scholarly journals Diffusion in LanCoIn3n+2 Phases Studied by Perturbed Angular Correlation

2012 ◽  
Vol 323-325 ◽  
pp. 453-458 ◽  
Author(s):  
Randal Newhouse ◽  
Gary S. Collins

Jump frequencies of 111In/Cd tracer atoms were measured for a series of layered phases LanCoIn3n+2 using the technique of perturbed angular correlation of gamma rays (PAC). The frequencies were determined by analysis of nuclear quadrupole relaxation produced by fluctuating electric field gradients. Samples were synthesized having nominal values n= 1, 2, 3, 5 and , with n= corresponding to the L12 phase LaIn3. The phases form heuristically from LaIn3 by replacing every (n+1)th (100) mixed plane of La and In atoms with a plane of Co-atoms. For the n=1 phase, LaCoIn5, jump frequencies were too small to detect. Two signals were observed, one for indium atoms next to the Co-planes and the other for more distant indium atoms. No relaxation was observed for atoms next to the Co-planes, indicating that there is no diffusion across the Co-planes. With increasing n, jump rates for the other In-atoms increased toward values observed for LaIn3. Jump frequency activation enthalpies for n= 3 and 5 were observed to be the same as for n=, suggesting the same diffusion mechanism. However, the jump-frequency prefactors were found to be smaller for small n, which is attributed to reductions in the connectivity of the diffusion sublattice. We conclude that diffusion in the layered phases is remarkably similar to diffusion in LaIn3 once the reduced connectivity is taken into account.

2012 ◽  
Vol 323-325 ◽  
pp. 447-452
Author(s):  
Randal Newhouse ◽  
Justine Minish ◽  
Gary S. Collins

Diffusional jumps can produce fluctuating electric field gradients at nuclei of jumping atoms. Using perturbed angular correlation of gamma rays (PAC), jumps of probe atoms cause nuclear quadrupole relaxation that can be fitted to obtain the mean jump frequency. An overview is given of the application of this approach to highly ordered intermetallic compounds having the L12(Cu3Au) crystal structure. New results are then presented for jump frequencies of111In/Cd probe atoms in pseudo-binary L12compounds of the forms In3(La1-xPrx) and (In1-xSnx)3La. For the mixed rare-earth system, jump frequencies are found to scale with composition between jump frequencies of the end-member phases In3La and In3Pr. However, for the mixed sp-element system, a large decrease in jump frequency is observed as Sn atoms substitute for In-atoms. This difference in behavior appears to depend on whether atomic disorder is on the diffusion sublattice (In-Sn substitution), as opposed to a neighboring sublattice (La-Pr substitution), whether or not there is a difference in diffusion mechanism between end-member phases, and/or whether or not there is a valence difference between the mixing atoms. All three conditions apply for only (In1-xSnx)3La.


2009 ◽  
Vol 289-292 ◽  
pp. 755-761 ◽  
Author(s):  
Stephanie Lage ◽  
Gary S. Collins

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.


2005 ◽  
Vol 237-240 ◽  
pp. 195-200 ◽  
Author(s):  
Gary S. Collins ◽  
A. Favrot ◽  
L. Kang ◽  
D. Solodovnikov ◽  
Matthew O. Zacate

The jump frequency of Cd tracer atoms was measured as a function of temperature in seven rare-earth tri-indide intermetallic compounds having the L12, or Cu3Au, structure. The frequency, proportional to the diffusivity, was detected by relaxation of nuclear quadrupole interaction at Cd nuclei caused by reorientation of the electric field gradient in each diffusive jump. Measurements were made using perturbed angular correlation of gamma rays, sensitive to jump frequencies in the range 1-1000 MHz. Results are as follows. (1) Jump frequencies measured in LaIn3 and CeIn3 were observed to be 10-100 times greater at the more In-rich boundary composition than the less In-rich boundary composition, even though the phases appear as line compounds in phase diagrams. (2) Arrhenius plots of the jump frequency were fitted to activation enthalpies that increase from 0.535 to 1.80 eV across the series of phases LaIn3, CeIn3, PrIn3, and NdIn3.


1986 ◽  
Vol 73 ◽  
Author(s):  
Herbert Jaeger ◽  
John A. Gardner ◽  
Ohn C. Haygarth ◽  
Robert L. Rasera

ABSTRACTPerturbed Angular Correlation spectroscopy of 181Ta nuclei occupying cation sites has been used to investigate microscopic structural properties of several pure and stabilized zirconia materials. The PAC spectra are used to derive the electric field gradients at the tracer nucleus. Thse are compared with calculations based on a simple point-ion model. Agreement between experiment and theory is good for stabilized material and qualitatively reasonable for pure zirconia.


1998 ◽  
Vol 53 (6-7) ◽  
pp. 349-354 ◽  
Author(s):  
P. Wodniecki ◽  
A. Kulińska ◽  
B. Wodniecka ◽  
A. Z. Hrynkiewicz

Abstract The quadrupole interaction in Au-In compounds of different stoichiometrics was studied with the perturbed angular correlation technique. The electric field gradients at 111Cd probes were measured and the temperature dependences of the quadrupole frequencies were determined. A new high temperature phase of Auln above 630 K and a new metastable modification of Au7In3 were found.


2009 ◽  
Vol 289-292 ◽  
pp. 725-732 ◽  
Author(s):  
Xia Jiang ◽  
Matthew O. Zacate ◽  
Gary S. Collins

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.


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