Theoretical Description of Attosecond X-ray Absorption Spectroscopy of Frenkel Exciton Dynamics

Molecules. 2023 Jun 1;28(11):4502. doi: 10.3390/molecules28114502.

Abstract

Frenkel excitons are responsible for the transport of light energy in many molecular systems. Coherent electron dynamics govern the initial stage of Frenkel-exciton transfer. Capability to follow coherent exciton dynamics in real time will help to reveal their actual contribution to the efficiency of light-harvesting. Attosecond X-ray pulses are the tool with the necessary temporal resolution to resolve pure electronic processes with atomic sensitivity. We describe how attosecond X-ray pulses can probe coherent electronic processes during Frenkel-exciton transport in molecular aggregates. We analyze time-resolved absorption cross section taking broad spectral bandwidth of an attosecond pulse into account. We demonstrate that attosecond X-ray absorption spectra can reveal delocalization degree of coherent exciton transfer dynamics.

Keywords: Frenkel excitons; X-ray absorption spectroscopy; attosecond spectroscopy; coherent electron dynamics; energy transfer.

MeSH terms

  • X-Ray Absorption Spectroscopy*
  • X-Rays