Articles | Volume 13, issue 18
https://doi.org/10.5194/acp-13-9461-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-13-9461-2013
© Author(s) 2013. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Direct photolysis of carbonyl compounds dissolved in cloud and fog~droplets
S. A. Epstein
Department of Chemistry, University of California, Irvine, 1102 Natural Sciences 2, Irvine, CA 92697-2025, USA
E. Tapavicza
Department of Chemistry, University of California, Irvine, 1102 Natural Sciences 2, Irvine, CA 92697-2025, USA
F. Furche
Department of Chemistry, University of California, Irvine, 1102 Natural Sciences 2, Irvine, CA 92697-2025, USA
S. A. Nizkorodov
Department of Chemistry, University of California, Irvine, 1102 Natural Sciences 2, Irvine, CA 92697-2025, USA
Related authors
No articles found.
Fabian Mahrt, Long Peng, Julia Zaks, Yuanzhou Huang, Paul E. Ohno, Natalie R. Smith, Florence K. A. Gregson, Yiming Qin, Celia L. Faiola, Scot T. Martin, Sergey A. Nizkorodov, Markus Ammann, and Allan K. Bertram
Atmos. Chem. Phys., 22, 13783–13796, https://doi.org/10.5194/acp-22-13783-2022, https://doi.org/10.5194/acp-22-13783-2022, 2022
Short summary
Short summary
The number of condensed phases in mixtures of different secondary organic aerosol (SOA) types determines their impact on air quality and climate. Here we observe the number of phases in individual particles that contain mixtures of two different types of SOA. We find that SOA mixtures can form one- or two-phase particles, depending on the difference in the average oxygen-to-carbon (O / C) ratios of the two SOA types that are internally mixed within individual particles.
Kristian J. Kiland, Kevin L. Marroquin, Natalie R. Smith, Shaun Xu, Sergey A. Nizkorodov, and Allan K. Bertram
Atmos. Meas. Tech., 15, 5545–5561, https://doi.org/10.5194/amt-15-5545-2022, https://doi.org/10.5194/amt-15-5545-2022, 2022
Short summary
Short summary
Information on the viscosity of secondary organic aerosols is needed when making air quality, climate, and atmospheric chemistry predictions. Viscosity depends on temperature, so we developed a new method for measuring the temperature-dependent viscosity of small samples. As an application of the method, we measured the viscosity of farnesene secondary organic aerosol at different temperatures.
Alexandra L. Klodt, Marley Adamek, Monica Dibley, Sergey A. Nizkorodov, and Rachel E. O'Brien
Atmos. Chem. Phys., 22, 10155–10171, https://doi.org/10.5194/acp-22-10155-2022, https://doi.org/10.5194/acp-22-10155-2022, 2022
Short summary
Short summary
We investigated photochemistry of a secondary organic aerosol under three different conditions: in a dilute aqueous solution mimicking cloud droplets, in a solution of concentrated ammonium sulfate mimicking deliquesced aerosol, and in an organic matrix mimicking dry organic aerosol. We find that rate and mechanisms of photochemistry depend sensitively on these conditions, suggesting that the same organic aerosol compounds will degrade at different rates depending on their local environment.
Arttu Ylisirniö, Angela Buchholz, Claudia Mohr, Zijun Li, Luis Barreira, Andrew Lambe, Celia Faiola, Eetu Kari, Taina Yli-Juuti, Sergey A. Nizkorodov, Douglas R. Worsnop, Annele Virtanen, and Siegfried Schobesberger
Atmos. Chem. Phys., 20, 5629–5644, https://doi.org/10.5194/acp-20-5629-2020, https://doi.org/10.5194/acp-20-5629-2020, 2020
Short summary
Short summary
We studied the chemical composition and volatility of secondary organic aerosol (SOA) particles formed from emissions of Scots pines and compared those results to SOA formed from α-pinene and from a sesquiterpene mixture. We found that SOA formed from single precursors cannot capture the properties of SOA formed from real plant emissions.
