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A multiple pass optical cell and method comprising providing a pair of opposed mirrors, one cylindrical and one spherical, introducing light into the cell via an entrance mechanism, and extracting light from the cell via an exit mechanism, wherein the entrance mechanism and exit mechanism are coextensive or non-coextensive.
A multiple pass optical cell and method comprising providing a pair of opposed cylindrical mirrors having curved axes with substantially equal focal lengths, positioning an entrance hole for introducing light into the cell and an exit hole for extracting light from the cell, wherein the entrance hole and exit hole are coextensive or non-coextensive, introducing light into the cell through the entrance hole, and extracting light from the cell through the exit hole.
In this paper we report line shape parameters of 12CH4 for several hundred 2V(sub 3) transitions in the spectral regions 5891-5996 cm( exp -1) (P branch) and 6015-6115 cm(exp -1) (R branch). Air- and self-broadening coefficients were measured as a function of temperature; line mixing via off-diagonal relaxation matrix element coefficients was also obtained for 47 transition pairs. In total, nearly 1517 positions and intensities were retrieved, but many transitions were too weak for the line shape study. For this analysis, we used 25 high-resolution (0.0056 and 0.0067 cm(ex[ -1) and high signal-to-noise (S/N) spectra of high-purity 12CH4 and the same high-purity 12CH4 broadened by dry air recorded at different sample temperatures between 130 K and 295 K with the Bruker IFS 125HR Fourier transform spectrometer at JPL. Three different absorption cells were used (1) a White cell set to a path length of 13.09 m for room temperature data, (2) a single-pass 0.2038 m long coolable cell (for self-broadening) and (3) a multipass cell with 20.941 m total path coolable Herriott cell (for air-broadening). In total there were 13 spectra with pure 12CH4 (0.27-599 Torr) and 12 air-broadened spectra with total sample pressures of 80-805 Torr and volume mixing ratios (VMR) of methane between 0.18 and 1.0. An interactive multispectrum nonlinear least-squares technique was employed to fit the individual P10-P1 and R0-R10 manifolds in all the spectra simultaneously. Results obtained from the present analysis are compared to other recent measurements.
We present a miniaturized and simplified version of a gas correlation radiometer (GCR) capable of simultaneously mapping multiple trace gases and identifying active regions on the Mars surface. Gas correlation radiometry (GCR) has been shown to be a sensitive and versatile method for detecting trace gases in Earth's atmosphere. Reduction of the size and mass of the GCR was achieved by implementing compact, light-weight 1 mm inner diameter hollow-core optical fibers (hollow waveguides) as the gas correlation cells. In a comparison with an Earth orbiting CO2 GCR instrument, exchanging the 10 m multipass cells with hollow waveguide gas correlation cells of equivalent path length reduces the mass from approximately 150 kg to approximately 0.5 kg, and reduces the volume from 1.9 m x 1.3 m x 0.86 m to a small bundle of fiber coils approximately 1 meter in diameter by 0.05 m in height (mass and volume reductions of greater than 99%). A unique feature of this instrument is its stackable module design, with a single module for each trace gas. Each of the modules is self-contained, and fundamentally identical; differing by the bandpass filter wavelength range and gas mixtures inside the hollow-waveguide absorption cells. The current configuration contains four stacked modules for simultaneous measurements of methane (CH4), formaldehyde (H2CO), water vapor (H2O), and deuterated water vapor (HDO) but could easily be expanded to include measurements of additional species of interest including nitrous oxide (N2O), hydrogen sulfide (H2S), methanol (CH3OH), and sulfur dioxide (SO2), as well as carbon dioxide (CO2) for a simultaneous measure of mass balance. Preliminary results indicate that a 1 ppb detection limit is possible for both formaldehyde and methane with one second of averaging. Using non-optimized components, we have demonstrated an instrument sensitivity equivalent to approximately 30 ppb for formaldehyde, and approximately 500 ppb for methane. We expect custom bandpass filters and 6 m long waveguides to significantly improve these promising results. Ongoing testing is being conducted on water vapor and deuterated water vapor.
