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Pathways to dewetting in hydrophobic confinement.

Richard C Remsing¹, Erte Xi¹, Srivathsan Vembanur²

¹Department of Chemical & Biomolecular Engineering, University of Pennsylvania, Philadelphia, PA 19104;

Proceedings of the National Academy of Sciences of the United States of America

|June 24, 2015

Summary

Dewetting transitions in confined water face large barriers. New simulations reveal these barriers are smaller than expected, driven by water density fluctuations, not classical vapor tubes.

Keywords:

assembly capillary evaporation fluctuations kinetic barriers

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Area of Science:

Physical Chemistry
Nanotechnology
Fluid Dynamics

Background:

Liquid water can be metastable in hydrophobic confinement, leading to dewetting.
Macroscopic theory predicts large kinetic barriers for dewetting due to critical vapor tube nucleation.
These barriers arise from the free energy cost of forming a vapor tube spanning hydrophobic surfaces.

Purpose of the Study:

To investigate the kinetic barriers of dewetting transitions in nanoscopic hydrophobic confinement.
To determine if classical macroscopic theory accurately describes dewetting barriers at the nanoscale.
To elucidate the role of water density fluctuations in dewetting kinetics.

Main Methods:

Extensive molecular simulations of water confined between two nanoscopic hydrophobic surfaces.
Advanced sampling techniques to overcome simulation limitations.
Analysis of dewetting pathways and free energy barriers.

Main Results:

The dewetting barrier does not involve classical critical vapor tube nucleation.
An abrupt transition occurs from isolated cavities to gap-spanning vapor tubes larger than critical.
The observed dewetting barrier is smaller than predicted by macroscopic theory.
Enhanced water density fluctuations near hydrophobic surfaces facilitate nonclassical dewetting pathways.

Conclusions:

Water density fluctuations play a crucial role in reducing dewetting barriers in hydrophobic confinement.
Novel dewetting pathways circumvent classical nucleation barriers.
These findings have implications for phenomena like Cassie-Wenzel transitions and biomolecular assembly.