The search for quantum spin liquids (QSL) and chemical doping in such materials to explore superconductivity have continuously attracted intense interest. Here, we report the discovery of a potential QSL candidate, pyrochlore-lattice β-NaYbO. Colorless and transparent NaYbO single crystals, layered α-NaYbO (∼250 μm on edge) and octahedral β-NaYbO (∼50 μm on edge), were grown for the first time. Synchrotron X-ray single-crystal diffraction unambiguously determined that the newfound β-NaYbO belongs to the three-dimensional pyrochlore structure characterized by the 3̅ space group, corroborated by synchrotron X-ray and neutron powder diffraction and pair distribution function. Magnetic measurements revealed no long-range magnetic order or spin glass behavior down to 0.4 K with a low boundary spin frustration factor of 17.5, suggesting a potential QSL ground state. Under high magnetic fields, the potential QSL state was broken and spins order. Our findings reveal that NaYbO is a fertile playground for studying novel quantum states.
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