An efficient time-domain implementation of the multichromophoric Förster resonant energy transfer method

The excitation energy transfer (EET) process for photosynthetic antenna complexes consisting of subunits, each comprised of multiple chromophores, remains challenging to describe. The multichromophoric Förster resonance energy transfer theory is a popular method to describe the EET process in such s...

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Main Authors: Zhong, Kai, Nguyen, Hoang Long, Do, Thanh Nhut, Tan, Howe-Siang, Knoester, Jasper, Jansen, Thomas L. C.
Other Authors: School of Chemistry, Chemical Engineering and Biotechnology
Format: Article
Language:English
Published: 2023
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Online Access:https://hdl.handle.net/10356/169368
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Institution: Nanyang Technological University
Language: English
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spelling sg-ntu-dr.10356-1693682023-07-21T15:31:50Z An efficient time-domain implementation of the multichromophoric Förster resonant energy transfer method Zhong, Kai Nguyen, Hoang Long Do, Thanh Nhut Tan, Howe-Siang Knoester, Jasper Jansen, Thomas L. C. School of Chemistry, Chemical Engineering and Biotechnology Engineering::Chemical engineering Antennas Energy Transfer The excitation energy transfer (EET) process for photosynthetic antenna complexes consisting of subunits, each comprised of multiple chromophores, remains challenging to describe. The multichromophoric Förster resonance energy transfer theory is a popular method to describe the EET process in such systems. This paper presents a new time-domain method for calculating energy transfer based on the combination of multichromophoric Förster resonance energy transfer theory and the Numerical Integration of the Schrödinger Equation method. After validating the method on simple model systems, we apply it to the Light-Harvesting antenna 2 (LH2) complex, a light harvesting antenna found in purple bacteria. We use a simple model combining the overdamped Brownian oscillators to describe the dynamic disorder originating from the environmental fluctuations and the transition charge from the electrostatic potential coupling model to determine the interactions between chromophores. We demonstrate that with this model, both the calculated spectra and the EET rates between the two rings within the LH2 complex agree well with experimental results. We further find that the transfer between the strongly coupled rings of neighboring LH2 complexes can also be well described with our method. We conclude that our new method accurately describes the EET rate for biologically relevant multichromophoric systems, which are similar to the LH2 complex. Computationally, the new method is very tractable, especially for slow processes. We foresee that the method can be applied to efficiently calculate transfer in artificial systems as well and may pave the way for calculating multidimensional spectra of extensive multichromophoric systems in the future. Ministry of Education (MOE) Published version H.-S.T. gratefully acknowledges the financial support from the Singapore Ministry of Education Tier 1 grant (MOE-RG14/20). 2023-07-17T02:31:10Z 2023-07-17T02:31:10Z 2023 Journal Article Zhong, K., Nguyen, H. L., Do, T. N., Tan, H., Knoester, J. & Jansen, T. L. C. (2023). An efficient time-domain implementation of the multichromophoric Förster resonant energy transfer method. Journal of Chemical Physics, 158(6), 064103-. https://dx.doi.org/10.1063/5.0136652 0021-9606 https://hdl.handle.net/10356/169368 10.1063/5.0136652 36792497 2-s2.0-85147967498 6 158 064103 en MOE-RG14/20 Journal of Chemical Physics © 2023 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/). https://doi.org/10.1063/5.0136652 application/pdf
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering::Chemical engineering
Antennas
Energy Transfer
spellingShingle Engineering::Chemical engineering
Antennas
Energy Transfer
Zhong, Kai
Nguyen, Hoang Long
Do, Thanh Nhut
Tan, Howe-Siang
Knoester, Jasper
Jansen, Thomas L. C.
An efficient time-domain implementation of the multichromophoric Förster resonant energy transfer method
description The excitation energy transfer (EET) process for photosynthetic antenna complexes consisting of subunits, each comprised of multiple chromophores, remains challenging to describe. The multichromophoric Förster resonance energy transfer theory is a popular method to describe the EET process in such systems. This paper presents a new time-domain method for calculating energy transfer based on the combination of multichromophoric Förster resonance energy transfer theory and the Numerical Integration of the Schrödinger Equation method. After validating the method on simple model systems, we apply it to the Light-Harvesting antenna 2 (LH2) complex, a light harvesting antenna found in purple bacteria. We use a simple model combining the overdamped Brownian oscillators to describe the dynamic disorder originating from the environmental fluctuations and the transition charge from the electrostatic potential coupling model to determine the interactions between chromophores. We demonstrate that with this model, both the calculated spectra and the EET rates between the two rings within the LH2 complex agree well with experimental results. We further find that the transfer between the strongly coupled rings of neighboring LH2 complexes can also be well described with our method. We conclude that our new method accurately describes the EET rate for biologically relevant multichromophoric systems, which are similar to the LH2 complex. Computationally, the new method is very tractable, especially for slow processes. We foresee that the method can be applied to efficiently calculate transfer in artificial systems as well and may pave the way for calculating multidimensional spectra of extensive multichromophoric systems in the future.
author2 School of Chemistry, Chemical Engineering and Biotechnology
author_facet School of Chemistry, Chemical Engineering and Biotechnology
Zhong, Kai
Nguyen, Hoang Long
Do, Thanh Nhut
Tan, Howe-Siang
Knoester, Jasper
Jansen, Thomas L. C.
format Article
author Zhong, Kai
Nguyen, Hoang Long
Do, Thanh Nhut
Tan, Howe-Siang
Knoester, Jasper
Jansen, Thomas L. C.
author_sort Zhong, Kai
title An efficient time-domain implementation of the multichromophoric Förster resonant energy transfer method
title_short An efficient time-domain implementation of the multichromophoric Förster resonant energy transfer method
title_full An efficient time-domain implementation of the multichromophoric Förster resonant energy transfer method
title_fullStr An efficient time-domain implementation of the multichromophoric Förster resonant energy transfer method
title_full_unstemmed An efficient time-domain implementation of the multichromophoric Förster resonant energy transfer method
title_sort efficient time-domain implementation of the multichromophoric förster resonant energy transfer method
publishDate 2023
url https://hdl.handle.net/10356/169368
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