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Rheological Behavior of Magnetorheological Suspensions under Shear, Creep

and Large Amplitude Oscillatory Shear (LAOS) flow

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Suraj Deshmukh Gareth H. Mckinley

Dow AgroSciences Massachusetts Institute of Technology
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 Proc. XIVth Int. Congr. on Rheology August 22-27, 2004
Edited by: Seoul, Korea
Copyright 2004 – The Korean Society of Rheology

Rheological Behavior of Magnetorheological Suspensions under Shear,

Creep and Large Amplitude Oscillatory Shear (LAOS) flow
Suraj S. Deshmukh and Gareth H. McKinley

Hatsopoulos Microfluids Laboratory (HML) & Institute of Soldier Nanotechnologies (ISN),

Department of Mechanical Engineering, Massachusetts Institute of Technology

ABSTRACT
Magnetorheological (MR) fluids are an important class of ‘field-responsive’ fluids that undergo liquid to
solid-like transition in the presence of applied magnetic fields. Magnetorheological suspensions based on
different carrier fluids with viscoplastic additives have been prepared, and the dependence of the yield-
stress on the magnetic field strength has been compared to commercially available MR fluids. Analysis of
creep behavior in the solid-like state below the yield stress provides useful information on the
characteristic response of these field-responsive fluids. The evolution of chain structure and plastic
collapse in these suspensions has been investigated using large amplitude oscillatory shear flow (LAOS).
A new visco-elasto-plastic constitutive model for yield-stress fluids has been used to explain this
behavior. The model also predicts a universal rheological scaling w.r.t. a dimensionless stress ( σ σ y ) that
is observed in creep and oscillatory flow experiments.

stress or under oscillations with large amplitude.

INTRODUCTION Despite their potential significance there are very
few studies of MR fluid response under such
Field-responsive fluids (FRFs) may be deformations. The aim of this paper is therefore to
characterized as materials that undergo large systematically study rheological behavior of
changes in their rheological (i.e. flow) properties commercial and in-house MR fluids under creep
in response to changes in magnetic, electric or and large amplitude oscillatory shear (LAOS)
stress fields [1-3]. Many applications utilize flow.
variable flow rate or force characteristics of FRFs
in either damping or torque transfer scenarios and EXPERIMENTAL
proposed applications include shock absorbers,
clutches, brakes, actuators and artificial joints [4]. TA Instruments’ AR series stress-controlled
These large, rapid and reversible changes in fluid rheometers with a roughened parallel-plate or
properties have also been used to modulate the cone-plate arrangement were used for the
energy absorption capacity and mechanical experiments. The top and bottom plates of the
properties of cellular solids [5]. rheometer were roughened by coating a very thin
Magnetorheological fluids (‘MR fluids’) belong layer of carbonyl iron particles, such that the
to the class of field-responsive fluids and roughness was of the order of the MRF particle
normally, in the field-off state, are liquid with a size. Since the fluid properties are a strong
viscosity ~ 0.1-1 Pa.s. However, when a magnetic function of the magnetic field, a custom-made
field is applied, the soft magnetic particles acquire fixture has been designed and built as a
a dipole moment and align with the external field removable attachment for control and generation
to form fibrous columns or aggregates [4]. These of uniform magnetic field in the fluid sample
columns must be deformed and broken for the space. MR fluids have been synthesized using
suspension to flow giving rise to a yield stress [6] different sizes of carbonyl iron particles (CIP)
that is a function of the magnetic flux density. (BASF Corp.) at a volume fraction of 36% in a
Many earlier studies have focused on determining silicone oil base (Gelest Inc., DMS-S21). A
this yield stress and other rheological properties viscoplastic base (Dow Corning) has been utilized
of MR fluids under steady shear and oscillatory to provide a low off-state yield stress in order to
shear flow [4,7]. However, many damper & prevent particle settling and a PDMS surfactant
controllable energy absorption applications (Gelest Inc.) stabilizes the particles against
operate under loading conditions below the yield agglomeration.
 Proc. XIVth Int. Congr. on Rheology August 22-27, 2004
Edited by: Seoul, Korea
Copyright 2004 – The Korean Society of Rheology

RESULTS AND DISCUSSION response, which has been observed to be a strong

function of the magnetic field and the applied
The MR fluid shows a yield stress increasing stress. The creep behavior of the 7 µm CIP based
monotonically and sub-quadratically with MR fluid is shown in figure 2(a) and two distinct
magnetic field strength (see Figure 1). Particle regimes can be observed. Below the yield stress
chains are formed on application of a magnetic (σ σ y ) < 1 , a steady value of the total
field, which then evolve as the stress is ramped accumulated strain is typically reached within a
up, until a sharp yield point is reached at which few relaxation times whereas above the yield
point structural collapse occurs. stress (σ σ y ) > 1 , there is steady flow leading to
Despite roughening of the plates, the material an exponential increase in the deformation with
slips at higher shear rates leading to sample time. The accumulated strain is observed (figure
migration and causing the viscosity-stress curves 2(b)) to be a strong function of the dimensionless
to bend over as indicated in figure 1(a) by hollow stress ( s = σ σ y ) but independent of the MR fluid
symbols. composition, magnetic field strength and the
measurement technique (cone & plate or parallel
plate). The rise time to this steady strain value,
however, is determined by the magnetic field and
also the applied stress (τ = τ ( B, s ) ) .

