Articles | Volume 23, issue 2
https://doi.org/10.5194/acp-23-1619-2023
© 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-23-1619-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
27 Jan 2023
Research article |
| 27 Jan 2023
| 27 Jan 2023
Long-term monitoring of cloud water chemistry at Whiteface Mountain: the emergence of a new chemical regime
Christopher E. Lawrence
Atmospheric Sciences Research Center (ASRC), University at Albany, SUNY ETEC building, 1220 Washington Ave, Albany NY 12226, USA
Paul Casson
Atmospheric Sciences Research Center (ASRC), University at Albany, SUNY ETEC building, 1220 Washington Ave, Albany NY 12226, USA
Richard Brandt
Atmospheric Sciences Research Center (ASRC), University at Albany, SUNY ETEC building, 1220 Washington Ave, Albany NY 12226, USA
James J. Schwab
Atmospheric Sciences Research Center (ASRC), University at Albany, SUNY ETEC building, 1220 Washington Ave, Albany NY 12226, USA
James E. Dukett
Adirondack Lake Survey Corporation (ALSC), 1115 NYS Rt.86, P.O. Box 296, Ray Brook NY 12977, USA
Phil Snyder
Adirondack Lake Survey Corporation (ALSC), 1115 NYS Rt.86, P.O. Box 296, Ray Brook NY 12977, USA
Elizabeth Yerger
Paul Smith's College Adirondack Watershed Institute (AWI), P.O. Box 265, Routes 86 and 30, Paul Smiths NY 12970, USA
Daniel Kelting
Paul Smith's College Adirondack Watershed Institute (AWI), P.O. Box 265, Routes 86 and 30, Paul Smiths NY 12970, USA
Trevor C. VandenBoer
Department of Chemistry, York University, Toronto, Ontario, M3J 1P3, Canada
Sara Lance
CORRESPONDING AUTHOR
Atmospheric Sciences Research Center (ASRC), University at Albany, SUNY ETEC building, 1220 Washington Ave, Albany NY 12226, USA
Related authors
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
EGUsphere, https://doi.org/10.5194/egusphere-2024-715, https://doi.org/10.5194/egusphere-2024-715, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This work uses WRF-Chem and chemical box modeling to study the gas and aqueous phase production of organic acid concentrations measured in cloud water the summit of Whiteface Mountain on July 1st, 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
EGUsphere, https://doi.org/10.5194/egusphere-2024-715, https://doi.org/10.5194/egusphere-2024-715, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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This work uses WRF-Chem and chemical box modeling to study the gas and aqueous phase production of organic acid concentrations measured in cloud water the summit of Whiteface Mountain on July 1st, 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Christopher J. Hennigan, Michael McKee, Vikram Pratap, Bryanna Boegner, Jasper Reno, Lucia Garcia, Madison McLaren, and Sara M. Lance
Atmos. Chem. Phys., 23, 14437–14449, https://doi.org/10.5194/acp-23-14437-2023, https://doi.org/10.5194/acp-23-14437-2023, 2023
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This study characterized the optical properties of light-absorbing organic compounds, called brown carbon (BrC), in atmospheric cloud water samples. In all samples, light absorption by BrC increased linearly with increasing pH. There was variability in the sensitivity of the absorption–pH relationship, depending on the degree of influence from fire emissions. Overall, these results show that the climate forcing of BrC is quite strongly affected by its pH-dependent absorption.
Alessia A. Colussi, Daniel Persaud, Melodie Lao, Bryan K. Place, Rachel F. Hems, Susan E. Ziegler, Kate A. Edwards, Cora J. Young, and Trevor C. VandenBoer
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2023-231, https://doi.org/10.5194/amt-2023-231, 2023
Revised manuscript accepted for AMT
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We present a novel and inexpensive solution to the collection of automated atmospheric wet deposition samples away from source regions at integrated monthly timescales, with all components provided freely for replication.
Teles C. Furlani, Patrick R. Veres, Kathryn E. R. Dawe, J. Andrew Neuman, Steven S. Brown, Trevor C. VandenBoer, and Cora J. Young
Atmos. Meas. Tech., 14, 5859–5871, https://doi.org/10.5194/amt-14-5859-2021, https://doi.org/10.5194/amt-14-5859-2021, 2021
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This study characterized and validated a commercial spectroscopic instrument for the measurement of hydrogen chloride (HCl) in the atmosphere. Near the Earth’s surface, HCl acts as the dominant reservoir for other chlorine-containing reactive chemicals that play an important role in atmospheric chemistry. The properties of HCl make it challenging to measure. This instrument can overcome many of these challenges, enabling reliable HCl measurements.
Melodie Lao, Leigh R. Crilley, Leyla Salehpoor, Teles C. Furlani, Ilann Bourgeois, J. Andrew Neuman, Andrew W. Rollins, Patrick R. Veres, Rebecca A. Washenfelder, Caroline C. Womack, Cora J. Young, and Trevor C. VandenBoer
Atmos. Meas. Tech., 13, 5873–5890, https://doi.org/10.5194/amt-13-5873-2020, https://doi.org/10.5194/amt-13-5873-2020, 2020
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Nitrous acid (HONO) is a key intermediate in the generation of oxidants and fate of nitrogen oxides in the atmosphere. High-purity calibration sources that produce stable atmospherically relevant levels under field conditions have not been made to date, reducing measurement accuracy. In this study a simple salt-coated tube humidified with water vapor is demonstrated to produce pure stable low levels of HONO, with modifications allowing the generation of higher amounts.
Fangqun Yu, Gan Luo, Arshad Arjunan Nair, James J. Schwab, James P. Sherman, and Yanda Zhang
Atmos. Chem. Phys., 20, 2591–2601, https://doi.org/10.5194/acp-20-2591-2020, https://doi.org/10.5194/acp-20-2591-2020, 2020
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Particle number concentration (PNC) is a key parameter important for the health and climate impacts of atmospheric aerosols. We show that, even during wintertime, regional nucleation occurs and contributes significantly to number concentrations of ultrafine particles and cloud condensation nuclei. Due to low biogenic emissions, wintertime regional nucleation is solely controlled by inorganic species, and ternary ion-mediated nucleation is able to capture the observed variations in PNC.
