Quantum Bi-stability and Robust Room-Temperature Spin Excitation in a Single-Ion Magnet

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Abstract The search for single-ion magnetism (SIM) has been largely focused on hybrid metal-organic systems. Here, we experimentally demonstrate the spin-relaxation mechanism of SIM in a pure inorganic transition-metal oxide, Sr2Ca2Mn2CoO9, an Ising-chain magnet, employing neutron diffraction and inelastic neutron scattering (INS), complemented by SpinW simulations and a machine-learning framework. Interestingly, SIM mechanism persists even in the presence of long-range magnetic ordering, a phenomenon that is rarely observed. This pioneering investigation shows that bistability between the two quantum states Ms=±3/2 is maintained at zero magnetic field, driven by a dominant Orbach spin-relaxation mechanism with an effective energy barrier, U=4.4 meV. This behaviour arises from strong spin-phonon coupling in the presence of negative axial anisotropy (D approx -2.2meV) and the high-spin state S=3/2 of the Co(II) ion. Furthermore, we observe that magnon excitations persist up to room temperature, reflecting low-dimensional magnetic interactions and extended magnetic correlations within the oxide lattice. This interplay between single-ion magnetism and room-temperature spin excitations underscores the chemical tunability of magnetic anisotropy in oxide lattices.
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Quantum Bi-stability and Robust Room-Temperature Spin Excitation in a Single-Ion Magnet | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Quantum Bi-stability and Robust Room-Temperature Spin Excitation in a Single-Ion Magnet Tathamay Basu, Gourrab Roy, Mohit Kumar, Jhuma Sannigrahi, Vincent Caignaert, and 5 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8591958/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract The search for single-ion magnetism (SIM) has been largely focused on hybrid metal-organic systems. Here, we experimentally demonstrate the spin-relaxation mechanism of SIM in a pure inorganic transition-metal oxide, Sr2Ca2Mn2CoO9, an Ising-chain magnet, employing neutron diffraction and inelastic neutron scattering (INS), complemented by SpinW simulations and a machine-learning framework. Interestingly, SIM mechanism persists even in the presence of long-range magnetic ordering, a phenomenon that is rarely observed. This pioneering investigation shows that bistability between the two quantum states Ms=±3/2 is maintained at zero magnetic field, driven by a dominant Orbach spin-relaxation mechanism with an effective energy barrier, U=4.4 meV. This behaviour arises from strong spin-phonon coupling in the presence of negative axial anisotropy (D approx -2.2meV) and the high-spin state S=3/2 of the Co(II) ion. Furthermore, we observe that magnon excitations persist up to room temperature, reflecting low-dimensional magnetic interactions and extended magnetic correlations within the oxide lattice. This interplay between single-ion magnetism and room-temperature spin excitations underscores the chemical tunability of magnetic anisotropy in oxide lattices. Physical sciences/Physics/Condensed-matter physics/Magnetic properties and materials Physical sciences/Materials science/Condensed-matter physics/Magnetic properties and materials Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SCMCOSI.pdf Quantum Bi-stability and Robust Room-Temperature Spin Excitation in a Single-Ion Magnet Cite Share Download PDF Status: Posted Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. 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