NONLINEAR SPECTROSCOPY: EXPERIMENTS WITH MOLECULES IN A TWO COLOUR RESONANT IR RADIATION FIELD AND THE THEORETICAL MODELLING BASED ON THE OPTICAL BLOCH EQUATION.

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1995

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Ohio State University

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The recent achievements in the nonlinear optics opened the new possibilities in the IR high resolution spectroscopy. In this contribution a two colour spectroscopy of cooled SF6 and C2H4 seeded to He beam is presented. The molecules were excited by CWCO2 laser beam crossing the molecular beam. The frequencies of laser beams were tuned near CO2 lines by Optoacoustic Modulators (OAM) in the range ±500MHz. The spectral resolution 2 MHz was achieved. The excitation spectra were modelled in the frames of dressed state picture (DSP) and optical Bloch equations (OBE). In C2H4 the one quantum transition (ν=0,{4,1,3}→ν=1,{5,0,5} was investigated. At the moderate intensities of the laser fields (ν1andν2) the UP-DOWN-UP - (UDU) scheme of excitation was realized. The P*** \marginpar{Check*} with the frequencies ν1 and ν2 satisfying the resonant condition (N+1)⋅ν1Nν2=νtranstition at N = 1 and N = 2 were observed. The AC - Stark shifts of peaks were measured being in the agreement with the results of computer modelling based on OBE. The modelling showed that the increasing of the laser intensities leads to the transition from the UDU picture to the AC - Stark split one photon line picture. In SF6 the two quantum ladder type transitions (ν3=0,J=4→ν3=1,J=3→ν3=2,J=3) were investigated. The frequency ν1 was varied near the frequency of the first transition while ν2 was varied near as the frequency of the second transition and the frequency of the two photon transition. The peaks of the dressed states were observed and the AC - Stark shifts of different M - components were measured. The variation of the intensities of peaks due to the interference of many paths of excitation was observed. The DSP was used for the qualitative analysis of the interference effect and the quantitative modelling was based on OBE. The good agreement between measured and simulated spectra was achieved.

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General Physics Institute, Vavilov str. 38, 117942 Moscow, Russia Support by NATO collaborative research grant is gratefully acknowledged


Author Institution: Catholic University of Nijmegen, Toernooiveld, NL - 6525 ED Nijmegen, Netherlands

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