Articles | Volume 23, issue 10
https://doi.org/10.5194/acp-23-5851-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-23-5851-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
On the importance of multiphase photolysis of organic nitrates on their global atmospheric removal
Juan Miguel González-Sánchez
CORRESPONDING AUTHOR
Aix Marseille
Univ, CNRS, LCE, Marseille, France
Aix Marseille
Univ, CNRS, ICR, Marseille, France
Nicolas Brun
Aix Marseille
Univ, CNRS, LCE, Marseille, France
Aix Marseille
Univ, CNRS, ICR, Marseille, France
Junteng Wu
Aix Marseille
Univ, CNRS, LCE, Marseille, France
Sylvain Ravier
Aix Marseille
Univ, CNRS, LCE, Marseille, France
Jean-Louis Clément
Aix Marseille
Univ, CNRS, ICR, Marseille, France
Anne Monod
CORRESPONDING AUTHOR
Aix Marseille
Univ, CNRS, LCE, Marseille, France
Related authors
Juan Miguel González-Sánchez, Miquel Huix-Rotllant, Nicolas Brun, Julien Morin, Carine Demelas, Amandine Durand, Sylvain Ravier, Jean-Louis Clément, and Anne Monod
Atmos. Chem. Phys., 23, 15135–15147, https://doi.org/10.5194/acp-23-15135-2023, https://doi.org/10.5194/acp-23-15135-2023, 2023
Short summary
Short summary
Organic nitrates play a crucial role in air pollution, as they are nitrogen oxide (NOx) reservoirs. This work investigated the reaction products and mechanisms of their reactivity with light in the aqueous phase (cloud and fog conditions and wet aerosol). Our findings reveal that this chemistry leads to the formation of atmospheric nitrous acid (HONO).
Junteng Wu, Nicolas Brun, Juan Miguel González-Sánchez, Badr R'Mili, Brice Temime Roussel, Sylvain Ravier, Jean-Louis Clément, and Anne Monod
Atmos. Meas. Tech., 15, 3859–3874, https://doi.org/10.5194/amt-15-3859-2022, https://doi.org/10.5194/amt-15-3859-2022, 2022
Short summary
Short summary
This work quantified and tentatively identified the organic impurities on ammonium sulfate aerosols generated in the laboratory. They are likely low volatile and high mass molecules containing oxygen, nitrogen, and/or sulfur. Our results show that these organic impurities likely originate from the commercial AS crystals. It is recommended to use AS seeds with caution, especially when small particles are used, in terms of AS purity and water purity when aqueous solutions are used for atomization.
Juan Miguel González-Sánchez, Nicolas Brun, Junteng Wu, Julien Morin, Brice Temime-Roussel, Sylvain Ravier, Camille Mouchel-Vallon, Jean-Louis Clément, and Anne Monod
Atmos. Chem. Phys., 21, 4915–4937, https://doi.org/10.5194/acp-21-4915-2021, https://doi.org/10.5194/acp-21-4915-2021, 2021
Short summary
Short summary
Organic nitrates play a crucial role in air pollution as they are considered NOx reservoirs. This work lights up the importance of their reactions with OH radicals in the aqueous phase (cloud/fog, wet aerosol), which is slower than in the gas phase. For compounds that significantly partition in water such as polyfunctional biogenic nitrates, these aqueous-phase reactions should drive their atmospheric removal, leading to a broader spatial distribution of NOx than previously accounted for.
Anil Kumar Mandariya, Junteng Wu, Anne Monod, Paola Formenti, Bénédicte Picquet-Varrault, Mathieu Cazaunau, Stephan Mertes, Laurent Poulain, Antonin Berge, Edouard Pangui, Andreas Tilgner, Thomas Schaefer, Liang Wen, Hartmut Herrmann, and Jean-François Doussin
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2023-206, https://doi.org/10.5194/amt-2023-206, 2024
Revised manuscript has not been submitted
Short summary
Short summary
An optimized and controlled protocol for generating quasi-adiabatic expansion clouds under simulated dark and light conditions was presented. The irradiated clouds clearly showed a gradual activation of seed particles into droplets. In contrast, non-irradiated clouds faced a flash activation. This paper will lay the foundation for multiphase photochemical studies implying water-soluble volatile organic compounds and particulate matter formation during cloud formation-evaporation cycles.
Juan Miguel González-Sánchez, Miquel Huix-Rotllant, Nicolas Brun, Julien Morin, Carine Demelas, Amandine Durand, Sylvain Ravier, Jean-Louis Clément, and Anne Monod
Atmos. Chem. Phys., 23, 15135–15147, https://doi.org/10.5194/acp-23-15135-2023, https://doi.org/10.5194/acp-23-15135-2023, 2023
Short summary
Short summary
Organic nitrates play a crucial role in air pollution, as they are nitrogen oxide (NOx) reservoirs. This work investigated the reaction products and mechanisms of their reactivity with light in the aqueous phase (cloud and fog conditions and wet aerosol). Our findings reveal that this chemistry leads to the formation of atmospheric nitrous acid (HONO).
Junteng Wu, Nicolas Brun, Juan Miguel González-Sánchez, Badr R'Mili, Brice Temime Roussel, Sylvain Ravier, Jean-Louis Clément, and Anne Monod
Atmos. Meas. Tech., 15, 3859–3874, https://doi.org/10.5194/amt-15-3859-2022, https://doi.org/10.5194/amt-15-3859-2022, 2022
Short summary
Short summary
This work quantified and tentatively identified the organic impurities on ammonium sulfate aerosols generated in the laboratory. They are likely low volatile and high mass molecules containing oxygen, nitrogen, and/or sulfur. Our results show that these organic impurities likely originate from the commercial AS crystals. It is recommended to use AS seeds with caution, especially when small particles are used, in terms of AS purity and water purity when aqueous solutions are used for atomization.
