Magnetic structure and crystal field states ofPr2Pd3Ge5:μSRand neutron scattering investigations

Abstract

We present the results of muon spin relaxation ($\ensuremath{\mu}\mathrm{SR}$), neutron powder diffration (NPD), and inelastic neutron scattering (INS) investigations on polycrystalline ${\mathrm{Pr}}_{2}{\mathrm{Pd}}_{3}{\mathrm{Ge}}_{5}$. The polycrystalline ${\mathrm{Pr}}_{2}{\mathrm{Pd}}_{3}{\mathrm{Ge}}_{5}$ is known to exhibit two antiferromagnetic transitions near ${T}_{\mathrm{N}1}=8.3$ K and ${T}_{\mathrm{N}2}=7.5$ K which is confirmed by the heat capacity measurements on the present sample. In the magnetically ordered state the NPD data show clear evidence for magnetic Bragg peaks, which for $T<{T}_{\mathrm{N}2}$ could be indexed with a propagation vector k = (1, 0, 0), and with k = (1, 0, 0.07) for ${T}_{\mathrm{N}2}<T<{T}_{\mathrm{N}1}$. We have determined the magnetic structure and found a canted antiferromagnetic structure of ordered ${\mathrm{Pr}}^{3+}$ moments. At 7.6 K we find an amplitude modulated incommensurate antiferromagnetic arrangement of ordered moments with a maximum ordered moment of 1.64(3) ${\ensuremath{\mu}}_{\mathrm{B}}$/Pr lying in the $ab$ plane tilted at about ${26}^{\ensuremath{\circ}}$ from the $b$ axis. At 1.8 K the antiferromagnetic structure is found to be commensurate with an ordered moment of 2.80(6) ${\ensuremath{\mu}}_{\mathrm{B}}$/Pr lying in the $ab$ plane tilted at about ${28}^{\ensuremath{\circ}}$ from the $b$ axis. Our zero-field $\ensuremath{\mu}\mathrm{SR}$ spectra at 1.5 K and at shorter time scale (below 0.5 $\ensuremath{\mu}\mathrm{s}$) reveal two oscillatory frequencies further supporting a long-range-ordered magnetic ground state. We have calculated the muon sites using the density functional theory calculation and present the results of internal field calculations at the muon stopping sites, which are in good agreement with the experimental observations. In the paramagnetic state, the INS data show three well defined CEF excitations near 8.0, 12.3, and 18.1 meV arising from the crystal electric field (CEF) split $J=4$ ground state of ${\mathrm{Pr}}^{3+}$. The CEF level scheme is deduced by analyzing the INS data by a model based on the CEF model.