Sulfate aerosols exert profound impacts on human and ecosystem health, weather, and climate, but their formation mechanism remains uncertain. Atmospheric models consistently underpredict sulfate levels under diverse environmental conditions. From atmospheric measurements in two Chinese megacities and complementary laboratory experiments, we show that the aqueous oxidation of SO 2 by NO 2 is key to efficient sulfate formation but is only feasible under two atmospheric conditions: on fine aerosols with high relative humidity and NH 3 neutralization or under cloud conditions. Under polluted environments, this SO 2 oxidation process leads to large sulfate production rates and promotes formation of nitrate and organic matter on aqueous particles, exacerbating severe haze development. Effective haze mitigation is achievable by intervening in the sulfate formation process with enforced NH 3 and NO 2 control measures. In addition to explaining the polluted episodes currently occurring in China and during the 1952 London Fog, this sulfate production mechanism is widespread, and our results suggest a way to tackle this growing problem in China and much of the developing world.sulfate aerosol | severe haze | pollution | human health | climate

Particles larger than 50-100 nm in diameter have been considered to be effective cloud condensation nuclei (CCN) under typical atmospheric conditions. We studied the growth of newly formed particles (NPs) in the atmosphere and the conditions for these particles to grow beyond 50 nm at a suburban coastal site in Hong Kong. Altogether, 17 new particle formation events each lasting over 1 h were observed in 17 days during 8 Mar-28 Apr and 1 Nov-30 Dec 2011. In 12 events, single-stage growth of NPs was observed in daytime when the median mobility diameter of NPs (Dp) increased up to ∼40 nm but did not increase further. In three events, two-stage particle growth to 61-97 nm was observed at nighttime. The second stage growth was preceded by a first-stage growth in daytime when the Dp reached 43 ± 4 nm. In all these 15 events, organics and sulfuric acid were major contributors to the first-stage growth in daytime. Ammonium nitrate unlikely contributed to the growth in daytime, but it was correlated with the second-stage growth of ∼40 nm NPs to CCN sizes at nighttime. The remaining two events apparently showed second-stage growth in late afternoon but were confirmed to be due to mixing of NPs with pre-existing particles. We conclude that daytime NP growth cannot reach CCN sizes at our site, but nighttime NP growth driven by organics and NH4NO3 can.

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