Understanding the transient large amplitude oscillatory shear behavior of

This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
yield stress fluids
Krutarth M. Kamani,1, a) Gavin J. Donley,1, a) Rekha Rao,2 Anne M. Grillet,2 Christine Roberts,2 Abhishek
Shetty,3 and Simon A. Rogers1
1) Department of Chemical and Biomolecular Engineering, University of Illinois at Urbana-Champaign, Illinois,
USA 61801
2) Sandia National Laboratories, New Mexico, Albuquerque, United States
3) Rheology Division, Anton Paar USA, Ashland, VA 23005

(*Electronic mail: sarogers@illinois.edu)

(Dated: 9 December 2022)
A full understanding of the sequence of processes exhibited by yield stress fluids under large amplitude oscillatory
shearing is developed using multiple experimental and analytical approaches. A novel component rate Lissajous curve,
where the rates at which strain is acquired unrecoverably and recoverably are plotted against each other, is introduced
and its utility is demonstrated by application to the analytical responses of four simple viscoelastic models. Using the
component rate space, yielding and unyielding are identified by changes in the way strain is acquired, from recoverably
to unrecoverably and back again. The behaviors are investigated by comparing the experimental results with predictions
from the elastic Bingham model that is constructed using the Oldroyd-Prager formalism and the recently proposed
continuous model by Kamani, Donley, and Rogers in which yielding is enhanced by rapid acquisition of elastic strain.
The physical interpretation gained from the transient LAOS data is compared to the results from the analytical sequence
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of physical processes framework and a novel time-resolved Pipkin space. The component rate figures therefore provide
an independent test of the interpretations of the sequence of physical processes analysis that can also be applied to other
LAOS analysis frameworks. Each of these methods, the component rates, the sequence of physical processes analysis,
and the time-resolved Pipkin diagrams, unambigiously identifies the same material physics, showing that yield stress
fluids go through a sequence of physical processes that includes elastic deformation, gradual yielding, plastic flow, and
gradual unyielding.

I. INTRODUCTION instantaneous yielding process was assumed in addition to in-

A. Yield Stress Fluids and Yielding
Yield stress fluids (YSFs) are soft materials that often de-
form as a viscoelastic solid under small loads and yield and
flow plastically under large applied loads. This combination
of behaviors has a wide range of applications in daily life,
from foods and personal care products to numerous industrial
and environmental processes. A range of systems with a va-
riety of microstructures have been shown to yield including
foams, emulsions, pastes, suspensions of microgels and gran-
ular particles1–13 as well as polymer networks, colloidal gels,
capillary suspensions, and magnetorheological fluids14–22 .
Traditionally, yielding has been described as an abrupt tran-
sition, where it is often assumed that a critical stress must
be exceeded to initiate any plastic flow. This description
is often attributed to Bingham’s original experiments on the
steady flow behavior of concentrated clay suspensions in a se-
ries of capillaries where it was observed that measurable flow
was induced only when a finite pressure, or yield stress, was
exceeded23 .
Early attempts at modeling the behavior of YSFs, such as
those of Bingham, Herschel and Bulkley, and Casson, focused
exclusively on the creation of a flow rule to describe the steady
flowing state24–26 . When applied to transient conditions, an
a) KMK and GJD contributed equally to this work
finitely rigid preyielding behavior. These early attempts were
expanded by the work of Oldroyd, who explicitly modeled
both the unyielded and yielded regimes. Oldroyd proposed
that YSFs behave as an elastic solid when the applied stress
is below the yield stress, and flow plastically above it ac-
cording to the behavior laid out by Bingham27 . This two-
regime behavior has become known as the as Oldroyd-Prager
formalism27–29 . A number of models invoke this formalism
and describe the unyielded solid and yielded viscoplastic be-
haviors with distinct physics27,30,31 . An often overlooked,
yet important point is that Oldroyd specifically intended his
model to describe the quasi-static case that did not include
rapid transience. However, his model, and others that invoke
the same formalism, have been used to describe transient sit-
uations by assuming instantaneous yielding and unyielding
transitions.
The idea of instantaneous yield transition remained unchal-
lenged experimentally until 1985, when Barnes and Walters
famously suggested that yielding was an illusion caused by
data of limited accuracy32 . To determine whether the yield-
ing was a real behavior or a "myth", a range of rheological
protocols were rigorously applied to yielding materials, in-
cluding creep, amplitude sweeps, stress growth, stress relax-
ation, slump, inclined plane avalanche and static equilibrium
tests. The conclusion of this phase of inquiry was that, regard-
less of whether it was actually “real", the yielding transition
should be considered an engineering reality due to its practical
usefulness.33
While many protocols and analyses currently exist to char-

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acterize yielding behavior, different methods can give sub-
stantially different values for “the” yield point34,35 . This
raises the question of which, if any, of these proposed
points are the correct measure of yielding. More fundamen-
tally, it merits consideration of what these quantities phys-
ically represent, and whether a single instantaneous quan-
tity can capture the yielding transition under all flow proto-
cols. This becomes even more pressing when considering
that a number of experimental rheological observations exist
that are fundamentally inconsistent with the idea of instan-
taneous yielding at a specific point. These include multi-
stage transitions, shear localization, and shear banding un-
der uniform stress36–38 . In addition, rheo-structural tests
such as ultrasonic speckle velocimetry39–42 , diffusing-wave
spectroscopy43 , rheo-microscopy44 and rheo-scattering45,46
have reported that irreversible structural rearrangements take
place below the rheological yield stress. The commonality
among these issues is that the yielding transition appears to
occur gradually in time and/or space. The growing accep-
tance that yielding is a gradual transition means that there is
a requirement to be able to study its evolution. The need for
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an instantaneous understanding of yielding is especially im-
portant given that many of the applications of YSFs rely on
transient, rather than steady flow conditions.
B. Large-Amplitude Oscillatory Shear (LAOS)
To replicate the flow and deformation conditions encoun-
tered in practical applications of YSFs, both linear and non-
linear rheological protocols are required. Sinusoidal oscilla-
tory shearing is frequently employed in the study of YSFs47–52
as it allows independent control of the timescale and extent
of deformation, enabling the impact of each on the material
properties to be investigated47,48 . As large deformations are
required to yield the sample, large-amplitude oscillatory shear
(LAOS) is often used in these investigations.
There are a range of approaches available to interpret
LAOS behavior, which rely on different physical interpreta-
tions of the total applied strain and resultant stress data. These
fall into three main classes: 1) approaches that use Fourier
series53–57 or power series expansions58,59 of the stress re-
sponse to sinusoidal oscillatory shearing; 2) mathematical
decomposition techniques such as the stress decomposition
(SD)60,61 , the Chebyshev description62 of the SD parameters
and superpositions of four “fundamental” basis functions63 ;
and 3) derivative-based techniques that view the LAOS re-
sponse as a sequence of physical processes, such as the se-
quence of physical processes (SPP) framework of Rogers and
collaborators12,64–70 . Each of the techniques has their ben-
efits and drawbacks in the interpretation of material proper-
ties, primarily arising from the mathematical framework of
the respective method. There has been difficulty assigning
physical meaning to the individual harmonics or elements of
the series-based approaches62 . The mathematical decompo-
sitions are constructed to solve this particular issue, but they
have been shown to conflate distinct physical behaviors un-
der various rheological responses, particularly when yielding
2
is occurring64 . The SPP framework is the least restrictive of
the three, as it does not require a full period to analyse, but
still results in moduli that combine linearly at all points in
time.64,69 In all cases, the independent corroboration of such
methods has yet to be reported in terms of experiments that
are independent of the particular LAOS analysis framework
being used.
C. LAOS and Pipkin Space
When attempting to characterize nonlinear deformations,
it is typical to try to classify them by looking at the relative
values of dimensionless groups. Two particular groups that
quantify dimensionless frequency and flow strength are the
Deborah number and the Weissenberg number. These respec-
tive groups represent the abscissa and the ordinate of “Pipkin
space"71 , which has been treated as a universal way to classify
material deformations.
The solid-like behavior and liquid-like behavior in a soft
material under deformation can be differentiated by the use
of the Deborah number, which is usually denoted as De. The
Deborah number was first introduced by Reiner72 , who sug-
gested that it be defined as the ratio of material relaxation time
to an experimental observation time. In the same set of re-
marks in which he introduced the Deborah number, Reiner
also cautioned, “In every problem of rheology make sure that
you use the right Deborah number." In practice, Reiner’s sug-
gestion to use a ratio of material and experimental timescales
has resulted in the definition De = λ ω for oscillatory tests,
where λ is the longest material relaxation time and ω is the
angular frequency73 .
The Weissenberg number, usually denoted as Wi, was first
proposed by White74 , and is intended to describe the strength
of the flow. He defined the Weissenberg number as the product
of the relaxation time and the shear rate, Wi = λ γ˙0 , interpret-
ing it as the amount of recoverable strain in the fluid.
The common LAOS definitions for these two dimension-
less groups come with implicit assumptions about the nature
of oscillatory deformation which may not hold in all cases,
particularly in the nonlinear regime. Firstly, assumptions are
made that the period of oscillation and the time taken to ac-
quire one strain unit at the highest rate are the relevant ex-
perimental timescales (ω −1 in De and γ˙0 −1 in Wi), and that
the properties of the material, specifically the linear-regime
relaxation time λ , are constant throughout the period. While
these assumptions hold for small-amplitude oscillatory shear
(SAOS) measurements, where the small amplitudes perturb
the structure without destroying it, they may require reeval-
uation as the deformation enforces structural rearrangements
and nonlinear behaviors are elicited.
The choice of timescales for LAOS deformations of YSFs is
particularly difficult, as they have been shown to yield and un-
yield within a single period of oscillation64,67,75 . This means
that at one instant during an oscillation the YSF will behave
elastically, which should be reflected by a high value of De,
and at another instant during the same oscillation the YSF is
flowing plastically, which should be reflected by a low value

