Directive giant upconversion by supercritical bound states in the continuum.

Photonic bound states in the continuum (BICs), embedded in the spectrum of free-space waves1,2 with diverging radiative quality factor, are topologically non-trivial dark modes in open-cavity resonators that have enabled important advances in photonics3,4. However, it is particularly challenging to achieve maximum near-field enhancement, as this requires matching radiative and non-radiative losses. Here we propose the concept of supercritical coupling, drawing inspiration from electromagnetically induced transparency in near-field coupled resonances close to the Friedrich-Wintgen condition2. Supercritical coupling occurs when the near-field coupling between dark and bright modes compensates for the negligible direct far-field coupling with the dark mode. This enables a quasi-BIC field to reach maximum enhancement imposed by non-radiative loss, even when the radiative quality factor is divergent. Our experimental design consists of a photonic-crystal nanoslab covered with upconversion nanoparticles. Near-field coupling is finely tuned at the nanostructure edge, in which a coherent upconversion luminescence enhanced by eight orders of magnitude is observed. The emission shows negligible divergence, narrow width at the microscale and controllable directivity through input focusing and polarization. This approach is relevant to various physical processes, with potential applications for light-source development, energy harvesting and photochemical catalysis.

Optimized array nanostructure for plasmonically induced motion force generation.

The growing demand to manipulate objects with long-range techniques has increasingly called for the development of techniques capable of intensifying and spatially concentrating electromagnetic fields with the aim of improving the electromagnetic forces acting on objects. In this context, one of the most interesting techniques is based on the use of plasmonic phenomena that have the ability to amplify and structure the electric field in very small areas. In this paper, we report the simulation analysis of a plasmonic nanostructure useful for optimizing the profile of the induced plasmonic field distribution and thus the motion dynamics of a nanoparticle, overcoming some limitations observed in the literature for similar structures. The elementary cell of the proposed nanostructure consists of two gold scalene trapezoids forming a planar V-groove. The spatial replication of this elementary cell to form linear or circular array sequences is used to improve the final nanoparticle velocity. The effect of the geometry variation on the plasmonic behaviour and consequently on the force generated, was analyzed in detail. The results suggest that this optimized plasmonic structure has the potential to efficiently propel macroscopic objects, with implications for various fields such as aerospace and biomedical research.

SERS Quantification of Galunisertib Delivery in Colorectal Cancer Cells by Plasmonic-Assisted Diatomite Nanoparticles.

The small molecule Galunisertib (LY2157299, LY) shows multiple anticancer activities blocking the transforming growth factor-ß1 receptor, responsible for the epithelial-to-mesenchymal transition (EMT) by which colorectal cancer (CRC) cells acquire migratory and metastatic capacities. However, frequent dosing of LY can produce highly toxic metabolites. Alternative strategies to reduce drug side effects can rely on nanoscale drug delivery systems that have led to a medical revolution in the treatment of cancer, improving drug efficacy and lowering drug toxicity. Here, a hybrid nanosystem (DNP-AuNPs-LY@Gel) made of a porous diatomite nanoparticle decorated with plasmonic gold nanoparticles, in which LY is retained by a gelatin shell, is proposed. The multifunctional capability of the nanosystem is demonstrated by investigating the efficient LY delivery, the enhanced EMT reversion in CRCs and the intracellular quantification of drug release with a sub-femtogram resolution by surface-enhanced Raman spectroscopy (SERS). The LY release trigger is the pH sensitivity of the gelatin shell to the CRC acidic microenvironment. The drug release is real-time monitored at single-cell level by analyzing the SERS signals of LY in CRC cells. The higher efficiency of LY delivered by the DNP-AuNPs-LY@Gel complex paves the way to an alternative strategy for lowering drug dosing and consequent side effects.

Tuning the exponential sensitivity of a bound-state-in-continuum optical sensor.

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.

Resistance and Raman spectroscopy analysis of Parageobacillus thermantarcticus spores after γ-ray exposure.

Spores of the genus Bacillus are able to resist ionizing radiations and therefore they are a suitable biological model for studies in Astrobiology, i.e. the multidisciplinary approach to the study of the origin and evolution of life on Earth and in the universe. The resistance to γ-radiation is an important issue in Astrobiology in relation to the search for bacterial species that could adapt to life in space. This study investigates the resistance of spores of the thermophilic bacteria Parageobacillus thermantarcticus to γ-rays. The analysis of spores' response to irradiation at a molecular level is performed by means of Raman spectroscopy that allows to get insights in the sequence of events taking place during inactivation. The role of the γ-rays' dose in the inactivation of spores is also investigated, allowing to highlight the mechanism(s) of inactivation including DNA damage, protein denaturation and calcium dipicolinate levels.

