Observation of long range magnetic ordering in pyrohafnate Nd2Hf2O7: A neutron diffraction study

TL;DR

This study reports the discovery of long-range antiferromagnetic order in Nd2Hf2O7, confirmed by neutron diffraction, with a unique all-in/all-out magnetic structure and evidence of strong quantum fluctuations.

Contribution

First observation of long-range magnetic ordering in pyrohafnate Nd2Hf2O7 using neutron diffraction, revealing an all-in/all-out antiferromagnetic structure with reduced magnetic moments.

Findings

Antiferromagnetic transition at T_N = 0.55 K

All-in/all-out magnetic structure confirmed by neutron diffraction

Ordered magnetic moment significantly reduced due to quantum fluctuations

Abstract

We have investigated the physical properties of a pyrochlore hafnate Nd2Hf2O7 using ac magnetic susceptibility \chi_ac(T), dc magnetic susceptibility \chi(T), isothermal magnetization M(H) and heat capacity C_p(T) measurements, and determined the magnetic ground state by neutron powder diffraction study. An upturn is observed below 6 K in C_p(T)/T, however both C_p(T) and \chi(T) do not show any clear anomaly down to 2 K. The \chi_ac(T) shows a well pronounced anomaly indicating an antiferromagnetic transition at T_N = 0.55 K. The long range antiferromagnetic ordering is confirmed by neutron diffraction. The refinement of neutron diffraction pattern reveals an all-in/all-out antiferromagnetic structure, where for successive tetrahedra, the four Nd3+ magnetic moments point alternatively all-into or all-out-of the tetrahedron, with an ordering wavevector k = (0, 0, 0) and an ordered state magnetic moment of m = 0.62(1) \mu_B/Nd at 0.1 K. The ordered moment is strongly reduced reflecting strong quantum fluctuations in ordered state.