Patrick Chazette, Cyrille Flamant, Harald Sodemann, Julien Totems, Anne Monod, Elsa Dieudonné, Alexandre Baron, Andrew Seidl, Hans Christian Steen-Larsen, Pascal Doira, Amandine Durand, and Sylvain Ravier
Atmos. Chem. Phys., 21, 10911–10937, https://doi.org/10.5194/acp-21-10911-2021, https://doi.org/10.5194/acp-21-10911-2021, 2021
Short summary
Short summary
To gain understanding on the vertical structure of atmospheric water vapour above mountain lakes and to assess its link to the isotopic composition of the lake water and small-scale dynamics, the L-WAIVE field campaign was conducted in the Annecy valley in the French Alps in June 2019. Based on a synergy between ground-based, boat-borne, and airborne measuring platforms, significant gradients of isotopic content have been revealed at the transitions to the lake and to the free troposphere.
Juan Miguel González-Sánchez, Nicolas Brun, Junteng Wu, Julien Morin, Brice Temime-Roussel, Sylvain Ravier, Camille Mouchel-Vallon, Jean-Louis Clément, and Anne Monod
Atmos. Chem. Phys., 21, 4915–4937, https://doi.org/10.5194/acp-21-4915-2021, https://doi.org/10.5194/acp-21-4915-2021, 2021
Short summary
Short summary
Organic nitrates play a crucial role in air pollution as they are considered NOx reservoirs. This work lights up the importance of their reactions with OH radicals in the aqueous phase (cloud/fog, wet aerosol), which is slower than in the gas phase. For compounds that significantly partition in water such as polyfunctional biogenic nitrates, these aqueous-phase reactions should drive their atmospheric removal, leading to a broader spatial distribution of NOx than previously accounted for.
Camille Mouchel-Vallon, Laurent Deguillaume, Anne Monod, Hélène Perroux, Clémence Rose, Giovanni Ghigo, Yoann Long, Maud Leriche, Bernard Aumont, Luc Patryl, Patrick Armand, and Nadine Chaumerliac
Geosci. Model Dev., 10, 1339–1362, https://doi.org/10.5194/gmd-10-1339-2017, https://doi.org/10.5194/gmd-10-1339-2017, 2017
Short summary
Short summary
The Cloud Explicit Physico-chemical Scheme (CLEPS 1.0) describes oxidation of water-soluble organic compounds resulting from isoprene oxidation. It is based on structure activity relationships (SARs) (global rate constants and branching ratios for HO• abstraction and addition) and GROMHE SAR (Henry's law constants for undocumented species). It is coupled to the MCM gas phase mechanism and is included in a model using the DSMACC model and KPP to analyze experimental and field data.
L. Brégonzio-Rozier, C. Giorio, F. Siekmann, E. Pangui, S. B. Morales, B. Temime-Roussel, A. Gratien, V. Michoud, M. Cazaunau, H. L. DeWitt, A. Tapparo, A. Monod, and J.-F. Doussin
Atmos. Chem. Phys., 16, 1747–1760, https://doi.org/10.5194/acp-16-1747-2016, https://doi.org/10.5194/acp-16-1747-2016, 2016
Short summary
Short summary
The impact of cloud events on isoprene secondary organic aerosol (SOA) formation has been studied from an isoprene/ NOx/light system in an atmospheric simulation chamber. aqSOA formation can be linked to water soluble volatile organic compounds' dissolution in the aqueous phase and to further aqueous phase reactions. Cloud-induced SOA formation is experimentally demonstrated in this study, thus highlighting the importance of aqueous multiphase systems in atmospheric SOA formation estimations.
B. Ervens, P. Renard, S. Tlili, S. Ravier, J.-L. Clément, and A. Monod
Atmos. Chem. Phys., 15, 9109–9127, https://doi.org/10.5194/acp-15-9109-2015, https://doi.org/10.5194/acp-15-9109-2015, 2015
Short summary
Short summary
A detailed chemical mechanism is developed based on laboratory studies that predicts the formation of high molecular weight compounds in the aqueous phase of atmospheric aerosol particles. Model simulations using this mechanism for atmospheric conditions show that these pathways are likely not a substantial source of particle mass, unless unidentified precursors for these compounds exist that were not taken into account so far and/or the solubility of oxygen in aerosol water is overestimated.
H. L. DeWitt, S. Hellebust, B. Temime-Roussel, S. Ravier, L. Polo, V. Jacob, C. Buisson, A. Charron, M. André, A. Pasquier, J. L. Besombes, J. L. Jaffrezo, H. Wortham, and N. Marchand
Atmos. Chem. Phys., 15, 4373–4387, https://doi.org/10.5194/acp-15-4373-2015, https://doi.org/10.5194/acp-15-4373-2015, 2015
Short summary
Short summary
By performing source-apportionment modeling, the amount of primary and secondary organic emissions was resolved from a bulk aerosol data set measured adjacent to a major highway in France. Over 70% of vehicles on this highway were diesel, and a high concentration of BC and NOx were measured. Even close to a major highway, the bulk of the aerosol mass was secondary in nature. Radiocarbon data revealed that most of the fossil organic carbon was from primary vehicular emissions and not from SOA.
C. Denjean, P. Formenti, B. Picquet-Varrault, E. Pangui, P. Zapf, Y. Katrib, C. Giorio, A. Tapparo, A. Monod, B. Temime-Roussel, P. Decorse, C. Mangeney, and J. F. Doussin
Atmos. Chem. Phys., 15, 3339–3358, https://doi.org/10.5194/acp-15-3339-2015, https://doi.org/10.5194/acp-15-3339-2015, 2015
L. Brégonzio-Rozier, F. Siekmann, C. Giorio, E. Pangui, S. B. Morales, B. Temime-Roussel, A. Gratien, V. Michoud, S. Ravier, M. Cazaunau, A. Tapparo, A. Monod, and J.-F. Doussin
Atmos. Chem. Phys., 15, 2953–2968, https://doi.org/10.5194/acp-15-2953-2015, https://doi.org/10.5194/acp-15-2953-2015, 2015
Short summary
Short summary
First- and higher order -generation products formed from the oxidation of isoprene and methacrolein with OH radicals in the presence of NOx have been studied in a simulation chamber. Differences in light source are proposed to partially explain the discrepancies observed between different studies in the literature for both isoprene- and methacrolein-SOA mass yields. According to our results, these SOA yields in the atmosphere could be lower than suggested by most of the current chamber studies.