(a)

(b)
Figure 1. Rheological measurements under shear flow
at different magnetic field strengths. (a) Viscosity vs
shear stress plots for laboratory-synthesized MR fluid
composed of 7µm carbonyl iron particles (b) Yield
stress comparison for different MR fluids with sub-
quadratic model fits. Figure 2. Rheological behavior of MR fluids under
creep flow (a) Compliance as a function of time
The yield stress is observed to be a strong illustrated for a magnetic field of 0.09 T (σy ~ 3.9 kPa).
function of the particle size. Larger sizes of Visco-elasto-plastic model fits (equation 1) are shown
particles result in MR fluids with a significantly as dotted lines. (b) Scaling for different fluid
increased yield stress, in comparison to compositions, magnetic fields and measurement
commercially available fluids, owing to a higher techniques observed w.r.t. dimensionless stress
(s=σ/σy).
saturation magnetization.
Creep flow allows for systematic quantification of
fluid behavior at constant stresses below and Modeling efforts for MR fluids have typically
above the yield stress. Also, creep flow studies been based on the GNF model in which the
enable characterization of the MR fluid temporal viscosity is described as a function of shear rate
 Proc. XIVth Int. Congr. on Rheology August 22-27, 2004
Edited by: Seoul, Korea
Copyright 2004 – The Korean Society of Rheology

and the yield stress [6]. These models, however, oscillatory stress approaches the yield stress.
are incapable of describing the viscoelastic solid-
like response of MR fluids in creep and
oscillatory flows. A microscopic model that
probes the origin of plastic collapse in yield stress
fluids would describe the behavior in a better
fashion. Such a model, that follows the evolution
of the population of ‘interaction sites’ leading to
plastic deformation, is currently in development.
This model formulation when related to the
suspension macrostructure results in evolution
equations for the shear rate and internal variables
in terms of three macroscopic parameters; yield
stress, modulus and relaxation time. For shear
flows, the model becomes,
1  Gσ 
γ =  σ − G∆ (t ) ; ∆ = γ 1 − 2 ∆ (t )  (1)
τG  σy 
 
where σ is the applied stress and γ is the shear
rate. Here σy is the yield stress, τ is the relaxation
time, and G is the modulus; these parameters may
all be functions of the applied magnetic field.
An analytical solution exists for the creep
response under constant stress

γ =
 2
( 2
σ  (1 − s )exp −(1 − s ) t τ 

) (2)
(
τ G 1 − s 2 exp −(1 − s 2 ) t τ 

 ) 
where s=(σ/σy) is the dimensionless stress.
The creep behavior of yield stress fluids is well
described by this visco-elasto-plastic model, as
shown in figure 2(a) for a representative case
(7micron CIP-based MR fluid). There are,
however, small discrepancies in model fits and the
modulus values that are possibly due to the use of
a single relaxation mode to describe the complex
gel-like MR fluid response.
Figure 3. Oscillatory flow behavior of MR fluids (a)
MR fluids show highly non-linear behavior in Storage modulus (1st harmonic) at different magnetic
oscillatory shear flow that can be analyzed using field strengths for oscillatory stress sweeps at a
Fourier Transform rheology. In figure 3(a) we frequency of 1 Hz (b) Lissajous curve with a visco-
show the 1st harmonic information as a function elasto-plastic model fit at a moderate dimensionless
of the stress amplitude. The loss modulus is found stress. (c) LAOS shapes at the yield point normalized to
to be an order of magnitude smaller than the illustrate scaling for different magnetic field strengths.
storage modulus, though both the moduli show a Also shown is the Lissajous curve predicted by the
plateau region for σ << σ y . As the stress model at the yield point.
increases, the chain structure evolves, until the
yield point is attained when the structure collapses A universal scaling with the dimensionless stress
leading to a sharp decrease in the elastic modulus. (σ/σy), analogous to that found in creep, is
In order to elucidate this non-linear response observed for different magnetic field strengths
under oscillatory loading, Lissajous curves have and various fluid compositions (see figure 3(c)).
been reconstructed from the measured stress- The model predictions are in excellent agreement
strain response (figure 3(b)). The curves with the observed LAOS behavior and the
increasingly deviate from the elliptical shape, progressive deviation from ellipticity is well
leading to enhanced energy dissipation, as the described.
 Proc. XIVth Int. Congr. on Rheology August 22-27, 2004
Edited by: Seoul, Korea
Copyright 2004 – The Korean Society of Rheology

CONCLUSIONS
We have systematically tested and analyzed the
behavior of MR fluids under constant stress and
oscillatory stress loadings. A universal scaling is
demonstrated with respect to the dimensionless
stress (σ/σy). A visco-elasto-plastic model based
on microscopic mechanisms of plastic
deformation shows good agreement with the
observed creep and oscillatory flow behavior.

REFERENCES
1. R. G. Larson, The Structure and Rheology of
Complex Fluids, 1st ed. (Oxford University Press,
1998), pp. 360.
2. H. A. Barnes, J. Rheol. 33, 329 (1989).
3. J. M. Ginder, Encyclopedia of Applied Physics,
Vol. 16 (VCH Publishers Inc., 1996), pp. 487.
4. D. J. Klingenberg, AIChE J. 47, 246 (2001).
5. S. S. Deshmukh, and G. H. McKinley, US Pat.
Appl. No. 10/378 129, 2002.
6. H. A. Barnes, J. Non-Newt. Fluid Mech. 81,
133 (1999).
7. B. D. Chin, J. H. Park, M. H. Kwon, and O. O.
Park, Rheol. Acta 40, 211 (2001).

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