Magnetic and crystal electric field studies in the rare-earth-based square lattice antiferromagnet NdKNaNbO$_5$

Abstract

The interplay of magnetic correlations, crystal electric field interactions, and spin-orbit coupling in low-dimensional frustrated magnets fosters novel ground states with unusual excitations. Here, we report the magnetic properties and crystal electric field (CEF) scheme of a rare-earth-based square-lattice antiferromagnet NdKNaNbO$_5$ investigated via magnetization, specific heat, electron spin resonance (ESR), and inelastic neutron scattering (INS) experiments. The low-temperature Curie-Weiss temperature $\theta_{\rm CW} \simeq -0.6$ K implies net antiferromagnetic interactions between the Nd$^{3+}$ ions. Two broad maxima are observed in the low temperature specific heat data in magnetic fields, indicating multilevel Schottky anomalies due to the effect of CEF. No magnetic long-range-order is detected down to 0.4 K. The CEF excitations of Kramers' ion Nd$^{3+}$ ($J=9/2$) probed via INS experiments evince dispersionless excitations characterizing the transitions among the CEF energy levels. The fit of the INS spectra enabled the mapping of the CEF Hamiltonian and the energy eigenvalues of the Kramers' doublets. The simulation using the obtained CEF parameters reproduces the broad maxima in specific heat in zero-field as well as in different applied fields. The significant contribution from $J_z = \pm 1/2$ state to the wave function of the ground state doublet indicates the role of strong quantum fluctuations at low temperatures. The magnetic ground state is found to be a Kramers' doublet with effective spin $J_{\rm eff} = 1/2$ at low temperatures.