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Byrne Advanced Manufacturing Science (AMS) Research Centre, Mechanical Engineering, University College Dublin, Belfield, Dublin 4, Ireland. ABSTRACT Smart materials are materials with properties that can be significantly altered in a controlled fashion by external stimuli, such as stress, temperature, pH, moisture, electric or magnetic fields. An elastomer comprising a matrix interspersed with micron sized ferromagnetic particles is known as a Magnetorheological Elastomer (MRE). The rheological properties of MREs (the deformation and flow behaviour under stress) are altered by the application of an external magnetic field. The characteristic response will be influenced by many factors including; the elastomer matrix, the size, distribution, composition and percentage volume of the ferromagnetic particles, and whether the ferromagnetic particles are aligned in chains or randomly dispersed. A review is presented in this paper of the rheological properties of magnetorheological elastomers and how these properties are affected by varying magnetic fields and the indicated compositional parameters. As well as describing the fundamental behaviour of MREs, various applications of MREs are analysed and compared. KEYWORDS: Smart Material, Magnetorheological Elastomer 1. INTRODUCTION TO SMART MATERIALS

Magnetorheological Elastomers (MREs) belong to a class of materials known as Smart Materials. Smart materials are classified as materials that have the ability to change one or more of their material properties under the influence of an external stimulant. Material properties can be controlled by many external factors, including application of stress, pH level, moisture content, electric fields or in the case of MREs, magnetic fields. Common examples of smart materials are memory shape alloys and piezoelectric materials. Magnetorheological materials, similar in principle to electrorheological materials, have their viscoelastic and rheological properties altered in the presence of a magnetic field. They exhibit a fast response to external stimuli, of the order of milliseconds [1].

Figure 1: Magnetorheological fluid attracted by an electro-magnetic field []

Magnetorheological materials can be fluid, gel or even a solid material such as an elastomer. Magnetorheological materials have magnetically polarisable colloidal particles suspended in some functional suspension, i.e. viscous fluid (e.g. silicone oil) or elastomer matrix (e.g. silicone rubber). A magnetorheological fluid operates on the principle that the magnetic particles are randomly distributed in the liquid when no magnetic field is applied, but then the particles acquire a magnetic polarisation and form chains in the presence of a magnetic field of sufficient strength, as indicated in figure 2 below. The strength of this chain is dependant on the magnetic field density. Following from this, it is the strength of the particle chains which determines the increase in rheological properties for the fluid [2].

Ferromagnetic Particle

Silicone Oil

Figure 2: Structure of Magnetorheological Fluid, Ferromagnetic particles in a silicone oil suspension; (a) under no magnetic field, and (b) with magnetic field applied. [3] The structure of magnetorheological fluids shows that when a magnetic field is applied the ferromagnetic particles arrange into chains (particle clusters) parallel to the magnetic field lines. Chains may interconnect and branch off forming fibrils. In order to shear the magnetorheological fluid under a magnetic field extra force must be exerted to break the cluster of chains/fibrils.

Figure 3: Magnetic induction curves for three MR fluids of different iron volume percents. Experimental (thin lines) and model (thick lines) results are shown. [4]

Most magnetic materials in use are alloys (e.g. Iron, Nickel, Cobalt), ceramics (e.g. a sintered composition of iron oxide and barium/ strontium carbonate), or rare earth magnets (e.g. neodymium and the marginally weaker samarium-cobalt magnets). These materials have a low susceptibility to elastic deformation, and ceramics are also hard and brittle. Iron or cobalt alloys are generally used for the ferromagnetic particles as they have a high permeability and a low hysteresis loss. 2. MAGNETORHEOLOGICAL ELASTOMERS

