Vacancy motion in rare-earth-deficient<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mi>R</mml:mi><mml:mrow><mml:mn>1</mml:mn><mml:mo>−</mml:mo><mml:mi>x</mml:mi></mml:mrow></mml:msub><mml:msub><mml:mrow><mml:mi mathvariant="normal">Ni</mml:mi></mml:mrow><mml:mn>2</mml:mn></mml:msub></mml:mrow></mml:math>Laves phases observed by perturbed angular correlation spectroscopy
作者:M. Forker、P. de La Presa、S. Müller、A. Lindbaum、E. Gratz
DOI:10.1103/physrevb.70.014302
日期:——
Rare-earth-deficient R1-xNi2 Laves phases, which reportedly crystallize in a C15 superstructure with ordered R vacancies, have been investigated by perturbed angular correlation (PAC) measurements of electric quadrupole interactions at the site of the probe nucleus Cd-111. Although Cd-111 resides on the cubic R site, a strong axially symmetric quadrupole interaction (QI) with frequencies nu(q)approximate to265-275 MHz has been found in the paramagnetic phases of R1-xNi2 with R=Pr,Nd,Sm,Gd. This interaction is not observed for the heavy R constituents R=Tb,Dy,Ho,Er. The fraction of probe nuclei subject to the QI in R1-xNi2, R=Pr,Nd,Sm,Gd, decreases from 100% at low temperatures to zero at T>300 K and 500 K for R=Sm,Gd and R=Pr,Nd, respectively. At T=100 K the QI is static within the PAC time window, but at T=200 K fluctuations with correlation times tau(C)<10(-6) s, have been detected. These observations can be explained consistently by two assumptions: (i) the mother isotope In-111 of the PAC probe Cd-111 constitutes an attractive potential for vacancies and (ii) the R vacancies in R1-xNi2 are highly mobile at temperatures T<300 K, which is incompatible with a static vacancy superstructure. The measurements indicate a decrease of the vacancy-probe binding energy from the light to the heavy R constituents of R1-xNi2. For R=Pr,Nd,Sm,Gd the binding energy is in the range 0.15-0.40 eV. The activation energy E-A for vacancy jumps near the probe derived from the temperature dependence of the nuclear spin relaxation at 200 Kless than or equal toTless than or equal to300 K is small. The values observed in different samples cover a range of 0.1 eVless than or equal toE(A)less than or equal to0.23 eV. The trial frequency w(0) of these jumps appears to be correlated to the activation energy: ln w(0)(MHz)approximate to58E(A)(eV). At high temperatures T>500 K nuclear spin relaxation related to vacancy hopping is observed in nearly all R1-xNi2. Auxiliary Cd-111 PAC measurements have been carried in Sc0.95Ni2, ScNi2, ScNi0.97, Gd2Ni17, GdNi5, GdNi3, and GdNi.