Abstract

The present work reveals that at the sub-millimeter length-scale, molecules in the liquid state are not dynamically free but elastically correlated. It is possible to “visualize” these hidden elastic correlations by using the birefringent properties of pretransitional swarms persistent in liquids presenting a weak first order transition. The strategy consists in observing the optical response of the isotropic phase of mesogenic fluids to a weak (low energy) mechanical excitation. We show that a synchronized optical response is observable at frequencies as low as 0.01Hz and at temperatures far away from any phase transition (up to at least 15°C above the transition). The observation of a synchronized optical signal at very low frequencies points out a collective response and supports the existence of long-range elastic (solid-like) correlations existing at the sub-millimeter length-scale in agreement to weak solid-like responses already identified in various liquids including liquid water. This concept of elastically linked molecules differs deeply with the academic view of molecules moving freely in the liquid state and has profound consequences on the mechanisms governing collective effects as glass formation, gelation and transport, or synchronized processes in physiological media.

Highlights

  • Liquids differ from solids by a delayed response to a shear mechanical solicitation; i.e. they have no shear elasticity and exhibit a flow behavior at low frequency (< 1Hz)

  • Several recent experimental observations [1,2,3,4,5,6,7,8] highlight the existence of low frequency shear elasticity at the sub-millimeter scale supporting the hypothesis that the liquid state forms a resilient weakly bounded self-assembly

  • LCF1 [3] is a 40 repetitive unit cyanobiphenyl ended side-chain polyacrylate of 4.4nm hydrodynamic radius and LCF2 [10] is a 12 repetitive unit cyanobiphenyl ended side-chain polyacrylate of 1.4nm hydrodynamic radius. They differ by a butyl (LCF1) and a propyl (LCF2) group presenting nematic to isotropic (LCF1) and smectic to isotropic phase transitions (LCF2) respectively

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Summary

Introduction

Liquids differ from solids by a delayed response to a shear mechanical solicitation; i.e. they have no shear elasticity and exhibit a flow behavior at low frequency (< 1Hz). The optical birefringent response reproduces a similar dynamic behaviour versus strain as previous stress measurements [1,3,4,5,6,7,8] and supports fully the assumption that liquids possess a shear elastic regime at low strain values prior to the conventional liquid or flow behavior.

Results
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