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Monitoring tautomerization of single hypericin molecules in a tunable optical λ/2 microcavity

  • Hypericin tautomerization that involves the migration of the labile protons is believed to be the primary photophysical process relevant to its light-activated antiviral activity. Despite the difficulty in isolating individual tautomers, it can be directly observed in single-molecule experiments. We show that the tautomerization of single hypericin molecules in free space is observed as an abrupt flipping of the image pattern accompanied with fluorescence intensity fluctuations, which are not correlated with lifetime changes. Moreover, the study can be extended to a λ/2 Fabry–Pérot microcavity. The modification of the local photonic environment by a microcavity is well simulated with a theoretical model that shows good agreement with the experimental data. Inside a microcavity, the excited state lifetime and fluorescence intensity of single hypericin molecules are correlated, and a distinct jump of the lifetime and fluorescence intensity reveals the temporal behavior of the tautomerization with high sensitivity and high temporal resolution. The observed changes are also consistent with time-dependent density functional theory calculations. Our approach paves the way to monitor and even control reactions for a wider range of molecules at the single molecule level.

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Metadaten
Author of HS ReutlingenBrecht, Marc; Wackenhut, Frank
DOI:https://doi.org/10.1063/5.0078117
ISSN:0021-9606
eISSN:1089-7690
Erschienen in:The journal of chemical physics
Publisher:American Institute of Physics
Place of publication:Melville, NY
Document Type:Journal article
Language:English
Publication year:2022
Volume:156
Issue:1
Page Number:9
Article Number:014203
DDC classes:540 Chemie
Open access?:Nein
Licence (German):License Logo  In Copyright - Urheberrechtlich geschützt