Three-photon head-mounted microscope for imaging deep cortical layers in freely moving rats.

We designed a head-mounted three-photon microscope for imaging deep cortical layer neuronal activity in a freely moving rat. Delivery of high-energy excitation pulses at 1,320 nm required both a hollow-core fiber whose transmission properties did not change with fiber movement and dispersion compensation. These developments enabled imaging at >1.1 mm below the cortical surface and stable imaging of layer 5 neuronal activity for >1 h in freely moving rats performing a range of behaviors.

Low-noise supercontinuum generation in chiral all-normal dispersion photonic crystal fibers.

We present the advantages of supercontinuum generation in chiral, therefore circularly birefringent, all-normal dispersion fibers. Due to the absence of nonlinear power transfer between the polarization eigenstates of the fiber, chiral all-normal dispersion fibers do not exhibit any polarization instabilities and thus are an ideal platform for a low-noise supercontinuum generation. By pumping a chiral all-normal dispersion fiber at 802 nm, we obtained an octave-spanning, robustly circularly polarized supercontinuum with a low noise.

In situ Detection of Cobaloxime Intermediates During Photocatalysis Using Hollow-Core Photonic Crystal Fiber Microreactors.

Hollow-core photonic crystal fibers (HC-PCFs) provide a novel approach for in situ UV/Vis spectroscopy with enhanced detection sensitivity. Here, we demonstrate that longer optical path lengths than afforded by conventional cuvette-based UV/Vis spectroscopy can be used to detect and identify the CoI and CoII states in hydrogen-evolving cobaloxime catalysts, with spectral identification aided by comparison with DFT-simulated spectra. Our findings show that there are two types of signals observed for these molecular catalysts; a transient signal and a steady-state signal, with the former being assigned to the CoI state and the latter being assigned to the CoII state. These observations lend support to a unimolecular pathway, rather than a bimolecular pathway, for hydrogen evolution. This study highlights the utility of fiber-based microreactors for understanding these and a much wider range of homogeneous photocatalytic systems in the future.

Optofluidic Photonic Crystal Fiber Microreactors for In Situ Studies of Carbon Nanodot-Driven Photoreduction.

Performing quantitative in situ spectroscopic analysis on minuscule sample volumes is a common difficulty in photochemistry. To address this challenge, we use a hollow-core photonic crystal fiber (HC-PCF) that guides light at the center of a microscale liquid channel and acts as an optofluidic microreactor with a reaction volume of less than 35 nL. The system was used to demonstrate in situ optical detection of photoreduction processes that are key components of many photocatalytic reaction schemes. The photoreduction of viologens (XV2+) to the radical XV•+ in a homogeneous mixture with carbon nanodot (CND) light absorbers is studied for a range of different carbon dots and viologens. Time-resolved absorption spectra, measured over several UV irradiation cycles, are interpreted with a quantitative kinetic model to determine photoreduction and photobleaching rate constants. The powerful combination of time-resolved, low-volume absorption spectroscopy and kinetic modeling highlights the potential of optofluidic microreactors as a highly sensitive, quantitative, and rapid screening platform for novel photocatalysts and flow chemistry in general.

Scaling rules for high quality soliton self-compression in hollow-core fibers.

Soliton dynamics can be used to temporally compress laser pulses to few fs durations in many different spectral regions. Here we study analytically, numerically and experimentally the scaling of soliton dynamics in noble gas-filled hollow-core fibers. We identify an optimal parameter region, taking account of higher-order dispersion, photoionization, self-focusing, and modulational instability. Although for single-shots the effects of photoionization can be reduced by using lighter noble gases, they become increasingly important as the repetition rate rises. For the same optical nonlinearity, the higher pressure and longer diffusion times of the lighter gases can considerably enhance the long-term effects of ionization, as a result of pulse-by-pulse buildup of refractive index changes. To illustrate the counter-intuitive nature of these predictions, we compressed 250 fs pulses at 1030 nm in an 80-cm-long hollow-core photonic crystal fiber (core radius 15 µm) to ∼5 fs duration in argon and neon, and found that, although neon performed better at a repetition rate of 1 MHz, stable compression in argon was still possible up to 10 MHz.

Cross-phase modulational instability of circularly polarized helical Bloch modes carrying optical vortices in a chiral three-core photonic crystal fiber.