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of De. The traditional definition, De = λ ω, by contrast, as-
signs a single value to the entire period. The transient nature
of the yielding transition during LAOS requires that De be de-
fined in a way that reflects the transience of the underlying
physics. Similar logic also applies to Wi. The exact choice for
the definition to use is unclear from the LAOS deformation
alone, and is made more difficult by our incomplete under-
standing of the yielding transition in general67,69 .
D. Recovery Rheology
Rheological studies have typically described mechanical
deformations of materials in terms of the total stress, σ , and
strain, γ. More information can be gained, however, by under-
standing the strain in the sample as the sum of a recoverable or
elastic strain, γrec , and a unrecoverable or plastic strain, γunrec .
The benefit of this description was originally put forward by
Weissenberg76 and Reiner77 . Discrimination of the two com-
ponents can be performed experimentally by measuring the
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
strain response to a zero-stress step at the end of an experi-
ment. In this “recovery step", the recoverable strain or elastic
strain is the amount of strain recovered by the material, while
the unrecoverable strain is the portion of the original strain left
over.
In recent years, a number of experimental studies have
adapted this technique in an iterative manner to decompose
a range of rheological responses into recoverable and unre-
coverable behaviors75,78–81 . These methods, which we refer
to here as ‘recovery rheology’, are unique in that their inter-
pretation of material physics does not depend on any mathe-
matical formulation, but rather on the separability of the strain
components. This fact makes the use of such recovery tests in
conjunction with LAOS deformation enticing, as it provides
an experimentally verifiable test for the different LAOS analy-
sis frameworks that have been proposed, and exposes the fun-
damental rheological physics of the LAOS deformation more
explicitly.
An example of the utility of recovery rheology is seen in
the work of Donley et al.75 , which showed that the overshoot
in the loss modulus seen in amplitude sweeps of YSFs was
the result of a gradual change in the strain acquisition be-
havior, from predominantly recoverable at small amplitudes
to predominantly unrecoverable at larger amplitudes with no
clearly identifiable single yield point. The results of that work
led to the development of a model that unifies the rheologi-
cal physics of YSFs above and below the yield stress81 . This
model consists of a single differential equation that accounts
for both the linear and nonlinear rheology of model yield
stress fluids without incorporating the abrupt yielding thresh-
old of the Oldroyd-Prager formalism.
E. Recovery Rheology and Pipkin Space
In addition to helping understand particular rheological be-
haviors, several recent studies have used the ideas of recovery
3
rheology to reconsider the traditional definitions of the Debo-
rah and Weissenberg numbers69,78 using the decomposed re-
coverable and unrecoverable strains. Singh et al.78 proposed
that the Deborah number be redefined as the ratio of the re-
coverable and unrecoverable strain rates, De = γ̇rec /γ̇unrec ,
and that the the Weissenberg number be redefined as the re-
coverable strain, Wi = γrec , based on the original sugges-
tion from White74 . These definitions are innately able to be
time resolved, and while Singh et al. focused predominantly
on steady shear deformation, they are adaptable for use in
time-resolved LAOS tests. This implies that the combination
of these definitions with the oscillatory shear/recovery tests
should be helpful in understanding the instantaneous flow or
deformation behavior of YSFs; in particular, providing a pos-
sible way to discern whether a material has yielded or not and
as a means to track the evolution of the yielding process.
F. Time-resolved tests for yielding
Strain-controlled oscillatory tests, as illustrated in fig. 1 (a-
d), are often used to provide information about the average
and transient material behavior in terms of the total applied
strain. Oscillatory shear/recovery tests75,79 , illustrated in fig. 1
(e), provide additional information on the relative extent of the
solid-like and fluid-like deformations of the material as illus-
trated in fig. 1 (f-i). Prior studies75,81 have focused on the aver-
age decomposition behavior of YSFs through experiments and
theoretical modeling, an example of which is shown in fig. 1
(i). In this manuscript, we focus on understanding and classi-
fying the transient instantaneous behavior of an ideal YSF us-
ing the model of Kamani, Donley, and Rogers81 . We refer to
this as the KDR model. Using recovery rheology, we develop
a full understanding of the entire LAOS response, including
the gradual yielding, that is averaged to obtain the dynamic
moduli presented previously75,81 and illustrated in fig. 1 (d,i).
The analysis of the transient LAOS data using oscillatory
recovery rheology serves as an independent method by which
the physical interpretations of the different proposed LAOS
analyses can be assessed. Until now, results from LAOS anal-
ysis frameworks have only been compared mathematically
and not to other non-LAOS rheological tests. Our results
provide support for the interpretations of the analytical SPP
framework, demonstrating that the SPP analysis accurately re-
flects the sequence of processes occurring in the response of
YSFs to LAOS. The predictive capability of SPP is also tested
by comparing recoverable strain measured experimentally and
predicted by the analytical SPP framework using only the to-
tal strain and total stress data. We therefore demonstrate that
the sequence of physical process framework is a comprehen-
sive theoretical approach for understanding the time-resolved
behavior of yield stress fluids.
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FIG. 1. Comparison between the the accessible rheological information from a traditional oscillatory shear test (a-d), and the additional
information gained from an oscillatory shear/recovery test (e-i). All data is from Carbopol 980. The traditional oscillatory shear protocol (a)
consists of applying sinusoidal strain. The stress response can be plotted vs. (b) total strain (c) total rate, known as Lissajous figures, providing
information about transient behavior. The average behavior is plotted as amplitude sweep (d), in terms of G0 (ω) and G”(ω). Oscillatory shear
with recovery protocol (e) includes determination of component strain during a period of oscillation. In addition to traditional Lissajous curves
and dynamic moduli (b-d), the stress response can be plotted vs. recoverable strain (f), recoverable (g) and unrecoverable rate (h), and allows
for the average behavior of each component to be expressed as component moduli (i).

II. THEORY moduli because they are directly related to the energy stored
elastically per unit volume and the rate at which energy is dis-
A. Large-amplitude oscillatory shear (LAOS) sipated viscously per unit volume respectively, averaged over
the entire oscillation in both cases49 .
1. Oscillatory deformation

While both strain- and stress-controlled oscillations have
been used in the literature, strain-controlled experiments are
more common. In strain-controlled oscillatory rheology, a si-
nusoidal strain is applied to the material,
γ(t) = γ0 sin(ωt),
where γ0 is the amplitude of the applied strain, and ω is the an-
gular frequency. The periodic stress response of the material
is then measured, and can be used to define the frequency-
dependent dynamic moduli, G0 (ω) and G00 (ω). When the de-
formation is small and linear responses are elicited,
σ (t) = γ0 (G0 (ω) sin(ωt) + G00 (ω) cos(ωt)).
The dynamic moduli are interpreted as representing the
solid-like and liquid-like components of the material response
because they are in phase and out-of-phase with the strain, re-
spectively. They are also referred to as the storage and loss
2. Time-resolved data and Lissajous curves
Large amplitude oscillatory shearing is a useful method
for studying the yielding transition, since yielding is a non-
linear process and solid-like and liquid-like behaviors can
occur sequentially during a single period of oscillation. To
(1)
study the transient behavior of YSFs during LAOS, the tra-
ditional Lissajous curves have been used where the stress is
plotted against the strain in an elastic Lissajous curve, and
against strain rate to create a viscous Lissajous curve48 . Since
the Lissajous curves are typically plotted in terms of the to-
tal strain, interpreting physics from them has proven diffi-
cult. A common approach to understanding LAOS has been
to use an analysis framework such as Fourier series53–57 , or
(2) power series expansions of the stress response58,59 , stress
decomposition (SD)60,61 , the Chebyshev description of the
SD parameters62 , superpositions of four "fundamental" ba-
sis functions63 , or the sequence of physical processes (SPP)
approach12,64–70 . Interpretations of LAOS data from such
methods intimately depend on the their mathematical frame-

