Attosecond transient absorption probing of electronic superpositions of bound states in neon: detection of quantum beats

Annelise R Beck; Birgitta Bernhardt; Erika R Warrick; Mengxi Wu; Shaohao Chen; Mette B Gaarde; Kenneth J Schafer; Daniel M Neumark; Stephen R Leone

doi:10.1088/1367-2630/16/11/113016

New Journal of Physics (Jan 2014)

Attosecond transient absorption probing of electronic superpositions of bound states in neon: detection of quantum beats

Annelise R Beck,
Birgitta Bernhardt,
Erika R Warrick,
Mengxi Wu,
Shaohao Chen,
Mette B Gaarde,
Kenneth J Schafer,
Daniel M Neumark,
Stephen R Leone

Affiliations

Annelise R Beck: Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California, 94720, USA; Department of Chemistry, University of California , Berkeley, California 94720, USA
Birgitta Bernhardt: Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California, 94720, USA; Department of Chemistry, University of California , Berkeley, California 94720, USA
Erika R Warrick: Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California, 94720, USA; Department of Chemistry, University of California , Berkeley, California 94720, USA
Mengxi Wu: Department of Physics and Astronomy, Louisiana State University , Baton Rouge, Louisiana, 70803, USA
Shaohao Chen: Department of Physics and Astronomy, Louisiana State University , Baton Rouge, Louisiana, 70803, USA
Mette B Gaarde: Department of Physics and Astronomy, Louisiana State University , Baton Rouge, Louisiana, 70803, USA
Kenneth J Schafer: Department of Physics and Astronomy, Louisiana State University , Baton Rouge, Louisiana, 70803, USA
Daniel M Neumark: Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California, 94720, USA; Department of Chemistry, University of California , Berkeley, California 94720, USA
Stephen R Leone: Ultrafast X-ray Science Laboratory, Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California, 94720, USA; Department of Chemistry, University of California , Berkeley, California 94720, USA; Department of Physics, University of California , Berkeley, California, 94720, USA

DOI: https://doi.org/10.1088/1367-2630/16/11/113016
Journal volume & issue: Vol. 16, no. 11
p. 113016

Abstract

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Electronic wavepackets composed of multiple bound excited states of atomic neon lying between 19.6 and 21.5 eV are launched using an isolated attosecond pulse. Individual quantum beats of the wavepacket are detected by perturbing the induced polarization of the medium with a time-delayed few-femtosecond near-infrared (NIR) pulse via coupling the individual states to multiple neighboring levels. All of the initially excited states are monitored simultaneously in the attosecond transient absorption spectrum, revealing Lorentzian to Fano lineshape spectral changes as well as quantum beats. The most prominent beating of the several that were observed was in the spin–orbit split 3 d absorption features, which has a 40 femtosecond period that corresponds to the spin–orbit splitting of 0.1 eV. The few-level models and multilevel calculations confirm that the observed magnitude of oscillation depends strongly on the spectral bandwidth and tuning of the NIR pulse and on the location of possible coupling states.

Published in New Journal of Physics

ISSN: 1367-2630 (Online)
Publisher: IOP Publishing
Country of publisher: United Kingdom
LCC subjects: Science: Physics
Website: https://iopscience.iop.org/journal/1367-2630

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