Crystallisation is among the most common everyday physical phenomena. Yet in the principle material in which quantitative comparison has been made between experiment and theory hard spheres predictions of crystal nucleation rates are up to 20 orders of magnitude slower than measurements, the "second worst prediction in physics" [1].

This discrepancy casts doubt upon the theoretical methods concerned importance sampling which is important not only for crystallisation, because these methods are used to tackle a very wide range of problems, such as drug uptake in cells and chemical reaction pathways. While particle-resolved studies reveal in intimate detail local mechanisms of structural change, they can only access rather fast crystallisation, where there is no discrepancy [2]. However gravitational sedimentation may influence the local structure of the colloidal liquid, which we show can drastically alter crystallisation [3]. We further image nano-particles with STED "nanoscopy", whose timescales are orders of magnitude faster than the larger colloids: thus by "rescaling time", we access new dynamical regimes where the massive discrepancy is found.

  1. Jade Taffs, SW Williams, H Tanaka and C Patrick Royall, Structure and kinetics in the freezing of nearly hard spheres, Soft Matter, 9, 297 - 305 (2013). Link to paper
  2. Jade Taffs and C Patrick Royall, The Role of Fivefold Symmetry in Suppressing Crystallization. Nature Communications 7 (2016). Link to paper
  3. Nicholas Wood, John Russo, Francesco Turci, and C Patrick Royall. Coupling of Sedimentation and Liquid Structure: Influence on Hard Sphere Nucleation. The Journal of Chemical Physics (2018) Link to paper
  4. Willem Gispen, Gabriele M. Coli G, Robin van Damme, C. Patrick Royall and Marjolein Dijkstra, "Crystal polymorph selection mechanism of hard spheres hidden in the fluid", ACS Nano, 17 8807–8814 (2023). link to PDF
  5. C. Patrick Royall, Patrick Charbonneau, Marjolein Dijkstra, John Russo, Frank Smallenburg, Thomas Speck and Chantal Valeriani. Colloidal Hard Spheres: Triumphs, Challenges and Mysteries ArXiV (2023) Link to ArXiV