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

  • Author(s): Beck, AR;
  • Bernhardt, B;
  • Warrick, ER;
  • Wu, M;
  • Chen, S;
  • Gaarde, MB;
  • Schafer, KJ;
  • Neumark, DM;
  • Leone, SR
  • et al.

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 3d 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.

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