Spooktroscopy: a ghost imaging approach to ultrafast absorption spectroscopy

ORAL

Abstract

With the advent of an X-ray free-electron laser, scientists can probe femtosecond ultrafast molecular dynamics with atomic-site specificity. One well-established technique is transient absorption spectroscopy, where transient sample absorption is determined by scanning the central photon energy and recording the resultant photoproducts. When using sub-femtosecond pulses, this method is limited in spectral resolution due to the large energy bandwidth inherent to the short pulses. Here, we present a novel technique based on the principle of ghost imaging, and demonstrate sub-bandwidth absorption spectroscopy measurements with sub-femtosecond pulses. We show both one-dimensional and two-dimensional results. Our method is applicable to any spectral measurement limited by the bandwidth or noise level of the probing source, provided the probe spectrum is known at each shot.

*This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. Use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515.

Authors

  • Siqi Li

    • SLAC National Accelerator Laboratory
    • SLAC Natl. Accelerator Lab.
  • Joseph Duris

    • SLAC National Accelerator Laboratory
  • Thomas J. Lane

    • SLAC National Accelerator Laboratory
  • Agostino Marinelli

    • SLAC National Accelerator Laboratory
    • SLAC - Natl Accelerator Lab
    • SLAC Natl. Accelerator Lab.
  • Daniel Ratner

    • SLAC National Accelerator Laboratory
  • Elio G. Champenois

    • SLAC National Accelerator Laboratory
    • Stanford PULSE Institute, SLAC National Accelerator Laboratory
    • Stanford PULSE Institute/LCLS
  • James Cryan

    • SLAC National Accelerator Laboratory
    • Stanford PULSE Institute, SLAC National Accelerator Laboratory
    • Stanford PULSE Institute/LCLS
  • Taran Driver

    • SLAC National Accelerator Laboratory
  • Oliver Alexander

    • Imperial College London
  • Thomas Barillot

    • Imperial College London
  • Douglas Garratt

    • Imperial College London
  • Jon Marangos

    • Imperial College London