Quantitative rotational spectroscopy for HITRAN
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Remote sensing of rotational transitions in the Earth's atmosphere has become an important method for the retrieval of geophysical temperatures, pressures and chemical composition profiles that requires accurate spectral information. This paper highlights the current status of rotational data that are useful for atmospheric measurements, with a discussion of the types the rotational lineshape measurements that are not generally available in either online repository.
Rotational spectroscopy of atmospheric molecules has long been a hallmark of laboratory and field studies at the Jet Propulsion Laboratory. in addition to maintenance of the millimeter and submillimeter spectral line catalog, the laboratory has actively purued the challenging laboratory tasks of quantitative linewidth measurements and transient species identification.
The status of modelling the coherent anti-Stokes Raman spectroscopy (CARS) spectra of molecules important in combustion, such as N2, H2O, and CO2, is reviewed. It is shown that accurate modelling generally requires highly precise knowledge of line positions and reasonable estimates of Raman linewidths, and the sources of these data are discussed. CARS technique and theory is reviewed, and the status of modelling the phenomenon of collisional narrowing at pressures well above atmospheric for N2, H2O, and CO2 is described. It is shown that good agreement with experiment can be achieved using either the Gordon rotational diffusion model or phenomenological models for inelastic energy transfer rates.
Various lidar methods have been developed for measuring the atmospheric temperature, making use of the temperature dependant characteristics of rotational Raman scattering (RRS) from nitrogen and oxygen, and Rayleigh or Rayleigh-Brillowin scattering (RS or RBS). These methods have various advantages and disadvantages as compared to each other but their potential accuracies are principal characteristics of their efficiency. No systematic attempt has been undertaken so far to compare the efficiences, in the above meaning, of different temperature lidar methods. Two RRS techniques have been compared. Here, we do such a comparison using two methods based on the detection and analysis of RS (RBS) spectra. Four methods are considered here for measuring the atmospheric temperature. One of them (Schwiesow and Lading, 1981) is based on an analysis of the RS linewidth with two Michelson interferometers (MI) in parallel. The second method (Shimisu et al., 1986) employs a high-resolution analysis of the RBS line shape. The third method (Cooney, 1972) employs the temperature dependance of the RRS spectrum envelope. The fourth method (Armstrong, 1974) makes use of a scanning Fabry-Perot interferometer (FPI) as a comb filter for processing the periodic RRS spectrum of the nitrogen. Let us denote the corresponding errors in measuring the temperature by sigma(sub MI), sigma(sub HR), sigma(sub ENV), and sigma(sub FPI). Let us also define the ratios chi(sub 1) = sigma(sub MI)/sigma(sub ENV), chi(sub 2) = sigma(sub HR)/sigma(sub ENV), and chi(sub 3) = sigma(sub FPI)/sigma(sub ENV) interpreted as relative errors with respect to sigma(sub ENV).