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Remote emission sensing (RES) is a non-intrusive measurement method based on absorption spectroscopy, which allows for the determination of pollutant concentrations in vehicle exhaust plumes. By measuring the absorption of the exhaust plume from the roadside using a light/laser barrier, concentration ratios of pollutants, such as nitrogen oxides to carbon dioxide, can be estimated. Computational fluid dynamics (CFD) has been employed to simulate vehicle exhaust plumes due to uncertainties in RES capabilities. In a previous study, Unsteady Reynolds-Averaged Navier-Stokes (URANS) simulations were conducted to investigate the dispersion of vehicle exhaust plumes under various ambient/driving conditions and provide insights for RES applications. However, the accuracy of these simulations can be further improved. Therefore, this study focuses on enhancing the simulation accuracy by employing large eddy simulations (LES).