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Publication abstract: Vibrational sum-frequency generation (vSFG) spectroscopy is used to determine the molecular structure of water at the interface of palmitic acid monolayers. Both measured and calculated spectra display specific features due to third-order contributions to the vSFG response which are associated with finite interfacial electric potentials. We demonstrate that theoretical modeling enables to separate the third-order contributions, thus allowing for a systematic analysis of the strictly surface-sensitive, second-order component of the vSFG response. This study provides fundamental, molecular-level insights into the interfacial structure of water in a neutral surfactant system with relevance to single layer bio-membranes and environmentally relevant sea-spray aerosols. Our results emphasize the key role that computer simulations can play in interpreting vSFG spectra and revealing microscopic details of water at complex interfaces, which can be difficult to extract from experiments due to the mixing of second-order, surface-sensitive and third-order, bulk-dependent contributions to the vSFG response. Research Data Curation Program, UC San Diego, La Jolla, 92093-0175 (https://lib.ucsd.edu/rdcp) Reddy, Sandeep K.; Thiraux, Raphael; Wellen Rudd, Bethany A.; Lin, Lu; Adel, Tehseen; Joutsuka, Tatsuya; Geiger, Franz M.; Allen, Heather C.; Morita, Akihiro; Paesani, Francesco. (2018). Data from: Bulk Contributions Modulate the Sum-Frequency Generation Spectra of Interfacial Water on Model Sea-Spray Aerosols. In Center for Aerosol Impacts on Chemistry of the Environment (CAICE). UC San Diego Library Digital Collections. https://doi.org/10.6075/J08C9TFW Reddy, Sandeep K.; Thiraux, Raphael; Wellen Rudd, Bethany A.; Lin, Lu; Adel, Tehseen; Joutsuka, Tatsuya; Geiger, Franz M.; Allen, Heather C.; Morita, Akihiro; Paesani, Francesco, Bulk Contributions Modulate the Sum-Frequency Generation Spectra of Interfacial Water on Model Sea-Spray Aerosols, Chem, Submitted.