Spiral Spin Liquid in a Frustrated Honeycomb Antiferromagnet: A Single-Crystal Study of GdZnPO

Phys Rev Lett. 2024 Dec 6;133(23):236704. doi: 10.1103/PhysRevLett.133.236704.

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 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.