Ultrafast Jahn-Teller Photoswitching in Cobalt Single-Ion Magnets
(2023) In Advanced Science 10(21).- Abstract
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... (More)
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.
(Less)
- author
- organization
- publishing date
- 2023-07-27
- type
- Contribution to journal
- publication status
- published
- subject
- keywords
- Jahn-Teller effect, photoswitching, single-ion-magnets, XFEL science
- in
- Advanced Science
- volume
- 10
- issue
- 21
- article number
- 2206880
- publisher
- John Wiley & Sons Inc.
- external identifiers
-
- pmid:37196414
- scopus:85159625158
- ISSN
- 2198-3844
- DOI
- 10.1002/advs.202206880
- language
- English
- LU publication?
- yes
- id
- cb0d92b8-6feb-4833-918f-4b154e51c9d7
- date added to LUP
- 2023-09-25 09:32:12
- date last changed
- 2024-04-19 01:34:50
@article{cb0d92b8-6feb-4833-918f-4b154e51c9d7,
abstract = {{<p>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)<sub>2</sub>]<sup>2+</sup> (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.</p>}},
author = {{Canton, Sophie E. and Biednov, Mykola and Pápai, Mátyás and Lima, Frederico A. and Choi, Tae Kyu and Otte, Florian and Jiang, Yifeng and Frankenberger, Paul and Knoll, Martin and Zalden, Peter and Gawelda, Wojciech and Rahaman, Ahibur and Møller, Klaus B. and Milne, Christopher and Gosztola, David J. and Zheng, Kaibo and Retegan, Marius and Khakhulin, Dmitry}},
issn = {{2198-3844}},
keywords = {{Jahn-Teller effect; photoswitching; single-ion-magnets; XFEL science}},
language = {{eng}},
month = {{07}},
number = {{21}},
publisher = {{John Wiley & Sons Inc.}},
series = {{Advanced Science}},
title = {{Ultrafast Jahn-Teller Photoswitching in Cobalt Single-Ion Magnets}},
url = {{http://dx.doi.org/10.1002/advs.202206880}},
doi = {{10.1002/advs.202206880}},
volume = {{10}},
year = {{2023}},
}