We report the first, to the best of our knowledge, observation of cross-phase modulational instability (XPMI) of circularly polarized helical Bloch modes carrying optical vortices in a twisted photonic crystal fiber with a three-fold symmetric core, formed by spinning the fiber preform during the draw. When the fiber is pumped by a superposition of left-circular polarization (LCP) and right-circular polarization (RCP) modes, a pair of orthogonal circularly polarized sidebands of opposite topological charge is generated. When, on the other hand, a pure LCP (or RCP) mode is launched, the XPMI gain is zero, and no sidebands are seen. This observation has not been seen before in any system and is unique to chiral structures with N-fold rotational symmetry. The polarization state and topological charge of the generated sidebands are measured. By decomposing the helical Bloch modes into their azimuthal harmonics, we are able to deduce the selection rules for the appearance of modulational instability sidebands. We showed that the four waves in the nonlinear mixing process must exhibit the same set of azimuthal harmonic orders.

Non-invasive real-time characterization of hollow-core photonic crystal fibers using whispering gallery mode spectroscopy.

Single-ring hollow-core photonic crystal fibers, consisting of a ring of one or two thin-walled glass capillaries surrounding a central hollow core, hold great promise for use in optical communications and beam delivery, and are already being successfully exploited for extreme pulse compression and efficient wavelength conversion in gases. However, achieving low loss over long (km) lengths requires highly accurate maintenance of the microstructure-a major fabrication challenge. In certain applications, for example adiabatic mode transformers, it is advantageous to taper the fibers, but no technique exists for measuring the delicate and complex microstructure without first cleaving the taper at several positions along its length. In this Letter, we present a simple non-destructive optical method for measuring the diameter of individual capillaries. Based on recording the spectrum scattered from whispering gallery modes excited in the capillary walls, the technique is highly robust, allowing real-time measurement of fiber structure during the draw with sub-micron accuracy.

Generation of broadband circularly polarized supercontinuum light in twisted photonic crystal fibers.

We compare the properties of the broadband supercontinuum (SC) generated in twisted and untwisted solid-core photonic crystal fibers when pumped by circularly polarized 40 picosecond laser pulses at 1064 nm. In the helically twisted fiber, fabricated by spinning the preform during the draw, the SC is robustly circularly polarized across its entire spectrum whereas, in the straight fiber, axial fluctuations in linear birefringence and polarization-dependent nonlinear effects cause the polarization state to vary randomly with the wavelength. Theoretical modelling confirms the experimental results. Helically twisted photonic crystal fibers permit the generation of pure circularly polarized SC light with excellent polarization stability against fluctuations in input power and environmental perturbations.

Pump-probe multi-species CARS in a hollow-core PCF with a 20 ppm detection limit under ambient conditions.

We report coherent anti-Stokes Raman spectroscopy (CARS) in a gas-filled single-ring hollow-core photonic crystal fiber (SR-PCF) using a pump-probe configuration. The long collinear path length offered by an SR-PCF strongly enhances the efficiency of the Raman interactions. Pressure tuning the zero-dispersion wavelength (ZDW) of the SR-PCF allows the Raman coherence prepared by seeded pumping at 515 nm to be used in the visible for phase-matched generation of an anti-Stokes signal from a probe in the ultraviolet. The unique dispersion profile in the vicinity of the ZDW enables simultaneous phase matching of all known Raman transitions. We demonstrate that simultaneous multi-species CARS with a detection limit of 20 ppm is possible with only 20 kW of peak pump power delivered by a single laser source.

Excitation of higher-order modes in optofluidic photonic crystal fiber.

Higher-order modes up to LP33 are controllably excited in water-filled kagomé- and bandgap-style hollow-core photonic crystal fibers (HC-PCF). A spatial light modulator is used to create amplitude and phase distributions that closely match those of the fiber modes, resulting in typical launch efficiencies of 10-20% into the liquid-filled core. Modes, excited across the visible wavelength range, closely resemble those observed in air-filled kagomé HC-PCF and match numerical simulations. Mode indices are obtained by launching plane-waves at specific angles onto the fiber input-face and comparing the resulting intensity pattern to that of a particular mode. These results provide a framework for spatially-resolved sensing in HC-PCF microreactors and fiber-based optical manipulation.

Generation of broadband mid-IR and UV light in gas-filled single-ring hollow-core PCF.

