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Capturing Ultrafast Spin Dynamics in Single-Molecule Magnets Using Femtosecond X-ray Emission Spectroscopy

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

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


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.


Publication metadata

Author(s): Barlow K, Phelps R, Eng J, Ingle RA, Khakhulin D, Biednov M, Dutta S, Jiang Y, Lima FA, Tiwari V, Milne C, Katayama T, Coletta M, Brechin EK, Penfold TJ, Johansson O

Publication type: Article

Publication status: Published

Journal: Journal of Physical Chemistry Letters

Year: 2025

Volume: 16

Pages: 4148–4154

Print publication date: 21/04/2025

Online publication date: 17/04/2025

Acceptance date: 14/04/2025

Date deposited: 21/04/2025

ISSN (electronic): 1948-7185

Publisher: American Chemical Society

URL: https://doi.org/10.1021/acs.jpclett.5c00383

DOI: 10.1021/acs.jpclett.5c00383


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Funding

Funder referenceFunder name
EP/X035514/1
EP/V010573/1
EPSRC

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