Gan Luo, Fangqun Yu, and James Schwab
Geosci. Model Dev., 12, 3439–3447, https://doi.org/10.5194/gmd-12-3439-2019, https://doi.org/10.5194/gmd-12-3439-2019, 2019
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GEOS-Chem 12.0.0 has been recognized to significantly overestimate the concentrations of gaseous nitric acid, aerosol nitrate, and aerosol ammonium over the United States. In this study, we show that most or all of the overestimation issue appears to be associated with wet scavenging processes. With the updated wet scavenging scheme in this work, we successfully improve the skill of the model in predicting the three species concentrations, which are important for air quality and climate studies.
Jie Zhang, Sara Lance, Jeffrey M. Freedman, Yele Sun, Brian A. Crandall, Xiuli Wei, and James J. Schwab
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-529, https://doi.org/10.5194/acp-2018-529, 2018
Preprint retracted
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The impact of fireworks (FW) events on air quality was studied using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and collocated instruments during the Independence Day (July 4) holiday. The Independence Day FW events resulted in significant increases in both organic and inorganic (potassium, sulfate, chloride) chemical components, and the contribution from different aerosol sources was discussed.
Jie Zhang, Joseph P. Marto, and James J. Schwab
Atmos. Meas. Tech., 11, 2995–3005, https://doi.org/10.5194/amt-11-2995-2018, https://doi.org/10.5194/amt-11-2995-2018, 2018
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The performance of two kinds of optical instruments for aerosol mass measurements was explained by a Mie scattering theory. At the same time, the response of optical instruments for ambient aerosol with different size, chemical composition, and refractive index were also studied. These would help evaluate the applicability and limitations of these optical scattering instruments.
Ryan D. Cook, Ying-Hsuan Lin, Zhuoyu Peng, Eric Boone, Rosalie K. Chu, James E. Dukett, Matthew J. Gunsch, Wuliang Zhang, Nikola Tolic, Alexander Laskin, and Kerri A. Pratt
Atmos. Chem. Phys., 17, 15167–15180, https://doi.org/10.5194/acp-17-15167-2017, https://doi.org/10.5194/acp-17-15167-2017, 2017
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Reactions occur within water in both atmospheric particles and cloud droplets, yet little is known about the organic compounds in cloud water. In this work, cloud water samples were collected at Whiteface Mountain, New York, and analyzed using ultra-high-resolution mass spectrometry to investigate the molecular composition of the dissolved organic compounds. The results focus on changes in cloud water composition with air mass origin – influences of forest, urban, and wildfire emissions.
K. Max Zhang, George Allen, Bo Yang, Geng Chen, Jiajun Gu, James Schwab, Dirk Felton, and Oliver Rattigan
Atmos. Chem. Phys., 17, 11441–11452, https://doi.org/10.5194/acp-17-11441-2017, https://doi.org/10.5194/acp-17-11441-2017, 2017
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Woodsmoke is a worldwide public health concern. A reliable marker for woodsmoke will be very useful in air-quality management. DC (Delta-C) has been proposed as a woodsmoke marker in previous studies. However, several researchers raised concerns of whether it is reliable. Our study took advantage of aerosol light absorption and PM2.5 data collected at three US cities/towns dominated by woodsmoke. We showed that DC can be a good qualitative and semi-quantitive marker, but with limitations.
Bryan K. Place, Aleya T. Quilty, Robert A. Di Lorenzo, Susan E. Ziegler, and Trevor C. VandenBoer
Atmos. Meas. Tech., 10, 1061–1078, https://doi.org/10.5194/amt-10-1061-2017, https://doi.org/10.5194/amt-10-1061-2017, 2017
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Amines are important drivers in particle formation and growth, which has implications for Earth’s climate. We developed a novel ion chromatographic method for separating and quantifying the 11 most abundant atmospheric alkyl amines, including three sets of structural isomers and two diamines. The detection limits are in the picogram per injection range. We quantified these analytes in two Canadian biomass burning aerosol samples with ammonium ratios of 1 : 2 up to 1000 : 1.
Chantelle R. Lonsdale, Jennifer D. Hegarty, Karen E. Cady-Pereira, Matthew J. Alvarado, Daven K. Henze, Matthew D. Turner, Shannon L. Capps, John B. Nowak, J. Andy Neuman, Ann M. Middlebrook, Roya Bahreini, Jennifer G. Murphy, Milos Z. Markovic, Trevor C. VandenBoer, Lynn M. Russell, and Amy Jo Scarino
Atmos. Chem. Phys., 17, 2721–2739, https://doi.org/10.5194/acp-17-2721-2017, https://doi.org/10.5194/acp-17-2721-2017, 2017
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This study takes advantage of the high-resolution observations of NH3(g) made by the TES satellite instrument over Bakersfield during the CalNex campaign, along with campaign measurements, to compare CMAQ model results in the San Joaquin Valley, California. Additionally we evaluate the CMAQ bi-directional ammonia flux results using the CARB emissions inventory against these satellite and campaign measurements, not previously explored in combination.
F. Yu, G. Luo, S. C. Pryor, P. R. Pillai, S. H. Lee, J. Ortega, J. J. Schwab, A. G. Hallar, W. R. Leaitch, V. P. Aneja, J. N. Smith, J. T. Walker, O. Hogrefe, and K. L. Demerjian
Atmos. Chem. Phys., 15, 13993–14003, https://doi.org/10.5194/acp-15-13993-2015, https://doi.org/10.5194/acp-15-13993-2015, 2015
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The role of low-volatility organics in new particle formation (NPF) in the atmosphere is assessed. An empirical formulation in which formation rate is a function of the concentrations of sulfuric acid and low-volatility organics significantly overpredicts NPF in the summer.
Two different schemes predict quite different nucleation rates (including their spatial patterns), concentrations of cloud condensation nuclei, and aerosol first indirect radiative forcing in North America.
