Site-specific Interrogation of an Ionic Chiral Fragment During Photolysis Using an X-ray Free-Electron Laser

Autor: Ilchen, Markus, Schmidt, Philipp, Novikovskiy, Nikolay M., Hartmann, Gregor, Rupprecht, Patrick, Coffee, Ryan N., Ehresmann, Arno, Galler, Andreas, Hartmann, Nick, Helml, Wolfram, Huang, Zhirong, Inhester, Ludger, Lutman, Alberto A., MacArthur, James P., Maxwell, Timothy, Meyer, Michael, Music, Valerija, Nuhn, Heinz-Dieter, Osipov, Timur, Ray, Dipanwita, Wolf, Thomas J. A., Bari, Sadia, Walter, Peter, Li, Zheng, Moeller, Stefan, Knie, Andr��, Demekhin, Philipp
Jazyk: angličtina
Rok vydání: 2020
Předmět:
Zdroj: Communications chemistry 4(1), 119 (2021). doi:10.1038/s42004-021-00555-6
Communications Chemistry, Vol 4, Iss 1, Pp 1-9 (2021)
Popis: Communications chemistry 4(1), 119 (2021). doi:10.1038/s42004-021-00555-6
Short-wavelength free-electron lasers with their ultrashort pulses at high intensities have originated new approaches for tracking molecular dynamics from the vista of specific sites. X-ray pump X-ray probe schemes even allow to address individual atomic constituents with a ���trigger���-event that preludes the subsequent molecular dynamics while being able to selectively probe the evolving structure with a time-delayed second X-ray pulse. Here, we use a linearly polarized X-ray photon to trigger the photolysis of a prototypical chiral molecule, namely trifluoromethyloxirane (C$_3$H$_3$F$_3$O), at the fluorine K-edge at around 700 eV. The created fluorine-containing fragments are then probed by a second, circularly polarized X-ray pulse of higher photon energy in order to investigate the chemically shifted inner-shell electrons of the ionic mother-fragment for their stereochemical sensitivity. We experimentally demonstrate and theoretically support how two-color X-ray pump X-ray probe experiments with polarization control enable XFELs as tools for chiral recognition.
Published by Macmillan Publishers Limited, part of Springer Nature, [London]
Databáze: OpenAIRE