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Printed in the UK

magnetorheological materials

Mark R Jolly, J David Carlson and Beth C Muñoz

Lord Corporation, Thomas Lord Research Center, 405 Gregson Drive, Cary, North

Carolina 27511, USA

rheological properties may be rapidly varied by application of a magnetic field.

These materials typically consist of micron-sized ferrous particles dispersed in a

fluid or an elastomer. A quasi-static, one-dimensional model is developed that

examines the mechanical and magnetic properties of magnetorheological materials.

This model attempts to account for magnetic non-linearities and saturation by

establishing a mechanism by which magnetic flux density is distributed within the

composite material. Experimental evidence of the viscoelastic behaviour and

magnetic properties of magnetorheological fluids and elastomers suggests that the

assumptions made in the model development are reasonable. It is shown that the

model is semi-empirical in that it must be fit to the experimental data by adjusting a

parameter that accounts for unmodelled magnetic interactions.

for exercise equipment (Carlson et al 1995, Gentry et

Magnetorheological (MR) materials consist of micron al 1995, Anon 1995, Chase 1996). MR elastomers

size (typically 3 to 5 microns) magnetically permeable will ultimately find use in applications where stiffness or

particles suspended in a non-magnetic medium. Upon resonance tunability is sought (Jolly et al 1996, Kasahara

application of a magnetic field, the rheological properties et al 1994). Other applications may also make use of

of these materials are rapidly and reversibly altered. The the unique mechanical, magnetic and thermal anisotropic

mechanism responsible for this bulk effect is the induced properties of these elastomer composites (Bowen et al

magnetic interaction of particles within the matrix. In 1995).

the case of MR fluids, this mutual interaction amongst Most models of MR material behaviour are based

the particles causes the formation of chain-like structures on magnetic dipole interactions between adjacent particles

aligned roughly parallel to the applied magnetic field. The within a particle chain (Harpavat 1974, Spasojevic et

configuration and rigidity of this structure will depend upon al 1974). These interparticle interactions are then

several factors including the strength and distribution of averaged over the entire sample to yield a model of the

the applied magnetic field. A finite stress must develop to bulk magnetorheological effect. Many such models are

yield these chain structures. Hence, MR fluids are often borrowed from models developed to understand similar

modelled as Bingham plastics with a field dependent yield interparticle interactions within electrorheological (ER)

stress (Spasojevic et al 1974). Yield stresses of nearly fluids (e.g., Block and Kelly 1988 and references therein,

100 kPa have been reported in commercially available Gast and Zukoski 1989). Still a weakness unique to MR

fluids (Lord 1994). MR solids have also been developed material modelling is an understanding of how magnetic

by incorporating magnetically permeable particles into flux density distributes itself within the particle network.

elastomer media (Rigbi and Jilken 1983, Muñoz and Jolly Such an understanding needs to take into account magnetic

1995, Jolly et al 1996). Typically, magnetic fields are nonlinearities and the effects of particle saturation. There

applied to the elastomer during crosslinking such that has been recent interest in this problem using finite

particle chain structures form and become locked in place element approaches (Ginder and Davis 1994) and analytical

upon final cure (see figure 1). At low strains (< 2%), approximations (Carlson 1991, Ginder et al 1995, Jolly et

these elastomers exhibit a field dependent modulus. A field- al 1996).

induced change in modulus of up to 40% has been reported In this paper, the simple dipole model of particle energy

(Jolly et al 1995). interaction is reviewed. From this we obtain a model of

MR fluids are beginning to find commercial success the MR effect as a function of particle magnetization. In

in applications where controlled energy dissipation is particular, it is seen that MR material stress is quadratically

required. Such applications include controllable dampers related to particle magnetization. This theory is then

for primary and secondary vehicle suspensions (Carlson augmented with an approximate model of the relationship

0964-1726/96/050607+08$19.50

c 1996 IOP Publishing Ltd 607

M R Jolly et al

viscoelastic properties of the composite are the sum of

the viscoelastic properties of the composite with no field

applied (which are not modelled here) and the elastic/plastic

properties induced by interparticle magnetic force.

