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Multiple phase-coherent laser pulses in optical spectroscopy. I. The technique and experimental applications

Publication ,  Journal Article
Warren, WS; Zewail, AH
Published in: The Journal of Chemical Physics
January 1, 1983

In this series of papers we report on the generation and application of multiple pulse phase coherent sequences in optical spectroscopy. In this paper the effects of intense pulse trains on systems with only two resonant energy levels are analyzed, with particular attention to the effects of extreme inhomogeneous broadening and population depletion to nonresonant levels. It is shown that these effects, which are present in virtually all optical systems, make the simple gyroscopic model of optical coherent transients invalid. Exact calculations show, e.g., that a two-pulse photon echo is not maximized by a 1:2 length ratio for the pulses; that the maximum excited state population is not created by a 180° pulse; and that three equal pulses are almost as effective as a 1:2:1 ratio for producing three pulse echoes. The role of pulse phase is extensively analyzed. Pulse sequences are proposed and experimentally demonstrated which permit optical phase sensitive detection and measurement of ground state relaxation parameters. The experimental results are based on an extension of the acousto-optic modulation and fluoresence detection techniques of Zewail and Orlowski [Zewail et al., Chem. Phys. Lett. 48, 256 (1977); Orlowski et al., ibid 54, 197 (1978)]. The relative merits of fluorescence and transverse polarization detection are discussed, and fluorescence detection is shown to be more generally useful for these new sequences. Finally, composite pulse trains are shown to be capable of substantially increasing the signal available from highly inhomogenously broadened transitions. In paper II we extend the treatment to multilevel systems with some emphasis on solid state applications. © 1983 American Institute of Physics.

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Published In

The Journal of Chemical Physics

DOI

ISSN

0021-9606

Publication Date

January 1, 1983

Volume

78

Issue

5

Start / End Page

2279 / 2297

Related Subject Headings

  • Chemical Physics
  • 51 Physical sciences
  • 40 Engineering
  • 34 Chemical sciences
  • 09 Engineering
  • 03 Chemical Sciences
  • 02 Physical Sciences
 

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Warren, W. S., & Zewail, A. H. (1983). Multiple phase-coherent laser pulses in optical spectroscopy. I. The technique and experimental applications. The Journal of Chemical Physics, 78(5), 2279–2297. https://doi.org/10.1063/1.445083
Warren, W. S., and A. H. Zewail. “Multiple phase-coherent laser pulses in optical spectroscopy. I. The technique and experimental applications.” The Journal of Chemical Physics 78, no. 5 (January 1, 1983): 2279–97. https://doi.org/10.1063/1.445083.
Warren WS, Zewail AH. Multiple phase-coherent laser pulses in optical spectroscopy. I. The technique and experimental applications. The Journal of Chemical Physics. 1983 Jan 1;78(5):2279–97.
Warren, W. S., and A. H. Zewail. “Multiple phase-coherent laser pulses in optical spectroscopy. I. The technique and experimental applications.” The Journal of Chemical Physics, vol. 78, no. 5, Jan. 1983, pp. 2279–97. Scopus, doi:10.1063/1.445083.
Warren WS, Zewail AH. Multiple phase-coherent laser pulses in optical spectroscopy. I. The technique and experimental applications. The Journal of Chemical Physics. 1983 Jan 1;78(5):2279–2297.

Published In

The Journal of Chemical Physics

DOI

ISSN

0021-9606

Publication Date

January 1, 1983

Volume

78

Issue

5

Start / End Page

2279 / 2297

Related Subject Headings

  • Chemical Physics
  • 51 Physical sciences
  • 40 Engineering
  • 34 Chemical sciences
  • 09 Engineering
  • 03 Chemical Sciences
  • 02 Physical Sciences