Capturing Ultrafast Spin Dynamics in Single-Molecule Magnets Using Femtosecond X-ray Emission Spectroscopy
Achieving ultrafast photomagnetic switching of single-molecule magnets (SMMs) could lead to simultaneous fast and dense data storage devices. To facilitate this, a thorough understanding of the ultrafast dynamics emerging after ultrashort laser pulse excitation is essential. However, the complex nature of these materials means there is a lack of established experimental techniques that can probe the spin dynamics in SMMs. Herein, we perform femtosecond time-resolved Mn K-edge X-ray emission spectroscopy on a Mn(III)-based trinuclear SMM (Mn<sub>3</sub>) and the model system Mn(acac)<sub>3</sub>. The spectral changes of Mn(acac)<sub>3</sub> are consistent with switching between Jahn-Teller distorted structures expected after photoexcitation. A similar result is observed for Mn<sub>3</sub>; however, the Kβ signal also reveals insight into the distribution of spin states populated within 100 fs. The importance of using probes across the electromagnetic spectrum to gain a thorough understanding of the dynamics of exchange-coupled complexes is highlighted.
Authors
- Tetsuo Katayama (ORCID: https://orcid.org/0000-0002-2681-8316)
- Dmitry Khakhulin (ORCID: https://orcid.org/0000-0002-4453-1204)
- Julien Eng (ORCID: https://orcid.org/0000-0002-7118-7242)
- Kyle Barlow (ORCID: https://orcid.org/0000-0003-3694-3505)
- Yifeng Jiang (ORCID: https://orcid.org/0000-0003-0685-0498)
- J. Olof Johansson (ORCID: https://orcid.org/0000-0002-9320-447X)
- Ryan Phelps (ORCID: https://orcid.org/0000-0001-9036-2133)
- Marco Coletta (ORCID: https://orcid.org/0000-0003-2212-5456)
- Thomas J. Penfold (ORCID: https://orcid.org/0000-0003-4490-5672)
- Sharmistha Paul Dutta
- Vandana Tiwari (ORCID: https://orcid.org/0000-0003-1961-7257)
- Rebecca A. Ingle (ORCID: https://orcid.org/0000-0002-0566-3407)
- Mykola Biednov (ORCID: https://orcid.org/0000-0003-2219-155X)
- Frederico A. Lima (ORCID: https://orcid.org/0000-0001-8106-2892)
- Euan K. Brechin (ORCID: https://orcid.org/0000-0002-9365-370X)
- Christopher J. Milne (ORCID: https://orcid.org/0000-0003-4714-9139)
Institutions
- SPring-8 (JP)
- Japan Synchrotron Radiation Research Institute (JP)
- University College London (GB)
- Newcastle University (GB)
- European X-Ray Free-Electron Laser (DE)
- University of Edinburgh (GB)
Publication Details
- Journal
- The Journal of Physical Chemistry Letters
- Published
- 2025-04-17
- DOI
- https://doi.org/10.1021/acs.jpclett.5c00383
- Primary Topic
- Magnetism in coordination complexes
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- Engineering and Physical Sciences Research Council