ArticleProceedings of the National Academy of Sciences of the United States of America2015
Pathways to dewetting in hydrophobic confinement.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2015. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 23 papers.
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23 citing papers in PubMed, 112 citations in OpenAlex.
- Onset of cavitation and vapor bubble development over hydrophilic and hydrophobic surfaces.Proceedings of the National Academy of Sciences of the United States of America · 2025Article
- On the engulfment of antifreeze proteins by ice.Proceedings of the National Academy of Sciences of the United States of America · 2024Article
- Markov State Model of Solvent Features Reveals Water Dynamics in Protein-Peptide Binding.The journal of physical chemistry. B · 2023Article
- Hydrophobic Homopolymer's Coil-Globule Transition and Adsorption onto a Hydrophobic Surface under Different Conditions.The journal of physical chemistry. B · 2023Article
- Subnanometer Topological Tuning of the Liquid Intrusion/Extrusion Characteristics of Hydrophobic Micropores.Nano letters · 2022Article
- Machine-Learned Free Energy Surfaces for Capillary Condensation and Evaporation in Mesopores.Entropy (Basel, Switzerland) · 2022Article
- Structure and dynamics of water confined in cylindrical nanopores with varying hydrophobicity.Philosophical transactions. Series A, Mathematical, physical, and engineering sciences · 2021Article
- A molecular twist on hydrophobicity.Chemical science · 2021Article
- Water in Nanopores and Biological Channels: A Molecular Simulation Perspective.Chemical reviews · 2020Review
- Free energy of hydrophilic and hydrophobic pores in lipid bilayers by free energy perturbation of a restraint.The Journal of chemical physics · 2020Article
- Dynamical control by water at a molecular level in protein dimer association and dissociation.Proceedings of the National Academy of Sciences of the United States of America · 2020Article
- A unified description of hydrophilic and superhydrophobic surfaces in terms of the wetting and drying transitions of liquids.Proceedings of the National Academy of Sciences of the United States of America · 2019Article
- The Excess Chemical Potential of Water at the Interface with a Protein from End Point Simulations.The journal of physical chemistry. B · 2018Article
- Generic Mechanism for Pattern Formation in the Solvation Shells of Buckminsterfullerene.ACS omega · 2018Article
- Water is an active matrix of life for cell and molecular biology.Proceedings of the National Academy of Sciences of the United States of America · 2017Article
- Intrusion and extrusion of water in hydrophobic nanopores.Proceedings of the National Academy of Sciences of the United States of America · 2017Article
- Effect of material flexibility on the thermodynamics and kinetics of hydrophobically induced evaporation of water.Proceedings of the National Academy of Sciences of the United States of America · 2017Article
- Stochastic level-set variational implicit-solvent approach to solute-solvent interfacial fluctuations.The Journal of chemical physics · 2016Article
- Spontaneous recovery of superhydrophobicity on nanotextured surfaces.Proceedings of the National Academy of Sciences of the United States of America · 2016Article
- The hydrophobic effect, and fluctuations: The long and the short of it.Proceedings of the National Academy of Sciences of the United States of America · 2016Article
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Authors and funding
7 authors at 3 institutions in 1 country.
Funding
No grant is acknowledged in the PubMed record.
Abstract
Liquid water can become metastable with respect to its vapor in hydrophobic confinement. The resulting dewetting transitions are often impeded by large kinetic barriers. According to macroscopic theory, such barriers arise from the free energy required to nucleate a critical vapor tube that spans the region between two hydrophobic surfaces--tubes with smaller radii collapse, whereas larger ones grow to dry the entire confined region. Using extensive molecular simulations of water between two nanoscopic hydrophobic surfaces, in conjunction with advanced sampling techniques, here we show that for intersurface separations that thermodynamically favor dewetting, the barrier to dewetting does not correspond to the formation of a (classical) critical vapor tube. Instead, it corresponds to an abrupt transition from an isolated cavity adjacent to one of the confining surfaces to a gap-spanning vapor tube that is already larger than the critical vapor tube anticipated by macroscopic theory. Correspondingly, the barrier to dewetting is also smaller than the classical expectation. We show that the peculiar nature of water density fluctuations adjacent to extended hydrophobic surfaces--namely, the enhanced likelihood of observing low-density fluctuations relative to Gaussian statistics--facilitates this nonclassical behavior. By stabilizing isolated cavities relative to vapor tubes, enhanced water density fluctuations thus stabilize novel pathways, which circumvent the classical barriers and offer diminished resistance to dewetting. Our results thus suggest a key role for fluctuations in speeding up the kinetics of numerous phenomena ranging from Cassie-Wenzel transitions on superhydrophobic surfaces, to hydrophobically driven biomolecular folding and assembly.
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