Noncentrosymmetric Triangular Magnet CaMnTeO 6 : Strong Quantum Fluctuations and Role of s 0 versus s 2 Electronic States in Competing Exchange Interactions

Huai, Xudong; Acheampong, Emmanuel; Delles, Erich; Winiarski, Michał J.; Sorolla, II, Maurice; Nassar, Lila; Liang, Mingli; Ramette, Caleb; Ji, Huiwen; Scheie, Allen; Calder, Stuart; Mourigal, Martin; Tran, Thao T.

doi:10.1002/adma.202313763

Title: Noncentrosymmetric Triangular Magnet CaMnTeO ₆ : Strong Quantum Fluctuations and Role of s ⁰ versus s ² Electronic States in Competing Exchange Interactions

Journal Article · 26 March 2024 · Advanced Materials

DOI: https://doi.org/10.1002/adma.202313763 · OSTI ID:2329341

Huai, Xudong ^[1]; Acheampong, Emmanuel ^[1]; Delles, Erich ^[1]; Winiarski, Michał J. ^[2]; Sorolla, II, Maurice ^[3]; Nassar, Lila ^[4]; Liang, Mingli ^[5]; Ramette, Caleb ^[6]; Ji, Huiwen ^[6]; Scheie, Allen ^[7]; Calder, Stuart ^[8]; Mourigal, Martin ^[4];

^[1]

Department of Chemistry Clemson University Clemson SC 29634 USA
Applied Physics and Mathematics and Advanced Materials Center Gdansk University of Technology Gdansk 80‐233 Poland
Institute of Chemistry University of the Philippines Diliman Quezon City 1101 Philippines
School of Physics Georgia Institute of Technology Atlanta GA 30332 USA
Department of Chemistry University of Houston Houston TX 77204 USA
Department of Materials Science and Engineering University of Utah Salt Lake City UT 84112 USA
MPA‐Q Los Alamos National Laboratory Los Alamos NM 87545 USA, Neutron Scattering Division Oak Ridge National Laboratory Oak Ridge TN 37830 USA
Neutron Scattering Division Oak Ridge National Laboratory Oak Ridge TN 37830 USA

Abstract Noncentrosymmetric triangular magnets offer a unique platform for realizing strong quantum fluctuations. However, designing these quantum materials remains an open challenge attributable to a knowledge gap in the tunability of competing exchange interactions at the atomic level. Here, a new noncentrosymmetric triangular S = 3/2 magnet CaMnTeO ₆ is created based on careful chemical and physical considerations. The model material displays competing magnetic interactions and features nonlinear optical responses with the capability of generating coherent photons. The incommensurate magnetic ground state of CaMnTeO ₆ with an unusually large spin rotation angle of 127°(1) indicates that the anisotropic interlayer exchange is strong and competing with the isotropic interlayer Heisenberg interaction. The moment of 1.39(1) µB , extracted from low‐temperature heat capacity and neutron diffraction measurements, is only 46% of the expected value of the static moment 3 µB . This reduction indicates the presence of strong quantum fluctuations in the half‐integer spin S = 3/2 CaMnTeO ₆ magnet, which is rare. By comparing the spin‐polarized band structure, chemical bonding, and physical properties of AMnTeO ₆ ( A = Ca, Sr, Pb), how quantum‐chemical interpretation can illuminate insights into the fundamentals of magnetic exchange interactions, providing a powerful tool for modulating spin dynamics with atomically precise control is demonstrated.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2329341

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 24 Vol. 36; ISSN 0935-9648

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

Country of Publication:: Germany

Language:: English

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Title: Noncentrosymmetric Triangular Magnet CaMnTeO 6 : Strong Quantum Fluctuations and Role of s 0 versus s 2 Electronic States in Competing Exchange Interactions

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Title: Noncentrosymmetric Triangular Magnet CaMnTeO ₆ : Strong Quantum Fluctuations and Role of s ⁰ versus s ² Electronic States in Competing Exchange Interactions