Cube-shape diffuse scattering and the ground state of $\mathrm{BaMg}_{1/3}\mathrm{Ta}_{2/3} \mathrm{O}_3$

TL;DR

This study reveals unusual cube-shaped diffuse scattering in BaMg$_{1/3}$Ta$_{2/3}$O$_3$, linked to partial B-site occupancy correlations, showing power-law decay and suggesting a metastable, kinetically locked ground state.

Contribution

It uncovers a novel diffuse scattering pattern in a cubic perovskite and links it to partial occupancy correlations, expanding understanding of complex ordering phenomena.

Findings

Diffuse scattering forms cube-like objects in reciprocal space.

Power-law decay of correlations indicates non-short-range order.

Monte Carlo simulations reproduce observed diffuse scattering.

Abstract

A quite unusual diffuse scattering phenomenology was observed in the single-crystal X-ray diffraction pattern of cubic perovskite BMT ($\mathrm{BaMg}_{1/3}\mathrm{Ta}_{2/3}\mathrm{O}_3$). The intensity of the scattering is parametrized as a set of cube-like objects located at the centers of reciprocal space unit cells, resembling very broad and cubic-shaped (1/2,1/2,1/2)-satellites. BMT belongs to perovskites of formula AB$'_{1/3}$B$"_{2/3}$O$_{3}$ (A=Mg, B$'=$Ta, B$"=$Mg). The cubes of the intensity can be attributed to the partial correlations of the occupancies of the B site. The pair correlation function is the Fourier transform of the diffuse scattering intensity and the latter's idealized form yields the unusual property of a power-law correlation decay with distance. Up to now this is observed only in a few exotic instances of magnetic order or nematic crystals. Therefore it cannot be classified as a short-range order phenomenon, as in most situations originating diffuse scattering. A Monte-Carlo search in configuration space yielded solutions that reproduce faithfully the observed diffuse scattering. Analysis of the results in terms of the electrostatic energy and the entropy point to this phase of BMT as a metastable state, kinetically locked, which could be the equilibrium state just below the melting point.