Related subject area
Subject: Clouds and Precipitation | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Influences of sources and weather dynamics on atmospheric deposition of Se species and other trace elements
Response patterns of moss to atmospheric nitrogen deposition and nitrogen saturation in an urban-agro-forest transition
Molecular composition of clouds: a comparison between samples collected at tropical (Réunion Island, France) and mid-north (puy de Dôme, France) latitudes
Revealing the chemical characteristics of Arctic low-level cloud residuals – in situ observations from a mountain site
Measurement report: Closure analysis of aerosol–cloud composition in tropical maritime warm convection
Free amino acid quantification in cloud water at the Puy de Dôme station (France)
Wet deposition in the remote western and central Mediterranean as a source of trace metals to surface seawater
Insights into tropical cloud chemistry in Réunion (Indian Ocean): results from the BIO-MAÏDO campaign
Measurement report: Molecular characteristics of cloud water in southern China and insights into aqueous-phase processes from Fourier transform ion cyclotron resonance mass spectrometry
Total organic carbon and the contribution from speciated organics in cloud water: airborne data analysis from the CAMP2Ex field campaign
A link between the ice nucleation activity and the biogeochemistry of seawater
Impact of convection on the upper-tropospheric composition (water vapor and ozone) over a subtropical site (Réunion island; 21.1° S, 55.5° E) in the Indian Ocean
Chemical characteristics of cloud water and the impacts on aerosol properties at a subtropical mountain site in Hong Kong SAR
Diurnal cycle of iodine, bromine, and mercury concentrations in Svalbard surface snow
Wet deposition of inorganic ions in 320 cities across China: spatio-temporal variation, source apportionment, and dominant factors
Deposition of ionic species and black carbon to the Arctic snowpack: combining snow pit observations with modeling
Mercury and trace metal wet deposition across five stations in Alaska: controlling factors, spatial patterns, and source regions
Drivers of atmospheric deposition of polycyclic aromatic hydrocarbons at European high-altitude sites
Cloud scavenging of anthropogenic refractory particles at a mountain site in North China
Composition of ice particle residuals in mixed-phase clouds at Jungfraujoch (Switzerland): enrichment and depletion of particle groups relative to total aerosol
Snow scavenging and phase partitioning of nitrated and oxygenated aromatic hydrocarbons in polluted and remote environments in central Europe and the European Arctic
Continuous non-marine inputs of per- and polyfluoroalkyl substances to the High Arctic: a multi-decadal temporal record
Biogenic, urban, and wildfire influences on the molecular composition of dissolved organic compounds in cloud water
The single-particle mixing state and cloud scavenging of black carbon: a case study at a high-altitude mountain site in southern China
Composition, size and cloud condensation nuclei activity of biomass burning aerosol from northern Australian savannah fires
Five-year records of mercury wet deposition flux at GMOS sites in the Northern and Southern hemispheres
Atmospheric wet and litterfall mercury deposition at urban and rural sites in China
Hydroxyl radical in/on illuminated polar snow: formation rates, lifetimes, and steady-state concentrations
Cloud water composition during HCCT-2010: Scavenging efficiencies, solute concentrations, and droplet size dependence of inorganic ions and dissolved organic carbon
Fog composition at Baengnyeong Island in the eastern Yellow Sea: detecting markers of aqueous atmospheric oxidations
Wet deposition of atmospheric inorganic nitrogen at five remote sites in the Tibetan Plateau
Atmospheric wet and dry deposition of trace elements at 10 sites in Northern China
Natural or anthropogenic? On the origin of atmospheric sulfate deposition in the Andes of southeastern Ecuador
Temporal variations in rainwater methanol
Comprehensive assessment of meteorological conditions and airflow connectivity during HCCT-2010
Influence of cloud processing on CCN activation behaviour in the Thuringian Forest, Germany during HCCT-2010
Classification of clouds sampled at the puy de Dôme (France) based on 10 yr of monitoring of their physicochemical properties
Preliminary signs of the initiation of deep convection by GNSS
Dissolved organic carbon (DOC) and select aldehydes in cloud and fog water: the role of the aqueous phase in impacting trace gas budgets
Insights into dissolved organic matter complexity in rainwater from continental and coastal storms by ultrahigh resolution Fourier transform ion cyclotron resonance mass spectrometry
Dynamics of the chemical composition of rainwater throughout Hurricane Irene
Spatial and temporal distributions of total and methyl mercury in precipitation in core urban areas, Chongqing, China
Wet and dry deposition of atmospheric nitrogen at ten sites in Northern China
Spatial distribution of mercury deposition fluxes in Wanshan Hg mining area, Guizhou province, China
Molecular characterization of water soluble organic nitrogen in marine rainwater by ultra-high resolution electrospray ionization mass spectrometry
Five-year record of atmospheric precipitation chemistry in urban Beijing, China
Mercury deposition in Southern New Hampshire, 2006–2009
Chemical composition of rainwater at Maldives Climate Observatory at Hanimaadhoo (MCOH)
Chemistry of rain events in West Africa: evidence of dust and biogenic influence in convective systems
Atmospheric deposition of mercury and major ions to the Pensacola (Florida) watershed: spatial, seasonal, and inter-annual variability
Esther S. Breuninger, Julie Tolu, Iris Thurnherr, Franziska Aemisegger, Aryeh Feinberg, Sylvain Bouchet, Jeroen E. Sonke, Véronique Pont, Heini Wernli, and Lenny H. E. Winkel
Atmos. Chem. Phys., 24, 2491–2510, https://doi.org/10.5194/acp-24-2491-2024, https://doi.org/10.5194/acp-24-2491-2024, 2024
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Atmospheric deposition is an important source of selenium (Se) and other health-relevant trace elements in surface environments. We found that the variability in elemental concentrations in atmospheric deposition reflects not only changes in emission sources but also weather conditions during atmospheric removal. Depending on the sources and if Se is derived more locally or from further away, the Se forms can be different, affecting the bioavailability of Se atmospherically supplied to soils.