The model is quasi-static, therefore the dynamic effects

of the magnetic field as well as inertial and rate-dependent

effects of the particles are ignored. The particles are

assumed to be uniform, homogenous spheres that can

be magnetically modelled as identical induced dipole

moments. It is also assumed that particles are aligned

in perfect chains (albeit with gaps between particles), and

that quasi-static shear strains and associated stresses are

uniformly distributed over the length of each particle chain.

polarization

Figure 2 shows two adjacent particles (dipoles) in a chain

along with the direction of applied magnetic field. The

interaction energy of the two dipoles of equal strength |m|

and direction is (Rosensweig 1985)

|m|2 (1 − 3 cos2 θ )

E12 =

4π µ1 µ0 |r|3

r02 (1)

|m|2 1 − 3 r 2 +x 2

= 0

4π µ1 µ0 (r02 + x 2 )3/2

where µ1 is the relative permeability of the medium and

where some basic trigonometric identities have been used

in the second equality. By defining the scalar shear strain

of the particle chain as = x/r0 , the interaction energy

can be written as

( 2 − 2)|m|2

E12 = (2)

4π µ1 µ0 r03 ( 2 + 1)5/2

Now it is assumed that the particles are aligned in

long chains and that there is only magnetic interaction

between adjacent particles within the chain, i.e., there

are no multipole interactions. Then the total energy

Figure 1. SEM images of magnetic particles in a polymeric density (energy per unit volume) associated with the one-

elastomer matrix; (upper) randomly dispersed particles, dimensional shear strain can be calculated by multiplying

(lower) particles aligned by applied magnetic field. The the particle-to-particle energy, given by equation (2), by the

width of the images is 70 microns. total number of particles and dividing by the total volume:

3φ( 2 − 2)|m|2

between particle magnetization and average composite flux U= (3)

2π 2 µ1 µ0 d 3 r03 (1 + 2 )5/2

density—a quantitiy that can be measured. This model

takes into account the gradual saturation of the permeable where φ is the volume fraction of particles in the composite

particles as applied field increases. This theory is then and d is the particle diameter. The stress induced by the

compared to experimental data on MR fluids and MR application of a magnetic field can be computed by taking

elastomers. the derivative of inter-particle energy density with respect

to the scalar shear strain:

σ = U= . (4)

∂ 2π µ1 µ0 d 3 r03 (1 + 2 )7/2

2

The present model examines the magnetomechanical Next, it is noted that the average particle polarization Jp is

properties of parallel chains of magnetically permeable the dipole moment magnitude per unit particle volume, i.e.

spherical particles. In particular, a magnetic field is |m| = Jp Vi , where Jp has SI units of Tesla:

applied parallel to the chains and the shear stress of

the chains caused by interparticle magnetic force is φ(4 − 2 )Jp2

σ = (5)

modelled. It is assumed that if these particle chains are 8µ1 µ0 h3 (1 + 2 )7/2

608

A magnetorheological material behaviour model

chain yield strain is 0.01–0.02 in MR elastomers (Jolly et al

1995) and substantially less than 0.01 in fluids (Weiss et al

1994). Theories that a majority of strain and the ultimate

yielding of a given chain occurs between a single (or a few)

pairs of particles (Tang et al 1995) are typical justification

for this large discrepancy between theory and experimental

evidence.

A small strain approximation of stress given by

equation (5) is

φJp2

σ ' < 0.1 (8)

2µ1 µ0 h3

for which a 3.6% error results when strain = 0.1. The

preyield modulus G of the particle network is simply stress

divided by strain, or, from equation (8)

φJp2

G' < 0.1. (9)

2µ1 µ0 h3

Furthermore, the maximum possible field induced change

in stress (and modulus) occurs when the aligned particles

become magnetically saturated, i.e. when Jp = Js .

