A SINGLE PULSE PICOSECOND LASER STUDY OF EXCITON DYNAMICS IN CHLOROPLASTS
Abstract
Abstract. Using single picosecond laser pulses at 610 nm, the fluorescence yield (φ) of spinach chloroplasts as a function of intensity (I) (10 12‐10 16 photons/pulse/cm 2) was studied in the range of 21–300 K. The quantum yield decreases with increasing intensity and the φ vs I curves are identical at the emission maxima of 685 and 735 nm. This result is interpreted in terms of singlet exciton‐exciton annihilation on the level of the light‐harvesting pigments which occurs before energy is transferred to the Photosystem I pigments which emit at 735 nm. The yield φ is decreased by factors of 12 and 43 at 300 and 21 K, respectively. The shapes of the φ vs I curves are not well accounted for in terms of a model which is based on a Poisson distribution of photon hits in separate photosynthetic units, but can be satisfactorily described using a one‐parameter fit and an exciton‐exciton annihilation model. The bimolecular annihilation rate constant is found to be γ= (5–15) times 10‐9 cm 3 s‐1 and to exhibit only a minor temperature dependence. Lower bound values of the singlet exciton diffusion coefficient (≥ 10‐3 cm 2 s‐1), diffusion length (≥ 2 times 10‐6 cm) and Förster energy transfer rates (≥ 3 ≥ 10 10 s‐1) are estimated from γ using the appropriate theoretical relationships.
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The 2D tryptophan photoexcitation diffusion length of 6.64 nm is surprisingly high in microtubules given their structural roles and the chlorophyll a equivalent value of 20-80 nm.
“The two-dimensional tryptophan photoexcitation diffusion length of 6.64 nm is surprisingly high in microtubules, given that they are optimized to play structural roles in the cell and that the equivalent value for chlorophyll a, which is optimized for electronic energy transfer, is only 20–80 nm.”
From Electronic energy migration in microtubules (2023) · cites this paper as [25]
The 2D diffusion length in microtubules is comparable to that observed in some photosynthetic complexes and organic photovoltaic devices.
“Stern–Volmer analysis revealed that the 2D diffusion length of tryptophan photoexcitation in microtubules is comparable to that observed in some photosynthetic complexes23−25 and organic photovoltaic devices.45−47”
From Electronic energy migration in microtubules (2023) · cites this paper as [25]
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Electronic energy migration in microtubules
Kalra, A. P., Benny, A., Travis, S. M., Zizzi, E. A., Morales-Sanchez, A., Oblinsky, D. G., Craddock, T. J. A., Hameroff, S. R., MacIver, M. B., Tuszyński, J. A., et al. (2023) · ACS Central Science · doi:10.1021/acscentsci.2c01114 · Cited by 80 · see citing works
LASER PULSE EXCITATION STUDIES OF THE FLUORESCENCE OF CHLOROPLASTS
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- Authors
- Geacintov, N. E., Breton, J., Swenberg, C. E., & Paillotin, G.
- Affiliations
- New York University (US)
- CEA Paris-Saclay - Etablissement de Saclay (FR)
- Venue
- Photochemistry and Photobiology
- Publisher
- Wiley
- Published
- 1977-12
- Volume
- 26
- Issue
- 6
- Pages
- 629-638
- ISSN
- 0031-8655 (ISSN-L)
- 1751-1097
- OpenAlex
- W2049622161
- Cited by
- 65
- References
- 37
- Citations by year
- 2023: 1 · 2020: 1 · 2015: 1 · 2013: 1
- FWCI
- 3.14
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Photochemistry and Photobiology (publishedVersion)
- Topics
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › Photosynthetic Processes and Mechanisms
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
- Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
- Keywords
- exciton dynamics, chloroplasts, fluorescence yield, intensity dependence, photosystem I, light-harvesting pigments, exciton diffusion coefficient, fluorescence resonance energy transfer, temperature dependence, picosecond laser excitation, spinach
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