Magnetic and crystal electric field excitations in a spin-orbit coupled frustrated hyperkagome magnet Nd$_3$Li$_3$W$_2$O$_{12}$

Abstract

Rare-earth based garnets provide a viable platform for studying the frustrated driven magnetic properties of the hyperkagome lattices. Herein, we report a comprehensive study of the magnetic properties and crystal electric field (CEF) scheme of a new Nd$^{3+}$ based hyperkagome antiferromagnet, Nd$_3$Li$_3$W$_2$O$_{12}$ belonging to the garnet family via magnetization, heat capacity, and inelastic neutron scattering (INS) measurements. Magnetization measurement reveals a dominant antiferromagnetic interaction with a low temperature Curie-Weiss temperature $θ_{\rm CW}^{\rm LT} \simeq -0.2$ K. Two broad maxima are observed in the magnetic heat capacity data under magnetic fields, implying multilevel Schottky anomalies due to the effect of CEF and display a two-step magnetic entropy release. No magnetic long-range order is observed down to 0.1 K. The CEF excitations of the Nd$^{3+}$ ($J=9/2$) ion with $D_2$ point group symmetry, probed via INS experiments, show non-dispersive excitations characterizing the transitions among the CEF energy levels. The simultaneous fit of the INS spectra at different temperatures enabled the mapping of the CEF Hamiltonian and the energy eigenvalues of the Kramers' doublets. The simulation using the obtained CEF parameters reproduces the experimental magnetic susceptibility, magnetic isotherms, and magnetic heat capacity data. The thermodynamic properties and INS-derived crystal-field scheme confirm a Kramers' doublet ground state with an effective spin $J_{\rm eff} = 1/2$ at low temperatures.