Gas correlation radiometry (GCR) has been shown to be a sensitive and versatile method for detecting trace gases in Earth's atmosphere. Here, we present a miniaturized and simplified version of this instrument capable of mapping multiple trace gases and identifying active regions on the Mars surface. Reduction of the size and mass of the GCR instrument has been achieved by implementing a lightweight, 1 mm inner diameter hollow-core optical fiber (hollow waveguide) for the gas correlation cell. Based on a comparison with an Earth orbiting CO2 gas correlation instrument, replacement of the 10 meter mUltipass cell with hollow waveguide of equivalent pathlength reduces the cell mass from approx 150 kg to approx 0.5 kg, and reduces the volume from 1.9 m x 1.3 m x 0.86 m to a small bundle of fiber coils approximately I meter in diameter by 0.05 m in height (mass and volume reductions of >99%). This modular instrument technique can be expanded to include measurements of additional species of interest including nitrous oxide (N2O), hydrogen sulfide (H2S), methanol (CH3OH), and sulfur dioxide (SO2), as well as carbon dioxide (CO2) for a simultaneous measure of mass balance.
A high-power, narrow-linewidth Yb fiber laser with a fiber Bragg grating (FBG) pumped difference frequency generation (DFG) in a periodically poled lithium niobate (PPLN) crystal was investigated in detail. A mid-IR power of approximately 2.3 microW at 3.3 micrometers with a slope efficiency of 0.85 mW/W2 was achieved. A Doppler-broadened absorption spectrum of CH4 at 3038.497 cm-1 (3.2911 micrometers) was obtained with a 0.1-m long-gas cell at a pressure of 133 Pa. The linewidth of the DFG source was evaluated to be less than 96 MHz from the observed spectral linewidth. Real-time monitoring of CH4 (approximately 1.78 ppm) in ambient air in a multipass cell which has an optical path length of 10 m was also demonstrated.
A detailed study of the detection of trace gases at atmospheric pressure using tunable diode lasers is described. The influence of multipass cells, retroreflectors and topographical targets is examined. The minimum detectable infrared absorption ranges from 0.1 percent for a pathlength of 1.2 km to 0.01 percent over short pathlengths. The factors which limit this sensitivity are discussed, and the techniques are illustrated by monitoring atmospehric CO2 and CH4.
A simple method is described for substantially reducing the amplitude of interference fringes that limit the sensitivities of tunable-laser high-resolution absorption spectrometers. A lead-salt diode laser operating in the 7-micron region is used with a single Brewster-plate spoiler to reduce the fringe amplitude by a factor of 30 and also to allow the detection of absorptances 0.001 percent in a single laser scan without subtraction techniques, without complex frequency modulation, and without distortion of the molecular line-shape signals. Application to multipass-cell spectrometers is described.
Oscillating Brewster plate reduces effects of unwanted interference fringes on absorption-spectroscopic measurements obtained with tuned diode lasers. Plate modulates optical-path length past several resonance peaks causing interference fringes to pass by rapidly and become blurred. Thus, fringe effects averaged out over time. Technique used at other wavelengths from ultraviolet to infrared and in spectrometers with short or long optical paths, including those with retroreflectors or multipass cells.
A simple optomechanical method and apparatus is described for substantially reducing the amplitude of unwanted multiple interference fringes which often limit the sensitivities of tunable laser absorption spectrometers. An exterior cavity is defined by partially transmissible surfaces such as a laser exit plate, a detector input, etc. That cavity is spoiled by placing an oscillating plate in the laser beam. For tunable diode laser spectroscopy in the mid-infrared region, a Brewster-plate spoiler allows the harmonic detection of absorptances of less than 10 to the -5 in a single laser scan. Improved operation is achieved without subtraction techniques, without complex laser frequency modulation, and without distortion of the molecular lineshape signal. The technique is applicable to tunable lasers operating from UV to IR wavelengths and in spectrometers which employ either short or long pathlengths, including the use of retroreflectors or multipass cells.
The nu3 transitions of N3 radicals produced by HN3-Cl reactions in a multipass cell (effective path length 100 m) are investigated experimentally using a Fourier-transform spectrometer with maximum resolution 0.004/cm. A total of 176 rotation-vibration lines are listed in a table and used, in combination with published data on 240 optical lines (Douglas and Jones, 1965), to determine the nu3 molecular constants. The lower-than-expected value of the nu3 fundamental frequency (1644.6784/cm) is attributed to the vibronic interaction discussed by Kawaguchi et al. (1981).
Interpretation of planetary methane (CH4) visible-near IR spectra, used to develop models of planetary atmospheres, has been hampered by a lack of suitable laboratory spectroscopic data. The particular CH4 spectral bands are due to intrinsically weak, high overtone-combination transitions too complex for classical spectroscopic analysis. The traditional multipass cell approach to measuring spectra of weakly absorbing species is insufficiently sensitive to yield reliable results for some of the weakest CH4 absorption features and is difficult to apply at the temperatures of the planetary environments. A time modulated form of intracavity laser spectroscopy (ILS), has been shown to provide effective absorption pathlengths of 100 to 200 km with sample cells less than 1 m long. The optical physics governing this technique and the experimental parameters important for obtaining reliable, quantitative results are now well understood. Quantitative data for CH4 absorption obtained by ILS have been reported recently. Illustrative ILS data for CH4 absorption in the 619.7 nm and 681.9 nm bands are presented. New ILS facilities at UM-St. Louis will be used to measure CH4 absorption in the 700 to 1000 nm region under conditions appropriate to the planetary atmospheres.
