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

Naumova, Maria A. ; Kalinko, Aleksandr ; Wong, Joanne W.L. ; Abdellah, Mohamed LU ; Geng, Huifang LU ; Domenichini, Edoardo ; Meng, Jie ; Gutierrez, Sol Alvarez ; Mante, Pierre Adrien LU and Lin, Weihua LU , et al. (2020) In The Journal of Physical Chemistry Letters 11(6). p.2133-2141
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... (More)

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.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
in
The Journal of Physical Chemistry Letters
volume
11
issue
6
pages
9 pages
publisher
The American Chemical Society (ACS)
external identifiers
  • scopus:85082099243
  • pmid:32069410
ISSN
1948-7185
DOI
10.1021/acs.jpclett.9b03883
language
English
LU publication?
yes
id
01f0745d-1cb8-4248-90d4-a002cd2187db
date added to LUP
2020-04-03 12:33:13
date last changed
2025-01-10 09:39:18
@article{01f0745d-1cb8-4248-90d4-a002cd2187db,
  abstract     = {{<p>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.</p>}},
  author       = {{Naumova, Maria A. and Kalinko, Aleksandr and Wong, Joanne W.L. and Abdellah, Mohamed and Geng, Huifang and Domenichini, Edoardo and Meng, Jie and Gutierrez, Sol Alvarez and Mante, Pierre Adrien and Lin, Weihua and Zalden, Peter and Galler, Andreas and Lima, Frederico and Kubicek, Katharina and Biednov, Mykola and Britz, Alexander and Checchia, Stefano and Kabanova, Victoria and Wulff, Michael and Zimara, Jennifer and Schwarzer, Dirk and Demeshko, Serhiy and Murzin, Vadim and Gosztola, David and Jarenmark, Martin and Zhang, Jianxin and Bauer, Matthias and Lawson Daku, Max Latevi and Gawelda, Wojciech and Khakhulin, Dmitry and Bressler, Christian and Meyer, Franc and Zheng, Kaibo and Canton, Sophie E.}},
  issn         = {{1948-7185}},
  language     = {{eng}},
  number       = {{6}},
  pages        = {{2133--2141}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{The Journal of Physical Chemistry Letters}},
  title        = {{Revealing Hot and Long-Lived Metastable Spin States in the Photoinduced Switching of Solvated Metallogrid Complexes with Femtosecond Optical and X-ray Spectroscopies}},
  url          = {{http://dx.doi.org/10.1021/acs.jpclett.9b03883}},
  doi          = {{10.1021/acs.jpclett.9b03883}},
  volume       = {{11}},
  year         = {{2020}},
}