Insights into the mechanisms and dynamics of energy transfer in plant light-harvesting complexes from two-dimensional electronic spectroscopy

During the past two decades, two-dimensional electronic spectroscopy (2DES) and related techniques have emerged as a potent experimental toolset to study the ultrafast elementary steps of photosynthesis. Apart from the highly engaging albeit controversial analysis of the role of quantum coherences in the photosynthetic processes, 2DES has been applied to resolve the dynamics and pathways of energy and electron transport in various light-harvesting antenna systems and reaction centres, providing unsurpassed level of detail. In this paper we discuss the main technical approaches and their applicability for solving specific problems in photosynthesis. We then recount applications of 2DES to study the exciton dynamics in plant and photosynthetic light-harvesting complexes, especially light-harvesting complex II (LHCII) and the fucoxanthin-chlorophyll proteins of diatoms, with emphasis on the types of unique information about such systems that 2DES is capable to deliver. This article is part of a Special Issue entitled Light harvesting, edited by Dr. Roberta Croce.