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work and their underlying assumptions.
3. Sequence of Physical Processes (SPP) framework
The sequence of physical processes (SPP)
framework12,67,68,70 allows for time-resolved investiga-
tion of a material’s properties. While the full framework is
outlined elsewhere70 , the salient points are presented here.
The SPP framework views the stress response of a given
material at any point in time to be of the form:
σ (t) = Gt0 (t)γ(t) + Gt00 (t)γ̇(t)/ω + σ d (t), (3)
where Gt0 (t) and Gt00 (t) are the instantaneous dynamic mod-
uli, and σ d is the displacement stress that geometrically rep-
resents the vertical shifting of the osculating plane and phys-
ically accounts for yield stresses and strains. In this repre-
sentation, the time-dependent moduli can be defined using the
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partial derivatives of the transient material response:
∂ σ (t)
Gt0 (t) = , (4)
∂ γ(t)
∂ σ (t)
Gt00 (t) = ω . (5)
∂ γ̇(t)
The changes in these moduli over time are then utilized
to track behavioral transitions that occur within a single pe-
riod of oscillation. Specifically, Gt0 (t) tracks the elastic be-
havior of the material and Gt00 (t) tracks the viscous behav-
ior. Changes in Gt0 (t) indicate stiffening or softening, while
changes in Gt00 (t) indicate thickening or thinning. Addition-
ally, at times where Gt0 (t) > Gt00 (t), the material response can
be said to be predominantly solid-like and the reverse indi-
cates predominantly fluid-like behavior. Therefore, as the ma-
terial transitions across the Gt0 (t) = Gt00 (t) line, the transitions
can be classified as fluidizing or solidifying.
At points in the period where Gt0 (t)  Gt00 (t), it has been
suggested that the recoverable strain in the system can be di-
rectly estimated from the SPP70 ,
σ (t)
γrec (t) ∼
= , (6)
Gt0 (t)
thereby showing that the SPP scheme not only consists of a
method to analyze responses to LAOS, but it also provides
testable hyoptheses.
B. Recovery Rheology
The basic physical observation behind recovery rheology is
that the total strain acquired by a material can be decomposed
into recoverable and unrecoverable components, γrec (t) and
γunrec (t),
5
γ(t) = γrec (t) + γunrec (t). (7)
This summation behavior also applies to the component
strain rates,
γ̇(t) = γ̇rec (t) + γ̇unrec (t). (8)
In this recovery rheology representation, the recoverable
component is related to elastic processes and the unrecover-
able component is related to plastic events.
This decomposition can be accomplished experimentally
by performing a constrained recovery step at any instant dur-
ing a traditional experiment, as shown in fig. 1 (e). To de-
termine the recoverable and unrecoverable strain responses in
a time-resolved manner, recovery tests are performed itera-
tively, with the recovery step being initiated at different points
in time75,79 . While recovery tests can be performed in con-
junction with strain-controlled or stress-controlled tests, they
require that the rheometer be able to apply σ = 0 reliably to
the material in question.
C. Understanding the time-resolved recovery rheology
1. Motivation for component rate Lissajous curves
Recent studies have made use of the results of iterative re-
covery tests to enable an enhanced physical understanding of
the dynamics involved with the yielding transition75,81 . These
works have focused on the gradual, continuous nature of
yielding with increasing applied strain and the development of
the YSF model with unified physics across the yielding tran-
sition. While these improvements are substantial, they rely on
viewing the effects of yielding averaged out over the course
of the entire period. This is useful when comparing to exist-
ing time-averaged measures, but other work has also demon-
strated that there are important transient behaviors that exist
on timescales significantly shorter than a period in YSFs67,68 .
It is therefore important to develop a time-resolved under-
standing of the experimentally decomposed strain data from
recovery rheology tests.
The recoverable and unrecoverable strains at any given time
represent the solid-like and fluid-like deformations of the ma-
terial. The component rates at the same moment represent
the instantaneous changes in deformation in the solid-like and
fluid-like components. If a response is predominantly solid-
like, the instantaneous recoverable rate will be larger in mag-
nitude than the instantaneous unrecoverable rate, while the re-
verse is true for a more fluid-like response. We will therefore
use plots of unrecoverable rate vs. recoverable rate, which we
will call a component rate Lissajous curve, to visually distin-
guish whether a solid-like deformation or fluid-like flow dom-
inates at any given point in the oscillation.
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FIG. 2. Demonstration of time-resolved analysis for four linear-viscoelastic materials: an elastic solid (i), a Newtonian fluid (ii), a Kelvin-
Voigt viscoelastic solid (iii), and a Maxwell viscoelastic material (iv). For each model material, the data is shown in five curves; from left
to right: a total strain elastic Lissajous curve (a), a total rate viscous Lissajous curve (b), a recoverable rate viscous Lissajous curve (c), an
unrecoverable rate viscous Lissajous curve (d), and the new component rate Lissajous curve (e). Black arrows show the direction of trajectory.
The shaded area in the component rate Lissajous curves denotes the region where γ̇rec > γ̇unrec (i.e. where the deformation is instantaneously
more solid-like).

2. Simple viscoelastic models Gγ); 2) a Newtonian fluid (σ = η γ̇); 3) a Kelvin-Voigt vis-

To demonstrate the utility of our proposed component rate
representation, we begin by looking at the analytical response
of four linear viscoelastic models: 1) an elastic solid (σ =
coelastic solid (σ = Gγ + ηs γ̇) with G = ηs ; and 4) a Maxwell
viscoelastic liquid ( ησf + G
σ̇
= γ̇) with G = η f .
These responses are visualized in fig. 2. For each model,
we show five different Lissajous curves in the panels of the

