Resolving Length Scale Dependent Transient Disorder Through an Ultrafast Phase Transition
arxiv(2023)
摘要
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_2S_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.
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