Discriminating ferrotoroidic from antiferrotoroidic ground states using a 3d quantum spin sensor

Abstract Molecular toroidal states have come to the forefront as candidates for next-generation quantum information devices owing to their bistability and protection from weak, short-range magnetic interactions. The protection offered by these non-magnetic vortex spin states proves to be a double-ed...

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Main Authors: Kieran Hymas, Alessandro Soncini, Kuduva R. Vignesh, Deepanshu Chauhan, Abinash Swain, Sophie L. Benjamin, Dipanti Borah, Maheswaran Shanmugam, Wolfgang Wernsdorfer, Gopalan Rajaraman, Stuart K. Langley, Keith S. Murray
Format: Article
Language:English
Published: Nature Portfolio 2024-12-01
Series:npj Quantum Materials
Online Access:https://doi.org/10.1038/s41535-024-00712-9
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author Kieran Hymas
Alessandro Soncini
Kuduva R. Vignesh
Deepanshu Chauhan
Abinash Swain
Sophie L. Benjamin
Dipanti Borah
Maheswaran Shanmugam
Wolfgang Wernsdorfer
Gopalan Rajaraman
Stuart K. Langley
Keith S. Murray
author_facet Kieran Hymas
Alessandro Soncini
Kuduva R. Vignesh
Deepanshu Chauhan
Abinash Swain
Sophie L. Benjamin
Dipanti Borah
Maheswaran Shanmugam
Wolfgang Wernsdorfer
Gopalan Rajaraman
Stuart K. Langley
Keith S. Murray
author_sort Kieran Hymas
collection DOAJ
description Abstract Molecular toroidal states have come to the forefront as candidates for next-generation quantum information devices owing to their bistability and protection from weak, short-range magnetic interactions. The protection offered by these non-magnetic vortex spin states proves to be a double-edged sword as inferring their existence in a molecular system has yet to be achieved through experimental means alone. Here, we investigate the anomalous, sickle-shaped, single-crystal magnetisation profile arising in μ-SQUID measurements of a novel CrDy3 molecule. Theoretical modelling supported by ab initio calculations demonstrates that the weak field CrDy3 spin dynamics is resultant from quantum superposition of the CrIII spin states determined by three competing interactions: (i) the alignment of the CrIII magnetic moment to the external magnetic field, (ii) the zero-field splitting of the CrIII ground quartet, and (iii) coupling to the remnant magnetisation of the toroidal ground state in the Dy3 triangle. If zero-field splitting of the central transition metal ion is quenched, it operates as a quantum spin sensor, which can be exploited to experimentally discriminate between ferrotoroidic and antiferrotoroidic ground states in MDy6 double triangle complexes through electron paramagnetic resonance experiments and single-crystal magnetisation measurements with a restricted field sweeping domain.
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spelling doaj-art-0f7cae24994b4f3395aa41c801db671c2025-01-05T12:07:50ZengNature Portfolionpj Quantum Materials2397-46482024-12-019111010.1038/s41535-024-00712-9Discriminating ferrotoroidic from antiferrotoroidic ground states using a 3d quantum spin sensorKieran Hymas0Alessandro Soncini1Kuduva R. Vignesh2Deepanshu Chauhan3Abinash Swain4Sophie L. Benjamin5Dipanti Borah6Maheswaran Shanmugam7Wolfgang Wernsdorfer8Gopalan Rajaraman9Stuart K. Langley10Keith S. Murray11Commonwealth Scientific and Industrial Research Organisation (CSIRO)Department of Chemical Sciences, University of PadovaDepartment of Chemical Sciences, Indian Institute of Science Education and Research (IISER) MohaliDepartment of Chemistry, Indian Institute of Technology BombayDepartment of Chemistry, Indian Institute of Technology BombaySchool of Science and Technology, Nottingham Trent UniversityDepartment of Chemistry, Indian Institute of Technology BombayDepartment of Chemistry, Indian Institute of Technology BombayInstitute of Quantum Materials and Technologies, Karlsruhe Institute of TechnologiesDepartment of Chemistry, Indian Institute of Technology BombayDepartment of Natural Sciences, Chemistry, Manchester Metropolitan UniversitySchool of Chemistry, Monash UniversityAbstract Molecular toroidal states have come to the forefront as candidates for next-generation quantum information devices owing to their bistability and protection from weak, short-range magnetic interactions. The protection offered by these non-magnetic vortex spin states proves to be a double-edged sword as inferring their existence in a molecular system has yet to be achieved through experimental means alone. Here, we investigate the anomalous, sickle-shaped, single-crystal magnetisation profile arising in μ-SQUID measurements of a novel CrDy3 molecule. Theoretical modelling supported by ab initio calculations demonstrates that the weak field CrDy3 spin dynamics is resultant from quantum superposition of the CrIII spin states determined by three competing interactions: (i) the alignment of the CrIII magnetic moment to the external magnetic field, (ii) the zero-field splitting of the CrIII ground quartet, and (iii) coupling to the remnant magnetisation of the toroidal ground state in the Dy3 triangle. If zero-field splitting of the central transition metal ion is quenched, it operates as a quantum spin sensor, which can be exploited to experimentally discriminate between ferrotoroidic and antiferrotoroidic ground states in MDy6 double triangle complexes through electron paramagnetic resonance experiments and single-crystal magnetisation measurements with a restricted field sweeping domain.https://doi.org/10.1038/s41535-024-00712-9
spellingShingle Kieran Hymas
Alessandro Soncini
Kuduva R. Vignesh
Deepanshu Chauhan
Abinash Swain
Sophie L. Benjamin
Dipanti Borah
Maheswaran Shanmugam
Wolfgang Wernsdorfer
Gopalan Rajaraman
Stuart K. Langley
Keith S. Murray
Discriminating ferrotoroidic from antiferrotoroidic ground states using a 3d quantum spin sensor
npj Quantum Materials
title Discriminating ferrotoroidic from antiferrotoroidic ground states using a 3d quantum spin sensor
title_full Discriminating ferrotoroidic from antiferrotoroidic ground states using a 3d quantum spin sensor
title_fullStr Discriminating ferrotoroidic from antiferrotoroidic ground states using a 3d quantum spin sensor
title_full_unstemmed Discriminating ferrotoroidic from antiferrotoroidic ground states using a 3d quantum spin sensor
title_short Discriminating ferrotoroidic from antiferrotoroidic ground states using a 3d quantum spin sensor
title_sort discriminating ferrotoroidic from antiferrotoroidic ground states using a 3d quantum spin sensor
url https://doi.org/10.1038/s41535-024-00712-9
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