A near-infrared laser dispersion spectrometer with phase modulation for open-path methane sensing.

A laser-based open-path dispersion spectrometer for measuring atmospheric methane has been developed with the goal of achieving a very simple architecture, yet enabling molecular dispersion measurements immune to optical power variation. Well-mature, near-infrared photonics components were retained to demonstrate a compact, cost-effective, and low-power consumption dispersion spectrometer. In particular, measurements immune to received optical power variations are demonstrated despite the use of only phase modulation and are supported by the development of the corresponding physical model.

Long-term continuous monitoring of methane emissions at an oil and gas facility using a multi-open-path laser dispersion spectrometer.

A method for methane emissions monitoring at industrial facility level was developed based on a high precision multi-open-path laser dispersion spectrometer combined with Bayesian analysis algorithms using Monte Carlo Markov Chain (MCMC) inference. From the methane path-averaged concentrations spatially distributed over the facility under study, together with the wind vector, the analysis allows detection, localization and quantification of fugitive methane emissions. This paper describes the very first long term (3 months), continuous (24 h/7 days) deployment of this monitoring system at an operational gas processing and distribution facility.

Locating and Quantifying Methane Emissions by Inverse Analysis of Path-Integrated Concentration Data Using a Markov-Chain Monte Carlo Approach.

The action to reduce anthropogenic greenhouse gas emissions is severely constrained by the difficulty of locating sources and quantifying their emission rates. Methane emissions by the energy sector are of particular concern. We report results achieved with a new area monitoring approach using laser dispersion spectroscopy to measure path-averaged concentrations along multiple beams.

Broadband gas phase absorber detection and quantification by chirped laser dispersion spectroscopy at 1.55 µm.

The demonstration and first evaluation of chirped laser dispersion spectroscopy (CLaDS) for quantitative measurements of gas molecules with broad spectral features is reported. The demonstration is conducted on propyne (methyl acetylene) gas, using a widely tunable external cavity near infrared laser, λ ≈ 1.55 µm, whose frequency can be swept at 2.

Trace gas analysis with laser dispersion spectroscopy.

Trace gas analysis provides a wide range of insights into environmental processes, particularly with regards to global warming and air quality. With the urgent need to identify sources and accurately measure the harmful emissions negatively impacting our planet, Laser Dispersion Spectroscopy (LDS) offers a unique approach. LDS technology measures optical molecular dispersion via a differential phase measurement of light and, operating in the mid-infrared, provides highly sensitive and robust measurements.

Hollow waveguide-miniaturized quantum cascade laser heterodyne spectro-radiometer.

A miniature thermal infrared laser heterodyne spectro-radiometer based on hybrid optical integration is demonstrated. A quantum cascade laser emitting at 953 cm (10.5 μm) is used as the local oscillator.

Hollow waveguide integrated laser spectrometer for CO/CO analysis.

Using hollow waveguide hybrid optical integration, a miniaturized mid-infrared laser absorption spectrometer for CO/CO isotopologue ratio analysis is presented. The laser analyzer described focuses on applications where samples contain a few percent of CO, such as breath analysis and characterization of geo-carbon fluxes, where miniaturization facilitates deployment. As part of the spectrometer design, hollow waveguide mode coupling and propagation is analyzed to inform the arrangement of the integrated optical system.

Spectrally resolved thermal emission of atmospheric gases measured by laser heterodyne spectrometry.

The demonstration of thermal infrared quantum cascade laser heterodyne spectrometry to resolve local thermodynamic equilibrium molecular emission lines from earth's atmospheric constituents is presented. The instrument is described, as well as the early steps towards radiometric calibration. Room temperature ethylene emission line measurements carried out in the laboratory are used to validate the instrument.

Demonstration and characterization of ultrafast laser-inscribed mid-infrared waveguides in chalcogenide glass IG2.

