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Issue 28, 2016
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Mixing of exciton and charge-transfer states in light-harvesting complex Lhca4

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Abstract

Lhca4 is one of the peripheral antennae of higher plant photosystem I and it is characterized by the presence of chlorophyll a with absorption and emission bands around 30 nm red-shifted compared to those of the other chlorophylls associated with plant complexes. In this work we have investigated the origin of this red shift by using the recent structure of Lhca4 (Qin et al., Science, 2015, 348, 989) to build an exciton model that includes a charge-transfer (CT) state mixed with the excited-state manifold. A simultaneous quantitative fit of absorption, linear dichroism, fluorescence, and Stark absorption spectra of the wild-type Lhca4 and NH mutant (where the sites involved in CT are affected) enables us to determine the origin of the CT state and explore its spectral signatures. A huge borrowing of dipole strength by the CT, accompanied by anomalous broadening and red-shifting of the fluorescence as well as dramatic changes in the Stark spectrum, can be accounted for by a model implying an exciton-type mixing between excited states and CT states.

Graphical abstract: Mixing of exciton and charge-transfer states in light-harvesting complex Lhca4

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Publication details

The article was received on 05 Apr 2016, accepted on 22 Jun 2016 and first published on 23 Jun 2016


Article type: Paper
DOI: 10.1039/C6CP02225A
Citation: Phys. Chem. Chem. Phys., 2016,18, 19368-19377
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    Mixing of exciton and charge-transfer states in light-harvesting complex Lhca4

    V. I. Novoderezhkin, R. Croce, Md. Wahadoszamen, I. Polukhina, E. Romero and R. van Grondelle, Phys. Chem. Chem. Phys., 2016, 18, 19368
    DOI: 10.1039/C6CP02225A

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