Single-photon absorption and emission from a natural photosynthetic complex

Journal Article · Wed Jun 14 00:00:00 EDT 2023 · Nature (London)

DOI:https://doi.org/10.1038/s41586-023-06121-5· OSTI ID:2229287

Li, Quanwei ^[1]; Orcutt, Kaydren ^[2]; Cook, Robert L. ^[1]; Sabines-Chesterking, Javier ^[3]; Tong, Ashley L. ^[4]; Schlau-Cohen, Gabriela S. ^[4]; Zhang, Xiang ^[1]; Fleming, Graham R. ^[2]; Whaley, K. Birgitta ^[1]

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1. University of California, Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)
2. University of California, Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
3. National Institute of Standards and Technology (NIST) and University of Maryland, Gaithersburg, MD. Joint Quantum Institute
4. Massachusetts Institute of Technology (MIT), Cambridge, MA (United States)

Photosynthesis is generally assumed to be initiated by a single photon from the Sun, which, as a weak light source, delivers at most a few tens of photons per nanometre squared per second within a chlorophyll absorption band1. Yet much experimental and theoretical work over the past 40 years has explored the events during photosynthesis subsequent to absorption of light from intense, ultrashort laser pulses. Here, we use single photons to excite under ambient conditions the light-harvesting 2 (LH2) complex of the purple bacterium Rhodobacter sphaeroides, comprising B800 and B850 rings that contain 9 and 18 bacteriochlorophyll molecules, respectively. Excitation of the B800 ring leads to electronic energy transfer to the B850 ring in approximately 0.7 ps, followed by rapid B850-to-B850 energy transfer on an approximately 100-fs timescale and light emission at 850–875 nm. Using a heralded single photon source20,21 along with coincidence counting, we establish time correlation functions for B800 excitation and B850 fluorescence emission and demonstrate that both events involve single photons. We also find that the probability distribution of the number of heralds per detected fluorescence photon supports the view that a single photon can upon absorption drive the subsequent energy transfer and fluorescence emission and hence, by extension, the primary charge separation of photosynthesis. An analytical stochastic model and a Monte Carlo numerical model capture the data, further confirming that absorption of single photons is correlated with emission of single photons in a natural light-harvesting complex.

• 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; SC0018097; SC0019728
• OSTI ID: 2229287
• Journal Information: Nature (London), Journal Name: Nature (London) Journal Issue: 7969 Vol. 619; ISSN 0028-0836
• Publisher: Nature Publishing Group
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Atomic and molecular physics
Biophysics
Energy harvesting
Physical chemistry