Fiber-interfaced hollow-core light cage: a platform for on-fiber-integrated waveguides.

Here, we demonstrate the realization of hollow-core light cages (LCs) on commercial step-index fibers using 3D nanoprinting, resulting in fully fiber-integrated devices. Two different light cage geometries with record-high aspect ratio strands and unique sidewise access to the core have been implemented, exhibiting excellent optical and mechanical properties. These achievements are based on the use of 3D nanoprinting to fabricate light cages and stabilize them with customized support elements. Overall, this approach results in novel, to the best of our knowledge, fiber-interfaced hollow-core devices that combine several advantages in a lab-on-a-fiber platform that is particularly useful for diffusion-related applications in environmental sciences, nanosciences, and quantum technologies.

Nanoprinted microstructure-assisted light incoupling into high-numerical aperture multimode fibers.

The coupling of light into optical fibers is limited by the numerical aperture (NA). Here, we show that large-area polymer axial-symmetric microstructures printed on silica multimode fibers improve their incoupling performance by two to three orders of magnitude beyond the numerical aperture limit. A ray-optical mathematical model describing the impact of the grating-assisted light coupling complements the experimental investigation. This study clearly demonstrates the improvement of incoupling performance by nanoprinting microstructures on fibers, opening new horizons, to the best of our knowledge, for multimode fiber applications in life sciences, quantum technologies, and "lab-on-fiber" devices.

3D-nanoprinted on-chip antiresonant waveguide with hollow core and microgaps for integrated optofluidic spectroscopy.

Here, we unlock the properties of the recently introduced on-chip hollow-core microgap waveguide in the context of optofluidics which allows for intense light-water interaction over long lengths with fast response times. The nanoprinted waveguide operates by the anti-resonance effect in the visible and near-infrared domain and includes a hollow core with defined gaps every 176 µm. The spectroscopic capabilities are demonstrated by various absorption-related experiments, showing that the Beer-Lambert law can be applied without any modification. In addition to revealing key performance parameters, time-resolved experiments showed a decisive improvement in diffusion times resulting from the lateral access provided by the microgaps. Overall, the microgap waveguide represents a pathway for on-chip spectroscopy in aqueous environments.

Optical heating-induced spectral tuning of supercontinuum generation in liquid core fibers using multiwall carbon nanotubes.

In this work, we demonstrate the optical heating modulation of soliton-based supercontinuum generation through the employment of multi-walled carbon nanotubes (MW-CNTs) acting as fast and efficient heat generators. By utilizing highly dispersion-sensitive liquid-core fibers in combination with MW-CNTs coated to the outer wall of the fiber, spectral tuning of dispersive waves with response times below one second via exploiting the strong thermo-optic response of the core liquid was achieved. Local illumination of the MW-CNTs coated fiber at selected points allowed modulation of the waveguide dispersion, thus controlling the soliton fission process. Experimentally, a spectral shift of the two dispersive waves towards the region of anomalous dispersion was observed at increasing temperatures. The presented tuning concept shows great potential in the context of nonlinear photonics, as complex and dynamically reconfigurable dispersion profiles can be generated by using structured light fields. This allows investigating nonlinear frequency conversion processes under unconventional conditions, and realizing nonlinear light sources that are reconfigurable quickly.

Ultrafast supercontinuum generation in halomethane-filled liquid-core fibers.

Here, we demonstrate the properties of bromotrichloromethane (CBrCl3) in the context of ultrafast supercontinuum generation in liquid-core fibers. Broadband interferometric and spectroscopic measurements of liquids and fibers indicate suitable optical properties of this halomethane for near-IR supercontinuum generation, which were confirmed in corresponding experiments using ultrashort pulses. The associated simulations showed consistent broadband power redistributions, thus confirming that this halomethane is a suitable candidate for ultrafast nonlinear frequency conversion in liquid-core fibers. It uniquely combines the advantages of an inorganic, i.e., CH-free, material with a non-vanishing hyperpolarizability, allowing to anticipate an integration of second-order nonlinearity into the fiber.

Nanoparticle Tracking in Single-Antiresonant-Element Fiber for High-Precision Size Distribution Analysis of Mono- and Polydisperse Samples.

