Observation of molecular resonant double-core excitation driven by intense X-ray pulses
Abstract The ultrashort and intense pulses of X-rays produced at X-ray free electron lasers (XFELs) have enabled unique experiments on the atomic level structure and dynamics of matter, with time-resolved studies permitted in the femto- and attosecond regimes. To fully exploit them, it is paramount to obtain a comprehensive understanding of the complex nonlinear interactions that can occur at such extreme X-ray intensities. Herein, we report on the experimental observation of a resonant double-core excitation scheme in N 2 , where two 1 σ core-level electrons are resonantly promoted to unoccupied $$1{\pi }_{g}^{* }$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mn>1</mml:mn> <mml:msubsup> <mml:mrow> <mml:mi>π</mml:mi> </mml:mrow> <mml:mrow> <mml:mi>g</mml:mi> </mml:mrow> <mml:mrow> <mml:mo>*</mml:mo> </mml:mrow> </mml:msubsup> </mml:math> molecular orbitals by a single few-femtosecond broad-bandwidth XFEL pulse. The production of these neutral two-site double core hole states is evidenced through their characteristic decay channels, which are observed in good agreement with high-level theoretical calculations. Such multi-core excitation schemes, benefiting from the high interaction cross sections and state- and site-selective nature of resonant X-ray interactions, should be generally accessible in XFEL irradiated molecules, and provide interesting opportunities for chemical analysis and for monitoring ultrafast dynamic processes.
Authors
- Sergey I. Bokarev (ORCID: https://orcid.org/0000-0003-0779-5013)
- Dimitris Koulentianos (ORCID: https://orcid.org/0000-0002-5499-4659)
- Adam E. A. Fouda (ORCID: https://orcid.org/0000-0002-9445-5537)
- R. Püttner (ORCID: https://orcid.org/0000-0002-8761-6873)
- M. Simon (ORCID: https://orcid.org/0000-0002-2525-5435)
- Gilles Doumy (ORCID: https://orcid.org/0000-0001-8672-4138)
- Linda Young (ORCID: https://orcid.org/0000-0002-2251-039X)
- Gilbert Grell (ORCID: https://orcid.org/0000-0001-6103-5846)
- Iyas Ismail (ORCID: https://orcid.org/0000-0003-2007-6419)
- Björn Senfftleben (ORCID: https://orcid.org/0000-0003-1716-5445)
- Eetu Pelimanni (ORCID: https://orcid.org/0000-0002-4550-6430)
- Th. Baumann (ORCID: https://orcid.org/0009-0004-9612-221X)
- A. De Fanis (ORCID: https://orcid.org/0000-0002-4967-903X)
- Simon Dold (ORCID: https://orcid.org/0000-0001-5332-8251)
- Phay J. Ho (ORCID: https://orcid.org/0000-0001-5214-2180)
- Daniel E. Rivas (ORCID: https://orcid.org/0000-0002-7540-4902)
- Michael Meyer (ORCID: https://orcid.org/0000-0002-1444-6770)
- Tommaso Mazza (ORCID: https://orcid.org/0000-0003-3105-459X)
- MariaNovella Piancastelli
Institutions
- Madrid Institute for Advanced Studies (ES)
- Argonne National Laboratory (US)
- Centre National de la Recherche Scientifique (FR)
- Universität Hamburg (DE)
- Deutsches Elektronen-Synchrotron DESY (DE)
- Sorbonne Université (FR)
- University of Chicago (US)
- Laboratoire de Chimie Physique - Matière et Rayonnement (FR)
- Center for Free-Electron Laser Science (DE)
- University of Rostock (DE)
- Technical University of Munich (DE)
- Freie Universität Berlin (DE)
- European X-Ray Free-Electron Laser (DE)
Publication Details
- Journal
- Communications Physics
- Published
- 2024-10-17
- DOI
- https://doi.org/10.1038/s42005-024-01804-5
- Citations
- 5
- Primary Topic
- Atomic and Molecular Physics
- Type
- article
- Field-Weighted Citation Impact
- 1.69
Funders
- U.S. Department of Energy
- Deutsche Forschungsgemeinschaft
- Office of Science
- Basic Energy Sciences
- Chemical Sciences, Geosciences, and Biosciences Division