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Direct measurements of growing amorphous order and non-monotonic dynamic correlations in a colloidal glass-former

Nature Physics volume 11, pages 403408 (2015) | Download Citation

Abstract

The transformation of flowing liquids into rigid glasses is thought to involve increasingly cooperative relaxation dynamics as the temperature approaches that of the glass transition. However, the precise nature of this motion is unclear, and a complete understanding of vitrification thus remains elusive. Of the numerous theoretical perspectives1,2,3,4 devised to explain the process, random first-order theory (RFOT; refs 2, 5) is a well-developed thermodynamic approach, which predicts a change in the shape of relaxing regions as the temperature is lowered. However, the existence of an underlying ‘ideal’ glass transition predicted by RFOT remains debatable, largely because the key microscopic predictions concerning the growth of amorphous order and the nature of dynamic correlations lack experimental verification. Here, using holographic optical tweezers, we freeze a wall of particles in a two-dimensional colloidal glass-forming liquid and provide direct evidence for growing amorphous order in the form of a static point-to-set length. We uncover the non-monotonic dependence of dynamic correlations on area fraction and show that this non-monotonicity follows directly from the change in morphology and internal structure of cooperatively rearranging regions6,7. Our findings support RFOT and thereby constitute a crucial step in distinguishing between competing theories of glass formation.

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Acknowledgements

The authors thank W. Kob for illuminating discussions. K.H.N. thanks the Council for Scientific and Industrial Research (CSIR), India for a Senior Research Fellowship. S.G. thanks CSIR, India for a Shyama Prasad Mukherjee Fellowship. A.K.S. thanks Department of Science and Technology (DST), India for support under a J. C. Bose Fellowship and R.G. thanks the International Centre for Materials Science (ICMS) and the Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR) for financial support.

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Affiliations

  1. Chemistry and Physics of Materials Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore 560064, India

    • K. Hima Nagamanasa
  2. Department of Physics, Indian Institute of Science, Bangalore 560012, India

    • Shreyas Gokhale
    •  & A. K. Sood
  3. International Centre for Materials Science, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore 560064, India

    • A. K. Sood
    •  & Rajesh Ganapathy

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Contributions

K.H.N., S.G., A.K.S. and R.G. designed the research, analysed the data and wrote the paper. K.H.N. performed the experiments.

Competing interests

The authors declare no competing financial interests.

Corresponding authors

Correspondence to K. Hima Nagamanasa or Rajesh Ganapathy.

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https://doi.org/10.1038/nphys3289

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