We report generation of an ultrafast supercontinuum extending into the mid- infrared in gas-filled single-ring hollow-core photonic crystal fiber (SR-PCF) pumped by 1.7 µm light from an optical parametric amplifier. The simple fiber structure offers shallow dispersion and flat transmission in the near and mid-infrared, enabling the generation of broadband spectra extending from 270 nm to 3.1 µm, with a total energy of a few µJ. In addition, we demonstrate the emission of ultraviolet dispersive waves whose frequency can be tuned simply by adjusting the pump wavelength. SR-PCF thus constitutes an effective means of compressing and delivering tunable ultrafast pulses in the near and mid-infrared spectral regions.

Continuously wavelength-tunable high harmonic generation via soliton dynamics.

We report the generation of high harmonics in a gas jet pumped by pulses self-compressed in a He-filled hollow-core photonic crystal fiber through the soliton effect. The gas jet is placed directly at the fiber output. As the energy increases, the ionization-induced soliton blueshift is transferred to the high harmonics, leading to emission bands that are continuously tunable from 17 to 45 eV.

High-resolution wavefront shaping with a photonic crystal fiber for multimode fiber imaging.

We demonstrate that a high-numerical-aperture photonic crystal fiber allows lensless focusing at an unparalleled resolution by complex wavefront shaping. This paves the way toward high-resolution imaging exceeding the capabilities of imaging with multi-core single-mode optical fibers. We analyze the beam waist and power in the focal spot on the fiber output using different types of fibers and different wavefront shaping approaches. We show that the complex wavefront shaping technique, together with a properly designed multimode photonic crystal fiber, enables us to create a tightly focused spot on the desired position on the fiber output facet with a subwavelength beam waist.

Broadband robustly single-mode hollow-core PCF by resonant filtering of higher-order modes.

We report a hollow-core photonic crystal fiber that is engineered so as to strongly suppress higher-order modes, i.e., to provide robust LP01 single-mode guidance in all the wavelength ranges where the fiber guides with low loss. Encircling the core is a single ring of nontouching glass elements whose modes are tailored to ensure resonant phase-matched coupling to higher-order core modes. We show that the resulting modal filtering effect depends on only one dimensionless shape parameter, akin to the well-known d/Λ parameter for endlessly single-mode solid-core PCF. Fabricated fibers show higher-order mode losses some ∼100 higher than for the LP01 mode, with LP01 losses <0.2 dB/m in the near-infrared and a spectral flatness ∼1 dB over a >110 THz bandwidth.

Supercontinuum generation in ZBLAN glass photonic crystal fiber with six nanobore cores.

Photonic crystal fibers (PCFs) made from ZBLAN glass are of great interest for generating broadband supercontinua extending into the ultraviolet and mid-infrared regions. Precise sub-micrometer structuring makes it possible to adjust the modal dispersion over a wide range, making the generation of new frequencies more efficient. Here we report a novel ZBLAN PCF with six cores, each containing a central nanobore of a diameter ∼330 nm. Each nanobore core supports several guided modes, and the presence of the nanobore significantly modifies the dispersion, strongly influencing the dynamics and the extent of supercontinuum generation. Spectral broadening is observed when a single core is pumped in the fundamental and first higher order core modes with 200 fs long pulses at a wavelength of 1042 nm. Frequency-resolved optical gating is used to characterize the output pulses when pumping in the lowest order mode. The results are verified by numerical simulations.

Real-time Doppler-assisted tomography of microstructured fibers by side-scattering.

We introduce the concept of Doppler-assisted tomography (DAT) and show that it can be applied successfully to non-invasive imaging of the internal microstructure of a photonic crystal fiber. The fiber is spun at ~10 Hz around its axis and laterally illuminated with a laser beam. Monitoring the time-dependent Doppler shift of the light scattered by the hollow channels permits the azimuthal angle and radial position of individual channels to be measured. An inverse Radon transform is used to construct an image of the microstructure from the frequency-modulated scattered signal. We also show that DAT can image sub-wavelength features and monitor the structure along a tapered fiber, which is not possible using other techniques without cutting up the taper into several short pieces or filling it with index-matching oil. The non-destructive nature of DAT means that it could potentially be applied to image the fiber microstructure as it emerges from the drawing tower, or indeed to carry out tomography on any transparent microstructured cylindrical object.

Low-Volume Reaction Monitoring of Carbon Dot Light Absorbers in Optofluidic Microreactors.

