A recent National Research Council report highlighted the potential utility of atmospheric observations and models for detecting trends in concentrated emissions from localized regions, such as urban areas. The Salt Lake City (SLC), Utah, area was chosen for a pilot study to determine the feasibility of using ground-based sensors to identify trends in anthropogenic urban emissions over a range of time scales (from days to years). The Weather Research and Forecasting model (WRF) was combined with a Lagrangian particle dispersion model and an emission inventory to model carbon dioxide (CO2) concentrations that can be compared with in situ measurements. An accurate representation of atmospheric transport requires a faithful modeling of the meteorological conditions. This study examines in detail the ability of different configurations of WRF to reproduce the observed local and mesoscale circulations, and the diurnal evolution of the planetary boundary layer (PBL) in the SLC area. Observations from the Vertical Transport and Mixing field experiment in 2000 were used to examine the sensitivity of WRF results to changes in the PBL parameterization and to the inclusion of an urban canopy model (UCM). Results show that for urban locations there is a clear benefit from parameterizing the urban canopy for simulation of the PBL and near-surface conditions, particularly for temperature evolution at night. Simulation of near-surface CO2 concentrations for a 2-week period in October 2006 showed that running WRF at high resolution (1.33 km) and with a UCM also improves the simulation of observed increases in CO2 during the early evening.