Ouping Deng, Yuanyuan Chen, Jingze Zhao, Xi Li, Wei Zhou, Ting Lan, Dinghua Ou, Yanyan Zhang, Jiang Liu, Ling Luo, Yueqiang He, Hanqing Yang, and Rong Huang
EGUsphere, https://doi.org/10.5194/egusphere-2023-2718, https://doi.org/10.5194/egusphere-2023-2718, 2023
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Estimating atmospheric nitrogen (N) deposition is critical to understanding the biogeochemical N cycle. Moss has long been considered as a bio-indicator for N deposition due to their accumulation of N from the atmosphere. Here, we improved the method for atmospheric N deposition monitoring using mosses. The sampling frequency and time was optimized. Eventually, this study contributed to improve the accuracy of the model of quantifying N deposition by using mosses.
Lucas Pailler, Laurent Deguillaume, Hélène Lavanant, Isabelle Schmitz, Marie Hubert, Edith Nicol, Micakël Ribeiro, Jean-Marc Pichon, Mickaël Vaïtilingom, Pamela Dominutti, Frédéric Burnet, Pierre Tulet, Maud Leriche, and Angelica Bianco
EGUsphere, https://doi.org/10.5194/egusphere-2023-2706, https://doi.org/10.5194/egusphere-2023-2706, 2023
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The composition of cloud water dissolved organic matter has been investigated through non-targeted high resolution mass spectrometry only on few samples, collected in the Northern hemisphere (NH). In this work, the chemical composition of samples collected at Reunion Island (SH) is investigated and compared to samples collected at the puy de Dôme (NH). Sampling, analysis and data treatment with the same methodology produced a unique dataset for investigating the molecular composition of clouds.
Yvette Gramlich, Karolina Siegel, Sophie L. Haslett, Gabriel Freitas, Radovan Krejci, Paul Zieger, and Claudia Mohr
Atmos. Chem. Phys., 23, 6813–6834, https://doi.org/10.5194/acp-23-6813-2023, https://doi.org/10.5194/acp-23-6813-2023, 2023
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In this study, we investigate the chemical composition of aerosol particles forming clouds in the Arctic. During year-long observations at a mountain site on Svalbard, we find a large contribution of naturally derived aerosol particles in the fraction forming clouds in the summer. Our observations indicate that most aerosol particles can serve as cloud seeds in this remote environment.
Ewan Crosbie, Luke D. Ziemba, Michael A. Shook, Claire E. Robinson, Edward L. Winstead, K. Lee Thornhill, Rachel A. Braun, Alexander B. MacDonald, Connor Stahl, Armin Sorooshian, Susan C. van den Heever, Joshua P. DiGangi, Glenn S. Diskin, Sarah Woods, Paola Bañaga, Matthew D. Brown, Francesca Gallo, Miguel Ricardo A. Hilario, Carolyn E. Jordan, Gabrielle R. Leung, Richard H. Moore, Kevin J. Sanchez, Taylor J. Shingler, and Elizabeth B. Wiggins
Atmos. Chem. Phys., 22, 13269–13302, https://doi.org/10.5194/acp-22-13269-2022, https://doi.org/10.5194/acp-22-13269-2022, 2022
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The linkage between cloud droplet and aerosol particle chemical composition was analyzed using samples collected in a polluted tropical marine environment. Variations in the droplet composition were related to physical and dynamical processes in clouds to assess their relative significance across three cases that spanned a range of rainfall amounts. In spite of the pollution, sea salt still remained a major contributor to the droplet composition and was preferentially enhanced in rainwater.
Pascal Renard, Maxence Brissy, Florent Rossi, Martin Leremboure, Saly Jaber, Jean-Luc Baray, Angelica Bianco, Anne-Marie Delort, and Laurent Deguillaume
Atmos. Chem. Phys., 22, 2467–2486, https://doi.org/10.5194/acp-22-2467-2022, https://doi.org/10.5194/acp-22-2467-2022, 2022
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Amino acids (AAs) have been quantified in cloud water collected at the Puy de Dôme station (France). Concentrations and speciation of those compounds are highly variable among the samples. Sources from the sea surface and atmospheric transformations during the air mass transport, mainly in the free troposphere, have been shown to modulate AA levels in cloud water.
Karine Desboeufs, Franck Fu, Matthieu Bressac, Antonio Tovar-Sánchez, Sylvain Triquet, Jean-François Doussin, Chiara Giorio, Patrick Chazette, Julie Disnaquet, Anaïs Feron, Paola Formenti, Franck Maisonneuve, Araceli Rodríguez-Romero, Pascal Zapf, François Dulac, and Cécile Guieu
Atmos. Chem. Phys., 22, 2309–2332, https://doi.org/10.5194/acp-22-2309-2022, https://doi.org/10.5194/acp-22-2309-2022, 2022
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This article reports the first concurrent sampling of wet deposition samples and surface seawater and was performed during the PEACETIME cruise in the remote Mediterranean (May–June 2017). Through the chemical composition of trace metals (TMs) in these samples, it emphasizes the decrease of atmospheric metal pollution in this area during the last few decades and the critical role of wet deposition as source of TMs for Mediterranean surface seawater, especially for intense dust deposition events.
Pamela A. Dominutti, Pascal Renard, Mickaël Vaïtilingom, Angelica Bianco, Jean-Luc Baray, Agnès Borbon, Thierry Bourianne, Frédéric Burnet, Aurélie Colomb, Anne-Marie Delort, Valentin Duflot, Stephan Houdier, Jean-Luc Jaffrezo, Muriel Joly, Martin Leremboure, Jean-Marc Metzger, Jean-Marc Pichon, Mickaël Ribeiro, Manon Rocco, Pierre Tulet, Anthony Vella, Maud Leriche, and Laurent Deguillaume
Atmos. Chem. Phys., 22, 505–533, https://doi.org/10.5194/acp-22-505-2022, https://doi.org/10.5194/acp-22-505-2022, 2022
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We present here the results obtained during an intensive field campaign conducted in March to April 2019 in Reunion. Our study integrates a comprehensive chemical and microphysical characterization of cloud water. Our investigations reveal that air mass history and cloud microphysical properties do not fully explain the variability observed in their chemical composition. This highlights the complexity of emission sources, multiphasic exchanges, and transformations in clouds.
