Ultrafast Jahn‐Teller Photoswitching in Cobalt Single‐Ion Magnets

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

doi:10.1002/advs.202206880

Title: Ultrafast Jahn‐Teller Photoswitching in Cobalt Single‐Ion Magnets

Journal Article · 16 May 2023 · Advanced Science

DOI: https://doi.org/10.1002/advs.202206880 · OSTI ID:1974081

^[1]; Biednov, Mykola ^[2]; Pápai, Mátyás ^[3]; Lima, Frederico A. ^[2]; Choi, Tae‐Kyu ^[4]; Otte, Florian ^[2]; Jiang, Yifeng ^[2]; Frankenberger, Paul ^[2]; Knoll, Martin ^[2]; Zalden, Peter ^[2]; Gawelda, Wojciech ^[5]; Rahaman, Ahibur ^[6]; Møller, Klaus B. ^[7]; Milne, Christopher ^[2]; Gosztola, David J. ^[8]; Zheng, Kaibo ^[6]; Retegan, Marius ^[9]; Khakhulin, Dmitry ^[2]

European XFEL Holzkoppel 4 22869 Schenefeld Germany, Department of Chemistry Technical University of Denmark Kongens Lyngby DK‐2800 Denmark
European XFEL Holzkoppel 4 22869 Schenefeld Germany
Department of Chemistry Technical University of Denmark Kongens Lyngby DK‐2800 Denmark, Wigner Research Centre for Physics P.O. Box 49 Budapest H‐1525 Hungary
European XFEL Holzkoppel 4 22869 Schenefeld Germany, XFEL Division Pohang Accelerator Laboratory Jigok‐ro 127‐80 Pohang 37673 Republic of Korea
European XFEL Holzkoppel 4 22869 Schenefeld Germany, Departamento de Química Universidad Autónoma de Madrid Madrid 28049 Spain, IMDEA‐Nanociencia Calle Faraday 9 Madrid 28049 Spain, Faculty of Physics Adam Mickiewicz University Poznan 61‐614 Poland
Department of Chemistry Technical University of Denmark Kongens Lyngby DK‐2800 Denmark, Chemical Physics and NanoLund Lund University Box 124 Lund 22100 Sweden
Department of Chemistry Technical University of Denmark Kongens Lyngby DK‐2800 Denmark
Center for Nanoscale Materials Argonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA
European Synchrotron Radiation Facility 71 Avenue des Martyrs Grenoble 38000 France

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 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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Danish Council for Independent Research; Hungarian National Research, Development and Innovation Fund; MINECO; National Science Centre Poland (NCN); Swedish Research Council; USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1974081

Journal Information:: Advanced Science, Journal Name: Advanced Science Journal Issue: 21 Vol. 10; ISSN 2198-3844

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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