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Material functionality can be strongly determined by structure extending onlyover nanoscale distances. The pair distribution function presents anopportunity to shift structural studies beyond idealized crystal models andinvestigate structure over varying length scales. Applying this method withultrafast time resolution has the potential to similarly disrupt the study ofstructural dynamics and phase transitions. Here, we demonstrate such ameasurement of CuIr$_{2}$S$_{4}$ optically pumped from its low temperatureIr-dimerized phase. Dimers are optically removed without spatial correlation,generating a structure whose level of disorder depends strongly on lengthscale. The re-development of structural ordering over tens of picoseconds isdirectly tracked over both space and time as a non-equilibrium state isapproached. This measurement demonstrates both the crucial role of localstructure and disorder in non-equilibrium processes and the feasibility ofaccessing this information with state-of-the-art XFEL facilities.

Resolving Length Scale Dependent Transient Disorder Through an Ultrafast Phase Transition