Ubiquitous atmospheric production of organic acids mediated by cloud droplets

Franco, Bruno; Blumenstock, Thomas; Cho, Changmin; Clarisse, Lieven; Clerbaux, Cathy; Coheur, Pierre‐François; Mazière, Martine De; Smedt, Isabelle De; Dorn, H.-P.; Emmerichs, Tamara; Fuchs, Hendrik; Gkatzelis, Georgios I.; Griffith, David; Gromov, Sergey; Hannigan, J. W.; Hase, Frank; Hohaus, Thorsten; Jones, Nicholas; Kerkweg, Astrid; Kiendler‐Scharr, Astrid; Lutsch, Erik; Mahieu, Emmanuel; Novelli, Anna; Ortega, Ivan; Paton-Walsh, Clare; Pommier, Matthieu; Pozzer, Andrea; Reimer, David; Rosanka, Simon; Sander, R.; Schneider, M.; Strong, Kimberly; Tillmann, Ralf; Roozendaël, Michel Van; Vereecken, Luc; Vigouroux, Corinne; Wahner, Andreas; Taraborrelli, Domenico

doi:10.1038/s41586-021-03462-x

Cited by 95 publications

(160 citation statements)

References 54 publications

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“…Although this underestimation of the model results is less apparent compared to that of the total column observations, it must be noted that only a limited number of merged data (53, see Table 2) is available for the comparison with aircraft observations and therefore such a comparison provides only an indication rather than a quantitative estimate. It must be stressed that Franco et al (2021) showed the importance of in-cloud chemistry for this tracer, which is missing in this study. The lack of adequate in-cloud chemistry would therefore explain the almost ubiquitous underestimation of this tracer.…”

Section: Hcoohmentioning

confidence: 63%

“…On the other hand, the large model versus observations differences in Southeast Asia also point to missing emissions from biomass burning. Finally, in-cloud chemistry could be important in the CH 3 COOH formation, analogously to formic acid (Franco et al, 2021), and this process could bring model results and observations to a closer agreement.…”

Section: Ch 3 Coohmentioning

confidence: 87%

“…MOM represents the chemistry of alkanes, alkenes, terpenes (isoprene and monoterpenes) and monocyclic aromatics. The mechanism has been employed to study the impact of isoprene OH−recycling above pristine tropical forests (Taraborrelli et al, 2012), oxidation of monoterpenes as a source of HO 2 (Hens et al, 2014;Mallik et al, 2018) and the influence of aromatics on tropospheric ozone (Taraborrelli et al, 2021). Furthermore, MOM has been used with extensions in order to simulate product yields of β-caryophyllene oxidation (van Eijck et al, 2013), the oxidation of alkyl amines and formamide as source of HNCO (Rosanka et al, 2020), the atmospheric losses of stabilised Criegee intermediates (Vereecken et al, 2017), and the most recent OH-recycling mechanisms in isoprene oxidation (Novelli et al, 2020).…”

Section: Introductionmentioning

confidence: 99%

“…(ii) primary species common to MIM and MOM would be influenced only by the different sinks (mainly OH), and a detail description of OH budget is presented here; (iii) the model bias with respect to secondary species, e.g. oxygenated VOCs, has been linked to a mis-representation or lack thereof processes like in-cloud chemistry (Rosanka et al, 2021b;Franco et al, 2021). Therefore any comparison of VOC simulations between MOM and MIM would not give any additional information on the model-observation discrepancy and aid any future model improvement.…”

Section: Introductionmentioning

confidence: 99%

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Simulation of organics in the atmosphere: evaluation of EMACv2.54 with the Mainz Organic Mechanism (MOM) coupled to the ORACLE (v1.0) submodel

Pozzer

Reifenberg

Kumar

et al. 2021

Preprint

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Abstract. An updated and expanded representation of organics in the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) has been evaluated. First, the comprehensive Mainz Organic Mechanism (MOM) in the submodel MECCA (Module Efficiently Calculating the Chemistry of the Atmosphere) was activated with explicit degradation of organic species up to five carbon atoms and a simplified mechanism for larger molecules. Second, the ORACLE submodel (version 1.0) considers now condensation on aerosols for all organics in the mechanism. Parameterizations for aerosol yields are used only for the lumped species that are not included in the explicit mechanism. The simultaneous usage of MOM and ORACLE allows an efficient estimation, not only of the chemical degradation of the simulated volatile organic compounds, but also of the contribution of organics to the growth and fate of (organic) aerosol, with a complexity of the mechanism largely increased compared to EMAC simulations with more simplified chemistry. The model evaluation presented here reveals that the OH concentration is well reproduced globally, while significant biases for observed oxygenated organics are present. We also investigate the general properties of the aerosols and their composition, showing that the more sophisticated and process-oriented secondary aerosol formation does not degrade the good agreement of previous model configurations with observations at the surface, allowing further research in the field of gas-aerosol interactions.

