Articles | Volume 19, issue 7
https://doi.org/10.5194/acp-19-5021-2019
© Author(s) 2019. 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-19-5021-2019
© Author(s) 2019. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
12 Apr 2019
Research article |
| 12 Apr 2019
| 12 Apr 2019
Aqueous reactions of organic triplet excited states with atmospheric alkenes
Richie Kaur
Department of Land, Air, and Water Resources, University of
California, Davis, California 95616, USA
Agricultural & Environmental Chemistry Graduate Group, University
of California, Davis, California 95616, USA
Brandi M. Hudson
Department of Chemistry, University of California, Davis,
California 95616, USA
Joseph Draper
Department of Land, Air, and Water Resources, University of
California, Davis, California 95616, USA
now at: Fresno Metropolitan Flood Control District, Fresno,
California 93727, USA
Dean J. Tantillo
Department of Chemistry, University of California, Davis,
California 95616, USA
Department of Land, Air, and Water Resources, University of
California, Davis, California 95616, USA
Agricultural & Environmental Chemistry Graduate Group, University
of California, Davis, California 95616, USA
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Richie Kaur, Jacqueline R. Labins, Scarlett S. Helbock, Wenqing Jiang, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 19, 6579–6594, https://doi.org/10.5194/acp-19-6579-2019, https://doi.org/10.5194/acp-19-6579-2019, 2019
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We measured hydroxyl radical (•OH), singlet oxygen (1O2*), and organic triplets (3C*) in illuminated aqueous particle extracts. After measuring the impact of dilution on oxidant concentrations, we extrapolated our results to predict them in ambient particles – 1O2* and 3C* concentrations appear to be greatly enhanced, while •OH appears largely unchanged. Two of these oxidants (1O2*, 3C*) are not yet included in atmospheric models, and our results make it possible to include them in the future.
Michael Oluwatoyin Sunday, Laura Marie Dahler Heinlein, Junwei He, Allison Moon, Sukriti Kapur, Ting Fang, Kasey C. Edwards, Fangzhou Guo, Jack Dibb, James H. Flynn III, Becky Alexander, Manabu Shiraiwa, and Cort Anastasio
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This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Hydrogen peroxide (HOOH) is an important oxidant that forms atmospheric sulfate. We demonstrate that illumination of brown carbon can rapidly form HOOH within particles, even under the low sunlight conditions of Fairbanks, Alaska during winter. This in-particle formation of HOOH is fast enough that it forms sulfate at significant rates. In contrast, the formation of HOOH in the gas phase during the campaign is expected to be negligible because of high NOx levels.
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Atmos. Chem. Phys., 24, 4473–4485, https://doi.org/10.5194/acp-24-4473-2024, https://doi.org/10.5194/acp-24-4473-2024, 2024
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We measured changes in light absorption during the aqueous oxidation of six phenols with hydroxyl radical (●OH) or an organic triplet excited state (3C*). All the phenols formed light-absorbing secondary brown carbon (BrC), which then decayed with continued oxidation. Extrapolation to ambient conditions suggest ●OH is the dominant sink of secondary phenolic BrC in fog/cloud drops, while 3C* controls the lifetime of this light absorption in particle water.
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We developed a method that uses aqueous S(IV) to quantitatively convert NO2 to NO2−, which allows both species to be quantified using the Griess method. As an example of the utility of the method, we quantified both photolysis channels of nitrate, with and without a scavenger for hydroxyl radical (·OH). The results show that without a scavenger, ·OH reacts with nitrite to form nitrogen dioxide, suppressing the apparent quantum yield of NO2− and enhancing that of NO2.
Lan Ma, Reed Worland, Laura Heinlein, Chrystal Guzman, Wenqing Jiang, Christopher Niedek, Keith J. Bein, Qi Zhang, and Cort Anastasio
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We measured concentrations of three photooxidants – the hydroxyl radical, triplet excited states of organic carbon, and singlet molecular oxygen – in fine particles collected over a year. Concentrations are highest in extracts of fresh biomass burning particles, largely because they have the highest particle concentrations and highest light absorption. When normalized by light absorption, rates of formation for each oxidant are generally similar for the four particle types we observed.
