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Initial electron donor and acceptor in isolated Photosystem II reaction centers identified with femtosecond mid-IR spectroscopy.

ABSTRACT: Despite the apparent similarity between the plant Photosystem II reaction center (RC) and its purple bacterial counterpart, we show in this work that the mechanism of charge separation is very different for the two photosynthetic RCs. By using femtosecond visible-pump-mid-infrared probe spectroscopy in the region of the chlorophyll ester and keto modes, between 1,775 and 1,585 cm(-1), with 150-fs time resolution, we show that the reduction of pheophytin occurs on a 0.6- to 0.8-ps time scale, whereas P+, the precursor state for water oxidation, is formed after approximately 6 ps. We conclude therefore that in the Photosystem II RC the primary charge separation occurs between the "accessory chlorophyll" Chl(D1) and the pheophytin on the so-called active branch.

SUBMITTER: Groot ML

PROVIDER: S-EPMC1196200 | biostudies-literature | 2005 Sep

REPOSITORIES: biostudies-literature

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Initial electron donor and acceptor in isolated Photosystem II reaction centers identified with femtosecond mid-IR spectroscopy.

Groot Marie Louise ML Pawlowicz Natalia P NP van Wilderen Luuk J G W LJ Breton Jacques J van Stokkum Ivo H M IH van Grondelle Rienk R

Proceedings of the National Academy of Sciences of the United States of America 20050831 37

Despite the apparent similarity between the plant Photosystem II reaction center (RC) and its purple bacterial counterpart, we show in this work that the mechanism of charge separation is very different for the two photosynthetic RCs. By using femtosecond visible-pump-mid-infrared probe spectroscopy in the region of the chlorophyll ester and keto modes, between 1,775 and 1,585 cm(-1), with 150-fs time resolution, we show that the reduction of pheophytin occurs on a 0.6- to 0.8-ps time scale, whe ...[more]

PMID: 16135567

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Project description:One of the most effective approaches to optimizing the performance of perovskite solar cells is to fully understand the ultrafast carrier dynamics at the interfaces between absorber and transporting layers at both the molecular and atomic levels. Here, the injection dynamics of hot and relaxed charge carriers at the interface between the hybrid perovskite, formamidinium lead bromide (FAPbBr3), and the organic electron acceptor, IEICO-4F, are investigated and deciphered by using femtosecond (fs) mid-infrared (IR), transient absorption (TA), and fluorescence spectroscopies. The visible femtosecond-TA measurements reveal the generation of hot carriers and their transition to free carriers in the pure FAPbBr3 film. Meanwhile, the efficient extraction of hot carriers in the mixed FAPbBr3/IEICO-4F film is clearly evidenced by the complete disappearance of their spectral signature. More specifically, the time-resolved results reveal that hot carriers are injected from FAPbBr3 to IEICO-4F within 150 fs, while the transfer time for the relaxed carriers is about 205 fs. The time-resolved mid-IR experiments also demonstrate the ultrafast formation of two peaks at 2115 and 2233 cm-1, which can be attributed to the C≡N symmetrical and asymmetrical vibrational modes of anionic IEICO-4F, thus providing crystal clear evidence for the electron transfer process between the donor and acceptor units. Moreover, photoluminescence (PL) lifetime measurements reveal an approximately 10-fold decrease in the donor lifetime in the presence of IEICO-4F, thereby confirming the efficient electron injection from the perovskite to the acceptor unit. In addition, the efficient electron injection at the FAPbBr3/IEICO-4F interface and its impact on the C≡N bond character are experimentally evidenced and align with density functional theory (DFT) calculations. This work offers new insights into the electron injection process at the FAPbBr3/IEICO-4F interface, which is crucial for developing efficient optoelectronic devices.

Dataset Information

Initial electron donor and acceptor in isolated Photosystem II reaction centers identified with femtosecond mid-IR spectroscopy.

Publications

Initial electron donor and acceptor in isolated Photosystem II reaction centers identified with femtosecond mid-IR spectroscopy.

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