ArticleProceedings of the National Academy of Sciences of the United States of America2016
Ultrafast energy relaxation in single light-harvesting complexes.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2016. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 12 papers.
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Who cites it
12 citing papers in PubMed.
- Solution-phase sample-averaged single-particle spectroscopy of quantum emitters with femtosecond resolution.Nature materials · 2024Article
- Coarse-Grained Approach to Simulate Signatures of Excitation Energy Transfer in Two-Dimensional Electronic Spectroscopy of Large Molecular Systems.Journal of chemical theory and computation · 2024Article
- Real-Time Feedback-Driven Single-Particle Tracking: A Survey and Perspective.Small (Weinheim an der Bergstrasse, Germany) · 2022Review
- Facing the fluctuations.Nature chemistry · 2022Article
- Observation of robust energy transfer in the photosynthetic protein allophycocyanin using single-molecule pump-probe spectroscopy.Nature chemistry · 2022Article
- Spectrally-tunable femtosecond single-molecule pump-probe spectroscopy.Optics express · 2021Article
- Fluorescence-Detected Pump-Probe Spectroscopy.Angewandte Chemie (International ed. in English) · 2021Article
- Quantum dissipation driven by electron transfer within a single molecule investigated with atomic force microscopy.Nature communications · 2020Article
- The future of quantum biology.Journal of the Royal Society, Interface · 2018Review
- The contributions of 49ers to the measurements and models of ultrafast photosynthetic energy transfer.Photosynthesis research · 2018Article
- Robust light harvesting by a noisy antenna.Physical chemistry chemical physics : PCCP · 2018Article
- Single Molecule Spectroscopy of Monomeric LHCII: Experiment and Theory.Scientific reports · 2016Article
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5 authors.
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Abstract
Energy relaxation in light-harvesting complexes has been extensively studied by various ultrafast spectroscopic techniques, the fastest processes being in the sub-100-fs range. At the same time, much slower dynamics have been observed in individual complexes by single-molecule fluorescence spectroscopy (SMS). In this work, we use a pump-probe-type SMS technique to observe the ultrafast energy relaxation in single light-harvesting complexes LH2 of purple bacteria. After excitation at 800 nm, the measured relaxation time distribution of multiple complexes has a peak at 95 fs and is asymmetric, with a tail at slower relaxation times. When tuning the excitation wavelength, the distribution changes in both its shape and position. The observed behavior agrees with what is to be expected from the LH2 excited states structure. As we show by a Redfield theory calculation of the relaxation times, the distribution shape corresponds to the expected effect of Gaussian disorder of the pigment transition energies. By repeatedly measuring few individual complexes for minutes, we find that complexes sample the relaxation time distribution on a timescale of seconds. Furthermore, by comparing the distribution from a single long-lived complex with the whole ensemble, we demonstrate that, regarding the relaxation times, the ensemble can be considered ergodic. Our findings thus agree with the commonly used notion of an ensemble of identical LH2 complexes experiencing slow random fluctuations.
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