Revealing Hot and Long-Lived Metastable Spin States in the Photoinduced Switching of Solvated Metallogrid Complexes with Femtosecond Optical and X-ray Spectroscopies

Forskningsoutput: TidskriftsbidragArtikel i vetenskaplig tidskrift

Abstract

An atomistic understanding of the photoinduced spin-state switching (PSS) within polynuclear systems of d4-d7 transition metal ion complexes is required for their rational integration into light-driven reactions of chemical and biological interest. However, in contrast to mononuclear systems, the multidimensional dynamics of the PSS in solvated molecular arrays have not yet been elucidated due to the expected complications associated with the connectivity between the metal centers and the strong interactions with the surroundings. In this work, the PSS in a solvated triiron(II) metallogrid complex is characterized using transient optical absorption and X-ray emission spectroscopies on the femtosecond time scale. The complementary measurements reveal the photoinduced creation of energy-rich (hot) and long-lived quintet states, whose dynamics differ critically from their mononuclear congeners. This finding opens major prospects for developing novel schemes in solution-phase spin chemistry that are driven by the dynamic PSS process in compact oligometallic arrays.

Detaljer

Författare
  • Maria A. Naumova
  • Aleksandr Kalinko
  • Joanne W.L. Wong
  • Huifang Geng
  • Edoardo Domenichini
  • Jie Meng
  • Sol Alvarez Gutierrez
  • Peter Zalden
  • Andreas Galler
  • Frederico Lima
  • Katharina Kubicek
  • Mykola Biednov
  • Alexander Britz
  • Stefano Checchia
  • Victoria Kabanova
  • Michael Wulff
  • Jennifer Zimara
  • Dirk Schwarzer
  • Serhiy Demeshko
  • Vadim Murzin
  • David Gosztola
  • Jianxin Zhang
  • Matthias Bauer
  • Max Latevi Lawson Daku
  • Wojciech Gawelda
  • Dmitry Khakhulin
  • Christian Bressler
  • Franc Meyer
  • Sophie E. Canton
Enheter & grupper
Externa organisationer
  • German Electron Synchrotron (DESY)
  • University of Paderborn
  • University of Göttingen
  • South Valley University
  • ELI-HU Non-profit Ltd
  • ELI Attosecond Light Pulse Source (ELI-ALPS)
  • University of Strasbourg
  • Technical University of Denmark
  • Hong Kong Polytechnic University
  • European XFEL GmbH
  • European Synchrotron Radiation Facility
  • Max Planck Institute for Biophysical Chemistry
  • University of Wuppertal
  • Argonne National Laboratory
  • Tianjin Polytechnic University
  • University of Geneva
  • Adam Mickiewicz University in Poznań
  • University of Hamburg
Forskningsområden

Ämnesklassifikation (UKÄ) – OBLIGATORISK

  • Fysikalisk kemi
Originalspråkengelska
Sidor (från-till)2133-2141
Antal sidor9
TidskriftThe Journal of Physical Chemistry Letters
Volym11
Utgåva nummer6
StatusPublished - 2020
PublikationskategoriForskning
Peer review utfördJa