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| Azevedo, Nuno Monteiro |
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Retegan, Marius
European Synchrotron Radiation Facility
in Cooperation with on an Cooperation-Score of 37%
Topics
Publications (6/6 displayed)
- 2024Nonadiabatic charge-transfer within photoexcited nickel porphyrinscitations
- 2024Nonadiabatic Charge Transfer within Photoexcited Nickel Porphyrins
- 2024Nonadiabatic Charge Transfer within Photoexcited Nickel Porphyrinscitations
- 2024Nonadiabatic Charge Transfer within Photoexcited Nickel Porphyrinscitations
- 2023New insights on Fe–N–C catalyst structure from valence-to-core X-ray emission and absorption spectroscopiescitations
- 2017A high-valent non heme μ-oxo MnIV dimer generated from a thiolate-bound MnII complex and O2citations
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document
Nonadiabatic Charge Transfer within Photoexcited Nickel Porphyrins
Abstract
Metalloporphyrins with open d-shell ions can drive biochemical energy cycles. However, their utilization in photoconversion is hampered by rapid deactivation. Mapping the relaxation pathways is essential for elaborating strategies that can favorably alter the charge dynamics through chemical design and photoexcitation conditions. Here, we combine transient optical absorption spectroscopy and transient X-ray emission spectroscopy with femtosecond resolution to probe directly the coupled electronic and spin dynamics within a photoexcited nickel porphyrin in solution. Measurements and calculations reveal that a state with charge-transfer character mediates the formation of the thermalized excited state, thereby advancing the description of the photocycle for this important representative molecule. More generally, establishing that intramolecular charge-transfer steps play a role in the photoinduced dynamics of metalloporphyrins with open d-shell sets a conceptual ground for their development as building blocks capable of boosting nonadiabatic photoconversion in functional architectures through "hot" charge transfer down to the attosecond time scale.