C. Denjean, P. Formenti, B. Picquet-Varrault, M. Camredon, E. Pangui, P. Zapf, Y. Katrib, C. Giorio, A. Tapparo, B. Temime-Roussel, A. Monod, B. Aumont, and J. F. Doussin
Atmos. Chem. Phys., 15, 883–897, https://doi.org/10.5194/acp-15-883-2015, https://doi.org/10.5194/acp-15-883-2015, 2015
P. Renard, F. Siekmann, G. Salque, C. Demelas, B. Coulomb, L. Vassalo, S. Ravier, B. Temime-Roussel, D. Voisin, and A. Monod
Atmos. Chem. Phys., 15, 21–35, https://doi.org/10.5194/acp-15-21-2015, https://doi.org/10.5194/acp-15-21-2015, 2015
J.-F. Doussin and A. Monod
Atmos. Chem. Phys., 13, 11625–11641, https://doi.org/10.5194/acp-13-11625-2013, https://doi.org/10.5194/acp-13-11625-2013, 2013
P. Renard, F. Siekmann, A. Gandolfo, J. Socorro, G. Salque, S. Ravier, E. Quivet, J.-L. Clément, M. Traikia, A.-M. Delort, D. Voisin, V. Vuitton, R. Thissen, and A. Monod
Atmos. Chem. Phys., 13, 6473–6491, https://doi.org/10.5194/acp-13-6473-2013, https://doi.org/10.5194/acp-13-6473-2013, 2013
Related subject area
Subject: Clouds and Precipitation | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Direct formation of HONO through aqueous-phase photolysis of organic nitrates
Effects of pH and light exposure on the survival of bacteria and their ability to biodegrade organic compounds in clouds: implications for microbial activity in acidic cloud water
Towards a chemical mechanism of the oxidation of aqueous sulfur dioxide via isoprene hydroxyl hydroperoxides (ISOPOOH)
On the importance of atmospheric loss of organic nitrates by aqueous-phase ●OH oxidation
Lignin's ability to nucleate ice via immersion freezing and its stability towards physicochemical treatments and atmospheric processing
Biodegradation of phenol and catechol in cloud water: comparison to chemical oxidation in the atmospheric multiphase system
Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions – Part 2: Quartz and amorphous silica
Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions – Part 3: Aluminosilicates
Aqueous reactions of organic triplet excited states with atmospheric alkenes
The quasi-liquid layer of ice revisited: the role of temperature gradients and tip chemistry in AFM studies
Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions – Part 1: The K-feldspar microcline
Direct molecular-level characterization of different heterogeneous freezing modes on mica – Part 1
Chemistry of riming: the retention of organic and inorganic atmospheric trace constituents
Surface-charge-induced orientation of interfacial water suppresses heterogeneous ice nucleation on α-alumina (0001)
Screening of cloud microorganisms isolated at the Puy de Dôme (France) station for the production of biosurfactants
Comparing contact and immersion freezing from continuous flow diffusion chambers
A better understanding of hydroxyl radical photochemical sources in cloud waters collected at the puy de Dôme station – experimental versus modelled formation rates
Deposition and immersion-mode nucleation of ice by three distinct samples of volcanic ash
Organic matter matters for ice nuclei of agricultural soil origin
Effect of atmospheric organic complexation on iron-bearing dust solubility
Are sesquiterpenes a good source of secondary organic cloud condensation nuclei (CCN)? Revisiting β-caryophyllene CCN
Ice nucleation efficiency of clay minerals in the immersion mode
Atmospheric chemistry of carboxylic acids: microbial implication versus photochemistry
Yields of hydrogen peroxide from the reaction of hydroxyl radical with organic compounds in solution and ice
In-cloud processes of methacrolein under simulated conditions – Part 1: Aqueous phase photooxidation
In-cloud processes of methacrolein under simulated conditions – Part 2: Formation of secondary organic aerosol
Juan Miguel González-Sánchez, Miquel Huix-Rotllant, Nicolas Brun, Julien Morin, Carine Demelas, Amandine Durand, Sylvain Ravier, Jean-Louis Clément, and Anne Monod
Atmos. Chem. Phys., 23, 15135–15147, https://doi.org/10.5194/acp-23-15135-2023, https://doi.org/10.5194/acp-23-15135-2023, 2023
Short summary
Short summary
Organic nitrates play a crucial role in air pollution, as they are nitrogen oxide (NOx) reservoirs. This work investigated the reaction products and mechanisms of their reactivity with light in the aqueous phase (cloud and fog conditions and wet aerosol). Our findings reveal that this chemistry leads to the formation of atmospheric nitrous acid (HONO).
Yushuo Liu, Chee Kent Lim, Zhiyong Shen, Patrick K. H. Lee, and Theodora Nah
Atmos. Chem. Phys., 23, 1731–1747, https://doi.org/10.5194/acp-23-1731-2023, https://doi.org/10.5194/acp-23-1731-2023, 2023
Short summary
Short summary
We investigated how cloud water pH and solar radiation impact the survival and energetic metabolism of two neutrophilic bacteria species and their biodegradation of organic acids. Experiments were performed using artificial cloud water that mimicked the pH and composition of cloud water in South China. We found that there is a minimum cloud water pH threshold at which neutrophilic bacteria will survive and biodegrade organic compounds in cloud water during the daytime and/or nighttime.
Eleni Dovrou, Kelvin H. Bates, Jean C. Rivera-Rios, Joshua L. Cox, Joshua D. Shutter, and Frank N. Keutsch
Atmos. Chem. Phys., 21, 8999–9008, https://doi.org/10.5194/acp-21-8999-2021, https://doi.org/10.5194/acp-21-8999-2021, 2021
Short summary
Short summary
We examined the mechanism and products of oxidation of dissolved sulfur dioxide with the main isomers of isoprene hydroxyl hydroperoxides, via laboratory and model analysis. Two chemical mechanism pathways are proposed and the results provide an improved understanding of the broader atmospheric chemistry and role of multifunctional organic hydroperoxides, which should be the dominant VOC oxidation products under low-NO conditions, highlighting their significant contribution to sulfate formation.