Wei Sun, Yuzhen Fu, Guohua Zhang, Yuxiang Yang, Feng Jiang, Xiufeng Lian, Bin Jiang, Yuhong Liao, Xinhui Bi, Duohong Chen, Jianmin Chen, Xinming Wang, Jie Ou, Ping'an Peng, and Guoying Sheng
Atmos. Chem. Phys., 21, 16631–16644, https://doi.org/10.5194/acp-21-16631-2021, https://doi.org/10.5194/acp-21-16631-2021, 2021
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We sampled cloud water at a remote mountain site and investigated the molecular characteristics. CHON and CHO are dominant in cloud water. No statistical difference in the oxidation state is observed between cloud water and interstitial PM2.5. Most of the formulas are aliphatic and olefinic species. CHON, with aromatic structures and organosulfates, are abundant, especially in nighttime samples. The in-cloud and multi-phase dark reactions likely contribute significantly.
Connor Stahl, Ewan Crosbie, Paola Angela Bañaga, Grace Betito, Rachel A. Braun, Zenn Marie Cainglet, Maria Obiminda Cambaliza, Melliza Templonuevo Cruz, Julie Mae Dado, Miguel Ricardo A. Hilario, Gabrielle Frances Leung, Alexander B. MacDonald, Angela Monina Magnaye, Jeffrey Reid, Claire Robinson, Michael A. Shook, James Bernard Simpas, Shane Marie Visaga, Edward Winstead, Luke Ziemba, and Armin Sorooshian
Atmos. Chem. Phys., 21, 14109–14129, https://doi.org/10.5194/acp-21-14109-2021, https://doi.org/10.5194/acp-21-14109-2021, 2021
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A total of 159 cloud water samples were collected and measured for total organic carbon (TOC) during CAMP2Ex. On average, 30 % of TOC was speciated based on carboxylic/sulfonic acids and dimethylamine. Results provide a critical constraint on cloud composition and vertical profiles of TOC and organic species ranging from ~250 m to ~ 7 km and representing a variety of cloud types and air mass source influences such as biomass burning, marine emissions, anthropogenic activity, and dust.
Martin J. Wolf, Megan Goodell, Eric Dong, Lilian A. Dove, Cuiqi Zhang, Lesly J. Franco, Chuanyang Shen, Emma G. Rutkowski, Domenic N. Narducci, Susan Mullen, Andrew R. Babbin, and Daniel J. Cziczo
Atmos. Chem. Phys., 20, 15341–15356, https://doi.org/10.5194/acp-20-15341-2020, https://doi.org/10.5194/acp-20-15341-2020, 2020
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Sea spray is the largest aerosol source on Earth. These aerosol particles can impact climate by inducing ice formation in clouds. The role that ocean biology plays in determining the composition and ice nucleation abilities of sea spray aerosol is unclarified. In this study, we demonstrate that atomized seawater from highly productive ocean regions is more effective at nucleating ice than seawater from lower-productivity regions.
Damien Héron, Stéphanie Evan, Jérôme Brioude, Karen Rosenlof, Françoise Posny, Jean-Marc Metzger, and Jean-Pierre Cammas
Atmos. Chem. Phys., 20, 8611–8626, https://doi.org/10.5194/acp-20-8611-2020, https://doi.org/10.5194/acp-20-8611-2020, 2020
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Using a statistical method, summer variations (between 2013 and 2016) of ozone and water vapor are characterized in the upper troposphere above Réunion island (21° S, 55° E). It suggests a convective influence between 9 and 13 km. As deep convection is rarely observed near Réunion island, this study provides new insights on the long-range impact of deep convective outflow from the Intertropical Convergence Zone (ITCZ) on the upper troposphere over a subtropical site.
Tao Li, Zhe Wang, Yaru Wang, Chen Wu, Yiheng Liang, Men Xia, Chuan Yu, Hui Yun, Weihao Wang, Yan Wang, Jia Guo, Hartmut Herrmann, and Tao Wang
Atmos. Chem. Phys., 20, 391–407, https://doi.org/10.5194/acp-20-391-2020, https://doi.org/10.5194/acp-20-391-2020, 2020
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This work presents a field study of cloud water chemistry and interactions of cloud, gas, and aerosols in the polluted coastal boundary layer in southern China. Substantial dissolved organic matter in the acidic cloud water was observed, and the gas- and aqueous-phase partitioning of carbonyl compounds was investigated. The results demonstrated the significant role of cloud processing in altering aerosol properties, especially in producing aqueous organics and droplet-mode aerosols.
Andrea Spolaor, Elena Barbaro, David Cappelletti, Clara Turetta, Mauro Mazzola, Fabio Giardi, Mats P. Björkman, Federico Lucchetta, Federico Dallo, Katrine Aspmo Pfaffhuber, Hélène Angot, Aurelien Dommergue, Marion Maturilli, Alfonso Saiz-Lopez, Carlo Barbante, and Warren R. L. Cairns
Atmos. Chem. Phys., 19, 13325–13339, https://doi.org/10.5194/acp-19-13325-2019, https://doi.org/10.5194/acp-19-13325-2019, 2019
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The main aims of the study are to (a) detect whether mercury in the surface snow undergoes a daily cycle as determined in the atmosphere, (b) compare the mercury concentration in surface snow with the concentration in the atmosphere, (c) evaluate the effect of snow depositions, (d) detect whether iodine and bromine in the surface snow undergo a daily cycle, and (e) evaluate the role of metereological and atmospheric conditions. Different behaviours were determined during different seasons.
Rui Li, Lulu Cui, Yilong Zhao, Ziyu Zhang, Tianming Sun, Junlin Li, Wenhui Zhou, Ya Meng, Kan Huang, and Hongbo Fu
Atmos. Chem. Phys., 19, 11043–11070, https://doi.org/10.5194/acp-19-11043-2019, https://doi.org/10.5194/acp-19-11043-2019, 2019
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Acid deposition is still an important environmental issue in China. Rainwater samples in 320 cities in China were collected to determine the acidic ion concentrations and identify their spatiotemporal variations and sources. The higher acidic ions showed higher concentrations in winter. Furthermore, the highest acidic ion concentrations were mainly distributed in YRD and SB. These acidic ions were mainly sourced from industrial emissions and agricultural activities.
