Atom motion in solids following nuclear transmutation

TL;DR

This study investigates atomic motion of daughter isotopes in solids after nuclear decay, revealing anomalous rapid jumps and complex diffusion behaviors influenced by material composition and temperature.

Contribution

It provides new insights into the atomic-scale dynamics of daughter atoms post-decay, challenging traditional defect-mediated diffusion models and proposing alternative mechanisms.

Findings

Cd-probes jump in nanoseconds at high temperature

Anomalous motion linked to lanthanide expansion

Different diffusion regimes observed across series

Abstract

Following nuclear decay, a daughter atom in a solid will "stay in place" if the recoil energy is less than the threshold for displacement. At high temperature, it may subsequently undergo long-range diffusion or some other kind of atomic motion. In this paper, motion of 111Cd tracer probe atoms is reconsidered following electron-capture decay of 111In in the series of In3R phases (R= rare-earth). The motion produces nuclear relaxation that was measured using the method of perturbed angular correlation. Previous measurements along the entire series of In3R phases appeared to show a crossover between two diffusional regimes. While relaxation for R= Lu-Tb is consistent with a simple vacancy diffusion mechanism, relaxation for R= Nd-La is not. More recent measurements in Pd3R phases demonstrate that the site-preference of the parent In-probe changes along the series and suggests that the same behavior occurs for daughter Cd-probes. The anomalous motion observed for R= Nd-La is attributed to "lanthanide expansion" occurring towards La end-member phases. For In3La, the Cd-tracer is found to jump away from its original location on the In-sublattice in an extremely short time, of order 0.5 ns at 1000 K and 1.2 ms at room temperature, a residence time too short to be consistent with defect-mediated diffusion. Several scenarios that can explain the relaxation are presented based on the hypothesis that daughter Cd-probes first jump to neighboring interstitial sites and then are either trapped and immobilized, undergo long-range diffusion, or persist in a localized motion in a cage.