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Transient magnetorheological response of magnetoactive elastomers to step and pyramid excitations
(2016)
Transient rheological response of magnetoactive elastomers is experimentally studied using dynamic torsion at a fixed oscillation frequency in temporally stepwise changing magnetic fields and oscillation amplitudes. For step magnetic-field excitations, at least three exponential functions are required to reasonably describe the time behavior of the storage shear modulus over long time scales (>10(3) s). The deduced characteristic time constants of the corresponding rearrangement processes of the filler network differ approximately by one order of magnitude: tau(1) less than or similar to 10(1) s, tau(2) similar to 10(2) s, and tau(3) similar to 10(3) s. The sudden imposition of the external magnetic field activates a very fast rearrangement process with the characteristic time under 10 s, which cannot be determined more precisely due to the measurement conditions. Even more peculiar transient behavior has been observed during pyramid excitations, when either the external magnetic field was first stepwise increased and then decreased in a staircase manner at a fixed strain amplitude gamma or the strain amplitude gamma was first stepwise increased and then decreased in a staircase manner at a fixed magnetic field. In particular, the so-called "cross-over effect'' has been identified in both dynamical loading programs. This cross-over effect seems to be promoted by the application of the external magnetic field. The experimental results are discussed in the context of the specific rearrangement of the magnetic filler network under the simultaneous action of the external magnetic field and shear deformation. Striking similarities of the observed phenomena to the structural relaxation processes in glassy materials and to the jamming transition of granular materials are pointed out. The obtained results are important for fundamental understanding of material behavior in magnetic fields as well as for the development of devices on the basis of magnetoactive elastomeric materials.
Magnetodielectric properties of magnetoactive elastomers comprising micrometer-sized iron particles dispersed in compliant elastomer matrices are experimentally studied in stepwise time-varying dc magnetic fields. It is found that imposition of magnetic field significantly increases both the effective lossless permittivity of these composite materials as well as their effective conductivity. These magnetodielectric effects are more pronounced for larger concentrations of soft-magnetic filler particles and softer elastomer matrices. The largest observed relative change of the effective dielectric constant in the maximum magnetic field of 0.57 T is of the order of 1000%. The largest observed absolute change of the loss tangent is approximately 0.8. The transient response of the magnetodielectric effect to a step magnetic-field excitation can be rather complex. It changes from a simple monotonic growth with time for small magnetic-field steps (<0.1 T) to a non-monotonic behavior with a significant rapidly appearing overshoot for large magnetic-field steps (>0.3 T). The settling time to the magnetic-field step excitation can reach roughly 1000 s and it depends on the applied magnetic field and sample composition. There is also significant hysteresis of the magnetodielectric effect on the externally applied magnetic field. These findings are attributed to the rearrangement of ferromagnetic filler particles in external magnetic fields. The results will be useful for understanding and predicting the transient behavior of magnetoactive elastomers in applications where the control magnetic field is time dependent. (C) 2017 Elsevier Ltd. All rights reserved.
The dynamic shear modulus of magnetoactive elastomers containing 70 and 80 mass % of carbonyl iron microparticles is measured as a function of strain amplitude via dynamic torsion oscillations in various magnetic fields. The results are presented in terms of the mechanical energy density and considered in the framework of the conventional Kraus model. The form exponent of the Kraus model is further related to a physical model of Huber et al. [Huber et al., J. Phys.: Condens. Matter 8, 409 (1996)] that uses a realistic representation for the cluster network possessing fractal structure. Two mechanical loading regimes are identified. At small strain amplitudes the exponent beta of the Kraus model changes in an externally applied magnetic field due to rearrangement of ferromagnetic-filler particles, while at large strain amplitudes, the exponent beta seems to be independent of the magnetic field. The critical mechanical energy characterizing the transition between these two regimes grows with the increasing magnetic field. Similarities between agglomeration and deagglomeration of magnetic filler under simultaneously applied magnetic field and mechanical shear and the concept of jamming transition are discussed. It is proposed that the magnetic field should be considered as an additional parameter to the jamming phase diagram of rubbers filled with magnetic particles.
