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Abstract As one of the least understood aerosol processes, nucleation can be a dominant source of atmospheric aerosols. Sulfuric acid (SA)-amine binary nucleation with dimethylamine (DMA) has been recognized as a governing mechanism in the polluted continental boundary layer. Here we demonstrate the importance of trimethylamine (TMA) for nucleation in the complex atmosphere and propose a molecular-level SA-DMA-TMA ternary nucleation mechanism as an improvement upon the conventional binary mechanism. Using the proposed mechanism, we could connect the gaseous amines to the SA-amine cluster signals measured in the atmosphere of urban Beijing. Results show that TMA can accelerate the SA-DMA-based new particle formation in Beijing by 50–100%. Considering the global abundance of TMA and DMA, our findings imply comparable importance of TMA and DMA to nucleation in the polluted continental boundary layer, with probably higher contributions from TMA in polluted rural environments and future urban environments with controlled DMA emissions. 

Abstract Transformation of low-volatility gaseous precursors to new particles affects aerosol number concentration, cloud formation and hence the climate. The clustering of acid and base molecules is a major mechanism driving fast nucleation and initial growth of new particles in the atmosphere. However, the acid–base cluster composition, measured using state-of-the-art mass spectrometers, cannot explain the measured high formation rate of new particles. Here we present strong evidence for the existence of base molecules such as amines in the smallest atmospheric sulfuric acid clusters prior to their detection by mass spectrometers. We demonstrate that forming (H2SO4)1(amine)1 is the rate-limiting step in atmospheric H2SO4-amine nucleation and the uptake of (H2SO4)1(amine)1 is a major pathway for the initial growth of H2SO4 clusters. The proposed mechanism is very consistent with measured new particle formation in urban Beijing, in which dimethylamine is the key base for H2SO4 nucleation while other bases such as ammonia may contribute to the growth of larger clusters. Our findings further underline the fact that strong amines, even at low concentrations and when undetected in the smallest clusters, can be crucial to particle formation in the planetary boundary layer. 

Abstract. It has been widely observed around the world that the frequency and intensityof new particle formation (NPF) events are reduced during periods of highrelative humidity (RH). The current study focuses on how RH affects theformation of highly oxidized molecules (HOMs), which are key components ofNPF and initial growth caused by oxidized organics. The ozonolysis ofα-pinene, limonene, and Δ³-carene, with and without OHscavengers, were carried out under low NO_x conditions undera range of RH (from ∼3 % to ∼92 %) in atemperature-controlled flow tube to generate secondary organic aerosol (SOA).A Scanning Mobility Particle Sizer (SMPS) was used to measure the sizedistribution of generated particles, and a novel transverse ionizationchemical ionization inlet with a high-resolution time-of-fight massspectrometer detected HOMs. A major finding from this work is that neitherthe detected HOMs nor their abundance changed significantly with RH, whichindicates that the detected HOMs must be formed from water-independentpathways. In fact, the distinguished OH- and O₃-derived peroxyradicals (RO₂), HOM monomers, and HOM dimers could mostly beexplained by the autoxidation of RO₂ followed by bimolecularreactions with other RO₂ or hydroperoxy radicals (HO₂),rather than from a water-influenced pathway like through the formation of astabilized Criegee intermediate (sCI). However, as RH increased from ∼3 % to ∼92 %, the total SOA number concentrations decreased bya factor of 2–3 while SOA mass concentrations remained relatively constant. These observations show that, whilehigh RH appears to inhibit NPF as evident by the decreasing numberconcentration, this reduction is not caused by a decrease inRO₂-derived HOM formation. Possible explanations for these phenomenawere discussed. 

To tackle the severe fine particle (PM_2.5) pollution in China, the government has implemented stringent control policies mainly on power plants, industry, and transportation since 2005, but estimates of the effectiveness of the policy and the temporal trends in health impacts are subject to large uncertainties. By adopting an integrated approach that combines chemical transport simulation, ambient/household exposure evaluation, and health-impact assessment, we find that the integrated population-weighted exposure to PM_2.5(IPWE) decreased by 47% (95% confidence interval, 37–55%) from 2005 [180 (146–219) μg/m³] to 2015 [96 (83–111) μg/m³]. Unexpectedly, 90% (86–93%) of such reduction is attributed to reduced household solid-fuel use, primarily resulting from rapid urbanization and improved incomes rather than specific control policies. The IPWE due to household fuels for both cooking and heating decreased, but the impact of cooking is significantly larger. The reduced household-related IPWE is estimated to avoid 0.40 (0.25–0.57) million premature deaths annually, accounting for 33% of the PM_2.5-induced mortality in 2015. The IPWE would be further reduced by 63% (57–68%) if the remaining household solid fuels were replaced by clean fuels, which would avoid an additional 0.51 (0.40–0.64) million premature deaths. Such a transition to clean fuels, especially for heating, requires technology innovation and policy support to overcome the barriers of high cost of distribution systems, as is recently being attempted in the Beijing–Tianjin–Hebei area. We suggest that household-fuel use be more highly prioritized in national control policies, considering its effects on PM_2.5exposures.