Antonio Ambrosio

Light-induced spiral mass transport in azo-polymer films under vortex-beam illumination

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.

Broadband and chiral binary dielectric meta-holograms

This is a study of basic holographic principles in designing new nanostructured devices that enable broadband and chiral imaging. Subwavelength structured surfaces, known as meta-surfaces, hold promise for future compact and optically thin devices with versatile functionalities. By revisiting the concept of detour phase, we demonstrate high-efficiency holograms with broadband and chiral imaging functionalities. In our devices, the apertures of binary holograms are replaced by subwavelength structured microgratings. We achieve broadband operation from the visible to the near infrared and efficiency as high as 75% in the 1.0 to 1.4 μm range by compensating for the inherent dispersion of the detour phase with that of the subwavelength structure. In addition, we demonstrate chiral holograms that project different images depending on the handedness of the reference beam by incorporating a geometric phase. Our devices’ compactness, lightness, and ability to produce images even at large angles have significant potential for important emerging applications such as wearable optics.

Controlled steering of Cherenkov surface plasmon wakes with a one-dimensional metamaterial.

In the Cherenkov effect a charged particle moving with a velocity faster than the phase velocity of light in the medium radiates light that forms a cone with a half angle determined by the ratio of the two speeds. In this paper, we show that by creating a running wave of polarization along a one dimensional metallic nanostructure consisting of subwavelength spaced rotated apertures that propagates faster than the surface plasmon polariton phase velocity, we can generate surface plasmon wakes, which are the two-dimensional analogue of Cherenkov radiation. The running wave of polarization travels with a speed determined by the angle of incidence and the photon spin angular momentum. We utilize this running wave of polarization to demonstrate controlled steering of the wakes by changing both the angle of incidence and the polarization of light, which we measure through near-field scanning optical microscopy.

Two-photon patterning of a polymer containing Y-shaped azochromophores

We report on the patterning of the free surface of azo-based polymer films by means of mass migration driven by one- or two-photon absorption. A symmetric donor-acceptor-donor structured Y-shaped azochromophore is specifically synthesized to enhance two-photon absorption in the polymer. The exposure of the polymer film to a focused laser beam results in light-driven mass migration for both one- and two-photon absorptions. Features with subdiffraction resolution (250 nm) are realized and the patterning dynamics is investigated as a function of the light dose. Furthermore, functional photonic structures, such as diffraction gratings with periods ranging between 0.5 and 2.0 μm, have been realized.

Arbitrary spin-to–orbital angular momentum conversion of light

From spins to spirals The polarization state of light can be used in imaging applications and optical communications. Light can also be structured into vortices that carry optical angular momentum, which can be used for micromanipulation and enhancing the capacity of optical communication channels. Devlin et al. present a metasurface converter for optical states that transforms polarization states into optical angular momentum states. The coupling between arbitrary spin and optical angular momentum states of light in a compact planar structure may find applications in producing complex structured light fields. Science, this issue p. 896 A designed metasurface can transform polarization states into optical angular momentum states. Optical elements that convert the spin angular momentum (SAM) of light into vortex beams have found applications in classical and quantum optics. These elements—SAM-to–orbital angular momentum (OAM) converters—are based on the geometric phase and only permit the conversion of left- and right-circular polarizations (spin states) into states with opposite OAM. We present a method for converting arbitrary SAM states into total angular momentum states characterized by a superposition of independent OAM. We designed a metasurface that converts left- and right-circular polarizations into states with independent values of OAM and designed another device that performs this operation for elliptically polarized states. These results illustrate a general material-mediated connection between SAM and OAM of light and may find applications in producing complex structured light and in optical communication.

Optical probing of sample heating in scanning near-field experiments with apertured probes

We have used the inherent thermochromism of conjugated polymers to investigate substrate heating effects in scanning near-field experiments with metal-coated “apertured” probes. Chemically etched and pulled fibers were used to provide near-field excitation of fully converted films of poly(p-phenylene vinylene), PPV, and of poly(4,4′-diphenylene diphenylvinylene). We detect no significant blueshift of the photoluminescence spectra generated with near-field excitation, in comparison to those collected with far-field excitation. We conclude that polymer heating in the region contributing to the luminescence is less than 40K. We also demonstrate that thermolithography of the PPV precursor is not significant by comparing UV (325nm) and red (670nm) illumination.

Photoconductivity in defective carbon nanotube sheets under ultraviolet–visible–near infrared radiation

Multiwalled carbon nanotube sheets of relatively large area have been grown on a sapphire substrate by chemical vapor deposition at the substrate temperature of 500 and 750°C. The photoconductivity measurements, performed under white light and monochromatic radiation in the ultraviolet–visible–near infrared region, show that the highly defective sample grown at 500°C has a higher photosensitivity, thus revealing the crucial role of structural defects in determining the overall photoresponse of the nanotube’s sheets. The spectral photoresponse of these nanostructured films increases with the increase in photon energy, and is strongly correlated to the absorbance. The photoconductivity properties of these materials are favorable in potential development of large area light sensors as well as optoelectronic nanodevices.

Holographic Metalens for Switchable Focusing of Surface Plasmons

Surface plasmons polaritons (SPPs) are light-like waves confined to the interface between a metal and a dielectric. Excitation and control of these modes requires components such as couplers and lenses. We present the design of a new lens based on holographic principles. The key feature is the ability to switchably control SPP focusing by changing either the incident wavelength or polarization. Using phase-sensitive near-field imaging of the surface plasmon wavefronts, we have observed their switchable focusing and steering as the wavelength or polarization is changed.

Controlling spontaneous surface structuring of azobenzene-containing polymers for large-scale nano-lithography of functional substrates

In this work, we investigate the effect of illumination parameters which is light polarization, wavelength, and beam focalization, on the large-scale patterning of the surface of azobenzene-containing polymer films by means of spontaneous surface structuring. This is a phenomenon due to the interference at the sample surface between different light modes originated by scattering from the primary illuminating beam. In particular, the surface patterning in regions of a few squared millimeters with a spatial resolution down to 180 nm is achieved by means of a single beam illumination. The realized topographical structures are both preferentially oriented gratings and isotropically distributed topographical protrusions (dots), with sub-wavelength features.

Thermal processes in metal-coated fiber probes for near-field experiments

We have used a ray optics model to calculate the optical power absorbed in the metal coating of apertured probes for scanning near-field optical microscopy. We have then introduced the absorbed power profile into the heat balance equation to calculate the temperature of the probe as a function of the distance from the apex. By comparing our results with available experimental data, we demonstrate accurate prediction of both the temperature profile along the probe, and the temperature increase per mW of power launched into the fiber (60.7 versus 60K∕mW at 25μm from the apex).