Field experiments at Montana State University are conducted for the U.S. Department of Energy as part of the Zero Emissions Research and Technology Center (ZERT) to test and verify monitoring techniques for carbon capture and storage (CCS). A controlled release of CO2 with an added perfluorocarbon tracer was conducted in July 2009 in a multi-laboratory study of atmospheric transport and detection technologies. Tracer plume dispersion was measured with various meteorological conditions using a tethered balloon system with Multi-Tube Remote Samplers (MTRS) at elevations of 10m, 20m, and 40m above ground level (AGL), as well as a ground-based portable tower with monitors containing sorbent material to collect the tracer at 1m, 2m, 3m, and 4m AGL. Researchers designed a horizontal grid of sampling locations centered at the tracer plume source, with the tower positioned at 10m and 30m in both upwind and downwind directions, and the MTRS spaced at 50m and 90m downwind and 90m upwind. Tracer was consistently detected at elevated concentrations at downwind sampling locations. With very few exceptions, higher tracer concentrations correlated with lower elevations. Researchers observed no statistical difference between sampling at 50m and 90m downwind at the same elevation. The US EPA AERMOD model applied using site-specific information predicted transport and dispersion of the tracer. Model results are compared to experimental data from the 2009 ZERT experiment. Successful characterization of the tracer plume simulated by the ZERT experiment is considered a step toward demonstrating the feasibility of remote sampling with unmanned aerial systems (UAS’s) at future sequestration sites.