Juan Miguel González-Sánchez, Nicolas Brun, Junteng Wu, Julien Morin, Brice Temime-Roussel, Sylvain Ravier, Camille Mouchel-Vallon, Jean-Louis Clément, and Anne Monod
Atmos. Chem. Phys., 21, 4915–4937, https://doi.org/10.5194/acp-21-4915-2021, https://doi.org/10.5194/acp-21-4915-2021, 2021
Short summary
Short summary
Organic nitrates play a crucial role in air pollution as they are considered NOx reservoirs. This work lights up the importance of their reactions with OH radicals in the aqueous phase (cloud/fog, wet aerosol), which is slower than in the gas phase. For compounds that significantly partition in water such as polyfunctional biogenic nitrates, these aqueous-phase reactions should drive their atmospheric removal, leading to a broader spatial distribution of NOx than previously accounted for.
Sophie Bogler and Nadine Borduas-Dedekind
Atmos. Chem. Phys., 20, 14509–14522, https://doi.org/10.5194/acp-20-14509-2020, https://doi.org/10.5194/acp-20-14509-2020, 2020
Short summary
Short summary
To study the role of organic matter in ice crystal formation, we investigated the ice nucleation ability of a subcomponent of organic aerosols, the biopolymer lignin, using a droplet-freezing technique. We found that lignin is an ice-active macromolecule with changing abilities based on dilutions. The effects of atmospheric processing and of physicochemical treatments on the ability of lignin solutions to freeze were negligible. Thus, lignin is a recalcitrant ice-nucleating macromolecule.
Saly Jaber, Audrey Lallement, Martine Sancelme, Martin Leremboure, Gilles Mailhot, Barbara Ervens, and Anne-Marie Delort
Atmos. Chem. Phys., 20, 4987–4997, https://doi.org/10.5194/acp-20-4987-2020, https://doi.org/10.5194/acp-20-4987-2020, 2020
Short summary
Short summary
Current atmospheric multiphase models do not include biotransformations of organic compounds by bacteria, although many previous studies of our and other research groups have shown microbial activity in cloud water. The current lab/model study shows that for water-soluble aromatic compounds, biodegradation by bacteria may be as efficient as chemical reactions in cloud water.
Anand Kumar, Claudia Marcolli, and Thomas Peter
Atmos. Chem. Phys., 19, 6035–6058, https://doi.org/10.5194/acp-19-6035-2019, https://doi.org/10.5194/acp-19-6035-2019, 2019
Short summary
Short summary
This paper not only interests the atmospheric science community but has a potential to cater to a broader audience. We discuss both long- and
short-term effects of various
atmospherically relevantchemical species on a fairly abundant mineral surface
Quartz. We of course discuss these chemical interactions from the perspective of fate of airborne mineral dust but the same interactions could be interesting for studies on minerals at the ground level.
Anand Kumar, Claudia Marcolli, and Thomas Peter
Atmos. Chem. Phys., 19, 6059–6084, https://doi.org/10.5194/acp-19-6059-2019, https://doi.org/10.5194/acp-19-6059-2019, 2019
Short summary
Short summary
This paper not only interests the Atmospheric Science community but has a potential to cater to a broader audience. We discuss both long- and short-term effects of various
atmospherically relevantchemical species on fairly abundant mineral surfaces like feldspars and clays. We of course discuss these chemical interactions from the perspective of fate of airborne mineral dust but the same interactions could be interesting for studies on minerals at the ground level.
Richie Kaur, Brandi M. Hudson, Joseph Draper, Dean J. Tantillo, and Cort Anastasio
Atmos. Chem. Phys., 19, 5021–5032, https://doi.org/10.5194/acp-19-5021-2019, https://doi.org/10.5194/acp-19-5021-2019, 2019
Short summary
Short summary
Organic triplets are an important class of aqueous photooxidants, but little is known about their reactions with most atmospheric organic compounds. We measured the reaction rate constants of a model triplet with 17 aliphatic alkenes; using their correlation with oxidation potential, we predicted rate constants for some atmospherically relevant alkenes. Depending on their reactivities, triplets can be minor to important sinks for isoprene- and limonene-derived alkenes in cloud or fog drops.
Julián Gelman Constantin, Melisa M. Gianetti, María P. Longinotti, and Horacio R. Corti
Atmos. Chem. Phys., 18, 14965–14978, https://doi.org/10.5194/acp-18-14965-2018, https://doi.org/10.5194/acp-18-14965-2018, 2018
Short summary
Short summary
Numerous studies have shown that ice surface is actually coated by a thin layer of water even for temperatures below melting temperature. This quasi-liquid layer is relevant in the atmospheric chemistry of clouds, polar regions, glaciers, and other cold regions. We present new results of atomic force microscopy on pure ice, which suggests a thickness for this layer below 1 nm between -7 ºC and -2 ºC. We propose that in many cases previous authors have overestimated this thickness.
Anand Kumar, Claudia Marcolli, Beiping Luo, and Thomas Peter
Atmos. Chem. Phys., 18, 7057–7079, https://doi.org/10.5194/acp-18-7057-2018, https://doi.org/10.5194/acp-18-7057-2018, 2018
Short summary
Short summary
We have performed immersion freezing experiments with microcline (most active ice nucleation, IN, K-feldspar polymorph) and investigated the effect of ammonium and non-ammonium solutes on its IN efficiency. We report increased IN efficiency of microcline in dilute ammonia- or ammonium-containing solutions, which opens up a pathway for condensation freezing occurring at a warmer temperature than immersion freezing.
Ahmed Abdelmonem
Atmos. Chem. Phys., 17, 10733–10741, https://doi.org/10.5194/acp-17-10733-2017, https://doi.org/10.5194/acp-17-10733-2017, 2017
Short summary
Short summary
On the basis of supercooled SHG spectroscopy, I report molecular-level evidence for the existence of one- and two-step deposition freezing depending on the surface type and the supersaturation conditions. In addition, immersion freezing shows a transient ice phase with a lifetime of c. 1 min. This study provides new insights into atmospheric processes and can impact various industrial and research branches, particularly climate change, weather modification, and tracing water in the hydrosphere.
