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Science1 publisher2 min readPublished

Cooperative clusters in a simulated cooling liquid start shrinking below a certain temperature

Corentin Laudicina tracked the groups of particles that move together in a simulated liquid of spheres. Their size grows as the liquid cools and then falls again, where older theories of the glass transition predicted growth without limit.

The Scientist · Science desk

Illustration accompanying Cooperative clusters in a simulated cooling liquid start shrinking below a certain temperature

What happened

  • Laudicina describes the puzzle of glass as a mismatch: near the glass transition viscosity rises far faster than expected, while the material's internal structure barely changes.
  • To study it he simulated a model liquid of perfectly spherical particles with simple interactions, running the simulations through the TU/e Supercomputing Center.
  • Following the groups of particles that move together, he found the clusters get larger as the liquid cools and then start getting smaller again below a certain temperature.
  • Older theories that leave these clusters out predicted the opposite, with cluster growth continuing indefinitely until the liquid suddenly became stuck.
  • Laudicina reports that the clusters put a natural brake on their own growth, and says this is why no abrupt transition is seen in the laboratory or in simulations.

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Why it matters

  • constraint A cluster size that peaks at an intermediate temperature is a feature any competing account of the slowdown now has to reproduce, and a length scale that grows without bound misses it.
  • capability Since no microscope can follow millions of particles for the times involved, the quantity that separates the two pictures currently exists only inside simulations. Anyone who wants to check it has to run them.
  • exposure Anyone leaning on the self-limiting picture is leaning on a dissertation as described in an interview; phys.org cites no journal publication for the cluster result.

The clusters Laudicina measured are defined by how the particles move. Some particles in a supercooled liquid barely move at all, while others form groups that travel together, and his simulations tie the large changes in viscosity to that unevenness [7][8]. He described the crowding this way: "A bit like at a festival, where, in the crowded areas, everyone has to move a little if you want to get a beer at the back of the field." [18]

In the phys.org interview Laudicina said that around the glass transition "the viscosity increases extremely rapidly" while "the material's internal structure barely changes" [3]. A glass, he said, "behaves like a solid, while its internal structure is more like that of a liquid" [2]. The static arrangement is the part that stays put; the simulations follow how the motion sorts itself into groups [7].

The simplification was deliberate. Theoretical physicists are primarily "striving for simplicity", Laudicina said, and here that meant reducing real liquids to a system of perfectly spherical particles interacting in relatively simple ways [17][5]. Time scales are the hard part of the measurement. He pointed to the University of Queensland's pitch drop livestream: pitch is rock-hard at room temperature and still an extremely viscous liquid, dripping on average once every ten years [13].

What he set out to measure was how the clusters change as the liquid cools, and how that relates to the gradual slowing of the liquid through the glass transition [19]. The method was to measure the different clusters precisely and track them over longer periods of time [20]. The simulated particles were spheres interacting simply, so the turnover he reports cannot say whether a liquid of real molecules shows the same maximum [5][9].

What to watch

  • A journal publication giving the crossover temperature and the cluster sizes at the maximum, which other groups would need to reproduce it.
  • Colloid experiments, where particles are large enough to track directly, testing whether cluster size turns over on cooling.
  • Whether the same maximum appears in model liquids built from something other than simple spheres.
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