Interplay of short-range bond order and A-type antiferromagnetic order in metallic triangular lattice GdZn${}_3$P${}_3$

Abstract

We investigate a hexagonal ScAl${}_3$C${}_3$-type antiferromagnet GdZn${}_3$P${}_3$ single crystal. Compared with antiferromagnetic topological material EuM${}_2$X${}_2$ (M=Zn, Cd; X=P, As), the GdZn${}_3$P${}_3$ features an additional ZnP${}_3$ trigonal planar units. Notably, single-crystal X-ray diffraction analysis reveals that Zn and P atoms within trigonal planar layer exhibit significant anisotropic displacement parameters with a space group of P63/mmc. Meanwhile, scanning transmission electron microscopy experiment demonstrates the presence of interstitial P atoms above and below the ZnP honeycomb lattice, suggesting potential ZnP bond instability within the ZnP${}_3$ trigonal layers. Concerning the triangular Gd${}^{3+}$ layer, the magnetic susceptibility $\chi$$(T)$ and heat capacity measurements reveal long-range antiferromagnetic order at T${}_N$ = 4.5 K. Below T${}_N$, the in-plane $\chi$$(T)$ is nearly 4 times the $\chi$$(T)$ along $c$ axis, indicative of strong magnetic anisotropy. The Curie Weiss fitting to the low temperature $\chi$$(T)$ data reveals ferromagnetic interaction ($\theta$${}_{CW}$ = 5.2 K) in ab-plane, and antiferromagnetic interaction ($\theta$${}_{CW}$ = -1 K) along c axis, suggesting the ground state as an A-type antiferromagnetic order. Correspondingly, the density function theory calculation shows that GdZn${}_3$P${}_3$ is an indirect semiconductor with a band gap 0.27 eV, supported by the resistivity measurement on polycrystal sample. Interestingly, the GdZn${}_3$P${}_3$ single crystal exhibits metallic conductivity with an anomaly at T${}_N$, likely associated with the observation of interstitial P atoms mentioned above. Therefore, our results establish GdZn${}_3$P${}_3$ system as a concrete example for investigating the coupling between charge carrier and triangular lattice magnetism in the two-dimensional lattice framework, on the background of short-range bond order.

This manuscript contains 18 pages and 6 figures, with Supplemental Materials not included

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Cited by in corpus (1)

• Interleaved bond frustration in a triangular lattice antiferromagnet