A topical review of numerical and experimental studies of supercontinuum generation in photonic crystal fiber is presented over the full range of experimentally reported parameters, from the femtosecond to the continuous-wave regime. Results from numerical simulations are used to discuss the temporal and spectral characteristics of the supercontinuum, and to interpret the physics of the underlying spectral broadening processes. Particular attention is given to the case of supercontinuum generation seeded by femtosecond pulses in the anomalous group velocity dispersion regime of photonic crystal fiber, where the processes of soliton fission, stimulated Raman scattering, and dispersive wave generation are reviewed in detail. The corresponding intensity and phase stability properties of the supercontinuum spectra generated under different conditions are also discussed.

Supercontinuum generation, photonic crystal fiber

Highly nonlinear effects are observed in graded-index multimode optical fibres. Multimode fibres are of interest for next-generation telecommunications systems and the construction of high-energy fibre lasers. However, relatively little work has explored nonlinear pulse propagation in multimode fibres. Here, we consider highly nonlinear ultrashort pulse propagation in the anomalous-dispersion regime of a graded-index multimode fibre. Low modal dispersion and strong nonlinear coupling between the fibre's many spatial modes result in interesting behaviour. We observe spatiotemporal effects reminiscent of nonlinear optics in bulk media—self-focusing and multiple filamentation1,2—at a fraction of the usual power. By adjusting the spatial initial conditions, we generate on-demand, megawatt, ultrashort pulses tunable between 1,550 and 2,200 nm; dispersive waves over one octave; intense combs of visible light; and a multi-octave-spanning supercontinuum. Our results indicate that multimode fibres present unique opportunities for observing new spatiotemporal dynamics and phenomena. They also enable the realization of a new type of tunable, broadband fibre source that could be useful for many applications.

Controllable spatiotemporal nonlinear effects in multimode fibres

Until very recently, handheld spectrometers were the domain of major analytical and security instrument companies, with turnkey analyzers using spectroscopic techniques from X-ray fluorescence (XRF) for elemental analysis (metals), to Raman, mid-infrared, and near-infrared (NIR) for molecular analysis (mostly organics). However, the past few years have seen rapid changes in this landscape with the introduction of handheld laser-induced breakdown spectroscopy (LIBS), smartphone spectroscopy focusing on medical diagnostics for low-resource areas, commercial engines that a variety of companies can build up into products, hyphenated or dual technology instruments, low-cost visible-shortwave NIR instruments selling directly to the public, and, most recently, portable hyperspectral imaging instruments. Successful handheld instruments are designed to give answers to non-scientist operators; therefore, their developers have put extensive resources into reliable identification algorithms, spectroscopic libraries or databases, and qualitative and quantitative calibrations. As spectroscopic instruments become smaller and lower cost, “engines” have emerged, leading to the possibility of being incorporated in consumer devices and smart appliances, part of the Internet of Things (IOT). This review outlines the technologies used in portable spectroscopy, discusses their applications, both qualitative and quantitative, and how instrument developers and vendors have approached giving actionable answers to non-scientists. It outlines concerns on crowdsourced data, especially for heterogeneous samples, and finally looks towards the future in areas like IOT, emerging technologies for instruments, and portable hyphenated and hyperspectral instruments.

https://journals.sagepub.com/doi/pdf/10.1177/0003702818809719

EXPRESS: Portable Spectroscopy:

A compact source that generates sub-two-cycle-duration pulses with an average power of 0.1 W spanning 6.8–16.4 μm combines the properties of power scalability, high repetition rate and phase coherence for the first time in this spectral region. Powerful coherent light with a spectrum spanning the mid-infrared (MIR) spectral range is crucial for a number of applications in natural as well as life sciences, but so far has only been available from large-scale synchrotron sources1. Here we present a compact apparatus that generates pulses with a sub-two-cycle duration and with an average power of 0.1 W and a spectral coverage of 6.8–16.4 μm (at −30 dB). The demonstrated source combines, for the first time in this spectral region, a high power, a high repetition rate and phase coherence. The MIR pulses emerge via difference-frequency generation (DFG) driven by the nonlinearly compressed pulses of a Kerr-lens mode-locked ytterbium-doped yttrium–aluminium–garnet (Yb:YAG) thin-disc oscillator. The resultant 100 MHz MIR pulse train is hundreds to thousands of times more powerful than state-of-the-art frequency combs that emit in this range2,3,4, and offers a high dynamic range for spectroscopy in the molecular fingerprint region4,5,6,7 and an ideal prerequisite for hyperspectral imaging8 as well as for the time-domain coherent control of vibrational dynamics9,10,11.

