Absence of Jahn−Teller transition in the hexagonal Ba 3 CuSb 2 O 9 single crystal

The quantum spin liquid state has been intensively pursued since Anderson proposed the resonating valence bond model. On the other hand, quantum liquids based on another electronic degree of freedom, orbital, has been believed unrealistic, because the energy scale of orbital correlation is normally one order of magnitude higher than spin exchange coupling, resulting in an orbital ordering at a signicantly high temperature accompanied by a cooperative Jahn−Teller (JT) distortion. In this paper, we present striking complete suppression of the JT transition in the copper oxide, 6 H -Ba 3 CuSb 2 O 9 based on comprehensive structural studies, indicating the realization of the novel “spin–orbital liquid” state. With decreasing temperature, liquids generally freeze into a solid state, losing entropy in the process. However, exceptions to this trend exist, such as quantum liquids, which may remain unfrozen down to absolute zero owing to strong quantum entanglement effects that stabilize a disordered state with zero entropy. Examples of such liquids include Bose−Einstein condensation of cold atoms, superconductivity, quantum Hall state of electron systems, and quantum spin liquid state in the frustrated magnets. Moreover, recent studies have clarified the possibility of another exotic quantum liquid state based on the spin–orbital entanglement in FeSc 2 S 4 . To confirm this exotic ground state, experiments based on single-crystalline samples are essential. However, no such single-crystal study has been reported to date. Here, we report, to our knowledge, the first single-crystal study on the spin–orbital liquid candidate, 6 H -Ba 3 CuSb 2 O 9 , and we have confirmed the absence of an orbital frozen state. In strongly correlated electron systems, orbital ordering usually appears at high temperatures in a process accompanied by a lattice deformation, called a static Jahn−Teller distortion. By combining synchrotron X-ray diffraction, electron spin resonance, Raman spectroscopy, and ultrasound measurements, we find that the static Jahn−Teller distortion is absent in the present material, which indicates that orbital ordering is suppressed down to the lowest temperatures measured. We discuss how such an unusual feature is realized with the help of spin degree of freedom, leading to a spin–orbital entangled quantum liquid state.