Effect of antifluorite layer on the magnetic order in Eu-based 1111 compounds, EuTAsF (T = Zn, Mn, and Fe). Issue 6 (24th January 2023)

• Record Type: Journal Article
• Authors: Plokhikh, Igor V.; Tsirlin, Alexander A.; Khalyavin, Dmitry D.; Fischer, Henry E.; Shevelkov, Andrei V.; Pfitzner, Arno
• Is Part Of: Physical chemistry chemical physics. Volume 25:Issue 6(2023)
• Page Start: 4862
• Page End: 4871
• Publication Date: 2023-01-24
• Subjects: Chemistry, Physical and theoretical -- Periodicals; 541.3
• DOI: 10.1039/d2cp04863a
• Languages: English
• ISSNs: 1463-9076

Abstract

Abstract : Neutron powder diffraction and DFT calculations explain the difference between magnetic structures in layered 1111-type compounds EuTAsF (T = Zn, Mn and Fe) depending on the properties (magnetism, metallicity) of the T-containing layer. Abstract : The 1111 compounds with an alternating sequence of fluorite and antifluorite layers serve as structural hosts for the vast family of Fe-based superconductors. Here, we use neutron powder diffraction and density-functional-theory (DFT) band-structure calculations to study magnetic order of Eu 2+ in the [EuF] + fluorite layers depending on the nature of the [TAs] − antifluorite layer that can be non-magnetic semiconducting (T = Zn), magnetic semiconducting (T = Mn), or magnetic metallic (T = Fe). Antiferromagnetic transitions at T N ∼ 2.4–3 K due to an ordering of the Eu 2+ magnetic moments were confirmed in all three EuTAsF compounds. Whereas in EuTAsF (T = Zn and Mn), the commensurate k 1 = (½ ½ 0) stripe order pattern with magnetic moments within the a – b plane is observed, the order in EuFeAsF is incommensurate with k = (0 0.961(1) ½) and represents a cycloid of Eu 2+ magnetic moments confined within the bc -plane. Additionally, the Mn 2+ sublattice in EuMnAsF features a robust G-type antiferromagnetic order that persists at least up to room temperature, with magnetic moments along the c -direction. Although DFT calculations suggest stripe antiferromagnetic order in the Fe-sublattice of EuFeAsF as the ground state, neutron diffraction reveals no evidence of long-range magnetic order associated with Fe. We show that the frustrating interplane interaction J 3 between the adjacent [EuF] + layers is comparable with in-plane J 1 – J 2 interactions already in the case of semiconducting fluorite layers [TAs] − (T = Zn and Mn) and becomes dominant in the case of the metallic [FeAs] − ones. The latter, along with a slight orthorhombic distortion, is proposed to be the origin of the incommensurate magnetic structure observed in EuFeAsF.