Resolving Length Scale Dependent Transient Disorder Through an Ultrafast Phase Transition

Material functionality can be strongly determined by structure extending only over nanoscale distances. The pair distribution function presents an opportunity to shift structural studies beyond idealized crystal models and investigate structure over varying length scales. Applying this method with ultrafast time resolution has the potential to similarly disrupt the study of structural dynamics and phase transitions. Here, we demonstrate such a measurement of CuIr$_{2}$S$_{4}$ optically pumped from its low temperature Ir-dimerized phase. Dimers are optically suppressed without spatial correlation, generating a structure whose level of disorder depends strongly on length scale. The re-development of structural ordering over tens of picoseconds is directly tracked over both space and time as a transient state is approached. This measurement demonstrates both the crucial role of local structure and disorder in non-equilibrium processes and the feasibility of accessing this information with state-of-the-art XFEL facilities.
Comment: 14 page manuscript with 4 figures. 13 page Supplementary with 17 figures. 27 pages and 21 figures in total