Alexander Jost, Miklós Szakáll, Karoline Diehl, Subir K. Mitra, and Stephan Borrmann
Atmos. Chem. Phys., 17, 9717–9732, https://doi.org/10.5194/acp-17-9717-2017, https://doi.org/10.5194/acp-17-9717-2017, 2017
Short summary
Short summary
During riming of graupel and hail, soluble chemical trace constituents contained in the liquid droplets could be retained while freezing onto the glaciated particle, or released back to the air potentially at other altitudes as retained. Quantification of retention constitutes a major uncertainty in numerical models for atmospheric chemistry and improvements hinge upon experimental determination of retention for carboxylic acids, aldehydes, SO2, H2O2, NH2, and others, as presented in this paper.
Ahmed Abdelmonem, Ellen H. G. Backus, Nadine Hoffmann, M. Alejandra Sánchez, Jenée D. Cyran, Alexei Kiselev, and Mischa Bonn
Atmos. Chem. Phys., 17, 7827–7837, https://doi.org/10.5194/acp-17-7827-2017, https://doi.org/10.5194/acp-17-7827-2017, 2017
Short summary
Short summary
We report the effect of surface charge on heterogeneous immersion freezing for the atmospherically relevant sapphire surface. Combining linear and nonlinear optical techniques and investigating isolated drops, we find that charge-induced surface templating is detrimental for ice nucleation on α-alumina surface. This study provides new insights into atmospheric processes and can impact various industrial and research branches, particularly climate change and tracing of water in the hydrosphere.
Pascal Renard, Isabelle Canet, Martine Sancelme, Nolwenn Wirgot, Laurent Deguillaume, and Anne-Marie Delort
Atmos. Chem. Phys., 16, 12347–12358, https://doi.org/10.5194/acp-16-12347-2016, https://doi.org/10.5194/acp-16-12347-2016, 2016
Short summary
Short summary
A total of 480 microorganisms collected from 39 clouds sampled in France were isolated and identified. This unique collection was screened for biosurfactant production by measuring the surface tension. 41 % of the tested strains were active producers. Pseudomonas, the most frequently detected genus in clouds, was the dominant group for the production of biosurfactants. Further, the potential impact of the production of biosurfactants by cloud microorganisms on atmospheric processes is discussed.
Baban Nagare, Claudia Marcolli, André Welti, Olaf Stetzer, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 8899–8914, https://doi.org/10.5194/acp-16-8899-2016, https://doi.org/10.5194/acp-16-8899-2016, 2016
Short summary
Short summary
The relative importance of contact freezing and immersion freezing at mixed-phase cloud temperatures is the subject of debate. We performed experiments using continuous-flow diffusion chambers to compare the freezing efficiency of ice-nucleating particles for both these nucleation modes. Silver iodide, kaolinite and Arizona Test Dust were used as ice-nucleating particles. We could not confirm the dominance of contact freezing over immersion freezing for our experimental conditions.
A. Bianco, M. Passananti, H. Perroux, G. Voyard, C. Mouchel-Vallon, N. Chaumerliac, G. Mailhot, L. Deguillaume, and M. Brigante
Atmos. Chem. Phys., 15, 9191–9202, https://doi.org/10.5194/acp-15-9191-2015, https://doi.org/10.5194/acp-15-9191-2015, 2015
G. P. Schill, K. Genareau, and M. A. Tolbert
Atmos. Chem. Phys., 15, 7523–7536, https://doi.org/10.5194/acp-15-7523-2015, https://doi.org/10.5194/acp-15-7523-2015, 2015
Short summary
Short summary
Fine volcanic ash can influence cloud glaciation and, therefore, global climate. In this work we examined the heterogeneous ice nucleation properties of three distinct types of volcanic ash. We find that, in contrast to previous studies, these volcanic ash samples have different ice nucleation properties in the immersion mode. In the deposition mode, however, they nucleate ice with similar efficiency. We show that this behavior may be due to their mineralogy.
Y. Tobo, P. J. DeMott, T. C. J. Hill, A. J. Prenni, N. G. Swoboda-Colberg, G. D. Franc, and S. M. Kreidenweis
Atmos. Chem. Phys., 14, 8521–8531, https://doi.org/10.5194/acp-14-8521-2014, https://doi.org/10.5194/acp-14-8521-2014, 2014
R. Paris and K. V. Desboeufs
Atmos. Chem. Phys., 13, 4895–4905, https://doi.org/10.5194/acp-13-4895-2013, https://doi.org/10.5194/acp-13-4895-2013, 2013
X. Tang, D. R. Cocker III, and A. Asa-Awuku
Atmos. Chem. Phys., 12, 8377–8388, https://doi.org/10.5194/acp-12-8377-2012, https://doi.org/10.5194/acp-12-8377-2012, 2012
V. Pinti, C. Marcolli, B. Zobrist, C. R. Hoyle, and T. Peter
Atmos. Chem. Phys., 12, 5859–5878, https://doi.org/10.5194/acp-12-5859-2012, https://doi.org/10.5194/acp-12-5859-2012, 2012
M. Vaïtilingom, T. Charbouillot, L. Deguillaume, R. Maisonobe, M. Parazols, P. Amato, M. Sancelme, and A.-M. Delort
Atmos. Chem. Phys., 11, 8721–8733, https://doi.org/10.5194/acp-11-8721-2011, https://doi.org/10.5194/acp-11-8721-2011, 2011
T. Hullar and C. Anastasio
Atmos. Chem. Phys., 11, 7209–7222, https://doi.org/10.5194/acp-11-7209-2011, https://doi.org/10.5194/acp-11-7209-2011, 2011
Yao Liu, I. El Haddad, M. Scarfogliero, L. Nieto-Gligorovski, B. Temime-Roussel, E. Quivet, N. Marchand, B. Picquet-Varrault, and A. Monod
Atmos. Chem. Phys., 9, 5093–5105, https://doi.org/10.5194/acp-9-5093-2009, https://doi.org/10.5194/acp-9-5093-2009, 2009
I. El Haddad, Yao Liu, L. Nieto-Gligorovski, V. Michaud, B. Temime-Roussel, E. Quivet, N. Marchand, K. Sellegri, and A. Monod
Atmos. Chem. Phys., 9, 5107–5117, https://doi.org/10.5194/acp-9-5107-2009, https://doi.org/10.5194/acp-9-5107-2009, 2009
Cited articles
Atkinson, R. and Aschmann, S. M.: Rate constants for the reactions of the OH
radical with the propyl and butyl nitrates and 1-nitrobutane at
298 ± 2 K, Int. J. Chem. Kinet., 21, 1123–1129,
https://doi.org/10.1002/kin.550211205, 1989.
