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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Veröffentlicht in:Advanced science Jg. 10; H. 21; S. e2206880 - n/a
Hauptverfasser: 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
Sprache:Englisch
Veröffentlicht: Germany John Wiley & Sons, Inc 01.07.2023
Wiley Open Access
Wiley
John Wiley and Sons Inc
Schlagworte:
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
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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. 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.
AbstractList 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.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.
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 display 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 SIM complex [Co(terpy)2]2+ (terpy = 2,2′:6′,2″-terpyridine) in solution phase. The combined measurements and their analysis supported by 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 photoswitching between two different spin multiplicities. Adding new Co-based complexes as possible contenders in the search for Jahn-Teller photoswitching SIMs will greatly widen the possibilities for implementing magnetic multifunctionality and eventually controlling ultrafast magnetisation with optical photons.
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.
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.
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.
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.
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) ] (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.
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.
Author Choi, Tae‐Kyu
Zalden, Peter
Otte, Florian
Retegan, Marius
Pápai, Mátyás
Gawelda, Wojciech
Biednov, Mykola
Rahaman, Ahibur
Gosztola, David J.
Khakhulin, Dmitry
Zheng, Kaibo
Milne, Christopher
Frankenberger, Paul
Knoll, Martin
Jiang, Yifeng
Lima, Frederico A.
Møller, Klaus B.
Canton, Sophie E.
AuthorAffiliation 8 Chemical Physics and NanoLund Lund University Box 124 Lund 22100 Sweden
2 Department of Chemistry Technical University of Denmark Kongens Lyngby DK‐2800 Denmark
5 Departamento de Química Universidad Autónoma de Madrid Madrid 28049 Spain
6 IMDEA‐Nanociencia Calle Faraday 9 Madrid 28049 Spain
4 XFEL Division Pohang Accelerator Laboratory Jigok‐ro 127‐80 Pohang 37673 Republic of Korea
10 European Synchrotron Radiation Facility 71 Avenue des Martyrs Grenoble 38000 France
9 Center for Nanoscale Materials Argonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA
3 Wigner Research Centre for Physics P.O. Box 49 Budapest H‐1525 Hungary
7 Faculty of Physics Adam Mickiewicz University Poznan 61‐614 Poland
1 European XFEL Holzkoppel 4 22869 Schenefeld Germany
AuthorAffiliation_xml – name: 1 European XFEL Holzkoppel 4 22869 Schenefeld Germany
– name: 2 Department of Chemistry Technical University of Denmark Kongens Lyngby DK‐2800 Denmark
– name: 9 Center for Nanoscale Materials Argonne National Laboratory 9700 South Cass Avenue Lemont IL 60439 USA
– name: 6 IMDEA‐Nanociencia Calle Faraday 9 Madrid 28049 Spain
– name: 7 Faculty of Physics Adam Mickiewicz University Poznan 61‐614 Poland
– name: 3 Wigner Research Centre for Physics P.O. Box 49 Budapest H‐1525 Hungary
– name: 4 XFEL Division Pohang Accelerator Laboratory Jigok‐ro 127‐80 Pohang 37673 Republic of Korea
– name: 8 Chemical Physics and NanoLund Lund University Box 124 Lund 22100 Sweden
– name: 5 Departamento de Química Universidad Autónoma de Madrid Madrid 28049 Spain
– name: 10 European Synchrotron Radiation Facility 71 Avenue des Martyrs Grenoble 38000 France
Author_xml – sequence: 1
  givenname: Sophie E.
  orcidid: 0000-0003-4337-8129
  surname: Canton
  fullname: Canton, Sophie E.
  email: sophie.canton@xfel.eu
  organization: Technical University of Denmark
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  givenname: Mátyás
  surname: Pápai
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  organization: Wigner Research Centre for Physics
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  givenname: Frederico A.
  surname: Lima
  fullname: Lima, Frederico A.
  organization: European XFEL
– sequence: 5
  givenname: Tae‐Kyu
  surname: Choi
  fullname: Choi, Tae‐Kyu
  organization: Pohang Accelerator Laboratory
– sequence: 6
  givenname: Florian
  surname: Otte
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  givenname: Yifeng
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  organization: European XFEL
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  fullname: Zalden, Peter
  organization: European XFEL
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  givenname: Wojciech
  surname: Gawelda
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  organization: Adam Mickiewicz University
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  givenname: Ahibur
  surname: Rahaman
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  organization: Lund University
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  givenname: Klaus B.
  surname: Møller
  fullname: Møller, Klaus B.
  organization: Technical University of Denmark
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  givenname: Christopher
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  givenname: David J.
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  givenname: Kaibo
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  givenname: Marius
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  fullname: Retegan, Marius
  organization: European Synchrotron Radiation Facility
– sequence: 18
  givenname: Dmitry
  surname: Khakhulin
  fullname: Khakhulin, Dmitry
  email: dmitry.khakhulin@xfel.eu
  organization: European XFEL
BackLink https://www.ncbi.nlm.nih.gov/pubmed/37196414$$D View this record in MEDLINE/PubMed
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https://www.osti.gov/biblio/1974081$$D View this record in Osti.gov
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CorporateAuthor Argonne National Laboratory (ANL), Argonne, IL (United States)
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Lunds universitets profilområden
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Faculty of Engineering, LTH
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Department of Chemistry
Strategiska forskningsområden (SFO)
NanoLund: Centre for Nanoscience
Enheten för fysikalisk och teoretisk kemi
Kemisk fysik
Lunds universitet
Profile areas and other strong research environments
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Lund University
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Strategic research areas (SRA)
Profilområden och andra starka forskningsmiljöer
LTH profilområde: Nanovetenskap och halvledarteknologi
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Keywords single-ion-magnets
photoswitching
Jahn-Teller effect
XFEL science
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Snippet Single‐ion magnets (SIMs) constitute the ultimate size limit in the quest for miniaturizing magnetic materials. Several bottlenecks currently hindering...
Single-ion magnets (SIMs) constitute the ultimate size limit in the quest for miniaturizing magnetic materials. Several bottlenecks currently hindering...
Abstract Single-ion magnets (SIMs) constitute the ultimate size limit in the quest for miniaturizing magnetic materials. Several bottlenecks currently...
Single–ion magnets (SIMs) constitute the ultimate size limit in the quest for miniaturizing magnetic materials. Several bottlenecks currently hindering...
Abstract Single‐ion magnets (SIMs) constitute the ultimate size limit in the quest for miniaturizing magnetic materials. Several bottlenecks currently...
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SubjectTerms 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
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Title Ultrafast Jahn‐Teller Photoswitching in Cobalt Single‐Ion Magnets
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