Ultra-small-angle neutron scattering (USANS) experiments are reported on isotropic magnetoactive elastomer (MAE) samples with different concentrations of micrometer-sized iron particles in the presence of an in-plane magnetic field up to 350 mT. The effect of the magnetic field on the scattering curves is observed in the scattering vector range between 2.5 x 10(-5) and 1.85 x 10(-4) angstrom(-1). It is found that the neutron scattering depends on the magnetization history (hysteresis). The relation of the observed changes to the magnetic-field-induced restructuring of the filler particles is discussed. The perspectives of employing USANS for investigations of the internal microstructure and its changes in magnetic field are considered.
In composite materials, with field-dependent restructuring of the filler material (changes in the mutual arrangement of inclusions), the presence of an external magnetic field induces anisotropy of the dielectric properties, even if the composite is isotropic in the absence of an external field. A modified effective medium approximation is proposed for the calculation of the components of effective permittivity within a class of composites with reconfigurable microstructure, where both phases (the filler and the matrix) are isotropic and the inclusions have spherical shape. The effective physical properties are calculated in the parallel and perpendicular directions to an applied field. The appearance of the anisotropy of the permittivity is simulated by the introduction of two not-equal, possibly variable (field-dependent) percolation thresholds. The implications, of the proposed theoretical approach, are demonstrated for the case of the dielectric properties of magnetoactive elastomers (MAEs). In MAEs with soft polymer matrices, the mutual arrangement of micrometer-sized magnetic inclusions can significantly change in an applied magnetic field. A reasonable agreement between theory and experiment at a measurement frequency of 1 kHz is found, and is improved in comparison to the previous models. The components of the effective permittivity tensor, characterizing the dielectric properties along the direction of the applied magnetic field and in the orthogonal direction, grow with an increasing field. This growth is more pronounced for the permittivity component in the field direction. The possible extensions of the theoretical model and future directions of research are discussed. The presented theoretical approach can be useful for the application-driven development of a number of smart materials, in particular electro- and magnetorheological gels, elastomers and fluids.
Elongations of magnetoactive elastomers (MAEs) under ascending–descending uniform magnetic fields were studied experimentally using a laboratory apparatus specifically designed to measure large extensional strains (up to 20%) in compliant MAEs. In the literature, such a phenomenon is usually denoted as giant magnetostriction. The synthesized cylindrical MAE samples were based on polydimethylsiloxane matrices filled with micrometer-sized particles of carbonyl iron. The impact of both the macroscopic shape factor of the samples and their magneto-mechanical characteristics were evaluated. For this purpose, the aspect ratio of the MAE cylindrical samples, the concentration of magnetic particles in MAEs and the effective shear modulus were systematically varied. It was shown that the magnetically induced elongation of MAE cylinders in the maximum magnetic field of about 400 kA/m, applied along the cylinder axis, grew with the increasing aspect ratio. The effect of the sample composition is discussed in terms of magnetic filler rearrangements in magnetic fields and the observed experimental tendencies are rationalized by simple theoretical estimates. The obtained results can be used for the design of new smart materials with magnetic-field-controlled deformation properties, e.g., for soft robotics.
Large twists of a soft tube (hollow cylinder) in helical magnetic fields are presented for the first time. Such a phenomenon is usually denoted as the Wiedemann effect. The tube is fabricated from a soft magnetoactive elastomer material with the shear modulus of about 56 kPa. The composite material comprises 80 mass% of micrometer-sized iron particles embedded into a polydimethylsiloxane matrix. The circular magnetic field is generated by an electric current in a straight wire passing through the inner hole of the tube. The maximum value of approximately 350″/cm is observed in a longitudinal magnetic field of a few kA/m overlapped with a circumferential magnetic field of about 1.4 kA/m on the surface of the inner hole. A pronounced hysteresis in the dependence of the Wiedemann effect on the circular magnetic field is found. The ways to enhance the Wiedemann twist in magnetoactive elastomers are discussed. The observed large effect is promising for application in magnetic-field controlled torsional actuators, in particular for soft robotics.