Nanosphere Lithography on Fiber: Towards Engineered Lab-On-Fiber SERS Optrodes.

In this paper we report on the engineering of repeatable surface enhanced Raman scattering (SERS) optical fiber sensor devices (optrodes), as realized through nanosphere lithography. The Lab-on-Fiber SERS optrode consists of polystyrene nanospheres in a close-packed arrays configuration covered by a thin film of gold on the optical fiber tip. The SERS surfaces were fabricated by using a nanosphere lithography approach that is already demonstrated as able to produce highly repeatable patterns on the fiber tip. In order to engineer and optimize the SERS probes, we first evaluated and compared the SERS performances in terms of Enhancement Factor (EF) pertaining to different patterns with different nanosphere diameters and gold thicknesses. To this aim, the EF of SERS surfaces with a pitch of 500, 750 and 1000 nm, and gold films of 20, 30 and 40 nm have been retrieved, adopting the SERS signal of a monolayer of biphenyl-4-thiol (BPT) as a reliable benchmark. The analysis allowed us to identify of the most promising SERS platform: for the samples with nanospheres diameter of 500 nm and gold thickness of 30 nm, we measured values of EF of 4 × 105, which is comparable with state-of-the-art SERS EF achievable with highly performing colloidal gold nanoparticles. The reproducibility of the SERS enhancement was thoroughly evaluated. In particular, the SERS intensity revealed intra-sample (i.e., between different spatial regions of a selected substrate) and inter-sample (i.e., between regions of different substrates) repeatability, with a relative standard deviation lower than 9 and 15%, respectively. Finally, in order to determine the most suitable optical fiber probe, in terms of excitation/collection efficiency and Raman background, we selected several commercially available optical fibers and tested them with a BPT solution used as benchmark. A fiber probe with a pure silica core of 200 µm diameter and high numerical aperture (i.e., 0.5) was found to be the most promising fiber platform, providing the best trade-off between high excitation/collection efficiency and low background. This work, thus, poses the basis for realizing reproducible and engineered Lab-on-Fiber SERS optrodes for in-situ trace detection directed toward highly advanced in vivo sensing.

Insights into the interaction of the N-terminal amyloidogenic polypeptide of ApoA-I with model cellular membranes.

BACKGROUND: About twenty variants of apolipoprotein A-I (ApoA-I) are associated to hereditary systemic amyloidoses. Although the molecular bases of this disease are still largely unknown, it has been hypothesized that ApoA-I proteolysis is a key event in pathogenesis, since it triggers the release of an N-terminal fragment (80-100 residue long) that misfolds to form amyloid deposits in peripheral organs and tissues. It is also known that cell membrane lipids play a key role in the fibrillogenic pathway. In the case of ApoA-I related amyloidosis caused by L174S mutation, the 93-residue N-terminal fragment of ApoA-I ([1-93]ApoA-I) was found to be the major constituent of ex vivo fibrils. METHODS: With the main goal to investigate the interaction of either [1-93]ApoA-I and ApoA-I with biomimetic membranes, we set-up an experimental system based on the Raman Tweezers methodology. We tested GUVs composed by two types of zwitterionic lipids with a different fluidity degree, i.e. dioleoylphosphatidylcholine (DOPC) and dipalmitoylphosphatidylcholine (DPPC). RESULTS: We found that [1-93]ApoA-I induces conformational disorder in an ordered lipid bilayer. When interacting with fluid phases, instead, the fragment was found to be able to penetrate the membrane bilayer inducing an alignment of lipid chains. CONCLUSIONS: The interaction features of [1-93]ApoA-I with biomimetic membranes strongly depend on the lipid phase. Full-length ApoA-I was found to have similar effects, even if significantly less pronounced. GENERAL SIGNIFICANCE: Our observations shed light on still largely unknown molecular bases of ApoA-I fibrillogenic domain interaction with membranes.

Dark spots along slowly scaling chains of plasmonic nanoparticles.

We numerically investigate the optical response of slowly scaling linear chains of mismatched silver nanoparticles. Hybridized plasmon chain resonances manifest unusual local field distributions around the nanoparticles that result from symmetry breaking of the geometry. Importantly, we find localization patterns characterized by bright hot-spots alternated by what we term dark spots. A dark spot is associated to dark plasmons that have collinear and antiparallel dipole moments along the chain. As a result, the field amplification in the dark interjunction gap is extinguished for incident polarization parallel to the chain axis. Despite the strong plasmonic coupling, the nanoparticles on the sides of this dark gap experience a dramatic asymmetric field amplification with amplitude gain contrast > 2×102. Remarkably, also for polarization orthogonal to the axis, gap hot-spots form on resonance.

