Time differential perturbed angular correlation studies of hafnium hydrides

The dependence of the electric field gradients (EFG) in Hafnium-Hydride systems as a function of the composition H/Hf in the cubic δ and tetragonal ε phases were investigated using the time-dependent perturbed angular correlation (TDPAC) technique, with¹⁸¹Ta as the nuclear probe. Two EFGs were found in the ε phase, indicating the existence of two major symmetries surrounding the Ta probe. The results indicate that the trend of the EFGs, in the ε phase, are due to the changes in the lattice parametersa _o,c _o as hydrogen is added to the Hf-H system. In the δ phase, only one major symmetry was found. Both phases are characterized by broad frequency distributions and large anisotropies.     

Fe-Hydroxysulphates from Bacterial Fe2+ Oxidation

The perturbed angular correlation method (PAC) was applied to investigate the lattice location of implanted ¹¹¹In probe ions in Hf₂Ni and Zr₂Ni intermetallic compounds. It is concluded that the ¹¹¹In/¹¹¹Cd probe nuclei experiencing the highly asymmetric electric field gradient (EFG) occupy the unique hafnium or zirconium 8(h) sites in the investigated phases. Above room temperature, the EFGs decrease linearly with temperature. The results are compared with that of previous PAC measurements with ¹⁸¹Ta probes.     

Quadrupole interaction at Ta and lattice location of Hf in Be

The time-differential perturbed angular correlation technique (TDPAC) has been applied to the 482 keV excited state of¹⁸¹Ta, to determine the nuclear electric quadrupole interaction (QI) at Ta in Be. Sources were prepared by ion-implantation of¹⁸¹Hf in Be. Particle channeling measurements have revealed that. Hf impurities implanted in Be reside primarily at the tetrahedral interstitial site. The fundamental QI frequency obtained for Ta at this interstitial site in Be is |v _Q| =e ² qQ/h = 227.0 ± 2.2 MHz which corresponds to an electric field gradient |eq|=(3.71±0.15)×10¹⁷ V/cm². This result is discussed in terms of results for Cd impurities in the same system and the systematics of the impurity QI in metals.     

PAC Studies on Zr-Based Intermetallic Compounds

The Zr₂Al, Zr₃Al₂ and Zr₆NiAl₂ intermetallic compounds were characterized by means of time differential perturbed angular correlation (TDPAC) and X-ray diffraction. Our interest in these Zr(Hf) aluminides comes from crystallization studies of Zr(Hf)-based bulk metallic glasses which have a wide supercooled liquid region.     

The Nonanuclear [Mo(IV){(CN)Fe(III)(3-ethoxy-saldptn)}8]Cl4 Complex Compound Exhibits Multiple Spin Transitions Observed by Mössbauer Spectroscopy

The hyperfine interactions at ¹⁸¹Ta ions on Fe³⁺ sites in α-Fe₂O₃ (hematite) were studied in the temperature range 11–1100 K by means of the perturbed angular correlation (PAC) technique. The ¹⁸¹Hf(β⁻)¹⁸¹Ta probe nuclei were introduced chemically into the sample during the preparation. The hyperfine interaction measurements allow to observe the magnetic phase transition and to characterize the supertransferred hyperfine magnetic field B_hf and the electric field gradient (EFG) at the impurity sites. The angles between B_hf and the principal axes of the EFG were determined. The Morin transition was also observed. The results are compared with those of similar experiments carried out using ¹¹¹Cd probe. ^aAlso at Comisión de Investigaciones Científicas de la Provincia de Buenos Aires, Argentina.     

Magnetic and electric hyperfine interactions of181Ta implanted in thulium

The magnetic and electric hyperfine interaction at the site of dilute¹⁸¹Ta impurities in the rare earth metal Tm has been investigated as a function of temperature by TDPAC measurements. The samples were prepared by ion implantation of radioactive¹⁸¹Hf. In the paramagnetic phase between 100 K and 700 K the electric fieldgradient is a linear function of temperature: V_zz(T)=V_zz(O)·(1-A·T) with A=4.6·10^?4K^?1 and V_zz(293K)=6.4 (4)·10¹⁷v/cm². The TDPAC spectrum observed at 4.2 K reflects the 4 magnetically non-equivalent sites for an impurity in magnetically ordered Tm. The relative values and amplitudes of the corresponding 4 magnetic hyperfine fields are consistent with the predictions of the RKKY theory.     

Quadrupole interaction at111Cd in RRh3B2 compounds (R=Ce to Gd) and absence of transferred hyperfine field at111Cd in GdRh3B2

The quadrupole interaction at¹¹¹Cd in RRh₃B₂ compounds studied by the TDPAC technique supports the prediction that Ce in CeRh₃B₂ is not trivalent. The highly anisotropic EFG indicates that¹¹¹Cd in GdRh₃B₂ cannot occupy the rare earth site. The transferred magnetic hyperfine field at¹¹¹Cd is nearly zero which supports the conjecture that the impurity probe nuclei are at the 3g(Rh) site.     

