Urban pollution greatly enhances formation of natural aerosols over the Amazon rainforest

Shrivastava, Manish; Andreae, Meinrat O.; Artaxo, Paulo; Barbosa, H. M.; Berg, Larry K.; Brito, Joël; Ching, Joseph; Easter, Richard C.; Fan, Jiwen; Fast, Jerome D.; Feng, Zhe; Fuentes, José D.; Glasius, Marianne; Goldstein, Allen H.; Alves, Eliane Gomes; Gomes, Heliofábio Barros; Gu, Dasa; Guenther, Alex; Jathar, Shantanu H.; Kim, Saewung; Liu, Ying; Lou, Sijia; Martin, Scot T.; McNeill, V. Faye; Medeiros, Adan S. S.; de, Suzane S.; Shilling, John E.; Springston, Stephen; Souza, R. A. F. D.; Thornton, Joel A.; Isaacman‐VanWertz, Gabriel; Yee, L. D.; Ynoue, Rita Yuri; Zaveri, Rahul A.; Zelenyuk, Alla; Zhao, Chun

doi:10.1038/s41467-019-08909-4

Cited by 160 publications

(194 citation statements)

References 106 publications

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“…At the same time, NO x had little effect on the mass concentration of SOA. Other studies, on the other hand, indicate a strong increase in biogenic SOA due to NO x (e.g., Shrivastava et al, ). It is possible that organonitrate HOMs (HOM‐ONs), which are formed from biogenic vapors in the presence of NO x , are much less efficient in forming particles than other HOMs (Lehtipalo et al, ), probably due to their higher volatilities, but they might still be efficient in the aerosol growth.…”

Section: Nucleation and Growth Mechanisms: New Results From Laboratormentioning

confidence: 93%

“…Tröstl et al (2016) showed that GR of 5 to 50 nm particles cannot be explained by HOMs alone, suggesting that LVOCs that are not measured by the nitrate-CIMS and some additional SVOCs may be also involved in the growth. Hao et al (2009) Shrivastava et al, 2019). It is possible that organonitrate HOMs (HOM-ONs), which are formed from biogenic vapors in the presence of NO x , are much less efficient in forming particles than other HOMs , probably due to their higher volatilities, but they might still be efficient in the aerosol growth.…”

Section: Homs Formed From Vocs Oxidation Reactionsmentioning

confidence: 99%

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New Particle Formation in the Atmosphere: From Molecular Clusters to Global Climate

et al. 2019

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New particle formation (NPF) represents the first step in the complex processes leading to formation of cloud condensation nuclei. Newly formed nanoparticles affect human health, air quality, weather, and climate. This review provides a brief history, synthesizes recent significant progresses, and outlines the challenges and future directions for research relevant to NPF. New developments include the emergence of state‐of‐the‐art instruments that measure prenucleation clusters and newly nucleated nanoparticles down to about 1 nm; systematic laboratory studies of multicomponent nucleation systems, including collaborative experiments conducted in the Cosmics Leaving Outdoor Droplets chamber at CERN; observations of NPF in different types of forests, extremely polluted urban locations, coastal sites, polar regions, and high‐elevation sites; and improved nucleation theories and parameterizations to account for NPF in atmospheric models. The challenges include the lack of understanding of the fundamental chemical mechanisms responsible for aerosol nucleation and growth under diverse environments, the effects of SO2 and NOx on NPF, and the contribution of anthropogenic organic compounds to NPF. It is also critical to develop instruments that can detect chemical composition of particles from 3 to 20 nm and improve parameterizations to represent NPF over a wide range of atmospheric conditions of chemical precursor, temperature, and humidity.

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Section: Nucleation and Growth Mechanisms: New Results From Laboratormentioning

confidence: 93%

Section: Homs Formed From Vocs Oxidation Reactionsmentioning

confidence: 99%

New Particle Formation in the Atmosphere: From Molecular Clusters to Global Climate

et al. 2019

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“…The dependence of OH on NO 2 concentrations inferred from the analysis in Figure is consistent with several previous observations, including the Tropospheric OH Photochemistry Experiment (Eisele et al, ), measurements made during the Biosphere Effects on Aerosols and Photochemistry Experiment II (BEARPEX09) (Mao et al, ), measurements made at a ground site during the SENEX study (Feiner et al, ), and with the OH dependence on NO 2 predicted from well‐known chemical reactions in the troposphere (McKeen et al, ). Indirect evidence for increased oxidation rates of VOCs at enhanced NO x concentrations was obtained downwind from Manaus in the Amazon during GoAmazon2014/5 (Shrivastava et al, ). Our analysis does not provide evidence for higher than expected OH concentrations at lower NO x concentrations as suggested by the recent summary of OH measurements (Rohrer et al, ).…”