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figure from left to right: the traditional elastic and viscous
Lissajous curves; the solid and fluid viscous Lissajous curves
introduced by Donley et al.75 in which the stress is plotted
against the recoverable and unrecoverable rates; and our pro-
posed component rate Lissajous curve in which we plot the
unrecoverable rate against the recoverable rate.
In the elastic solid, all of the applied deformation is recover-
able. This leads to its response lying entirely along the x-axis
of the component rate Lissajous curve shown in fig. 2(i.e),
indicating that its deformation is fully solid-like and recover-
able. In contrast, the applied deformation in the Newtonian
fluid is fully unrecoverable, and its component rate Lissajous
curve shown in fig. 2(ii.e) lies entirely on the y-axis, indicat-
ing that its deformation is fully fluid-like.
The two viscoelastic cases are slightly more complicated,
with both the Kelvin-Voigt solid and Maxwell fluid showing
the same total strain behavior as seen in fig. 2(iii.a) and fig.
2(iv.a), respectively. These two materials produce the same
dynamic moduli, G0 and G00 , under traditional analyses at this
combination of frequency and amplitude. Despite this, the
difference in the construction of the two models leads them
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to differ in their component rates. The Kelvin-Voigt solid has
only a non-zero recoverable strain/rate component, while the
Maxwell fluid has both recoverable and unrecoverable com-
ponents. The deformation behavior shown in fig. 2(iii.e) and
fig. 2(iv.e), is therefore substantially different. As the strain in
the Kelvin-Voigt solid is exclusively recoverable, it is shown
as entirely solid-like by the component rate Lissajous curve
displayed as fig. 2(iii.e). The instantaneous behavior of the
Maxwell fluid, by comparison, moves between predominantly
solid-like and fluid-like deformation throughout the period as
can be seen in fig. 2(iv.e). This is not due to changes in the me-
chanical behavior, as both G and η f are constant, but is rather
a consequence of the oscillatory nature of the deformation and
the strain additivity of the model. As the applied strain and
rate are out of phase with each other, the solid-like and fluid-
like portions of the deformation are also out of phase, and the
instantaneous deformation behavior oscillates between them.
3. Elastic Bingham Model
So far we have looked exclusively at the component rate be-
havior of linear viscoelastic models. If we wish to understand
yielding, we must also investigate how non-linear responses
can be understood from the perspective of the component rate
representation. We therefore inspect the response of an elastic
Bingham model82 , the simplest YSF model that follows the
Oldroyd-Prager formalism, and contains both recoverable and
unrecoverable deformations, as shown in fig. 3:
( 2.
Gγrec if |σ | < σy
σ (t) = . (9)
Gγrec + η f γ̇ if |σ | ≥ σy
This model contains a binary yielding condition, and is
therefore either acquiring strain exclusively recoverably be-
low the yield stress or unrecoverably above the yield stress.
7
This binary nature results in the presence of four distinct pro-
cesses throughout the period of oscillation: 1) an interval of
elastic deformation shown in fig. 3(i), where the component
rate curve indicates perfectly solid-like behavior; 2) an abrupt
yielding transition, where the response moves from the recov-
erable rate axis to the unrecoverable rate axis, indicated in
fig. 3(ii) with a discontinuity in the stress and an instanta-
neous jump; 3) a region of plastic flow shown in fig. 3(iii)
where the component rate curve indicates exclusively fluid-
like behavior; 4) an instantaneous unyielding process, where
the response moves from the unrecoverable rate axis back to
the recoverable rate axis, as shown in fig. 3(iv). The discon-
tinuity at the yielding point is a result of the digital nature
of the yielding element in the system, and is also a signature
of applying the Oldroyd-Prager formalism to transient flow
conditions27,67,81,83 .
By comparing the behavior of the elastic Bingham model in
fig. 3 to the Maxwell model in fig. 2(iv), we can see that both
of these systems show a shift between predominantly solid-
like and predominantly fluid-like deformation behavior. In
the Maxwell case, this change is solely the result of the time-
dependent shear in the system, while the shift in the behavior
in the elastic Bingham model is due to a discontinuous, piece-
wise change in the mechanical properties of the material. The
abrupt behavior of yielding seen here in the elastic Bingham
model is not typically replicated experimentally, with studies
on YSFs showing a gradual transition67 .
To distinguish the presence of yielding from the behavior of
a simple viscoelastic fluid, the presence of the motion across
the solid-fluid boundary in the component rate plane is a nec-
essary but not sufficient condition, as this is seen in both the
Maxwell fluid and elastic Bingham model. The difference be-
tween the response of a viscoelastic fluid and a YSF must
therefore be related to how the transition progresses, which
requires a justifiable metric for the instantaneous viscoelastic-
ity of the material.
III. MATERIALS AND METHODS
A. Experiments
1. Carbopol 980
We study the response of an aqueous suspension of Car-
bopol 980, which is a soft polymer microgel that has been
shown to be a YSF that exhibits behavior that is not signifi-
cantly affected by shear history.84 The 1 wt% Carbopol formu-
lation used in this study was prepared as in prior studies67,75 .
Rheometer Setup and Characterization
Measurements were made with an Anton Paar Modular
Compact Rheometer (MCR) 702 operating in combined mo-
tor/transducer mode. No corrections for parallel plate were
made to the data obtained from rheometer software. While
this device is a natively stress-controlled rheometer, its use of
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FIG. 3. Demonstration of time-resolved analysis for an elastic Bingham model at γ0 = 10 [-]. The grey lines indicate the whole response,
while black sections indicate the (i) elastic deformation, (ii) abrupt yielding, (iii) plastic flow, and (iv) instantaneous unyielding. Black arrows
show the direction of trajectory. The shaded area in the component rate Lissajous curves denotes the region where γ̇rec > γ̇unrec (i.e. where the
deformation is instantaneously more solid-like).

an electronically commutated synchronous motor allows for
both stress-controlled and strain-controlled test modes. The
instrument also allows for rapid switching on the order of
milliseconds between strain- and stress-controlled modes, en-
abling the oscillatory shear/recovery experiments shown here.
Measurements were performed using 50 mm parallel plate
geometries with a gap of 1 mm. To minimize the possibility
of wall slip, 240 grit waterproof sandpaper was attached to the
geometry using double-sided tape. This was chosen to repli-
cate existing works in the literature for this system tested67,75 .
A basic rheological characterization of the Carbopol was
performed that consisted of a linear-regime frequency sweep,

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FIG. 4. (a) The dynamic moduli across the frequency, G0 (ω) and
G”(ω) for Carbopol 980. (b) Steady shear flow curve behavior: vis-
cosity as a function of shear rate. The inset shows stress as a function
of the stress as a function of shear rate. The line denotes the best fit
to the Herschel-Bulkley model.
which is shown in fig. 4(a), and the steady shear flow curve,
which is shown in fig. 4(b). The frequency sweep was ob-
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tained by varying the angular frequency, ω, of the oscilla-
tion over the range 0.01-10 rad/s while maintaining a constant
strain amplitude of γ0 = 0.00316 strain units. The steady shear
flow curve was collected by holding the shear rate, γ̇, at rates
over the range 0.01-31.6 1/s until steady state was reached.
3. Oscillatory shear/recovery experiments
Oscillatory shear/recovery tests were performed as de-
scribed by Donley et al.75 , with each test consisting of a se-
ries of experiments of the following form: 1) application of
a sinusoidal strain for a time sufficient to achieve steady al-
ternance; 2) continuation of the oscillatory strain for an addi-
tional fraction of a period; and 3) the application of zero shear
stress to allow the material to recover to its ground state. This
procedure was carried out in the forward and reverse direc-
tions, with the average result used to eliminate potential di-
rectional artifacts. To obtain results throughout the period of
oscillation, the protocol, including both forward and reverse
directions, was iterated 40 times per amplitude by changing
the length of the second step between successive experiments
such that each forward/reverse pair was spaced evenly in time
with 32 points per half period.
An angular frequency of ω = 1 rad/s was used for the oscil-
latory portion of all tests shown here. The strain amplitude, γ0 ,
of the oscillations used ranged from 0.00562-10 strain units
for different tests.
This protocol provides us with time-trajectories of the total
strain, γ(t), from the strain at the end of each iterated step 2,
and the unrecoverable strain, γunrec (t), from the strain at the
end of each iterated step 3. The recoverable strain trajectory,
γrec (t), can be then be calculated from eqn. 7, and the corre-
sponding rates can be obtained by numerical differentiation.
9
B. Modeling - Experimentally-informed Kamani, Donley, and
Rogers (KDR) model
The recently-proposed KDR model81 unifies the physics of
yielding below and above the yield stress. The full details of
the model, including a 3D tensorial version, can be found in
Kamani et al.81 . The 1D version used here is,
 
σy n−1 ηs 
σ + λ (γ̇)σ̇ = + k|γ̇| γ̇ + γ̈ , (10)
|γ̇| G
with elastic modulus G, structural viscosity ηs , and a rate-
dependent relaxation time λ (γ̇) that is a consequence of com-
bining the recoverable and unrecoverable components,
σy
|γ̇| + k|γ̇|n−1 + ηs
λ (γ̇) = . (11)
G
The values used for the model parameters were taken from
the rheological characterization of the Carbopol 980 described
above. We set G = G0lin = 430 Pa and ηs = G00lin /ω = 23 Pa-s
based on the linear regime moduli at ω = 1 rad/s shown in
fig. 4(a), and set σy = 94 Pa, k = 27.93 Pa sn , and n = 0.416
based on a Herschel-Bulkley fit to the steady shear flow curve
shown in fig. 4 (b). The rationale for choosing these specific
parameters can be found in Appendix A.
We note that there are other models that could also be used
to describe the non-linear behavior of YSFs, such as the kine-
matic hardening model of Dimitriou et al85 . We have prefer-
entially selected the KDR model for this work as it has many
distinct advantages. The parameters in the KDR model can
be obtained from only two common rheological tests. These
parameters can be intuitively related to macroscopic mate-
rial properties due to the simple tests from which they are
derived81 . The KDR model accurately describes the overshoot
in the loss modulus and predicts the correct average recover-
able and unrecoverable components during amplitude sweeps.
The simplicity of the KDR model also allows for analytical
expressions to be derived for other experimental protocols,
where the model accurately predicts avalanches and viscosity
bifurcations in creep experiments and a rate-dependent appar-
ent yield strain in steady-shear start-up tests. Even though the
KDR model uses values of stress and strain that are averaged
across the gap, it explains the yielding behavior in terms of
non-local physics and thus accounts for spatially distinct de-
formation profiles. Rapid elastic deformation that occurs in
a part of the material enhances plastic rearrangement some-
where else. There are also parameter ranges that have not
yet been fully investigated for which the model predicts stress
overshoots in the transient LAOS responses.
C. Data processing
Experimental data was collected via Anton Paar’s commer-
cially available RheoCompass software. The results of the
KDR model were calculated numerically using MATLAB. All

