Mid-Infrared Spectroscopy and Challenges in Industrial Environment

In recent years, Mid-Infrared spectroscopy has garnered lot of attention from researchers and industries due to the availability of industrial grade room temperature Intra-band and Quantum Cascade Lasers. These lasers are repeatable in their performance and along with Near-Infrared Lasers, it has opened the entire Infra-red spectral band for industrial applications. This enabled widespread applications of tunable laser absorption spectroscopy for real-time, in-situ and non-invasive gas sensing. Though several spectroscopy techniques are currently available, Mid-Infrared Absorption Spectroscopy offers us a unique advantage of measurement of trace gas concentrations of few gases which has very weak transitions in Near-Infrared region. The objectives of this chapter are to discuss about the spectroscopy technique commonly used for Mid-Infrared Lasers, a comparative study with other techniques, noise and some challenges remaining for industrial applications

Synthesizing gas-filled fiber Raman lines enables access to the molecular fingerprint region

The synthesis of multiple narrow optical spectral lines, precisely and independently tuned across the near- to mid-infrared (IR) region, is a pivotal research area that enables selective and real-time detection of trace gas species within complex gas mixtures. However, existing methods for developing such light sources suffer from limited flexibility and very low pulse energy, particularly in the mid-IR domain. Here, we introduce a new concept based on the gas-filled anti-resonant hollow-core fiber (ARHCF) technology that enables the synthesis of multiple independently tunable spectral lines with high pulse energy of >1 {\mu}J and a few nanoseconds pulse width in the near- and mid-IR region. The number and wavelengths of the generated spectral lines can be dynamically reconfigured. A proof-of-concept laser beam synthesized of two narrow spectral lines at 3.99 {\mu}m and 4.25 {\mu}m wavelengths is demonstrated and combined with photoacoustic (PA) modality for real-time SO2 and CO2 detection. The proposed concept also constitutes a promising way for IR multispectral microscopic imaging.Comment: 39 page

Broadband detection of methane and nitrous oxide using a distributed-feedback quantum cascade laser array and quartz-enhanced photoacoustic sensing

Here we report on the broadband detection of nitrous oxide (N2O) and methane (CH4) mixtures in dry nitrogen by using a quartz-enhanced photoacoustic (QEPAS) sensor exploiting an array of 32 distributed-feedback quantum cascade lasers, within a spectral emission range of 1190−1340 cm−1 as the excitation source. Methane detection down to a minimum detection limit of 200 ppb at 10 s lock-in integration time was achieved. The sensor demonstrated a linear response in the range of 200−1000 ppm. Three different mixtures of N2O and CH4 in nitrogen at atmospheric pressure have been analyzed. The capability of the developed QEPAS sensor to selectively determine the N2O and CH4 concentrations was demonstrated, in spite of significant overlap in their respective absorption spectra in the investigated spectral range

High-brightness lasers with spectral beam combining on silicon

Modern implementations of absorption spectroscopy and infrared-countermeasures demand advanced performance and integration of high-brightness lasers, especially in the molecular fingerprint spectral region. These applications, along with others in communication, remote-sensing, and medicine, benefit from the light source comprising a multitude of frequencies. To realize this technology, a single multi-spectral optical beam of near-diffraction-limited divergence is created by combining the outputs from an array of laser sources. Full integration of such a laser is possible with direct bonding of several epitaxially-grown chips to a single silicon (Si) substrate. In this platform, an array of lasers is defined with each gain material, creating a densely spaced set of wavelengths similar to wavelength division multiplexing used in communications.Scaling the brightness of a laser typically involves increasing the active volume to produce more output power. In the direction transverse to the light propagation, larger geometries compromise the beam quality. Lengthening the cavity provides only limited scaling of the output power due to the internal losses. Individual integrated lasers have low brightness due to combination of thermal effects and high optical intensities. With heterogeneous integration, many lasers can be spectrally combined on a single integrated chip to scale brightness in a compact platform. Recent demonstrations of 2.0-µm diode and 4.8-µm quantum cascade lasers on Si have extended this heterogeneous platform beyond the telecommunications band to the mid-infrared.In this work, low-loss beam combining elements spanning the visible to the mid-infrared are developed and a high-brightness multi-spectral laser is demonstrated in the range of 4.6–4.7-µm wavelengths. An architecture is presented where light is combined in multiple stages: first within the gain-bandwidth of each laser material and then coarsely between each spectral band to a single output waveguide. All components are demonstrated on a common material platform with a Si substrate, which lends feasibility to the complete system integration. Particular attention is focused on improving the efficiency of arrayed waveguide gratings (AWGs), used in the dense wavelength combining stage. This requires development of a refined characterization technique involving AWGs in a ring-resonator configuration to reduce measurement uncertainty. New levels of low-loss are achieved for visible, near-infrared, and mid-infrared multiplexing devices. Also, a multi-spectral laser in the mid-infrared is demonstrated by integrating an array of quantum cascade lasers and an AWG with Si waveguides. The output power and spectra are measured, demonstrating efficient beam combining and power scaling. Thus, a bright laser source in the mid-infrared has been demonstrated, along with an architecture and the components for incorporating visible and near-infrared optical bands