The first demonstration and characterization of ultrafast laser-inscribed mid-infrared (mid-IR) waveguides in GeAsSe chalcogenide glass (IG2) is presented. From mode profile and throughput measurements, combined with modelling, the characteristics of the waveguides inscribed in IG2 are studied at 7.8 μm, and compared to those of waveguides inscribed in gallium lanthanum sulfide for reference.

Immediate biofeedback for energy balance via expired breath δ(13)CO2.

Expired breath δ(13)CO2 measured in real time serves as a useful biomarker of altered macronutrient metabolism in response to changes in energy balance. Altered breath δ(13)CO2 is believed to be a result of changes in macronutrient oxidation and the kinetic isotope effect where enzymatic processes discriminate against metabolites naturally enriched with (13)C. Use of breath δ(13)CO2 as a rapid biofeedback of energy balance status will enhance an individual's ability to modify behavior during weight loss efforts.

Broadband standoff detection of large molecules by mid-infrared active coherent laser spectrometry.

A widely tunable active coherent laser spectrometer (ACLaS) has been demonstrated for standoff detection of broadband absorbers in the 1280 to 1318 cm spectral region using an external cavity quantum cascade laser as a mid-infrared source. The broad tuning range allows detection and quantification of vapor phase molecules, such as dichloroethane, ethylene glycol dinitrate, and tetrafluoroethane. The level of confidence in molecular mixing ratios retrieved from interfering spectral measurements is assessed in a quantitative manner.

Analysis and demonstration of atmospheric methane monitoring by mid-infrared open-path chirped laser dispersion spectroscopy.

Atmospheric methane concentration levels were detected using a custom built laser dispersion spectrometer in a long open-path beam configuration. The instrument is driven by a chirped distributed feedback mid-infrared quantum cascade laser centered at ~1283.46 cm and covers intense rotational-vibrational transitions from the fundamental ν band of methane.

Pump and probe spectroscopy with continuous wave quantum cascade lasers.

This paper details infra-red pump and probe studies on nitric oxide conducted with two continuous wave quantum cascade lasers both operating around 5 μm. The pump laser prepares a velocity selected population in a chosen rotational quantum state of the v = 1 level which is subsequently probed using a second laser tuned to a rotational transition within the v = 2 ← v = 1 hot band. The rapid frequency scan of the probe (with respect to the molecular collision rate) in combination with the velocity selective pumping allows observation of marked rapid passage signatures in the transient absorption profiles from the polarized vibrationally excited sample.

Waveguide-enhanced 2D-IR spectroscopy in the gas phase.

A method for obtaining high-quality 2D-IR spectra of gas-phase samples is presented. Time-resolved IR absorption spectroscopy techniques, such as 2D-IR spectroscopy, often require that beams are focused into the sample. This limits the exploitable overlapped path length through samples to a few millimeters.

Middle infrared active coherent laser spectrometer for standoff detection of chemicals.

Using a quantum cascade laser emitting at 7.85 μm, a middle infrared active coherent laser spectrometer has been developed for the standoff detection of vapor phase chemicals. The first prototype has been tested using diffuse target backscattering at ranges up to ~30 m.

Intracavity widely-tunable quantum cascade laser spectrometer.

A grating-tuned extended-cavity quantum cascade laser (EC-QCL) operating around 7.6 µm was assembled to provide a tuning range of ~80 cm⁻¹ with output power of up to 30 mW. The EC-QCL output power was shown to be sensitive to the presence of a broadband absorbing gas mixture contained in a 2-cm cell introduced inside the extended laser cavity.

Coherent transient spectroscopy with continuous wave quantum cascade lasers.

A high power continuous wave quantum cascade laser operating around 1900 cm(-1) has been used to conduct Lamb dip spectroscopy on a low pressure sample of NO. The widths of the Lamb dips indicate that the laser linewidth is 800 ± 60 kHz and the power sufficient to induce significant population transfer of up to 35%. While the Lamb dip signals are symmetric at low laser chirp rates, they become increasingly asymmetric as the chirp rate increases, further confirming the significant degree of population transfer.

