Quantum spin liquid ground state with the evidence of roton-like excitations at elevated temperatures in the triangular-lattice delafossite YbCuSe$_2$

Abstract

We present a comprehensive experimental investigation of the temperature evolution of magnetic states in triangular-lattice delafossite YbCuSe$_2$. Magnetization measurements on high-quality single crystals reveal easy-plane anisotropy. Specific heat, magnetization, and muon spin relaxation ($μ$SR) establish the absence of magnetic order or spin freezing down to 0.03 K ($\leq J_{\mathrm{avg}}/250$), demonstrating a dynamically fluctuating quantum spin liquid (QSL) ground state. Thermodynamic measurements uncover multiple characteristic energy scales at $T_H \approx 4.5$ K, $T_L \approx 1.8$ K, and $T^* \approx 0.7$ K. Below $T^*$, $μ$SR detects a dynamical phase separation in which the majority of the spins are forming a QSL state whereas the remaining spins form a sporadic, disorder-induced state decoupled from the dominant QSL component. Remarkably, the unconventional temperature dependence of the $μ$SR relaxation rate indicates roton-like excitations emerging between $T_H$ and $T_L$, a feature not previously observed in any QSL system, preceding the stabilization of the low-temperature QSL at 0.3 K. These findings identify YbCuSe$_2$ as a unique QSL platform, providing valuable insights for further experimental and theoretical exploration.