It can be seen that the maximum field-induced stress

rises quadratically with saturation magnetization Js of the

Figure 2. (a) Geometry of two particles of diameter d

within a particle chain. Adjacent chains are a distance y

particle material. This observation advocates the use of a

apart and h = r0 /d . (b) Magnetic interaction of the two particulate material with a high saturation magnetization.

particles modelled as dipole moments m and sheared with Pure iron has the highest saturation magnetization of

respect to one another. known elements with Js = 2.1 T. However, alloys of

iron and cobalt (e.g. Permendur) have higher saturation

where we have defined h = r0 /d which is an indication of magnetizations with Js ≈ 2.4 T.

the gap between particles in a chain. This is illustrated in

figure 2. 2.2. The relationship between particle polarization and

Note that the stress-strain relationship given in average composite flux density

equation (5) is independent of particle size. The size of

The average composite flux density is relatively straightfor-

the gap between the particles in a chain can be seen to be a

ward to measure experimentally. For example, flux meters

very important parameter—magnetic field induced stress is

employing field probes or sense coils can typically measure

inversely proportional to this gap cubed. Say, for example,

the flux density at the composite sample directly. Alterna-

that the gap between particles is equal to one quarter of a

tively, if assumptions are made regarding the reluctance of

particle diameter (h = 1.25). Gaps of this size will cause a

the magnetic circuit, the flux density at the composite sam-

factor of two reduction in the magnetically induced stress.

ple can be calculated as a function of the applied magneto-

From figure 2, simple geometry indicates that adjacent

motive force. On the other hand, the particle polarization

particle chains will touch (y = d) when the particle gap is

is impossible to measure directly and is very difficult to

such that h = π/6φ. And particles will be evenly spaced

compute. In this section, theory is developed on the basis

within the matrix (y = dh) when h3 = π/6φ.

that saturation begins in the particle’s polar regions at a

The yield stress of the particle chains occurs at the strain

very low applied field and increases towards total particle

for which stress is maximum. This is found by setting the

saturation as applied field increases. Average particle polar-

first derivative of stress with respect to quasi-static shear

ization is then computed as a function of average composite

strain to zero:

flux density.

∂σ (4 4 − 27 2 + 4)φJp2 Consider the schematic in figure 3. We, again, isolate a

= =0 (6) single chain of particles from an array of parallel chains. It

∂ 8µ1 µ0 h3 (1 + 2 )9/2

is assumed that uniform saturation occurs in each particle

from which yield strain and corresponding yield stress can in region (s) shown in figure 3. Furthermore, distance

be found: s decreases from r to zero as average composite flux

p √ density increases from zero to some large level. Letters

27 − 665 in parentheses in figure 3 correspond to subscripts used in

y = = 0.389 (7a)

23/2 the following development. The magnetic model is one-

0.1143φJp2 dimensional, therefore vector quantities are expressed as

σy = . (7b) scalar magnitudes.

µ1 µ0 h3

609

M R Jolly et al

structures with more than two contact points per particle

that may locally be face center cubic or body center

cubic arrangements. Parameter k may also be used to

accommodate for situations where µm 6= 1. Such a situation

may arise when there are particles within the matrix that

are not within a chain. These particles may contribute

little to the desired field dependency of the composite yet

may act to increase the effective permeability of the matrix

Figure 3. Particle saturation model. Quantities are (analogous to the concept of effective dielectric constant

consistent with those defined in figure 2. Letters in

parentheses indicate different regions: (s) region where

in electrorheological fluids discussed by Adriani and Gast

particle is saturated (shaded), (u) region where particle is 1988). The following area ratio can be calculated

unsaturated, (m) matrix region with assumed relative

As π(r 2 − s 2 ) 3

permeability µm = 1. Letters in parentheses also = 2

= φ 1 − α2 . (14)

correspond to subscripts used in theory development. A y 2

Now, by substituting equations (13) and (14) into (10), the

It is assumed that the flux through the unsaturated quantity α as a function of B can be solved for in terms of

and saturated particle regions is uniformly distributed and known parameters.

remains constant, i.e., 8p = Bp Ap = Bs As = Bu Au . We now seek to develop a relationship between B and

Given that the reluctance of the matrix Rm and the H , the applied field. It is known that

reluctance of the particle Rp are in parallel, the flux

µ0 H = B − Jf (15)

distribution between the two regions can then be expressed

as where hJf i is the average polarization density of the

1 composite. Since it has been assumed that µm = 1, all

8p = Bs As = BA (10)

