Noncontact characterization of microstructured optical fibers coating in real time.

Functional nanocoatings have allowed hollow-core microstructured optical fibers (HC-MOFs) to be introduced into biosensing and photochemistry applications. However, common film characterization tools cannot evaluate the coating performance in situ. Here we report the all-optical noncontact characterization of the HC-MOF coating in real time. Self-assembled multilayers consisting of inversely charged polyelectrolytes (PEs) are deposited on the HC-MOF core capillary, and a linear spectral shift in the position of the fiber transmission minima with increasing the film thickness is observed as small as ∼1.5-6nm per single PE bilayer. We exemplify the practical performance of our approach by registering an increase in the coating thickness from 6±1 to 11±1nm per PE bilayer with increasing ionic strength in the PE solutions from 0.15 to 0.5 M NaCl. Additionally, we show real-time monitoring of pH-induced coating dissolving. Simplicity and high sensitivity make our approach a promising tool allowing noncontact analysis of the HC-MOF coating which is still challenging for other methods.

Ultrasmooth, biocompatible, and removable nanocoating for hollow-core microstructured optical fibers.

Functional nanocoatings of hollow-core microstructured optical fibers (HC-MOFs) have extended the domain of their applications to biosensing and photochemistry. However, novel modalities typically come with increased optical losses since a significant surface roughness of functional layers gives rise to additional light scattering, restricting the performance of functionalization. Here, the technique that enables a biocompatible and removable nanocoating of HC-MOFs with low surface roughness is presented. The initial functional film is formed by a layer-by-layer assembly of bovine serum albumin (BSA) and tannic acid (TA). The alkaline etching at pH 9 results in the reduction of surface roughness from 26 nm to 3 nm and decreases fiber optical losses by three times. The nanocoating can be fully removed within 7 min of the treatment. Natural biocompatibility of BSA alongside antibacterial and antifouling properties of TA makes the presented nanocoating promising for biophotonic applications.

Golden Vaterite as a Mesoscopic Metamaterial for Biophotonic Applications.

Mesoscopic photonic systems with tailored optical responses have great potential to open new frontiers in implantable biomedical devices. However, biocompatibility is typically a problem, as engineering of optical properties often calls for using toxic compounds and chemicals, unsuitable for in vivo applications. Here, a unique approach to biofriendly delivery of optical resonances is demonstrated. It is shown that the controllable infusion of gold nanoseeds into polycrystalline sub-micrometer vaterite spherulites gives rise to a variety of electric and magnetic Mie resonances, producing a tuneable mesoscopic optical metamaterial. The 3D reconstruction of the spherulites demonstrates the capability of controllable gold loading with volumetric filling factors exceeding 28%. Owing to the biocompatibility of the constitutive elements, "golden vaterite" paves the way to introduce designer-made Mie resonances to cutting-edge biophotonic applications. This concept is exemplified by showing efficient laser heating of gold-filled vaterite spherulites at red and near-infrared wavelengths, highly desirable in photothermal therapy, and photoacoustic tomography.

Multispectral sensing of biological liquids with hollow-core microstructured optical fibres.

The state of the art in optical biosensing is focused on reaching high sensitivity at a single wavelength by using any type of optical resonance. This common strategy, however, disregards the promising possibility of simultaneous measurements of a bioanalyte's refractive index over a broadband spectral domain. Here, we address this issue by introducing the approach of in-fibre multispectral optical sensing (IMOS). The operating principle relies on detecting changes in the transmission of a hollow-core microstructured optical fibre when a bioanalyte is streamed through it via liquid cells. IMOS offers a unique opportunity to measure the refractive index at 42 wavelengths, with a sensitivity up to ~3000 nm per refractive index unit (RIU) and a figure of merit reaching 99 RIU-1 in the visible and near-infra-red spectral ranges. We apply this technique to determine the concentration and refractive index dispersion for bovine serum albumin and show that the accuracy meets clinical needs.

Biological Kerker Effect Boosts Light Collection Efficiency in Plants.

