Publication date: 21st July 2025
By taking advantage of adjustable short-range attractive interactions of electrostatically stabilized colloidal nanocrystals, we demonstrate an unusual degree of control over the phase behaviour of a nanoscale system, studied via in situ small angle X-ray scattering (SAXS). This control is exemplified through the use of a metastable liquid intermediate state that enables varying the colloidal crystallization rate by over three orders of magnitude, along with predictive control of crystal yield, size, and crystallinity. Most strikingly, we reveal that crystallinity can be increased simultaneously with the crystallization rate.
To further elucidate how the short-range interactions dictate the phase behaviour at the nanoscale, we also resolve the microscopic dynamics of colloidal suspensions and liquid droplets of the nanocrystals via MHz X-ray photon correlation spectroscopy (XPCS). The attractive interactions suppress self-diffusion in the liquid state, suggesting design rules for the shape of interaction potentials not only to leverage liquid intermediates in crystallization processes but also to avoid gelation for better control of phase behaviours.
Finally, we show how light absorption and the associated photochemistry systematically alters the system phase behaviour through a combination of optical transient absorption spectroscopy, time-resolved wide-angle X-ray scattering, MHz XPCS, and in situ SAXS. Results suggest electrostatically driven solvation shell redistribution that renormalizes binodal curves on the nanocrystal phase diagram. Ultimately, the multiscale characterization of and manipulation of electrostatically stabilized nanocrystals paves the way to more clearly explain the design rules for nanoscale interaction potentials so that nanomaterial assemblies can achieve more effective functionalities via deterministic and predictive control.
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