Research ArticlePHYSICS

Multidimensional spectroscopy with attosecond extreme ultraviolet and shaped near-infrared pulses

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Science Advances  28 Sep 2018:
Vol. 4, no. 9, eaau3783
DOI: 10.1126/sciadv.aau3783
  • Fig. 1 Experiment description.

    (A) Experiment design. In the non-multidimensional experiment, the pulse shaper is bypassed. (B) Geometry and timing diagram used over the course of the study. (C) Energy diagram. The shaded areas represent the wave packet created by the corresponding broadband pulse. (D) Phase-matching geometry. (E) Example of a double-sided Feynman diagram leading to 4WM signal emission.

  • Fig. 2 Spatial separation of interaction orders and 4WM time evolution.

    (A) Camera images at time 0 for 3 × 1012 W/cm2. (B) Time evolution of the 4WM signal. In this experiment, τ is set to 0 and T is scanned as indicated by the inset.

  • Fig. 3 Bright- and dark-state 2D spectra.

    (A) 4WM emission spectrum of the dark-state wave packet obtained with an unshaped pulse. The geometry and timing of the experiment in configuration I (T = 0, τ = 200 fs) are shown in the inset. The shaped pulse in the 2D experiment is indicated by an asterisk. A.U., arbitrary units. (B) 2D spectrum obtained from (A) in milli optical density (mOD). White lines link features originating from the same dark state. The main spectrum was collected with an SLM pixel binning of 10 pixels, while the inset spectrum was collected without pixel binning and shows the feature at (14.85 eV; 1.755 eV). The blue circles indicate the features following the time evolutions of [2P1/2]4p and [2P3/2]4p. (C) Bright-state emission spectrum obtained with an unshaped pulse and using the geometry and timing of configuration II (T = 60, τ = 60 fs) depicted in the inset. (D) 2D spectrum probing the bright-state wave packet at T = 60 fs obtained by shaping the pulse indicated by an asterisk in the inset of (C). The blue arrows indicate features following the time evolution of [2P3/2]5d/7s and [2P3/2]4d.

  • Fig. 4 Separation of emission pathways and suppression of quantum beats.

    (A) Time evolution of the dark-state 2D spectral feature at (14.85 eV; 1.76 eV). (B) Time evolution of the emission feature at 14.85 eV in the non-multidimensional experiment. The coherent sum of emission pathways leads to quantum beat oscillation in the time evolution of the emission line in (B). Quantum beat oscillations are not present in the time evolution of the 2D spectral feature in (A), indicating an efficient pathway separation.

  • Fig. 5 Effect of pulse shaping on time resolution.

    (A) Dark-state 4WM signal spectrum at T = 200 fs with NIR pulse with 0 radian phase shaping (blue) and π radian phase shaping. The beam geometry is shown in the inset. (B) Time evolution of the emission feature at 15.02 eV for the three types of modulations at 2.04 eV. The emission pathways at this energy are not resonant with the modulated NIR frequency; thus, the time traces are overlapped. (C) Time evolution of the emission feature at 15.38 eV for the two types of modulations at 2.04 eV. The pathways emitting at this energy are resonant with the shaped frequency and show strong modifications with phase shaping.

Supplementary Materials

  • Supplementary Materials

    This PDF file includes:

    • Fig. S1. Double-sided Feynman and Jablonski diagrams of two interfering pathways.
    • Fig. S2. Pulse characterization.
    • Fig. S3. Dark-state probing time evolution.

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