Polarization-dependent effects in vibrational absorption spectra of 2D finite-size adsorbate islands on dielectric substrates.

In the last few years, infrared reflection-absorption spectroscopy (IRRAS) has become a standard technique to study vibrational excitations of molecules. These investigations are strongly motivated by potential applications in monitoring chemical processes. For a better understanding of the adsorption mechanism of molecules on dielectrics, the polarization-dependence of an interaction of infrared light with adsorbates on dielectric surfaces is commonly used. Thus, the peak positions in absorption spectra could be different for s- and p-polarized light. This shift between the peak positions depends on both the molecule itself and the dielectric substrate. While the origin of this shift is well understood for infinite two-dimensional adsorbate layers, finite-size samples, which consist of 2D islands of a small number of molecules, have never been considered. Here, we present a study on polarization-dependent finite-size effects in the optical response of such islands on dielectric substrates. The study uses a multi-scale modeling approach that connects quantum chemistry calculations with Maxwell scattering simulations. We distinguish the optical response of a single molecule, a finite number of molecules, and a two-dimensional adsorbate layer. We analyze CO and CO2 molecules deposited on CeO2 and Al2O3 substrates. The evolution of the shift between the polarization-dependent absorbance peaks is first studied for a single molecule, which does not exhibit any shifting at all, and for finite molecular islands, where it increases with increasing island size, as well as for an infinite two-dimensional adsorbate layer. In the latter case, the agreement between the obtained results and the experimental IRRAS data and more traditional three/four-layer model theoretical studies supports the predictive power of the multi-scale approach.

Interferometric imaging of reflective micro-objects in the presence of strong aberrations.

Some imaging techniques reduce the effect of optical aberrations either by detecting and actively compensating for them or by utilizing interferometry. A microscope based on a Mach-Zehnder interferometer has been recently introduced to allow obtaining sharp images of light-transmitting objects in the presence of strong aberrations. However, the method is not capable of imaging microstructures on opaque substrates. In this work, we use a Michelson interferometer to demonstrate imaging of reflecting and back-scattering objects on any substrate with micrometer-scale resolution. The system is remarkably insensitive to both deterministic and random aberrations that can completely destroy the object's intensity image.

Highly birefringent metamaterial structure as a tunable partial polarizer.

We consider a highly anisotropic metamaterial structure, composed of parallel metal nanostripes, and show that a thin layer of the material can be used as a tunable partial polarizer. The transmittance of the structure for TE-polarized waves depends strongly on the incidence angle, while for TM-polarized waves, it stays high and essentially constant. In particular, using the structure, the degree of polarization of a partially polarized or unpolarized light can be tuned by changing the incidence angle. The TE-wave transmittance drops from, c.a., 1 to 0 when the incidence angle increases by 5 deg only, owing to the presence of an unusual higher-order odd-symmetric TM mode that we have revealed in the structure. The tuning can be made smoother by introducing another layer of a similar metal-nanostripe structure on top of the first one. The new design allows the TE-wave transmittance to decrease gradually towards 0 with the incidence angle increasing from 0 to about 30 deg. Our structures serve as an essential optical component for studies involving partially polarized light.

Optical wave retarder based on metal-nanostripe metamaterial.

Wave retarders, including quarter- and half-wave plates, are used in many optical systems for polarization conversion. They are usually realized with anisotropic crystalline materials. However, much thinner and possibly also less expensive wave plates can be made of micro- and nanostructures. We present a new way to create thin-film optical retarders based on a highly birefringent metamaterial. The wave plate is capable of low-loss, broadband operation, which we verify both numerically and experimentally. Owing to the remarkable simplicity of our design, the wave plates operating on the proposed principle can meet the requirements of large-scale production and find widespread application in optics and photonics.

Theoretical description and design of nanomaterial slab waveguides: application to compensation of optical diffraction.

