Tracking nuclear motion in single-molecule magnets using femtosecond X-ray absorption spectroscopy

Kyle Barlow, Ryan Phelps, Julien Eng, Tetsuo Katayama, Erica Sutcliffe, Marco Coletta, Euan K. Brechin, Thomas J. Penfold () and J. Olof Johansson ()
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Kyle Barlow: University of Edinburgh
Ryan Phelps: University of Edinburgh
Julien Eng: Newcastle University
Tetsuo Katayama: Japan Synchrotron Radiation Research Institute
Erica Sutcliffe: University of Edinburgh
Marco Coletta: University of Edinburgh
Euan K. Brechin: University of Edinburgh
Thomas J. Penfold: Newcastle University
J. Olof Johansson: University of Edinburgh

Nature Communications, 2024, vol. 15, issue 1, 1-7

Abstract: Abstract The development of new data storage solutions is crucial for emerging digital technologies. Recently, all-optical magnetic switching has been achieved in dielectrics, proving to be faster than traditional methods. Despite this, single-molecule magnets (SMMs), which are an important class of magnetic materials due to their nanometre size, remain underexplored for ultrafast photomagnetic switching. Herein, we report femtosecond time-resolved K-edge X-ray absorption spectroscopy (TR-XAS) on a Mn(III)-based trinuclear SMM. Exploiting the elemental specificity of XAS, we directly track nuclear dynamics around the metal ions and show that the ultrafast dynamics upon excitation of a crystal-field transition are dominated by a magnetically active Jahn-Teller mode. Our results, supported by simulations, reveal minute bond length changes from 0.01 to 0.05 Å demonstrating the sensitivity of the method. These geometrical changes are discussed in terms of magneto-structural relationships and consequently our results illustrate the importance of TR-XAS for the emerging area of ultrafast molecular magnetism.

Date: 2024
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DOI: 10.1038/s41467-024-48411-0

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