Journal Article

PUBDB-2024-00986

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Nonadiabatic charge-transfer within photoexcited nickel porphyrins

Naumova, M.XFEL.EU*DESY* ; paveliuc, g. ; Biednov, M.CFEL*XFEL.EU* ; Kubicek, K.XFEL.EU* ; Kalinko, A.DESY* ; Meng, J.Extern*XFEL.EU* ; Liang, M.Extern*XFEL.EU* ; Rahaman, A.Extern*XFEL.EU* ; Abdellah, M. ; Checchia, S.Extern*XFEL.EU* ; Alves Lima, F.XFEL.EU* ; Zalden, P.XFEL.EU* ; Gawelda, W.XFEL.EU* ; Bressler, C.XFEL.EU* ; Geng, H.Extern*XFEL.EU* ; Lin, W.Extern*XFEL.EU* ; Liu, Y. ; Zhao, Q.Extern*XFEL.EU* ; Pan, Q.Extern*XFEL.EU* ; Akter, M. ; Kong, Q.Extern*XFEL.EU* ; Retegan, M. ; Gosztola, D.Extern*XFEL.EU* ; Papai, M.Extern* ; Khakhulin, D.XFEL.EU* ; Lawson Daku, L. (Corresponding author)Extern*XFEL.EU* ; Zheng, K. (Corresponding author)Extern*XFEL.EU* ; Canton, S. (Corresponding author)XFEL.EU*

2024
ACS Washington, DC

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Please use a persistent id in citations: doi:10.1021/acs.jpclett.4c00375  doi:10.3204/PUBDB-2024-00986

Abstract: Metalloporphyrins with open d-shell ions can drive biochemical energy cycles.However, their utilization in photoconversion is hampered by rapid deactivation. Mappingthe relaxation pathways is essential for elaborating strategies that can favorably alter thecharge dynamics through chemical design and photoexcitation conditions. Here, we combinetransient optical absorption spectroscopy and transient X-ray emission spectroscopy withfemtosecond resolution to probe directly the coupled electronic and spin dynamics within aphotoexcited nickel porphyrin in solution. Measurements and calculations reveal that a statewith charge-transfer character mediates the formation of the thermalized excited state,thereby advancing the description of the photocycle for this important representativemolecule. More generally, establishing that intramolecular charge-transfer steps play a role inthe photoinduced dynamics of metalloporphyrins with open d-shell sets a conceptual groundfor their development as building blocks capable of boosting nonadiabatic photoconversionin functional architectures through “hot” charge transfer down to the attosecond time scale.

Note: This publication is licensed under CC-BY 4.0.This work received funding fromthe VILLUM FONDEN (VIL50350), and the SwedishResearch Council No. 2021-05319 (KZ). This work receivedfunding from the Hungarian National Research, Developmentand Innovation Fund under Grant Nos. NKFIH FK 145967(MP) and TKP2021-NVA-04 (MP). KK gratefully acknowl-edges funding by the DFG within the program “Sachbeihilfe”project ID 497431350 (KU 4184/1-1). CB and KK acknowl-edge support by the Deutsche Forschungsgemeinschaft (DFG)via the Cluster of Excellence ‘Advanced Imaging of Matter’,EXC 2056, Project ID 390715994, and via SFB925 ID170620586 (TP A4). WG acknowledges funding from SpanishMIU through “Ayudas Beatriz Galindo” (BEAGAL18/00092),Comunidad de Madrid and Universidad Autónoma de Madridthrough “Proyecto de I+D para Investigadores del ProgramaBeatriz Galindo” (SI2/PBG/2020-00003), Spanish MICIUthrough Proyecto de I+D+i 2019 (PID2019-108678GB-I00),and IMDEA-Nanociencia support from the Severo OchoaProgramme for Centers of Excellence in R&D (MINECO,grant CEX2020-001039-S). WG further acknowledges partialsupport from the National Science Centre in Poland underSONATA BIS 6 Grant 2016/22/E/ST4/00543 and thesupport to access the European XFEL under a grant of thePolish Ministry of Education and Science - decision no. 2022/WK/13. DG acknowledges support from the Center forNanoscale Materials, a U.S. Department of Energy Office ofScience User Facility, supported by the U.S. DOE, Office ofBasic Energy Sciences, under Contract No. DE-AC02-06CH11357. MP acknowledges support from the János BolyaiScholarship of the Hungarian Academy of Sciences.

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Contributing Institute(s):

1. PETRA-S (FS-PETRA-S)
2. The European XFEL Users (XFEL-User)
3. FXE (XFEL_E1_FXE)

Research Program(s):

1. 631 - Matter – Dynamics, Mechanisms and Control (POF4-631) (POF4-631)
2. DFG project 194651731 - EXC 1074: Hamburger Zentrum für ultraschnelle Beobachtung (CUI): Struktur, Dynamik und Kontrolle von Materie auf atomarer Skala (194651731) (194651731)
3. DFG project 390715994 - EXC 2056: CUI: Advanced Imaging of Matter (390715994) (390715994)

Experiment(s):

1. FXE: Femtosecond X-ray Experiments (SASE1)

Appears in the scientific report 2024

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Database coverage:
; ; ; Clarivate Analytics Master Journal List ; Current Contents - Physical, Chemical and Earth Sciences ; Essential Science Indicators ; IF >= 5 ; JCR ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection

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