The development and applications of multidimensional biomolecular spectroscopy illustrated by photosynthetic light harvesting

Fleming, Graham R.; Scholes, Gregory D.

doi:10.1017/s003358352400009x

Title: The development and applications of multidimensional biomolecular spectroscopy illustrated by photosynthetic light harvesting

Journal Article · 21 October 2024 · Quarterly Reviews of Biophysics

DOI: https://doi.org/10.1017/s003358352400009x · OSTI ID:2477941

^[1]; Scholes, Gregory D. ^[2]

Kavli Energy NanoScience Institute, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Princeton Univ., NJ (United States)

The parallel and synergistic developments of atomic resolution structural information, new spectroscopic methods, their underpinning formalism, and the application of sophisticated theoretical methods have led to a step function change in our understanding of photosynthetic light harvesting, the process by which photosynthetic organisms collect solar energy and supply it to their reaction centers to initiate the chemistry of photosynthesis. The new spectroscopic methods, in particular multidimensional spectroscopies, have enabled a transition from recording rates of processes to focusing on mechanism. We discuss two ultrafast spectroscopies – two-dimensional electronic spectroscopy and two-dimensional electronic-vibrational spectroscopy – and illustrate their development through the lens of photosynthetic light harvesting. Both spectroscopies provide enhanced spectral resolution and, in different ways, reveal pathways of energy flow and coherent oscillations which relate to the quantum mechanical mixing of, for example, electronic excitations (excitons) and nuclear motions. The new types of information present in these spectra provoked the application of sophisticated quantum dynamical theories to describe the temporal evolution of the spectra and provide new questions for experimental investigation. While multidimensional spectroscopies have applications in many other areas of science, we feel that the investigation of photosynthetic light harvesting has had the largest influence on the development of spectroscopic and theoretical methods for the study of quantum dynamics in biology, hence the focus of this review. We conclude with key questions for the next decade of this review.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)

Grant/Contract Number:: AC02-05CH11231; SC0015429

OSTI ID:: 2477941

Journal Information:: Quarterly Reviews of Biophysics, Journal Name: Quarterly Reviews of Biophysics Vol. 57; ISSN 0033-5835

Publisher:: Cambridge University PressCopyright Statement

Country of Publication:: United States

Language:: English

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