In analyzing optical properties of multilayered LB films with the uniaxial anisotropy around the surface normal, a new method for calculating infrared reflection-absorbances was developed, by extending Drude's anisotropic calculation theory for two-phase system to Hansen's optical theory for thin isotropic multilayers. With this method, infrared external reflection spectra of a 9-monolayer LB film of cadmium stearate prepared on a gallium arsenide substrate were analyzed to obtain molecular orientations. The result was in fair agreement with that obtained by X-ray diffractometry. Reflection-absorbance spectra of the same LB film on a silver-evaporated slide glass at various temperatures were also analyzed by the same method and the orientation angle of each molecular group was quantitatively obtained, clarifying the process of disordering with the increase of temperature. Further, the dependence of the degree of disordering on the monolayer location in LB films were discussed in light of the isotope substitution experiment.
The development of self-propelled motors that mimic biological motors is an important challenge for the transport of either themselves or some material in a small space, since biological systems exhibit high autonomy and various types of responses, such as taxis and swarming. In this perspective, we review non-living systems that behave like living matter. We especially focus on nonlinearity to enhance autonomy and the response of the system, since characteristic nonlinear phenomena, such as oscillation, synchronization, pattern formation, bifurcation, and hysteresis, are coupled to self-motion of which driving force is the difference in the interfacial tension. Mathematical modelling based on reaction-diffusion equations and equations of motion as well as physicochemical analysis from the point of view of the molecular structure are also important for the design of non-living motors that mimic living motors.
A novel measurement technique has been developed to simultaneously obtain polarized spectra of in-plane (IP) and out-of-plane (OP) vibrational modes in optically thin films deposited on a nonmetallic substrate without using a polarizer. These spectra correspond to the conventional infrared transmission and reflectionabsorption (RA) spectra, respectively. It has been commonly believed that the mode-selective measurements require polarizers and a specific surface. In particular, the OP-mode measurements always require a metallic surface to generate the surface-normal electric field in the films. The present technique overcomes the limitations of the measurements by considering the concept of virtual longitudinal-wave light using a new arithmetic regression model. The nonpolarized transmitted infrared ray through thin films on a transparent material (Ge) was collected at different angles of incidence, and the transmittance single-beam spectra were subjected to the chemometric spectral resolution, so that absorbance spectra were finally obtained. The two spectra resolved from the nonpolarization spectra were found to perfectly correspond to the conventional transmission and RA spectra. Since this technique is not affected by the enhancement factor that depends on a dielectric property of the metal surface, the band-intensity ratio of the two resolved spectra can be used for direct evaluation of molecular orientation in the films. Further, band shifts due to TO-LO splitting have clearly been observed on the nonmetallic substrate.
We have found that single-chain schizophyllan and curdlan (s-SPG and s-curdlan, respectively) can dissolve as-grown and cut single-walled carbon nanotubes (ag-SWNTs and c-SWNTs, respectively) in aqueous solution. The vis-NIR spectra of the composites suggest that c-SWNTs are dissolved as a bundle, whereas ag-SWNTs exist as one or only a few pieces in the tubular hollow constructed by the helical structure inherent to these beta-1,3-glucans. EDX and CLSM measurements and TEM observation established that the distribution map of these polysaccharides overlaps well with the image of SWNTs, indicating that these two components form a composite. Very interestingly, when c-SWNTs were dissolved with the aid of s-SPG or s-curdlan in water, a clear periodical structure with inclined stripes, as detected by AFM, appeared on the fibrous composite surface. Because this periodical structure has never been recognized for the composites with other water-soluble polymers, one can regard that s-SPG or s-curdlan wraps c-SWNTs constructing a helically twined structure. High-resolution TEM observation of an ag-SWNTs/s-SPG composite gave a clearer image in that two s-SPG chains twine one ag-SWNT and the helical motif is right-handed. When this sample was subjected to the AFM measurement, the composite showed the 2-3 nm height. This height implies that one piece of ag-SWNT is included in the s-SPGs helical structure. As a summary, it has been established that beta-1,3-glucans such as s-SPG and s-curdlan not only dissolve SWNTs but also create a novel superstructure on the surface.
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