In this work, the resonance enhancement of magnetoelectric (ME) coupling at the two lowest bending resonance frequencies was investigated in layered cantilever structures comprising a magnetoactive elastomer (MAE) slab and a commercially available piezoelectric polymer multilayer. A cantilever was fixed at one end in the horizontal plane and the magnetic field was applied horizontally. Five composite structures, each containing an MAE layer of different thicknesses from 0.85 to 4 mm, were fabricated. The fundamental bending resonance frequency in the absence of a magnetic field varied between roughly 23 and 55 Hz. It decreased with the increasing thickness of the MAE layer, which was explained by a simple theory. The largest ME voltage coefficient of about 7.85 V/A was measured in a sample where the thickness of the MAE layer was ≈2 mm. A significant increase in the bending resonance frequencies in the applied DC magnetic field of 240 kA/m up to 200% was observed. The results were compared with alternative designs for layered multiferroic structures. Directions for future research were also discussed.
Surface topographical modifications of a soft magnetoactive elastomer (MAE) in response to variable applied magnetic field are investigated. The analysis is performed in situ and is based on optical microscopy, spread optical reflection and optical profilometry measurements. Optical profilometry analysis shows that the responsivity of magnetic field-induced surface roughness with respect to external magnetic field is in the range of 1 mu m/T. A significant hysteresis of surface modifications takes place for increasing and decreasing fields. Investigations of shape of sessile water droplets deposited on the MAE surface reveal that field-induced topographical modifications affect the contact angle of water at the surface. This effect is reversible and the responsivity to magnetic field is in the range of 20 degrees/T. Despite the increased surface roughness, the apparent contact angle decreases with increasing field, which is attributed to the field-induced protrusion of hydrophilic microparticles from the surface layer.
The voltage response to pulsed uniform magnetic fields and the accompanying bending deformations of laminated cantilever structures are investigated experimentally in detail. The structures comprise a magnetoactive elastomer (MAE) slab and a commercially available piezoelectric polymer multilayer. The magnetic field is applied vertically and the laminated structures are customarily fixed in the horizontal plane or, alternatively, slightly tilted upwards or downwards. Six different MAE compositions incorporating three concentrations of carbonyl iron particles (70 wt%, 75 wt% and 80 wt%) and two elastomer matrices of different stiffness are used. The dependences of the generated voltage and the cantilever's deflection on the composition of the MAE layer and its thickness are obtained. The appearance of the voltage between the electrodes of a piezoelectric material upon application of a magnetic field is considered as a manifestation of the direct magnetoelectric (ME) effect in a composite laminated structure. The ME voltage response increases with the increasing total quantity of the soft-magnetic filler in the MAE layer. The relationship between the generated voltage and the cantilever's deflection is established. The highest observed peak voltage around 5.5 V is about 8.5-fold higher than previously reported values. The quasi-static ME voltage coefficient for this type of ME heterostructures is about 50 V/A in the magnetic field of approximate to 100 kA/m, obtained for the first time. The results could be useful for the development of magnetic field sensors and energy harvesting devices relying on these novel polymer composites.
In this work, multiferroic cantilevers comprise a layer of a magnetoactive elastomer (MAE) and a commercially available piezoelectric polymer-based vibration sensor. The structures are fixed at one end in the horizontal plane and the magnetic field is applied vertically. First, the magnetoelectric (ME) response to uniform, triangle-wave magnetic fields with five different slew rates is investigated experimentally. Time and field dependences of the generated voltage, electric charge, and observed mechanical deflection are obtained and compared for four different thicknesses of the MAE layer. The ME responses to triangular and sinusoidal wave excitations are examined in contrast. Second, the ME response at low frequencies (≤3 Hz) is studied by the standard method of harmonic magnetic field modulation. The highest ME coupling coefficient is observed in the bias magnetic field strength of ≈73 kA/m and it is estimated to be about 3.3 ns/m (ME voltage coefficient ≈ 25 V/A) at theoretically vanishing modulation frequency (f→0 Hz). Presented results demonstrate that the investigated heterostructures are promising for applications as magnetic-field sensors and energy harvesting devices.
