Weihua Lin
Postdoctoral fellow
Nonadiabatic Charge Transfer within Photoexcited Nickel Porphyrins
Author
Summary, in English
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.
Department/s
- LTH Profile Area: Nanoscience and Semiconductor Technology
- LU Profile Area: Light and Materials
- Chemical Physics
- NanoLund: Centre for Nanoscience
- Department of Chemistry
- LTH Profile Area: Photon Science and Technology
Publishing year
2024
Language
English
Pages
3627-3638
Publication/Series
Journal of Physical Chemistry Letters
Volume
15
Issue
13
Document type
Journal article
Publisher
The American Chemical Society (ACS)
Topic
- Theoretical Chemistry (including Computational Chemistry)
- Atom and Molecular Physics and Optics
Status
Published
ISBN/ISSN/Other
- ISSN: 1948-7185