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A new method for highly selective remote sensing of atmospheric trace polarmolecular gases is described. Based on infrared/terahertz double resonancespectroscopic techniques, the molecule- specific coincidence between the linesof a CO2 laser and rotational-vibrational molecular absorption transitionsprovide two dimensions of recognition specificity: infrared coincidencefrequency and the corresponding terahertz frequency whose absorption strengthis modulated by the laser. Atmospheric pressure broadening expands themolecular recognition "specificity matrix" by simultaneously relaxing theinfrared coincidence requirement and strengthening the corresponding terahertzsignature. Representative double resonance spectra are calculated forprototypical molecules CH3F and CH3Cl and their principal isotopomers, fromwhich a heuristic model is developed to estimate the specificity matrix anddouble resonance signature strength for any polar molecule.

Infrared/Terahertz double resonance spectroscopy of CH3F and CH3Cl at atmospheric pressure