Lauren T. Fleming, Peng Lin, James M. Roberts, Vanessa Selimovic, Robert Yokelson, Julia Laskin, Alexander Laskin, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 20, 1105–1129, https://doi.org/10.5194/acp-20-1105-2020, https://doi.org/10.5194/acp-20-1105-2020, 2020
Short summary
Short summary
We have explored the nature and stability of molecules that give biomass burning smoke its faint brown color. Different types of biomass fuels were burned and the resulting smoke was collected for a detailed chemical analysis. We found that brown molecules in smoke become less colored when they are irradiated by sunlight, but this photobleaching process is very slow. This means that biomass burning smoke will remain brown-colored for a long time and efficiently warm up the atmosphere.
Mijung Song, Adrian M. Maclean, Yuanzhou Huang, Natalie R. Smith, Sandra L. Blair, Julia Laskin, Alexander Laskin, Wing-Sy Wong DeRieux, Ying Li, Manabu Shiraiwa, Sergey A. Nizkorodov, and Allan K. Bertram
Atmos. Chem. Phys., 19, 12515–12529, https://doi.org/10.5194/acp-19-12515-2019, https://doi.org/10.5194/acp-19-12515-2019, 2019
Brigitte Rooney, Ran Zhao, Yuan Wang, Kelvin H. Bates, Ajay Pillarisetti, Sumit Sharma, Seema Kundu, Tami C. Bond, Nicholas L. Lam, Bora Ozaltun, Li Xu, Varun Goel, Lauren T. Fleming, Robert Weltman, Simone Meinardi, Donald R. Blake, Sergey A. Nizkorodov, Rufus D. Edwards, Ankit Yadav, Narendra K. Arora, Kirk R. Smith, and John H. Seinfeld
Atmos. Chem. Phys., 19, 7719–7742, https://doi.org/10.5194/acp-19-7719-2019, https://doi.org/10.5194/acp-19-7719-2019, 2019
Short summary
Short summary
Approximately 3 billion people worldwide cook with solid fuels, such as wood, charcoal, and agricultural residues, that are often combusted in inefficient cookstoves. Here, we simulate the distribution of the two major health-damaging outdoor pollution species (PM2.5 and O3) using state-of-the-science emissions databases and atmospheric chemical transport models to estimate the impact of household combustion on ambient air quality in India.
Angela Buchholz, Andrew T. Lambe, Arttu Ylisirniö, Zijun Li, Olli-Pekka Tikkanen, Celia Faiola, Eetu Kari, Liqing Hao, Olli Luoma, Wei Huang, Claudia Mohr, Douglas R. Worsnop, Sergey A. Nizkorodov, Taina Yli-Juuti, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 19, 4061–4073, https://doi.org/10.5194/acp-19-4061-2019, https://doi.org/10.5194/acp-19-4061-2019, 2019
Short summary
Short summary
We studied the evaporation of α-pinene secondary organic aerosol particles in clean air to derive their volatility from the observed size changes. We found that the particles became more resilient to evaporation with increased oxidative age, possibly increasing their lifetime in the atmosphere. Also, increased relative humidity increased the particle evaporation. Mass spectrometry measurements of the particles at different stages of evaporation revealed some water-induced composition changes.
Dagny A. Ullmann, Mallory L. Hinks, Adrian M. Maclean, Christopher L. Butenhoff, James W. Grayson, Kelley Barsanti, Jose L. Jimenez, Sergey A. Nizkorodov, Saeid Kamal, and Allan K. Bertram
Atmos. Chem. Phys., 19, 1491–1503, https://doi.org/10.5194/acp-19-1491-2019, https://doi.org/10.5194/acp-19-1491-2019, 2019
Short summary
Short summary
We measured the viscosity and diffusion of organic molecules in secondary organic aerosol (SOA) generated from the ozonolysis of limonene. The results suggest that the mixing times of large organics in the SOA studied are short (< 1 h) for conditions found in the planetary boundary layer. The results also show that the Stokes–Einstein equation gives accurate predictions of diffusion coefficients of large organics within the studied SOA up to a viscosity of 102 to 104 Pa s.
