Abstract
A method for highly selective remote sensing of atmospheric trace polar molecular gases is described. Based on infrared-terahertz double-resonance spectroscopic techniques, the molecule-specific coincidence between the lines of a CO${}_{2}$ laser and rotational-vibrational molecular absorption transitions provide two dimensions of recognition specificity: infrared coincidence frequency and the corresponding terahertz frequency whose absorption strength is modulated by the laser. Atmospheric pressure broadening expands the molecular recognition ``specificity matrix'' by simultaneously relaxing the infrared coincidence requirement and strengthening the corresponding terahertz signature. Representative double-resonance spectra are calculated for prototypical molecules CH${}_{3}$F and CH${}_{3}$Cl and their principal isotopomers from which a heuristic model is developed to estimate the specificity matrix and double-resonance signature strength for any polar molecule.
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