Defects in Solids Group, Hyperfine Interactions Laboratory, Physics, Washington State University, Pullman, WA, USA

Publications 2006-2010

All publications are based in part upon work supported by the National Science Foundation (Metals Program) under Grant DMR 05-04843 and predecessor grants and the Praveen Sinha Fund for Physics Research.  Opinions, findings, conclusions and recommendations expressed in these publications are those of the authors and do not necessarily reflect views of the National Science Foundation or of the Praveen Sinha Fund.

Change of diffusion mechanism with lattice parameter in the series of lanthanide indides having L12 structure, Gary S. Collins, Xia Jiang, John P. Bevington, Farida Selim and Matthew O. Zacate, Physical Review Letters 102, 155901 (2009).  http://link.aps.org/abstract/PRL/v102/e155901

Using perturbed angular correlation spectroscopy (PAC), jump frequencies of Cd tracer atoms were measured for 12 indides In3B (B= rare earth) in paired samples having compositions at each of the opposing phase boundaries.   Jump frequencies in heavy lanthanide indides were observed to be smaller for In-richer compositions than for In-poorer compositions, but greater in the light lanthanide indides.  These findings signal an unmistakable change in diffusion mechanism from the simple In-sublattice vacancy mechanism for heavy lanthanides to a B-vacancy mechanism for light lanthanides.

Jump frequencies of Cd tracer atoms in L12 lanthanide gallides,  Xia Jiang, Matthew O. Zacate and Gary S. Collins,  Defect and Diffusion Forum 289-292, 725 (2009).  Presented at the Seventh International Conference on  Diffusion in Materials, Canary Islands, October 28-31, 2008).

Jump frequencies of Cd tracer atoms were measured in three lanthanide gallides having the L12 structure:  DyGa3, ErGa3 and LuGa3.  111In/Cd impurity probe atoms were observed to occupy the non-cubic Ga-sites through the nuclear quadrupole interaction using the method of perturbed angular correlation of gamma rays (PAC).  Measurements at elevated temperatures exhibited nuclear relaxation (damping) of quadrupolar perturbation functions attributed to diffusional jumps of the probes among orientationally inequivalent Ga-sites.  Accurate values of jump frequencies were determined from fits of the measured perturbation functions using a model of stochastically fluctuating electric-field gradients, as in previous work [e.g., Matthew O. Zacate, Aurélie Favrot and Gary S. Collins: Physical Review Letters Vol. 92 (2004) p. 225901].  Arrhenius plots of jump frequencies for the three systems exhibited jump-frequency activation enthalpies in the range 0.86-1.05 eV and prefactors of about 2 THz.   The activation enthalpy for ErGa3, 0.86(2) eV is compared with those for ErAl3, 1.40(4) eV, and ErIn3, 1.34(5) eV.
Motion of cadmium traver atoms in Al11R3 phases (R= La, Ce, Pr), Stephanie Lage and Gary S. Collins,  Defect and Diffusion Forum 289-292, 755 (2009).   Presented at the Seventh International Conference on  Diffusion in Materials, Canary Islands, October 28-31, 2008).

Jump frequencies of Cd tracer atoms were measured in three phases having the orthorhombic Al11R3 structure, with R= La, Ce, or Pr.   The structure has four inequivalent Al-sites and two inequivalent R-sites.   111In/Cd tracer atoms were observed to occupy several sites via the nuclear quadrupole interaction using perturbed angular correlation of gamma rays (PAC).   Time-domain PAC spectra became damped as the temperature increased, which is attributed to nuclear relaxation caused by diffusional jumps of Cd tracer atoms leading to changes in orientations and/or magnitudes of electric field gradients (EFG’s).  Maximum relaxations were observed near 770 K.  A method is proposed for estimating the mean jump frequency at that temperature, giving a mean jump frequency w averaged over all sites of about 100 MHz.  At still higher temperatures, damping decreased due to motional averaging, and the quadrupole perturbations evolved into unique signals having lower frequencies and corresponding in each phase to the averages of EFG tensors of all sites visited by the Cd tracer atoms.  For Al11La3, the jump frequency at 1073 K was estimated to be 1.9 GHz.  Such jump frequencies imply unusually high diffusivities in these phases.
Site preferences if indium impurity atoms in intermetallics having Al3Ti or Al3Zr crystal structures, John P. Bevington, Farida Selim and Gary S. Collins, Hyperfine Interactions 177, numbers 1-3, June 2008.  DOI:10.1007/s10751-008-9615-y;  International Conference on Hyperfine Interactions, Iguassu Falls, Brazil,  5-10 August 2007.

