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The distribution of electric fields within the electrochemical double layerdepends on both the electrode and electrolyte in complex ways. These fieldsstrongly influence chemical dynamics in the electrode-electrolyte interface,but cannot be measured directly with sub-molecular resolution. We reportexperimental capacitance measurements for aqueous interfaces of CO-terminatedPt(111). By comparing these measurements with first-principlesdensity-functional theory (DFT) calculations, we infer microscopic fielddistributions and decompose contributions to the inverse capacitance fromvarious spatial regions of the interface. We find that the CO is stronglyelectronically coupled to the Pt, and that most of the interfacial potentialdifference appears across the gap between the terminating O and water, and notacross the CO molecule as previously hypothesized. This `gap capacitance'resulting from hydrophobic termination lowers the overall capacitance of theaqueous Pt-CO interface, and makes it less sensitive to electrolyteconcentration compared to the bare metal.

Electrochemical Capacitance of CO-terminated Pt(111) is Dominated by CO-Solvent Gap