Structural lattice defects in silicon observed at111in by perturbed angular correlation

Probing of structural defects in silicon by the perturbed γγ angular correlation (PAC) technique is demonstrated between 77 K and 1300 K. The behaviour of radioactive¹¹¹ In probe atoms implanted at 295 K, is monitored during isochronal annealing in n-type, p-type and intrinsic Si. Trapping of defects, produced by the¹¹¹In implantation itself or by postirradiation is studied in P-doped crystals (10¹⁶/cm³-10¹⁷/cm³).     

Laser surface-melting of metals studied by PAC

High purity Pt, Ni, Cu, Fe and Al metal foils were electroplated with carrier-free¹¹¹In probe atoms and melted at 293 K using 32 ns ruby laser pulses with energy densities in the range 1–10 J cm⁻². Three distinct lattice locations of the probe atoms were detected in the melted surface layers using perturbed γ-γ angular correlation spectroscopy: (i) defect-free substitutional sites, (ii) non-unique sites with broad distributions of quadrupole interactions, and (iii) a probemonovacancy complex (for Pt only). The defect-free fraction was found to approach 100% when Pt is irradiated at 9 J cm⁻². The fraction of probes on defect-free sites was found to increase with the energy density of the pulse and with the solubility of In in the metals. The data are consistent with the idea that laser surface-melting produces high concentrations of vacancies and lattice sinks, although no thermal trapping of point defects was detected. Supported in part by National Science Foundation grant DMR 86-19688 (Metallurgy Program).     

PAC investigations of Au(110) 1×2-surfaces

Au(110) surfaces with (1×2)-reconstruction have been investigated using perturbed -angular correlation (PAC) spectroscopy. From the two observed electric-field-gradient tensors at¹¹¹In probe atoms, deposited at room temperature in a concentration of about 10^–4 ML, the occupation of substitutional sites in the densely-packed rows along [110]-directions and ninefold coordinated sites within the (111)-oriented microfacets, respectively, can be concluded. Annealing to about 600 K leads to bulk migration of the In atoms, detected by an increase of probe atoms with cubic surroundings. Due to this behaviour the order-disorder transitions of these surfaces occurring atT _c=649 K cannot be detected in our PAC experiments.     

Stacking fault defects in hep cobalt studied by PAC

A study was made of lattice defects in hep Co metal using the technique of perturbed γ-γ angular correlations. Lattice sites of¹¹¹Cd impurities were characterized by their nuclear magnetic dipole and electric quadrupole interaction frequencies, respectively ω_L and ω_O. The signal for defect-free substitutional Cd impurities was found to have collinear interactions at 77K, with ω_L=438 Mrad/s and ω_O=7 Mrad/s. Analysis of measurements after heavy deformation at 100 K and after annealings up to 700 K gave little evidence of thermal trapping of point defects. However, in all spectral measured after deformation, a highly stable defect site with ω_L=418 and ω_O Mrad/s, and showing collinear interactions, was also observed. It is attributed to a¹¹¹Cd probe in a stacking fault (SF). Assuming a random distribution of proble atoms and SF's, a SF density of 20% was estimated.     

Hyperfine Interactions in CeT2Ge2 (T = Mn,Co) Heavy Fermions Compounds Measured by TDPAC

Time Differential Perturbed γ–γ Angular Correlation (TDPAC) technique was used to measure the magnetic hyperfine field at both Ge and Ce sites in CeMn₂Ge₂ and CeCo₂Ge₂ intermetallic compounds. The ¹¹¹In (¹¹¹Cd) probe nuclei was used to investigate the hyperfine interaction at Ge sites, while the ¹⁴⁰La (¹⁴⁰Ce) nuclei was used to measure the magnetic hyperfine field at Ce site. The present measurements cover the temperature ranges from 10–460 K for CeMn₂Ge₂ and 9–295 K for CeCo₂Ge₂, respectively. The result for ¹¹¹Cd probe showed two distinct electric quadrupole frequencies above magnetic transition temperatures, in both compounds and a combined interaction in the magnetic region. The temperature dependence of the magnetic hyperfine field at ¹¹¹Cd at Mn site for the CeMn₂Ge₂ compound showed a transition from ferromagnetic to antiferromagnetic phase around 320 K and from antiferromagnetic to paramagnetic phase at 420 K. While a small magnetic field was measured on ¹¹¹Cd at Co site, no magnetic field on ¹⁴⁰Ce site was observed in CeCo₂Ge₂. This revised version was published online in September 2006 with corrections to the Cover Date.     

