In the near future, there will be several new instruments measuring atmospheric composition from geostationary orbit over North America, East Asia, and Europe. This constellation of satellites will provide high resolution, time resolved measurements of trace gases and aerosols for monitoring air quality and tracking pollution sources. This paper describes a detailed, fast, and accurate (less than 1.0% uncertainty) method for calculating synthetic top of the atmosphere (TOA) radiances from a global simulation with a mesoscale free running model, the GEOS-5 Nature Run, for remote sensing instruments in geostationary orbit that measure in the ultraviolet-visible spectral range (UV-Vis). Generating these synthetic observations is the first step of an Observing System Simulation Experiment (OSSE), a framework for evaluating the impact of a new observation or algorithm. This paper provides details of the model sampling, aerosol and cloud optical properties, surface reflectance modeling, Rayleigh scattering calculations, and a discussion of the uncertainties of the simulated TOA radiance. An application for the simulated TOA radiance observations is demonstrated in the manuscript. Simulated TEMPO (Tropospheric Emissions: Monitoring of Pollution) and GOES-R (Geostationary Operational Environmental Satellites) observations were used to show how observations from the two instruments could be combined to facilitate aerosol type discrimination. The results demonstrate the viability of a detailed instrument simulator for radiance measurements in the UV-Vis that is capable of accurately simulating high resolution, time-resolved measurements with reasonable computational efficiency.Atmosphere 2019, 10, 2 2 of 36 spectral range (UV-Vis). The large-scale, time-resolved measurements of these pollutants provided by the geostationary constellation are important for managing air quality, and understanding how human activity impacts local, regional, and global distributions of pollution, as well as global climate.Aerosols are one of the most important forcing agents in the climate system. They can be transported around the globe [4], and interact with weather systems [5], scatter and absorb radiation [6][7][8], and modify cloud properties [9,10]. Routine measurements of various aerosol parameters, such as aerosol optical depth (AOD), absorbing aerosol optical depth (AAOD), aerosol index (AI), and single scattering albedo (SSA), are currently available from several sensors in low earth orbit (LEO). These sensors include the twin MODIS (Moderate Resolution Imaging Spectroradiometer) instruments (on-board Terra and Aqua), MISR (Multi-angle Imaging SpectroRadiometer), OMI (Ozone Monitoring Instrument), and POLDER (Polarization and Directionality of the Earth Reflectances) (see Table 1 in [11]). In addition, CALIOP, a spaceborne LiDAR, measures the vertical distribution of aerosol backscattering.Instruments in LEO provide one or two measurements per day, but as aerosol parameters cannot be retrieved under cloudy conditions there can be a l...