A two-state vibrational wave packet is prepared in a low-lying Rydberg state of jet cooled (, and ) by two-photon excitation with pulses from an ultrafast laser. The wave packet is detected by autoionization following excitation with time-delayed pulses to the and Rydberg states in the angular momentum core state. Autoionization of each state occurs to the state of the ion through spin-orbit ionization. Photoelectron spectroscopy is used to differentiate between the and ejected photoelectrons. Detection of the wave packet recurrences via the and Rydberg states reveals a phase-shift difference of the recurrences between the two final states. In each case, transitions are observed since wave packet recurrences are detected. By fitting the observed phase change of the recurrences with a simple model for the overlap amplitudes and assumptions about the potentials, we estimate, within the context of the model, that approximately 0.6% of the transitions may be attributed to transitions between the initial Rydberg superposition state and the final Rydberg detection state.
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7 May 2006
Research Article|
May 04 2006
Coherent ultrafast photoelectron spectroscopy in : An alternative method for measuring transitions in Rydberg-to-Rydberg excitations
Vasilios G. Stavros;
Vasilios G. Stavros
a)
Departments of Chemistry and Physics and Lawrence Berkeley National Laboratory,
University of California
, Berkeley, California 94720
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Lana Lau;
Lana Lau
Departments of Chemistry and Physics and Lawrence Berkeley National Laboratory,
University of California
, Berkeley, California 94720
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Daniel Strasser;
Daniel Strasser
Departments of Chemistry and Physics and Lawrence Berkeley National Laboratory,
University of California
, Berkeley, California 94720
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Stephen R. Leone
Stephen R. Leone
Departments of Chemistry and Physics and Lawrence Berkeley National Laboratory,
University of California
, Berkeley, California 94720
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a)
Present address: Department of Chemistry, University of Warwick, Coventry, CV4 7AL, United Kingdom.
J. Chem. Phys. 124, 174307 (2006)
Article history
Received:
February 07 2006
Accepted:
March 03 2006
Citation
Vasilios G. Stavros, Lana Lau, Daniel Strasser, Stephen R. Leone; Coherent ultrafast photoelectron spectroscopy in : An alternative method for measuring transitions in Rydberg-to-Rydberg excitations. J. Chem. Phys. 7 May 2006; 124 (17): 174307. https://doi.org/10.1063/1.2190218
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