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2021-08-12Author
Ilchen, MarkusSchmidt, PhilippNovikovskiy, Nikolay M.Hartmann, GregorRupprecht, PatrickCoffee, Ryan N.Ehresmann, ArnoGaller, AndreasHartmann, NickHelml, WolframHuang, ZhirongInhester, LudgerLutman, Alberto A.MacArthur, James P.Maxwell, TimothyMeyer, MichaelMusic, ValerijaNuhn, Heinz-DieterOsipov, TimurRay, DipanwitaWolf, Thomas J. A.Bari, SadiaWalter, PeterLi, ZhengMoeller, StefanKnie, AndréDemekhin, Philipp V.Metadata
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Site-specific interrogation of an ionic chiral fragment during photolysis using an X-ray free-electron laser
Abstract
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 (C3H3F3O), 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.
Citation
In: Communications Chemistry Volume: 4 (2021-08-12) eissn: 2399-3669Sponsorship
Gefördert durch den Publikationsfonds der Universität KasselCitation
@article{doi:10.17170/kobra-202201215584,
author={Ilchen, Markus and Schmidt, Philipp and Novikovskiy, Nikolay M. and Hartmann, Gregor and Rupprecht, Patrick and Coffee, Ryan N. and Ehresmann, Arno and Galler, Andreas and Hartmann, Nick and Helml, Wolfram and Huang, Zhirong and Inhester, Ludger and Lutman, Alberto A. and MacArthur, James P. and Maxwell, Timothy and Meyer, Michael and Music, Valerija and Nuhn, Heinz-Dieter and Osipov, Timur and Ray, Dipanwita and Wolf, Thomas J. A. and Bari, Sadia and Walter, Peter and Li, Zheng and Moeller, Stefan and Knie, André and Demekhin, Philipp V.},
title={Site-specific interrogation of an ionic chiral fragment during photolysis using an X-ray free-electron laser},
journal={Communications Chemistry},
year={2021}
}
0500 Oax 0501 Text $btxt$2rdacontent 0502 Computermedien $bc$2rdacarrier 1100 2021$n2021 1500 1/eng 2050 ##0##http://hdl.handle.net/123456789/13603 3000 Ilchen, Markus 3010 Schmidt, Philipp 3010 Novikovskiy, Nikolay M. 3010 Hartmann, Gregor 3010 Rupprecht, Patrick 3010 Coffee, Ryan N. 3010 Ehresmann, Arno 3010 Galler, Andreas 3010 Hartmann, Nick 3010 Helml, Wolfram 3010 Huang, Zhirong 3010 Inhester, Ludger 3010 Lutman, Alberto A. 3010 MacArthur, James P. 3010 Maxwell, Timothy 3010 Meyer, Michael 3010 Music, Valerija 3010 Nuhn, Heinz-Dieter 3010 Osipov, Timur 3010 Ray, Dipanwita 3010 Wolf, Thomas J. A. 3010 Bari, Sadia 3010 Walter, Peter 3010 Li, Zheng 3010 Moeller, Stefan 3010 Knie, André 3010 Demekhin, Philipp V. 4000 Site-specific interrogation of an ionic chiral fragment during photolysis using an X-ray free-electron laser / Ilchen, Markus 4030 4060 Online-Ressource 4085 ##0##=u http://nbn-resolving.de/http://hdl.handle.net/123456789/13603=x R 4204 \$dAufsatz 4170 5550 {{Freies Elektron}} 5550 {{Röntgenlaser}} 5550 {{Fotolyse}} 7136 ##0##http://hdl.handle.net/123456789/13603
2022-02-04T08:57:58Z 2022-02-04T08:57:58Z 2021-08-12 doi:10.17170/kobra-202201215584 http://hdl.handle.net/123456789/13603 Gefördert durch den Publikationsfonds der Universität Kassel eng Namensnennung 4.0 International http://creativecommons.org/licenses/by/4.0/ 540 Site-specific interrogation of an ionic chiral fragment during photolysis using an X-ray free-electron laser Aufsatz 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 (C3H3F3O), 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. open access 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, André Demekhin, Philipp V. doi:10.1038/s42004-021-00555-6 Freies Elektron Röntgenlaser Fotolyse publishedVersion eissn: 2399-3669 Communications Chemistry Volume: 4 false Article number: 119
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