4.7 Article

Structural and short-time vibrational properties of colloidal glasses and supercooled liquids in the vicinity of the re-entrant glass transition

Journal

JOURNAL OF CHEMICAL PHYSICS
Volume 155, Issue 7, Pages -

Publisher

AMER INST PHYSICS
DOI: 10.1063/5.0059084

Keywords

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Funding

  1. National Natural Science Foundation [DMR2003659]
  2. Penn MRSEC grant [DMR1720530]

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The study reveals that in two-dimensional, bidisperse colloidal glasses and supercooled liquids, the anharmonicity of in-cage vibrations and effective spring constants show non-monotonic variations with increasing interparticle depletion attraction strength.
We investigate the short-time vibrational properties and structure of two-dimensional, bidisperse, colloidal glasses and supercooled liquids in the vicinity of the re-entrant glass transition, as a function of interparticle depletion attraction strength. The long-time spatiotemporal dynamics of the samples are measured to be non-monotonic, confirming that the suspensions evolve from repulsive glass to supercooled liquid to attractive glass with increasing depletion attraction. Here, we search for vibrational signatures of the re-entrant behavior in the short-time spatiotemporal dynamics, i.e., dynamics associated with particle motion inside its nearest-neighbor cage. Interestingly, we observe that the anharmonicity of these in-cage vibrations varies non-monotonically with increasing attraction strength, consistent with the non-monotonic long-time structural relaxation dynamics of the re-entrant glass. We also extract effective spring constants between neighboring particles; we find that spring stiffness involving small particles also varies non-monotonically with increasing attraction strength, while stiffness between large particles increases monotonically. Last, from study of depletion-dependent local structure and vibration participation fractions, we gain microscopic insight into the particle-size-dependent contributions to short-time vibrational modes in the glass and supercooled liquid states.

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