Planar optical waveguides made of designable spatially dispersive nanomaterials can offer new capabilities for nanophotonic components. As an example, a thin slab waveguide can be designed to compensate for optical diffraction and provide divergence-free propagation for strongly focused optical beams. Optical signals in such waveguides can be transferred in narrow channels formed by the light itself. We introduce here a theoretical method for characterization and design of nanostructured waveguides taking into account their inherent spatial dispersion and anisotropy. Using the method, we design a diffraction-compensating slab waveguide that contains only a single layer of silver nanorods. The waveguide shows low propagation loss and broadband diffraction compensation, potentially allowing transfer of optical information at a THz rate.

Optical wave parameters for spatially dispersive and anisotropic nanomaterials.

Spatial dispersion is an intriguing property of essentially all nanostructured optical media. In particular, it makes optical waves with equal frequencies and polarizations have different wavelengths, if they propagate in different directions. This can offer new approaches to control light radiation and propagation. Spatially dispersive nanomaterials, such as metamaterials, are often treated in terms of wave parameters, such as refractive index and impedance retrieved from reflection and transmission coefficients of the material at each incidence angle. Usually, however, the waves are approximated as transverse, which simplifies the description, but yields wrong results, if spatial dispersion or optical anisotropy is significant. In this work, we present a method to calculate the wave parameters of a general spatially dispersive and optically anisotropic medium without applying such an approximation. The method allows one to evaluate the true impedances and field vectors of the effective waves, obtaining thus the true light intensity and energy propagation direction in the medium. The equations are applied to several examples of spatially dispersive and anisotropic materials. The method introduces new insights into optics of nanostructured media and extends the design of such media towards optical phenomena involving significant spatial dispersion.

Optical-image transfer through a diffraction-compensating metamaterial.

Cancellation of optical diffraction is an intriguing phenomenon enabling optical fields to preserve their transverse intensity profiles upon propagation. In this work, we introduce a metamaterial design that exhibits this phenomenon for three-dimensional optical beams. As an advantage over other diffraction-compensating materials, our metamaterial is impedance-matched to glass, which suppresses optical reflection at the glass-metamaterial interface. The material is designed for beams formed by TM-polarized plane-wave components. We show, however, that unpolarized optical images with arbitrary shapes can be transferred over remarkable distances in the material without distortion. We foresee multiple applications of our results in integrated optics and optical imaging.

Cantilever-enhanced photoacoustic measurement of HTO in water vapor.

A photoacoustic detection of tritiated water (HTO) is presented. The method uses cantilever-enhanced photoacoustic spectroscopy (CEPAS) to reach sub-ppb sensitivity for HTO in the gas phase. A noise equivalent concentration of 0.88 ppb is reached with a sampling time of 1 min. The high performance and small sample volume of CEPAS allows sensitive detection of HTO from a sample with low total activity.

Intravenous delivery of hydrophobin-functionalized porous silicon nanoparticles: stability, plasma protein adsorption and biodistribution.

Rapid immune recognition and subsequent elimination from the circulation hampers the use of many nanomaterials as carriers to targeted drug delivery and controlled release in the intravenous route. Here, we report the effect of a functional self-assembled protein coating on the intravenous biodistribution of (18)F-labeled thermally hydrocarbonized porous silicon (THCPSi) nanoparticles in rats. (18)F-Radiolabeling enables the sensitive and easy quantification of nanoparticles in tissues using radiometric methods and allows imaging of the nanoparticle biodistribution with positron emission tomography. Coating with Trichoderma reesei HFBII altered the hydrophobicity of (18)F-THCPSi nanoparticles and resulted in a pronounced change in the degree of plasma protein adsorption to the nanoparticle surface in vitro. The HFBII-THCPSi nanoparticles were biocompatible in RAW 264.7 macrophages and HepG2 liver cells making their intravenous administration feasible. In vivo, the distribution of the nanoparticles between the liver and spleen, the major mononuclear phagocyte system organs in the body, was altered compared to that of uncoated (18)F-THCPSi. Identification of the adsorbed proteins revealed that certain opsonins and apolipoproteins are enriched in HFBII-functionalized nanoparticles, whereas the adsorption of abundant plasma components such as serum albumin and fibrinogen is decreased.