Efficient fitting of single-crystal diffuse scattering in interaction space: a mean-field approach

Abstract: The diffraction patterns of crystalline materials with strongly-correlated disorder are characterised by the presence of structured diffuse scattering. Conventional analysis approaches generally seek to interpret this scattering either atomistically or in terms of pairwise (Warren--Cowley) correlation parameters. Here we demonstrate how a mean-field methodology allows efficient fitting of diffuse scattering directly in terms of a microscopic interaction model. In this way the approach gives as its output the underlying physics responsible for correlated disorder. Moreover, the use of a very small number of parameters during fitting renders the approach surprisingly robust to data incompleteness, a particular advantage when seeking to interpret single-crystal diffuse scattering measured in complex sample environments. We use as the basis of our proof-of-concept study a toy model based on strongly-correlated disorder in diammine mercury(II) halides.