Since the discovery in 1951 of the magneto-rheological phenomenon by Thomas Rabinow [2] magnetorheological fluids have proven to be commercially viable and suited to many applications. MR fluids have many advantages over the similar electrorheological fluids, such as larger change in modulus, lower power consumption, and the avoidance of the high voltages needed for ER fluids. However there are still many concerns regarding the achievable yield stress, the stability and durability of the fluid [5]. Settling due to differences in specific gravities and wear of the magnetic particles can also lead to a reduction in the fluids performance and eventual failure of the MR device [6]. Although not suited to the all the same applications magnetorheological elastomers overcome many of these problems. Magnetorheological Elastomers (MREs) generally consist of a natural or synthetic rubber matrix interspersed with micron sized (typically 3 to 5 microns [4]) ferromagnetic particles. This solid matrix for the particles avoids some common problems such as settling of particles normally associated with MR fluids and gels. Elastomers such as rubber are used as they are generally soft and/or deformable at room temperature, elastomers can have the ability to reversibly extend from 5-700%, depending on the specific material. Pure iron is generally used for the micron sized particles in the rubber matrix, but some alloys of iron and cobalt can also be used to good effect, however they are not as common. The ferromagnetic particles are added to the elastomer before it is cured. The configuration and rigidity of the chain structures depend on several factors including the strength and distribution of the applied magnetic field [4].

35 Microns

35 Microns

Figure 4: SEM images of particles in an elastomer; (left) randomly dispersed particles, (right) particles aligned by applied magnetic field. [4]

The images in Fig.4 above are Scanning Electron Micrographs (SEMs) of ferromagnetic particles in a silicone polymeric elastomer matrix, the image on the left is an elastomer ferromagnet composite, note the randomly dispersed particles, and the image on the right is a magnetorheological elastomer, in which the aligned ferromagnetic particle chains can be clearly seen. If the elastomer, with suspended ferromagnetic particles, is cured in the presence of a magnetic field, the magnetisable particles will form chains along the direction of the magnetic field prior to the elastomer cross linking process (curing) and a MRE is produced. However if the mixture is not cured in the presence of a magnetic field, and the particles are hence left randomly distributed, an Elastomer Ferromagnet Composite (EFC) is produced. Both EFCs and MREs contain ferromagnetic particles in an elastomer matrix, differing only in their structure. Once cured, the solid elastomer matrix in an EFC prevents the ferromagnetic particles forming chains in the presence of a magnetic field, and so has many different isotropic properties to MREs once it is subjected to a magnetic field. 3. PROPERTIES OF MAGNETORHEOLOGICAL ELASTOMERS

There are numerous factors which can affect the manner in which an MRE will behave; for example, the elastomer matrix will have its own material properties of elastic modulus, density, etc. Therefore, material selection for the elastomer matrix is very important for the viscoelastic behaviour of the MRE. And similarly the material selected for the micron sized magnetisable particles will have its own affect on the overall MRE behaviour. It is assumed that the ferromagnetic particles are uniformly magnetised, which is valid if the particles are small enough (1.5m for iron). Negligible anisotropy effects in the magnetisation is also assumed, which is justified for iron and iron-cobalt alloys (due to them being cubic crystalline ferromagnetic materials. Very low eddy current loss and a low total core loss (relative to laminated steel) are also properties of MREs. [8] The maximum possible magnetic field induced change in stress (and modulus) occurs when the aligned particles become magnetically saturated. This observation supports the use of a particle material with high magnetisation saturation. Pure iron has the highest saturation magnetisation of known elements, but some alloys of iron and cobalt have even higher saturation magnetisations. Research [7] has shown that uniaxial field structured composites consisting of magnetic particles in an elastomer (a basic MRE) exhibit a larger increase in modulus than random particle distributions (such as an EFC), the increase in modulus is most significant if the applied stress is parallel to the particle alignment. Many other features of the particles such as their size/shape, distribution in the matrix and percentage volume (see figure 6) of the ferromagnetic particles in the elastomer matrix can have effects on the overall behaviour of the MRE. In general, magnetic forces arise due to the movement of electrical charge. This can occur in two ways; the movement of electrons in an electric current, which results in what is known as electromagnetism, or the quantum-mechanical spin and orbital motion of electrons in an atom. The latter of these is the fundamental force in permanent or hard magnets. Hard magnets remain magnetised when removed from a magnetic field, however soft magnets lose their magnetisation immediately when removed from the field. If a piece of iron, or other ferromagnetic material, in an unmagnetised state is placed in a weak magnetic field a magnetic moment is induced. Such a field may be produced by wrapping a current carrying electric wire around the sample or by placing it in the vicinity of a permanent magnet. Hysteresis develops as the magnetic field increases. The hysteresis loop from saturation is a characteristic of the