High-power sub-two-cycle mid-infrared pulses at 100 MHz repetition rate

Silica-based photonic crystal fibre has proven highly successful for supercontinuum generation, with smooth and flat spectral power densities. However, fused silica glass suffers from strong material absorption in the mid-infrared (>2,500 nm), as well as ultraviolet-related optical damage (solarization), which limits performance and lifetime in the ultraviolet (<380 nm). Supercontinuum generation in silica photonic crystal fibre is therefore only possible between these limits. A number of alternative glasses have been used to extend the mid-infrared performance, including chalcogenides, fluorides and heavy-metal oxides, but none has extended the ultraviolet performance. Here, we describe the successful fabrication (using the stack-and-draw technique) of a ZBLAN photonic crystal fibre with a high air-filling fraction, a small solid core, nanoscale features and near-perfect structure. We also report its use in the generation of ultrabroadband, long-term stable, supercontinua spanning more than three octaves in the spectral range 200–2,500 nm. A low-loss ZBLAN micro-structured fibre is used to generate a supercontinuum spanning from the UV to the mid-IR (200 nm–2,500 nm). The material has high resistance even after extended operation and can withstand large spectral power densities.

Deep-ultraviolet to mid-infrared supercontinuum generated in solid-core ZBLAN photonic crystal fibre

Mid-infrared supercontinuum generation with a record-breaking spectral coverage of 1.4–13.3 µm is demonstrated by launching intense ultra-short pulses into short pieces of ultra-high numerical aperture step-index chalcogenide glass optical fibre consisting of a GaAsSe cladding and an As2Se3 core.

Mid-infrared supercontinuum covering the 1.4–13.3 μm molecular fingerprint region using ultra-high NA chalcogenide step-index fibre

In this work, we investigated how the reductive activation of CO2 with an atomic bismuth model catalyst changes under aprotic solvation. IR photodissociation spectroscopy of mass-selected [Bi(CO2)n]− cluster ions was used to follow the structural evolution of the core ion with increasing cluster size. We interpreted the IR spectra by comparison with density-functional-theory calculations. The results show that CO2 binds to a bismuth atom in the presence of an excess electron to form a metalloformate ion, BiCOO−. Solvation with additional CO2 molecules leads to the stabilization of a bismuth(I) oxalate complex and results in a core ion switch.

Solvent-Driven Reductive Activation of CO2 by Bismuth: Switching from Metalloformate Complexes to Oxalate Products.

Using femtosecond upconversion we investigate the time and wavelength structure of infrared supercontinuum generation. It is shown that radiation is scattered into higher order spatial modes (HOMs) when generating a supercontinuum using fibers that are not single-moded, such as a step-index ZBLAN fiber. As a consequence of intermodal scattering and the difference in group velocity for the modes, the supercontinuum splits up spatially and temporally. Experimental results indicate that a significant part of the radiation propagates in HOMs. Conventional simulations of super-continuum generation do not include scattering into HOMs, and including this provides an extra degree of freedom for tailoring supercontinuum sources.

Generation of infrared supercontinuum radiation: spatial mode dispersion and higher-order mode propagation in ZBLAN step-index fibers.

We report infrared photodissociation spectra of manganese–CO2 cluster anions, [Mn(CO2)n]− (n = 2–10) to probe structural motifs characterizing the interaction between Mn and CO2 in the presence of an excess electron. We interpret the experimental spectra through comparison with infrared spectra predicted from density functional theory calculations. The cluster anions consist of core ions combining a Mn atom with a variety of ligands, solvated by additional CO2 molecules. Structural motifs of ligands evolve with increasing cluster size from simple monodentate and bidentate CO2 ligands to oxalate ligands and combinations of these structural themes.

Interaction of CO2 with Atomic Manganese in the Presence of an Excess Negative Charge Probed by Infrared Spectroscopy of [Mn(CO2)n]− Clusters

We present an cross-correlation frequency-resolved optical gating (XFROG) measurement of a megahertz IR supercontinuum generated in a step-index ZBLAN fiber. The resulting spectrogram gives the dispersion characteristics of the fiber and reveals that it has three zero-dispersion wavelengths. A comparison of the measured spectrogram with numerical simulations shows that this dispersion profile allows a notable dispersive-wave generation toward long wavelengths. Furthermore, the sum-frequency generation process in the XFROG measurement gives the possibility of measuring the IR light with fast Si-based detectors, such as CCD arrays.

Jacob Ramsay

Papers

Mid-infrared supercontinuum covering the 1.4–13.3 μm molecular fingerprint region using ultra-high NA chalcogenide step-index fibre

Solvent-Driven Reductive Activation of CO2 by Bismuth: Switching from Metalloformate Complexes to Oxalate Products.

Generation of infrared supercontinuum radiation: spatial mode dispersion and higher-order mode propagation in ZBLAN step-index fibers.

Interaction of CO2 with Atomic Manganese in the Presence of an Excess Negative Charge Probed by Infrared Spectroscopy of [Mn(CO2)n]− Clusters

Up-conversion of a megahertz mid-IR supercontinuum