1 + Rp /Rm polarization is due to the polarization of the particles such

that

where As is the particle area at x = s, and A = y 2 is the

µ0 H = B − φ Jp (16)

total area. It is further assumed that the reluctance of the

particle is the sum of the reluctance of the unsaturated and where hJp i is the average polarization density of the

saturated regions of the particle: particles and may be calculated by

Z s Z r

1

Rp = Ru + Rs Jp = J π r 2

−x 2

dx+ J π r 2

−x 2

dx

Z s 2/3π r 3 0

x s

2 1 2 r −s s

= dx + (17)

µp µ0 0 π(r − x )

2 2 µ0 π(r 2 − s 2 ) where Js is the saturation polarization of the particles and

2 r −s Jx is the polarization density at a distance x within the

' (11)

µ0 π(r 2 − s 2 ) unsaturated region of the particle and may be written as

Jx = Bs . (18)

(r 2 − x 2 )

2r

Rm = (12) Since, in equation (11), it has been assumed that the

µ0 (y 2 − πr 2 )

reluctance of the unsaturated portion of the particle is

where the following additional assumptions have been negligible compared to that of the saturated region (i.e.,

made: µp 1 implying that reluctance of the unsaturated all of the field appears across the saturated region), it can

region is negligible; flux lines are perpendicular to the be stated that Bs ≈ Js + µ0 H , which when combined with

secants that define the saturated region; the relative (16) and (17) yields

permeability of the matrix and the saturated portion of the Z

3/2φ s 2

particle are unity, i.e., µm = µs = 1; and for the sake µ0 H = B − 3 Js + µ0 H r − s 2 dx

r 0

of brevity the gap between particles within a chain are Z r

assumed negligible, i.e., h = 1. Inclusion of h > 1 is not

+ Js r 2 − x 2 dx . (19)

difficult but would detract from the clarity of exposition s

sought here. Integration of equation (19) with some algebra yields

The ratio of reluctances required by equation (10) can

now be calculated as B − φ(1 − α 3 )Js

µ0 H = (20)

Rp 2/3φ − 1 1 + 3/2φα 3

=k (13)

Rm (1 + α) and the average polarization density (or intrinsic induction)

of the composite is hJf i = B − µ0 H = φhJp i, where, from

where α = s/r, and particle volume fraction φ = 2π r 2 /3y 2 equation (16), the average particle polarization density is:

has been substituted, and k ≥ 1 is a factor that has been

3/2α 3 B + (1 − α 3 )Js

added to accommodate for magnetic interaction between Jp = Jp = . (21)

adjacent particle chains and packing arrangements that are 1 + 3/2φα 3

610

A magnetorheological material behaviour model

Figure 4. Magnetic induction curves for three MR fluids of Figure 5. Experimental yield stress as a function of applied

different iron volume percents. Experimental (thin lines) magnetic field for two MR fluids containing approximately

and model (thick lines) results are shown. 30% iron by volume. Theoretical model results are also

shown for k = 8 (solid) and k = 5 (broken).

3. Magnetorheological fluids

3.2. Magnetorheological effect

3.1. Magnetic properties of MR fluids

The magnetic properties of three MR fluid samples were Experimental evidence has confirmed that MR fluids in

assessed using a magnetic hysteresigraph (KJS Assoc. Inc., the presence of a magnetic field exhibit both a pre-yield

Model HG-500, per ASTM A773-91). The fluid samples regime, characterized by an elastic response, and a post-

contained three different iron loadings: 10%, 20% and 30% yield regime, characterized by a viscous response. The

by volume. The magnetic induction curves (also called the transition between these two regimes has been reported to

B–H curves) of the three samples are shown in figure 4. occur at a yield strain on the order of 0.5% (Weiss et al

Also shown are theoretical model results computed from 1994). Since MR fluids typically operate in a continuous

equation (20). As the theory predicts, magnetic induction yield regime, they are usually characterized by their field

increases with field strength until saturation of the fluid dependent yield stress.

