Synthetic fluorescent protein chromophores have been reported for their singlet state fluorescence properties and applications in bioimaging, but rarely for the triplet state chemistries. Herein, we enabled their photo‐sensitizing and photo‐crosslinking properties through rational modulations. Extension of molecular conjugation and introduction of heavy atoms promoted the generation of reactive oxygen species. Unlike other photosensitizers, these chromophores selectively photo‐crosslinked aggregated proteins and uncovered the interactome profiles. We also exemplified their general applications in chromophore‐assisted light inactivation, photodynamic therapy and photo induced polymerization. Theoretical calculation, pathway analysis and transient absorption spectroscopy provided mechanistic insights for this triplet state chemistry. Overall, this work expands the function and application of synthetic fluorescent protein chromophores by enabling their triplet excited state properties.
- Award ID(s):
- 1764264
- PAR ID:
- 10374203
- Date Published:
- Journal Name:
- Chemistry – A European Journal
- Volume:
- 28
- Issue:
- 3
- ISSN:
- 0947-6539
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Synthetic fluorescent protein chromophores have been reported for their singlet state fluorescence properties and applications in bioimaging, but rarely for the triplet state chemistries. Herein, we enabled their photo‐sensitizing and photo‐crosslinking properties through rational modulations. Extension of molecular conjugation and introduction of heavy atoms promoted the generation of reactive oxygen species. Unlike other photosensitizers, these chromophores selectively photo‐crosslinked aggregated proteins and uncovered the interactome profiles. We also exemplified their general applications in chromophore‐assisted light inactivation, photodynamic therapy and photo induced polymerization. Theoretical calculation, pathway analysis and transient absorption spectroscopy provided mechanistic insights for this triplet state chemistry. Overall, this work expands the function and application of synthetic fluorescent protein chromophores by enabling their triplet excited state properties.
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Background: Little data is available for the pygmy dipole resonance (PDR) in axially deformed nuclei. Photon scattering experiments are complicated by high level densities in the PDR region and the small energy difference of transitions to the ground state and to excited states. Purpose: We report on an experimental study of the low-energy dipole strength distribution of the well-deformed nucleus 164Dy between 4.0–7.7 MeV. Methods: The low-lying photoresponse of 164Dy has been investigated using the method of nuclear resonance fluorescence using a quasimonochromatic linearly polarized γ -ray beam in the energy range of 4.0–7.7 MeV in steps of 0.2 MeV. Results: For excitation energies between 4 MeV and 5 MeV, sufficiently low level densities allow for the identification of individual states, including level energies, reduced transition widths and branching ratios. Energy-averaged mean decay branching ratios, mean population ratios and partial absorption cross sections were determined above 5 MeV up to the neutron-separation threshold at 7.7 MeV. A Lorentzian-shaped enhancement of the partial photo absorption cross section followed by decays back to the ground-state band is found at 6.10(5) MeV with a width of 0.77(23) MeV. A comparison with results from complementary measurements is performed using the framework of the statistical model. Conclusions: The experimental results for the mean population ratios deviate systematically from the statistical model simulation by 30(6)%. However, they are in agreement within one standard deviation of the simulation.more » « less
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1002/chem.202103346
