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Infrared Physics & Technology

Infrared neoclassical superradiance in a system of molecules with quasiequidistant spectrum of vibrational levels

Vl. V. Kocharovsky, Vl. V. Kocharovsky

Published Oct 1, 1995• 6 citations
Publisher
DOI
10.1016/1350-4495(95)00024-s

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The Journal of Physical Chemistry A•Jul 1, 2009•2 citations
Several polar molecules possessing strong far-infrared (FIR) transitions have been optically pumped by a mode-locked CO2TEA laser in a single-pass configuration. All the resulting FIR pulses are shorter than the sub-T2pump pulses; subnanosecond FIR pulses are observed. These short FIR pulses exhibit lethargic gain, stimulated Raman emission, and multiple-pulse superradiance. The experimental results are modeled by numerical solution of the Maxwell-density matrix equations for two fields interacting with a three-level system. Level degeneracy is included, and the pump is described by a multimode power spectrum with a parabolic envelope, resulting in a periodic train of pulses. Variation of the detuning of the pump from resonance allows simulation of the superradiant or Raman cases. This fully coherent model, which is the major contribution of this paper, explains key experimental observations such as the noncoincidence of the Raman peak with the pump modulation minimum and the enhancement of multiple-pulse superradiance due to remanent polarization.
In connection with attempts to form molecular Bose-Einstein condensates, there have been reports in the literature of the preparation of samples of translationally cold alkali metal dimers. The molecules in these samples are generally in excited vibrational levels. To form a stable Bose-Einstein condensate, the molecules must be de-excited to their lowest vibrational state. In this paper, we demonstrate that through the use of optimal control theory, it is possible to design a sequence of infrared laser pulses that will de-excite a sample of (7)Li2 molecules from the v = 10 vibrational level of their (1)Sigma(g)+ ground electronic state to their lowest v = 0 vibrational level with an overall efficiency of 91.1%.