Abstract
Based on ab initio three-dimensional functions of potential energy, electric dipole and transition moments, the rovibronic energy levels, eigenfunctions, and radiative transition probabilitiw have been calculated for several triatomic molecules (H 2 O, HDO, SiH 2 , and the Renner-Teller system of NH 2 ). Using ultrashort infrared picosecond laser pulses, the state-selective multiphoton excitations of the υ 1 =4 (symmetric stretching) vibrational eigenstate of these molecules as well as the corresponding diatomics OH, SiH, and NH have been investigated. The OH stretching mode in HDO and in H 2 O can be selectively populated. Strong anharmonic coupling (SiH 2 ) or Renner-Teller coupling to another electronic state (NH 2 ) may, however, considerably reduce the achievable state selectivity
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