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analysis of the recovery rheology data was performed in MAT-
LAB, using code previously published in Mendeley data86 .
The SPP analysis was implemented via SPPplus, a freely
available MATLAB code package, using Fourier domain fil-
tering to reduce noise in the data. All MATLAB computation
and analysis code can be provided upon request.
IV. RESULTS AND DISCUSSION
A. Time-resolved Recovery Rheology
1. Carbopol 980
The results of the largest amplitude oscillatory
shear/recovery test corresponding to an amplitude of
γ0 = 10 strain units performed on Carbopol 980 are shown
in fig. 5. The traditional elastic Lissajous curve is shown in
fig. 5 (a), the traditional viscous Lissajous curve is shown in
fig. 5 (b), and component rates are shown in fig. 5 (c,d), as
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well as the relative behavior of the component rates in fig.
5 (e). The loops observed in the component rate curve in
fig. 5 (e) near the unrecoverable rate axis are the result of
differentiation of experimental data with a small unavoidable
noise content. The material response shows some similarities
to the results from the elastic Bingham model shown in fig. 3,
particularly in the presence of 4 distinct behavioral regimes
corresponding to elastic deformation, yielding, plastic flow
within the period, and unyielding as well as the roughly
linear movement between the two axes of the component rate
Lissajous curve shown in fig. 5(ii.e).
Unlike the elastic Bingham model and other models that
follow the Oldroyd-Prager formalism with an abrupt yield-
ing element, Carbopol does not yield and unyield instanta-
neously. This can be discerned from the significant portions
of the period that elapse during the yielding and unyielding
steps shown in fig. 5(ii.a-b) and 5(iv.a-b), respectively.
The region of elastic deformation starts at strain reversal,
which correlates with the predominantly elastic behavior of
yield stress fluids at short times under transient startup of
shear. In this regime, the recoverable rate is large and the unre-
coverable rate is nearly zero. As the acquisition of recoverable
deformation slows, the unrecoverable deformation increases,
and the sample yields gradually, becoming progressively more
fluid-like with time. This happens as the shear stress ap-
proaches its plateau value. Once that plateau is reached, the
recoverable rate has died down to zero, and the unrecover-
able rate accounts for all acquisition of strain. After traveling
along this curve at the plateau for some time, the decreas-
ing total rate triggers the onset of elasticity again, resulting in
the sequence of processes repeating twice per period. While
it is not impossible to infer the locations of these processes
from either the traditional Lissajous curves shown in fig. 5
(a,b) or the newer recoverable/unrecoverable rate Lissajous
curves shown in fig. 5 (c,d), the component rate Lissajous
curve shown in fig. 5 (e) allows for significantly more robust,
physically-motivated identification of where in the period of
oscillation the various physical processes are occurring.
10
The data here indicate that there is a significant difference
between yielding process, as shown in fig. 5 (ii.e), where the
response moves from the recoverable rate axis to the unrecov-
erable rate axis, and the unyielding process shown in fig. 5
(iv.e) where the response moves from the unrecoverable rate
axis back to the recoverable rate axis. By looking at the behav-
ior of each of the rate components, it is also possible to discern
that yielding is triggered by the material being pulled out of
the linear viscoelastic regime, while unyielding is much more
the result of the deformation slowing to a point that non-linear
behaviors are no longer supported. Finally, while the yielding
transition shows nearly linear motion between the two axes,
the shape of the unyielding process is more hyperbolic.
2. KDR model
The results of the KDR model are shown in fig. 6 for the
same large amplitude of γ0 = 10 strain units as the experimen-
tal response in fig. 5.
Upon direct comparison, it is clear that the predictions of
the model are very close to the experimentally measured re-
coverable and unrecoverable rates, which is non-trivial given
that the model requires no "fit" to the LAOS data, with only
the SAOS and steady flow behaviors required. The series of
four processes that repeat twice per period that are captured
in the experimental response of the Carbopol are also repli-
cated by the model. There are regions where the deformation
is nearly entirely solid-like, as seen in fig. 6 (i), or fluid-like
as seen in fig. 6 (iii), but also features a gradual transition be-
tween these two extremes, shown in fig. 6 (ii, iv), and shows
no abrupt discontinuity.
Additionally, the model accurately captures the differences
in the yielding process, where the response moves from the
recoverable rate axis to the unrecoverable rate axis, and the
unyielding process, where the response moves from the unre-
coverable rate axis back to the recoverable rate axis. While
yielding takes place when the system reaches a large value of
the recoverable rate, unyielding takes place when both rates
are small. This asymmetry can be understood in terms of the
nonlocal physics at the heart of the model. The rapid elastic
deformation that occurs in a part of the material can induce
plastic rearrangements somewhere else. In this manner, yield-
ing is expected to be observed when the recoverable rate is
large. Conversely, the unyielding process has no rapid elastic
deformation to assist in either reforming structure or acting
against any flow. Unyielding therefore only occurs when both
the component rates are small and non-linear deformations are
no longer supported. The yielding and unyielding processes
are therefore asymmetric.
3. Comparison between experiments and model at different
strain amplitudes
Having demonstrated the utility of the component rate Lis-
sajous curve, γ̇unrec (t) vs. γ̇rec (t), in identifying physical pro-
cesses in both experimental and theoretical systems, we now
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FIG. 5. Demonstration of time-resolved analysis for Carbopol 980 at γ0 = 10 [-]. The grey lines indicate the whole response, while black
sections indicate the (i) elastic deformation, (ii) gradual yielding (iii) plastic flow, and (iv) gradual unyielding. Black arrows show the direction
of trajectory. The shaded area in the component rate Lissajous curves denotes the region where γ̇rec > γ̇unrec (i.e. where the deformation is
instantaneously more solid-like).

apply it more broadly to the full range of amplitudes from both there is minimal evolution in the material properties through-
the Carbopol 980 and the KDR model in fig. 7. out the period.

At the smallest strain amplitudes, shown as grey, purple,
and blue curves in fig. 7, the material and model both spend
the majority of the period running along the x-axis of the com-
ponent rate Lissajous curve, indicating that elastic deforma-
tion is the single predominant process in the period, and that
As the strain amplitude becomes large enough to elicit sub-
stantially non-linear behavior, indicated by the green and yel-
low curves, a second process emerges wherein each of the
curves leaves the recoverable rate axis and follows a diag-
onal line up toward the more fluid-like region. These di-
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FIG. 6. Demonstration of time-resolved analysis for our viscoplastic model at γ0 = 10 [-]. The grey lines indicate the whole response, while
black sections indicate the (i) elastic deformation, (ii) gradual yielding (iii) plastic flow, and (iv) gradual unyielding. Black arrows show
the direction of trajectory. The shaded area in the component rate Lissajous curves denotes the region where γ̇rec > γ̇unrec (i.e. where the
deformation is instantaneously more solid-like).

agonal paths show that the responses are exhibiting either dominate, one can assume γ̈ ≈ (G/ηs )γ̇rec . The slope of the
pre-yielding behaviors, which stay predominantly below the line when the stress is equal to the yield stress, σ = σy , can
γ̇rec = γ̇unrec line, or yielding responses, which cross into the be calculated to be:
predominantly fluid-like region of the component rate Lis-
yσ ω2
σy +kγ̇ n +ηs γ̇ − 2
sajous curve. The slope of the line observed during the yield- ∂ γ̇unrec (t)
ing process is relatively constant as a function of strain ampli- = . (12)
∂ γ̇rec (t) σ ω2
tude. For the KDR model, approaching the yield stress after 1 − σy +kyγ̇ n +ηs γ̇
the elastic deformation process, where recoverable processes
This expression therefore provides the rate at which yielding

