Time-resolved wind tunnel experiments are performed for three periodic street canyon configurations: one of uniform (H/W = 1) and two of variable building height (consisting of 0.5H and 1.5H tall towers in aligned and staggered arrangements) for perpendicular wind direction. The velocity field is mapped using Laser Doppler Anemometry (LDA), and the tracer gas concentration is sampled using Fast Flame Ionization Detection (FFID). The concentration field is characterized by the mean concentration and the characteristic percentiles of the concentration-time series, such as the median and the peak, represented by the 99th percentile, in a total of 1138 sampling points. The probability distribution of the concentration in each point is modeled using the gamma distribution, which is fitted based on the mean and the variance of the measured time series. The results show that the mean pedestrian exposure to air pollutants is significantly lower in the case of heterogeneous roof height, although the mean concentration at the leeward corner of the source canyon can locally exceed those of the uniform street canyons for both tower arrangements of variable building height. Moreover, it is shown that the concentration peaks for both tower configurations can significantly exceed those of the uniform canyons case, especially near the sources.