Hans-Werner Jacobi, Friedrich Obleitner, Sophie Da Costa, Patrick Ginot, Konstantinos Eleftheriadis, Wenche Aas, and Marco Zanatta
Atmos. Chem. Phys., 19, 10361–10377, https://doi.org/10.5194/acp-19-10361-2019, https://doi.org/10.5194/acp-19-10361-2019, 2019
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By combining atmospheric, precipitation, and snow measurements with snowpack simulations for a high Arctic site in Svalbard, we find that during wintertime the transfer of sea salt components to the snowpack was largely dominated by wet deposition. However, dry deposition contributed significantly for nitrate, non-sea-salt sulfate, and black carbon. The comparison of monthly deposition and snow budgets indicates an important redistribution of the impurities in the snowpack even during winter.
Christopher Pearson, Dean Howard, Christopher Moore, and Daniel Obrist
Atmos. Chem. Phys., 19, 6913–6929, https://doi.org/10.5194/acp-19-6913-2019, https://doi.org/10.5194/acp-19-6913-2019, 2019
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Precipitation-based deposition of mercury and other trace metals throughout Alaska provides a significant input of pollutants. Deposition shows significant seasonal and spatial variability, largely driven by precipitation patterns. Annual wet deposition of Hg at all AK collection sites is consistently lower than other monitoring stations throughout the CONUS. Hg showed no clear relationship to other metals, likely due to its highly volatile nature and capability of long-range transport.
Lourdes Arellano, Pilar Fernández, Barend L. van Drooge, Neil L. Rose, Ulrike Nickus, Hansjoerg Thies, Evzen Stuchlík, Lluís Camarero, Jordi Catalan, and Joan O. Grimalt
Atmos. Chem. Phys., 18, 16081–16097, https://doi.org/10.5194/acp-18-16081-2018, https://doi.org/10.5194/acp-18-16081-2018, 2018
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Mountain areas are key for studying the impact of diffuse pollution due to human activities on the continental areas. Polycyclic aromatic hydrocarbons (PAHs), human carcinogens with increased levels since the 1950s, are significant constituents of this pollution. We determined PAHs in monthly atmospheric deposition collected in European high mountain areas. The number of sites, period of study and sampling frequency provide the most comprehensive description of PAH fallout at remote sites.
Lei Liu, Jian Zhang, Liang Xu, Qi Yuan, Dao Huang, Jianmin Chen, Zongbo Shi, Yele Sun, Pingqing Fu, Zifa Wang, Daizhou Zhang, and Weijun Li
Atmos. Chem. Phys., 18, 14681–14693, https://doi.org/10.5194/acp-18-14681-2018, https://doi.org/10.5194/acp-18-14681-2018, 2018
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Using transmission electron microscopy, we studied individual cloud droplet residual and interstitial particles collected in cloud events at Mt. Tai in the polluted North China region. We found that individual cloud droplets were an extremely complicated mixture containing abundant refractory soot (i.e., black carbon), fly ash, and metals. The complicated cloud droplets have not been reported in clean continental or marine air before.
Stine Eriksen Hammer, Stephan Mertes, Johannes Schneider, Martin Ebert, Konrad Kandler, and Stephan Weinbruch
Atmos. Chem. Phys., 18, 13987–14003, https://doi.org/10.5194/acp-18-13987-2018, https://doi.org/10.5194/acp-18-13987-2018, 2018
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It is important to study ice-nucleating particles in the environment to learn more about cloud formation. We studied the composition of ice particle residuals and total aerosol particles sampled in parallel during mixed-phase cloud events at Jungfraujoch and discovered that soot and complex secondary particles were not present. In contrast, silica, aluminosilicates, and other aluminosilicates were the most important ice particle residual groups at site temperatures between −11 and −18 °C.
Pourya Shahpoury, Zoran Kitanovski, and Gerhard Lammel
Atmos. Chem. Phys., 18, 13495–13510, https://doi.org/10.5194/acp-18-13495-2018, https://doi.org/10.5194/acp-18-13495-2018, 2018
Heidi M. Pickard, Alison S. Criscitiello, Christine Spencer, Martin J. Sharp, Derek C. G. Muir, Amila O. De Silva, and Cora J. Young
Atmos. Chem. Phys., 18, 5045–5058, https://doi.org/10.5194/acp-18-5045-2018, https://doi.org/10.5194/acp-18-5045-2018, 2018
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Perfluoroalkyl acids (PFAAs) are persistent, bioaccumulative compounds found in the environment far from source regions, including the remote Arctic. We collected a 15 m ice core from the Canadian High Arctic to measure a 38-year deposition record of PFAAs, proving information about major pollutant sources and production changes over time. Our results demonstrate that PFAAs have continuous and increasing deposition, despite recent North American regulations and phase-outs.
Ryan D. Cook, Ying-Hsuan Lin, Zhuoyu Peng, Eric Boone, Rosalie K. Chu, James E. Dukett, Matthew J. Gunsch, Wuliang Zhang, Nikola Tolic, Alexander Laskin, and Kerri A. Pratt
Atmos. Chem. Phys., 17, 15167–15180, https://doi.org/10.5194/acp-17-15167-2017, https://doi.org/10.5194/acp-17-15167-2017, 2017
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Reactions occur within water in both atmospheric particles and cloud droplets, yet little is known about the organic compounds in cloud water. In this work, cloud water samples were collected at Whiteface Mountain, New York, and analyzed using ultra-high-resolution mass spectrometry to investigate the molecular composition of the dissolved organic compounds. The results focus on changes in cloud water composition with air mass origin – influences of forest, urban, and wildfire emissions.
Guohua Zhang, Qinhao Lin, Long Peng, Xinhui Bi, Duohong Chen, Mei Li, Lei Li, Fred J. Brechtel, Jianxin Chen, Weijun Yan, Xinming Wang, Ping'an Peng, Guoying Sheng, and Zhen Zhou
Atmos. Chem. Phys., 17, 14975–14985, https://doi.org/10.5194/acp-17-14975-2017, https://doi.org/10.5194/acp-17-14975-2017, 2017
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The mixing state of black carbon (BC)-containing particles and the mass scavenging efficiency of BC in cloud were investigated at a mountain site (1690 m a.s.l.) in southern China. The measured BC-containing particles were internally mixed extensively with sulfate, and thus the number fraction of scavenged BC-containing particles is close to that of all the measured particles. BC-containing particles with higher fractions of organics were scavenged relatively less.
