Spiral spin liquid in a frustrated honeycomb antiferromagnet: A single-crystal study of GdZnPO

Abstract: The frustrated honeycomb spin model can stabilize a subextensively degenerate spiral spin liquid with nontrivial topological excitations and defects, but its material realization remains rare. Here, we report the experimental realization of this model in the structurally disorder-free compound GdZnPO. Using a single-crystal sample, we find that spin-7/2 rare-earth Gd$^{3+}$ ions form a honeycomb lattice with dominant second-nearest-neighbor antiferromagnetic and first-nearest-neighbor ferromagnetic couplings, along with easy-plane single-site anisotropy. This frustrated model stabilizes a unique spiral spin liquid with a degenerate contour around the $\mathrm{K}$${$1/3,1/3$}$ point in reciprocal space, consistent with our experiments down to 30 mK, including the observation of a giant residual specific heat. Our results establish GdZnPO as an ideal platform for exploring the stability of spiral spin liquids and their novel properties, such as the emergence of low-energy topological defects on the sublattices.