We studied a novel family of paraxial laser beams forming an overcomplete yet nonorthogonal set of modes. These modes have a singular phase profile and are eigenfunctions of the photon orbital angular momentum. The intensity profile is characterized by a single brilliant ring with the singularity at its center, where the field amplitude vanishes. The complex amplitude is proportional to the degenerate (confluent) hypergeometric function, and therefore we term such beams hypergeometric-Gaussian (HyGG) modes. Unlike the recently introduced hypergeometric modes [Opt. Lett. 32, 742 (2007)], the HyGG modes carry a finite power and have been generated in this work with a liquid-crystal spatial light modulator. We briefly consider some subfamilies of the HyGG modes as the modified Bessel Gaussian modes, the modified exponential Gaussian modes, and the modified Laguerre-Gaussian modes.

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Plasmonic substrates play a crucial role in the confinement and manipulation of localized electromagnetic fields at the nanoscale. The large electromagnetic field enhancement at metal/dielectric interfaces is widely exploited in surface-enhanced fluorescence (SEF) and surface-enhanced Raman scattering (SERS) spectroscopies. Despite the advantage of near-field enhancement, unfortunately, in metals, the large absorption at optical frequencies induces local heating of the analyte fluid with possible damage of the biological material. In addition, in SEF plasmonic substrates, spacer layers are necessary to minimize undesired fluorescence quenching due to nonradiative decay, which strongly depends on the distance between molecules and metallic substrates. Therefore, the possibility of managing surface electromagnetic states mimicking surface-plasmon resonances in terms of spatial localization, high-field intensity, and dispersion characteristics, while avoiding metallic losses is of great interest. However, dielectric nanoantennas can currently provide limited possibilities in the visible range of optical frequencies. We present the realization of all-dielectric metasurfaces made of nanostructured transparent silicon nitride supporting bound states in the continuum (BICs). We show that this special kind of Fano resonances can be effectively used in standard microscopy for practical applications. We achieved concurrent enhancements of ∼10 3 fold of fluorescence emission and Raman scattering farfield intensities of molecules dispersed on these metasurfaces. In addition, we demonstrate that the gain of conventional SERS signals can be increased by more than one order of magnitude by resonant matching of the localized surface plasmon resonance with the BIC field. Our results can find significant applications for enhanced sensing, Raman imaging, and nonlinear processes.

Label-free chemical imaging of live cell membranes can shed light on the molecular basis of cell membrane functionalities and their alterations under membrane-related diseases. In principle, this can be done by surface-enhanced Raman scattering (SERS) in confocal microscopy, but requires engineering plasmonic architectures with a spatially invariant SERS enhancement factor G(x, y) = G. To this end, we exploit a self-assembled isotropic nanostructure with characteristics of homogeneity typical of the so-called near-hyperuniform disorder. The resulting highly dense, homogeneous and isotropic random pattern consists of clusters of silver nanoparticles with limited size dispersion. This nanostructure brings together several advantages: very large hot spot density (∼10(4) μm(-2)), superior spatial reproducibility (SD < 1% over 2500 μm(2)) and single-molecule sensitivity (Gav ∼ 10(9)), all on a centimeter scale transparent active area. We are able to reconstruct the label-free SERS-based chemical map of live cell membranes with confocal resolution. In particular, SERS imaging is here demonstrated on red blood cells in vitro in order to use the Raman-resonant heme of the cell as a contrast medium to prove spectroscopic detection of membrane molecules. Numerical simulations also clarify the SERS characteristics of the substrate in terms of electromagnetic enhancement and distance sensitivity range consistently with the experiments. The large SERS-active area is intended for multi-cellular imaging on the same substrate, which is important for spectroscopic comparative analysis of complex organisms like cells. This opens new routes for in situ quantitative surface analysis and dynamic probing of living cells exposed to membrane-targeting drugs.