Barnes, I., Becker, K. H., and Zhu, T.: Near UV absorption spectra and
photolysis products of difunctional organic nitrates: Possible importance as
NOx reservoirs, J. Atmos. Chem., 17, 353–373,
https://doi.org/10.1007/BF00696854, 1993.
Bedjanian, Y., Morin, J., and Romanias, M. N.: Reactions of OH radicals with
2-methyl-1-butyl, neopentyl and 1-hexyl nitrates. Structure-activity
relationship for gas-phase reactions of OH with alkyl nitrates: An update,
Atmos. Environ., 180, 167–172,
https://doi.org/10.1016/j.atmosenv.2018.03.002, 2018.
Bianco, A., Passananti, M., Brigante, M., and Mailhot, G.: Photochemistry of
the cloud aqueous phase: A review, Molecules, 25, 423,
https://doi.org/10.3390/molecules25020423, 2020.
Browne, E. C., Min, K.-E., Wooldridge, P. J., Apel, E., Blake, D. R., Brune,
W. H., Cantrell, C. A., Cubison, M. J., Diskin, G. S., Jimenez, J. L.,
Weinheimer, A. J., Wennberg, P. O., Wisthaler, A., and Cohen, R. C.:
Observations of total RONO2 over the boreal forest: NOx sinks and
HNO3 sources, Atmos. Chem. Phys., 13, 4543–4562,
https://doi.org/10.5194/acp-13-4543-2013, 2013.
Carbajo, P. G. and Orr-Ewing, A. J.: NO2 quantum yields from ultraviolet
photodissociation of methyl and isopropyl nitrate, Phys. Chem.
Chem. Phys., 12, 6084–6091, https://doi.org/10.1039/c001425g, 2010.
Clemitshaw, K. C., Williams, J., Rattigan, O. v., Shallcross, D. E., Law, K.
S., and Anthony Cox, R.: Gas-phase ultraviolet absorption cross-sections and
atmospheric lifetimes of several C2–C5 alkyl nitrates, J. Photochem.
Photobiol.
A, 102, 117–126, https://doi.org/10.1016/S1010-6030(96)04458-9, 1997.
Darer, A. I., Cole-Filipiak, N. C., O'Connor, A. E., and Elrod, M. J.:
Formation and stability of atmospherically relevant isoprene-derived
organosulfates and organonitrates, Environ. Sci. Technol., 45, 1895–1902,
https://doi.org/10.1021/es103797z, 2011.
Fisher, J. A., Jacob, D. J., Travis, K. R., Kim, P. S., Marais, E. A.,
Miller, C. C., Yu, K., Zhu, L., Yantosca, R. M., Sulprizio, M. P., Mao, J.,
Wennberg, P. O., Crounse, J. D., Teng, A. P., Nguyen, T. B., Clair, J. M.
S., Cohen, R. C., Romer, P., Nault, B. A., Wooldridge, P. J., Jimenez, J.
L., Campuzano-Jost, P., Day, D. A., Hu, W., Shepson, P. B., Xiong, F.,
Blake, D. R., Goldstein, A. H., Misztal, P. K., Hanisco, T. F., Wolfe, G.
M., Ryerson, T. B., Wisthaler, A., and Mikoviny, T.: Organic nitrate
chemistry and its implications for nitrogen budgets in an isoprene- and
monoterpene-rich atmosphere: Constraints from aircraft (SEAC4RS) and
ground-based (SOAS) observations in the Southeast US, Atmos. Chem. Phys., 16,
5969–5991, https://doi.org/10.5194/acp-16-5969-2016, 2016.
González-Sánchez, J. M.: Replication Data for: On the importance of multiphase
photolysis of organic nitrates on their global atmospheric removal, Harvard
Dataverse [data set], https://doi.org/10.7910/DVN/O7HKJQ, 2023.
González-Sánchez, J. M., Brun, N., Wu, J., Morin, J., Temime-Roussel, B.,
Ravier, S., Mouchel-Vallon, C., Clément, J.-L., and Monod, A.: On the
importance of atmospheric loss of organic nitrates by aqueous-phase
⚫OH oxidation, Atmos. Chem. Phys., 21, 4915–4937,
https://doi.org/10.5194/acp-21-4915-2021, 2021.
Herrmann, H.: On the photolysis of simple anions and neutral molecules as
sources of O− OH, SO and Cl in aqueous
solution, Phys. Chem. Chem. Phys., 9, 3935–3964,
https://doi.org/10.1039/b618565g, 2007.
Hu, K. S., Darer, A. I., and Elrod, M. J.: Thermodynamics and kinetics of
the hydrolysis of atmospherically relevant organonitrates and
organosulfates, Atmos. Chem. Phys., 11, 8307–8320,
https://doi.org/10.5194/acp-11-8307-2011, 2011.
Jacobs, M. I., Burke, W. J., and Elrod, M. J.: Kinetics of the reactions of
isoprene-derived hydroxynitrates: Gas phase epoxide formation and solution
phase hydrolysis, Atmos. Chem. Phys., 14, 8933–8946,
https://doi.org/10.5194/acp-14-8933-2014, 2014.
Jenkin, M. E., Valorso, R., Aumont, B., Rickard, A. R., and Wallington, T.
