title: Sitting at the edge: how biomolecules use hydrophobicity to tune their interactions and function.
abstract: Water near extended hydrophobic surfaces is like that at a liquid-vapor interface, where fluctuations in water density are substantially enhanced compared to those in bulk water. Here we use molecular simulations with specialized sampling techniques to show that water density fluctuations are similarly enhanced, even near hydrophobic surfaces of complex biomolecules, situating them at the edge of a dewetting transition. Consequently, water near these surfaces is sensitive to subtle changes in surface conformation, topology, and chemistry, any of which can tip the balance toward or away from the wet state and thus significantly alter biomolecular interactions and function. Our work also resolves the long-standing puzzle of why some biological surfaces dewet and other seemingly similar surfaces do not.
authors.affiliation: Howard P. Isermann Department of Chemical & Biological Engineering, and Center for Biotechnology & Interdisciplinary Studies, Rensselaer Polytechnic Institute, Troy, New York 12180, USA.
authors.forename: Amish J
authors.initials: AJ
authors.lastname: Patel
authors.forename: Patrick
authors.initials: P
authors.lastname: Varilly
authors.forename: Sumanth N
authors.initials: SN
authors.lastname: Jamadagni
authors.forename: Michael F
authors.initials: MF
authors.lastname: Hagan
authors.forename: David
authors.initials: D
authors.lastname: Chandler
authors.forename: Shekhar
authors.initials: S
authors.lastname: Garde
mesh_terms: D049308:Dioxygenases / Q000737:chemistry* / Q000378:metabolism; D057927:Hydrophobic and Hydrophilic Interactions; D008555:Melitten / Q000737:chemistry; D008958:Models, Molecular; D014867:Water / Q000737:chemistry
chemical_list: D014867:Water; D008555:Melitten; D049308:Dioxygenases; C074272:2,3-dihydroxybiphenyl oxygenase