Diffuse scattering from dynamically compressed single-crystal zirconium following the pressure-induced $\alpha\to\omega$ phase transition

TL;DR

This study uses molecular dynamics simulations to explore the atomistic mechanisms of the alpha to omega phase transition in zirconium under dynamic compression, revealing new diffuse scattering signals linked to defect structures and heterogenous nucleation.

Contribution

It introduces a machine-learning-based simulation approach that predicts the transition mechanism and reproduces unique diffuse scattering patterns observed in experiments, advancing understanding of phase transition dynamics.

Findings

Transition proceeds via a modified Usikov-Zilberstein mechanism.

Diffuse scattering signals originate from thermal vibrations, residual grains, and defects.

Simulations match experimental diffraction patterns, revealing atomistic disorder.

Abstract

The prototypical $\alpha\to\omega$ phase transition in zirconium is an ideal test-bed for our understanding of polymorphism under extreme loading conditions. After half a century of study, a consensus had emerged that the transition is realized via one of two distinct displacive mechanisms, depending on the nature of the compression path. However, recent dynamic-compression experiments equipped with in situ diffraction diagnostics performed in the past few years have revealed new transition mechanisms, demonstrating that our understanding of the underlying atomistic dynamics and transition kinetics is in fact far from complete. We present classical molecular dynamics simulations of the $\alpha\to\omega$ phase transition in single-crystal zirconium shock-compressed along the [0001] axis using a machine-learning-class potential. The transition is predicted to proceed primarily via a modified version of the two-stage Usikov-Zilberstein mechanism, whereby the high-pressure $\omega$-phase heterogeneously nucleates at boundaries between grains of an intermediate $\beta$-phase. We further observe the fomentation of atomistic disorder at the junctions between $\beta$ grains, leading to the formation of highly defective interstitial material between the $\omega$ grains. We directly compare synthetic x-ray diffraction patterns generated from our simulations with those obtained using femtosecond diffraction in recent dynamic-compression experiments, and show that the simulations produce the same unique, anisotropic diffuse scattering signal unlike any previously seen from an elemental metal. Our simulations suggest that the diffuse signal arises from a combination of thermal diffuse scattering, nanoparticle-like scattering from residual kinetically stabilized $\alpha$ and $\beta$ grains, and scattering from interstitial defective structures.