Ultrafast Jahn‐Teller Photoswitching in Cobalt Single‐Ion Magnets

Single‐ion magnets (SIMs) constitute the ultimate size limit in the quest for miniaturizing magnetic materials. Several bottlenecks currently hindering breakthroughs in quantum information and communication technologies could be alleviated by new generations of SIMs displaying multifunctionality. He...

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Bibliographic Details
Published in:Advanced science Vol. 10; no. 21; pp. e2206880 - n/a
Main Authors: Canton, Sophie E., Biednov, Mykola, Pápai, Mátyás, Lima, Frederico A., Choi, Tae‐Kyu, Otte, Florian, Jiang, Yifeng, Frankenberger, Paul, Knoll, Martin, Zalden, Peter, Gawelda, Wojciech, Rahaman, Ahibur, Møller, Klaus B., Milne, Christopher, Gosztola, David J., Zheng, Kaibo, Retegan, Marius, Khakhulin, Dmitry
Format: Journal Article
Language:English
Published: Germany John Wiley & Sons, Inc 01.07.2023
Wiley Open Access
Wiley
John Wiley and Sons Inc
Subjects:
Condensed Matter Physics (including Material Physics, Nano Physics)
Den kondenserade materiens fysik (Här ingår: Materialfysik, nanofysik)
Fysik
Jahn-Teller effect
Ligands
MATERIALS SCIENCE
Natural Sciences
Naturvetenskap
photoswitching
Physical Sciences
Physics
single-ion magnets
Spectrum analysis
XFEL science
single-ion-magnets
photoswitching
Jahn-Teller effect
XFEL science
ISSN:2198-3844, 2198-3844
Online Access:Get full text
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Summary:Single‐ion magnets (SIMs) constitute the ultimate size limit in the quest for miniaturizing magnetic materials. Several bottlenecks currently hindering breakthroughs in quantum information and communication technologies could be alleviated by new generations of SIMs displaying multifunctionality. Here, ultrafast optical absorption spectroscopy and X‐ray emission spectroscopy are employed to track the photoinduced spin‐state switching of the prototypical complex [Co(terpy)2]2+ (terpy = 2,2′:6′,2″‐terpyridine) in solution phase. The combined measurements and their analysis supported by density functional theory (DFT), time‐dependent‐DFT (TD‐DFT) and multireference quantum chemistry calculations reveal that the complex undergoes a spin‐state transition from a tetragonally elongated doublet state to a tetragonally compressed quartet state on the femtosecond timescale, i.e., it sustains ultrafast Jahn‐Teller (JT) photoswitching between two different spin multiplicities. Adding new Co‐based complexes as possible contenders in the search for JT photoswitching SIMs will greatly widen the possibilities for implementing magnetic multifunctionality and eventually controlling ultrafast magnetization with optical photons. Combined optical and X‐ray spectroscopy experiments complemented by theoretical calculations reveal the photoinduced Jahn‐Teller photoswitching between two spin multiplicities in a Co(II)‐based molecular complex, which occurs on the femtosecond timescale. Unveiling the associated transient magnetic anisotropy will assist the development of such systems into light‐driven multifunctional single‐ion magnets and qubits.
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Danish Council for Independent Research
Hungarian National Research, Development and Innovation Fund
USDOE Office of Science (SC)
AC02-06CH11357; CEX2020-001039-S; 2016/22/E/ST4/00543; 4002-00272; 8021-00347B; 7026-0037B; 2017-05337; DE‐AC02‐ 06CH11357; 77424
Ministry of Economic Affairs and Digital Transformation of Spain (MINECO)
Swedish Research Council (SRC)
USDOE
National Science Centre Poland (NCN)
ISSN:2198-3844
2198-3844
DOI:10.1002/advs.202206880