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Phase and amplitude control in the formation and detection of rotational wave packets in the E 1 Sigma<sub>g</sub><sup>+</sup> state of Li2

J. Chem. Phys. 108, 9259 (1998); doi:10.1063/1.476381

Issue Date: 8 June 1998

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Radoslaw Uberna, Munira Khalil, Richard M. Williams, John M. Papanikolas, and Stephen R. Leone
JILA, National Institute of Standards and Technology and University of Colorado, Department of Chemistry and Biochemistry and Department of Physics, Boulder, Colorado 80309-0440
Femtosecond laser pulse amplitude/phase masking techniques are employed to control the formation and detection of rotational wave packets in the electronic E 1 Sigma<sub>g</sub><sup>+</sup> state of lithium dimer. The wave packets are prepared by coherent excitation of rovibronic E 1 Sigma<sub>g</sub><sup>+</sup>(nuE,JE) states of Li2 from a single intermediate state, A 1 Sigma<sub>u</sub><sup>+</sup>(nuA = 11, JA = 28), and probed by time-resolved photoionization. In the detection step, the wave packet is projected onto the X 2 Sigma<sub>g</sub><sup>+</sup> state of Li<sub>2</sub><sup> + </sup>. New resonance structure in the X 2 Sigma<sub>u</sub><sup>+</sup> ionic state continuum is obtained by measuring the wave packet signal modulation amplitude as a function of the frequencies removed from the spectrally dispersed probe pulse by insertion of a wire mask in a single-grating pulse shaper. A split glass phase mask inserted into the pulse shaper is used to produce step function changes in the spectral phase of the pulse. The phase relation among the wave packet states is varied by changing the relative phases of spectral components in the pump pulse and is monitored by measuring the changes in the phase of the rotational wave packet recurrences using an unmodified probe pulse. By altering the relative phases among the wave packet components, the spatial distribution of the initial wave packet probability density is varied, resulting in phase-dependent "alignment" of the probability density in angular space. Phase changes in the signal recurrences are also observed when a phase modified pulse is used in the wave packet detection step after wave packet preparation with an unmodified pulse. The formation and detection of the wave packets is discussed in terms of quantum interference between different excitation routes. The relative phase factors encoded in a single optical pulse (pump or probe) are transferred into the interference term of the measured signal through the molecule–photon interaction. ©1998 American Institute of Physics.
History: Received 27 January 1998; accepted 3 March 1998
Permalink: http://link.aip.org/link/?JCPSA6/108/9259/1
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KEYWORDS and PACS

Keywords
PACS
  • 33.15.Mt
    Molecular properties and interactions with photons Properties of molecules and molecular ions Rotation, vibration, and vibrationrotation constants
  • 33.20.Sn
    Molecular properties and interactions with photons Molecular spectra Rotational analysis
  • 42.65.Re
    Optics Nonlinear optics Ultrafast processes; optical pulse generation and pulse compression
  • 33.20.Wr
    Molecular properties and interactions with photons Molecular spectra Vibronic, rovibronic, and rotationelectron-spin interactions
  • 33.20.Vq
    Molecular properties and interactions with photons Molecular spectra Vibrationrotation analysis
  • YEAR: 1998

PUBLICATION DATA

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