Enhancement factor statistics of surface enhanced Raman scattering in multiscale heterostructures of nanoparticles.

Suitable metal nanostructures may induce surface-enhanced Raman scattering (SERS) enhancement factors (EFs) large-enough to reach single-molecule sensitivity. However, the gap hot-spot EF probability density function (PDF) has the character of a long-tail distribution, which dramatically mines the reproducibility of SERS experiments. Herein, we carry out electrodynamic calculations based on a 3D finite element method of two plasmonic nanostructures, combined with Monte Carlo simulations of the EF statistics under different external conditions. We compare the PDF produced by a homodimer of nanoparticles with that provided by a self-similar trimer. We show that the PDF is sensitive to the spatial distribution of near-field enhancement specifically supported by the nanostructure geometry. Breaking the symmetry of the plasmonic system is responsible for inducing particular modulations of the PDF tail resembling a multiple Poisson distribution. We also study the influence that molecular diffusion towards the hottest hot-spot, or selective hot-spot targeting, might have on the EF PDF. Our results quantitatively assess the possibility of designing the response of a SERS substrate so as to contain the intrinsic EF PDF variance and significantly improving, in principle, the reproducibility of SERS experiments.

Simultaneous measurements of electrophoretic and dielectrophoretic forces using optical tweezers.

Herein, charged microbeads handled with optical tweezers are used as a sensitive probe for simultaneous measurements of electrophoretic and dielectrophoretic forces. We first determine the electric charge carried by a single bead by keeping it in a predictable uniform electric field produced by two parallel planar electrodes, then, we examine same bead's response in proximity to a tip electrode. In this case, besides electric forces, the bead simultaneously experiences non-negligible dielectrophoretic forces produced by the strong electric field gradient. The stochastic and deterministic motions of the trapped bead are theoretically and experimentally analysed in terms of the autocorrelation function. By fitting the experimental data, we are able to extract simultaneously the spatial distribution of electrophoretic and dielectrophoretic forces around the tip. Our approach can be used for determining actual, total force components in the presence of high-curvature electrodes or metal scanning probe tips.

Silver plasmon resonance effects in AgPO3/silica photonic bandgap fiber.

We report on the application of an external electric field and its tuning effect in the guiding properties of a composite AgPO3/silica photonic bandgap fiber. The application of an electric field leads to the poling of the soft glass inclusion, resulting in the formation of a silver-induced plasmonic band, predominantly affecting the short wavelength guiding regimes while inducing polarization dependent losses. These spectral effects are attributed to the formation of silver nanoparticles within the AgPO3 glass matrix, driven by thermal poling.

Polarization-Addressable Optical Movement of Plasmonic Nanoparticles and Hotspot Spin Vortices.

Spin-orbit coupling in nanoscale optical fields leads to the emergence of a nontrivial spin angular momentum component, transverse to the orbital momentum. In this study, we initially investigate how this spin-orbit coupling effect influences the dynamics in gold monomers. We observe that localized surface plasmon resonance induces self-generated transverse spin, affecting the trajectory of the nanoparticles as a function of the incident polarization. Furthermore, we investigate the spin-orbit coupling in gold dimers. The resonant spin momentum distribution is characterized by the unique formation of vortex and anti-vortex spin angular momentum pairs on opposite surfaces of the nanoparticles, also affecting the particle motion. These findings hold promise for various fields, particularly for the precision control in the development of plasmonic thrusters and the development of metasurfaces and other helicity-controlled system aspects. They offer a method for the development of novel systems and applications in the realm of spin optics.

Holographic polymer-dispersed liquid crystal Bragg grating integrated inside a solid core photonic crystal fiber.

A polymer/liquid crystal-based fiber Bragg grating (PLC-FBG) is fabricated with visible two-beam holography by photo-induced modulation of a prepolymer/liquid crystal solution infiltrated into the hollow channels of a solid core photonic crystal fiber (PCF). The fabrication process and effects related to the photonic bandgap guidance into the infiltrated PCF, and characterization of the PLC-FBG, are discussed. Experimental data presented here demonstrate that the liquid crystal inclusions of the PLC-FBG lead to high thermal and bending sensitivities. The microscopic behavior of the polymer/liquid crystal phase separation inside the PCF capillaries is examined using scanning electron microscopy, and is discussed further.

Whispering gallery mode microsphere resonator integrated inside a microstructured optical fiber.

