4.6 Article

Translational dynamics of a rod-like probe in supercooled liquids: an experimentally realizable method to study Stokes-Einstein breakdown, dynamic heterogeneity, and amorphous order

Journal

SOFT MATTER
Volume 17, Issue 23, Pages 5738-5746

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1sm00509j

Keywords

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Funding

  1. intramural funds at TIFR Hyderabad from the Department of Atomic Energy (DAE)
  2. Swarna Jayanti Fellowship [DST/SJF/PSA-01/2018-19, SB/SFJ/2019-20/05]

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The use of probe molecules is a crucial technique in extracting local dynamical and structural properties of complex dynamical systems. This study shows how the translational dynamics of a rod-like particle in a supercooled liquid can provide information on the growth of correlation length scales and multi-body static correlations. Additionally, it presents a unified scaling theory that rationalizes the observed results in supercooled liquids and proposes a novel experimental method to measure important length scales in molecular glass-forming liquids.
The use of probe molecules to extract the local dynamical and structural properties of complex dynamical systems is an age-old technique both in simulations and in experiments. A lot of important information which is not immediately accessible from bulk measurements can be accessed via these local measurements. Still, a detailed understanding of how a probe particle dynamics is affected by the surrounding liquid medium is lacking, especially in the supercooled temperature regime. This work shows how the translational dynamics of a rod-like particle immersed in a supercooled liquid can give us information on the growth of the correlation length scales associated with dynamical heterogeneity and the multi-body static correlations in the medium. This work also provides an understanding of the breakdown of Stokes-Einstein and Stokes-Einstein-Debye relations in supercooled liquids along with a unified scaling theory that rationalizes all the observed results. Finally, this work proposes a novel yet simple method accessible in experiments to measure the growth of these important length scales in molecular glass-forming liquids.

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