specimen (figure 5a). The induction hysteresis loop has a different shape (figure 5b). The hysteresis properties of ferromagnets are largely properties of arrangements of magnetic domains [9].

Induction T

0.2 0.1 0.1 0.2 0.3 -0.1 Field T -0.2 (b)

-0.3 -0.2 -0.1


0.2 0.1 0.1 0.2 0.3 -0.1 Field T -0.2 (a)

-0.3 -0.2 -0.1

Figure 5: Magnetisation (a) and induction (b) hysteresis loops of a hard magnetic material. In (a) the unit used for the y-axis is 0M, equal to the magnetic polarisation J. [9] 4. BEHAVIOUR UNDER MAGNETIC FIELDS AND VARYING COMPOSITIONAL FACTORS

Rheology is defined as the study of the deformation and flow of matter under the influence of an applied stress. The rheological properties of a magnetorheological elastomer, such as viscosity, elasticity and plasticity, can be altered in response to an applied magnetic field. And a variable magnetic field can provide controllability to these properties. Research results exhibit that the shear strength of MR materials could vary from 2-3kPa to 100kPa in response to a change of the applied magnetic field from 0 - 3000 Oe [2] (Oersted, a unit of magnetic induction) equivalent to 0 0.3 T (Tesla SI unit for magnetic field induction in free space). Test specimen 30% (V/V) iron 20% (V/V) iron 10% (V/V) iron Nominal modulus, no field (MPa) 1.80 0.74 0.26 Max. modulus change, exper. (MPa) 0.56 (31%) 0.29 (39%) 0.08 (30%) Max modulus change, model, h = 1 (MPa) 0.55 0.36 0.17

Table 1: Values of the nominal absolute modulus, 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. [4]

Ferromagnetic composites with an elastomer matrix are characterised by unique properties which are not characteristic of monolithic magnetic materials. These properties have a high susceptibility to elastic strain in the magnetic field and the dependence of magnetic permeability on stress [10].

Fig. 6: The response of elastic modulus to applied field for 10% (h = 1:29, k = 5), 20% (h = 1:08, k = 12) and 30% (h = 1:0, k = 15)) iron by volume elastomer specimens. [4] Kallio [11] studied the influence of the alignment of the magnetic particles on the composite properties with and without applied magnetic fields. It was found that the stiffness and damping properties of both isotropic and aligned MREs can be modified by applying external magnetic field. In isotropic MREs the stiffness and damping increase in the magnetic field if the filler volume fraction exceeds 15 %. The damping also increases with the increasing volume fraction of iron and it has a maximum value at 27 vol.% when measured with applied magnetic field. The damping and stiffness properties of aligned MREs depend on the mutual directions of load, magnetic field and the particle alignment in the composite. It was also found that by optimizing the particle density and alignment, either the stiffness or the damping of MREs can be increased by applying the magnetic field. Calculations by Davis [12] using finite element analysis show that for typical elastomers the increase in shear modulus due to interparticle magnetic forces at saturation is about 50% of the zero field modulus. It was concluded from this study that the zero-field (magnetic) shear modulus of material with chains of particles, which have been aligned along a magnetic field during curing, is no larger than the modulus for the same material with randomly dispersed, rigid particles. And, similar to work by others, an optimum volume fraction of Fe particles was predicted to be 27%. 5. APPLICATIONS

