Directly Measuring the Connectivity between Isoenergetic Light-Harvesting Antennas in Plant Photosystem II at Physiological Temperature

The Journal of Physical Chemistry Letters, vol. 17, pp. 605–614

Abstract

The plant photosystem II (PSII) supercomplex features a relatively “flat” energy landscape in the excitonic energy transfer (EET) network between the light-harvesting antenna and core subunits. The resulting intersubunit EET proceeds predominantly between isoenergetic excitonic states. Visualizing these EET dynamics is difficult due to the heavy spectral overlaps between the components, particularly at physiological temperature. We employ polarization-resolved two-dimensional electronic spectroscopy to measure and compare the anisotropy kinetics between the LHCII-CP29-CP24 complex and some of its constituents. Using the orientational differences between the subunits, together with the EET time scales estimated from energy transfer theory and phenomenological kinetic modeling, we identify the contribution of intra- and intersubunit EET processes to the observed anisotropy decay components. The results suggest that EET rates between the antenna subunits are not homogeneous and can be sensitive to the interprotein arrangement. The approach provides an effective method for studying EET in large multichromophoric systems.

Authors 9

1. Hoàng Long Nguyễn

   Nanyang Technological University

   Affiliation as printed

   School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 21 Nanyang Link, 637371 Singapore

2. Kai Zhong

   University of Groningen · Nanyang Technological University · Zernike Institute for Advanced Materials

   Affiliation as printed

   School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 21 Nanyang Link, 637371 Singapore

   Zernike Institute for Advanced Materials, University of Groningen, Nijenborgh 3, 9747 AG Groningen, The Netherlands

3. Thanh Nhut

   Vrije Universiteit Amsterdam

   Affiliation as printed

   Department of Physics and Astronomy, Faculty of Science, Vrije Universiteit Amsterdam, De Boelelaan 1081, 1081 HZ Amsterdam, The Netherlands

4. Parveen Akhtar

   HUN-REN Szegedi Biológiai Kutatóközpont

   Affiliation as printed

   HUN-REN Biological Research Centre Szeged, Temesvári körút 62, Szeged 6726, Hungary

5. Petar H. Lambrev

   HUN-REN Szegedi Biológiai Kutatóközpont

   Affiliation as printed

   HUN-REN Biological Research Centre Szeged, Temesvári körút 62, Szeged 6726, Hungary

6. Thomas L. C. Jansen

   University of Groningen · Zernike Institute for Advanced Materials

   Affiliation as printed

   Zernike Institute for Advanced Materials, University of Groningen, Nijenborgh 3, 9747 AG Groningen, The Netherlands

7. Jasper Knoester Aachen Faculty of Science, Leiden University

   Leiden University · University of Groningen · Zernike Institute for Advanced Materials

   Affiliation as printed

   Faculty of Science, Leiden University, Einsteinweg 55, 2300 RA Leiden, The Netherlands

   Zernike Institute for Advanced Materials, University of Groningen, Nijenborgh 3, 9747 AG Groningen, The Netherlands

8. Stefano Caffarri

   Centre National de la Recherche Scientifique · Aix-Marseille Université · Commissariat à l'Énergie Atomique et aux Énergies Alternatives · Institut de Biosciences et Biotechnologies · Institut de Biosciences et biotechnologies d'Aix-Marseille

   Affiliation as printed

   Aix Marseille Université, CEA, CNRS, BIAM, LGBP

9. Howe‐Siang Tan corresponding

   Nanyang Technological University

   Affiliation as printed

   School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 21 Nanyang Link, 637371 Singapore