J.: Estimation of rate coefficients and branching ratios for gas-phase
reactions of OH with aliphatic organic compounds for use in automated
mechanism construction, Atmos. Chem. Phys., 18, 9297–9328,
https://doi.org/10.5194/acp-18-9297-2018, 2018.
Kiendler-Scharr, A., Mensah, A. A., Friese, E., Topping, D., Nemitz, E.,
Prevot, A. S. H., Äijälä, M., Allan, J., Canonaco, F.,
Canagaratna, M., Carbone, S., Crippa, M., Dall Osto, M., Day, D. A., de
Carlo, P., di Marco, C. F., Elbern, H., Eriksson, A., Freney, E., Hao, L.,
Herrmann, H., Hildebrandt, L., Hillamo, R., Jimenez, J. L., Laaksonen, A.,
McFiggans, G., Mohr, C., O'Dowd, C., Otjes, R., Ovadnevaite, J., Pandis, S.
N., Poulain, L., Schlag, P., Sellegri, K., Swietlicki, E., Tiitta, P.,
Vermeulen, A., Wahner, A., Worsnop, D., and Wu, H. C.: Ubiquity of organic
nitrates from nighttime chemistry in the European submicron aerosol, Geophys.
Res. Lett., 43, 7735–7744, https://doi.org/10.1002/2016GL069239, 2016.
Madronich, S.: Photodissociation in the atmosphere: 1. Actinic flux and the
effects of ground reflections and clouds, J. Geophys. Res., 92, 9740–9752,
https://doi.org/10.1029/jd092id08p09740, 1987.
Madronich, S. and Flocke, S.: The Role of Solar Radiation in Atmospheric
Chemistry, Springer, Berlin, Heidelberg, 1–26,
https://doi.org/10.1007/978-3-540-69044-3_1, 1999.
Morin, J., Bedjanian, Y., and Romanias, M. N.: Kinetics and Products of the
Reactions of Ethyl and n-Propyl Nitrates with OH Radicals, Int. J. Chem.
Kinet.,
48, 822–829, https://doi.org/10.1002/kin.21037, 2016.
Müller, J. F., Peeters, J., and Stavrakou, T.: Fast photolysis of
carbonyl nitrates from isoprene, Atmos. Chem. Phys., 14, 2497–2508,
https://doi.org/10.5194/acp-14-2497-2014, 2014.
Ng, N. L., Brown, S. S., Archibald, A. T., Atlas, E., Cohen, R. C., Crowley,
J. N., Day, D. A., Donahue, N. M., Fry, J. L., Fuchs, H., Griffin, R. J.,
Guzman, M. I., Herrmann, H., Hodzic, A., Iinuma, Y., Kiendler-Scharr, A.,
Lee, B. H., Luecken, D. J., Mao, J., McLaren, R., Mutzel, A., Osthoff, H.
D., Ouyang, B., Picquet-Varrault, B., Platt, U., Pye, H. O. T., Rudich, Y.,
Schwantes, R. H., Shiraiwa, M., Stutz, J., Thornton, J. A., Tilgner, A.,
Williams, B. J., and Zaveri, R. A.: Nitrate radicals and biogenic volatile
organic compounds: Oxidation, mechanisms, and organic aerosol, Atmos. Chem.
Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, 2017.
Nguyen, T. B., Crounse, J. D., Teng, A. P., Clair, J. M. S., Paulot, F.,
Wolfe, G. M., and Wennberg, P. O.: Rapid deposition of oxidized biogenic
compounds to a temperate forest, P. Natl. Acad. Sci. USA, 112,
E392–E401,
https://doi.org/10.1073/pnas.1418702112, 2015.
Nissenson, P., Dabdub, D., Das, R., Maurino, V., Minero, C., and Vione, D.:
Evidence of the water-cage effect on the photolysis of NO and
FeOH ,
Implications of this effect and of H2O2 surface accumulation on
photochemistry at the air-water interface of atmospheric droplets, Atmos.
Environ., 44, 4859–4866, https://doi.org/10.1016/j.atmosenv.2010.08.035,
2010.
Perring, A. E., Pusede, S. E., and Cohen, R. C.: An observational
perspective on the atmospheric impacts of alkyl and multifunctional nitrates
on ozone and secondary organic aerosol, Chem. Rev., 113, 5848–5870,
https://doi.org/10.1021/cr300520x, 2013.
Picquet-Varrault, B., Suarez-Bertoa, R., Duncianu, M., Cazaunau, M., Pangui,
E., David, M., and Doussin, J. F.: Photolysis and oxidation by OH radicals
of two carbonyl nitrates: 4-nitrooxy-2-butanone and 5-nitrooxy-2-pentanone,
Atmos. Chem. Phys., 20, 487–498, https://doi.org/10.5194/acp-20-487-2020,
2020.
Renard, P., Siekmann, F., Gandolfo, A., Socorro, J., Salque, G., Ravier, S.,
Quivet, E., Clément, J.-L. L., Traikia, M., Delort, A.-M. M., Voisin,
D., Vuitton, V., Thissen, R., and Monod, A.: Radical mechanisms of methyl
vinyl ketone oligomerization through aqueous phase OH-oxidation: On the
paradoxical role of dissolved molecular oxygen, Atmos. Chem. Phys., 13,
6473–6491, https://doi.org/10.5194/acp-13-6473-2013, 2013.
Rindelaub, J. D., McAvey, K. M., and Shepson, P. B.: The photochemical
production of organic nitrates from α-pinene and loss via
acid-dependent particle phase hydrolysis, Atmos. Environ., 100, 193–201,
https://doi.org/10.1016/j.atmosenv.2014.11.010, 2015.
Rindelaub, J. D., Borca, C. H., Hostetler, M. A., Slade, J. H., Lipton, M.
A., Slipchenko, L. V., and Shepson, P. B.: The acid-catalyzed hydrolysis of
an α-pinene-derived organic nitrate: Kinetics, products, reaction
mechanisms, and atmospheric impact, Atmos. Chem. Phys., 16, 15425–15432,
https://doi.org/10.5194/acp-16-15425-2016, 2016.
