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Ammonia (NH 3) is a vital precursor of secondary aerosols, which play an important role in urban air pollution. The passive observation of NH 3 in the urban atmosphere showed higher concentrations than conventionally believed; however, the NH 3 dynamics remain limited due to the paucity of active measurements with fast response instruments. In this study, intensive online measurements of ambient NH 3 were conducted using cavity ring-down spectroscopy in late spring and early summer 2020 at the megacities of Beijing and Shanghai in northern and southern China. The results show that the average NH 3 concentration in Beijing (23.1 ± 10.3 ppb) was nearly double that in Shanghai (12.0 ± 5.0 ppb). This spatial difference was confirmed by satellite column observations and bottom-up emission patterns. In addition, there was a significant increase in NH 3 concentrations during the morning in our study. This special diurnal profile was a universal feature, with an occurrence frequency exceeding 50% in both cities. These frequent morning increases were mainly caused by motor vehicle emissions, with an additional contribution from the residual layer breakup for one-quarter of the days in the morning increase. On these days, the NH 3 concentration increased by approximately 20% due to the downward mixing of the residual layer rupture. The unique data observed here could be used to validate the chemistry and transport models at a higher time resolution and improve the understanding of the current status of NH 3 pollution in the urban atmosphere. [Display omitted] • 1 Hz NH 3 observations were conducted at megacities of Beijing and Shanghai. • Atmospheric NH 3 concentrations in urban Beijing were double that in Shanghai. • A morning pulse of NH 3 levels was a common feature at Beijing and Shanghai. • Highly frequent morning increases of NH 3 were mainly caused by vehicle emissions. • Boundary layer rupture further enhanced the rapid increase of NH 3 in the morning. [ABSTRACT FROM AUTHOR]