Cavities in silicon investigated with the PAC-probe 111In

The perturbed angular correlation technique (PAC) was used to study the creation and development of He-induced cavities. In order to investigate the interaction of Indium atoms with cavities in Silicon the Bonn isotope separator was used to implant overlapping profiles of He (10 keV) and radioactive ¹¹¹In (160 keV) into undoped FZ-silicon. To get insight into the cavity formation mechanism samples were prepared with various He-doses (0.6, 2 and 6× 10¹⁶ ions/cm²). The samples were measured directly after implantation and after different annealing steps (t_hold= 10 min, T = 500–1100oC). Further, different implantation and annealing sequences were used. At higher He doses (2 and 6× 10¹⁶ ions/cm²) we find a large fraction of ¹¹¹In probe atoms subjected to an electric field gradient (EFG) corresponding to a quadrupole interaction frequency (QIF) of ν_Q= 411(6) MHz with η= 0.25(4). The corresponding defect configuration is formed most effectively after He implantation into annealed, ¹¹¹In doped Si. This and the affinity of In to vacancies leads us to the assumption that, similarly to the situation in metals, the Indium atoms act as nucleation centres for vacancy clusters (cavities) and are situated on the inner walls of the cavities. This revised version was published online in August 2006 with corrections to the Cover Date.     

High Pressure Mössbauer Studies on FCC Fe53Ni47 Alloy

Perturbed angular correlation measurements of the hyperfine interaction of ¹¹¹In in sapphire show, that after implantation and annealing at 1000°C, the fraction of undisturbed probe atoms exhibiting a unique quadrupole interaction with ν _Q = 219(1) MHz (η = 0) varies between 50% at 4 K, 5% at 100 K and 80% at 973 K in a reversible manner. A possible explanation for this surprising behaviour is the influence of so-called ‘after effects’ following the EC-decay of ¹¹¹In to ¹¹¹Cd. Immediately after the decay the ¹¹¹Cd is in an ionized state, then collects electrons from its surroundings and reaches the ground state. The different electronic configurations that arise during this relaxation process affect the amplitude (f _u) and the damping (δ _u) of the unique quadrupole interaction.     

Perturbed γ−γ angular correlations: A spectroscopy for point defects in metals and alloys

Atomic defects which migrate and trap at impurity probe atoms can be labelled by the changes they induce in the hyperfine interactions of the probe nuclei. Many studies have been made using perturbed γ−γ angular correlations (PAC) and the¹¹¹In probe because of the excellent resolution of different sites. Identification of the bound states is the key problem in applying hyperfine interactions methods to point defects studies. In this study three structure-sensitive methods are applied to help identify the atomic structures of various multivacancy complexes in Pt and Au: (1) Quadrupole interaction parameters are compared with results of point-charge calculations of electric-field gradients for 20 structures containing 1–4 vacancies in the fcc lattice. (2) Hyperfine interactions induced by decorating vacancy complexes with hydrogen atoms are measured and interpreted with the assistance of point-charge calculations. (3) Transformations between complexes observed by annihilation of vacancies by mobile self-interstitials are used to test the consistency of the identifications. Using these methods in conjunction with analysis of the trapping behavior which occurs during annealing of damaged samples, structural models are presented for divacancy (2V), 3V and 4V complexes in Pt, and 3V and 4V complexes in Au. The activation temperatures of the 3V defect in Au and Pt are determined to be 162 K and 390 K, respectively, and activation temperatures of defects in Ni, Cu, Pt and Au are compared. For Pt, trapping of H at 1V and 2V complexes is observed to lead to small changes in the quadrupole interactions, consistent with well shielded protonic charges. However, trapping at 3V and 4V complexes leads to very large changes which we attribute to atomic restructuring to the defect complexes. Finally, the application of the same methodology to interpret recent experiments on NiAl, an ordered alloy, is described.     

