Probing cavitand-organosilane hybrid bilayers via sum-frequency vibrational spectroscopy.

Quinoxaline cavitands (QxCav) are transferred by Langmuir-Schaefer method on self-assembled monolayers (SAMs) of octadecyltrichlorosilane (OTS) and N,N-dimethyl-N-octadecyl-3-aminopropyltrimethoxysilyl chloride (DMOAP) on fused silica substrates. The molecular architectures of both the hydrophobic SAMs templates and the hybrid cavitand-organosilanes bilayers at the solid-air interface are investigated and correlated by sum-frequency vibrational spectroscopy. The results show that QxCav are always in the closed vase configuration and orient with their principal axis normal to the substrates. The role of the alkyl chains density in the SAM templates on the QxCav transfer ratio is pointed out.

Polarization holograms allow highly efficient generation of complex light beams.

We report a viable method to generate complex beams, such as the non-diffracting Bessel and Weber beams, which relies on the encoding of amplitude information, in addition to phase and polarization, using polarization holography. The holograms are recorded in polarization sensitive films by the interference of a reference plane wave with a tailored complex beam, having orthogonal circular polarizations. The high efficiency, the intrinsic achromaticity and the simplicity of use of the polarization holograms make them competitive with respect to existing methods and attractive for several applications. Theoretical analysis, based on the Jones formalism, and experimental results are shown.

Tunable Surface Patterning of Azopolymer by Vectorial Holography: The Role of Photoanisotropies in the Driving Force.

The capability to pattern polymer surfaces at different length scales is an important goal in different research fields, including display technologies, microelectronics, optics, as well as biorelated and medical science. However, the ability to optically and dynamically manipulate topography is a key feature enabling remote control of associated effects/processes mediated by the surface. Azopolymers are largely investigated to this aim based on their sensitivity to optical fields and reconfigurability capabilities. In this work, surface relief formation induced by polarization patterns on an amorphous azopolymer structurally engineered to have large photoinduced birefringence has been investigated both experimentally and theoretically. Based on the different light polarization patterns, depth and shape of the relief grating can be controlled. An optically induced gradient force model that includes both the spatial distribution and the anisotropy of the material permittivity has been theoretically analyzed. The proposed approach is able to explain the experimental results and to overcome the limitation of existing models.

Surface-induced photorefractivity in twistable nematics: toward the all-optical control of gain.

We report the first two-beam coupling investigation of the surface-induced photorefractive effect (SIPRE) in optically twistable nematic liquid crystal cell. The unique space-charge field of SIPRE is exploited to achieve optical tuning of the photorefractive gain. A reconfigurable photoaligning substrate is used to adjust the twist angle, which is proved to be a control parameter for the photorefractive gain. The amplitude of the optical modulation increases gradually with the twist. Its phase shift changes from 0 degrees to 90 degrees with the polarization state of the two interfering beams. These results pave the way to the all-optical control of the photorefractive gain.

Liquid crystal as laser medium with tunable gain spectra.

Amplified spontaneous emission intensity and gain spectra in polarized light have been measured in a dye doped nematic liquid crystal for different orientation of its optical axis and pump intensity. A possibility for switching the gain of the liquid crystal by an external electric field is shown experimentally. The liquid crystal materials with field controlled gain can be used in microlasers and light micro-amplifiers in both planar and waveguiding geometry.

Electrically tunable two-dimensional liquid crystals gratings induced by polarization holography.

Two-dimensional (2D) gratings made up of an array of differently twisted nematic structures are obtained by crossed assembling of 1D polarization holograms recorded at the photoaligning substrates. The rotating linear polarization pattern, produced by the interference of two opposite circularly polarized beams, is recorded on the azo-dye doped polyimide aligning layers. The 2D gratings diffract light in different directions with different polarization states, that can be optically controlled. Orthogonal circularly and linearly polarized diffraction orders are simultaneously obtained irradiating the grating with a linearly polarized beam. An external ac voltage allows to completely control the diffracted energy distribution.

Light manipulation of nanoparticles in arrays of topological defects.

We report a strategy to assemble and manipulate nanoparticles arrays. The approach is based on the use of topological defects, namely disclination lines, created in chiral liquid crystals. The control of nanoparticle-loaded topological defects by low power light is demonstrated. Large-scale rotation, translation and deformation of quantum dots light-emitting chains is achieved by homogeneous LED illumination. Full reconfigurability and time stability make this approach attractive for future developments and applications.