A compact and robust scheme for broadband excitation of whispering gallery mode (WGM) resonances into a microsphere is demonstrated. A polymer microsphere (10 µm) is encapsulated into the capillary of a microstructured optical fiber, in direct contact with the guiding core. Such a configuration allows efficient and reproducible excitation of the in-MOF-microsphere resonator that is characterized by two launch/collection schemes: core input/scattering output, and sphere input/core output. The latter allows an excitation of the microsphere WGMs externally to the fiber. Numerically calculated WGM spectra are in agreement with experiments. Q factors in the range of 10(3) are typically measured.

Cancer metabolic features allow discrimination of tumor from white blood cells by label-free multimodal optical imaging.

Circulating tumor cells (CTCs) are tumor cells that have penetrated the circulatory system preserving tumor properties and heterogeneity. Detection and characterization of CTCs has high potential clinical values and many technologies have been developed for CTC identification. These approaches remain challenged by the extraordinary rarity of CTCs and the difficulty of efficiently distinguishing cancer from the much larger number of white blood cells in the bloodstream. Consequently, there is still a need for efficient and rapid methods to capture the broad spectrum of tumor cells circulating in the blood. Herein, we exploit the peculiarities of cancer metabolism for discriminating cancer from WBCs. Using deuterated glucose and Raman microscopy we show that a) the known ability of cancer cells to take up glucose at greatly increased rates compared to non-cancer cells results in the lipid generation and accumulation into lipid droplets and, b) by contrast, leukocytes do not appear to generate visible LDs. The difference in LD abundance is such that it provides a reliable parameter for distinguishing cancer from blood cells. For LD sensitive detections in a cell at rates suitable for screening purposes, we test a polarization-sensitive digital holographic imaging (PSDHI) technique that detects the birefringent properties of the LDs. By using polarization-sensitive digital holographic imaging, cancer cells (prostate cancer, PC3 and hepatocarcinoma cells, HepG2) can be rapidly discriminated from leukocytes with reliability close to 100%. The combined Raman and PSDHI microscopy platform lays the foundations for the future development of a new label-free, simple and universally applicable cancer cells' isolation method.

Control of the light transmission through a quasiperiodic waveguide.

We studied the waveguiding properties of a photonic quasicrystal based on an octagonal tiling. The structure exhibits intrinsic localisation in the band gap region, that can be exploited to manipulate the signal transmission through a linear defect. The electromagnetic characteristics are first numerically analysed using a full wave simulation and then experimentally verified by measurements carried out in the X-band microwave region. Possible photonic applications include tunable notch filters having large attenuation.

Photosensitive, all-glass AgPO3/silicaphotonic bandgap fiber.

Photonic bandgap (PBG) guidance is observed in a solid core photonic crystal fiber (PCF) consisting of silver metaphosphate (AgPO(3)) glass embedded into a silica cladding, realized by vacuum-assisted infiltration of the molten glass into the hollow channels of a commercial silica PCF. Morphologic analysis of the cladding microstructure by optical and scanning electron microscopy reveals the formation of highly homogeneous glass strands along the PCF length. The characteristic transmission spectrum of the fiber shows PBG guidance in the range between 350 and 1650 nm. The exposure of the cladding glass matrix, using 355 nm, 150 ps laser irradiation, allows photo-induced enhancement of the transmission-to-stop-band extinction ratio by ∼60 dB/cm and bandwidth tuning. Numerical calculations of the transmission pattern of the fabricated AgPO(3)/silica bandgap fiber are in good agreement with experiments.

Ultrasensitive Surface Refractive Index Imaging Based on Quasi-Bound States in the Continuum.

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, surface-enhanced 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.

Spatially resolved refractive index profiles of electrically switchable computer-generated holographic gratings.

We describe a spatially resolved interferometric technique combined with a phase reconstruction method that provides a quantitative two-dimensional profile of the refractive index and spatial distribution of the optical contrast between the on-off states of electrically switchable diffraction gratings as a function of the external electric field. The studied structures are holographic gratings optically written into polymer/liquid crystal composites through single-beam spatial light modulation by means of computer-generated holograms. The electro-optical response of the gratings is also discussed. The diffraction efficiency results to be dependent on the incident light polarization suggesting the possibility to develop polarization dependent switching devices.

Two-dimensional photonic quasicrystals by single beam computer-generated holography.

Recently important efforts have been dedicated to the realization of a new kind of photonic crystals, known as photonic quasicrystals, in which the lack of the translational symmetry is compensated by rotational symmetries not achievable by the conventional periodic crystals. Here we show a novel approach to their fabrication based on the use of a programmable Spatial Light Modulator encoding Computer-Generated Holograms. Using this single beam technique we fabricated Penrose-tiled structures possessing rotational symmetry up to 23-fold, and a two-dimensional Thue-Morse structure, which is an aperiodic structure not achievable by multiple beam holography.