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FIG. 7. Time resolved component Lissajous curve for Carbopol 980
at various strain amplitudes, between the (a) experiments and the
(b) viscoplastic model. The colored arrows denote the direction of
the trajectory and the locations of the four distinct transitions. The
shaded area in the component rate Lissajous curves denotes the re-
gion where γ̇rec > γ̇unrec (i.e. where the deformation is instanta-
neously more solid-like). At large strain amplitudes, the slope of
the line observed during the yielding process is relatively constant,
shown as black lines.
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takes place, and indicates the design parameters that control
the rate of yielding.
Subsequently, there is a region where the curve follows a
vertical line in or near the fluid region, indicating acquisition
of unrecoverable strain only. At the largest amplitudes we
tested, shown as red and pink curves in fig. 7, the unrecov-
erable rate can be seen to continue to increase after yielding
has completed. Finally, the response moves from the unre-
coverable rate axis to the recoverable rate axis in a hyperbolic
manner, a behavior that emerges only once large amplitudes
are imposed. The model accurately captures the same physical
behavior observed in the experiments across all strain ampli-
tudes.
B. Time-resolved Pipkin space
To extract the time-resolved changes in the material prop-
erties quantitatively, we now turn from the component rate
Lissajous curves to the motion through Pipkin space. Unlike
other studies of LAOS that define single values of Wi and De
for a whole period and create a table of Lissajous figures, we
consider a Pipkin diagram as a space that is moved through
during an oscillation. This motion is defined by the ordinate
Wit (t) = |γrec (t)|69,74,78 and abscissa Det (t). In Appendix B
we derive a new form of Det (t),
s though its range is capped at a maximum threshold. As the
γ̇rec (t)γ̈rec (t)
Det (t) = , (13)
γ̇unrec (t)γ̈unrec (t)
that can be used to determined the solid- or liquid-like char-
acteristics of a material response in an instantaneous manner
on the basis of measurable quantities. This new expression
also removes the difficulties in assessing the salient relax-
ation or experimental time scales. Prior work has suggested
13
FIG. 8. Comparison of the complex motion within Pipkin space de-
scribed in terms of instantaneous dimensionless numbers for Car-
bopol 980 between experiments (a,c) and the model (b,d) with strain
amplitudes varying from small to large. The black arrows denote
the direction of the trajectory and the locations of the four distinct
transitions as discussed in the text.
the Deborah number be defined as the ratio of recoverable
to unrecoverable rates78 . However, this leads to values that
go between 0 and ∞ twice per period. In contrast, our new
expression applied to the Maxwell model leads to a constant
value, Det (t) = λ ω, throughout the period.
We display paths through Pipkin space for both the experi-
mental data from Carbopol 980 and the KDR model in fig. 8.
It is clear that both show the same basic behavior due to the
similarity of their curves.
At small strain amplitudes, shown in fig. 8(a,b), the Deb-
orah number is almost always greater than 1, which indicates
that elastic deformation is dominant. At these amplitudes,
the dominant motion through Pipkin space is associated with
changes in the instantaneous Weissenberg number, and the de-
formation in the material is almost entirely recoverable.
At larger amplitudes, shown in fig. 8(c,d), we observe a
fully realized sequence of four processes, including elastic de-
formation, gradual yielding, plastic flow, and gradual unyield-
ing. Substantial variation of the Weissenberg number is ob-
served during the elastic deformation region, when Det > 1,
system begins to yield, we see a rapid increase in Wit as Det
falls below 1. In the plastic flow regime, the value of Wit
plateaus at a value which is relatively independent of strain
amplitude, indicating that the material has reached a limit in
the acquirable recoverable strain. We can therefore conclude
that the LAOS data provides us with a map of how the material
behavior transitions between two axes of Pipkin space.
There is a substantial asymmetry observed between the
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yielding, and unyielding processes. Yielding is observed by
the motion from the recoverable rate axis to the unrecoverable
rate axis, and occurs as the recoverable strain is increasing
rapidly, while the unyielding transition, where acquisition of
strain changes from being unrecoverable back to recoverable,
happens at a nearly constant recoverable strain.

C. Comparison between Recovery Rheology and analytical

SPP framework

1. Comparison of predicted transitions

The results of the time-resolved recoverable strain decom-

position clearly show a sequence of physical processes that re-
peats twice per period of oscillation, and evolves as a function
of the applied strain amplitude. This sequence is revealed in
both the novel component rate responses shown in figs. 5(e),
6(e), and 7, and the time-resolved Pipkin space shown in fig.
8 of both the experimental Carbopol 980 system and the KDR
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model. As we now have both a direct physical measurement

of these processes under LAOS and analyses to robustly ex-
tract them, we are in a position to evaluate the interpretations
of LAOS analysis frameworks that have been proposed.
For the purposes of this work, we will focus on comparing
our recovery rheology results to the results of the analytical
Sequence of Physical Processes (SPP) framework12,67,68,70 .
This is a natural comparison for a couple of reasons. One
reason is that the SPP analysis was the original inspiration
for making the iterative recovery measurements, as it distin-
guishes between the total and recoverable strain but only al-
lows accurate calculations of the recoverable strain under cer-
tain conditions. The reason we choose to employ the SPP
analysis and not Fourier harmonic analysis, the stress decom-
position, or the Chebyshev analysis is that these approaches
have been shown to make overly strict assumptions about the
symmetries that are present in yielding responses and interpre-
tations based on them conflate distinct physical processes12,64 .
Finally, the SPP framework defines physical, time-resolved
processes from looking at the changes in instantaneous mod-
uli, Gt0 (t) and Gt00 (t), defined by eqns. 4-5 that allow for a
determination of yielding within an oscillation.
The recovery rheology and SPP results are shown for com-
parison in figs. 9 and 10 for the case of γ0 = 10 strain units
for both the experimental measurements on Carbopol 980 and
the predictions of the KDR model. Detailed discussion on
how to read the time-dependent Cole-Cole plots from the SPP
analysis, shown as panel c. of each figure, can be found
elsewhere66,68,70 . For the purposes of this work it is suffi-
cient to state that variation in Gt0 (t) denotes changes in elas-
ticity such as stiffening or softening, variation in Gt00 (t) de-
notes changes in viscosity such as thickening or thinning, and
movement across the Gt0 (t) = Gt00 (t) line denotes transitions
between predominantly elastic and predominantly viscous re-
sponses.
It is immediately clear that the SPP approach indicates the
same four physical processes determined by the experimental
recovery rheology. Regimes of elastic deformation, gradual
FIG. 9. Comparison of the time-resolved strain decomposition and
analytical SPP analysis on the total deformation on Carbopol 980
at γ = 10[-] strain units. The new analysis results are displayed on
(a) a component rate Lissajous curve and (b) a traditional “elastic”
Lissajous curve. The SPP analysis results are shown on (c) a time-
dependent Cole-Cole plot and (d) a traditional “elastic” Lissajous
curve. The black arrows denote the direction of the trajectory. The
numbers denote the four distinct transitions as discussed in the text.
yielding, plastic flow, and gradual unyielding are clearly iden-
tifiable for both the Carbopol and model shown in fig. 9(a,c)
and fig. 10(a,c). The predicted locations of the transitions
within the period are similar, as represented by the traditional
elastic Lissajous curves in panels b. and d. of each figure,
with only minor deviations in both cases.
2. SPP results across different amplitudes
In fig. 11, we show the results of the SPP analysis on
the full range of amplitudes collected from the experiments
and model. These can be compared to the results of the
recovery rheology analysis shown in figs. 7 and 8. Mov-
ing from small to large amplitudes, we see that the instanta-
neous dynamic moduli transition from small variations around
a point Gt0  Gt00 that indicates predominantly elastic behavior
throughout the period, to a curve shape with significant fluc-
tuations in moduli throughout the period. At the larger ampli-
tudes, there are both predominantly elastic and predominantly
viscous regions, indicating that the material spends time in
both elastic deformation and plastic flow, and yields and un-
yields to transition between the two.

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FIG. 10. Comparison of the time-resolved strain decomposition and
analytical SPP analysis on the total deformation for the viscoplastic
model at γ = 10[-] strain units. The new analysis results are displayed
on (a) a component rate Lissajous curve and (b) a traditional “elastic”
Lissajous curve. The SPP analysis results are shown on (c) a time-
dependent Cole-Cole plot and (d) a traditional “elastic” Lissajous
curve. The black arrows denote the direction of the trajectory. The
numbers denote the four distinct transitions as discussed in the text.
FIG. 11. Comparison of the transient Cole-Cole plots for Carbopol
980 between experiments (a) and the model (b), at various strain am-
plitudes.
3. Comparison of predicted and measured recoverable strains
Under conditions where Gt0  Gt00 , the SPP framework can
be used to estimate the recoverable strain, γrec , from any ma-
terial response70 using eqn. 6. As we have measured this
quantity experimentally through the recovery rheology exper-
iments, we can provide an additional test of the accuracy of the
SPP analysis by comparing the predictions against the mea-
sured values.
We show in fig. 12 the comparison of the measured recov-
15
FIG. 12. Comparison of the recoverable strain between the analytical
SPP prediction and the measured value from the experimental strain
decomposition for (a) experiments and the (b) model.
erable strain from the recovery rheology experiments with the
predicted value from the SPP analysis at γ0 = 10 strain units
for both Carbopol and the KDR model. Only instances for
which Gt0 > 2Gt00 are shown. For both the experiments and the
model, the recoverable strain predicted by the SPP analysis is
nearly the same as that measured experimentally, and is signif-
icantly smaller than the applied strain amplitude. Deviations
from the SPP predictions are expected as Gt00 becomes more
prominent, as the derivation of the estimate in eqn. 6 relies
on elastic effects being much stronger than viscous ones. This
comparison indicates that the SPP not only provides accurate
information on the instants of material transitions, but is also
able to provide accurate predictions of other measurable quan-
tities.
From the comparisons to the recovery rheology results, we
are able to provide independent experimental corroboration
of the interpretations of the analytical SPP framework, and
demonstrate that the SPP analysis is capable of extracting
the relevant rheophysics of yield stress fluids. We conclude
that the SPP framework, separate from other proposed LAOS
frameworks, is more than simply a convenient analysis, but
is also a powerful predictive framework that provides reliable,
testable predictions of the material transitions and recoverable
strain.
V. SUMMARY AND CONCLUSION
In this study, we have used multiple experimental and ana-
lytical approaches to develop a detailed understanding of the
sequence of processes exhibited by yield stress fluids under
large amplitude oscillatory shearing. Our major findings are
summarized in fig. 13 with example responses taken from the
KDR model prediction. These techniques include: 1) a novel
component rate Lissajous curve, γ̇unrec vs γ̇rec , shown in fig.
13(a); p2) a novel time-resolved Pipkin space, Wit = γrec vs.
Det = (γ̇rec γ̈unrec )/((γ̇unrec γ̈rec )) shown in fig. 13(b); and 3)
the analytical SPP framework, Gt00 vs. Gt0 , shown in fig. 13(c).
We demonstrate that each of these methods of understand-
ing the LAOS response of YSFs identifies the same material
physics, showing a time-resolved sequence of physical pro-
cesses that includes 1) elastic deformation 2) gradual yielding
 16

