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A continuum model of magnetic field induced viscoelasticity in magnetorheological

Magnetorheological fluids experience significant changes when an external magnetic field is applied. Examples are fast and reversible acquisition of solid-like properties and a strong magnetoviscous effect. This makes them suitable for many applications, like shock absorbers, dampers or clutches. It is of practical importance to construct a macroscopic model, which is able to reproduce the behavior of MR fluids in many different geometries and on macroscopic length and time scales that are actually used in applications.

We have constructed a basic model, which takes into account the variables of the strain field and the magnetization. The motivation behind the inclusion of these variables is the following.

Under the application of an external magnetic field, columns of magnetic particles are formed.

They are the underlying reason for the observed solid-like properties. We model the magnetic properties by the magnetization, which is a variable included already in ferrofluids, while the solid-like properties are captured by the strain field εij. To discuss the rheological behavior of the MR fluid we include the equation for the linear momentum.

The statics of the MR fluid can be split into the magnetic part, which describes the induced magnetization, and the elastic energy associated with the deformation of the columns. It is described by the energy density (εij,M,g)

= 0−µ0HiMi+ 1

2αM2+1

4β(M2)2+ 1

2cijklεijεkl−1

ijklεijMkMl+ 1

2ρg2. (2.45) The coupling to an external magnetic field, ∼ µ0H, ensures the induced magnetization to be parallel to the field, while the next two terms describe the energy associated with the magnitude of the magnetization (modulus)M ≡√

M2. The elastic energy is described by the term∼cijkl. To ensure that elasticity vanishes, when there are no columns, the phenomenological coefficients

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A continuum model of magnetic field induced viscoelasticity in magnetorheological fluids

of cijkl are proportional toM2,

cijkl =c1M2δijδkl+c2M2ikδjlilδkj), (2.46) with c1 corresponding to compressible and c2 to shear strains. In the statics we have included a magnetostriction term ∼γijkl, which produces as one of the consequences, the tilting of the chains or compression induced magnetization,

γijkl1δijδkl2ikδjlilδkj). (2.47) As mentioned we model the dynamic interplay of the linear momentum, the magnetization and the strain field, which is described by the following equations

d

dtgi+∇j(pδij −ψijijthij) = 0, (2.48) d

dtMi+ijkMjωk+Xi = 0, (2.49) d

dtεijkjivkkijvk−Aij +Yij = 0, (2.50) where ψij is the elastic stress. The viscoelastic properties of MR fluids are captured by considering a relaxing strain variable. In Eq. (2.50) this is contained by the term Yij

1/τ

ijklψkl, where 1/τ

ijkl takes the form 1/τ

ijkl = 1

τ1M02δijδkl+ 1

τ2M02ikδjljkδil). (2.51) We first studied the influence of a static shear deformation. The upper plate is moved along the x axis, perpendicularly to the columns. This is a common experimental technique to determine the stress-strain curves. Experimental results show that the elastic stress first increases linearly with the shear strain Γ. If one increases the strain further a saturation in the elastic stress is observed. In our model, the elastic stress is simply

ψxz =c2M2Γ−γ2MxMz, (2.52) where the magnetization M is determined from

µ0H = αMz+c2Γ2Mz −γ2ΓMx, (2.53) 0 = αMx+c2Γ2Mx−γ2ΓMz. (2.54) The elastic shear stress was calculated as a function of the shear strain, see Fig. 2.13. We find a quadratic dependence of the static yield stress ψxzyield as a function of the magnetic field, in accordance with the experiments,

ψxzyield ≈ 3√ 3 16

√αc2

1− 3

16 γ22 αc2

µ20H2

α2 . (2.55)

A continuum model of magnetic field induced viscoelasticity in

magnetorheological fluids 31

μ0H=0.1 T μ0H=0.2 T μ0H=0.3 T

0.000 0.01 0.02 0.03 0.04 0.05 0.06

2 4 6 8

Γ ψxz[Pa]

Figure 2.13: The elastic shear stress as a function of the shear strain γ2 = 0 at three different values of the applied magnetic field. The black dashed parts of the curves represent the unstable regime, where the elastic shear stress decreases with the shear strain. Figure taken from Ref. [147].

A desirable property of MR fluids is a large yield stress. This can to some extent be achieved by a large magnetic field, however at large magnetic fields the magnetization saturates and with it also the yield stress. It was found that compressing the MR fluid uniaxially along the columns increases the shear yield stress, which can be understood by the fact that the compression makes the columns thicker, which can better resist the forces, compare Fig. 2.14. We have found that the magnetostriction coefficient ∼ γ1 accounts for these experimental findings. As a result of the compression, the magnetization Mz increases due to the magnetostrictive coupling ∼ γ1

(Mx vanishes in the γ2 = 0 approximation), Mz ≈ µ0H

(α+c2Γ2)+ γ1

¯

c1µ0HP. (2.56)

This leads to an increase of the yield stress linearly in the pressure for small pressures,

ψxzyield(P) =ψyieldxz (0) +kP, (2.57)

where ψyieldxz (0) is the static yield stress without compression, and the slope k is k≈ 9

32 γ1

¯ c1

r3c2

α . (2.58)

Dynamically, we have investigated the rheology of MR fluids under the influence of a steady shear and an oscillatory shear. We assume simple shear with a linear velocity profile of the form v= ˙γzeˆx, where the so-called shear rate is constant for a steady shear flow, ˙γ = ˙γ0, and time-dependent for oscillatory flow, ˙γ = ˙γ0cos(ωt), with ω the oscillatory frequency.