Light-induced rotations of chiral birefringent microparticles in optical tweezers.

We study the rotational dynamics of solid chiral and birefringent microparticles induced by elliptically polarized laser light in optical tweezers. We find that both reflection of left circularly polarized light and residual linear retardance affect the particle dynamics. The degree of ellipticity of laser light needed to induce rotations is found. The experimental results are compared with analytical calculations of the transfer of angular moment from elliptically polarized light to chiral birefringent particles.

Chiral resolution of spin angular momentum in linearly polarized and unpolarized light.

Linearly polarized (LP) and unpolarized (UP) light are racemic entities since they can be described as superposition of opposite circularly polarized (CP) components of equal amplitude. As a consequence they do not carry spin angular momentum. Chiral resolution of a racemate, i.e. separation of their chiral components, is usually performed via asymmetric interaction with a chiral entity. In this paper we provide an experimental evidence of the chiral resolution of linearly polarized and unpolarized Gaussian beams through the transfer of spin angular momentum to chiral microparticles. Due to the interplay between linear and angular momentum exchange, basic manipulation tasks, as trapping, spinning or orbiting of micro-objects, can be performed by light with zero helicity. The results might broaden the perspectives for development of miniaturized and cost-effective devices.

Photorefractive effect due to a photoinduced surface-charge modulation in undoped liquid crystals.

We demonstrate that some peculiarities of the surface-induced photorefractive effect (SIPRE) in undoped nematic planar cells can be simply explained considering the electric field induced by a modulated surface-charge distribution. Polarization-dependent forced light scattering and two-beam coupling experiments indicate that the observed anisotropy of the diffraction efficiency and the energy transfer between the pump beams strongly depend on the experimental geometry. The investigation suggests that the unusual dichotomy between local and nonlocal behavior can be ascribed to a modulated longitudinal electric field component, in phase with the interference pattern, which is not accountable by the conventional photorefractivity. In a simple and general approach we demonstrate that the conceived charge distribution model for the SIPRE produces a space-charge field having two orthogonal modulated components, in-phase and pi/2 out of phase, respectively. The electric field configuration within the nematic sample gives reason for the main experimental features.

Influence of the ions on the dynamical response of a nematic cell submitted to a dc voltage.

The influence of the ions present in a liquid crystal on the dynamical response of a nematic slab submitted to a dc voltage is studied. The evolution of the system toward the equilibrium state is investigated by solving the continuity equation for the electric charge, taking into account the current of drift and of diffusion. Our analysis shows that the formation of the double layers close to the electrodes strongly modifies the distribution of the electric field across the sample. We evaluate the surface polarization due to the ions movements and the contribution to the anisotropic part of the surface energy having a dielectric origin. We show also that, even if the optical response of the liquid crystal is a slow phenomenon, the distribution of the ionic charge is rather fast. Consequently, the presence of the ions cannot be neglected in the determination of the flexoelectric coefficients when the nematic sample is submitted to a square wave having a period of the order of 1 s.

Polarization-dependent optomechanics mediated by chiral microresonators.

Chirality is one of the most prominent and intriguing aspects of nature, from spiral galaxies down to aminoacids. Despite the wide range of living and non-living, natural and artificial chiral systems at different scales, the origin of chirality-induced phenomena is often puzzling. Here we assess the onset of chiral optomechanics, exploiting the control of the interaction between chiral entities. We perform an experimental and theoretical investigation of the simultaneous optical trapping and rotation of spherulite-like chiral microparticles. Due to their shell structure (Bragg dielectric resonator), the microparticles function as omnidirectional chiral mirrors yielding highly polarization-dependent optomechanical effects. The coupling of linear and angular momentum, mediated by the optical polarization and the microparticles chiral reflectance, allows for fine tuning of chirality-induced optical forces and torques. This offers tools for optomechanics, optical sorting and sensing and optofluidics.

Molecular orientation and alignment of rubbed poly(vinyl cinnamate) surfaces.

We observed that weakly and strongly rubbed polyvinyl-cinnamate surfaces align liquid crystal films perpendicular and parallel to the rubbing direction, respectively. Surface-specific sum-frequency vibrational spectroscopy was used to probe molecular orientations and alignments of the rubbed surfaces and provide a molecular-level understanding of the observation.