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Circular dichroism in the photoelectron angular distribution of achiral molecules

Christian S. Kern1,*, Xiaosheng Yang2,3,4, Giovanni Zamborlini1,5, Simone Mearini5, Matteo Jugovac5, Vitaliy Feyer5, Umberto De Giovannini6,7, Angel Rubio6,8, Serguei Soubatch2,3 et al.

Michael G. Ramsey1, F. Stefan Tautz2,3,4,†, and Peter Puschnig1,‡

  • *Contact author: christian.kern@uni-graz.at
  • †Contact author: s.tautz@fz-juelich.de
  • ‡Contact author: peter.puschnig@uni-graz.at
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Phys. Rev. Research 8, 023275 – Published 11 June, 2026

DOI: https://doi.org/10.1103/6bkb-4rm3

Abstract

Circular dichroism in the angular distribution (CDAD) is the effect that the angular intensity distribution of photoemitted electrons depends on the handedness of the incident circularly polarized light. The origin of CDAD can be manifold, including intrinsic properties of the system under study, such as chirality, spin-orbit interaction, or quantum-geometrical properties, but CDAD can also originate from final-state effects influenced by the experimental geometry. For example, CDAD has been reported for achiral organic molecules at the interface to metallic substrates. For this latter case, we investigate two prototypical π-conjugated molecules, namely, tetracene and pentacene, whose frontier orbitals have a similar shape but exhibit distinctly different symmetries. By comparing experimental CDAD momentum maps with simulations within time-dependent density functional theory, we show how the final state of the photoelectron must be regarded as the source of the CDAD in such otherwise achiral and quantum-geometrically trivial systems. We gain additional insight into the mechanism by employing a simple scattering model for the final state, which allows us to decompose the CDAD signal into partial wave contributions.

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Phys. Rev. Research 8, 023275– Published 11 June, 2026
  • Received 21 July 2025
  • Accepted 20 April 2026
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