Coexistence of static order and spin dynamics in an S = 5/2 frustrated triangular antiferromagnet

Abstract

Frustrated triangular-lattice antiferromagnets in the classical high-spin limit provide a paradigmatic setting in which the interplay of competing exchange interactions, anisotropy, and collective degrees of freedom can lead to unconventional low-energy excitations, anomalous criticality, and persistent dynamical responses. Here, we present comprehensive thermodynamic, $\hat{I}¼$SR, and neutron diffraction experiments, along with first-principles calculations, on a triangular-lattice antiferromagnet, MnSnB${}_2$O${}_6$, where Mn${}^{2+}$ ($S=5/2$) moments form a nearly perfect 2D triangular network without any anti-site disorder. The Curie-Weiss fit to the magnetic susceptibility yields a moderate Curie-Weiss temperature of $-12$ K, indicating dominant antiferromagnetic interactions between Mn${}^{2+}$ moments, which is supported by first-principles calculations. Specific-heat measurements reveal the onset of long-range magnetic order at $T_{\mathrm{N}}\approx 1$ K, which is ascribed to intraplane exchange interactions. The specific heat exhibits pronounced short-range correlations above $T_{\mathrm{N}}$ and an unconventional power-law behavior, $C\propto T^{1.37}$, deep in the ordered state, suggesting the presence of non-trivial low-energy excitations. Zero-field $\hat{I}¼$SR experiments down to 50~mK confirm the presence of magnetic ordering below $T_{\mathrm{N}}$, in agreement with thermodynamic and neutron diffraction experiments. The $\hat{I}¼$SR measurements detect persistent spin dynamics coexisting with static magnetic order. The temperature evolution of the order parameter down to 50~mK from neutron diffraction suggests that the ordered state is consistent with a 3D Ising-like antiferromagnet. This family of archetypal frustrated magnets offers a promising venue for the experimental realization of emergent phenomena governed by competing exchange interactions and exotic low-energy excitations.