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Fatima, Anam 
ORCID: https://orcid.org/0000-0003-2388-4390, He, Yongle, Rosenberger, Danielle, Greetham, Gregory M., Malakar, Partha, Lukacs, Andras, Tonge, Peter J. and Meech, Stephen R. ORCID: https://orcid.org/0000-0001-5561-2782
(2026)
Dynamics and mechanism of off- to on-switching in Dreiklang a decoupled reversibly switchable fluorescent protein.
Angewandte Chemie International Edition, 65 (1).
ISSN 1433-7851
Abstract
Dreiklang is a reversibly switchable (rs) fluorescent protein (FP) with a unique off-state, a UV absorbing hydrated form of the typical FP chromophore. Here we report ultrafast dynamics of the off- to on-state transition in Dreiklang using complementary ultrafast optical and vibrational transient absorption to resolve chromophore driven protein structural dynamics. This approach allows observation of the real-time response in a protein to bond breaking and forming events. The excited electronic state decays in a nonsingle exponential fashion in tens to hundreds of picoseconds, undergoing photodehydration with a yield of several per-cent. The primary photoproduct formed is identified as the cis protonated form of the FP chromophore, initially in a perturbed H-bonded environment. This primary product relaxes on a few microseconds timescale by a mechanism involving changes to a glutamic acid residue and modifications of the amide backbone, possibly involving a carbonyl to imine tautomerization. The temporal and spectral resolution of Dreiklang's photodehydration provides data against which to test quantum chemical calculations of reaction dynamics in proteins and suggests a route to modifying and potentially enhancing its photoswitching properties.
| Item Type: | Article |
|---|---|
| Additional Information: | Data Availability Statement: The data that support the findings of this study are available from the corresponding author upon reasonable request. |
| Uncontrolled Keywords: | biophysics,fluorescent protein,infra-red,photophysics,photoswitching,ultrafast,general chemistry,catalysis,3* ,/dk/atira/pure/subjectarea/asjc/1600/1600 |
| Faculty \ School: | Faculty of Science > School of Chemistry, Pharmacy and Pharmacology |
| UEA Research Groups: | Faculty of Science > Research Groups > Centre for Photonics and Quantum Science (former - to 2025) Faculty of Science > Research Groups > Chemistry of Light and Energy (former - to 2025) |
| Related URLs: | |
| Depositing User: | LivePure Connector |
| Date Deposited: | 14 Nov 2025 16:30 |
| Last Modified: | 18 Jun 2026 20:47 |
| URI: | https://ueaeprints.uea.ac.uk/id/eprint/100998 |
| DOI: | 10.1002/anie.202518264 |
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