Shape coexistence near the double-midshell nucleus 111Rh

The decay of ¹¹¹Ru obtained from fast on-line chemical and mass separation has been investigated by β-γ-t and γ-γ coincidence techniques. Earlier spin and parity assignments of ¹¹¹Rh levels based on extrapolations of level systematics are confirmed. In particular, the K=1/2 intruder band is supported by the hindrance of E2 transitions between deformed and spherical states and enhancement of intraband E2 transitions. The excitation energies of intruder band members in Rh isotopes show a minimum at ¹⁰⁹Rh₆₄, with two neutrons less than ¹¹¹Rh at the N=66 midshell. This trend, which differs from the one in the higher-Z neighbouring elements Ag and Cd with minima at N=66, follows the evolution of deformation observed in the lower-Z elements Ru and Mo. Received: 25 June 1997 / Revised version: 10 September 1997     

Indium solubility in iron studied with perturbed angular correlations

Segregation of In in Fe-based alloys containing 0.11–2.12 at.% In has been studied by measuring the perturbed angular correlations of γ-rays emitted in the nuclear decay of ¹¹¹In. The probe atoms were introduced into the alloys by either adding the carrier-free ¹¹¹In during melting or via ion implantation. Ageing of the samples at elevated temperatures followed by a slow cooling to room temperature allowed us to determine the upper limit of the solubility at room temperature, S(300 K)≤ 30 at. ppm. This value is far below the one reported in the published phase diagram. Quenching of the samples in water from 973–1373 K resulted in the determination of the indium solubility in iron at these elevated temperatures. This revised version was published online in August 2006 with corrections to the Cover Date.     

Measurements of the electric field gradient at cadmium in the high Tc superconductor YBa2Cu3O6+x

The electric field gradient (EFG) at¹¹¹Cd probe atoms in YBa₂Cu₃O_6+x has been studied by the perturbed angular correlation (PAC) spectroscopy. After annealing at temperatures below 1000 K the probe atoms are located at the Cu(1) site; above 1100 K they preferentially occupy the Y site, whereas in the intermediate temperature range they also reside on the Ba site. A reduction of the oxygen content from x=1.0 to 0.2 resulted in a decrease of the asymmetry parameter measured at the Ba site, but in an increase of it at the Y site, indicating there a local distortion of the YBa₂Cu₃O_6+x lattice by the Cd impurity. Two different surroundings for the Cd atoms at the Cu(1) site were observed.     

Defect trapping by100Pd in fcc metals

Lattice defects in Al, Cu, Ag and Au were studied by the perturbed angular correlation technique (PAC) using the probe atom¹⁰⁰Pd/¹⁰⁰Rh. The comparison of data obtained on interstitial trapping in Cu and Au at different probe atoms (¹⁰⁰pd,¹¹¹In) allows defect characterisation less affected by the respective probe. The trapping efficiency of¹⁰⁰Pd for vacancy like defects is quite different to that of¹¹¹In atoms.     

Electric field gradient at111In on Cu (100) surfaces and its utilization for indium surface diffusion

The electric field gradient at¹¹¹In probe atoms on Cu (100) surfaces was studied. At clean surfaces all probes are exposed to a well-defined surface field gradient. This is used to investigate indium surface diffusion, where the applied PAC method allows to observe diffusion steps on an atomistic scale. The jump rate for indium on Cu (100) was found to be in the order of 10^–3 Hz at 200 K.     

Cavity formation at indium impurities in bcc metals

The defect formation in the bcc metals W and Mo above annealing stage III and the influence of rare gases on this process were investigated by means of the perturbed angular correlation technique using¹¹¹In as radioactive probe. In both metals a relatively high electric field gradient (EFG) could be observed at the indium site, characterized by the quadrupole interaction frequencies υ_Q=263 MHz, ν=0 and υ_Q=220 MHz, ν≈0.15 for W and Mo, respectively. The observations are assigned to the growth of threedimensional vacancy clusters at the probe atoms with the indium atoms situated in the inner surface of this cavities, thus experiencing the corresponding surface EFG.     

