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Wave-packet dynamics in the Li2 E(1Sigma<sup> + </sup><sub>g</sub>) shelf state: Simultaneous observation of vibrational and rotational recurrences with single rovibronic control of an intermediate state

J. Chem. Phys. 103, 7269 (1995); doi:10.1063/1.470301

Issue Date: 1 November 1995

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John M. Papanikolas, Richard M. Williams, Paul D. Kleiber, Jeffrey L. Hart, Carsten Brink, Stephen D. Price, and Stephen R. Leone
JILA, National Institute of Standards and Technology and University of Colorado, Department of Chemistry and Biochemistry, University of Colorado, Boulder, Colorado 80309-0440
A three-step excitation sequence is used to study the wave-packet dynamics in the E(1Sigma<sup> + </sup><sub>g</sub>) ``shelf'' state of lithium dimer. In the first excitation step, a continuous wave (cw) dye laser prepares a single rovibrational level (v=14, J=22) in the intermediate 7Li2 A(1Sigma<sup> + </sup><sub>u</sub>) state. Ultrafast excitation of this single level with a 200 fs laser pulse centered at 803 nm creates a rovibrational wave packet (v=13–16; J=21 and 23) in the shelf region of the E(1Sigma<sup> + </sup><sub>g</sub>) state. The motion of this three-dimensional wave packet is probed via ionization by a second ultrafast laser pulse of the same color. The initial cw excitation step allows precise control of the states that compose the wave packet. Fourier analysis of the pump–probe transients shows 15 frequency components that correspond to energy differences between the levels that constitute the wave packet. Because of the large rotational energy splitting, the rotational beats occur in the same frequency range as the vibrational beats. Experiments performed with parallel and perpendicular pump-probe polarizations provide a ``magic angle'' transient in which only the pure vibrational beats are observed, thus aiding in the spectroscopic assignment. The observed beat frequencies agree well with conventional high resolution frequency-domain spectroscopy. Applications of the intermediate-state control of the initial wave packet are discussed. ©1995 American Institute of Physics.
History: Received 15 May 1995; accepted 20 July 1995
Permalink: http://link.aip.org/link/?JCPSA6/103/7269/1
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KEYWORDS and PACS

Keywords
PACS
  • 33.20.Sn
    Molecular properties and interactions with photons Molecular spectra Rotational analysis
  • 33.20.Tp
    Molecular properties and interactions with photons Molecular spectra Vibrational analysis
  • 33.20.Vq
    Molecular properties and interactions with photons Molecular spectra Vibrationrotation analysis
  • YEAR: 1995

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