Sediment transport by atmospheric flows shapes landscapes on Earth and other planets. Improving the ability to quantify and predict sand transport by windblown (aeolian) processes has important implications for managing erosion, land degradation, desertification, dust emissions, air quality, and other climate change hazards and risks. Despite progress since Bagnold's seminal works in the 1930s, the most frequently used aeolian sand transport equations show discrepancies between predicted and observed transport rates upwards of 300%. Differences of this magnitude strongly support re-examining how fundamental physical aeolian processes are expressed in predictive equations. Wind tunnel experiments using a Particle Imaging Velocimetry/Particle Tracking Velocimetry (PIV/PTV) system with a high-speed camera and high-powered laser were conducted to visualize fluid motions and sand particle trajectories to provide simultaneous measurements of wind flow and sand transport to re-examine the fundamental physical relationships between flow dynamics, sediment motions, and bedform development. The first experiment of this dissertation focuses on the characteristics of near-surface sand transport in the saltation cloud. From PTV particle trajectories, mean particle velocities appear independent of freestream wind speed, while velocity distribution characteristics (such as modality) and particle concentration intermittency vary with increasing sand transport. Particle trajectories from rippled bed runs show evidence of local slope influence on near-bed particle vectors. The second experiment used manual sand grain tracking to quantify particle-bed splash interactions. Results highlight that common rebound and ejecta functions do not sufficiently represent aeolian saltation splash events. Data indicate a shadowing effect of ripples, suggesting feedback between the saltation cloud, splash events, and bedform migration. The third experiment used dual PIV/PTV analysis to quantify fluid-particle interactions and compare sand concentrations with fluid stresses and turbulence characteristics through the saltation cloud. Results show that increased saltation leads to the disappearance of the constant fluid stress region, changes in aerodynamic roughness length, and increases in turbulence intensities. Leveraging technology advancements and multiple analysis methods, these results provide new, detailed information on the relationships between flow dynamics, sediment motions, and the presence of ripple bedforms. These novel empirical data illustrate some needed corrections to the theoretical and numerical frameworks for quantifying aeolian sand transport.