Being the polymorphs of calcium carbonate (CaCO3), vaterite and calcite have attracted a great deal of attention as promising biomaterials for drug delivery and tissue engineering applications. Furthermore, they are important biogenic minerals, enabling living organisms to reach specific functions. In nature, vaterite and calcite monocrystals typically form self-assembled polycrystal micro- and nanoparticles, also referred to as spherulites. Here, we demonstrate that alpine plants belonging to the Saxifraga genus can tailor light scattering channels and utilize multipole interference effect to improve light collection efficiency via producing CaCO3 polycrystal nanoparticles on the margins of their leaves. To provide a clear physical background behind this concept, we study optical properties of artificially synthesized vaterite nanospherulites and reveal the phenomenon of directional light scattering. Dark-field spectroscopy measurements are supported by a comprehensive numerical analysis, accounting for the complex microstructure of particles. We demonstrate the appearance of generalized Kerker condition, where several higher order multipoles interfere constructively in the forward direction, governing the interaction phenomenon. As a result, highly directive forward light scattering from vaterite nanospherulites is observed in the entire visible range. Furthermore, ex vivo studies of microstructure and optical properties of leaves for the alpine plants Saxifraga "Southside Seedling" and Saxifraga Paniculata Ria are performed and underline the importance of the Kerker effect for these living organisms. Our results pave the way for a bioinspired strategy of efficient light collection by self-assembled polycrystal CaCO3 nanoparticles via tailoring light propagation directly to the photosynthetic tissue with minimal losses to undesired scattering channels.

Microstructured Optical Waveguide-Based Endoscopic Probe Coated with Silica Submicron Particles.

Microstructured optical waveguides (MOW) are of great interest for chemical and biological sensing. Due to the high overlap between a guiding light mode and an analyte filling of one or several fiber capillaries, such systems are able to provide strong sensitivity with respect to variations in the refractive index and the thickness of filling materials. Here, we introduce a novel type of functionalized MOWs whose capillaries are coated by a layer-by-layer (LBL) approach, enabling the alternate deposition of silica particles (SiO2) at different diameters-300 nm, 420 nm, and 900 nm-and layers of poly(diallyldimethylammonium chloride) (PDDA). We demonstrate up to three covering bilayers consisting of 300-nm silica particles. Modifications in the MOW transmission spectrum induced by coating are measured and analyzed. The proposed technique of MOW functionalization allows one to reach novel sensing capabilities, including an increase in the effective sensing area and the provision of a convenient scaffold for the attachment of long molecules such as proteins.

Enabling magnetic resonance imaging of hollow-core microstructured optical fibers via nanocomposite coating.

Optical fibers are widely used in bioimaging systems as flexible endoscopes that are capable of low-invasive penetration inside hollow tissue cavities. Here, we report on the technique that allows magnetic resonance imaging (MRI) of hollow-core microstructured fibers (HC-MFs), which paves the way for combing MRI and optical bioimaging. Our approach is based on layer-by-layer assembly of oppositely charged polyelectrolytes and magnetite nanoparticles on the inner core surface of HC-MFs. Incorporation of magnetite nanoparticles into polyelectrolyte layers renders HC-MFs visible for MRI and induces the red-shift in their transmission spectra. Specifically, the transmission shifts up to 60 nm have been revealed for the several-layers composite coating, along with the high-quality contrast of HC-MFs in MRI scans. Our results shed light on marrying fiber-based endoscopy with MRI to open novel possibilities for minimally invasive clinical diagnostics and surgical procedures in vivo.

Non-Mie optical resonances in anisotropic biomineral nanoparticles.

The optical properties of nanoparticles have attracted continuous attention owing to their high fundamental and applied importance across many disciplines. A recently emerged field of all-dielectric nanophotonics employs optically induced electric and magnetic Mie resonances in dielectric nanoparticles with a high refractive index. This property allows obtaining additional valuable degrees of freedom to control the optical responses of nanophotonic structures. Here we propose a conceptually distinct approach towards reaching optical resonances in dielectric nanoparticles. We show that, lacking conventional Mie resonances, low-index nanoparticles can exhibit a novel anisotropy-induced family of non-Mie eigenmodes. Specifically, we investigate light interactions with calcite and vaterite nanospheres and compare them with the Mie scattering by a fused silica sphere. Having close permittivities and the same dimensions, these particles exhibit significantly different scattering behavior owing to their internal structure. While a fused silica sphere does not demonstrate any spectral features, the uniaxial structure of the permittivity tensor for calcite and the non-diagonal permittivity tensor for vaterite result in a set of distinguishable peaks in scattering spectra. Multipole decomposition and eigenmode analysis reveal that these peaks are associated with a new family of electric and magnetic resonances. We identify magnetic dipole modes of ordinary, extraordinary and hybrid polarization as well as complex electric dipole resonances, featuring a significant toroidal electric dipole moment. As both vaterite and calcite are biominerals, naturally synthesized and exploited by a variety of living organisms, our results provide an indispensable toolbox for understanding and elucidating the mechanisms behind the optical functionalities of true biological systems.

