Photosynthetic Energy Transfer: Missing in Action (Detected Spectroscopy)?

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  • Additional Information
    • Source:
      Publisher: American Chemical Society Country of Publication: United States NLM ID: 101526034 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1948-7185 (Electronic) Linking ISSN: 19487185 NLM ISO Abbreviation: J Phys Chem Lett Subsets: PubMed not MEDLINE; MEDLINE
    • Publication Information:
      Original Publication: Washington, D.C. : American Chemical Society
    • Abstract:
      In recent years, action-detected ultrafast spectroscopies have gained popularity offering distinct advantages over their coherently detected counterparts, such as spatially resolved and operando measurements with high sensitivity. However, there are also fundamental limitations connected to the process of signal generation in action-detected experiments. Here we perform fluorescence-detected two-dimensional electronic spectroscopy (F-2DES) of the light-harvesting II (LH2) complex from purple bacteria. We demonstrate that the B800-B850 energy transfer process in LH2 is weak but observable in F-2DES, unlike in coherently detected 2DES where the energy transfer is visible with 100% contrast. We explain the weak signatures using a disordered excitonic model that accounts for experimental conditions. We further derive a general formula for the presence of excited-state signals in multichromophoric aggregates, dependent on the aggregate geometry, size, excitonic coupling and disorder. We find that the prominence of excited-state dynamics in action-detected spectroscopy offers a unique probe of excitonic delocalization in multichromophoric systems.
    • Publication Date:
      Date Created: 20241209 Latest Revision: 20241219
    • Publication Date:
      20241219
    • Accession Number:
      10.1021/acs.jpclett.4c02665
    • Accession Number:
      39653033