Electronic and Vibrational Coherence in the Core Light-Harvesting Antenna of Rhodopseudomonas viridis
Abstract
In this paper we explain the wavelength-dependent oscillatory features in the pump−probe kinetics of the core LH1 antenna of Rhodopseudomonas viridis (Monshouwer, R.; Baltuška, A.; van Mourik, F.; van Grondelle, R. J. Phys. Chem. A 1998, 102, 4360). A quantitative fit of the data was obtained using the doorway−window representation of the nonlinear optical response in the vibrational eigenstate basis. In contrast to LH1/LH2 complexes from the BChl a- containing species, the LH1 antenna of Rps. viridis is characterized by a strong coupling of the excitonic states with two underdamped low-frequency modes (58 and 110 cm -1 at 77 K). Following a short femtosecond excitation pulse, this gives rise to the intense oscillations observed in the pump−probe traces, including their time and excitation/detection wavelength dependence. Furthermore, it leads to a pronounced and specific heterogeneity of the major absorption band due to the combined effects of the exciton splitting, disorder, and the presence of vibrational sidebands. The sharp maxima in the second derivative of the low-temperature absorption spectrum (Monshouwer, R.; Visschers, R. W.; van Mourik, F.; Freiberg, A.; van Grondelle, R. Biochim. Biophys. Acta 1995, 1229, 373) were assigned to the lowest exciton−vibrational transitions. The wavelength dependence of the experimentally observed oscillatory pattern suggests a different vibrational coherence decay for the ground- and excited-state wave packets. This can be explained by assuming the (incoherent) migration of the delocalized exciton (polaron) around the ringlike antenna with a characteristic time constant of 0.9−1.5 ps at 77K.
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With the advent of femtosecond transient absorption spectroscopy in the early 1990s, long-lived vibrational coherences, lasting on the order of a picosecond, were detected for bacterial and plant light-harvesting complexes.
“With the advent of femtosecond transient absorption spectroscopy in the early 1990s, long-lived vibrational coherences, lasting on the order of a picosecond, were detected for bacterial and plant light-harvesting complexes [35 -40].”
From The future of quantum biology (2018) · cites this paper as [39]
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- Authors
- Novoderezhkin, V., Monshouwer, R., & van Grondelle, R.
- Affiliations
- Lomonosov Moscow State University (RU)
- A. N. Belozersky Institute of Physico-Chemical Biology, Moscow State University, Moscow 119899, Russia, and Department of Biophysics, Faculty of Sciences, Vrije Universiteit, De Boelelaan 1081, 1081 HV Amsterdam, The Netherlands
- Venue
- The Journal of Physical Chemistry B
- Publisher
- American Chemical Society (ACS)
- Published
- 2000-11-29
- Volume
- 104
- Issue
- 50
- Pages
- 12056-12071
- ISSN
- 1520-5207 (ISSN-L)
- 1520-6106
- OpenAlex
- W2083898274
- Cited by
- 34
- References
- 84
- Citations by year
- 2026: 1 · 2025: 2 · 2024: 1 · 2022: 1 · 2020: 1 · 2018: 1 · 2017: 1 · 2016: 2 · 2014: 1 · 2013: 1 · 2012: 1
- FWCI
- 1.89
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- The Journal of Physical Chemistry B (publishedVersion)
- VU Research Portal (publishedVersion)
- Digital Academic REpository of VU University Amsterdam (Vrije Universiteit Amsterdam) (submittedVersion)
- Data Archiving and Networked Services (DANS) (submittedVersion)
- Topics
- 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
- Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › Photosynthetic Processes and Mechanisms
- Keywords
- Rhodopseudomonas viridis, light-harvesting complexes, pump-probe spectroscopy, vibrational coherence, exciton migration, exciton splitting, vibrational sidebands, low-frequency vibrational modes, polarons
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