Experiments and simulations were performed to examine the complex processes that occur in Rayleigh�Taylor driven mixing. A water channel facility was used to examine a buoyancy-driven Rayleigh�Taylor mixing layer. Measurements of �uctuating den- sity statistics and the molecular mixing parameter were made for Pr = 7 (hot/cold water) and Sc 103 (salt/fresh water) cases. For the hot/cold water case, a high- resolution thermocouple was used to measure instantaneous temperature values that were related to the density �eld via an equation of state. For the Sc 103 case, the degree of molecular mixing was measured by monitoring a di�usion-limited chemical reaction between the two �uid streams. The degree of molecular mixing was quanti- �ed by developing a new mathematical relationship between the amount of chemical product formed and the density variance 02. Comparisons between the Sc = 7 and Sc 103 cases are used to elucidate the dependence of on the Schmidt number. To further examine the turbulent mixing processes, a direct numerical simu- lation (DNS) model of the Sc = 7 water channel experiment was constructed to provide statistics that could not be experimentally measured. To determine the key physical mechanisms that in�uence the growth of turbulent Rayleigh�Taylor mixing layers, the budgets of the exact mean mass fraction em1, turbulent kinetic energy fE00, turbulent kinetic energy dissipation rate e 00, mass fraction variance gm002 1 , and mass fraction variance dissipation rate f 00 equations were examined. The budgets of the unclosed turbulent transport equations were used to quantitatively assess the relative magnitudes of di�erent production, dissipation, transport, and mixing processes. Finally, three-equation (fE00-e 00-gm002 1 ) and four-equation (fE00-e 00-gm002 1 -f 00) turbulent mixing models were developed and calibrated to predict the degree of molecular mix- ing within a Rayleigh�Taylor mixing layer. The DNS data sets were used to assess the validity of and calibrate the turbulent viscosity, gradient-di�usion, and scale- similarity closures a priori. The modeled transport equations were implemented in a one-dimensional numerical simulation code and were shown to accurately reproduce the experimental and DNS results a posteriori. The calibrated model parameters from the Sc = 7 case were used as the starting point for determining the appropri- ate model constants for the mass fraction variance gm002 1 transport equation for the Sc 103 case.