Mn Interstitials in Layered Mn1+xSb2-2/3xTe4: Structural Modification and Curie Temperature Boost

Research output: Contribution to journalResearch articleContributedpeer-review

Contributors

  • Ekaterina Kochetkova - , University of Amsterdam, Leibniz Institute for Solid State and Materials Research Dresden (Author)
  • Marie Tardieux - , University of Amsterdam (Author)
  • Manaswini Sahoo - , Clusters of Excellence ct.qmat: Complexity and Topology in Quantum Matter, Leibniz Institute for Solid State and Materials Research Dresden, University of Parma (Author)
  • Falk Pabst - , University of Amsterdam (Author)
  • Laura Folkers - , Leibniz Institute for Solid State and Materials Research Dresden, STOE & Cie (Author)
  • Anja U.B. Wolter - , Leibniz Institute for Solid State and Materials Research Dresden, Würzburg-Dresden Cluster of Excellence ct.qmat (Author)
  • Laura T. Corredor - , Leibniz Institute for Solid State and Materials Research Dresden, Dortmund University of Technology, Research Center Future Energy Materials and Systems (RC FEMS) (Author)
  • Irene Aguilera - , University of Amsterdam (Author)
  • Anna Isaeva - , University of Amsterdam, Leibniz Institute for Solid State and Materials Research Dresden, Dortmund University of Technology, Research Center Future Energy Materials and Systems (RC FEMS) (Author)

Abstract

Layered ternary (MnX2Te4)(X2Te3)n (X = Bi or Sb, n = 0-3) tellurides are intensely studied as perspective magnetic topological insulators: MnBi2Te4 and MnBi4Te7 demonstrate the quantum anomalous Hall effect up to several Kelvin. To enlarge the temperature range for this quantum behavior, the materials require a net magnetization and a high Curie temperature, TC. Recently, we found that Mn enrichment and Mn/Sb site intermixing increase the TC from 30 K in MnSb2Te4 to 58 K in Mn2.01(1)Sb1.19(1)Te4. Here, we synthesize the utmost manganese-rich members of this materials family, with an average Mn content of 28-32 at. % and the record TC = 65-73 K nearing the liquid-nitrogen threshold. By combining single-crystal X-ray diffraction, ab initio modeling and bulk DC magnetization, we pinpoint the relationship between the lattice symmetry and the magnetic order. The trigonal Mn1.90(1)Sb1.39(1)Te4 phase with manganese atoms in the van der Waals gap hosts the highest-TC ferrimagnetic state. We get the first insights into its electronic structure and topological nature by ab initio modeling using density functional theory. Initiated by the filling of the van der Waals gap, the compound mimics a structural transition from a trigonal (sp. gr. R3̅m) to a cubic lattice (sp. gr. Fm3̅m), which is reminiscent of the structural polymorphism of the Ge-Sb-Te thermoelectrics.

Details

Original languageEnglish
Pages (from-to)1446-1456
Number of pages11
JournalChemistry of materials
Volume37
Issue number4
Publication statusPublished - 25 Feb 2025
Peer-reviewedYes