title: Perspective: Detecting and measuring exciton delocalization in photosynthetic light harvesting.
abstract: Photosynthetic units perform energy transfer remarkably well under a diverse range of demanding conditions. However, the mechanism of energy transfer, from excitation to conversion, is still not fully understood. Of particular interest is the possible role that coherence plays in this process. In this perspective, we overview photosynthetic light harvesting and discuss consequences of excitons for energy transfer and how delocalization can be assessed. We focus on challenges such as decoherence and nuclear-coordinate dependent delocalization. These approaches complement conventional spectroscopy and delocalization measurement techniques. New broadband transient absorption data may help uncover the difference between electronic and vibrational coherences present in two-dimensional electronic spectroscopy data. We describe how multipartite entanglement from quantum information theory allows us to formulate measures that elucidate the delocalization length of excitation and the details of that delocalization even from highly averaged information such as the density matrix.
authors.affiliation: Department of Chemistry, University of Toronto, 80 St. George St., Toronto, Ontario M5S 3H6, Canada.
authors.forename: Gregory D
authors.initials: GD
authors.lastname: Scholes
authors.affiliation: Department of Chemistry, University of Toronto, 80 St. George St., Toronto, Ontario M5S 3H6, Canada.
authors.forename: Cathal
authors.initials: C
authors.lastname: Smyth
mesh_terms: D004583:Electrons; D004735:Energy Transfer; D008027:Light; D045342:Light-Harvesting Protein Complexes / Q000737:chemistry* / Q000378:metabolism; D008958:Models, Molecular; D011789:Quantum Theory; D014732:Vibration
chemical_list: D045342:Light-Harvesting Protein Complexes