Excited State Assignment and State‐Resolved Photoelectron Circular Dichroism in Chalcogen‐Substituted Fenchones

Excited electronic states of fenchone, thiofenchone, and selenofenchone are characterized and assigned with different gas-phase spectroscopic methods and ab initio quantum chemical calculations. With an increasing atomic number of the chalcogen, increasing bathochromic (red) shifts are observed, which vary in strength for Rydberg states, valence-excited states, and ionization energies. The spectroscopic insight is used to state-resolve the contributions in multiphoton photoelectron circular dichroism with femtosecond laser pulses. This is shown to be a sensitive observable of molecular chirality in all studied chalcogenofenchones. This 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 near-ultraviolet spectral regions.

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Journal
ChemPhysChem
Published
2025-11-03
DOI
https://doi.org/10.1002/cphc.202500319
Primary Topic
Laser-Matter Interactions and Applications
Type
article
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article

Excited State Assignment and State‐Resolved Photoelectron Circular Dichroism in Chalcogen‐Substituted Fenchones

Tonio Rosen, Catmarna Küstner‐Wetekam, Arno Ehresmann, Denis Kargin et al.
ChemPhysChem
Laser-Matter Interactions and Applications
article

Excited State Assignment and State‐Resolved Photoelectron Circular Dichroism in Chalcogen‐Substituted Fenchones

Tonio Rosen, Catmarna Küstner‐Wetekam, Arno Ehresmann, Denis Kargin, Tim Schäfer, V. YA. POPKOVA, Thomas F. Giesen, Arne Senftleben, Lutz Marder, Nicolas Ladda, Hendrike Braun, Simon T. Ranecky, Rudolf Pietschnig, Igor Vidanović, Robert Berger, Sudheendran Vasudevan, Manjinder Kour, Steffen M. Giesen, Guido Fuchs, Andreas Hans, Thomas Baumert, Jochen Mikosch, Han‐gyeol Lee, Sagnik Das
article en

Abstract

Excited electronic states of fenchone, thiofenchone, and selenofenchone are characterized and assigned with different gas-phase spectroscopic methods and ab initio quantum chemical calculations. With an increasing atomic number of the chalcogen, increasing bathochromic (red) shifts are observed, which vary in strength for Rydberg states, valence-excited states, and ionization energies. The spectroscopic insight is used to state-resolve the contributions in multiphoton photoelectron circular dichroism with femtosecond laser pulses. This is shown to be a sensitive observable of molecular chirality in all studied chalcogenofenchones. This 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 near-ultraviolet spectral regions.

ChemPhysChemVol. 26(23)
University of Kassel (DE), Philipps University of Marburg (DE), University of Göttingen (DE)
Openalex Percentile: Top 74%
Laser-Matter Interactions and Applications
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