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Section: Hcoohmentioning

confidence: 63%

Section: Ch 3 Coohmentioning

confidence: 87%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Simulation of organics in the atmosphere: evaluation of EMACv2.54 with the Mainz Organic Mechanism (MOM) coupled to the ORACLE (v1.0) submodel

Pozzer

Reifenberg

Kumar

et al. 2021

Preprint

Self Cite

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“…They come from their dissolution from the gas and particulate phases or result from chemical transformations from organic precursors in the aqueous phase (Rose et al, 2018). For 400 example, the oxidative processing of aldehydes leads to the formation of carboxylic acids (Ervens et al, 2013;Franco et al, 2021) that can contribute to "aqSOA".…”

Section: Carboxylic Acidsmentioning

confidence: 99%

Insights into tropical cloud chemistry at Reunion Island (Indian Ocean): results from the BIO-MAÏDO campaign

Dominutti¹,

Renard²,

Vaïtilingom³

et al. 2021

Preprint

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Abstract. We present here the results obtained during an intensive field campaign conducted in the framework of the French “BIO-MAÏDO” (Bio-physico-chemistry of tropical clouds at Maïdo (Réunion Island): processes and impacts on secondary organic aerosols’ formation) project. This study integrates an exhaustive chemical and microphysical characterization of cloud water obtained in March–April 2019 at Reunion Island (Indian Ocean). Fourteen cloud samples have been collected along the slope of this mountainous island. A comprehensive chemical characterization of these samples is performed, including inorganic ions, metals, oxidants, and organic matter (organic acids, sugars, amino acids, carbonyls, and low-soluble volatile organic compounds (VOCs)). Cloud water presents high molecular complexity with elevated water-soluble organic matter content partly modulated by microphysical cloud properties. As expected, our findings show the presence of compounds of marine origin in cloud water samples (e.g., chloride, sodium) demonstrating ocean–cloud exchanges. However, the non-sea salt fraction of sulphate varies between 38 and 91 %, indicating the presence of other sources. Also, the presence of amino acids and for the first time in cloud waters of sugars, clearly indicates that biological activities contribute to the cloud water chemical composition. A significant variability between events is observed in the dissolved organic content (25.5 ± 18.4 mgC L−1), with levels reaching up to 62 mgC L−1. This variability was not similar for all the measured compounds, suggesting the presence of dissimilar emission sources or production mechanisms. For that, a statistical analysis is performed based on back-trajectory calculations using the CAT (Computing Atmospheric Trajectory Tool) model associated with land cover registry. These investigations reveal that air mass origins and microphysical variables do not fully explain the variability observed in cloud chemical composition, highlighting the complexity of emission sources, multiphasic transfer, and chemical processing in clouds. Additionally, several VOCs (oxygenated and low-soluble VOCs) were analysed in both gas and aqueous phases. Significant levels of biogenic low-soluble VOCs were detected in the aqueous phase, indicating the cloud-terrestrial vegetation exchange. Cloud scavenging of VOCs is assessed and compared to Henry’s law equilibrium to evaluate potential super or sub saturation conditions. The evaluation reveals the supersaturation of low-soluble VOCs from both natural and anthropogenic sources. Our results depict even higher supersaturation of terpenoids, suggesting their importance in the aqueous phase chemistry in highly impacted tropical areas.

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Changes in tropospheric air quality related to the protection of stratospheric ozone in a changing climate

Madronich

Sulzberger

Longstreth³

et al. 2023

Photochem Photobiol Sci

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Ultraviolet (UV) radiation drives the net production of tropospheric ozone (O3) and a large fraction of particulate matter (PM) including sulfate, nitrate, and secondary organic aerosols. Ground-level O3 and PM are detrimental to human health, leading to several million premature deaths per year globally, and have adverse effects on plants and the yields of crops. The Montreal Protocol has prevented large increases in UV radiation that would have had major impacts on air quality. Future scenarios in which stratospheric O3 returns to 1980 values or even exceeds them (the so-called super-recovery) will tend to ameliorate urban ground-level O3 slightly but worsen it in rural areas. Furthermore, recovery of stratospheric O3 is expected to increase the amount of O3 transported into the troposphere by meteorological processes that are sensitive to climate change. UV radiation also generates hydroxyl radicals (OH) that control the amounts of many environmentally important chemicals in the atmosphere including some greenhouse gases, e.g., methane (CH4), and some short-lived ozone-depleting substances (ODSs). Recent modeling studies have shown that the increases in UV radiation associated with the depletion of stratospheric ozone over 1980–2020 have contributed a small increase (~ 3%) to the globally averaged concentrations of OH. Replacements for ODSs include chemicals that react with OH radicals, hence preventing the transport of these chemicals to the stratosphere. Some of these chemicals, e.g., hydrofluorocarbons that are currently being phased out, and hydrofluoroolefins now used increasingly, decompose into products whose fate in the environment warrants further investigation. One such product, trifluoroacetic acid (TFA), has no obvious pathway of degradation and might accumulate in some water bodies, but is unlikely to cause adverse effects out to 2100. Graphical abstract

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Ubiquitous atmospheric production of organic acids mediated by cloud droplets

Cited by 95 publications

References 54 publications

Simulation of organics in the atmosphere: evaluation of EMACv2.54 with the Mainz Organic Mechanism (MOM) coupled to the ORACLE (v1.0) submodel

Simulation of organics in the atmosphere: evaluation of EMACv2.54 with the Mainz Organic Mechanism (MOM) coupled to the ORACLE (v1.0) submodel

Insights into tropical cloud chemistry at Reunion Island (Indian Ocean): results from the BIO-MAÏDO campaign

Changes in tropospheric air quality related to the protection of stratospheric ozone in a changing climate

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