summary figure.png

This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583

FIG. 13. Comparison of the sequence of physical processes at large strain amplitudes of γ0 = 3.16, 5.62 and 10[−] strain units from the (a,d)
proposed component rate Lissajous curve, (b,e) Pipkin space and (c,e) analytical SPP analysis. The numbers denote the four distinct transitions
as discussed in the text.

3) plastic flow and 4) gradual unyielding. This sequence can
be seen to occur twice per period, with smooth and continu-
ous transitions occurring between each regime. Additionally,
the different techniques predict nearly identical durations and
transitions for each of these processes, as illustrated in fig.
13(d-f).
Our ability to describe the time-resolved rheophysics of
YSFs using the instantaneous component strains and rates
from recovery rheology suggests that these quantities are the
native way to understand how soft materials behave on a con-
stitutive level. These quantities also suggest meaningful av-
enues of connecting oscillatory studies of elastoviscoplastic
rheology to quantities determined from other tests, including
steady shear startup and steady creep tests81 .
The mapping of the LAOS transitions of YSFs in time-
resolved Pipkin space indicates how LAOS acts as a bridge
between the two axes of that space corresponding to SAOS
and steady shear. The recently-proposed KDR model used in
this work81 , is explicitly defined based on a characterization
consisting of those two limiting tests, and successfully cap-
tures the same behavior that is seen in experimental LAOS
of YSFs by acknowledging the nonlocal physics that leads
to rapid elastic straining enhancing plastic deformation. The
model includes a single value of yield stress, σy , obtained
from the steady shear flow curve, but is able to capture the
transient large amplitude oscillatory shear response.
While we have focused in this work on the LAOS defor-
mation of YSFs, the novel techniques developed here, partic-
ularly the component rate Lissajous curves and time-resolved
Pipkin space, are not restricted to use in LAOS, nor YSFs,
and should allow for direct comparison of disparate rheo-
logical protocols in a wide range of materials. While this
information-rich and protocol agnostic rheological approach
can be applied to all soft materials, connection of the recovery
measurements to structural parameters will require additional
information from other techniques such as small angle scat-
tering or simulations79,87–89 . By using these techniques based
on the ideas of recovery rheology, we have additionally devel-
oped a framework by which the assumptions made by analyt-
ical frameworks for rheological data in general, and LAOS in
particular, can be experimentally tested.
The results of the recovery rheology experiments have pro-
 17

This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
vided independent verification of the interpretations offered solid like behavior while steady shear flow curve behavior
by the analytical SPP framework for the LAOS of YSFs. provides information about only the steady flow properties of
While such an analysis still remains to be done for other the material. To connect the two, it becomes necessary to look
classes of materials, similar methodology can be utilized. The at the LAOS behavior, which transitions between the two ex-
fact that the SPP is able to give comparable physical insights tremes.
to the more complicated recovery rheology experiments on Under oscillatory shear, the dynamic moduli are defined en-
YSFs is impressive, especially when comparing the relative ergetically as49 :
difficulty of the experimental procedures. The SPP analysis
can be performed directly on any oscillatory data set where
4(Wstored (ω))avg 2(γ(t)σ (t))avg
waveforms of strain and stress are collected. An entire am- G0 (ω, γ0 ) = 2
= , (A1)
plitude sweep can be collected and analyzed by the SPP ap- γ0 γ02
proach in a small fraction of the time taken to perform the
iterative recovery rheology.
2(Ẇdiss. (ω))avg 2(γ̇(t)σ (t))avg
G00 (ω, γ0 ) = = . (A2)
γ02 γ02
ACKNOWLEDGMENTS
In the linear regime, the dynamic moduli are related to the
energy stored per unit volume and energy dissipated per unit
We thank Anton Paar for the use of the TwinDrive MCR volume, respectively. While the linear relationship in eqn.2 in
702 through their academic research program. We also thank the main text does not hold as the strain amplitude increases,
Lubrizol for providing the Carbopol used in this work. Useful the energetic definitions in eqns. A1 and A2 do still hold in
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583

discussions with Piyush Singh are acknowledged. This ma-
terial is based upon work supported by NSF Grant 1847389
and the Laboratory Directed Research and Development pro-
gram at Sandia National Laboratories. Sandia National Lab-
oratories is a multimission laboratory managed and operated
by National Technology and Engineering Solutions of Sandia
LLC, a wholly owned subsidiary of Honeywell International
Inc. for the US Department of Energy’s National Nuclear Se-
curity Administration Contract DE-NA0003525.
DATA AVAILABILITY STATEMENT
a time-averaged sense, though the energy storage and dissipa-
tion are no longer uniform throughout the period.
Donley et al.75 demonstrated that it was possible to utilize
the component strains to define component moduli which sep-
arate the contributions of viscoelastic solid-like and viscoplas-
tic fluid-like deformation of a material to the traditional dy-
namic moduli:
2(γrec (t)σ (t))avg
G0solid (ω, γ0 ) = , (A3)
γ02

2(γ̇rec (t)σ (t))avg

The data that support the findings of this study are available G00solid (ω, γ0 ) = , (A4)
from the corresponding author upon reasonable request. ωγ02

2(γ̇unrec (t)σ (t))avg

Appendix A: Motivation for KDR model G00f luid (ω, γ0 ) = . (A5)
ωγ02
In order to appropriately model a yield stress fluid’s be- When performing recovery rheology on the LAOS of Car-
havior both below and above yielding, the model must be bopol 980, we get the component moduli in fig. 14 (a).
able to capture both the material’s linear visco-elastic behav- While the component moduli discussed in eqns.A3-A5 are
ior (shown in fig. 4 (a) as a frequency sweep) and non-linear useful for decomposing the relative contributions from re-
flow behavior (shown in fig. 4 (b) as a flow curve). The linear coverable and unrecoverable processes to experimental LAOS
behavior of YSFs consists of dynamic moduli G0 and G00 that measurements75 , the fact that they are normalized by the total
are weakly or negligibly dependent on the frequency, consis- strain amplitude is not immediately intuitive from the material
tent with a Kelvin-Voight viscoelastic solid. This suggests that perspective, as the material has no way of knowing the over-
the solid-like, recoverable portion of the model should consist all deformation placed on it. If we want to gain information
of a viscoelastic solid element with both an elastic modulus from the material perspective it is more natural to instead nor-
of G = G0 (ω) and a structural viscosity ηs = G00 /ω. Mean- malize the component moduli by their respective component
while, the steady-state flow behavior of the YSF seems to be strain amplitudes,
well characterized by a Herschel-Bulkley fit to the flow curve.
This suggests that it should be characterized by a flow viscos- 2(γrec (t)σ (t))avg
G0solid,raw (ω, γ0 ) = , (A6)
ity of the form η f = (σy + kγ̇ n )/γ̇. 2
γrec,0
While the two behavioral extremes are clear, the exact time-
resolved interplay between these two elements is not immedi-
ately apparent. The frequency sweep is conducted at small 2(γ̇rec (t)σ (t))avg
G00solid,raw (ω, γ0 ) = 2
, (A7)
strain amplitudes and provides information about only the ωγrec,0
 18