Accurate determination of the size distribution of nanoparticle ensembles remains a challenge in nanotechnology-related applications due to the limitations of established methods. Here, a microstructured fiber-assisted nanoparticle tracking analysis (FaNTA) realization is introduced that breaks existing limitations through the recording of exceptionally long trajectories of rapidly diffusing polydisperse nanoparticles, resulting in excellent sizing precision and unprecedented separation capabilities of bimodal nanoparticle mixtures. An effective-single-mode antiresonant-element fiber allows to efficiently confine nanoparticles in a light-guiding microchannel and individually track them over more than 1000 frames, while aberration-free imaging is experimentally confirmed by cross-correlation analysis. Unique features of the approach are (i) the highly precise determination of the size distribution of monodisperse nanoparticle ensembles (only 7% coefficient of variation) and (ii) the accurate characterization of individual components in a bimodal mixture with very close mean diameters, both experimentally demonstrated for polymer nanospheres. The outstanding performance of the FaNTA realization can be quantified by introducing a new model for the bimodal separation index. Since FaNTA is applicable to all types of nano-objects down to sub-20 nm diameters, the method will improve the precision standard of mono- and polydisperse nanoparticle samples such as nano-plastics or extracellular vesicles.

Interpreting light guidance in antiresonant and photonic bandgap waveguides and fibers by light scattering: analytical model and ultra-low guidance.

Here, we introduce a quasi-analytic model that allows studying mode formation in low refractive index core waveguides through solely focusing on the cladding properties. The model isolates the reflection properties of the cladding from the modes via correlating the complex amplitude reflection coefficient of the cladding to the complex effective index of the fundamental core mode. The relevance and validity of the model are demonstrated by considering a single-ring anti-resonant fiber, revealing unexpected situations of exceptionally low loss. Our model explains mode formation by light scattering, which conceptually provides deep insights into the relevant physics.

Spectral tailoring of photon pairs from microstructured suspended-core optical fibers with liquid-filled nanochannels.

We theoretically study the generation of photon pairs via spontaneous four-wave mixing (SFWM) in a liquid-filled microstructured suspended-core optical fiber. We show that it is possible to control the wavelength, group velocity, and bandwidths of the two-photon states. Our proposed fiber structure shows a large number of degrees of freedom to engineer the two-photon state. Here, we focus on the factorable state, which shows no spectral correlation in the two-photon components of the state, and allows the heralding of a single-photon pure state without the need for spectral post-filtering.

Colorimetric Biosensors Based on Polymer/Gold Hybrid Nanoparticles: Topological Effects of the Polymer Coating.

Gold nanoparticles decorated with analyte recognition units can form the basis of colorimetric (bio)sensors. The presentation of those recognition units may play a critical role in determining sensor sensitivity. Herein, we use a model system to investigate the effect of the architecture of a polymeric linker that connects gold nanoparticles with the recognition units. Our results show that the number of the latter that can be adsorbed during the assembly of the colorimetric sensors depends on the linker topology. We also show that this may lead to substantial differences in colorimetric sensor performance, particularly in situations in which the interactions with the analyte are comparably weak. Finally, we discuss design principles for efficient colorimetric sensor materials based on our findings.

The Optofluidic Light Cage - On-Chip Integrated Spectroscopy Using an Antiresonance Hollow Core Waveguide.

Emerging applications in spectroscopy-related bioanalytics demand for integrated devices with small geometric footprints and fast response times. While hollow core waveguides principally provide such conditions, currently used approaches include limitations such as long diffusion times, limited light-matter interaction, substantial implementation efforts, and difficult waveguide interfacing. Here, we introduce the concept of the optofluidic light cage that allows for fast and reliable integrated spectroscopy using a novel on-chip hollow core waveguide platform. The structure, implemented by 3D nanoprinting, consists of millimeter-long high-aspect-ratio strands surrounding a hollow core and includes the unique feature of open space between the strands, allowing analytes to sidewise enter the core region. Reliable, robust, and long-term stable light transmission via antiresonance guidance was observed while the light cages were immersed in an aqueous environment. The performance of the light cage related to absorption spectroscopy, refractive index sensitivity, and dye diffusion was experimentally determined, matching simulations and thus demonstrating the relevance of this approach with respect to chemistry and bioanalytics. The presented work features the optofluidic light cage as a novel on-chip sensing platform with unique properties, opening new avenues for highly integrated sensing devices with real-time responses. Application of this concept is not only limited to absorption spectroscopy but also includes Raman, photoluminescence, or fluorescence spectroscopy. Furthermore, more sophisticated applications are also conceivable in, e.g., nanoparticle tracking analysis or ultrafast nonlinear frequency conversion.