Marc D. Mallet, Luke T. Cravigan, Andelija Milic, Joel Alroe, Zoran D. Ristovski, Jason Ward, Melita Keywood, Leah R. Williams, Paul Selleck, and Branka Miljevic
Atmos. Chem. Phys., 17, 3605–3617, https://doi.org/10.5194/acp-17-3605-2017, https://doi.org/10.5194/acp-17-3605-2017, 2017
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This paper presents data on the size, composition and concentration of aerosol particles emitted from north Australian savannah fires and how these properties influence cloud condensation nuclei (CCN) concentrations. Both the size and composition of aerosol were found to be important in determining CCN. Despite large CCNc enhancements during periods of close biomass burning, the aerosol was very weakly hygroscopic which should be accounted for in climate models to avoid large CCNc overestimates.
Francesca Sprovieri, Nicola Pirrone, Mariantonia Bencardino, Francesco D'Amore, Helene Angot, Carlo Barbante, Ernst-Günther Brunke, Flor Arcega-Cabrera, Warren Cairns, Sara Comero, María del Carmen Diéguez, Aurélien Dommergue, Ralf Ebinghaus, Xin Bin Feng, Xuewu Fu, Patricia Elizabeth Garcia, Bernd Manfred Gawlik, Ulla Hageström, Katarina Hansson, Milena Horvat, Jože Kotnik, Casper Labuschagne, Olivier Magand, Lynwill Martin, Nikolay Mashyanov, Thumeka Mkololo, John Munthe, Vladimir Obolkin, Martha Ramirez Islas, Fabrizio Sena, Vernon Somerset, Pia Spandow, Massimiliano Vardè, Chavon Walters, Ingvar Wängberg, Andreas Weigelt, Xu Yang, and Hui Zhang
Atmos. Chem. Phys., 17, 2689–2708, https://doi.org/10.5194/acp-17-2689-2017, https://doi.org/10.5194/acp-17-2689-2017, 2017
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The results on total mercury (THg) wet deposition flux obtained within the GMOS network have been presented and discussed to understand the atmospheric Hg cycling and its seasonal depositional patterns over the 2011–2015 period. The data set provides new insight into baseline concentrations of THg concentrations in precipitation particularly in regions where wet deposition and atmospheric Hg species were not investigated before, opening the way for additional measurements and modeling studies.
Xuewu Fu, Xu Yang, Xiaofang Lang, Jun Zhou, Hui Zhang, Ben Yu, Haiyu Yan, Che-Jen Lin, and Xinbin Feng
Atmos. Chem. Phys., 16, 11547–11562, https://doi.org/10.5194/acp-16-11547-2016, https://doi.org/10.5194/acp-16-11547-2016, 2016
Zeyuan Chen, Liang Chu, Edward S. Galbavy, Keren Ram, and Cort Anastasio
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.
Dominik van Pinxteren, Khanneh Wadinga Fomba, Stephan Mertes, Konrad Müller, Gerald Spindler, Johannes Schneider, Taehyoung Lee, Jeffrey L. Collett, and Hartmut Herrmann
Atmos. Chem. Phys., 16, 3185–3205, https://doi.org/10.5194/acp-16-3185-2016, https://doi.org/10.5194/acp-16-3185-2016, 2016
A. J. Boris, T. Lee, T. Park, J. Choi, S. J. Seo, and J. L. Collett Jr.
Atmos. Chem. Phys., 16, 437–453, https://doi.org/10.5194/acp-16-437-2016, https://doi.org/10.5194/acp-16-437-2016, 2016
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Samples of fog water collected in the Yellow Sea during summer 2014 represent fog downwind of polluted regions and provide new insight into the fate of regional emissions. Organic and inorganic components reveal contributions from urban, biogenic, marine, and biomass burning emissions, as well as evidence of aqueous organic processing reactions. Many fog components are products of extensive photochemical aging during multiday transport, including oxidation within wet aerosols or fogs.
Y. W. Liu, Xu-Ri, Y. S. Wang, Y. P. Pan, and S. L. Piao
Atmos. Chem. Phys., 15, 11683–11700, https://doi.org/10.5194/acp-15-11683-2015, https://doi.org/10.5194/acp-15-11683-2015, 2015
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We investigated inorganic N wet deposition at five sites in the Tibetan Plateau (TP). Combining in situ measurements in this and previous studies, the average wet deposition of NH4+-N, NO3--N, and inorganic N in the TP was estimated to be 1.06, 0.51, and 1.58 kg N ha−1 yr−1, respectively. Results suggest that earlier estimations based on chemical transport model simulations and/or limited field measurements likely overestimated substantially the regional inorganic N wet deposition in the TP.
Y. P. Pan and Y. S. Wang
Atmos. Chem. Phys., 15, 951–972, https://doi.org/10.5194/acp-15-951-2015, https://doi.org/10.5194/acp-15-951-2015, 2015
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This paper presents the first concurrent measurements of wet and dry deposition of various trace elements in Northern China, covering an extensive area over 3 years in a global hotspot of air pollution. The unique field data can serve as a sound basis for the validation of regional emission inventories and biogeochemical or atmospheric chemistry models. The findings are very important for policy makers to create legislation to reduce the emissions and protect soil and water from air pollution.