occurs. This can be seen to occur at an intrinsic induction Figure 5 shows published results of yield stress for

of φJs . For example, the MR fluid sample loaded with 30% two MR fluids formulated with approximately 30% (V/V)

iron (which in bulk form saturates at 2.1 T) can be seen carbonyl iron (Lord 1994, Weiss et al 1993). Also

to saturate at about (0.3)(2.1 T) = 0.63 T. A very gradual shown are theoretical model results for two different values

increase in fluid induction is observed after saturation of the of parameter k (from equations (7b) and (21)). The

fluid. This effect—which has been observed during testing model results are seen to be in relatively good agreement

of other MR fluids (Carlson 1996)—is attributed to particle with the experimental data. The figure suggests that the

restructuring over time (Felici et al 1994) and increasing experimentally applied fields were not sufficient to saturate

field. The permeabilities of these fluids were found to be the MR fluid. This is suggested by the trend demonstrated

between approximately 2 µ0 and 6 µ0 when measured at by the model and also by the observation that increases

very low fields. These permeabilities are consistent with in field at higher experimental fields are still resulting in

results of similar experiments conducted by Göktürk et al corresponding substantial increases in yield stress.

(1993). It is anticipated that experimental hysteresigraph results

Parameter k, which was introduced in equation (13), can be used to calibrate the theoretical model. As was

was adjusted to fit the model to the experimental data. done in figure 4, such a calibration entails choosing a

Recall that parameter k is used to account for magnetic k that allows for a good fit between the model and the

interactions other than those between adjacent particles experimental induction curves. The values of k, which

within a chain. The values of k used to fit the model were are weakly dependent upon iron volume fraction, can then

5.0, 4.6, and 4.4 for the 30%, 20% and 10% iron by volume be used with the model for characterization and design

MR fluid samples, respectively. Since these values are purposes. Recall that k = 5 was used in conjunction with

accurate within about 10%, it can be seen that the model, the 30% (V/V) iron MR fluid sample in figure 4. The

when applied to MR fluids, is relatively insensitive to the experimental data in figure 5 can be seen to fall to the right

parameter k. In other words, a value of, say, k = 4.7 would of the theoretical model result for k = 5. It is speculated

provide reasonable model accuracy over a wide range of that this discrepancy is a result of losses in the magnetic

iron volume fractions. circuit used to generate the experimental results.

611

M R Jolly et al

segments (shaded) are 20 mm by 7.5 mm by 1.0 mm thick

and are sandwiched between an inner iron plate and two

outer iron plates. The vertical arrow indicates the direction

of applied field.

4. Magnetorheological elastomers

in a mould using silicone oil loaded with a specified volume Figure 7. The response of elastic modulus to applied field

percent of carbonyl iron particles of a 3–4 µm mean for 10% (h = 1.29, k = 5), 20% (h = 1.08, k = 12) and 30%

diameter (see figure 6). This formulation was then cured (h = 1.0, k = 15)) iron by volume elastomer specimens.

in the presence of a magnetic field of 0.8 × 106 A m−1 ◦

Experimental data (×, , M) and theoretical model data

(——) are shown.

applied in the direction shown in figure 6. This field

causes parallel particle chains to form while the silicone

is still liquid. Upon crosslinking (during which polymer

molecules interconnect), this particle structure is locked in Because the maximum change in modulus is independent

place. Three double lap shear specimens of MR elastomer of parameter k, these two parameters (k and h) can be

were prepared containing 10, 20 and 30% iron by volume. adjusted independently to best match the model with the

Testing of the double lap shear specimens was data. It can be seen that an increase in particle volume

conducted using a Dynastatr material testing system. This fraction results in a pronounced increase in k, implying that

system applies a fixed oscillatory strain to the specimen magnetic interaction between neighboring particle chains

and measures the amplitude and phase of the output is increasing. This is consistent with intuition because

force, from which stress and modulus can be calculated. as particle volume fraction increases, the distance between

Testing involved recording the complex modulus of various neighbouring chains decreases. It is also noted that there is

specimens at various frequencies, strains and applied much greater sensitivity to k when the model is applied to

magnetic fields. Magnetic fields were applied to the test MR elastomers as compared to MR fluids. This is attributed

specimens using a horseshoe-shaped electromagnet with to variations in particle structure for the two cases, resulting

poles that efficiently focused magnetic flux across the from the corresponding variations in the level of particle

elastomer segments in the direction shown in figure 6. The mobility in the presence of a field. It was also observed

induction field (in Tesla) across the elastomer segments was that as volume fraction of iron increases, the parameter

experimentally measured using an integrating flux meter h decreases suggesting that gaps between particles within

