Abstract
The generation of electronic ring currents in ring-shaped molecules by photoexcitation with circularly polarized laser light is considered in the presence of vibronic coupling effects. Jahn-Teller distortions, unavoidable by symmetry in the subset of electronic states supporting the ring current, mix the clockwise and anticlockwise circulation directions of the electrons and can suppress the maximum achievable current by at least one order of magnitude, already for moderate vibronic coupling strengths, as compared to the Born-Oppenheimer limit of fixed atomic positions. The circulation direction of the electrons is found to depend on the spectral region of the Hamiltonian. This fact results in the surprising effect that the same polarization direction of the laser pulse can trigger either clockwise or anticlockwise electronic dynamics depending on the wavelength of the photons. These findings are illustrated in a model of the triazine molecule.
- Received 26 May 2021
- Accepted 9 September 2021
- Corrected 12 November 2021
DOI:https://doi.org/10.1103/PhysRevResearch.3.L042003
Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.
Published by the American Physical Society
Physics Subject Headings (PhySH)
Corrections
12 November 2021
Correction: A minor error in the caption to Figure 2 has been fixed. The acronym LCPs has been changed to RCPs.