Influence of light coupling configuration and alignment on the stability of HWG-based gas sensor system for real-time detection of exhaled carbon dioxide

A mid-infrared tunable diode laser absorption spectroscopy (TDLAS) gas sensor based on hollow waveguide (HWG) gas cell for real-time exhaled carbon dioxide (eCO2) detection is reported. A 2.73 μm distributed feedback (DFB) laser was used to target a strong CO2 absorption line, and wavelength modulation spectroscopy (WMS) with the second harmonic (WMS-2.) was used to retrieve the CO2 concentration with high sensitivity. The influence of different parameters, including coupling configuration of HWG, laser-to-HWG and HWG-to-detector coupling alignment on the stability of the HWG sensor is systematically studied. The HWG eCO2 sensor showed a fast response time of 2.7s, detection limit of 17 ppmv, and measurement precision of 20.9 ppmv with a 0.54 s temporal resolution. The eCO2 concentrations changed in breath cycles were measured in real time. The Allan variance indicated that the detection limit can reach 1.7 ppmv, corresponding to a detection sensitivity of 1.3(215)10-8 cm-1Hz-1/2, as the integration time increases to 26 s. This work demonstrates the performance characteristics and merits of HWG eCO2 sensor for exhaled breath analysis and potential detection for other exhaled gases

NOVEL COMPACT NARROW-LINEWIDTH MID-INFRARED LASERS FOR SENSING APPLICATIONS

The mid-infrared (2-14 μm) spectral region contains the strong absorption lines of many important molecular species, which make this region crucial for several well-know applications such as spectroscopy, chemical and biochemical sensing, security, and industrial monitoring. To fully exploit this region through absorption spectroscopic techniques, compact and low-cost narrow-linewidth (NLW) mid-infrared (MIR) laser sources are of primary importance. This thesis is focused on three novel compact NLW MIR lasers: demonstration and characterization of a new glass-based spherical microlaser, investigation of the performance of a novel fiber laser, and the design of a monolithic laser on a silicon chip. Starting with fabrication of spherical microcavities based on MIR transparent materials, I showed the feasibility of achieving quality factors of more than 10 million in whispering- gallery mode (WGM) microresonators made of different types of fluoride glasses. Next using Erbium doped ZBLAN glass spherical microresonators, I demonstrated a new ultra- low threshold NLW MIR microlaser. In particular, all aspects of this room temperature continuous-wave (CW) microlaser with a wavelength of 2.71 μm are carefully characterized and studied and the origin of the measured mode structure and polarization is described using a simple analysis. To amplify the output power of this laser, I designed and fabricated a MIR fiber amplifier with a record gain of about 30 dB at 2.71 μm that facilitated the characterization process and boosted the MIR power level to usable level while preserving the laser linewidth. To demonstrate the application of MIR microresonators and microlasers, I studied intracavity absorption spectroscopy based on active and passive high quality WGM MIR microlasers and microresonators. I also estimated the sensitivity and detection limit of gas sensors based on these devices. The outcome of my analysis shows that ppm level sensitivity should be achievable using both active and passive microresonators. Next, I modeled the performance of two newly proposed configurations for NLW MIR generation based on stimulated Raman scattering. First, I studied a new family of Raman fiber lasers that are capable of generating any NLW MIR line in the 2.5-9.5 μm spectral region. I demonstrated the feasibility of this MIR laser family, calculated the threshold conditions, identified the condition for its single-mode operation, and laid the foundation for the first experimental demonstration of such lasers. Finally, I explored the performance of silicon-based on-chip Raman lasers and the parameters that have prevented expanding their wavelength to MIR range. Using the outcomes of this study, I proposed and then analyzed a new architecture for on-chip silicon Raman lasers capable of generating single NLW lines around 3.2 μm with sub-mW threshold pump power

