Time-resolved pump-probe spectroscopy with spooktroscopy

POSTER

Abstract

Pump-probe spectroscopy with X-ray pulses provides us with the tool to generate atomic-level movies of ultrafast processes, such as chemical bonding and charge transfer, by varying the delay between the pump and the probe pulses. Spectral domain ghost imaging, or spooktroscopy, on the other hand exploits the intrinsic variation in the X-ray pulses and enables us to probe the spectral properties with superb resolution beyond the bandwidth limit. In this work, we demonstrate a clear separation of the pump signal from the probe signal even though they are tightly overlapped in energy. Furthermore, we also show a variation of the spooktroscopy reconstruction algorithm which applies regularization on the time domain, reconstructing a time-resolved pump-probe spectroscopy measurement.

*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. The authors acknowledge the invaluable support of the technical and scientific staff of the LCLS at SLAC National Accelerator Laboratory. JPM, OA, BC, TD, DG acknowledge funding from EPSRC through grants EP/I032517/1, EP/N018680/1 and EP/R019509/1, and ERC Advanced Grant ASTEX (2012-17). JPC was supported by the U.S. Department of Energy Office of Science, Basic Energy Science Division. We gratefully acknowledge the contribution of the LR25 beamtime collaboration to the development of the experiment, data taking and the initial analysis.

Presenters

  • Siqi Li

    • SLAC National Lab
    • SLAC - Natl Accelerator Lab
    • SLAC NATIONAL ACCELERATOR LABORATORY

Authors

  • Siqi Li

    • SLAC National Lab
    • SLAC - Natl Accelerator Lab
    • SLAC NATIONAL ACCELERATOR LABORATORY

  • Taran Driver

    • SLAC - Natl Accelerator Lab
    • Stanford PULSE Institute; LCLS, SLAC National Laboratory
    • SLAC - Natl Accelerator Lab/Stanford PULSE Institute

  • Oliver Alexander

    • Quantum Optics and Laser Science Group, Blackett Laboratory,Imperial College Lon-don, London, SW7 2BW, UK

  • Bridgette Cooper

    • Atomic, Molecular, Optical and Positron Physics Group, Department of Physics andAstronomy, University College London, Gower Street London, WC1E 6BT, UK

  • Douglas Garratt

    • Imperial College London

  • Agostino Marinelli

    • SLAC- National Accelerator Laboratory
    • SLAC National Accelerator Laboratory
    • SLAC - Natl Accelerator Lab
    • SLAC National Accelerator Laboratory/Stanford University

  • James P Cryan

    • SLAC - Natl Accelerator Lab
    • Stanford PULSE Institute; LCLS, SLAC National Laboratory
    • SLAC - Natl Accelerator Lab/Stanford PULSE Institute
    • SLAC National Lab

  • Jonathan Marangos

    • Imperial College London
    • Quantum Optics and Laser Science Group, Blackett Laboratory,Imperial College Lon-don, London, SW7 2BW, UK