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The role of indium tin oxide (ITO) surface structure and chemistry on the formation of self-assembled monolayers (SAM) derived from organophosphonic acids has been investigated. The surface hydroxide content, crystal structure, and roughness of unmodified ITO surfaces were analyzed with X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), atomic force microscopy (AFM), and contact angle measurements. Organophosphonic acid monolayer modified ITO surfaces were then characterized using electrochemistry, contact angle measurements and impedance spectroscopy. To ascertain the extent of defects, Pb was underpotentially deposited (UPD) onto the monolayer modified ITO surfaces at defect sites and regions where the monolayer was weakly bound. The extent of defects, and the location of defects, in monolayers formed on different ITO surfaces were determined from the amount of charge …