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Investigation of the magnetic structure and crystal field states of pyrochlore antiferromagnet Nd2Zr2O7

We present synchrotron x-ray diffraction, neutron powder diffraction and time-of-flight inelastic neutron scattering measurements on the rare earth pyrochlore oxide Nd2Zr2O7 to study the ordered state magnetic structure and cystal field states. The structural characterization by high-resolution synchrotron x-ray diffraction confirms that the pyrochlore structure has no detectable O vacancies or Nd/Zr site mixing. The neutron diffraction reveals long range all-in/all-out antiferromagnetic order below T_N ~ 0.4 K with propagation vector k = (0 0 0) and an ordered moment of 1.26(2) μ_B/Nd at 0.1 K. The ordered moment is much smaller than the estimated moment of 2.65 μ_B/Nd for the local <111> Ising ground state of Nd3+ (J=9/2) suggesting that the ordering is partially suppressed by quantum fluctuations. The strong Ising anisotropy is further confirmed by the inelastic neutron scattering data which reveals a well-isolated dipolar-octupolar type Kramers doublet ground state. The crystal field level scheme and ground state wavefunction have been determined.