Orbital character of the spin-reorientation transition in TbMn6Sn6

S. X.M. Riberolles, Tyler J. Slade, R. L. Dally, P. M. Sarte, Bing Li, Tianxiong Han, H. Lane, C. Stock, H. Bhandari, N. J. Ghimire, D. L. Abernathy, P. C. Canfield, J. W. Lynn, B. G. Ueland, R. J. McQueeney

Research output: Contribution to journalArticlepeer-review

9 Scopus citations

Abstract

Ferromagnetic (FM) order in a two-dimensional kagome layer is predicted to generate a topological Chern insulator without an applied magnetic field. The Chern gap is largest when spin moments point perpendicular to the kagome layer, enabling the capability to switch topological transport properties, such as the quantum anomalous Hall effect, by controlling the spin orientation. In TbMn6Sn6, the uniaxial magnetic anisotropy of the Tb3+ ion is effective at generating the Chern state within the FM Mn kagome layers while a spin-reorientation (SR) transition to easy-plane order above TS R = 310 K provides a mechanism for switching. Here, we use inelastic neutron scattering to provide key insights into the fundamental nature of the SR transition. The observation of two Tb excitations, which are split by the magnetic anisotropy energy, indicates an effective two-state orbital character for the Tb ion, with a uniaxial ground state and an isotropic excited state. The simultaneous observation of both modes below TS R confirms that orbital fluctuations are slow on magnetic and electronic time scales < ps and act as a spatially-random orbital alloy. A thermally-driven critical concentration of isotropic Tb ions triggers the SR transition.

Original languageEnglish
Article number2658
JournalNature Communications
Volume14
Issue number1
DOIs
StatePublished - Dec 2023

Funding

The authors would like to acknowledge useful discussions and support from Liqin Ke, Igor Mazin, Allen Scheie, and Stephen Wilson. R.J.M., B.G.U., T.H., B.L., and S.X.M.R.’s work at the Ames Laboratory is supported by the U.S. Department of Energy (USDOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering. T.J.S. and P.C.C. are supported by the Center for the Advancement of Topological Semimetals (CATS), an Energy Frontier Research Center funded by the USDOE Office of Science, Office of Basic Energy Sciences, through the Ames National Laboratory. Ames National Laboratory is operated for the USDOE by Iowa State University under Contract No. DE-AC02-07CH11358. A portion of this research used resources at the Spallation Neutron Source, which is a USDOE Office of Science User Facility operated by the Oak Ridge National Laboratory. Crystal growth and properties characterization work at George Mason University was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science, and Engineering Division. The authors would like to acknowledge useful discussions and support from Liqin Ke, Igor Mazin, Allen Scheie, and Stephen Wilson. R.J.M., B.G.U., T.H., B.L., and S.X.M.R.’s work at the Ames Laboratory is supported by the U.S. Department of Energy (USDOE), Office of Basic Energy Sciences, Division of Materials Sciences and Engineering. T.J.S. and P.C.C. are supported by the Center for the Advancement of Topological Semimetals (CATS), an Energy Frontier Research Center funded by the USDOE Office of Science, Office of Basic Energy Sciences, through the Ames National Laboratory. Ames National Laboratory is operated for the USDOE by Iowa State University under Contract No. DE-AC02-07CH11358. A portion of this research used resources at the Spallation Neutron Source, which is a USDOE Office of Science User Facility operated by the Oak Ridge National Laboratory. Crystal growth and properties characterization work at George Mason University was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science, and Engineering Division.

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