Abstract

The family of rare earth chalcogenides ARECh2ARECh_{2} (A = alkali or monovalent ions, RE = rare earth, and Ch = O, S, Se, and Te) appears as an inspiring playground for studying quantum spin liquids (QSL). The crucial low-energy spin dynamics remain to be uncovered. By employing muon spin relaxation (μμSR) and zero-field (ZF) AC susceptibility down to 50 mK, we are able to identify the gapless QSL in NaYbSe2NaYbSe_{2}, a representative member with an effective spin-1/2, and explore its unusual spin dynamics. The ZF μμSR experiments unambiguously rule out spin ordering or freezing in NaYbSe2NaYbSe_{2} down to 50 mK, two orders of magnitude smaller than the exchange coupling energies. The spin relaxation rate, λλ, approaches a constant below 0.3 K, indicating finite spin excitations featured by a gapless QSL ground state. This is consistently supported by our AC susceptibility measurements. The careful analysis of the longitudinal field (LF) μμSR spectra reveals a strong spatial correlation and a temporal correlation in the spin-disordered ground state, highlighting the unique feature of spin entanglement in the QSL state. The observations allow us to establish an experimental H-T phase diagram. The study offers insight into the rich and exotic magnetism of the rare earth family.

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