Tip-enhanced Raman Scattering (TERS) has recently emerged as a powerful spectroscopic technique capable of providing subdiffraction morphological and chemical information on samples. In this work, we apply TERS spectroscopy for surface analysis of the Bacillus subtilis spore, a very attractive biosystem for a wide range of applications regulated by the spore surface properties. The observed spectra reflect the complex and heterogeneous environment explored by the plasmonic tip, therefore exhibiting significant point-to-point variations at the nanoscale. Herein, we demonstrate that TERS data processing via principal component analysis allows handling such spectral changes, thus enabling an unbiased correlative imaging based on TERS. Our experimental outcomes suggest a denser arrangement of both proteins and carbohydrates on specific spore surface regions simultaneously revealed by AFM phase imaging. Successful TERS analysis of spores' surface is useful for bacterial surface-display systems and drug delivery applications.

We report on the self-assembling of clusters of gold-nanoparticles (Au-NPs) directed by the phase separation of poly(styrene)-b-poly(methylmethacrylate) (PS-b-PMMA) block-copolymer (BCP) on indium tin oxide coated glass, which induces the onset of vertical lamellar domains. After thermal evaporation of gold on BCP, Au-NPs of 4 nm are selectively included into PS-nanodomains by thermal annealing, and then clustered with large density of hot spots (> 10(4) μm(2)) in a random two-dimensional pattern. The resulting nanostructure exhibits near-hyperuniform long-range correlations. The consequent large degree of homogeneity of this isotropic plasmonic pattern gives rise to a highly reproducible Surface-Enhanced Raman Scattering (SERS) enhancement factor over the centimeter scale (std. dev. ∼ 10% over 0.25 cm(2)). We also discuss the application of a static electric field for modulating the BCP host morphology. The electric field induces an alignment of Au-NP clusters into ordered linear chains, exhibiting a stronger SERS activity, but reduced SERS spatial reproducibility.

In this work, we investigate the evanescent field sensing mechanism provided by an all-dielectric metasurface supporting bound states in the continuum (BICs). The metasurface is based on a transparent photonic crystal with subwavelength thickness. The BIC electromagnetic field is localized along the direction normal to the photonic crystal nanoscale-thin slab (PhCS) because of a topology-induced confinement, exponentially decaying in the material to detect. On the other hand, it is totally delocalized in the PhCS plane, which favors versatile and multiplexing sensing schemes. Liquids with different refractive indices, ranging from 1.33 to 1.45, are infiltrated in a microfluidic chamber bonded to the sensing dielectric metasurface. We observe an experimental exponential sensitivity leading to differential values as large as 226 nm/RIU with excellent FOM. This behavior is explained in terms of the physical superposition of the field with the material under investigation and supported by a thorough numerical analysis. The mechanism is then translated to the case of molecular adsorption where a suitable theoretical engineering of the optical structure points out potential sensitivities as large as 4000 nm/RIU.

Herein, we demonstrate a cavity-enhanced hyperspectral refractometric imaging using an all-dielectric photonic crystal slab (PhCS). Our approach takes advantage of the synergy between two mechanisms, surfaceenhanced fluorescence (SEF) and refractometric sensing, both based on high-Q resonances in proximity of bound states in the continuum (BICs). The enhanced local optical field of the first resonance amplifies of 2 orders of magnitude the SEF emission of a probe dye. Simultaneously, hyperspectral refractometric sensing, based on Fano interference between second mode and fluorescence emission, is used for mapping the spatially variant refractive index produced by the specimen on the PhCS. The spectral matching between first resonance and input laser is modulated by the specimen local refractive index, and thanks to the calibrated dependence with the spectral shift of the Fano resonance, the cavity tuning is used to achieve an enhanced correlative refractometric map with a resolution of 10 −5 RIU within femtoliter-scale sampling volumes. This is experimentally applied also on live prostate cancer cells grown on the PhCS, reconstructing enhanced surface refractive index images at the single-cell level. This dual mechanism of quasi-BIC spatially variant gain tracked by quasi-BIC refractometric sensing provides a correlative imaging platform that can find application in many fields for monitoring physical and biochemical processes, such as molecular interactions, chemical reactions, or surface cell analysis.