Over the past century the study of gas exchange rates between the atmosphere and the ocean has received increased attention because of concern about the fate of greenhouse gases such as CO2 released into the atmosphere. Of interest is the oceanic uptake of CO2 in shallow water coastal regions as biological productivity in these regions is on average about three times larger than in the open ocean. It is well-known that in the absence of breaking surface waves, the water side turbulence controls gas transfer of sparingly soluble gases such as CO2 from the air to the water. The dependence of gas transfer on wind-driven shear turbulence and convection turbulence generated by surface cooling has been investigated previously by others. However, the effect of Langmuir turbulence generated by wave-current interaction has not been investigated before. More specifically, Langmuir turbulence is generated by the interaction of the wind-driven shear current with the Stokes drift velocity induced by surface gravity waves. In this dissertation, large-eddy simulations (LES) of wind-driven shallow water flows with Langmuir turbulence have been conducted and scalar transport and surface scalar transfer dynamics analyzed. The scalar represents the concentration of a dissolved gas such as CO2 in the water. In flows with Langmuir turbulence, the largest scales of the turbulence consist of full-depth Langmuir circulation (LC), parallel downwind-elongated, counter-rotating vortices acting as a secondary structure to the mean flow. LES guided by the full-depth LC field measurements of Gargett & Wells (2007) shows that Langmuir turbulence plays a major role in determining scalar transport throughout the entire water column and scalar transfer at the surface. Langmuir turbulence affects scalar transport and its surface transfer through 1. the full-depth homogenizing action of the large scale LC and 2. the near-surface vertical turbulence intensity induced by the Stokes drift velocity shear. Two key parameters controlling the extent of these two mechanisms are the dominant wavelength (λ) of the surface waves generating the turbulence and the turbulent Langmuir number, Lat , which is inversely proportional to wave forcing relative to wind forcing. Furthermore, LES representative of the field measurements of Gargett et al. (2004) shows that Langmuir turbulence increases transfer velocity (a measure of mass transfer efficiency across the air-water interface) dramatically with respect to shear-dominated turbulence. Finally, direct resolution of the surface mass transfer boundary layer allows for the LES to serve as a testing ground for bulk parameterizations of transfer velocity. Several wellestablished parameterizations are tested and a new parameterization based on Stokes drift velocity shear is proposed leading to encouraging results.