The quantity of interest is the total stress tensor, the momentum density current in Eq. (2.48), contains the elastic stress tensor ψij, as well as the dissipative and reversible phenomenological parts σijD and σRij,

−σtotxz2γ˙ + 2c2M2εxz+ 1

2(1−2cR20HMx+ 2cR2MxMz(α+βM2+ 4c2ε2xz). (2.59)

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A continuum model of magnetic field induced viscoelasticity in magnetorheological fluids

Figure 2.14: A schematic of the MR fluid in the uncompressed (left) and compressed state (right). The columns are thicker when the MR fluid is compressed, which corresponds in our model to a higher value of magnetization, Eq. (2.56).

We could produce flow curves, i.e. shear stress as a function of the shear rate, that are characterized by a fast initial increase at small shear rates, a peak at intermediate shear rates and a linear increase at large shear rates, see Fig. 2.15. The peak structure arises due to the fast increase of the elastic stress for small shear rates. At intermediate shear rates the magnetization starts to vanish quickly with the shear rate, which decreases the elastic stress contribution. Finally the flow curves converge to a linear increase of the shear stress with the shear rate given by the suspension viscosity ν2.

μ0H=0.1 T μ0H=0.2 T μ0H=0.3 T

0 20 40 60 80

0 5 10 15 20 25

γ[s-1] -σxztot[Pa]

Figure 2.15: The shear stress −σxztot as a function of the steady shear rate at three different values of the applied magnetic field. Figure taken from Ref. [147].

In the oscillatory shear mode, we were interested in the complex shear modulusG=G0+iG00, defined as the ratio of the shear stress σxztot, Eq. (2.59), and the imposed strain −γ ≡ γ/iω,˙ G = σxztot/γ. The real, G0, and the imaginary part, G00, are the storage and the loss modulus, describing the reactive and dissipative response, respectively.

Experimental results show that the storage modulus is larger than the loss modulus at

A continuum model of magnetic field induced viscoelasticity in

magnetorheological fluids 33

intermediate frequencies and that both increase with increasing magnetic field, which we could qualitatively reproduce, see Fig. 2.16. This means that the system behaves more like a solid than a liquid, which is expected, since a small amplitude shear oscillation can only slightly influence the strength of the columns. For smaller frequencies, the numerical results show that the system behaves, as expected, more like a liquid than a solid, Fig. 2.16.

For low frequencies, the storage modulus increases quickly with frequency and then saturates for larger frequencies. This can be seen in Fig. 2.16. The initial rise of the storage modulus is quadratic in the frequency

G0 ≈α

4(1 + 2cR2)2τm2 +c2τel2

M02ω2, (2.60)

while for larger frequencies the plateau value G0

Figure 2.16: Storage modulus G0 (left) and loss modulus G00 as a function of the frequency at three different values of the applied magnetic field. Figure taken from Ref. [147].

The loss modulus on the other hand, has a slightly more complicated behavior. Experimentally one has observed a maximum and a minimum in the frequency dependence of the loss modulus [148, 149]. We find that the frequency of the minimum ωmin shifts linearly with the field, which is a testable prediction, while the viscosity term needs to be subtracted first from the loss modulus, g00(ω) = (G00(ω)− ν2ω)/µ0H2. Since the characteristic time scales, τm and τel are independent of magnetic field, the master curves are obtained without the need to rescale the frequency variable.

We also discussed the dependence of the absolute value of the complex shear modulus

|G| =p

(G0)2+ (G00)2 on the frequency. After the initial linear increase, governed by the loss

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A continuum model of magnetic field induced viscoelasticity in magnetorheological fluids

modulus there is a plateau at intermediate frequencies, which is basically given by the plateau of the storage modulus G0, Eq. (2.61), since the loss modulusG00 is much smaller there. For high frequencies the loss modulus is dominating again, and|G|increases linearly with the frequency.

This scenario applies to the case of (almost) equal elastic and magnetic time scales. If these time scales are sufficiently well separated, a somewhat different behavior of |G|is found.

After the very steep initial rise a very narrow plateau is found at rather low frequencies, which is approximately of height c2M02 (for τel τm) and 14(1 + 2cR2)2αM02 (for τel τm). At intermediate frequencies |G| slowly increases to the combined plateau G0, Eq. (2.61), and finally converges to the asymptotic behavior independent of the relaxation times.

References 35