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Vibrational coherences in manganese single-molecule magnets after ultrafast photoexcitation

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

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This is the authors' accepted manuscript of an article that has been published in its final definitive form by Nature Publishing Group, 2020.

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Abstract

Magnetic recording using femtosecond laser pulses has recently been achieved in some dielectric media, showing potential for ultrafast data storage applications. Single-molecule magnets (SMMs) are metal complexes with two degenerate magnetic ground states and are promising for increasing storage density, but remain unexplored using ultrafast techniques. Here we have explored the dynamics occurring after photoexcitation of a trinuclear µ₃-oxo-bridged Mn(III)-based SMM, whose magnetic anisotropy is closely related to the Jahn–Teller distortion. Ultrafast transient absorption spectroscopy in solution reveals oscillations superimposed on the decay traces due to a vibrational wavepacket. Based on complementary measurements and calculations on the monomer Mn(acac)₃, we conclude that the wavepacket motion in the trinuclear SMM is constrained along the Jahn–Teller axis due to the µ₃-oxo and µ-oxime bridges. Our results provide new possibilities for optical control of the magnetization in SMMs on femtosecond timescales and open up new molecular-design challenges to control the wavepacket motion in the excited state of polynuclear transition-metal complexes.

Publication metadata

Author(s): Liedy F, Eng J, McNab R, Inglis R, Penfold TJ, Brechin EK, Johansson JO

Publication type: Article

Publication status: Published

Journal: Nature Chemistry

Year: 2020

Volume: 12

Issue: 5

Pages: 452-458

Print publication date: 01/05/2020

Online publication date: 02/03/2020

Acceptance date: 27/01/2020

Date deposited: 05/03/2020

ISSN (print): 1755-4330

ISSN (electronic): 1755-4349

Publisher: Nature Publishing Group

URL: https://doi.org/10.1038/s41557-020-0431-6

DOI: 10.1038/s41557-020-0431-6

Data Access Statement: https://doi.org/10.7488/ds/2751

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