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Sub-Doppler spectra of infrared hyperfine transitions of nitric oxide using a pulse modulated quantum cascade laser : rapid passage, free induction decay, and the ac Stark effect

Duxbury, Geoffrey and Kelly, James F. and Blake, Thomas A. and Langford, Nigel (2012) Sub-Doppler spectra of infrared hyperfine transitions of nitric oxide using a pulse modulated quantum cascade laser : rapid passage, free induction decay, and the ac Stark effect. Journal of Chemical Physics, 136 (17). ISSN 0021-9606

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Abstract

Using a low power, rapid (nsec) pulse-modulated quantum cascade (QC) laser, collective coherent effects in the 5 mu m spectrum of nitric oxide have been demonstrated by the observation of sub-Doppler hyperfine splitting and also Autler-Townes splitting of Doppler broadened lines. For nitrous oxide, experiments and model calculations have demonstrated that two main effects occur with pulse-modulated (chirped) quantum cascade lasers: free induction decay signals, and signals induced by rapid passage during the laser chirp. In the open shell molecule, NO, in which both Lambda-doubling splitting and hyperfine structure occur, laser field-induced coupling between the hyperfine levels of the two Lambda-doublet components can induce a large ac Stark effect. This may be observed as sub-Doppler structure, field-induced splittings, or Autler-Townes splitting of a Doppler broadened line. These represent an extension of the types of behaviour observed in the closed shell molecule nitrous oxide, using the same apparatus, when probed with an 8 mu m QC laser. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4710542]