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Atmos. Chem. Phys., 23, 8805–8821, https://doi.org/10.5194/acp-23-8805-2023, https://doi.org/10.5194/acp-23-8805-2023, 2023
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Although photooxidants are important in airborne particles, little is known of their concentrations. By measuring oxidants in a series of particle dilutions, we predict their concentrations in aerosol liquid water (ALW). We find •OH concentrations in ALW are on the order of 10−15 M, similar to their cloud/fog values, while oxidizing triplet excited states and singlet molecular oxygen have ALW values of ca. 10−13 M and 10−12 M, respectively, roughly 10–100 times higher than in cloud/fog drops.
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We studied how aqueous-phase secondary organic aerosol (aqSOA) form and evolve from a phenolic carbonyl commonly present in biomass burning smoke. The composition and optical properties of the aqSOA are significantly affected by photochemical reactions and are dependent on the oxidants' concentration and identity in water. During photoaging, the aqSOA initially becomes darker, but prolonged aging leads to the formation of volatile products, resulting in significant mass loss and photobleaching.
Ted Hullar, Theo Tran, Zekun Chen, Fernanda Bononi, Oliver Palmer, Davide Donadio, and Cort Anastasio
Atmos. Chem. Phys., 22, 5943–5959, https://doi.org/10.5194/acp-22-5943-2022, https://doi.org/10.5194/acp-22-5943-2022, 2022
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Chemicals are commonly found in snowpacks throughout the world and may be degraded by sunlight; some previous research has reported faster decay rates for chemicals on the surface of snow and ice compared to in water. We found photodegradation on snow can be as much as 30 times faster than in solution for the three dimethoxybenzene isomers. Our computational modeling found light absorbance by dimethoxybenzenes increases on the snow surface, but this only partially explains the decay rate.
Richie Kaur, Jacqueline R. Labins, Scarlett S. Helbock, Wenqing Jiang, Keith J. Bein, Qi Zhang, and Cort Anastasio
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We measured hydroxyl radical (•OH), singlet oxygen (1O2*), and organic triplets (3C*) in illuminated aqueous particle extracts. After measuring the impact of dilution on oxidant concentrations, we extrapolated our results to predict them in ambient particles – 1O2* and 3C* concentrations appear to be greatly enhanced, while •OH appears largely unchanged. Two of these oxidants (1O2*, 3C*) are not yet included in atmospheric models, and our results make it possible to include them in the future.
Ted Hullar and Cort Anastasio
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We study chemical reactions in snow and ice by freezing solutions in the laboratory. Although it is important to know where these chemicals are in the frozen sample (at the surface or buried in the ice), we do not understand this well. In this paper, we used X-rays to look at the chemical location in frozen samples. We found chemical location is sensitive to freezing method, sample container, and chemical characteristics, requiring careful experimental design and interpretation of results.
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Atmos. Chem. Phys., 16, 9579–9590, https://doi.org/10.5194/acp-16-9579-2016, https://doi.org/10.5194/acp-16-9579-2016, 2016
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We made the first measurements of the concentrations of hydroxyl radical (•OH), a dominant environmental oxidant, in snow grains. Concentrations of •OH in snow at Summit, Greenland, are comparable to values reported for midlatitude cloud and fog drops, even though impurity levels in the snow are much lower. At these concentrations, the lifetimes of organics and bromide in Summit snow are approximately 3 days and 7 h, respectively, suggesting that OH is a major oxidant for both species.
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The chemical evolution of SOA formed during aqueous reactions of phenolic compounds is studied via combined bulk and molecular analysis. Phenolic SOA evolve dynamically during photochemical aging, with different reaction mechanisms (oligomerization, fragmentation, and functionalization) leading to different generations of products that span an enormous range in volatilities and a large range in oxidation state and composition. Aqueous reactions of phenols are likely an important source of ELVOC.
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Related subject area
Subject: Clouds and Precipitation | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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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
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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
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A better understanding of hydroxyl radical photochemical sources in cloud waters collected at the puy de Dôme station – experimental versus modelled formation rates
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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
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Anand Kumar, Claudia Marcolli, and Thomas Peter
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This paper not only interests the atmospheric science community but has a potential to cater to a broader audience. We discuss both long- and
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atmospherically relevantchemical species on a fairly abundant mineral surface
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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
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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.
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
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Anand Kumar, Claudia Marcolli, Beiping Luo, and Thomas Peter
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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
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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
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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
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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
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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
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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
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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
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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.
Organic triplets are an important class of aqueous photooxidants, but little is known about...
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