Frontispiece: Direct Observation of Ultrafast Proton Rocking in the BLUF Domain

Phototriggers are useful molecular tools to initiate reactions in enzymes by light for the purpose of photoenzymatic design and mechanistic investigations. Here, we incorporated the non-natural amino acid 5-cyanotryptophan (W5CN) in a polypeptide scaffold and resolved the photochemical reaction of the W5CN–W motif using femtosecond transient UV/Vis and mid-IR spectroscopy. We identified a marker band of ∼2037 cm−1 from the CN stretch of the electron transfer intermediate W5CN·− in the transient IR measurement and found UV/Vis spectroscopic evidence for the W·+ radical at 580 nm. Through kinetic analysis, we characterized that the charge separation between the excited W5CN and W occurs in 253 ps, with a charge-recombination lifetime of 862 ps. Our study highlights the potential use of the W5CN–W pair as an ultrafast phototrigger to initiate reactions in enzymes that are not light-sensitive, making downstream reactions accessible to femtosecond spectroscopic detection.

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An ultrafast phototrigger of the Trp5CN–Trp motif in a β-hairpin peptide

Zhang

Zhou

Deng

et al. 2023

The Journal of Chemical Physics

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Frontispiece: Direct Observation of Ultrafast Proton Rocking in the BLUF Domain

Abstract: Electron Transfer In their Communication (e202114423), Bei Ding, Dongping Zhong et al. investigate the photoinduced proton‐coupled electron transfer processes of the OaPAC BLUF domain W mutant.

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An ultrafast phototrigger of the Trp5CN–Trp motif in a β-hairpin peptide

An ultrafast phototrigger of the Trp5CN–Trp motif in a β-hairpin peptide

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