An improved real-time methane monitor based on infrared absorption of the 3.39 micron line of a HeNe laser is described. Real time in situ measurement of methane has important applications in stratospheric and tropospheric chemistry, especially when high accuracy measurements can be made rapidly, providing fine spatial-scale information. The methane instrument provides 5 ppb resolution in a 1 sec averaging time. A key feature in this instrument is the use of magnetic (Zeeman) broadening to achieve continuous tunability with constant output power over a range of 0.017/cm. The instruments optical absorption path length is 47 m through sampled air held at 50 torr in a multipass cell of the Herriott (off-axis resonator) type. A microprocessor controls laser frequency and amplitude and collects data with minimal operator attention. The instrument recently has been used to measure methane emissions from a variety of natural and artificial terrestrial sources.
IR absorption using tunable diode laser spectroscopy provides a sensitive and quantitative detection method for laboratory kinetic studies of atmospheric trace gases. Improvements in multipass cell design, real time signal processing, and computer controlled data acquisition and analysis have extended the applicability of the technique. We have developed several optical systems using off-axis resonator mirror designs which maximize path length while minimizing both the sample volume and the interference fringes inherent in conventional 'White' cells. Computerized signal processing using rapid scan (300 kHz), sweep integration with 100 percent duty cycle allows substantial noise reduction while retaining the advantages of using direct absorption for absolute absorbance measurements and simultaneous detection of multiple species. Peak heights and areas are determined by curve fitting using nonlinear least square methods. We have applied these techniques to measurements of: (1) heterogeneous uptake chemistry of atmospheric trace gases (HCl, H2O2, and N2O5) on aqueous and sulfuric acid droplets; (2) vapor pressure measurements of nitric acid and water over prototypical stratospheric aerosol (nitric acid trihydrate) surfaces; and (3) discharge flow tube kinetic studies of the HO2 radical using isotopic labeling for product channel and mechanistic analysis. Results from each of these areas demonstrate the versatility of TDL absorption spectroscopy for atmospheric chemistry applications.
A vertical ozone profile obtained by an in situ ozone sonde from 16 km to 45 km, has allowed to observe local ozone concentration variations. These variations can be observed, thanks to a fast measurement system based on a UV absorption KrF excimer laser beam in a multipass cell. Ozone standard deviation versus altitude calculated from the mean is derived. Ozone variations or fluctuations are correlated with the different dynamic zones of the stratosphere.
Sub-micrometer sized sulfuric acid H2SO4 particles were generated using a constant output atomizer source. The particles were then exposed to water vapor before being injected into a low temperature cell. Multipass transmission Fourier Transformation Infrared (FTIR) spectroscopy was used to determine the phase and composition of the aerosols as a function of time for periods of up to five hours. Binary H2SO4H2O aerosols with compositions from 35 to 95 wt % H2SO4 remained liquid for over 3 hours at room temperatures ranging from 189-240 K. These results suggest that it is very difficut to freeze SSAs via homogeneous nucleation. Attempts to form aerosols more dilute than 35 wt % H2SO4 resulted in ice formation.
A variable duty cycle quasi-cw frequency scanning technique was applied to reduce thermal effects resulting from the high heat dissipation of type I quantum-cascade lasers. This technique was combined with a 100-m path-length multipass cell and a zero-air background-subtraction technique to enhance detection sensitivity to a parts-in-10(9) (ppb) concentration level for spectroscopic trace-gas detection of CH4, N2O, H2O, and C2H5OH in ambient air at 7.9 micrometers. A new technique for analysis of dense high resolution absorption spectra was applied to detection of ethanol in ambient air, yielding a 125-ppb detection limit.
A compact, portable and robust room temperature CH4 sensor is reported. By difference frequency mixing a 500 mW alpha-DFB diode laser at 1066 nm and an erbium-doped fiber amplified 1574 nm DFB diode laser in periodically poled lithium niobate up to 7 (mu)W of narrowband radiation at 3.3 microns is generated. Real-time monitoring of CH4 over a 7 day period using direct absorption in an open-path multipass cell (L = 36 m) demonstrates a detection precision of +/- 14 ppb.