Magnetic order in Nd₂PdSi₃ investigated using neutron scattering and muon spin relaxation

The rare-earth based ternary intermetallic compounds $R_2TX_3$ ($R$ = rare-earth, $T$ = transition-metal, $X$ = Si, Ge, Ga, In) have attracted considerable interest due to a wide range of interesting low temperature properties. Here we investigate the magnetic state of Nd$_{2}$PdSi$_{3}$ using neutron diffraction, muon spin relaxation ($\mu$SR) and inelastic neutron scattering (INS). This compound appears anomalous among the $R_{2}$PdSi$_{3}$ series, since it was proposed to order ferromagnetically, whereas others in this series are antiferromagnets. Although some members of the $R_2TX_3$ series have been reported to form ordered superstructures, our data are well described by Nd$_{2}$PdSi$_{3}$ adopting the AlB$_2$-type structure with a single Nd site, and we do not find evidence for superlattice peaks in neutron diffraction. Our results confirm the onset of long range magnetic order below $T_0=17$~K, where the whole sample enters the ordered state. Neutron diffraction measurements establish the presence of a ferromagnetic component in this compound, as well as an antiferromagnetic one which has a propagation vector $\mathbf{k_2}=(1/2,1/2,1/4-\delta)$ with a temperature dependent $\delta\approx0.02-0.04$, and moments orientated exclusively along the $c$-axis. $\mu$SR measurements suggest that these components coexist on a microscopic level, and therefore the magnetic structure of Nd$_{2}$PdSi$_{3}$ is predominantly ferromagnetic, with a sinusoidally modulated antiferromagnetic contribution which reaches a maximum amplitude at 11~K, and becomes smaller upon further decreasing the temperature. INS results show the presence of crystalline-electric field (CEF) excitations above $T_0$, and from our analysis we propose a CEF level scheme.