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Kalinko, Aleksandr
Deutsches Elektronen-Synchrotron DESY
in Cooperation with on an Cooperation-Score of 37%
Topics
Publications (10/10 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
- 2024Advanced science / Ultrafast two-color x-ray emission spectroscopy reveals excited state landscape in a base metal dyad
- 2024Ultrafast Two‐Color X‐Ray Emission Spectroscopy Reveals Excited State Landscape in a Base Metal Dyadcitations
- 2023The influence of Sb doping on the local structure and disorder in thermoelectric ZnO:Sb thin filmscitations
- 2021The role of Ga and Bi doping on the local structure of transparent zinc oxide thin filmscitations
- 2020Exploring the light-induced dynamics in solvated metallogrid complexes with femtosecond pulses across the electromagnetic spectrumcitations
- 2020Ruthenium 4d-to-2p X-ray Emission Spectroscopy: A Simultaneous Probe of the Metal and the Bound Ligandscitations
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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.