Understanding the role of disorder, and the correlations that exist within it, is one of the defining challenges in contemporary materials science. However, there are few material systems, devoid of other complex interactions, that can be used to systematically study the effects of crystallographic conflict on correlated disorder. Here, we report extensive diffuse x-ray scattering studies on the epitaxially stabilized alloy U 1−x Mo x , showing that a new form of intrinsically tuneable correlated disorder arises from a mismatch between the preferred symmetry of a crystallographic basis and the lattice upon which it is arranged. Furthermore, combining grazing incidence inelastic x-ray scattering and state-of-the-art ab initio molecular dynamics simulations, we discover strong disorder-phonon coupling. This breaks global symmetry and dramatically suppresses phonon lifetimes compared to alloying alone, providing an additional design strategy for phonon engineering. These findings have implications wherever crystallographic conflict can be accommodated, and they may be exploited in the development of future functional materials.

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