S. Makowski Giannoni, R. Rollenbeck, K. Trachte, and J. Bendix
Atmos. Chem. Phys., 14, 11297–11312, https://doi.org/10.5194/acp-14-11297-2014, https://doi.org/10.5194/acp-14-11297-2014, 2014
J. D. Felix, S. B. Jones, G. B. Avery, J. D. Willey, R. N. Mead, and R. J. Kieber
Atmos. Chem. Phys., 14, 10509–10516, https://doi.org/10.5194/acp-14-10509-2014, https://doi.org/10.5194/acp-14-10509-2014, 2014
A. Tilgner, L. Schöne, P. Bräuer, D. van Pinxteren, E. Hoffmann, G. Spindler, S. A. Styler, S. Mertes, W. Birmili, R. Otto, M. Merkel, K. Weinhold, A. Wiedensohler, H. Deneke, R. Schrödner, R. Wolke, J. Schneider, W. Haunold, A. Engel, A. Wéber, and H. Herrmann
Atmos. Chem. Phys., 14, 9105–9128, https://doi.org/10.5194/acp-14-9105-2014, https://doi.org/10.5194/acp-14-9105-2014, 2014
S. Henning, K. Dieckmann, K. Ignatius, M. Schäfer, P. Zedler, E. Harris, B. Sinha, D. van Pinxteren, S. Mertes, W. Birmili, M. Merkel, Z. Wu, A. Wiedensohler, H. Wex, H. Herrmann, and F. Stratmann
Atmos. Chem. Phys., 14, 7859–7868, https://doi.org/10.5194/acp-14-7859-2014, https://doi.org/10.5194/acp-14-7859-2014, 2014
L. Deguillaume, T. Charbouillot, M. Joly, M. Vaïtilingom, M. Parazols, A. Marinoni, P. Amato, A.-M. Delort, V. Vinatier, A. Flossmann, N. Chaumerliac, J. M. Pichon, S. Houdier, P. Laj, K. Sellegri, A. Colomb, M. Brigante, and G. Mailhot
Atmos. Chem. Phys., 14, 1485–1506, https://doi.org/10.5194/acp-14-1485-2014, https://doi.org/10.5194/acp-14-1485-2014, 2014
H. Brenot, J. Neméghaire, L. Delobbe, N. Clerbaux, P. De Meutter, A. Deckmyn, A. Delcloo, L. Frappez, and M. Van Roozendael
Atmos. Chem. Phys., 13, 5425–5449, https://doi.org/10.5194/acp-13-5425-2013, https://doi.org/10.5194/acp-13-5425-2013, 2013
B. Ervens, Y. Wang, J. Eagar, W. R. Leaitch, A. M. Macdonald, K. T. Valsaraj, and P. Herckes
Atmos. Chem. Phys., 13, 5117–5135, https://doi.org/10.5194/acp-13-5117-2013, https://doi.org/10.5194/acp-13-5117-2013, 2013
R. N. Mead, K. M. Mullaugh, G. Brooks Avery, R. J. Kieber, J. D. Willey, and D. C. Podgorski
Atmos. Chem. Phys., 13, 4829–4838, https://doi.org/10.5194/acp-13-4829-2013, https://doi.org/10.5194/acp-13-4829-2013, 2013
K. M. Mullaugh, J. D. Willey, R. J. Kieber, R. N. Mead, and G. B. Avery Jr.
Atmos. Chem. Phys., 13, 2321–2330, https://doi.org/10.5194/acp-13-2321-2013, https://doi.org/10.5194/acp-13-2321-2013, 2013
Y. M. Wang, D. Y. Wang, B. Meng, Y. L. Peng, L. Zhao, and J. S. Zhu
Atmos. Chem. Phys., 12, 9417–9426, https://doi.org/10.5194/acp-12-9417-2012, https://doi.org/10.5194/acp-12-9417-2012, 2012
Y. P. Pan, Y. S. Wang, G. Q. Tang, and D. Wu
Atmos. Chem. Phys., 12, 6515–6535, https://doi.org/10.5194/acp-12-6515-2012, https://doi.org/10.5194/acp-12-6515-2012, 2012
Z. H. Dai, X. B. Feng, J. Sommar, P. Li, and X. W. Fu
Atmos. Chem. Phys., 12, 6207–6218, https://doi.org/10.5194/acp-12-6207-2012, https://doi.org/10.5194/acp-12-6207-2012, 2012
K. E. Altieri, M. G. Hastings, A. J. Peters, and D. M. Sigman
Atmos. Chem. Phys., 12, 3557–3571, https://doi.org/10.5194/acp-12-3557-2012, https://doi.org/10.5194/acp-12-3557-2012, 2012
F. Yang, J. Tan, Z. B. Shi, Y. Cai, K. He, Y. Ma, F. Duan, T. Okuda, S. Tanaka, and G. Chen
Atmos. Chem. Phys., 12, 2025–2035, https://doi.org/10.5194/acp-12-2025-2012, https://doi.org/10.5194/acp-12-2025-2012, 2012
M. A. S. Lombard, J. G. Bryce, H. Mao, and R. Talbot
Atmos. Chem. Phys., 11, 7657–7668, https://doi.org/10.5194/acp-11-7657-2011, https://doi.org/10.5194/acp-11-7657-2011, 2011
R. Das, L. Granat, C. Leck, P. S. Praveen, and H. Rodhe
Atmos. Chem. Phys., 11, 3743–3755, https://doi.org/10.5194/acp-11-3743-2011, https://doi.org/10.5194/acp-11-3743-2011, 2011
K. Desboeufs, E. Journet, J.-L. Rajot, S. Chevaillier, S. Triquet, P. Formenti, and A. Zakou
Atmos. Chem. Phys., 10, 9283–9293, https://doi.org/10.5194/acp-10-9283-2010, https://doi.org/10.5194/acp-10-9283-2010, 2010
J. M. Caffrey, W. M. Landing, S. D. Nolek, K. J. Gosnell, S. S. Bagui, and S. C. Bagui
Atmos. Chem. Phys., 10, 5425–5434, https://doi.org/10.5194/acp-10-5425-2010, https://doi.org/10.5194/acp-10-5425-2010, 2010
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Short summary
Atmospheric aqueous chemistry can have profound effects on our environment, as illustrated by historical data from Whiteface Mountain (WFM) that were critical for uncovering the process of acid rain. The current study updates the long-term trends in cloud water composition at WFM for the period 1994 to 2021. We highlight the emergence of a new chemical regime at WFM dominated by organics and ammonium, quite different from the highly acidic regime observed in the past but not necessarily
clean.
Atmospheric aqueous chemistry can have profound effects on our environment, as illustrated by...
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