Roberts, J. M. and Fajer, R. W.: UV Absorption Cross Sections of Organic
Nitrates of Potential Atmospheric Importance and Estimation of Atmospheric
Lifetimes, Environ. Sci. Technol., 23, 945–951,
https://doi.org/10.1021/es00066a003, 1989.
Romer, P. S., Wooldridge, P. J., Crounse, J. D., Kim, M. J., Wennberg, P.
O., Dibb, J. E., Scheuer, E., Blake, D. R., Meinardi, S., Brosius, A. L.,
Thames, A. B., Miller, D. O., Brune, W. H., Hall, S. R., Ryerson, T. B., and
Cohen, R. C.: Constraints on Aerosol Nitrate Photolysis as a Potential
Source of HONO and NOx, Environ. Sci. Technol., 52, 13738–13746,
https://doi.org/10.1021/acs.est.8b03861, 2018.
Romer Present, P. S., Zare, A., and Cohen, R. C.: The changing role of
organic nitrates in the removal and transport of NOx, Atmos. Chem. Phys.,
20,
267–279, https://doi.org/10.5194/acp-20-267-2020, 2020.
Romonosky, D. E., Nguyen, L. Q., Shemesh, D., Nguyen, T. B., Epstein, S. A.,
Martin, D. B. C., Vanderwal, C. D., Gerber, R. B., and Nizkorodov, S. A.:
Absorption spectra and aqueous photochemistry of β-hydroxyalkyl
nitrates of atmospheric interest, Mol. Phys., 113, 2179–2190,
https://doi.org/10.1080/00268976.2015.1017020, 2015.
Shen, H., Zhao, D., Pullinen, I., Kang, S., Vereecken, L., Fuchs, H., Acir,
I. H., Tillmann, R., Rohrer, F., Wildt, J., Kiendler-Scharr, A., Wahner, A.,
and Mentel, T. F.: Highly Oxygenated Organic Nitrates Formed from NO3
Radical-Initiated Oxidation of β-Pinene, Environ. Sci. Technol., 55,
15658–15671, https://doi.org/10.1021/acs.est.1c03978, 2021.
Shepson, P. B.: Organic nitrates, Blackwell Publishing Ltd., Oxford, UK,
58–63, https://doi.org/10.1358/dnp.1999.12.1.863615, 1999.
Suarez-Bertoa, R., Picquet-Varrault, B., Tamas, W., Pangui, E., and Doussin,
J. F.: Atmospheric fate of a series of carbonyl nitrates: Photolysis
frequencies and OH-oxidation rate constants, Environ. Sci. Technol., 46,
12502–12509, https://doi.org/10.1021/es302613x, 2012.
Svoboda, O., Kubelová, L., and Slavíček, P.: Enabling forbidden
processes: Quantum and solvation enhancement of nitrate anion UV absorption,
J. Phys. Chem. A, 117, 12868–12877,
https://doi.org/10.1021/jp4098777, 2013.
Takeuchi, M. and Ng, N. L.: Chemical composition and hydrolysis of organic
nitrate aerosol formed from hydroxyl and nitrate radical oxidation of
α-pinene and β-pinene, Atmos. Chem. Phys, 19, 12749–12766,
https://doi.org/10.5194/acp-19-12749-2019, 2019.
Talukdar, R. K., Herndon, S. C., Burkholder, J. B., Roberts, J. M., and
Ravishankara, A. R.: Atmospheric fate of several alkyl nitrates: Part 1.
Rate coefficients of the reactions of alkyl nitrates with isotopically
labelled hydroxyl radicals, J. Chem. Soc. Faraday
T., 93, 2787–2796, https://doi.org/10.1039/a701780d, 1997a.
Talukdar, R. K., Burkholder, J. B., Hunter, M., Gilles, M. K., Roberts, J.
M., and Ravishankara, A. R.: Atmospheric fate of several alkyl nitrates:
Part 2. UV absorption cross-sections and photodissociation quantum yields,
J. Chem. Soc. Faraday T., 93, 2797–2805,
https://doi.org/10.1039/a701781b, 1997b.
Tilgner, A., Bräuer, P., Wolke, R., and Herrmann, H.: Modelling
multiphase chemistry in deliquescent aerosols and clouds using CAPRAM3.0i, J.
Atmos. Chem., 70, 221–256, https://doi.org/10.1007/s10874-013-9267-4, 2013.
Wang, Y., Piletic, I. R., Takeuchi, M., Xu, T., France, S., and Ng, N. L.:
Synthesis and Hydrolysis of Atmospherically Relevant Monoterpene-Derived
Organic Nitrates, Environ. Sci. Technol., 55, 14595–14606,
https://doi.org/10.1021/acs.est.1c05310, 2021.
Wängberg, I., Barnes, I., and Becker, K. H.: Atmospheric chemistry of
bifunctional cycloalkyl nitrates, Chem. Phys. Lett., 261, 138–144,
https://doi.org/10.1016/0009-2614(96)00857-3, 1996.
Warneck, P. and Wurzinger, C.: Product quantum yields for the 305-nm
photodecomposition of nitrate in aqueous solution, J. Phys. Chem, 92,
6278–6283, 1988.
Zare, A., Fahey, K. M., Sarwar, G., Cohen, R. C., and Pye, H. O. T.:
Vapor-Pressure Pathways Initiate but Hydrolysis Products Dominate the
Aerosol Estimated from Organic Nitrates, ACS Earth Space Chem., 3,
1426–1437, https://doi.org/10.1021/acsearthspacechem.9b00067, 2019.
Short summary
Organic nitrates play a crucial role in air pollution, as they are NOx reservoirs. This work investigated for the first time their reactivity with light in the aqueous phase (cloud and fog and wet aerosol), proving it slower than in the gas phase. Therefore, our findings reveal that partitioning of organic nitrates in the aqueous phase leads to longer atmospheric lifetimes of these compounds and thus a broader spatial distribution of their related pollution.
Organic nitrates play a crucial role in air pollution, as they are NOx reservoirs. This work...
Altmetrics
Final-revised paper
Preprint