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

Lookup NU author(s): Dr Julien EngORCiD, Professor Thomas Penfold

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This work is licensed under a Creative Commons Attribution 4.0 International License (CC BY 4.0).

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.

Publication metadata

Author(s): Barlow K, Phelps R, Eng J, Katayama T, Sutcliffe E, Coletta M, Brechin E, Penfold TJ, Johansson JO

Publication type: Article

Publication status: Published

Journal: Nature Communications

Year: 2024

Volume: 15

Online publication date: 14/05/2024

Acceptance date: 30/04/2024

Date deposited: 14/05/2024

ISSN (electronic): 2041-1723

Publisher: Springer Nature

URL: https://doi.org/10.1038/s41467-024-48411-0

DOI: 10.1038/s41467-024-48411-0

Data Access Statement: Raw data were generated at SACLA and are available from the corresponding authors. Derived data used to create the figures shown in the paper are provided in "Source Data.zip" attached to this paper. Source data are provided with this paper. Code availability: VCMaker used to generate the normal mode distortions can be found at https://github.com/JulienEng/VCMaker/

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