A surface relief grating with a period of 30 mu m is embossed onto the surface of magnetoactive elastomer (MAE) samples in the presence of a moderate magnetic field of about 180 mT. The grating, which is represented as a set of parallel stripes with two different amplitude reflectivity coefficients, is detected via diffraction of a laser beam in the reflection configuration. Due to the magnetic-field-induced plasticity effect, the grating persists on the MAE surface for at least 90 h if the magnetic field remains present. When the magnetic field is removed, the diffraction efficiency vanishes in a few minutes. The described effect is much more pronounced in MAE samples with larger content of iron filler (80 wt%) than in the samples with lower content of iron filler (70 wt%). A simple theoretical model is proposed to describe the observed dependence of the diffraction efficiency on the applied magnetic field. Possible applications of MAEs as magnetically reconfigurable diffractive optical elements are discussed. It is proposed that the described experimental method can be used as a convenient tool for investigations of the dynamics of magnetically induced plasticity of MAEs on the micrometer scale.
Magnetoactive elastomers (MAEs) are promising materials for realization of magnetic field-controlled soft actuators. Herein, a systematic investigation of magnetic field-induced macroscopic deformations of soft MAE cylinders with a diameter of 15 mm in uniform quasi-static magnetic fields directed parallel to the cylinder’s axis is reported. The measurements were based on image processing. Thirty-six MAE samples differing in the weight fraction of the iron filler (70 wt%, 75 wt% and 80 wt%), alignment of filling particles, and the aspect ratio (0.2, 0.4, 0.6, 0.8, 1.0 and 1.2) were fabricated. MAE cylinders exhibited high relative change in height (up to 35% in the field of 485 kA/m) and lateral contraction. The dependence of the maximum extensional strain on the aspect ratio was obtained and compared with theoretical considerations. A concave dent was formed on the free circular base in magnetic fields. This concavity was characterized experimentally. A significant volumetric strain of the order of magnitude of 10% was calculated in MAEs for the first time. In consequently repeated magnetization cycles, the remanent extensional strain significantly increased after each cycle. The results are qualitatively discussed in the framework of the modern views on the magnetically induced macroscopic deformations of MAEs. The directions of further research are outlined.
Herein, the effect of an applied moderate (~240 mT) magnetic field on the work of adhesion (WoA) of mechanically soft (the shear modulus ~10 kPa) magnetoactive elastomer (MAE) samples with two different mass fractions (70 and 80 wt%) of carbonyl iron powder (CIP) is concerned. The unfilled elastomer sample is used for comparison. Due to some sedimentation of filling particles, the concentration of inclusions in thin (~10 μm) subsurface layers is different. It is shown that the WoA increases (up to 1.8-fold) on the particle-enriched side (PES) in the magnetic field and its value is higher for higher filler concentration. On the particle-depleted side (PDS), WoA does not depend on particle concentration and on the magnetic field. Adhesion and friction are coupled in MAEs. No statistically significant difference in the friction coefficient, determined from the extended Amontons´ law, depending on sample side, CIP concentration, or presence of magnetic field is found. However, the PDS in the magnetic field demonstrates significantly higher critical shear stress compared to that for the PES or PDS in the absence of magnetic field. Correlations between different surface properties are discussed. Obtained results are useful for the development of magnetically controllable soft robots.