Ultrafast intermodal third harmonic generation in a liquid core step-index fiber filled with C2Cl4: erratum.

We provide a correction due to an erroneous repetition rate of one of the laser systems (90 fs pulse duration) in our previously published paper [Opt. Express28, 25037 (2020)10.1364/OE.399771].

Supercontinuum generation in a carbon disulfide core microstructured optical fiber.

We demonstrate supercontinuum generation in a liquid-core microstructured optical fiber using carbon disulfide as the core material. The fiber provides a specific dispersion landscape with a zero-dispersion wavelength approaching the telecommunication domain where the corresponding capillary-type counterpart shows unsuitable dispersion properties for soliton fission. The experiments were conducted using two pump lasers with different pulse duration (30 fs and 90 fs) giving rise to different non-instantaneous contributions of carbon disulfide in each case. The presented results demonstrate an extraordinary high conversion efficiency from pump to soliton and to dispersive wave, overall defining a platform that enables studying the impact of non-instantaneous responses on ultrafast soliton dynamics and coherence using straightforward pump lasers and diagnostics.

Ultrafast intermodal third harmonic generation in a liquid core step-index fiber filled with C2Cl4.

Third harmonic generation in a circular liquid core step-index fiber filled with a highly transparent inorganic solvent is demonstrated experimentally using ultrafast pump pulses of different durations in the telecom domain for the first time. Specifically we achieve intermodal phase matching to the HE13 higher order mode at the harmonic wavelength and found clear indications of a non-instantaneous molecular contribution to the total nonlinearity in the spectral broadening of the pump. Spectral power evolution and efficiency of the conversion process is studied for all pulse parameters, while we found the greatest photon yield for the longest pulses as well as an unexpected blue-shift of the third harmonic wavelength with increasing pump power. Our results provide the basis for future studies aiming at using this tunable fiber platform with a sophisticated nonlinear response in the context of harmonic generation.

Essentials of resonance-enhanced soliton-based supercontinuum generation.

Supercontinuum generation is a key process for nonlinear tailored light generation and strongly depends on the dispersion of the underlying waveguide. Here we reveal the nonlinear dynamics of soliton-based supercontinuum generation in case the waveguide includes a strongly dispersive resonance. Assuming a gas-filled hollow core fiber that includes a Lorentzian-type dispersion term, effects such as multi-color dispersive wave emission and cascaded four-wave mixing have been identified to be the origin of the observed spectral broadening, greatly exceeding the bandwidths of corresponding non-resonant fibers. Moreover, we obtain large spectral bandwidth at low soliton numbers, yielding broadband spectra within the coherence limit. Due to the mentioned advantages, we believe the concept of resonance-enhanced supercontinuum generation to be highly relevant for future nonlinear light sources.

Tailoring modulation instabilities and four-wave mixing in dispersion-managed composite liquid-core fibers.

We show that the ultrafast nonlinear dynamics in supercontinuum generation can be tailored via mixture-based liquid core fibers. Samples containing mixtures of inorganic solvents allow changing dispersion from anomalous to normal, i.e., shifting zero dispersion across pump laser wavelength. A significant control over modulation instability and four-wave mixing has been demonstrated experimentally in record-long (up to 60 cm) samples in agreement with simulations when using sub-psec pulses at 1.555 µm. The smallest concentration ratio yields indications of soliton-fission based supercontinuum generation at soliton numbers that are beyond the coherence limit. The presented dispersion tuning scheme allows creating unprecedented dispersion landscapes for accessing unexplored nonlinear phenomena and selected laser sources.

Third-harmonic generation with tailored modes in liquid core fibers with geometric birefringence.

