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Auteurs principaux: Vasudevan, Sudheendran, Giesen, Steffen M., Ranecky, Simon T., Marder, Lutz, Vidanović, Igor, Kour, Manjinder, Küstner-Wetekam, Catmarna, Ladda, Nicolas, Das, Sagnik, Rosen, Tonio, Popkova, Vidana, Lee, Hangyeol, Kargin, Denis, Schäfer, Tim, Hans, Andreas, Baumert, Thomas, Berger, Robert, Braun, Hendrike, Ehresmann, Arno, Fuchs, Guido W., Giesen, Thomas F., Mikosch, Jochen, Pietschnig, Rudolf, Senftleben, Arne
Format: Preprint
Publié: 2025
Sujets:
Accès en ligne:https://arxiv.org/abs/2503.14261
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author Vasudevan, Sudheendran
Giesen, Steffen M.
Ranecky, Simon T.
Marder, Lutz
Vidanović, Igor
Kour, Manjinder
Küstner-Wetekam, Catmarna
Ladda, Nicolas
Das, Sagnik
Rosen, Tonio
Popkova, Vidana
Lee, Hangyeol
Kargin, Denis
Schäfer, Tim
Hans, Andreas
Baumert, Thomas
Berger, Robert
Braun, Hendrike
Ehresmann, Arno
Fuchs, Guido W.
Giesen, Thomas F.
Mikosch, Jochen
Pietschnig, Rudolf
Senftleben, Arne
author_facet Vasudevan, Sudheendran
Giesen, Steffen M.
Ranecky, Simon T.
Marder, Lutz
Vidanović, Igor
Kour, Manjinder
Küstner-Wetekam, Catmarna
Ladda, Nicolas
Das, Sagnik
Rosen, Tonio
Popkova, Vidana
Lee, Hangyeol
Kargin, Denis
Schäfer, Tim
Hans, Andreas
Baumert, Thomas
Berger, Robert
Braun, Hendrike
Ehresmann, Arno
Fuchs, Guido W.
Giesen, Thomas F.
Mikosch, Jochen
Pietschnig, Rudolf
Senftleben, Arne
contents Excited electronic states of fenchone, thiofenchone, and selenofenchone are characterized and assigned with different gas-phase spectroscopic methods and \textit{ab initio} quantum chemical calculations. With an increasing atomic number of the chalcogen, we observe increasing bathochromic (red) shifts, which vary in strength for Rydberg states, valence-excited states, and ionization energies. The spectroscopic insight is used to state-resolve the contributions in multi-photon photoelectron circular dichroism with femtosecond laser pulses. This is shown to be a sensitive observable of molecular chirality in all studied chalcogenofenchones. Our work contributes new spectroscopic information, particularly on thiofenchone and selenofenchone. It may open a perspective for future coherent control experiments exploiting resonances in the visible and or near-ultraviolet spectral regions.
format Preprint
id arxiv_https___arxiv_org_abs_2503_14261
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Excited state assignment and state-resolved photoelectron circular dichroism in chalcogen-substituted fenchones
Vasudevan, Sudheendran
Giesen, Steffen M.
Ranecky, Simon T.
Marder, Lutz
Vidanović, Igor
Kour, Manjinder
Küstner-Wetekam, Catmarna
Ladda, Nicolas
Das, Sagnik
Rosen, Tonio
Popkova, Vidana
Lee, Hangyeol
Kargin, Denis
Schäfer, Tim
Hans, Andreas
Baumert, Thomas
Berger, Robert
Braun, Hendrike
Ehresmann, Arno
Fuchs, Guido W.
Giesen, Thomas F.
Mikosch, Jochen
Pietschnig, Rudolf
Senftleben, Arne
Chemical Physics
Excited electronic states of fenchone, thiofenchone, and selenofenchone are characterized and assigned with different gas-phase spectroscopic methods and \textit{ab initio} quantum chemical calculations. With an increasing atomic number of the chalcogen, we observe increasing bathochromic (red) shifts, which vary in strength for Rydberg states, valence-excited states, and ionization energies. The spectroscopic insight is used to state-resolve the contributions in multi-photon photoelectron circular dichroism with femtosecond laser pulses. This is shown to be a sensitive observable of molecular chirality in all studied chalcogenofenchones. Our work contributes new spectroscopic information, particularly on thiofenchone and selenofenchone. It may open a perspective for future coherent control experiments exploiting resonances in the visible and or near-ultraviolet spectral regions.
title Excited state assignment and state-resolved photoelectron circular dichroism in chalcogen-substituted fenchones
topic Chemical Physics
url https://arxiv.org/abs/2503.14261