Hyperfine interactions at R and In sites in RNiIn (R = Gd, Tb, Dy, Ho) compounds measured by perturbed angular correlation spectroscopy

Perturbed gamma–gamma angular correlation (PAC) technique was used to measure the magnetic hyperfine field (mhf) in RNiIn (R = Gd, Dy, Tb, Ho) intermetallic compounds using the ¹¹¹In→¹¹¹Cd and ¹⁴⁰La→¹⁴⁰Ce probe nuclei. The PAC spectra for ¹¹¹Cd measured above magnetic transition temperature show a major fraction with a well defined quadrupole interaction for all compounds except GdNiIn where a single frequency was observed. PAC measurements below T _C showed a combined electric quadrupole plus magnetic dipole interaction for ¹¹¹Cd probe at In sites, and a pure magnetic interaction for ¹⁴⁰Ce at R sites. The temperature dependence of mhf measured with ¹⁴⁰Ce at R sites shows that the values of fields drop to zero at temperatures around the expected T _C for each compound. However, in the measurements with ¹¹¹Cd at In sites, the mhf values become zero at temperatures which are smaller than T _C . The difference between the temperatures at which mhf is zero for ¹⁴⁰Ce and ¹¹¹Cd probes correlates with T _C . For each compound this difference decreases with T _C . The results are discussed in terms of the RKKY model for magnetic interactions and the existence of two magnetic systems, with distinct exchange interaction energies due to different types of atomic layers in these compounds.     

Study of Hyperfine Fields in CeIn3 by Electronic Structure Calculations

Electronic band structure calculations for the CeIn₃ compound utilizing the full potential linearized augmented plane waves method were performed with the aim to compute the hyperfine fields acting on Ce and In atoms. The latter are found to be in reasonable agreement with the values measured at low temperatures. The 4f orbital contribution dominates the magnetic hyperfine field at Ce ions while the contact field is negligible due to an almost complete cancellation of valence and core contributions. A non-zero magnetic hyperfine field appears at In sites due to the spin-polarization of the 5p sub-shells through the hybridization with the extended 6s, 6p and 5d Ce states which, in turn, are spin-polarized by the Ce 4f states. No net magnetic moment at In is observed since the sum of its 5p sub-shell spins is zero. The 5p shell of In is responsible for the presence of an electric field gradient at In nuclei. This revised version was published online in September 2006 with corrections to the Cover Date.     

Investigation of hyperfine interactions in RMO 3 (R = La, Nd; M = Cr, Fe) antiferromagnetic perovskite oxides using PAC spectroscopy

Because of its sensitivity to point defects atomically close to probe nuclei, it is reasonable to expect that perturbed angular correlation (PAC) spectroscopy has the potential to assist in the identification of diffusion mechanisms. It is of interest to characterize under what conditions diffusing defects are visible and how the defects affect relaxation in PAC spectra. This was investigated using a stochastic model to simulate PAC spectra for the special case of non-impurity PAC probes diffusing via a simple vacancy mechanism on the Cu-sublattice in Cu₃Au-structured compounds.     

Temperature dependence of electric field gradient in TbCoO3

The temperature dependence of the electric field gradient (efg) in TbCoO₃ perovskite was measured by perturbed angular correlation (PAC) technique using ¹¹¹Cd and¹⁸¹Ta nuclear probes. The radioactive parent nuclei ¹¹¹In and ¹⁸¹Hf were introduced into the compound through a chemical process during sample preparation. The electric quadrupole interactions at ¹¹¹Cd show two different sites, assigned to probe substituting Tb and Co atoms. The temperature dependence of quadrupole frequencies show sharp discontinuities which have been interpreted as thermally activated spin state transitions from low-spin ground state configuration to the intermediate-spin state and from intermediate-spin to high-spin state of Co^3?+? ion. For ¹⁸¹Ta only one interaction was observed, which was assigned to probe at Co site. Indication of a Jahn–Teller distortion, which stabilizes the intermediate-spin state with orbital ordering, is also pointed out. No magnetic order was observed till 77 K.     

