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Optical multiple pulse sequences for multiphoton selective excitation and enhancement of forbidden transitions

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

In this paper we present novel and simple pulse sequences for enhancing the intensity of forbidden or highly nonresonant optical transitions. These sequences provide a straightforward approach to circumventing the most serious limitation of optical coherent transient spectroscopy: Available laser intensities are often insufficient to excite a significant fraction of the ground state population into desired excited states, either because of large inhomogeneous broadening or, in the case of multiphoton absorption, large anharmonicities. Optical phase modulation (which can be produced by an acousto-optic modulator) or amplitude modulation (which can be produced by an interferometer) with carefully chosen pulse flip angles and delays can effectively remove even very large energy mismatches, thus permitting essentially complete population inversions arbitrarily far from resonance. Coherent averaging theory and computer calculations are used to derive particularly valuable sequences. Pumping enhancement of 103-10 5 (depending on individual molecular parameters) for these modulated pulse sequences are predicted. Specific applications to multiphoton pumping of local vibrational modes are discussed. © 1983 American institute of Physics.

Duke Scholars

Published In

The Journal of Chemical Physics

DOI

ISSN

0021-9606

Publication Date

January 1, 1983

Volume

78

Issue

6

Start / End Page

3583 / 3592

Related Subject Headings

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

Citation

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Warren, W. S., & Zewail, A. H. (1983). Optical multiple pulse sequences for multiphoton selective excitation and enhancement of forbidden transitions. The Journal of Chemical Physics, 78(6), 3583–3592. https://doi.org/10.1063/1.445186
Warren, W. S., and A. H. Zewail. “Optical multiple pulse sequences for multiphoton selective excitation and enhancement of forbidden transitions.” The Journal of Chemical Physics 78, no. 6 (January 1, 1983): 3583–92. https://doi.org/10.1063/1.445186.
Warren WS, Zewail AH. Optical multiple pulse sequences for multiphoton selective excitation and enhancement of forbidden transitions. The Journal of Chemical Physics. 1983 Jan 1;78(6):3583–92.
Warren, W. S., and A. H. Zewail. “Optical multiple pulse sequences for multiphoton selective excitation and enhancement of forbidden transitions.” The Journal of Chemical Physics, vol. 78, no. 6, Jan. 1983, pp. 3583–92. Scopus, doi:10.1063/1.445186.
Warren WS, Zewail AH. Optical multiple pulse sequences for multiphoton selective excitation and enhancement of forbidden transitions. The Journal of Chemical Physics. 1983 Jan 1;78(6):3583–3592.

Published In

The Journal of Chemical Physics

DOI

ISSN

0021-9606

Publication Date

January 1, 1983

Volume

78

Issue

6

Start / End Page

3583 / 3592

Related Subject Headings

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