Abstract

In this paper we describe a new technique for the generation of multiple pulse phase coherent sequences in optical spectroscopy. The technique is an extension of the acousto-optic modulation and fluorescence detection methods developed for optical transitions by Zewail and Orlowski (Zewail et al., Chem. Phys. Lett.48, 256 (1977); Orlowski et al., Chem. Phys. Lett.54, 197 (1978)). Application of these multiple pulse trains (of different phases) to optical transitions of two-level and multilevel systems is demonstrated experimentally. It is shown that they can be used to (i) suppress spontaneous emission background, (ii) enhance coherent transients such as photon echoes, (iii) measure additional relaxation parameters in systems with complex rotational-vibrational levels, and (iv) enhance the effective laser bandwidths through composite pulse trains, as demonstrated on I2 gas. Finally, the potential of this development is extended to the possibility of observing selective multiquantum excitation in molecules.