Effect of quenched disorder on the quantum spin liquid state of the triangular-lattice antiferromagnet 1T−TaS_{2}

Abstract

A quantum spin liquid (QSL) is an exotic state of matter characterized by quantum entanglement and the absence of any broken symmetry. A longstanding open problem, which is key for fundamental understanding the mysterious QSL states, is how the quantum fluctuations respond to randomness due to quenched disorder. Transition metal dichalcogenide 1T−TaS_{2} is a candidate material that hosts a QSL ground state with spin-1/2 on the two-dimensional perfect triangular lattice. Here, we performed systematic studies of low-temperature heat capacity and thermal conductivity on pure, Se-substituted, and electron-irradiated crystals of 1T−TaS_{2}, where the substitution of S by Se induces weak disorder and electron irradiation induces strong quenched disorder. In pure 1T−TaS_{2}, the linear temperature term of the heat capacity γT and the finite residual linear term of the thermal conductivity in the zero-temperature limit κ_{0}/T≡κ/T(T→0) are clearly resolved, consistent with the presence of gapless spinons with a Fermi surface. Moreover, while the strong magnetic field slightly enhances κ_{0}/T, it strongly suppresses γ. These unusual contrasting responses to magnetic field imply the coexistence of two types of gapless excitations with itinerant and localized characters. Introduction of additional weak random exchange disorder in 1T−Ta(S_{1−x}Se_{x})_{2} leads to vanishing of κ_{0}/T, indicating that the itinerant gapless excitations are sensitive to the disorder. On the other hand, in both pure and Se-substituted systems, the magnetic contribution of the heat capacity obeys a universal scaling relation, which is consistent with a theory that assumes the presence of localized orphan spins forming random singlets. These results appear to capture an essential feature of the QSL state of 1T−TaS_{2}; localized orphan spins induced by disorder form random valence bonds and are surrounded by a QSL phase with spinon Fermi surface. Electron irradiation in pure 1T−TaS_{2} largely enhances γ and changes the scaling function dramatically, suggesting a possible new state of spin liquid.