TDPAC measurements on phase transition and hydrogen up-take in C15 laves phases

Intermetallic compounds with C15 structure are studied by TDPAC in the search for changes in the electric field gradient (EFG) on¹⁸¹Ta probes due to martensitic phase transition and hydrogen absorption. The residual low EFG of the cubic phase of HfV₂, ZrV₂ and Hf₅Zr₅V₂ is distinctly increased in the low temperature modification. Hydrogen does not affect the distribution of probe sites, but influences the features of the martensitic transition. In TaV₂ the sites with low EFG are split into an unperturbed and a strongly perturbed fraction.     

Electric field gradients in Hf2Fe

Perturbed Angular Correlations (PAC) technique was applied to measure the electric field gradients (EFG) at ¹⁸¹Ta sites in Hf₂Fe. The compound has the cubic structure of the Ti₂Ni prototype with two non‐equivalent crystallographic sites for Hf atoms. EFGs for the two sites were measured as a function of the temperature. In addition, one more EFG was observed, which was assigned to the presence of defects in the lattice. The ratio of the measured EFG at the regular lattice sites has been used to assign charges to the ions through a simple calculation using the point charge model and it is shown that the lattice symmetry can explain the very different EFG at both sites. This revised version was published online in August 2006 with corrections to the Cover Date.     

Site occupation of indium and jump frequencies of cadmium in FeGa<Subscript><Emphasis Type="Bold">3</Emphasis></Subscript>

Perturbed angular correlation (PAC) measurements using the In-111 probe were carried out on FeGa₃ as part of a broader investigation of indium site occupation and cadmium diffusion in intermetallic compounds. One PAC signal was observed with hyperfine parameters ω ₁= 513.8(1) Mrad/s and η= 0.939(2) at room temperature. By comparison with quadrupole frequencies observed in PAC measurements on isostructural RuIn₃, it was determined that indium occupies only the 8j site in the FeGa₃ structure, denoted Ga(2) below because two out of the three Ga sites have this point symmetry. PAC spectra at elevated temperature exhibited damping characteristic of electric field gradients (EFGs) that fluctuate as Cd probes jump among Ga(2) sites within the lifetime of the excited PAC level. A stochastic model for the EFG fluctuations based on four conceivable, single-step jump-pathways connecting one Ga(2) site to neighboring Ga(2) sites was developed and used to fit PAC spectra. The four pathways lead to two observable EFG reorientation rates, and these reorientation rates were found to be strongly dependent on EFG orientation. Calculations using density functional theory were used to reduce the number of unknowns in the model with respect to EFG orientation. This made it possible to determine with reasonable precision the total jump rate of Cd among Ga(2) sites that correspond to a change in mirror plane orientation of site-symmetry. This total jump rate was found to be thermally activated with an activation enthalpy of 1.8 ±0.1 eV.     

Electric and magnetic interaction in181TaTb measured with TDPAC

The temperature and pressure dependence of the combined magnetic and electric interaction of¹⁸¹Ta in Tb have been measured using the TDPAC method. At 20K the field is 27.6 T and the EFG 7.32 10¹⁷ V/cm². The antiferromagnetic phase is suppressed by the 0.5 wt% Hf and T_C is shifted to 236K. No pressure dependence is observed at 140K in contrast to that of the magnetization while at 208K we obtain dlnB/dP=–13 (2) Mbars–1 essentially due to the pressure dependence of T_C.     

Zr-doped rutile TiO2: a nuclear quadrupole interaction study

Role of Zr atom on the quadrupole interaction of ¹⁸¹Ta in rutile TiO₂ has been investigated by time differential perturbed angular correlation (TDPAC) study. The quadrupole frequency remains same as that in the pure rutile TiO₂ but its distribution increases with the amount of Zr. This indicates a metal-metal interaction between probe atom and Zr-atom in the nearest neighbour.     

Helium implanted CuHf as studied by TDPAC and positron lifetime measurements

¹⁸¹Ta time differential perturbed angular correlation (TDPAC) and positron lifetime measurements were carried out on homogeneously α-implanted CuHf samples. TDPAC measurements indicate the trapping of vacancy clusters and helium associated defect complexes by Hf atoms. The presence of helium-vacancy complexes and helium stabilised voids has been identified by positron lifetime measurements. Further the nucleation and growth stages of helium bubbles have been identified. TDPAC and positron lifetime measurements indicate that Hf atoms act as heterogeneous nucleating centers for helium bubbles. Hf atoms are found to suppress the bubble growth in CuHf as indicated by the results of positron lifetime measurements.     

Experimental and ab initio study of the nuclear quadrupole interaction of 181 Ta-probes in an α-Fe2O3 single crystal

We report perturbed-angular-correlation (PAC) experiments on ¹⁸¹Hf (→¹⁸¹Ta)-implanted corundum α-Fe₂O₃ single crystal in order to determine the magnitude, symmetry and orientation of the electric-field-gradient (EFG) tensor at Ta donor impurity sites of this semiconductor. These results are analyzed in the framework of ab initio full-potential augmented-plane wave plus local orbital (FP-APW+lo) calculations. This combined analysis enables us to quantify the magnitude of the lattice relaxations induced by the presence of the impurity and to determine the charge state of the impurity donor level introduced by Ta in the band gap of the semiconductor.     