A simple method for structuring of the surface of a magnetoactive elastomer (MAE) on the tens of micrometers scale, which capabilities extend beyond conventional mold-based polymer casting, is reported. The method relies on the ablation of the material by absorption of nanosecond infrared pulses from a commercial laser. It is shown that it is possible to fabricate parallel lamellar structures with a high aspect ratio (up to 6:1) as well as structures with complex scanning trajectories. The method is fast (fabrication time for the 7 × 7 mm2 is about 60 s), and the results are highly reproducible. To illustrate the capabilities of the fabrication method, both orthogonal to the MAE surface and tilted lamellar structures are fabricated. These magnetosensitive lamellae can be easily bent by ±45° using an external magnetic field of about 230 mT. It is demonstrated that this bending allows one to control the sliding angle of water droplets in a great range between a sticky (>90°) and a sliding state (<20°). Perspectives on employing this fabrication technology for magnetosensitive smart surfaces in microfluidic devices and soft robotics are discussed.
The significant effect of an external dc magnetic field on the splashing behavior of ethanol drops impacting on the unstructured (flat) surface of soft magnetoactive elastomers (MAEs) is reported. The Weber number corresponding to the transition between the deposition and the splashing regime is reduced by ≈20% in a moderate magnetic field of ≈300 mT. Alongside this effect, a two-fold increase of the initial deceleration of the ejection sheet is observed for the softest sample. The main underlying mechanism for the observed phenomena is believed to be the magnetic-field-induced stiffening of the MAEs. Further possible mechanisms are magnetically induced changes in the surface roughness and magnetic-field-induced plasticity (magnetic shape memory effect). The potential application areas are magnetically regulable wetting and magneto-responsive surfaces for controlling the drop splashing.
Adaptive surface microstructures are used extensively in nature to control various surface properties such as wettability, adhesion, self-cleaning, drag reduction, etc. Regulation of these properties can be achieved with the appropriate employment of a multitude of smart materials, whose characteristics/response can be controlled by noncontact stimuli, e.g., light, heat, or magnetic field. One of the very promising magneto-regulable smart materials are magnetoactive elastomers (MAEs). They are comprised of a compliant polymer matrix with embedded micrometer-sized ferromagnetic particles. The particles interact with each other and a magnetic field. This results in remarkable tunability of the physical properties of MAEs. This paper reports a fast, resilient, and tailored method for direct surface micromachining of MAEs that enables micro-structuring without mechanical contact between the tool and the material, bypassing the usual constraints of conventional fabrication methods. It is shown that it is possible to fabricate a large variety of different microstructure geometries whose precision is limited predominantly by the size of magnetic particles. Lamellar structures with a high aspect ratio (up to 6:1) oriented either perpendicularly to the surface, can be strongly bent by applying magnetic fields in the range of 0–250 mT.
Significant deformations of bodies made from compliant magnetoactive elastomers (MAE) in magnetic fields make these materials promising for applications in magnetically controlled actuators for soft robotics. Reported experimental research in this context was devoted to the behaviour in the quasi-static magnetic field, but the transient dynamics are of great practical importance. This paper presents an experimental study of the transient response of apparent longitudinal and transverse strains of a family of isotropic and anisotropic MAE cylinders with six different aspect ratios in time-varying uniform magnetic fields. The time dependence of the magnetic field has a trapezoidal form, where the rate of both legs is varied between 52 and 757 kA/(s·m) and the maximum magnetic field takes three values between 153 and 505 kA/m. It is proposed to introduce four characteristic times: two for the delay of the transient response during increasing and decreasing magnetic field, as well as two for rise and fall times. To facilitate the comparison between different magnetic field rates, these characteristic times are further normalized on the rise time of the magnetic field ramp. The dependence of the normalized characteristic times on the aspect ratio, the magnetic field slew rate, maximum magnetic field values, initial internal structure (isotropic versus anisotropic specimens) and weight fraction of the soft-magnetic filler are obtained and discussed in detail. The normalized magnetostrictive hysteresis loop is introduced, and used to explain why the normalized delay times vary with changing experimental parameters.