Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore

Abstract

A quantum spin liquid is a state of matter where unpaired electrons’ spins, although entangled, do not show magnetic order even at the zero temperature. The realization of a quantum spin liquid is a long-sought goal in condensed-matter physics. Although neutron scattering experiments on the two-dimensional spin-1/2 kagome lattice ZnCu3(OD)6Cl2 and triangular lattice YbMgGaO4 have found evidence for the hallmark of a quantum spin liquid at very low temperature (a continuum of magnetic excitations), the presence of magnetic and non-magnetic site chemical disorder complicates the interpretation of the data. Recently, the three-dimensional Ce3+ pyrochlore lattice Ce2Sn2O7 has been suggested as a clean, effective spin-1/2 quantum spin liquid candidate, but evidence of a spin excitation continuum is still missing. Here, we use thermodynamic, muon spin relaxation and neutron scattering experiments on single crystals of Ce2Zr2O7, a compound isostructural to Ce2Sn2O7, to demonstrate the absence of magnetic ordering and the presence of a spin excitation continuum at 35 mK. With no evidence of oxygen deficiency and magnetic/non-magnetic ion disorder seen by neutron diffraction and diffuse scattering measurements, Ce2Zr2O7 may be a three-dimensional pyrochlore lattice quantum spin liquid material with minimum magnetic and non-magnetic chemical disorder. A detailed neutron scattering and muon spin relaxation study uncovers a continuum of magnetic excitations down to 35 mK in the pyrochlore lattice compound Ce2Zr2O7 with minimum chemical disorder, consistent with quantum spin liquid behaviour.