Ultrafast cryptography with indefinitely switchable optical nanoantennas.

Bistability is widely exploited to demonstrate all-optical signal processing and light-based computing. The standard paradigm of switching between two steady states corresponding to "0" and "1" bits is based on the rule that a transition occurs when the signal pulse intensity overcomes the bistability threshold, and otherwise, the system remains in the initial state. Here, we break with this concept by revealing the phenomenon of indefinite switching in which the eventual steady state of a resonant bistable system is transformed into a nontrivial function of signal pulse parameters for moderately intense signal pulses. The essential nonlinearity of the indefinite switching allows realization of well-protected cryptographic algorithms with a single bistable element in contrast to software-assisted cryptographic protocols that require thousands of logic gates. As a proof of concept, we demonstrate stream deciphering of the word "enigma" by means of an indefinitely switchable optical nanoantenna. An extremely high bitrate ranging from ~0.1 to 1 terabits per second and a small size make such systems promising as basic elements for all-optical cryptographic architectures.

Giant Optical Activity of Quantum Dots, Rods, and Disks with Screw Dislocations.

For centuries mankind has been modifying the optical properties of materials: first, by elaborating the geometry and composition of structures made of materials found in nature, later by structuring the existing materials at a scale smaller than the operating wavelength. Here we suggest an original approach to introduce optical activity in nanostructured materials, by theoretically demonstrating that conventional achiral semiconducting nanocrystals become optically active in the presence of screw dislocations, which can naturally develop during the nanocrystal growth. We show the new properties to emerge due to the dislocation-induced distortion of the crystal lattice and the associated alteration of the nanocrystal's electronic subsystem, which essentially modifies its interaction with external optical fields. The g-factors of intraband transitions in our nanocrystals are found comparable with dissymmetry factors of chiral plasmonic complexes, and exceeding the typical g-factors of chiral molecules by a factor of 1000. Optically active semiconducting nanocrystals-with chiral properties controllable by the nanocrystal dimensions, morphology, composition and blending ratio-will greatly benefit chemistry, biology and medicine by advancing enantiomeric recognition, sensing and resolution of chiral molecules.

Plasmonic kinks and walking solitons in nonlinear lattices of metal nanoparticles.

We study nonlinear effects in one-dimensional (1D) arrays and two-dimensional (2D) lattices composed of metallic nanoparticles with the nonlinear Kerr-like response and an external driving field. We demonstrate the existence of families of moving solitons in 1D arrays and characterize their properties such as an average drifting velocity. We also analyse the impact of varying external field intensity and frequency on the structure and dynamics of kinks in 2D lattices. In particular, we identify the kinks with positive, negative and zero velocity as well as breathing kinks with a self-oscillating profile.

Subwavelength solitons and Faraday waves in two-dimensional lattices of metal nanoparticles.

We demonstrate that optically driven two-dimensional lattices of nonlinear metal nanoparticles can support a variety of dissipative localized modes including Faraday ripples, trapped and walking solitons, oscillons, and switching waves connecting different polarization states.

Subwavelength modulational instability and plasmon oscillons in nanoparticle arrays.

We study modulational instability in nonlinear arrays of subwavelength metallic nanoparticles and analyze numerically nonlinear scenarios of the instability development. We demonstrate that modulational instability can lead to the formation of regular periodic or quasiperiodic modulations of the polarization. We reveal that such nonlinear nanoparticle arrays can support long-lived standing and moving oscillating nonlinear localized modes--plasmon oscillons.

Subwavelength plasmonic kinks in arrays of metallic nanoparticles.

We analyze nonlinear effects in optically driven arrays of nonlinear metallic nanoparticles. We demonstrate that such plasmonic systems are characterized by a bistable response, and they can support the propagation of dissipative switching waves (or plasmonic kinks) connecting the states with different polarization. We study numerically the properties of such plasmonic kinks which are characterized by a subwavelength extent and a tunable velocity.