Many next-generation technologies are limited by material performance, leading to increased interest in the discovery of advanced materials using combinatorial synthesis, characterization, and screening. Several combinatorial synthesis techniques, such as solution based methods, advanced manufacturing, and physical vapor deposition, are currently being employed for various applications. In particular, combinatorial magnetron sputtering is a versatile technique that provides synthesis of high-quality thin film composition libraries. Spatially addressing the composition of these thin films generally requires elemental quantification measurements using techniques such as energy-dispersive X-ray spectroscopy or X-ray fluorescence spectroscopy. Since these measurements are performed ex-situ and post-deposition, they are unable to provide real-time design of experiments, a capability that is required for rapid synthesis of a specific composition library. By using three quartz crystal monitors attached to a stage with translational and rotational degrees of freedom, we measure three-dimensional deposition profiles of deposition sources whose tilt with respect to the substrate is robotically controlled. We exhibit the utility of deposition profiles and tilt control to optimize the deposition geometry for specific combinatorial synthesis experiments.