Year: 2022
Type: article
Abstract: Inner-shell photoelectron spectroscopy provides an element-specific probe of molecular structure, as core-electron binding energies are sensitive to the chemical environment. Short-wavelength femtosecond light sources, such as Free-Electron Lasers (FELs), even enable time-resolved site-specific investigations of molecular photochemistry. Here, we study the ultraviolet photodissociation of the prototypical chiral molecule 1-iodo-2-methylbutane, probed by extreme-ultraviolet (XUV) pulses from the Free-electron LASer in Hamburg (FLASH) through the ultrafast evolution of the iodine 4d binding energy. Methodologically, we employ electron-ion partial covariance imaging as a technique to isolate otherwise elusive features in a two-dimensional photoelectron spectrum arising from different photofragmentation pathways. The experimental and theoretical results for the time-resolved electron spectra of the 4d3/2 and 4d5/2 atomic and molecular levels that are disentangled by this method provide a key step towards studying structural and chemical changes from a specific spectator site.
Source: Communications Chemistry
Authors: Felix Allum, Valerija Music, Ludger Inhester, Rebecca Boll, Benjamin Erk, Philipp Schmidt, Thomas M. Baumann, Günter Brenner, Michael Burt, Philipp V. Demekhin, Simon Dörner, Arno Ehresmann, Andreas Galler, Patrik Grychtol, David Heathcote, Denis Kargin, Mats Larsson, Jason W. L. Lee, Zheng Li, Bastian Manschwetus, Lutz Marder, Robert Mason, Michael Meyer, Huda Otto, Christopher Passow, Rudolf Pietschnig, Daniel Ramm, Kaja Schubert, Lucas Schwob, Richard D. Thomas, Claire Vallance, Igor Vidanović, Clemens von Korff Schmising, René Wagner, Peter Walter, Vitali Zhaunerchyk, Daniel Rolles, Sadia Bari, Mark Brouard, Markus Ilchen
Institutions: SLAC National Accelerator Laboratory, University of Oxford, University of Kassel, Deutsches Elektronen-Synchrotron DESY, European X-Ray Free-Electron Laser, Center for Free-Electron Laser Science, Stockholm University, AlbaNova, Peking University, Max-Born-Institute for Nonlinear Optics and Short Pulse Spectroscopy, University of Gothenburg, Kansas State University
Language: English
Subfield: Atomic and Molecular Physics, and Optics
Field: Physics and Astronomy
Domain: Physical Sciences
Open Access status: gold
Estimated APC paid: $2,990
Awards: G1077140421, G1317775495, G1434330249, SFB 1319: Extremes Licht zur Analyse und Kontrolle molekularer Chiralität (ELCH), G1797787269, Chemical Applications of Velocity and Spatial Imaging, G2684235734, G2759646434, G2978581158, G304333627, G3530777102, G3618824129, G3654309164, G392462602, G4336652674, Verbundprojekt: FSP 301 - FLASH: Nanoskopische Systeme. Teilprojekt 1.1: Universelle Experimentierkammer für Streuexperimente mit kohärenten Femtosekunden-Röntgenpulsen Multi Purpose Coherent Scattering Chamber for FLASH and XFEL 'MPscatt'., Verbundprojekt FSP 302 - Freie-Elektronen-Laser: Nanoskopische Systeme. Teilprojekt 4: Dynamik einzelner Nanoteilchen in Femtosekunden-Zeitlupe - Filmen mit ultrakurzen Röntgen-Doppelpulsen., G5103974534, G5368910837, Imaging Chemical Dynamics with Ultrafast Laser Spectroscopy, G6033966476, G631307236, G7501684951, Verbundprojekt: FSP 301 - FLASH: Nanoskopische Systeme. Teilprojekt 1.2: Universelle Experimentierkammer für Streuexperimente mit kohärenten Femtosekunden-Röntgenpulsen Multi Purpose Coherent Scattering Chamber for FLASH and XFEL 'MPscatt'., CAREER: Investigating Ultrafast Electronic and Structural Dynamics During Light-Driven Chemical Reactions, G786475436, New Directions in Molecular Scattering: Multiple Pathways and Products, G8395316192, Verbundprojekt 05K2016 - Nanoteilchenstruktur: Hochaufgelöste Struktur und Dynamik einzelner Nanoteilchen. Teilprojekt 1.
OpenAlex ID: W4221054852