The dynamics of two different side-chain liquid crystalline elastomers (SCLCE) exhibiting a smectic A phase is investigated by low-frequency shear and compression experiments. We find that both the isotropic and the smectic A phase have their own characteristic viscoelastic behavior, which seems to be independent of the compound under investigation and thus universal. The relaxation in the isotropic phase shows a distribution of relaxation times, which gives rise to a scaling law of the elastic moduli with an exponent of 0.5. The viscoelastic response in the smectic A phase, however, exhibits a much broader spectrum of relaxation times containing very long-lived modes. It appears that there exists a low-frequency scaling law with an exponent of 0.3 characterizing the smectic A phase. We propose that this result stems from a transient smectic network with a very long lifetime that was set up by the smectic domains. At the phase transition, this transient smectic network disappears, which leads to a sharp decrease of the dynamic shear as well as the compression modulus.

We investigate the rheological properties of polydomain smectic A Side-Chain Liquid Crystalline Elastomers (SCLCE) by dynamic shear and compression measurements and find a very similar behavior for both experiments. We show that the dynamic shear modulus G is independent of a precompression applied to the sample. In addition, we present the first dynamic measurements of the anisotropy of G observed for the corresponding Liquid Single Crystal Elastomers (LSCE). We find that these monodomains show dynamically a dramatic difference depending on whether the shear is in a plane parallel or perpendicular to the layer normal, demonstrating the in-plane fluidity of the smectic layering.

The analysis of the phase behavior of a smectic A (SA) elastomer reveals a nematic phase existing within a small temperature range below the isotropic state. Stress‐optical measurements in the pretransformational regime of the isotropic state indicate smectic as well as nematic fluctuations yielding a critical exponent of γ = 0.65. The formation of the liquid single crystal elastomer (LSCE) at the isotropic to liquid crystalline phase transformation equals a nematic LSCE. At the nematic to SA phase transformation, the orientation of the director remains constant while the tendency of the network strands towards an oblate equilibrium conformation is suppressed by the high modulus parallel to the smectic layer normal. The mechanical anisotropy of the SA‐LSCE as a function of the temperature is characterized by entropy elasticity perpendicular to the smectic layer normal. Parallel to the layer normal the mechanical response is determined by the enthalpy elastic response of the smectic layers having a modulus larger by about two orders of magnitude. In this direction the modulus decreases linearly with increasing temperature and reflects the falling stability of the layers. Accordingly, above a deformation of about 2% the homogeneous layered structure breaks down at a threshold stress that also falls linearly with increasing temperature while the threshold strain remains constant at about 2% elongation.

We investigate the behavior of the complex shear modulus of a series of elastomers including mono-domain and poly-domain liquid crystal samples, and a non-mesomorphic sample. We find that the dynamics of the glass transition are strongly modified by the nematic order. This result explains why the truly elastic response of liquid crystal elastomers can only be observed in the isotropic phase at very high temperatures and at very low frequencies. Between the elastic regime and the glassy state, the elastomers have a visco-elastic regime, which is characterized by a Rouse-like behavior for mono-domain and poly-domain samples, and by a Zimm-like behavior for the non-mesomorphic sample. We also show that the mono-domain sample exhibits marked anisotropy of the shear-modulus G . This anisotropy, which is observed for the first time, is a function of frequency and is inverted between low and high frequencies, due to relaxation effects of the orientational order.