Exploring the light-induced dynamics in solvated metallogrid complexes with femtosecond pulses across the electromagnetic spectrum
Authors:
- Maria A. Naumova,
- Aleksandr Kalinko,
- Joanne W. L. Wong,
- Sol Alvarez Gutierrez,
- Jie Meng,
- Mingli Liang,
- Mohamed Abdellah,
- Huifang Geng,
- Weihua Lin,
- Katharina Kubicek,
- Mykola Biednov,
- Frederico Lima,
- Andreas Galler,
- Peter Zalden,
- Stefano Checchia,
- Pierre-Adrien Mante,
- Jennifer Zimara,
- Dirk Schwarzer,
- Serhiy Demeshko,
- Vadim Murzin,
- David Gosztola,
- Martin Jarenmark,
- Jianxin Zhang,
- Matthias Bauer,
- Max Latevi Lawson Daku,
- Dmitry Khakhulin,
- Wojciech Miłosz Gawełda,
- Christian Bressler,
- Franc Meyer,
- Kaibo Zheng,
- Sophie E. Canton
Abstract
Oligonuclear complexes of d4–d7 transition metal ion centers that undergo spin-switching have long been developed for their practical role in molecular electronics. Recently, they also have appeared as promising photochemical reactants demonstrating improved stability. However, the lack of knowledge about their photophysical properties in the solution phase compared to mononuclear complexes is currently hampering their inclusion into advanced light-driven reactions. In the present study, the ultrafast photoinduced dynamics in a solvated [2 × 2] iron(II) metallogrid complex are characterized by combining measurements with transient optical-infrared absorption and x-ray emission spectroscopy on the femtosecond time scale. The analysis is supported by density functional theory calculations. The photocycle can be described in terms of intra-site transitions, where the FeII centers in the low-spin state are independently photoexcited. The Franck–Condon state decays via the formation of a vibrationally hot high-spin (HS) state that displays coherent behavior within a few picoseconds and thermalizes within tens of picoseconds to yield a metastable HS state living for several hundreds of nanoseconds. Systematic comparison with the closely related mononuclear complex [Fe(terpy)2]2+ reveals that nuclearity has a profound impact on the photoinduced dynamics. More generally, this work provides guidelines for expanding the integration of oligonuclear complexes into new photoconversion schemes that may be triggered by ultrafast spin-switching.
- Record ID
- UAM3aa74b06738e4b05b24ec7200305870f
- Author
- Journal series
- Journal of Chemical Physics, ISSN 0021-9606, e-ISSN 1089-7690, [1089-7690]
- Issue year
- 2020
- Vol
- 152
- No
- 21
- Article number
- 214301
- ASJC Classification
- ;
- DOI
- DOI:10.1063/1.5138641 Opening in a new tab
- Language
- (en) English
- Score (nominal)
- 100
- Score source
- journalList
- Score
- = 100.0, 11-02-2022, ArticleFromJournal
- Publication indicators
- = 4; = 3; : 2018 = 0.969; : 2019 (2 years) = 2.991 - 2019 (5 years) =2.835
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- Uniform Resource Identifier
- https://researchportal.amu.edu.pl/info/article/UAM3aa74b06738e4b05b24ec7200305870f/
- URN
urn:amu-prod:UAM3aa74b06738e4b05b24ec7200305870f
* presented citation count is obtained through Internet information analysis and it is close to the number calculated by the Publish or PerishOpening in a new tab system.