(Walker Scientific, Model MF-3D) and a sense coil wrapped a chain decreases. It is speculated that at lower volume

directly around the elastomer segments. fractions, particle forces that induce tight, gap-free particle

Figure 7 shows the effect of induced composite flux

chains are lower within the precured elastomer as a result

density on elastic modulus for the three test specimens. As

of an increase in the mean distance between particles.

can be seen, the maximum change in modulus increases

Onset of particle chain yielding in elastomer composites

monotonically with increasing volume percentage of iron.

has been observed in the vicinity of 1–2% strain (Jolly et

While the change in modulus increases to nearly 0.6 MPa

al 1996). As shown in figure 8, this yielding is manifested

as iron loading increases to 30% (V/V), we see from

table 1 that the zero field modulus also increases with by a pronounced drop off in the magnetorheological effect

particle loading. As a result, the percentage of maximum and an increase in field dependent energy dissipation

increase in modulus for the three samples remains relatively (tan δ). The theoretical yield strain has been observed

constant between 30% and 40%. The model results provide to be much higher than experimental evidence indicates.

reasonable predictions for the maximum change in modulus As with MR fluids, an explanation for this discrepancy

obtained at large saturating flux densities for the 20% (V/V) is that the majority of strain and the ultimate yielding of

and 30% (V/V) iron samples. Once again, in using the a given chain occurs between a single (or a few) pairs

present model at intermediate fields, the parameter k, which of particles. In other words, at a local level, it is likely

accounts for magnetic interaction between neighbouring that the theoretical yield strain is achieved, but the strain

particle chains, must be adjusted in order to ‘fit’ the averaged over an entire chain is considerably smaller. This

model to the experimental data. In addition, parameter phenomenon is attributed to imperfect chain structures and

h, which accounts for gaps between particles in a chain, non-uniformity in particle geometry and chain structure.

can be adjusted to match the maximum change in modulus Still, the solids exhibit a yield strain that is several times

predicted by the model to that observed experimentally. higher in magnitude than that of analogous MR fluids.

612

A magnetorheological material behaviour model

Table 1. Enumeration of the nominal absolute modulus (no field applied), the experimental maximum change in modulus for

specimens tested at 1.0% strain and 2.0 Hz, and the maximum change in modulus predicted by the model assuming no gaps

between particles (h = 1).

modulus, Max. change in modulus,

no field modulus, exper. model, h = 1

Test specimen (MPa) (MPa) (% change) (MPa)

30% (V/V) iron 1.80 0.56 (31%) 0.55

20% (V/V) iron 0.74 0.29 (39%) 0.36

10% (V/V) iron 0.26 0.08 (30%) 0.17

◦

Figure 8. The effect of peak strain on field induced change in modulus ( ) and change in tan δ (M). This data corresponds to

the 30%(V/V) iron specimen measured at 10 Hz and 0.85 T.

was also compared with model results. Once again it was

A model that examines the behaviour of MR materials observed that the model could be calibrated to provide a

has been presented. The model is based on the dipolar good fit with experimental data. The maximum change in

interaction of particles within an assumed structure. This modulus was observed to increase monotonically with iron

dipolar model was then augmented with a proposed loading—nearly 0.6 MPa was observed with an iron loading

mechanism of how magnetic flux density distributes itself of 30% (V/V). However, it was also observed that the

within the particle network. This mechanism takes into zero field modulus increases with particle loading such that

account magnetic non-linearities associated with the gradual the percentage of maximum increase in modulus remained

saturation of the permeable particles as applied field relatively constant between 30% and 40%.

increases. The theory is capable of examining both the Ongoing work on deterministic modelling of MR

magnetic and mechanical properties of MR materials. material behaviour will examine the magnetic properties

The developed theory was compared with experimental of more complex particle structures.

data taken on MR fluids and elastomers. Magnetic and post-

yield properties of MR fluids were examined. In particular,

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