A -type antiferromagnetic order in the Zintl-phase insulator EuZn2P2

Berry, Tanya; Stewart, Veronica J.; Redemann, Benjamin Y.; Lygouras, Chris; Varnava, Nicodemos; Vanderbilt, David; McQueen, Tyrel M.

doi:10.1103/physrevb.106.054420

A -type antiferromagnetic order in the Zintl-phase insulator EuZn2 P2

Journal Article · Wed Aug 17 00:00:00 EDT 2022 · Physical Review. B

DOI:https://doi.org/10.1103/physrevb.106.054420· OSTI ID:1979797

^[1]; Stewart, Veronica J. ^[2]; Redemann, Benjamin Y. ^[2]; Lygouras, Chris ^[2]; Varnava, Nicodemos ^[3]; Vanderbilt, David ^[3]; McQueen, Tyrel M. ^[2]

Johns Hopkins Univ., Baltimore, MD (United States); OSTI
Johns Hopkins Univ., Baltimore, MD (United States)
Rutgers Univ., Piscataway, NJ (United States)

Zintl phases, containing strongly covalently bonded frameworks with separate ionically bonded ions, have emerged as a critical materials family in which to couple magnetism and strong spin-orbit coupling to drive diverse topological phases of matter. Here we report the single-crystal synthesis, magnetic, thermodynamic, transport, and theoretical properties of the Zintl compound EuZn₂P₂ that crystallizes in the anti-La₂O₃ (CaAl₂Si₂) P-3m1 structure, containing triangular layers of Eu²⁺ ions. In-plane resistivity measurements reveal insulating behavior with an estimated activation energy of E_g = 0.11eV. Specific heat and magnetization measurements indicate antiferromagnetic ordering at T_N = 23K. Curie-Weiss analysis of in-plane and out of plane magnetic susceptibility from T = 150 to 300 K yields p_eff = 8.61 for μ₀H⊥c and p_eff = 7.74 for μ₀H//c, close to the expected values for the 4f⁷ J = S = 7/2 Eu²⁺ ion and indicative of weak anisotropy. Below T_N, a significant anisotropy of χ_⊥/χ_// ≈ 2.3 develops, consistent with A-type magnetic order as observed in isostructural analogs and as predicted by the density functional theory calculations reported herein. The positive Weiss temperatures of θ_W=19.2K for μ₀H⊥c and θ_W=41.9K for μ₀H//c show a similar anisotropy and suggest competing ferromagnetic and antiferromagnetic interactions. Comparing Eu magnetic ordering temperatures across trigonal EuM₂X₂ (M= divalent metal, X= pnictide) shows that EuZn₂P₂ exhibits the highest ordering temperature, with variations in T_N correlating with changes in expected dipolar interaction strengths within and between layers and independent of the magnitude of electrical conductivity. These results provide experimental validation of the crystochemical intuition that the cation Eu²⁺ layers and the anionic (M₂X₂)^2– framework can be treated as electronically distinct subunits, enabling further predictive materials design.

View Accepted Manuscript (DOE)

Research Organization:: Johns Hopkins Univ., Baltimore, MD (United States)

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

Grant/Contract Number:: SC0019331

OSTI ID:: 1979797

Alternate ID(s):: OSTI ID: 1882022

Journal Information:: Physical Review. B, Journal Name: Physical Review. B Journal Issue: 5 Vol. 106; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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