Feasibilities of nuclear techniques for the study of molecular defects in metals and semiconductors

Nuclear techniques, like Mössbauer effect and perturbed γγ angular correlation spectroscopy (PAC), have proven themselves to be sensitive tools for labelling and identifying probe atom-defect complexes. In these experiments, the “molecular defect” is investigated via the nuclear hyperfine interaction, which is measured at the site of the radioactive probe atom. Here, we shall put the emphasis on the PAC spectroscopy, which often uses¹¹¹In/¹¹¹Cd as radioactive probe atom. In metals, based on the identification of simple probe atom-defect pairs, the agglomeration of defects after cold-working and the interaction of vacancies with He atoms will be discussed. In semiconductors, it will be focussed on the interaction between dopant atoms, which strongly determines the electrical properties of these materials.     

Influence of x irradiation on internal friction in silicon

An investigation was made of the influence of γ irradiation on the temperature dependences of internal friction in disk-shaped silicon substrates in the kilohertz frequency range. After exposure to doses of 10⁴ and 10⁵ R, two dominant internal friction peaks were observed at ∼330 and ∼450 K with activation energies H ₁=0.6 eV and H ₂=0.9 eV, respectively. These peaks were evidently caused by reorientation of interstitial silicon atoms in dumbbell configurations. Fiz. Tverd. Tela (St. Petersburg) 40, 1257–1258 (July 1998)     

Phase transitions in the SrHfO3 perovskite measured with 111In/111Cd PAC

The temperature dependence of the hyperfine parameters in SrHfO₃ powder samples has been investigated by means of Perturbed Angular Correlation spectroscopy using implanted ¹¹¹In probes. Three quadrupole interactions have been established, with the largest fraction showing a pronounced dynamic interaction. We assign this fraction to ¹¹¹In / ¹¹¹Cd probe atoms on substitutional Hf sites. The temperature dependence of the dynamic interaction has been associated to the Pnma↔Imma phase transition at ∼700 K. We discuss the results in relation to those obtained for ¹⁸¹Hf / ¹¹¹Ta-probes in AHfO₃ (A=Ba, Sr, Ca) and for ¹¹¹In / ¹¹¹Cd-probes in PbZrO₃ and BaTiO₃. This revised version was published online in August 2006 with corrections to the Cover Date.     

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.     

Ionic and electronic transport in In2S3 studied via perturbed angular correlation spectroscopy

We report on Perturbed Angular Correlation measurements in polycrystalline In₂S₃ samples in the temperature range from 8 K to 1000 K where two different crystallographic phases β and α occur. As probes, implanted ¹¹¹In nuclei have been used. The three observed EFGs are attributed to probes residing substitutionally in the different sulfur-octahedra and -tetrahedra of β-In₂S₃. A strong damping between 150 K and 300 K has been attributed to EFG fluctuations following the ¹¹¹In(EC)¹¹¹Cd decay. The α-phase (above 680 K) is characterized by a different dynamical damping of the perturbation functions, caused by mobile In atoms. Therefore, the semiconductor In₂S₃ shows, in two different temperature ranges, dynamical PAC-spectra which correspond to different types of mobile charge carriers. Since ¹¹¹In is a self atom in In₂S₃, this compound is an ideal substance to study the charge transport phenomena by the PAC technique. This revised version was published online in August 2006 with corrections to the Cover Date.     

Mössbauer Studies on Nanocrystalline Diol Capped γ-Fe2O3

Nanocrystalline indium (nano-In) was prepared with different particle sizes by electrochemical deposition. The temperature dependence of the local electric field gradient (EFG) of nano-In was investigated in a temperature range of 20–300 K using the probe ¹¹¹In for perturbed γγ angular correlation (PAC) experiments. The temperature dependence of the EFG of nano-In can be described by a (1−BT ^3/2) dependence as in bulk-In. It is shown that the low temperature value of the EFG and the proportionality constant B vary systematically with particle size.