This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
terial experiences from its internal frame of reference. To do
this, we will look at the component rate curves.
It is immediately noticeable when comparing the Maxwell
model shown in fig. 2(iv) to the elastic Bingham model dis-
played in fig. 3 that there is a substantial difference in the
shape of the curves. The Maxwell model with G = η f dis-
plays a circular curve, which is elliptical in the general case
where G 6= η f . For a sinusoidally applied strain, as shown in
eqn. 1, the Maxwell viscoelastic fluid, ησf + Gσ̇
= γ̇, results in
the following stress response,

ωGη f γ0
FIG. 14. Component moduli related to recoverable and unrecover- σ (t) = (G cos(ωt) + ωη f sin(ωt)). (B1)
able strain for Carbopol 980 at ω = 1 rad/s as functions of total strain G2 + (ωη f )2
amplitude (a) normalized by total strain and (b) normalized by their
As all elastic components of the Maxwell are recoverable,
component strain amplitude.
and all viscous components are unrecoverable, the component
rates can be determined to be,
2(γ̇unrec (t)σ (t))avg
G00f luid,raw (ω, γ0 ) = 2
, (A8)
ωγunrec,0 ω(ωη f )γ0
γ̇rec (t) = (ωη f cos(ωt) − G sin(ωt)), (B2)
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583

G2 + (ωη f )2
These "raw" or "natural" component moduli (shown in
fig. 14 (b)) provide additional information that informs the
way to set up the physics of the model. The component mod- ωGγ0
γ̇unrec (t) = (G cos(ωt) + ωη f sin(ωt)). (B3)
uli related to recoverable processes, G0solid,raw and G00solid,raw , G2 + (ωη f )2
remain almost independent of the applied strain amplitude,
These form an ellipse in the component rate plane that is
suggesting that the two model parameters related to recover-
described by,
able deformation, G and ηs , should be constant throughout
the sweep. The component modulus related to the unrecover-
able portion of the deformation, G00f luid,raw , is equal to the flow G2 + (ωη f )2 2 G2 + (ωη f )2
viscosity determined from steady shear measurements, η f . It (γ̇ rec (t)) + (γ̇unrec (t))2 = (ωγ0 )2 .
(ωη f )2 G2
should be noted that this dependence is with regards to the to- (B4)
tal strain rate, and not just the unrecoverable portion, which If we ensure that the traditional definition of the Deborah
indicates that the viscosity related to the unrecoverable strain number holds, and substitute De = λr ω = ωη f /G and γ̇0 =
is dependent on the total strain rate, and plasticity is enhanced ωγ0 into eqn. B4, we obtain,
by the elastic deformation.
 
1
1 + 2 (γ̇rec (t))2 + (1 + De2 )(γ̇unrec (t))2 = γ̇02 , (B5)
Appendix B: Time-dependent Deborah number from Recovery De
Rheology
which represents the entire trajectory in the component rate
space when the material properties are constant.
The Deborah number72,73 is intended to characterize the ex- In contrast to the Maxwell fluid, which always displays
tent of solid-like or fluid-like behaviors in a material and was an elliptical response, the elastic Bingham model crosses the
suggested by Reiner to be a ratio of timescales. Traditionally, solid-fluid boundary instantaneously in a straight line. This
the Deborah number has been defined as the ratio of the ma- suggests that a yield stress fluid undergoing yielding moves
terial’s relaxation time (λr ) to some experimental observation between ellipses with progressively increasing eccentricity
time. When the relaxation time is longer than the timescale of along the unrecoverable rate axis, which corresponds to the
observation, De > 1, the material behaves as a solid, whereas instantaneous material properties becoming more fluid-like.
when the relaxation time is shorter than the observation time, To capture the transition in a time-resolved manner, we note
De < 1, it behaves as a fluid. In the case of oscillatory rhe- that the ellipse that corresponds to the instantaneous proper-
ology, the angular frequency ω is typically assumed to be the ties will be both centered at the origin in component rate space
inverse of the observation time, which leads to the common and tangent to the deformation trajectory instantaneously. The
representation of the Deborah number as De = λr ω. By re- tangent of the ellipse defined in eqn. B5 at an arbitrary instant
lying on the angular frequency to represent the inverse of the is
observation time, this measure can only be used to character-
ize the average state of the material over an entire oscillation.  
The definition of an instantaneous Deborah number requires 1
1 + 2 γ̇rec (t)x(t) + (1 + De2 )γ̇unrec (t)y(t) = γ̇02 , (B6)
identification and determination of the timescales that the ma- De

This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
where hx(t), y(t)i is a point in the component rate plane.
Through some algebra, we can solve for y(t),
γ̇02 (1 + 1/De2 )γ̇rec (t)
y(t) = 2
− x(t). (B7)
(1 + De )γ̇ unrec (t) (1 + De2 )γ̇unrec (t)
As the slope of this line must be equivalent to the instanta-
neous slope of the material’s trajectory through deformation
space, we deduce,
∂ γ̇unrec (t) γ̈unrec (t) (1 + 1/De2 )γ̇rec (t)
= =− . (B8)
∂ γ̇rec (t) γ̈rec (t) (1 + De2 )γ̇unrec (t)
Solving for the Deborah number, we obtain a time depen-
dent expression in terms of measurable rate components and
their derivatives,
s and fluid-like responses to deformation. In the component
γ̇rec (t)γ̈rec (t)
Det (t) = . (B9)
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
γ̇unrec (t)γ̈unrec (t)
This equation is similar in principle to the definition of the
Deborah number recently proposed by Singh et al.78 ,
γ̇rec (t)
Det (t) = . (B10)
γ̇unrec (t)
Singh et al. noted that this proposed definition leads to a
variation during oscillatory shearing from 0 to ∞ twice per
period, which makes it unsuitable for use as an instantaneous
measure. However, it was shown that the root mean square
value of eqn. B10 leads to the traditional measure. By con-
trast, inserting the expressions for the recoverable and unre-
coverable rates for the Maxwell model, shown in eqns. B2
and B3, into eqn. B9 leads to the traditional measure with-
out the need to calculate an average over the period. Our new
expression, eqn. B9, can therefore be used to determined the
solid- or liquid-like characteristics of a material response in
an instantaneous manner on the basis of measurable quanti-
ties. Use of eqn. B9 also removes the difficulties in assessing
the salient relaxation or experimental time scales.
When this time-dependent Deborah number, Det (t), is con-
sidered along with the fact that our ellipse must travel through
the point hγ̇rec (t), γ̇unrec (t)i at time t, the value of γ̇0 in eqn.
B5 must also be time-dependent to adjust the amplitude of the
tangent ellipse appropriately. This results in a value, γ̇0,t (t),
that acts as an instantaneous effective magnitude of the com-
plex rate vector in the component rate plane,
s  Colloidal phase behavior and rheology of soft spheres,” J. Chem. Phys. 111,
1
(γ̇rec (t))2 + 1 + Det2 (γ̇unrec (t))2 .


γ̇0,t (t) = 1+
Det2
(B11)
Application of eqn. B11 to the elastic Bingham model is il-
lustrative of its utility. In the elastic portion of the response,
the instantaneous Deborah number (see eqn. B9) is infinite
19
and γ̇unrec = 0, so eqn. B11 says γ̇0,t (t) = γ̇rec (t). By con-
trast, in the plastic part of the response, the instantaneous
Deborah number is zero and γ̇rec = 0 and eqn. B11 says
γ̇0,t (t) = γ̇unrec (t). The effective rate therefore changes be-
tween being recoverable and unrecoverable when yielding, as
illustrated in fig. 3.
That the material does not feel the overall rate amplitude at
all points of the oscillation is consistent with the observation
that the material does not react to the amplitude of deforma-
tion, but rather to the instantaneous deformation applied to it.
As this rate appears to be exclusively related to the component
rates, rather than the total rate, it strengthens the argument that
the decomposed strains and rates represent the deformation
from the natural perspective of the material.
By observing the time-resolved Deborah number through-
out the period, we can understand how the yielding transi-
tion manifests in soft materials. As with the traditional def-
inition, Det = 1 will act as the boundary between solid-like
rate Lissajous curves, yielding can be identified as follows:
1) The response spends a significant percentage of the period
at both extremes and transitions rapidly between them; and 2)
this complex behavior only evolves at large amplitudes.
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PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
21
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This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583
This is the author’s peer reviewed, accepted manuscript. However, the online version of record will be different from this version once it has been copyedited and typeset.
PLEASE CITE THIS ARTICLE AS DOI: 10.1122/8.0000583