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Nonadiabatic Charge Transfer within Photoexcited Nickel Porphyrins.
Naumova, Maria A; Paveliuc, Gheorghe; Biednov, Mykola; Kubicek, Katharina; Kalinko, Aleksandr; Meng, Jie; Liang, Mingli; Rahaman, Ahibur; Abdellah, Mohamed; Checchia, Stefano; Alves Lima, Frederico; Zalden, Peter; Gawelda, Wojciech; Bressler, Christian; Geng, Huifang; Lin, Weihua; Liu, Yan; Zhao, Qian; Pan, Qinying; Akter, Marufa; Kong, Qingyu; Retegan, Marius; Gosztola, David J; Pápai, Mátyás; Khakhulin, Dmitry; Lawson Daku, Max; Zheng, Kaibo; Canton, Sophie E.
Afiliação
  • Naumova MA; Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607 Hamburg, Germany.
  • Paveliuc G; Département de Chimie Physique, Université de Genève, Quai E. Ansermet 30, CH-1211 Genève, Switzerland.
  • Biednov M; European XFEL, Holzkoppel 4, 22869 Schenefeld, Germany.
  • Kubicek K; European XFEL, Holzkoppel 4, 22869 Schenefeld, Germany.
  • Kalinko A; The Hamburg Centre for Ultrafast Imaging, University of Hamburg, Luruper Chaussee 149, 22761 Hamburg, Germany.
  • Meng J; Fachbereich Physik, Universität Hamburg, Notkestraße 9-11, 22607 Hamburg, Germany.
  • Liang M; Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607 Hamburg, Germany.
  • Rahaman A; Department of Chemistry, Technical University of Denmark, Kongens Lyngby DK-2800, Denmark.
  • Abdellah M; Chemical Physics and NanoLund, Lund University, SE-221 00 Lund, Sweden.
  • Checchia S; Department of Chemistry, Technical University of Denmark, Kongens Lyngby DK-2800, Denmark.
  • Alves Lima F; Department of Chemistry, Technical University of Denmark, Kongens Lyngby DK-2800, Denmark.
  • Zalden P; Chemical Physics and NanoLund, Lund University, SE-221 00 Lund, Sweden.
  • Gawelda W; Chemical Physics and NanoLund, Lund University, SE-221 00 Lund, Sweden.
  • Bressler C; Department of Chemistry, United Arab Emirates University, P.O. Box 15551, Al Ain, United Arab Emirates.
  • Geng H; Department of Chemistry, Qena Faculty of Science, South Valley University, Qena 83523, Egypt.
  • Lin W; ESRF - The European Synchrotron, 71, avenue des Martyrs, CS 40220, 38043 Grenoble Cedex 9, France.
  • Liu Y; European XFEL, Holzkoppel 4, 22869 Schenefeld, Germany.
  • Zhao Q; European XFEL, Holzkoppel 4, 22869 Schenefeld, Germany.
  • Pan Q; European XFEL, Holzkoppel 4, 22869 Schenefeld, Germany.
  • Akter M; Departamento de Química, Universidad Autónoma de Madrid, Madrid 28049, Spain.
  • Kong Q; IMDEA-Nanociencia, Calle Faraday 9, Madrid 28049, Spain.
  • Retegan M; Faculty of Physics, Adam Mickiewicz University, Poznan 61-614, Poland.
  • Gosztola DJ; European XFEL, Holzkoppel 4, 22869 Schenefeld, Germany.
  • Pápai M; The Hamburg Centre for Ultrafast Imaging, University of Hamburg, Luruper Chaussee 149, 22761 Hamburg, Germany.
  • Khakhulin D; Fachbereich Physik, Universität Hamburg, Notkestraße 9-11, 22607 Hamburg, Germany.
  • Lawson Daku M; Department of Physics, Yantai University, 30 Qingquan Road, Yantai 264005, China.
  • Zheng K; Chemical Physics and NanoLund, Lund University, SE-221 00 Lund, Sweden.
  • Canton SE; Chemical Physics and NanoLund, Lund University, SE-221 00 Lund, Sweden.
J Phys Chem Lett ; 15(13): 3627-3638, 2024 Apr 04.
Article em En | MEDLINE | ID: mdl-38530393
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.

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: J Phys Chem Lett Ano de publicação: 2024 Tipo de documento: Article País de afiliação: Alemanha

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Idioma: En Revista: J Phys Chem Lett Ano de publicação: 2024 Tipo de documento: Article País de afiliação: Alemanha