We study the magneto-elastic coupling behavior of paramagnetic chains in soft polymer gels exposed to external magnetic fields. To this end, a laser scanning confocal microscope is used to observe the morphology of the paramagnetic chains together with the deformation field of the surrounding gel network. The paramagnetic chains in soft polymer gels show rich morphological shape changes under oblique magnetic fields, in particular a pronounced buckling deformation. The details of the resulting morphological shapes depend on the length of the chain, the strength of the external magnetic field, and the modulus of the gel. Based on the observation that the magnetic chains are strongly coupled to the surrounding polymer network, a simplified model is developed to describe their buckling behavior. A coarse-grained molecular dynamics simulation model featuring an increased matrix stiffness on the surfaces of the particles leads to morphologies in agreement with the experimentally observed buckling effects.

One of the central appealing properties of magnetic gels and elastomers is that their elastic moduli can reversibly be adjusted from outside by applying magnetic fields. The impact of the internal magnetic particle distribution on this effect has been outlined and analyzed theoretically. In most cases, however, affine sample deformations are studied and often regular particle arrangements are considered. Here we challenge these two major simplifications by a systematic approach using a minimal dipole-spring model. Starting from different regular lattices, we take into account increasingly randomized structures, until we finally investigate an irregular texture taken from a real experimental sample. On the one hand, we find that the elastic tunability qualitatively depends on the structural properties, here in two spatial dimensions. On the other hand, we demonstrate that the assumption of affine deformations leads to increasingly erroneous results the more realistic the particle distribution becomes. Understanding the consequences of the assumptions made in the modeling process is important on our way to support an improved design of these fascinating materials.

Embedding magnetic colloidal particles in an elastic polymer matrix leads to smart soft materials that can reversibly be addressed from outside by external magnetic fields. We discover a pronounced nonlinear superelastic stress-strain behavior of such materials using numerical simulations. This behavior results from a combination of two stress-induced mechanisms: a detachment mechanism of embedded particle aggregates as well as a reorientation mechanism of magnetic moments. The superelastic regime can be reversibly tuned or even be switched on and off by external magnetic fields and thus be tailored during operation. Similarities to the superelastic behavior of shape-memory alloys suggest analogous applications, with the additional benefit of reversible switchability and a higher biocompatibility of soft materials.The term "superelasticity" expresses the capability of certain materials to perform huge elastic deformations that are completely reversible 1,2 . It was initially introduced in the context of shape-memory alloys 3-5 . These metallic materials can perform large recoverable deformations due to stress-induced phase transitions. A transition to a more elongated lattice structure accommodates an externally imposed extension. Typically, this transition shows up as a pronounced "plateau-like" regime on the corresponding stress-strain curve. On this plateau, the samples are heterogeneous with domains of already transitioned material. Then, only relatively small additional stress induces a huge additional deformation. Smart material properties are observed 6-9 : upon stress release, shape-memory alloys can reversibly find back to their initial state. They self-reliantly adapt their appearance to changed environmental conditions.In the present letter, we demonstrate that an analogous phenomenological behavior can be realized for a very different class of materials, exploiting different underlying mechanisms. Moreover, we show that during operation the behavior can be reversibly tailored from outside by external magnetic fields. All of this is achieved by employing soft magnetic gels as working materials: colloidal magnetic particles embedded in a possibly swollen elastic polymer matrix 10 . Similarly to magnetic fluids 11-18 , magnetic gels allow to reversibly adjust their material properties by external magnetic fields. In this way, switching the elastic properties 19-23 offers a route to construct readily tunable dampers 24 or vibration absorbers 25 , while the possibility to switch the shape 19,26-28 allows application as soft actuators [29][30][31] . Here, we show that magnetic gels due to the interplay between magnetic and elastic interactions likewise feature superelastic behavior: it is enabled by a detachment mechanism of embedded magnetic particle aggregates and by a reorientation mechanism of magnetic moments. Both mechanisms are stress-induced and rea) Electronic mail: pcremer@thphy.uni-duesseldorf.de b) Electronic mail: menzel@thphy.uni-duesseldorf.de spond to external magnetic fields. Therefore, su...

Ferrogels and magnetic elastomers feature mechanical properties that can be reversibly tuned from outside through magnetic fields. Here we concentrate on the question how their dynamic response can be adjusted. The influence of three factors on the dynamic behavior is demonstrated using appropriate minimal models: first, the orientational memory imprinted into one class of the materials during their synthesis; second, the structural arrangement of the magnetic particles in the materials; and third, the strength of an external magnetic field. To illustrate the latter point, structural data are extracted from a real experimental sample and analyzed. Understanding how internal structural properties and external influences impact the dominant dynamical properties helps to design materials that optimize the requested behavior.