Sources and sinks driving sulfuric acid concentrations in contrasting environments: implications on proxy calculations

Dada, Lubna; Ylivinkka, Ilona; Baalbaki, Rima; Li, Chang; Guo, Yishuo; Yan, Chao; Yao, Lei; Sarnela, Nina; Jokinen, Tuija; Daellenbach, Kaspar R.; Yin, Rujing; Deng, Chao; Chu, Biwu; Nieminen, Tuomo; Wang, Yonghong; Lin, Zongkai; Thakur, Roseline C.; Kontkanen, Jenni; Stolzenburg, Dominik; Sipilä, Mikko; Hussein, Tareq; Paasonen, Pauli; Bianchi, Federico; Salma, Imre; Weidinger, Tamás; Pikridas, Michael; Sciare, Jean; Jiang, Jingkun; Liu, Yongchun; Petäj̈ä, Tuukka; Kerminen, Veli‐Matti; Kulmala, Markku

doi:10.5194/acp-20-11747-2020

Cited by 47 publications

(112 citation statements)

References 65 publications

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“…S8), indicating that HOMs were not the main driver for the formation of sub-3 nm particles. This phenomenon is in contrast with some previous observations in forested areas where oxidation products of biogenic VOCs, especially monoterpene, were the main contributor to the formation of clusters (Eerdekens et al, 2009;Lehtipalo et al, 2011;Kammer et al, 2018;Rose et al, 2018). Both observation (Rose et al, 2018) and laboratory experiments (Lehtipalo et al, 2018) have shown that HOM dimers with extremely low volatility play a key role in the initial forma- (Almeida et al, 2013;Kirkby et al, 2011).…”

Section: Atmospheric Implication: Contribution Of Nighttime Sulfuric Acid To Sub-3 Nm Particlescontrasting

confidence: 77%

Formation of nighttime sulfuric acid from the ozonolysis of alkenes in Beijing

Guo

Yan

et al. 2021

Atmos. Chem. Phys.

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Abstract. Gaseous sulfuric acid (SA) has received a lot of attention for its crucial role in atmospheric new particle formation (NPF). And for this reason, studies until now have mainly focused on daytime SA when most NPF events occur. While daytime SA production is driven by SO2 oxidation of OH radicals of photochemical origin, the formation of SA during nighttime and its potential influence on particle formation remains poorly understood. Here we present evidence for significant nighttime SA production in urban Beijing during winter, yielding concentrations between 1.0 and 3.0 × 106 cm−3. We found a high frequency (∼ 30 %) of nighttime SA events, which are defined by the appearance of a distinct SA peak observed between 20:00 and 04:00 local time, with the maximum concentration exceeding 1.0 × 106 cm−3. These events mostly occurred during unpolluted nights with a low vapor condensation sink. Furthermore, we found that under very clean conditions (visibility > 16.0 km) with abundant ozone (concentration > 2.0 × 1011 cm−3, ∼ 7 ppb), the overall sink of SA was strongly correlated with the products of O3, alkenes and SO2 concentrations, suggesting that the ozonolysis of alkenes played a major role in nighttime SA formation under such conditions. This is in light of previous studies showing that the ozonolysis of alkenes can form OH radicals and stabilized Criegee intermediates (SCIs), both of which are able to oxidize SO2 and thus lead to SA formation. However, we also need to point out that there exist additional sources of SA under more polluted conditions, which are not investigated in this study. Moreover, there was a strong correlation between SA concentration and the number concentration of sub-3 nm particles on both clean and polluted nights. Different from forest environments, where oxidized biogenic vapors are the main driver of nighttime clustering, our study demonstrates that the formation of nighttime cluster mode particles in urban environments is mainly driven by nighttime SA production.

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Section: Atmospheric Implication: Contribution Of Nighttime Sulfuric Acid To Sub-3 Nm Particlescontrasting

confidence: 77%

Formation of nighttime sulfuric acid from the ozonolysis of alkenes in Beijing

Guo

Yan

et al. 2021

Atmos. Chem. Phys.

