Coherent electron dynamics of core-excited molecules at an x-ray free-electron laser

ORAL

Abstract

A new generation of x-ray free-electron lasers (XFELs) offers the possibility to initiate and probe sub-femtosecond electron dynamics in molecules with atomic site specificity. We demonstrate the production of a core-excited electronic wavepacket using isolated attosecond soft x-ray pulses at the Linac Coherent Light Source. We time-resolve the subsequent Auger-Meitner decay process with sub-femtosecond resolution and observe that the evolution of the core-excited wavepacket maps to quantum interference in the emitted Auger-Meitner electron current. Sub-femtosecond precision is achieved by angular streaking and a novel self-referencing scheme. Control of the coherent electron dynamics is achieved by tuning the central photon energy of the exciting XFEL pulse. Mapping the time evolution of the core-excited state to the Auger-Meitner current offers a unique testbed for probing coherent electron dynamics in molecules on the attosecond timescale.

*This work is supported by the U.S. Department of Energy, Office of Science, Chemical Sciences, Geosciences, and Biosciences Division, Atomic, Molecular, and Optical Science Program. 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.

Presenters

  • Taran Driver

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

Authors

  • Taran Driver

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

    • SLAC National Lab
    • SLAC - Natl Accelerator Lab
    • SLAC NATIONAL ACCELERATOR LABORATORY
  • Elio G Champenois

    • SLAC National Accelerator Laboratory
    • Stanford PULSE Institute
    • SLAC National Accelerator Laboratory/Stanford University
  • Philipp Rosenberger

    • Ludwig-Maximilians-Universitaet (LMU-Munich)
  • Philip H Bucksbaum

    • Stanford Univ
    • Stanford PULSE Institute, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025, USA
    • Stanford Univ; Stanford PULSE Institute
  • Louis F DiMauro

    • Ohio State Univ - Columbus
  • Matthias F Kling

    • Ludwig-Maximilians-Universitaet (LMU-Munich)
  • Jonathan Marangos

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