The development and initial demonstration of a scanned-wavelength, first-harmonic-normalized, wavelength-modulation spectroscopy with nf detection (scanned-WMS-nf/1f) strategy for calibration-free measurements of gas conditions are presented. In this technique, the nominal wavelength of a modulated tunable diode laser (TDL) is scanned over an absorption transition to measure the corresponding scanned-WMS-nf/1f spectrum. Gas conditions are then inferred from least-squares fitting the simulated scanned-WMS-nf/1f spectrum to the measured scanned-WMS-nf/1f spectrum, in a manner that is analogous to widely used scanned-wavelength direct-absorption techniques. This scanned-WMS-nf/1f technique does not require prior knowledge of the transition linewidth for determination of gas properties. Furthermore, this technique can be used with any higher harmonic (i.e., n>1), modulation depth, and optical depth. Selection of the laser modulation index to maximize both signal strength and sensitivity to spectroscopic parameters (i.e., gas conditions), while mitigating distortion, is described. Last, this technique is demonstrated with two-color measurements in a well-characterized supersonic flow within the Stanford Expansion Tube. In this demonstration, two frequency-multiplexed telecommunication-grade TDLs near 1.4 μm were scanned at 12.5 kHz (i.e., measurement repetition rate of 25 kHz) and modulated at 637.5 and 825 kHz to determine the gas temperature, pressure, H2O mole fraction, velocity, and absorption transition lineshape. Measurements are shown to agree within uncertainty (1%-5%) of expected values.
SpectraPlot is a web-based application for simulating spectra of atomic and molecular gases. At the time this manuscript was written, SpectraPlot consisted of four primary tools for calculating: 1) atomic and molecular absorption spectra, 2) atomic and molecular emission spectra, 3) transition linestrengths, and 4) blackbody emission spectra. These tools currently employ the NIST ASD, HITRAN2012, and HITEMP2010 databases to perform line-by-line simulations of spectra. Spec-traPlot employs a modular, integrated architecture, enabling multiple simulations across multiple databases and/or thermodynamic conditions to be visualized in a single interactive plot window. The primary objective of this paper is to describe the architecture and spectroscopic models employed by SpectraPlot in order to provide its users with the knowledge required to understand the capabilities and limitations of simulations performed using SpectraPlot. Further, this manuscript discusses the accuracy of several underlying approximations used to decrease computational time, namely, the use of far-wing cutoff criteria.
In the current study, a quantum-cascade-laser-based dual-comb spectrometer (DCS) was used to paint a detailed picture of a 1.0 ms high-temperature reaction between propyne and oxygen. The DCS interfaced with a shock tube to provide pre-ignition conditions of 1225 K, 2.8 atm, and 2% p-C3H4/18% O2/Ar. The spectrometer consisted of two free-running, non-stabilized frequency combs each emitting at 179 wavelengths between 1174 and 1233 cm -1 . A free spectral range, , of 9.86 GHz and a difference in comb spacing, Δ , of 5 MHz, enabled a theoretical time resolution of 0.2 µs but the data was time-integrated to 4 µs to improve SNR. The accuracy of the spectrometer was monitored using a suite of independent laser diagnostics and good agreement observed. Key challenges remain in the fitting of available high-temperature spectroscopic models to the observed spectra of a post-ignition environment.
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