Capturing Ultrafast Spin Dynamics in Single-Molecule Magnets Using Femtosecond X‑ray Emission Spectroscopy
- Kyle Barlow, Ryan Phelps, Julien Eng, Rebecca A. Ingle, Dmitry Khakhulin, Mykola Biednov, Sharmistha Paul Dutta, Yifeng Jiang, Frederico A. Lima, Vandana Tiwari, Christopher Milne, Tetsuo Katayama, Marco Coletta, Euan K. Brechin, Thomas J. Penfold and J. Olof Johansson
- Publication , Project collaboration
- April 17, 2025
Abstract:
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 (Mn3) and the model system Mn(acac)3. The spectral changes of Mn(acac)3 are consistent with switching between Jahn–Teller distorted structures expected after photoexcitation. A similar result is observed for Mn3; 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.
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DOI:
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J. Phys. Chem. Lett. 2025, 16, 4148−4154
