title: The ion sensitivity of surface conductive single crystalline diamond.
abstract: Charge build-up at the solid/aqueous interface is a ubiquitous phenomenon that determines the properties of interfacial electrical double layers. Due to its unique properties, the surface of diamond offers an attractive platform to investigate charging mechanisms in aqueous solutions. We investigate the surface charge by studying the ion sensitivity of H-terminated single crystalline diamond surface conductive layers. The effect of monovalent and divalent salts has been probed at different pH values. For a pH above 3.5, increasing the ionic strength results in a decrease of the surface conductivity, in contrast to the results obtained for pH below 3.5. Electrokinetic experiments are in good agreement with the surface conductivity measurements, showing an isoelectric point at pH 3.5 for the H-terminated diamond surface. We discuss the results in terms of the Coulombic screening by electrolyte ions of the surface potential, which is induced by a pH-dependent surface charge. The origin of this surface charge is discussed in terms of charge regulation by amphoteric hydroxyl surface groups and unsymmetrical adsorption of hydroxide and hydronium ions induced by the hydrophobic nature of the H-terminated diamond surface. This surface charge can have important consequences for processes governed by the diamond/aqueous interface, such as electron transfer to charged redox molecules, adsorption of charged molecules and proteins, and ion sensitivity.
authors.affiliation: Walter Schottky Institut, Technische Universität München, Garching, Germany.
authors.forename: Andreas
authors.initials: A
authors.lastname: Härtl
authors.forename: Jose A
authors.initials: JA
authors.lastname: Garrido
authors.forename: Stefan
authors.initials: S
authors.lastname: Nowy
authors.forename: Ralf
authors.initials: R
authors.lastname: Zimmermann
authors.forename: Carsten
authors.initials: C
authors.lastname: Werner
authors.forename: Dominik
authors.initials: D
authors.lastname: Horinek
authors.forename: Roland
authors.initials: R
authors.lastname: Netz
authors.forename: Martin
authors.initials: M
authors.lastname: Stutzmann
mesh_terms: D000327:Adsorption; D003198:Computer Simulation; D018130:Diamond / Q000737:chemistry*; D004563:Electrochemistry; D004579:Electron Transport; D006863:Hydrogen-Ion Concentration; D057927:Hydrophobic and Hydrophilic Interactions; D006878:Hydroxides / Q000737:chemistry*; D007477:Ions; D008968:Molecular Conformation; D009861:Onium Compounds / Q000737:chemistry*; D009994:Osmolar Concentration; D010084:Oxidation-Reduction; D011506:Proteins / Q000737:chemistry; D013499:Surface Properties; D013501:Surface-Active Agents / Q000737:chemistry*; D014867:Water / Q000737:chemistry
chemical_list: D006878:Hydroxides; D007477:Ions; D009861:Onium Compounds; D011506:Proteins; D013501:Surface-Active Agents; D014867:Water; C027727:hydronium ion; D018130:Diamond