opportunity for improved understanding of the complexity of the

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