Excitation transfer and trapping kinetics in plant photosystem I probed by two-dimensional electronic spectroscopy
Photosystem I is a robust and highly efficient biological solar engine. Its capacity to utilize virtually every absorbed photon’s energy in a photochemical reaction generates great interest in the kinetics and mechanisms of excitation energy transfer and charge separation. In this work, we have empl...
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| Format: | Journal Article |
| Language: | English |
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2018
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| Online Access: | https://hdl.handle.net/10356/89330 http://hdl.handle.net/10220/44856 |
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| author | Akhtar, Parveen Zhang, Cheng Liu, Zhengtang Tan, Howe-Siang Lambrev, Petar H. |
| author2 | School of Physical and Mathematical Sciences |
| author_facet | School of Physical and Mathematical Sciences Akhtar, Parveen Zhang, Cheng Liu, Zhengtang Tan, Howe-Siang Lambrev, Petar H. |
| author_sort | Akhtar, Parveen |
| collection | NTU |
| description | Photosystem I is a robust and highly efficient biological solar engine. Its capacity to utilize virtually every absorbed photon’s energy in a photochemical reaction generates great interest in the kinetics and mechanisms of excitation energy transfer and charge separation. In this work, we have employed room-temperature coherent two-dimensional electronic spectroscopy and time-resolved fluorescence spectroscopy to follow exciton equilibration and excitation trapping in intact Photosystem I complexes as well as core complexes isolated from Pisum sativum. We performed two-dimensional electronic spectroscopy measurements with low excitation pulse energies to record excited-state kinetics free from singlet–singlet annihilation. Global lifetime analysis resolved energy transfer and trapping lifetimes closely matches the time-correlated single-photon counting data. Exciton energy equilibration in the core antenna occurred on a timescale of 0.5 ps. We further observed spectral equilibration component in the core complex with a 3–4 ps lifetime between the bulk Chl states and a state absorbing at 700 nm. Trapping in the core complex occurred with a 20 ps lifetime, which in the supercomplex split into two lifetimes, 16 ps and 67–75 ps. The experimental data could be modelled with two alternative models resulting in equally good fits—a transfer-to-trap-limited model and a trap-limited model. However, the former model is only possible if the 3–4 ps component is ascribed to equilibration with a “red” core antenna pool absorbing at 700 nm. Conversely, if these low-energy states are identified with the P700 reaction centre, the transfer-to-trap-model is ruled out in favour of a trap-limited model. |
| first_indexed | 2024-10-01T06:21:22Z |
| format | Journal Article |
| id | ntu-10356/89330 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T06:21:22Z |
| publishDate | 2018 |
| record_format | dspace |
| spelling | ntu-10356/893302023-02-28T19:36:06Z Excitation transfer and trapping kinetics in plant photosystem I probed by two-dimensional electronic spectroscopy Akhtar, Parveen Zhang, Cheng Liu, Zhengtang Tan, Howe-Siang Lambrev, Petar H. School of Physical and Mathematical Sciences Excitation Energy Transfer Light Harvesting Photosystem I is a robust and highly efficient biological solar engine. Its capacity to utilize virtually every absorbed photon’s energy in a photochemical reaction generates great interest in the kinetics and mechanisms of excitation energy transfer and charge separation. In this work, we have employed room-temperature coherent two-dimensional electronic spectroscopy and time-resolved fluorescence spectroscopy to follow exciton equilibration and excitation trapping in intact Photosystem I complexes as well as core complexes isolated from Pisum sativum. We performed two-dimensional electronic spectroscopy measurements with low excitation pulse energies to record excited-state kinetics free from singlet–singlet annihilation. Global lifetime analysis resolved energy transfer and trapping lifetimes closely matches the time-correlated single-photon counting data. Exciton energy equilibration in the core antenna occurred on a timescale of 0.5 ps. We further observed spectral equilibration component in the core complex with a 3–4 ps lifetime between the bulk Chl states and a state absorbing at 700 nm. Trapping in the core complex occurred with a 20 ps lifetime, which in the supercomplex split into two lifetimes, 16 ps and 67–75 ps. The experimental data could be modelled with two alternative models resulting in equally good fits—a transfer-to-trap-limited model and a trap-limited model. However, the former model is only possible if the 3–4 ps component is ascribed to equilibration with a “red” core antenna pool absorbing at 700 nm. Conversely, if these low-energy states are identified with the P700 reaction centre, the transfer-to-trap-model is ruled out in favour of a trap-limited model. MOE (Min. of Education, S’pore) Accepted version 2018-05-22T03:57:28Z 2019-12-06T17:23:02Z 2018-05-22T03:57:28Z 2019-12-06T17:23:02Z 2017 Journal Article Akhtar, P., Zhang, C., Liu, Z., Tan, H.-S., & Lambrev, P. H. (2018). Excitation transfer and trapping kinetics in plant photosystem I probed by two-dimensional electronic spectroscopy. Photosynthesis Research, 135(1-3), 239-250. 0166-8595 https://hdl.handle.net/10356/89330 http://hdl.handle.net/10220/44856 10.1007/s11120-017-0427-2 en Photosynthesis Research © 2017 Springer Science+Business Media B.V. This is the author created version of a work that has been peer reviewed and accepted for publication by Photosynthesis Research, Springer Science+Business Media B.V. It incorporates referee’s comments but changes resulting from the publishing process, such as copyediting, structural formatting, may not be reflected in this document. The published version is available at: [http://dx.doi.org/10.1007/s11120-017-0427-2]. 20 p. application/pdf |
| spellingShingle | Excitation Energy Transfer Light Harvesting Akhtar, Parveen Zhang, Cheng Liu, Zhengtang Tan, Howe-Siang Lambrev, Petar H. Excitation transfer and trapping kinetics in plant photosystem I probed by two-dimensional electronic spectroscopy |
| title | Excitation transfer and trapping kinetics in plant photosystem I probed by two-dimensional electronic spectroscopy |
| title_full | Excitation transfer and trapping kinetics in plant photosystem I probed by two-dimensional electronic spectroscopy |
| title_fullStr | Excitation transfer and trapping kinetics in plant photosystem I probed by two-dimensional electronic spectroscopy |
| title_full_unstemmed | Excitation transfer and trapping kinetics in plant photosystem I probed by two-dimensional electronic spectroscopy |
| title_short | Excitation transfer and trapping kinetics in plant photosystem I probed by two-dimensional electronic spectroscopy |
| title_sort | excitation transfer and trapping kinetics in plant photosystem i probed by two dimensional electronic spectroscopy |
| topic | Excitation Energy Transfer Light Harvesting |
| url | https://hdl.handle.net/10356/89330 http://hdl.handle.net/10220/44856 |
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