Dispersion Properties of Photonic Crystals and Silicon Nanostructures Investigated by Fourier-Space Imaging

State-of-the-art nanophotonic devices based on semiconductor technology use total internal reflection or the photonic bandgap effect to reduce the waveguide core dimensions down to hundreds of nanometers, ensuring strong optical confinement within the scale of the wavelength. Within the framework of this thesis, we investigate the light propagation in such devices by direct experimental reconstruction of their dispersion relation ω (k), where ω is the optical frequency and k the wave vector of the supported modes. Knowledge of the dispersion relation provides us with comprehensive information about the guided field, including the number of supported modes, their phase and group velocity as well as the higher order dispersion. As a principal characterization tool, an original experimental technique referred as Fourier-space imaging is used. It is based on far-field analysis of optical signal radiated out of the plane of the structure, which makes it possible to retrieve accurately, non-invasively and in one step the complex dispersion of both the leaky and the truly guided optical modes. The latter is feasible provided that the device is equipped with vanishingly weak grating probes that scatter a small part of the guided light into the light cone. The Fourier-space imaging technique was applied to study the optical properties of a large number of nanophotonic devices, ranging from simple nanowire waveguides to complex photonic crystal structures. In the first part of the work, silicon-on-insulator slot waveguides, coupled ridge waveguides and nanowire waveguide arrays are addressed. Besides the phase and group index dispersion, we investigate the phenomenon of mode splitting in coupled systems, being able to probe the coupling lengths with an accuracy of ±50 nm. In the case of waveguide arrays, beam steering using both thermo-optic effect and wavelength tuning was demonstrated. Concerning the photonic crystal devices, we primarily focus on the phenomenon of slow light propagation in line-defect and coupled-cavity photonic crystal waveguides. The latter represent a special type of a waveguide, which allows for substantial optical signal retardation by evanescent coupling along a chain of photonic crystal cavities. The main motivation was to accurately measure the group index of the slow light modes and recognize the main factors limiting its maximum achievable value. Among others, experimental observation of dispersion curve renormalization, enhanced out-of-plane and back-scattering as well as light localization due to residual disorder were reported. Finally, a detailed experimental study of hollow-core photonic crystal structures intended for optical sensing applications is presented

Active and passive mid-infrared photonic devices in ZnSe based materials

The work described in this thesis details the development of mid-infrared waveguide laser sources created through the fabrication of waveguide structures in Cr2+: ZnSe using ultrafast laser inscription (ULI). Current quantum cascade laser (QCL) technology in the 2 – 5 μm region offer compact and robust sources suited to use outside the laboratory but the technology does not offer the high average powers, >100 mW, and wide tuneability, 2 – 3.3 μm of Cr2+: ZnSe laser sources. The development of a Cr2+: ZnSe waveguide laser source provides an environmentally robust product with access to powers and tuneable ranges greater than that provided by QCL systems. The first phase of the investigation produced the first successful refractive index modification of ZnSe using ULI. Both positive and negative refractive index changes were achieved and utilised to fabricate a range of waveguides in ZnSe and Cr2+: ZnSe. Low loss near-infrared waveguides were demonstrated through exploitation of the positive refractive index change. Low loss mid-infrared depressed cladding waveguides were subsequently demonstrated utilising the negative refractive index change. These waveguides were characterised at wavelengths of 1928, 2300 and 3390 nm as representative of pump and signal wavelengths in Cr2+: ZnSe laser systems. Finally, the newly fabricated Cr2+: ZnSe waveguides were constructed into waveguide laser cavities and pumped with a thulium fibre laser source operating at 1928 nm. Laser operation is demonstrated in both waveguides devices at wavelengths of 2573 and 2486 nm with a maximum achieved output power of 285 mW and a slope efficiency of 45%. Furthermore, a tuneable laser source is constructed in the Littman-Metcalf configuration exhibiting a maximum tuning range of 510 nm, 2330-2840 nm, with output powers exceeding 25 mW across the full range. These waveguide laser devices offer an environmentally robust and compact source in the 2 – 3 μm region with improvements upon maximum power and tuneability ranges in current quantum cascade laser sources. The waveguide laser sources reported open the door to products offering the robust nature of QCL sources with the higher powers and 2 – 3 μm tuneability associated with current bulk Cr2+: ZnSe laser systems.Engineering and Physical Sciences Research Council (EPSRC