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Weihua Lin. Portrait.

Weihua Lin

Postdoctoral fellow

Weihua Lin. Portrait.

Nonadiabatic Charge Transfer within Photoexcited Nickel Porphyrins

Author

  • Maria A. Naumova
  • Gheorghe Paveliuc
  • Mykola Biednov
  • Katharina Kubicek
  • Aleksandr Kalinko
  • Jie Meng
  • Mingli Liang
  • Ahibur Rahaman
  • Mohamed Abdellah
  • Stefano Checchia
  • Frederico Alves Lima
  • Peter Zalden
  • Wojciech Gawelda
  • Christian Bressler
  • Huifang Geng
  • Weihua Lin
  • Yan Liu
  • Qian Zhao
  • Qinying Pan
  • Marufa Akter
  • Qingyu Kong
  • Marius Retegan
  • David J. Gosztola
  • Mátyás Pápai
  • Dmitry Khakhulin
  • Max Lawson Daku
  • Kaibo Zheng
  • Sophie E. Canton

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