Geometrically induced birefringence represents a pathway for precisely engineering the modes in fibers and is particularly relevant for applications that crucially depend on modal dispersion. Here liquid core fibers (LCFs) with elliptical cores are analyzed in view of modal properties and third-harmonic generation (THG) numerically and experimentally. Using finite element modeling, the impact of ellipticity on phase matching, inter-modal coupling, electric field distribution, and birefringence are investigated. Significant THG in practically relevant modes, in accordance with phase-matching calculations, was measured in inorganic solvent-based LCFs.

Tailoring soliton fission at telecom wavelengths using composite-liquid-core fibers.

Accurate dispersion management is key for efficient nonlinear light generation. Here, we demonstrate that composite-liquid-core fibers-fibers with binary liquid mixtures as the core medium-allow for accurate and tunable control of dispersion, loss, and nonlinearity. Specifically, we show numerically that mixtures of organic and inorganic solvents in silica capillaries yield anomalous dispersion and reasonable nonlinearity at telecommunication wavelengths. This favorable operation domain is experimentally verified in various liquid systems through dispersion-sensitive supercontinuum generation, with all results being consistent with theoretical designs and simulations. Our results confirm that mixtures introduce a cost-effective means for liquid-core fiber design that allows for loss control, nonlinear response variation, and dispersion engineering.

An improved spectrophotometric method tests the Einstein-Smoluchowski equation: a revisit and update.

Theoretical prediction and experimental measurements of light attenuation in chemically pure and optically transparent solvents have attracted continuous attention, due in part to their curious nature, and in part to the increasing requirements of solvent-related applications. Yet hitherto, a majority of accurate spectrophotometric measurements of transparent solvents upon visible light radiation often end up using long-path-length cells, usually over dozens of cm, rendering the measure costly and complex; meanwhile, the guidance for choosing the Einstein-Smoluchowski equation or its variants as the best formula to predict the light scattering in solvents has remained elusive. Here we demonstrate a simple, versatile and cost-effective spectrophotometric method, enabling a sensitivity of 10-4 dB cm-1 over a 0.5 cm differential path length based on using standard double-beam spectrophotometer. We prove that this method reduces the path length by a factor of 100 while still making its closest approach to the record-low measurement of solvent extinction. We also validate that all the present equations used for predicting the light scattering in the solvent possess similar capacities, suggesting that the criterion for the choice of the appropriate formula simply depends on the equation's practicability. Following the elucidation of the wavelength range where the light scattering dominates the extinction, we further identify differences between scattering coefficients via the theoretical predictions and experimental measures, exposing the need for an improved theory to account for the solvent scattering phenomenon.

Impact of deuteration on the ultrafast nonlinear optical response of toluene and nitrobenzene.

Nonlinear pulse propagation inside highly nonlinear media requires accurate knowledge on the temporal response function of the materials used particular in the case of liquids. Here we study the impact of deuteration on the ultrafast dynamics of toluene and nitrobenzene via all optical Kerr gating, showing substantially different electronic and molecular contributions, which was quantified by fitting a multichannel decay model to the data points. Specifically we found that deuteration imposes the time-integrated nonlinearities to reduce particular for toluene which could be caused by both reduced electronic hyperpolarizabilities as well as weaker intermolecular interactions. The results achieved reveal that deuterated organic solvents represent promising materials for infrared photonics since they offer extended infrared transmission compared to their non-deuterated counterparts while maintained strong nonlinear responses.

Approximate model for analyzing band structures of single-ring hollow-core anti-resonant fibers.

Precise knowledge of modal behavior is of essential importance for understanding light guidance, particularly in hollow-core fibers. Here we present a semi-analytical model that allows determination of bands formed in revolver-type anti-resonant hollow-core fibers. The approach is independent of the actual arrangement of the anti-resonant elements, does not enforce artificial lattice arrangements and allows determination of the effective indices of modes of preselected order. The simulations show two classes of modes: (i) low-order modes exhibiting effective indices with moderate slopes and (ii) a high number of high-order modes with very strong effective index dispersion, forming a quasi-continuum of modes. It is shown that the mode density scales with the square of the normalized frequency, being to some extent similar to the behavior of multimode fibers.