Ultrafast Anisotropy Decay Reveals Structure and Energy Transfer in Supramolecular Aggregates

Vesna Eric, Jorge Luis Castro, Xinmeng Li, Lolita Dsouza, Sean K. Frehan, A. Huijser, Alfred R. Holzwarth, Francesco Buda, G.J. Agur Sevink, Huub J.M. de Groot, Thomas L.C. Jansen*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

2 Citations (Scopus)
2 Downloads (Pure)

Abstract

Chlorosomes from green bacteria perform the most efficient light capture and energy transfer, as observed among natural light-harvesting antennae. Hence, their unique functional properties inspire developments in artificial light-harvesting and molecular optoelectronics. We examine two distinct organizations of the molecular building blocks as proposed in the literature, demonstrating how these organizations alter light capture and energy transfer, which can serve as a mechanism that the bacteria utilize to adapt to changes in light conditions. Spectral simulations of polarization-resolved two-dimensional electronic spectra unravel how changes in the helicity of chlorosomal aggregates alter energy transfer. We show that ultrafast anisotropy decay presents a spectral signature that reveals contrasting energy pathways in different chlorosomes.
Original languageEnglish
Pages (from-to)7487-7496
Number of pages9
JournalACS Physical Chemistry Au
Volume127
Issue number34
DOIs
Publication statusPublished - 18 Aug 2023

Keywords

  • Energy transfer
  • Excitons
  • Magnetic properties
  • Phase transitions
  • Polarity

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