Section: Resultsmentioning

confidence: 99%

Hydrocarbon Removal in Power Plant Plumes Shows Nitrogen Oxide Dependence of Hydroxyl Radicals

Gouw

Parrish

Brown

et al. 2019

Geophysical Research Letters

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During an airborne study in the Southeast United States, measured mixing ratios of biogenic hydrocarbons were systematically lower in air masses containing enhanced nitrogen oxides from power plants, which we attribute to increased concentrations of hydroxyl (OH) radicals within the power plant plumes. Plume transects at successively further downwind distances provide a decreasing gradient of nitrogen oxides (NOx) concentrations, which together with the implied loss rates of isoprene, constrains the OH dependence on NOx. We find that OH concentrations were highest at nitrogen dioxide concentrations near 1–2 ppbv and decreased at higher and at lower concentrations. These findings agree with the dependence of OH on NOx concentrations expected from known chemical reactions but are not consistent with some studies reporting direct OH measurements higher than expected in regions of the atmosphere with low NOx (NO < 0.08 and NO2 < 0.46 ppbv) and high biogenic hydrocarbon emissions.

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“…δ-limonene is the most emitted monoterpene (45%), followed by trans-β-ocimene (18%) and α-pinene (17%). NO soil emissions are also accounted for with a constant flux of 8.3×10 9 molec cm −2 s −1 following Shrivastava et al (2019).…”

Section: Biogenic Emissionsmentioning

confidence: 99%

“…Koss et al, 2017a, b), such 50 measurements are not available for the GoAmazon 2014/5 campaign. 3D models that were run for the Manaus situation offer an anonymized view of SOA composition (Shrivastava et al, 2019) because they rely on a Volatility Basis Set parameterization (VBS, Donahue et al, 2006). The Generator for Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A, Aumont et al, 2005;Camredon et al, 2007) is the ideal tool to model atmospheric organic chemistry with a detailed molecular view.…”

mentioning

confidence: 99%

Impact of Urban Emissions on a Biogenic Environment during the wet season: Explicit Modeling of the Manaus Plume Organic Chemistry with GECKO-A

Mouchel‐Vallon

Lee-Taylor

Hodžić

et al. 2019

Preprint

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The GoAmazon 2014/5 field campaign took place in Manaus (Brazil) and allowed the investigation the interaction between background level biogenic air masses and anthropogenic plumes. We present in this work a box model built to simulate the impact of urban chemistry on biogenic Secondary Organic Aerosol (SOA) formation and composition. An organic chemistry mechanism is generated with the Generator for Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) to simulate the explicit oxidation of biogenic and anthropogenic compounds. A parameterization is also included to account for 5 the reactive uptake of isoprene oxidation products on aqueous particles. After some reductions of biogenic emissions relative to existing emission inventories, the model is able to reproduce measured primary compounds, ozone and NOx for clean or polluted situations. The explicit model is able to reproduce background case SOA mass concentrations but is underestimating the enhancement observed in the urban plume. Oxidation of biogenic compounds is the major contributor to SOA mass. A Volatility Basis Set parameterization (VBS) applied to the same cases obtains better results than GECKO-A for predicting 10 SOA mass in the box model. The explicit mechanism may be missing SOA formation processes related to the oxidation of monoterpenes that could be implicitly accounted for in the VBS parameterization.

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Urban pollution greatly enhances formation of natural aerosols over the Amazon rainforest

Cited by 160 publications

References 106 publications

New Particle Formation in the Atmosphere: From Molecular Clusters to Global Climate

New Particle Formation in the Atmosphere: From Molecular Clusters to Global Climate

Hydrocarbon Removal in Power Plant Plumes Shows Nitrogen Oxide Dependence of Hydroxyl Radicals

Impact of Urban Emissions on a Biogenic Environment during the wet season: Explicit Modeling of the Manaus Plume Organic Chemistry with GECKO-A

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