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Ultrafast excited-state dynamics in land plants Photosystem I core and whole supercomplex under oxidised electron donor conditions

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Abstract

The kinetics of excited-state energy migration were investigated by femtosecond transient absorption in the isolated Photosystem I-Light-Harvesting Complex I (PSI-LHCI) supercomplex and in the isolated PSI core complex of spinach under conditions in which the terminal electron donor P700 is chemically pre-oxidised. It is shown that, under these conditions, the relaxation of the excited state is characterised by lifetimes of about 0.4 ps, 4.5 ps, 15 ps, 35 ps and 65 ps in PSI-LHCI and 0.15 ps, 0.3 ps, 6 ps and 16 ps in the PSI core complex. Compartmental spectral-kinetic modelling indicates that the most likely mechanism to explain the absence of long-lived (ns) excited states is the photochemical population of a radical pair state, which cannot be further stabilised and decays non-radiatively to the ground state with time constants in the order of 6–8 ps.

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Abbreviations

PSI:

Photosystem I

PSII:

Photosystem II

LHCI:

Light-Harvesting Complex I

RC:

Reaction centre

ET:

Electron transfer

EET:

Excitation energy transfer

TA:

Transient absorption

DADS:

Decay-associated differential absorption spectrum

SADS:

Species-associated differential absorption spectrum

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Acknowledgements

SS and APC acknowledge the support for this research from Fondazione Cariplo (CYAO Project), Grant Number 2016–0667, and thank Dr. A. Petrova for the assistance in biochemical sample preparation. GC acknowledges the support from the PRIN 2017 Project 201795SBA3 – HARVEST. VP, GC and MM acknowledge financial support from the Marie Sklodowska-Curie project 812992 – MUSIQ.

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Correspondence to Margherita Maiuri or Stefano Santabarbara.

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Russo, M., Petropoulos, V., Molotokaite, E. et al. Ultrafast excited-state dynamics in land plants Photosystem I core and whole supercomplex under oxidised electron donor conditions. Photosynth Res 144, 221–233 (2020). https://doi.org/10.1007/s11120-020-00717-y

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