Site-fractions of indium impurity probe atoms occupying up to three inequivalent Al-sites in Al3Ti, Al3V and Al3Zr phases were measured using perturbed angular correlation of gamma rays (PAC).   Sites were identified via characteristic nuclear quadrupole interactions.  Ratios of site-fractions were measured in thermal equilibrium in the range 600 to 1210 K.  Arrhenius plots of the ratios were fitted with thermally activated expressions, yielding differences in vibrational entropies and site-enthalpies.  Enthalpy differences were greatest for Al3Zr, ~0.22 eV, and smaller for Al3Ti and Al3V, which is correlated with the excess volume of the transition-metal (TM) atom over the Al-atom.   Vibrational entropy differences were small, in the range 0 to -0.25 kB.
Diffusion of 111Cd probes in Ga7Pt3 studied via nuclear quadrupole relaxation, Farida Selim, John P. Bevington and Gary S. Collins, Hyperfine Interactions 178, numbers 1-3, July 2008.  DOI:10.1007/s10751-008-9663-3;  International Conference on Hyperfine Interactions, Iguassu Falls, Brazil,  5-10 August 2007.

Diffusion of 111In/Cd impurity atoms was studied in Ga7Pt3 at the atomic level using the method of perturbed angular correlation of gamma rays (PAC).  As in previous measurements on Ga7Pd3, probes were observed to occupy two inequivalent Ga-sublattices.  Quadrupole interaction perturbation functions for each site exhibited damping at elevated temperatures that is attributed to nuclear relaxation caused by stochastic jumps of the probe atoms accompanied by reorientation of axes of the electric field gradient tensor.   Fitted relaxation frequencies, proportional to mean jump frequencies of the probe, were thermally activated.   Arrhenius plots revealed jump-frequency activation enthalpies of 0.94(8) and 0.67(4) eV for the two sites and frequency prefactors close to 1 THz.  Results were similar to those found previously for Ga7Pd3, although jump frequencies are about 100 times lower in Ga7Pt3.

Simultaneous measurement of tracer jump frequencies on different sublattices in Ga7Pd3 using PAC, Egbert R. Nieuwenhuis, Matthew O. Zacate and Gary S. Collins, Defect and Diffusion Forum 264, 27-32 (2007);  International Conference on Diffusion and Stresses, Lillafüred, Hungary, 19-22 September 2006.

Jump frequencies of tracer atoms in the intermetallic compound Ga7Pd3 were determined through observation of fluctuating nuclear quadrupole interactions caused by the jumps.  Measurements were made for 111Cd tracer atoms following decay of 111In using the method of perturbed angular correlation of gamma rays (PAC).  Tracers were found to occupy two inequivalent Ga-sublattices, with distinct quadrupole perturbation functions.  The two sublattices interpenetrate and long-range three-dimensional diffusion is possible on either sublattice via near-neighbor jumps.  Measurements at elevated temperature exhibited damping of static quadrupole perturbation functions G2static (t) that was fitted for each signal using the approximation G2 (t)= exp(-wt) G2static (t), in which w is the jump frequency of the tracer.  Arrhenius plots of w for the two sites exhibited thermal activation with activation enthalpies of 0.49(2) and 0.44(4) eV and jump frequency prefactors close to 2 × 1011 Hz.  Possible scenarios to interpret the results in terms of underlying inter- and intra-sublattice jumps are discussed.    

Nonstoichiometry in line compounds, Gary S. Collins, Journal of Materials Science 42, 1915-1919 (2007);  International Conference on Nonstoichiometric Compounds, Kauai, Hawai'i, April 3-8, 2005.  http://dx.doi.org/10.1007/s10853-006-0055-2

Phases having compositional fields narrower than about 1 at.% and appearing as lines in binary phase diagrams often are assumed to have properties independent of composition.  That such an assumption can be seriously in error is illustrated by recent measurements on pairs of samples prepared to have compositions at opposing phase boundaries.  Two microscopic properties, lattice locations of highly dilute solutes and diffusional jump frequencies, were studied, respectively, through measurement of static and dynamic nuclear quadrupole interactions using the method of perturbed angular correlation of gamma rays (PAC).   At opposing boundary compositions, PAC probe atoms have been observed to occupy different lattice sites or to have jump frequencies differing by a factor of 100.  Such gross differences suggest measurements of other properties of line compounds should be made on pairs of samples having the opposing boundary compositions in order to avoid inconsistent or unreproducible results.

Publications 2001-2005
Publications 1995-2000
Selected Publications prior to 1995


April 2009.  Back to Collins's group home page. You are visitor  since the last reset.