Electric quadrupole interactions in the CdTiO3 perovskite2

The TDPAC technique has been used to measure the EFG at the Cd site in the perovskite CdTiO₃. The experimental results obtained at 293 K are compared with ionic lattice sum calculations of the EFG. In addition measurements at 16 and 77 K show that no considerable modification of the EFG is observed at the Cd site at temperatures below and above the previously described phase transition at 50 K.     

Influence of the local environment on the hyperfine interactions in Zr(Fe1-xCox)2 compounds

Ferromagnetic Laves phase compounds Zr(Fe_1-xCo_x)₂ have been investigated by means of the Mössbauer effect (⁵⁷Fe) and by the time-dependent perturbed angular correlation of \gamma -rays (¹⁸¹Ta) technique. It has been concluded from ME experiments that by exchange of Fe by Co in the nearest neighbour shell of the nuclear probe the hyperfine magnetic field acting on ⁵⁷Fe decreases by 10--12 kG. The analysis of the TDPAC experiments revealed that two different hyperfine magnetic fields: B₁ ^hf(Ta)~ 61 kG and B₂ ^hf(Ta)~ 88 kG act on the ¹⁸¹Ta nuclei. Both have a negative sign.     

The Electric Field Gradients in (Zr/Hf)Al3 and (Zr/Hf)2Al3 Intermetallic Compounds Studied by 181Ta- and 111Cd-PAC Spectroscopy

The electric quadrupole hyperfine interactions for ¹⁸¹Hf/¹⁸¹Ta and for ¹¹¹In/¹¹¹Cd probes in polycrystalline ZrAl₃ and Zr₂Al₃ compounds were measured in the temperature range 30–1100 K and compared with the results for isostructural hafnium aluminides. On the basis of the similarities of the numbers, sizes and asymmetries of electric field gradients, lattice site allocations were made. In all matrices, ¹⁸¹Hf/¹⁸¹Ta was found to substitute the Hf/Zr site. The ¹¹¹In/¹¹¹Cd impurities were also assigned to the Hf/Zr site in the compounds (Zr/Hf)Al₃, but appear to substitute the two non-equivalent Al sites in the Zr₂Al₃ and Hf₂Al₃ phases. This revised version was published online in September 2006 with corrections to the Cover Date.     

Hyperfine interactions in Zr(Fe1−x Al x )2 measured forx≤0.20 by TDPAC and Mössbauer spectroscopy

Mössbauer (⁵⁷Fe) and TDPAC spectroscopy (¹⁸¹Hf) have been used to study quasibinary compounds Zr(Fe_1?x Al _x )₂ forx≤0.20. It has been found that the dependence of the mean values of the hyperfine magnetic field, quadrupole splitting and isomer shift on the Al concentrationx is strong. The dependence of the hyperfine magnetic field on the number of Al atoms as nearest and next-nearest neighbours of⁵⁷Fe has been established. The TDPAC results also indicate a dependence of the hyperfine field on¹⁸¹Ta on Al concentration.     

Electric-field gradients at Ta donor impurities in Cr2O3(Ta) semiconductor

We report perturbed-angular-correlation (PAC) experiments on ¹⁸¹Hf(→¹⁸¹Ta)-implanted corundum Cr₂O₃ powder samples in order to determine the magnitude and symmetry of the electric-field gradient (EFG) tensor at Ta donor impurity sites of this semiconductor. These results are analyzed in the framework of ab initio full-potential augmented-plane wave plus local orbitals (FP−APW+lo) calculations. The results are also compared with EFG results coming from PAC experiments in isomorphous α-Al₂O₃ and α-Fe₂O₃ doped with ¹¹¹In→¹¹¹Cd and ¹⁸¹Hf→¹⁸¹Ta tracers. This combined analysis enables us to quantify the magnitude of the lattice relaxations induced by the presence of the impurity and to determine the charge state of the impurity donor level introduced by Ta in the band gap of the semiconductor.     

Characterization of nanostructured HfO2 films using Perturbed Angular Correlation (PAC) technique

The hyperfine field at ¹⁸¹Ta lattice sites in nanostructured HfO₂ thin films was studied by the Perturbed Angular Correlation (PAC) technique. Thin oxide films were deposited by Electron Beam Evaporation on a silicon substrate. The thickness of the films was ~100 nm and ~250 nm. Radioactive ¹⁸¹Hf nuclei were produced by neutron activation of the film samples in the Brazilian Research Reactor (IPEN IEA-R1) by the reaction ¹⁸⁰Hf(n,γ)¹⁸¹Hf. PAC measurements were carried out after annealing at 1473 K. The PAC technique allows the determination of the electric field gradient (EFG) at the probe sites.