Investigation of Hyperfine Interactions in GdNiIn Compound

Perturbed gamma–gamma angular correlation technique was used to measure the hyperfine interactions in the compound GdNiIn using the ¹¹¹InCd → and ¹⁴⁰La¹⁴⁰Ce probe nuclei at the In and Gd sites, respectively. A unique quadrupole frequency with asymmetry parameter η = 0.78 was observed for ¹¹¹Cd probe at In sites for the measurements above Curie temperature. Below T _C , the spectra for ¹¹¹Cd show combined magnetic dipole and electric quadrupole interaction. Below 85 K, a unique magnetic interaction is observed at ¹⁴⁰Ce. A linear relationship between the saturated magnetic hyperfine field and the magnetic transition temperature was observed for both probes, indicating that the main contribution to the mhf comes from the conduction electron polarization.     

Temperature Dependence of the Magnetic Hyperfine Field at 140Ce on Gd Sites in GdAg Compound

Perturbed gamma–gamma angular correlation technique was used to measure the magnetic hyperfine field at Gd sites in the intermetallic compound GdAg using the ¹⁴⁰La→¹⁴⁰Ce nuclear probe. A major and well-defined magnetic interaction is observed at ¹⁴⁰Ce substituting Gd sites in GdAg below 130 K, corresponding to a ferromagnetic ordering of Gd moments. The temperature dependence of magnetic hyperfine field, however, shows a sharp deviation from an expected Brillouin-like behavior for temperatures below 75 K. This additional magnetic interaction is believed to result from the polarization of Ce spin moments induced by the magnetic field from Gd atoms.     

Investigation of the Magnetic Hyperfine Field at 140Ce on Gd Sites in GdCo2 Compound

Perturbed angular correlation experiments on ¹⁴⁰La–¹⁴⁰Ce probes substituting for the Gd positions on GdCo2 demonstrate that the magnetic hyperfine field (MHF) on Ce atoms follows an expected Brillouin function but with a substantially reduced saturation value as compared with the MHF acting on free Ce⁺³ ions. The results were interpreted with the aid of first principles electronic structure calculations showing that the reduced value of the MHF is a consequence of a small orbital contribution to the MHF which was attributed to the de-localization of the Ce 4f electronic state.     

Measurement of Quadrupole Interactions in LaMO3 (M = Cr,Fe, Co) Perovskites by TDPAC

The perturbed angular correlation (PAC) technique has been used to study the electric field gradient (EFG) in LaCoO₃ perovskite. The results are compared with those for LaCrO₃, LaFeO₃ measured earlier. The PAC probe, ¹¹¹In → ¹¹¹Cd, was introduced in the oxide lattice by means of chemical reaction during sample preparation. In the present work, the temperature dependence of the electric quadrupole interaction parameters, for LaCoO₃ was investigated. The resulting systematics of EFG at ¹¹¹Cd, in La(Cr,Fe,Co)O₃ perovskites, reveals a linear dependence with temperature. This revised version was published online in September 2006 with corrections to the Cover Date.     

PAC Measurements on New Ferromagnetic Compound Pd2TiSn

Magnetic hyperfine field (mhf) acting on ¹⁸¹Ta at the Ti site has been investigated in the alloy Pd₂TiSn by Perturbed Angular Correlation (PAC) measurements using the (133–482) keV – cascade in ¹⁸¹Ta following the ^– decay of ¹⁸¹Hf. The magnetic hyperfine field was measured as a function of temperature in the range of 45–1000K. The magnetization measurements were carried out with a vibrating sample magnetometer. The interpretation of the experimental results is based on the assumption that the probe nuclei occupy both the regular Ti sites as well as the Ti atom sites randomly distributed on the Pd sublattice.