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“…Thus, nucleating aerosols can largely contribute to the available aerosol surface area. The NPF frequency typically decreases with an increasing CS (Pikridas et al, 2012;Salma et al, 2016a;Dada et al, 2017;Dai et al, 2017;Hakala et al, 2019;Hussein et al, 2020). However, NPF has been observed in polluted environments at exceptionally high values of CS, indicating that inefficient cluster scavenging or enhanced cluster growth (or a combination of both) drives NPF regardless of the high load of pre-existing particles (Yao et al, 2018;Kulmala et al, 2017).…”

Section: The Driving Atmospheric Parameters Of the Npf Eventsmentioning

confidence: 99%

Towards understanding the characteristics of new particle formation in the Eastern Mediterranean

et al. 2021

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Abstract. To quantify the contribution of new particle formation (NPF) to ultrafine particle number and cloud condensation nuclei (CCN) budgets, one has to understand the mechanisms that govern NPF in different environments and its temporal extent. Here, we study NPF in Cyprus, an Eastern Mediterranean country located at the crossroads of three continents and affected by diverse air masses originating from continental, maritime, and desert-dust source areas. We performed 1-year continuous measurements of aerosol particles down to ∼ 1 nm in diameter for the first time in the Eastern Mediterranean and Middle East (EMME) region. These measurements were complemented with trace gas data, meteorological variables, and retroplume analysis. We show that NPF is a very frequent phenomenon at this site and has higher frequencies of occurrence during spring and autumn. NPF events were both of local and regional origin, and the local events occurred frequently during the month with the lowest NPF frequency. Some NPF events exhibited multiple onsets, while others exhibited apparent particle shrinkage in size. Additionally, NPF events were observed during the nighttime and during episodes of high desert-dust loadings. Particle formation rates and growth rates were comparable to those in urban environments, although our site is a rural one. Meteorological variables and trace gases played a role in explaining the intra-monthly variability of NPF events, but they did not explain why summer months had the least NPF frequency. Similarly, pre-existing aerosol loading did not explain the observed seasonality. The months with the least NPF frequency were associated with higher H2SO4 concentrations but lower NO2 concentrations, which is an indicator of anthropogenic influence. Air masses arriving from the Middle East were not observed during these months, which could suggest that precursor vapors important for nucleation and growth are transported to our site from the Middle East. Further comprehensive measurements of precursor vapors are required to prove this hypothesis.

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“…Lu et al 26 took into account O 3 and HONO concentrations to differentiate between OH originating from the O 3 and HONO photolysis. Dada et al 18 added the reaction of SO 2 with sCI as an additional H 2 SO 4 source to the proxy. These efforts largely improved the understanding of H 2 SO 4 in different environments, however, with obvious limitations.…”

Section: Introductionmentioning

confidence: 99%

Toward Building a Physical Proxy for Gas-Phase Sulfuric Acid Concentration Based on Its Budget Analysis in Polluted Yangtze River Delta, East China

Li-wen

Nie

Liu

et al. 2021

Environ. Sci. Technol.

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Gaseous sulfuric acid (H 2 SO 4 ) is a crucial precursor for secondary aerosol formation, particularly for new particle formation (NPF) that plays an essential role in the global number budget of aerosol particles and cloud condensation nuclei. Due to technology challenges, global-wide and long-term measurements of gaseous H 2 SO 4 are currently very challenging. Empirical proxies for H 2 SO 4 have been derived mainly based on short-term intensive campaigns. In this work, we performed comprehensive measurements of H 2 SO 4 and related parameters in the polluted Yangtze River Delta in East China during four seasons and developed a physical proxy based on the budget analysis of gaseous H 2 SO 4 . Besides the photo-oxidation of SO 2 , we found that primary emissions can contribute considerably, particularly at night. Dry deposition has the potential to be a non-negligible sink, in addition to condensation onto particle surfaces. Compared with the empirical proxies, the newly developed physical proxy demonstrates extraordinary stability in all the seasons and has the potential to be widely used to improve the understanding of global NPF fundamentally.

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Sources and sinks driving sulfuric acid concentrations in contrasting environments: implications on proxy calculations

Cited by 47 publications

References 65 publications

Formation of nighttime sulfuric acid from the ozonolysis of alkenes in Beijing

Formation of nighttime sulfuric acid from the ozonolysis of alkenes in Beijing

Towards understanding the characteristics of new particle formation in the Eastern Mediterranean

Toward Building a Physical Proxy for Gas-Phase Sulfuric Acid Concentration Based on Its Budget Analysis in Polluted Yangtze River Delta, East China

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