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Published 1983 | Published
Journal Article Open

Phase Coherence in Multiple Pulse Optical Spectroscopy


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.

Additional Information

Copyright © 1983 Hindawi Publishing Corporation. This is an open access article distributed under the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. This research was supported by the National Science Foundation through Grant No. DMR81-05034 to Caltech. WSW was a National Science Foundation Postdoctoral Fellow at Caltech (1981). We are grateful to the National Science Foundation for making this work possible. AHZ would like to thank R. Silbey for inventing ZEWAWA. [A.H.Z. was a] Camille and Henry Dreyfus Foundation Teacher-Scholar. Arthur Amos Noyes Laboratory of Chemical Physics Contribution No. 6803. Laser Spectroscopy and Coherence, Laser Chemistry, 2, special issue 1, http://www.hindawi.com/journals/lc/volume-2/si.1.html.

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October 16, 2023