Abstract

A hidden order that emerges in the frustrated pyrochlore Tb2+x_{2+x}Ti2−x_{2-x}O7+y_{7+y} with Tc=0.53T_{\text{c}}=0.53 K is studied using specific heat, magnetization, and neutron scattering experiments on a high-quality single crystal. Semi-quantitative analyses based on a pseudospin-1/2 Hamiltonian for ionic non-Kramers magnetic doublets demonstrate that it is an ordered state of electric quadrupole moments. The elusive spin liquid state of the nominal Tb2_2Ti2_2O7_7 is most likely a U(1) quantum spin-liquid state.

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