Optical monitoring and screening of photocatalytic batch reactions using cuvettes ex situ is time-consuming, requires substantial amounts of samples, and does not allow the analysis of species with low extinction coefficients. Hollow-core photonic crystal fibers (HC-PCFs) provide an innovative approach for in situ reaction detection using ultraviolet-visible absorption spectroscopy, with the potential for high-throughput automation using extremely low sample volumes with high sensitivity for monitoring of the analyte. HC-PCFs use interference effects to guide light at the center of a microfluidic channel and use this to enhance detection sensitivity. They open the possibility of comprehensively studying photocatalysts to extract structure-activity relationships, which is unfeasible with similar reaction volume, time, and sensitivity in cuvettes. Here, we demonstrate the use of HC-PCF microreactors for the screening of the electron transfer properties of carbon dots (CDs), a nanometer-sized material that is emerging as a homogeneous light absorber in photocatalysis. The CD-driven photoreduction reaction of viologens (XV2+) to the corresponding radical monocation XV•+ is monitored in situ as a model reaction, using a sample volume of 1 µL per measurement and with a detectability of <1 µM. A range of different reaction conditions have been systematically studied, including different types of CDs (i.e., amorphous, graphitic, and graphitic nitrogen-doped CDs), surface chemistry, viologens, and electron donors. Furthermore, the excitation irradiance was varied to study its effect on the photoreduction rate. The findings are correlated with the electron transfer properties of CDs based on their electronic structure characterized by soft X-ray absorption spectroscopy. Optofluidic microreactors with real-time optical detection provide unique insight into the reaction dynamics of photocatalytic systems and could form the basis of future automated catalyst screening platforms, where samples are only available on small scales or at a high cost.

Nonlinear fiber-optic strain sensor based on four-wave mixing in microstructured optical fiber.

We demonstrate a nonlinear fiber-optic strain sensor, which uses the shifts of four-wave mixing Stokes and anti-Stokes peaks caused by the strain-induced changes in the structure and refractive index of a microstructured optical fiber. The sensor thus uses the inherent nonlinearity of the fiber and does not require any advanced postprocessing of the fiber. Strain sensitivity of -0.23 pm/µÎµ is achieved experimentally and numerical simulations reveal that for the present fiber the sensitivity can be increased to -4.46 pm/µÎµ by optimizing the pump wavelength and power.

Nonreciprocal vortex isolator via topology-selective stimulated Brillouin scattering.

Optical nonreciprocity, which breaks the symmetry between forward and backward propagating optical waves, has become vital in photonic systems and enables many key applications. So far, all the existing nonreciprocal systems are implemented for linearly or randomly polarized fundamental modes. Optical vortex modes, with wavefronts that spiral around the central axis of propagation, have been extensively studied over the past decades and offer an additional degree of freedom useful in many applications. Here, we report a light-driven nonreciprocal isolation system for optical vortex modes based on topology-selective stimulated Brillouin scattering (SBS) in chiral photonic crystal fiber. The device can be reconfigured as an amplifier or an isolator by adjusting the frequency of the control signal. The experimental results show vortex isolation of 22 decibels (dB), which is at the state of the art in fundamental mode isolators using SBS. This device may find applications in optical communications, fiber lasers, quantum information processing, and optical tweezers.

Label-free monitoring of proteins in optofluidic hollow-core photonic crystal fibres.

The fluorescent detection of proteins without labels or stains, which affect their behaviour and require additional genetic or chemical preparation, has broad applications to biological research. However, standard approaches require large sample volumes or analyse only a small fraction of the sample. Here we use optofluidic hollow-core photonic crystal fibres to detect and quantify sub-microlitre volumes of unmodified bovine serum albumin (BSA) protein down to 100 nM concentrations. The optofluidic fibre's waveguiding properties are optimised for guidance at the (auto)fluorescence emission wavelength, enabling fluorescence collection from a 10 cm long excitation region, increasing sensitivity. The observed spectra agree with spectra taken from a conventional cuvette-based fluorimeter, corrected for the guidance properties of the fibre. The BSA fluorescence depended linearly on BSA concentration, while only a small hysteresis effect was observed, suggesting limited biofouling of the fibre sensor. Finally, we briefly discuss how this method could be used to study aggregation kinetics. With small sample volumes, the ability to use unlabelled proteins, and continuous flow, the method will be of interest to a broad range of protein-related research.