Atmospheric vertical profiles of O3, N2O, CH4, CCl2F2, and H2O retrieved from external-cavity quantum-cascade laser heterodyne radiometer measurements.

Atmospheric vertical profiles of ozone, nitrous oxide, methane, dichlorodifluoromethane, and water are retrieved from data collected with a widely tunable external-cavity quantum-cascade laser heterodyne radiometer (EC-QC-LHR) covering a spectral range between 1120 and 1238 cm(-1). The instrument was operated in solar occultation mode during a two-month measurement campaign at Rutherford Appleton Laboratory in Oxfordshire, UK, in winter 2010/2011, and ultrahigh-resolution (60 MHz or 0.002 cm(-1)) transmission spectra were recorded for multiple narrow spectral windows (~1 cm(-1) width) specific to each molecule.

Signal-to-noise ratio in chirped laser dispersion spectroscopy.

Quantitative studies and experimental validation of noise sources occurring in chirped laser dispersion spectroscopy (CLaDS) are reported. Their impact on the signal-to-noise ratio (SNR) achievable with the CLaDS sensing method is analyzed through a noise model supported by experimental results. In particular the model shows that the SNR is optimal for a given value of the laser chirp rate.

Hollow waveguide photomixing for quantum cascade laser heterodyne spectro-radiometry.

An integrated optic approach, using hollow waveguides, has been evaluated for a compact, rugged, high efficiency heterodyne optical mixing circuit in the middle infrared. The approach has involved the creation of hollow waveguides and alignment features for a beam combiner component in a glass-ceramic substrate. The performance of the integrated beam combiner was tested as part of a full laser heterodyne spectro-radiometer in which a quantum cascade laser local oscillator emitting at 9.

Atmospheric observations of multiple molecular species using ultra-high-resolution external cavity quantum cascade laser heterodyne radiometry.

We demonstrate a widely tunable laser heterodyne radiometer operating in the thermal IR during an atmospheric observation campaign in the solar occultation viewing mode. An external cavity quantum cascade laser tunable within a range of 1120 to 1238 cm(-1) is used as the local oscillator (LO) of the instrument. Ultra-high-resolution (60 MHz or 0.

Molecular dispersion spectroscopy for chemical sensing using chirped mid-infrared quantum cascade laser.

A spectroscopic method of molecular detection based on dispersion measurements using a frequency-chirped laser source is presented. An infrared quantum cascade laser emitting around 1912 cm(-1) is used as a tunable spectroscopic source to measure dispersion that occurs in the vicinity of molecular ro-vibrational transitions. The sample under study is a mixture of nitric oxide in dry nitrogen.

High-resolution broadband (>100 cm-1) infrared heterodyne spectro-radiometry using an external cavity quantum cascade laser.

Broadband thermal infrared heterodyne spectro-radiometry using an external cavity quantum cascade laser as a tunable local oscillator has been performed over a frequency range of more than 100 cm(-1) at a central frequency of 1190 cm(-1). Heterodyne spectro-radiometry is demonstrated for two local oscillator tuning modes: broadband tuning for transmission and emission spectroscopy of broadband absorbers (Freon 12), and broadband frequency selection in combination with fine continuous frequency tuning for high-resolution (0.021 cm(-1)) transmission spectroscopy (N(2)O).

Retrieval of atmospheric ozone profiles from an infrared quantum cascade laser heterodyne radiometer: results and analysis.

Following the recent development of a ground-based prototype quantum cascade laser heterodyne radiometer operating in the midinfrared, atmospheric ozone profile retrievals from a solar occultation measurement campaign performed at the Rutherford Appleton Laboratory on 21 September 2006 are presented. Retrieval is based on the optimal estimation method. High resolution (0.

Experimental investigation of high-frequency noise and optical feedback effects using a 9.7 microm continuous-wave distributed-feedback quantum-cascade laser.

An experimental investigation of high-frequency noise, i.e., up to 3 GHz, exhibited by a 9.