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Vibrational wave packets in the C 1Piu state of Cs2: Two color pump–probe experiments

J. Chem. Phys. 103, 10473 (1995); doi:10.1063/1.469897

Issue Date: 22 December 1995

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G. Rodriguez, P. C. John, and J. G. Eden
Everitt Laboratory, Department of Electrical and Computer Engineering, University of Illinois, Urbana, Illinois 61801
Two color, pump–probe laser experiments on the ~100 fs time scale have been applied to examining the dynamics of vibrational wave packets in the C 1Piu state of Cs2. Wave packets consisting of more than 20 C state vibrational levels are produced with an initial pulse having a central wavelength between ~620 and 680 nm. The temporal history of the wave packet is inferred from the time and energy-integrated photoelectron signal produced when the excited state is photoionized by a time-delayed pulse centered at 605, 610, 615, 617, or 620 nm. Because of the difference in equilibrium internuclear separations for the Cs2(C) and Cs<sup> + </sup><sub>2</sub>(X) states (DeltaRe[approximately-equal-to]0.75 Å), wave packets are readily observed (signal-to-noise ratio >~10) without the need to resort to mass selection techniques. Frequency analysis of the wave packet data shows a dominant (fundamental) component that decreases from 29 to ~28.3 cm−1 as the pump wavelength is tuned from 627 to 641 nm. Other spectral modes at ~23.5 and ~34 cm−1 and a weaker term at twice the fundamental frequency are also observed and quantum mechanical calculations of the wavepacket motion are in accord with the experimental results. ©1995 American Institute of Physics.
History: Received 10 August 1995; accepted 11 September 1995
Permalink: http://link.aip.org/link/?JCPSA6/103/10473/1
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KEYWORDS and PACS

Keywords
PACS
  • 33.20.Tp
    Molecular properties and interactions with photons Molecular spectra Vibrational analysis
  • 33.60.Cv
    Molecular properties and interactions with photons Photoelectron spectra Ultraviolet and vacuum ultraviolet photoelectron spectra
  • 39.30.+w
    Instrumentation and techniques for atomic and molecular physics Spectroscopic techniques
  • YEAR: 1995

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0021-9606 (print)   1089-7690 (online)
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