A new multivariate pseudodeterministic receptor model (PDRM), combining mass balance and Gaussian plume dispersion equations, was developed to exploit highly time-resolved ambient measurements of SO2 and particulate pollutants influencing air quality at a site in Sydney, Florida, during the Tampa Bay Regional Aerosol Chemistry Experiment (BRACE) in May 2002. The PDRM explicitly exploits knowledge of the number and locations of major stationary sources, source and transport wind directions, stack gas emission parameters, and meteorological plume dispersion parameters during sample collections to constrain solutions for individual sources. Model outputs include average emission rates and time-resolved ambient concentrations for each of the measured species and time-resolved meteorological dispersion factors for each of the sources. The model was applied to ambient Federal Reference Method SO2 and 30-min elemental measurements during an 8.5-hour period when winds swept a 70° sector containing six large stationary sources. Agreement between predicted and observed ambient SO2 concentrations was extraordinarily good: The correlation coefficient (R2) was 0.97, their ratio was 1.00 ± 0.18, and predicted SO2 emission rates for each of four large utility sources lie within 8% of their average continuous emission monitor values. Mean fractional bias, normalized mean square error, and the fractions of the predictions within a factor of 2 of the observed values are −2.7, 0.9, and 94%, respectively. For elemental markers of coal-fired (As and Se) and oil-fired (Ni) power plant emissions the average ratio of predicted and observed concentrations was 1.02 ± 0.18 for As, 0.96 ± 0.17 for Se, and 0.99 ± 0.41 for Ni, indicating that the six sources located in the wind sector between approximately 200° and 260° well accounted for background-corrected concentrations measured at the sampling site. Model results were relatively insensitive to the choice of upper bound used to constrain solutions.