Titel
Giving the Green Light to Photochemical Uncaging of Large Biomolecules in High Vacuum
Autor*in
Yong Hua
Department of Chemistry, University of Basel
Sergey Fisher
Van’t Hoff Institute for Molecular Sciences (HIMS), University of Amsterdam
... show all
Abstract
The isolation of biomolecules in a high vacuum enables experiments on fragile species in the absence of a perturbing environment. Since many molecular properties are influenced by local electric fields, here we seek to gain control over the number of charges on a biopolymer by photochemical uncaging. We present the design, modeling, and synthesis of photoactive molecular tags, their labeling to peptides and proteins as well as their photochemical validation in solution and in the gas phase. The tailored tags can be selectively cleaved off at a well-defined time and without the need for any external charge-transferring agents. The energy of a single or two green photons can already trigger the process, and it is soft enough to ensure the integrity of the released biomolecular cargo. We exploit differences in the cleavage pathways in solution and in vacuum and observe a surprising robustness in upscaling the approach from a model system to genuine proteins. The interaction wavelength of 532 nm is compatible with various biomolecular entities, such as oligonucleotides or oligosaccharides.
Stichwort
photocagesmolecular beamsgas-phase heterolysischarge reductionselective fragmentationbioconjugationbodipy chromophorebiomolecular mass spectrometry
Objekt-Typ
Sprache
Englisch [eng]
Persistent identifier
phaidra.univie.ac.at/o:2068601
Erschienen in
Titel
JACS Au
Band
3
Ausgabe
10
ISSN
2691-3704
Erscheinungsdatum
2023
Seitenanfang
2790
Seitenende
2799
Publication
American Chemical Society (ACS)
Fördergeber
Europäische Union (alle Programme) — 860713
Europäische Union (alle Programme) — 949397
Erscheinungsdatum
2023
Zugänglichkeit
Rechte
Rechteangabe
© 2023 The Authors
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