Due to the dynamic damping of Magnetorheological Fluids, much research has gone into their development for use in shock absorbers, clutches and brakes. These MRFs are also being developed as an innovative micro-machining method where abrasives are bonded to the ferromagnetic particles and the magnetic field is used to polish optical glass, ceramic and other

brittle materials of millimetre or sub-millimetre scale with a high efficiency [13]. Applications for Magnetorheological Elastomers include automotive bushings and engine mounts [14], where the significant changes in spring rate due to an applied magnetic field can be used to control stiffness. Ferromagnetic composites have also found many applications in sensors, converters and controlled vibration dampers [10], however their manufacture is not yet widespread with standards for production. There is some interest in developing soft, high strain materials as artificial muscles [15]. One possibility is elastomers filled with magnetic particles. When placed in a uniform magnetic field, such materials will tend to contract, an effect called magnetostiction. This contraction is due to the dependence of the composite susceptibility on strain, the susceptibility increasing along the direction of compression (in contrast, demagnetising fields can cause a material to elongate). ACKNOWLEDGEMENTS The authors would like to acknowledge that this research has been carried out as part of a project funded by Enterprise Ireland under the commercialisation technology development scheme. REFERENCES [1] A. Jorge, R. Corts, S. Leopoldo, V. Gonzlez and M. Martez, Characterisation, modelling and simulation of magnetorheological damper behaviour under triangular excitation. AZojomo Journal of Materials Online, Vol. 1, 2005. [2] M. Yalcintas and H. Dai, Magnetorheological and electrorheological materials in adaptive structures and their performance comparison. Smart Materials and Structures, Vol.8, 1999. [3] R. Tsuruizumi, T. Aoyama, H. Anzai, H.Sakurai, K.Isobe, K.Hino, K.Tanaka, Application of electrorheological fluids to precision clamping devices. Proc.4th euspen Int. Conf. 2004. [4] M. R. Jolly, J. D. Carlson, B. C. Muoz, A model of the behaviour of magnetorheological materials. Smart Materials and Structures Vol. 5 (1996) 607-614. [5] F.D. Goncalves, J.H. Koo, M. Ahmadian, A review of the state of the art in magnetorheological fluid technologies part 1: MR fluid and MR fluid models. The Shock and Vibration Digest, Vol. 38, No. 3, 203-219 (2006). [6] R.Bell, D.Zimmerman, A.Vavreck, Properties of magnetorheological fluids. Penn State Altoona Research,, 2005. [7] Z.Varga and G.Filipcsei, Smart composites with controlled anisotropy. Polymer 46 2005. [8] H. Shokrollahi and K. Janghorban, Soft magnetic composite materials (SMCs). Journal of Materials Processing Technology, 189 (2007) 1-12. [9] J. Crangle, Solid State Magnetism. Edward Arnold publishers 1991. ISBN: 0-340-54552-6 [10] S. Bednarek, Elastic and magnetic properties of heat-shrinkable ferromagnetic composites with elastomer matrix. Materials Science and Engineering B77 (2000) 120-127. [11] M. Kallio, The elastic and damping properties of magnetorheological elastomers. VTT publications, n 565, 2005 146p. [12] L.C. Davis, Model of magnetorheological elastomers. J. Applied Physics,85 1999. [13] J. B. Lu, Q. S. Yan, J. Yu, W. Q. Gao, A novel Micro Machining technology based on the Magnetorheological effect of abrasive slurry. Proc. of the 6th euspen Int. Conf. (2006). [14] L. Borcea and O. Bruno, On the magneto-elastic properties of elastomer-ferromagnet composites. Journal of the Mechanics and Physics of Solids, 49 (2001). [15] J. E. Martin, Using triaxial magnetic fields to create optimal particle composites. Composites: Part A 36 (2005) 545-548.