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Vibrational wave packets in the B 1Piu and D 1Sigma<sub>u</sub><sup>+</sup> states of Cs2: Determination of improved Cs<sub>2</sub><sup> + </sup>(X) and Cs2(B) spectroscopic constants

J. Chem. Phys. 113, 11009 (2000); doi:10.1063/1.1326065

Issue Date: 22 December 2000

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A. L. Oldenburg, P. C. John, and J. G. Eden
Laboratory for Optical Physics and Engineering, Department of Electrical and Computer Engineering, University of Illinois, Urbana, Illinois 61801
Vibrational wave packets in the B 1Piu and D 1Sigma<sub>u</sub><sup>+</sup> excited states of Cs2 have been studied on the ~100 fs time scale by pump–probe laser spectroscopy. The temporal behavior of the wave packets was monitored by photoionizing the electronically excited molecule with a time-delayed probe pulse and recording the time and energy-integrated photoelectron signal as a function of time delay between the pump and probe pulses. For the B 1Sigma<sub>u</sub><sup>+</sup> experiments, wave packets were produced by exciting the B 1Sigma<sub>u</sub><sup>+</sup><--X 1Sigma<sub>g</sub><sup>+</sup> transition in the ~740–790 nm region and subsequently detected by photoionizing the molecule at wavelengths between 565 nm and 600 nm. By simulating the experimentally observed transients with the density matrix formalism (and explicitly accounting for laser chirp and |Deltav|>1 coherences), improved values for the equilibrium internuclear separation for the Cs2(B 1Piu) state and Te for the Cs<sub>2</sub><sup>+</sup>(X) state were determined to be Re(B 1Piu) = 4.93±0.03 Å and Te[Cs<sub>2</sub><sup>+</sup>(X)] = 29 930±100 cm–1, respectively. Similar experiments were conducted for the D 1Sigma<sub>u</sub><sup>+</sup> state. Wave packets composed of vibrational levels (v[prime][approximate]40–50) perturbed by the bound 2 3Piou state were produced on the D 1Sigma<sub>u</sub><sup>+</sup> potential surface by driving the D 1Sigma<sub>u</sub><sup>+</sup><--X 1Sigma<sub>g</sub><sup>+</sup> transition in the 575–610 nm spectral interval. ©2000 American Institute of Physics.
History: Received 13 July 2000; accepted 26 September 2000
Permalink: http://link.aip.org/link/?JCPSA6/113/11009/1
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KEYWORDS and PACS

Keywords
PACS
  • 33.20.Kf
    Molecular properties and interactions with photons Molecular spectra Visible spectra
  • 33.20.Ea
    Molecular properties and interactions with photons Molecular spectra Infrared spectra
  • 33.15.Mt
    Molecular properties and interactions with photons Properties of molecules and molecular ions Rotation, vibration, and vibration–rotation constants
  • YEAR: 2000

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