As part of the U.K. contribution to the international Surface Ocean–Lower Atmosphere Study, a series of three related projects—DOGEE, SEASAW, and HiWASE—undertook experimental studies of the processes controlling the physical exchange of gases and sea spray aerosol at the sea surface. The studies share a common goal: to reduce the high degree of uncertainty in current parameterization schemes. The wide variety of measurements made during the studies, which incorporated tracer and surfactant release experiments, included direct eddy correlation fluxes, detailed wave spectra, wind history, photographic retrievals of whitecap fraction, aerosol-size spectra and composition, surfactant concentration, and bubble populations in the ocean mixed layer. Measurements were made during three cruises in the northeast Atlantic on the RRS Discovery during 2006 and 2007; a fourth campaign has been making continuous measurements on the Norwegian weather ship Polarfront since September 2006. This paper provides an overview of the three projects and some of the highlights of the measurement campaigns.