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 CaMnTeO6 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 CaMnTeO6 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 CaMnTeO6 magnet, which is rare. By comparing the spin-polarized band structure, chemical bonding, and physical properties of AMnTeO6 (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.
| Original language | English |
|---|---|
| Article number | 2313763 |
| Journal | Advanced Materials |
| Volume | 36 |
| Issue number | 24 |
| DOIs | |
| State | Published - Jun 13 2024 |
Funding
The work at Clemson University was supported by the Arnold and Mabel Backman Foundation as a 2023 BYI grant to T.T.T. The neutron experiment at the Oak Ridge National Laboratory was in part funded by the National Science Foundation under award NSF‐OIA‐2227933. Participation of E.A. was supported by the NSF‐CHE‐2050042. The authors greatly appreciate the Halasyamani group for the SHG measurements. The research at Gdańsk University of Technology was supported by the National Science Centre (Poland) under the SONATA‐15 grant (UMO‐ 2019/35/D/ST5/03769). The work at the University of Utah was supported by an NSF Career Award (DMR‐2145832). A portion of this research used resources at the High Flux Isotope Reactor, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. Use of the Advanced Photon Source at the Argonne National Laboratory was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE‐AC02‐06CH11357. This manuscript was authored by UT‐Batelle, LLC, under contract DE‐AC05‐00OR22725 with the US Department of Energy (DOE). The US government retained and the publisher, by accepting the article for publication, acknowledged that the US government retained a nonexclusive, paid‐up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allowed others to do so, for US government purposes. DOE would provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe‐public‐access‐plan ). The work of L.N. and M.M. at G.T. (single‐crystal thermomagnetic measurements) was funded by the U.S. Department of Energy, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under Award DE‐SC‐0018660.
Keywords
- exchange interactions
- frustrated magnets
- noncentrosymmetric magnets
- quantum dynamics
- quantum fluctuations
- triangular spin-lattices