Molecular dynamics and quantum chaos in small polyatomic molecules (CS_2, C_2H_2) through stimulated-emission pumping experiments and statistical Fourier-transform analysis - Laboratoire interdisciplinaire de Physique Accéder directement au contenu
Article Dans Une Revue Journal of the Optical Society of America B Année : 1990

Molecular dynamics and quantum chaos in small polyatomic molecules (CS_2, C_2H_2) through stimulated-emission pumping experiments and statistical Fourier-transform analysis

Résumé

The experimental study of the quantum properties of polyatomic molecules at high vibrational energy when classical chaos is present (quantum chaos) is discussed. Such a study requires the improvement of both experimental and analytical techniques. Methods by which stimulated-emission pumping spectroscopy and statistical Fourier-transform analysis of spectra can be successfully used to achieve this goal are emphasized. Stimulated-emission pumping and the statistical Fourier transform share the same concept of wave-packet preparation and evolution. This dynamical approach leads to interesting observations in molecular spectra. A numerical model of two coupled Morse oscillators provides information about the physical significance of the correlation hole observed in the Fourier transform of spectra of chaotic molecules. A relevant example in the experimental spectrum of CS2 shows the destabilization of given periodic orbits in a regime of soft chaos. In such a case the destabilizing process starts with Fermi resonances. In CS2 the chaos appears first in a portion of the degree of freedom (symmetric stretching and bending). In C2H2, in contrast, a new periodic orbit appears, corresponding to a new low-frequency mode that emerges from the chaotic bath of C2H2 and that could induce specific chemical reactions.
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Dates et versions

hal-01118144 , version 1 (18-02-2015)

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Jean-Paul, Pique. Molecular dynamics and quantum chaos in small polyatomic molecules (CS_2, C_2H_2) through stimulated-emission pumping experiments and statistical Fourier-transform analysis. Journal of the Optical Society of America B, 1990, 7 (9), pp.1816-1828. ⟨10.1364/JOSAB.7.001816⟩. ⟨hal-01118144⟩

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