The orientation of liquid crystal molecules is very sensitive towards contacting surfaces, and this phenomenon is critical during the fabrication of liquid crystal display panels, as well as optical and memory devices. To date, research has focused on designing and modifying solid surfaces. Here we report an approach to control the orientation of liquid crystals from the free (air) surface side: a skin layer at the free surface was prepared using a non-photoresponsive liquid crystalline polymer film by surface segregation or inkjet printing an azobenzene-containing liquid crystalline block copolymer. Both planar-planar and homoeotropic-planar mode patterns were readily generated. This strategy is applicable to various substrate systems, including inorganic substrates and flexible polymer films. These versatile processes require no modification of the substrate surface and are therefore expected to provide new opportunities for the fabrication of optical and mechanical devices based on liquid crystal alignment.

We prepared a mechanically tough, highly transparent elastomer by using a polyrotaxane cross-linker acting as a molecular pulley.

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An orientational change from homeotropic to planar of liquid crystal (LC) mesogens and the microphase separation (MPS) domains is attained by the segregated skin layer at the free surface. This allows for an efficient in-plane photoalignment of the cylindrical domains. The surface segregation strategy is very simple and is therefore expected to open up new possibilities for the orientation control of various types of LC materials.

Liquid crystal (LC) provides a suitable platform to exploit structural motions of molecules in a condensed phase. Amplification of the structural changes enables a variety of technologies not only in LC displays but also in other applications. Until very recently, however, a practical use of LCs for removable adhesives has not been explored, although a spontaneous disorganization of LC materials can be easily triggered by light-induced isomerization of photoactive components. The difficulty of such application derives from the requirements for simultaneous implementation of sufficient bonding strength and its rapid disappearance by photoirradiation. Here we report a dynamic molecular LC material that meets these requirements. Columnar-stacked V-shaped carbon frameworks display sufficient bonding strength even during heating conditions, while its bonding ability is immediately lost by a light-induced self-melting function. The light-melt adhesive is reusable and its fluorescence colour reversibly changes during the cycle, visualizing the bonding/nonbonding phases of the adhesive.

The pathways toward linearly polarized light (LPL)-induced alignment switching in a diblock copolymer film composed of liquid crystalline (LC) azobenzene (Az) and amorphous poly(butyl methacrylate) (PBMA) blocks were studied in detail using polarized UV−vis absorption spectroscopy, grazing incidence small-angle X-ray scattering measurements, and polarized optical microscopy and transmission electron microscopy observations. The hierarchical structures of microphaseseparated cylinders of PBMA in a smectic LC Az layer matrix were prealigned by LPL and then irradiated by orthogonal LPL, which resulted in alignment switching to the orthogonal direction. In this process, the large prealigned domains were divided into substantially smaller domains at the submicrometer level, and then the structures were realigned in the orthogonal direction in a strongly cooperative manner, most likely through the domain rotation mechanism. The alignment change consisted of three stages: (i) fluctuations in the smectic layer of LC Az side chains in the initial state and breaking up of smaller grains to the submicrometer level before the orientation change (induction period), (ii) actual rotation of the divided domains driven by the photoinduced reorientation of Az mesogens (action period), and (iii) slower fusion and growth of smaller domains in the orthogonally realigned direction (postgrowth period). New aspects of dynamic self-assembly behavior in which different hierarchical structures are involved are proposed.

Laminated bilayer films comprised of photoresponsive azobenzene-containing liquid crystalline polymer skin layers adhered on a thick elastomeric substrate were prepared, and the wrinkle formation upon uniaxial compression was investigated. Irradiation with UV light at 365 nm led to the disappearance of the wrinkle or reduction of wrinkle wavelength, depending on the content of azobenzene unit in the polymer. Such photoresponsive modulations of wrinkle formation could be well correlated with the photoinduced changes in the Young’s modulus determined by indentation–retraction force curve measurements using an AFM cantilever. Additionally, the thickness modulation of the skin layer caused by the photoinduced mass migration can also be applied to modify the wrinkle wavelength. These photoresponsive surface wrinkle modulations are anticipated to offer new possibilities for the surface microfabrication technology.

Studies of proton transport in confined thin polymer electrolytes are essential for providing additional information regarding the structure–property relationships of such materials.