When an azobenzene-containing polymer film is exposed to non-uniform illumination, a light-induced mass migration process may be induced, leading to the formation of relief patterns on the polymer-free surface. Despite many years of research effort, several aspects of this phenomenon remain poorly understood. Here we report the appearance of spiral-shaped relief patterns on the polymer film under the illumination of focused Laguerre–Gauss beams with helical wavefronts and an optical vortex at their axis. The induced spiral reliefs are sensitive to the vortex topological charge and to the wavefront handedness. These findings are unexpected because the doughnut-shaped intensity profile of Laguerre–Gauss beams contains no information about the wavefront handedness. We propose a model that explains the main features of this phenomenon through the surface-mediated interference of the longitudinal and transverse components of the optical field. These results may find applications in optical nanolithography and optical-field nanoimaging.
Dye sensitized solar cells (DSSC) are considered one of the most promising photovoltaic technologies as an alternative to traditional silicon-based solar cells, for their compatibility with low-cost production methods, their peculiar optical and mechanical properties and the high indoor efficiency. Photosensitizers represent one of the most important components of a DSSC device and probably the most thoroughly investigated in the last twenty years, with thousands of dyes that have been proposed and tested for this kind of application. In this review we aimed to provide an overview of the three main classes of DSSC photosensitizers, namely ruthenium(II) polypyridyl complexes, Zn-porphyrin derivatives and metal-free organic dyes. After a brief introduction about the architecture and operational principles of a DSSC and the state of the art of the other main components of this type of device, we focused our discussion on photosensitizers. We have defined the numerous requirements DSSC photosensitizers should satisfy and have provided an overview of their historical development over the years; by examining specific dyes reported in the literature, we attempted to highlight the molecular design strategies that have been established for the optimization of their performance in real devices both in terms of efficiency (which recently reaches an outstanding 14.3%) and operational stability. Finally, we discussed, in the last section, the possible future developments of this intriguing technology.
The ability of thermosalient solids, organic analogues of inorganic martensites, to move by rapid mechanical reconfiguration or ballistic event remains visually appealing and potentially useful, yet mechanistically elusive phenomenon. Here, with a material that undergoes both thermosalient and non-thermosalient phase transitions, we demonstrate that the thermosalient effect is preceded by anomalous thermal expansion of the unit cell. The crystal explosion occurs as sudden release of the latent strain accumulated during the anisotropic, exceedingly strong expansion of the unit cell with αa = 225.9 × 10−6 K−1, αb = 238.8 × 10−6 K−1 and αc = −290.0 × 10−6 K−1, the latter being the largest negative thermal expansivity observed for an organic compound thus far. The results point out to the occurence of the thermosalient effect in phase transitions as means to identify new molecular materials with strong positive and/or negative thermal expansion which prior to this work could only be discovered serendipitously.
The directional light-induced mass migration phenomenon arising in the photoresponsive azobenzene-containing materials has become an increasingly used approach for the fabrication of controlled tridimensional superficial textures. In the present work we demonstrate the tailoring of the superficial wettability of an azopolymer by means of the light-driven reconfiguration of an array of imprinted micropillars. Few simple illumination parameters are controlled to induce nontrivial wetting effects. Wetting anisotropy with controlled directionality, unidirectional spreading, and even polarization-intensity driven two-dimensional paths for wetting anisotropy are obtained starting from a single pristine pillar geometry. The obtained results prove that the versatility of the light-reconfiguration process, together with the possibility of reversible reshaping at reduced costs, represents a valid approach for both applications and fundamental studies in the field of geometry-based wettability of solid surfaces.
In optical devices like diffraction gratings and Fresnel lenses, light wavefront is engineered through the structuring of device surface morphology, within thicknesses comparable to the light wavelength. Fabrication of such diffractive optical elements involves highly accurate multistep lithographic processes that in fact set into stone both the surface morphology and optical functionality, resulting in intrinsically static devices. In this work, this fundamental limitation is overcome by introducing shapeshifting diffractive optical elements directly written on an erasable photoresponsive material, whose morphology can be changed in real time to provide different on-demand optical functionalities. First a lithographic configuration that allows writing/erasing cycles of aligned optical elements directly in the light path is developed. Then, the realization of complex diffractive gratings with arbitrary combinations of grating vectors is shown. Finally, a shapeshifting diffractive lens that is reconfigured in the light-path in order to change the imaging parameters of an optical system is demonstrated. The approach leapfrogs the state-of-the-art realization of optical Fourier surfaces by adding on-demand reconfiguration to the potential use in emerging areas in photonics, like transformation and planar optics.
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