Zhijian Li, Sergey A. Nizkorodov, Hong Chen, Xiaohui Lu, Xin Yang, and Jianmin Chen
Atmos. Chem. Phys., 19, 1343–1356, https://doi.org/10.5194/acp-19-1343-2019, https://doi.org/10.5194/acp-19-1343-2019, 2019
Short summary
Short summary
In this work, we found that acrolein, the smallest α,β-unsaturated aldehyde, has the potential to form light-absorbing heterocyclic secondary organic aerosol. In the gaseous phase, acrolein can react with gaseous ammonia, forming 3-picoline. In the liquid phase, the dissolved acrolein can react with ammonium to form higher molecular-weight pyridinium compounds. All the pyridinium compounds can increase the light absorptivity of aerosol particles.
Lauren T. Fleming, Robert Weltman, Ankit Yadav, Rufus D. Edwards, Narendra K. Arora, Ajay Pillarisetti, Simone Meinardi, Kirk R. Smith, Donald R. Blake, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 18, 15169–15182, https://doi.org/10.5194/acp-18-15169-2018, https://doi.org/10.5194/acp-18-15169-2018, 2018
Short summary
Short summary
Brushwood- and dung-burning cookstoves are used for cooking and heating and influence ambient air quality for millions of people. We report emission factors from the more efficient cookstove, the chulha, compared to the smoldering angithi, for carbon dioxide, carbon monoxide, and 76 volatile organic compounds. This comprehensive gas emission inventory should inform policy makers about the magnitude of the effect of cookstoves on the air quality in India.
Wing-Sy Wong DeRieux, Ying Li, Peng Lin, Julia Laskin, Alexander Laskin, Allan K. Bertram, Sergey A. Nizkorodov, and Manabu Shiraiwa
Atmos. Chem. Phys., 18, 6331–6351, https://doi.org/10.5194/acp-18-6331-2018, https://doi.org/10.5194/acp-18-6331-2018, 2018
Short summary
Short summary
The phase transition of organic particles between glassy and semi-solid states occurs at the glass transition temperature. We developed a method to predict glass transition temperatures and the viscosity of secondary organic aerosols using molecular composition, with consistent results with viscosity measurements. The viscosity of biomass burning particles was also estimated using the chemical composition measured by high-resolution mass spectrometry with two different ionization techniques.
Shupeng Zhu, Jeremy R. Horne, Julia Montoya-Aguilera, Mallory L. Hinks, Sergey A. Nizkorodov, and Donald Dabdub
Atmos. Chem. Phys., 18, 3641–3657, https://doi.org/10.5194/acp-18-3641-2018, https://doi.org/10.5194/acp-18-3641-2018, 2018
Short summary
Short summary
For the first time, the interaction between ammonia and secondary organic aerosol (SOA) is integrated in an air quality model and investigated on a national scale. Our original analysis from simulation results indicates that a significant reduction in gas-phase ammonia is possible due to its uptake onto SOA. Significant impact is also observed in the concentration of particulate matter, with a distinct spatial pattern over different seasons.
Lauren T. Fleming, Peng Lin, Alexander Laskin, Julia Laskin, Robert Weltman, Rufus D. Edwards, Narendra K. Arora, Ankit Yadav, Simone Meinardi, Donald R. Blake, Ajay Pillarisetti, Kirk R. Smith, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 18, 2461–2480, https://doi.org/10.5194/acp-18-2461-2018, https://doi.org/10.5194/acp-18-2461-2018, 2018
Short summary
Short summary
Household cooking emissions in India, which rely on traditional meal preparation with dung- and brushwood-fueled cookstoves, produce copious amounts of particulate matter. Detailed chemical analysis of the compounds found in this particulate matter detected a large number of previously unidentified nitrogen-containing organic compounds, originating from dung-fueled cookstoves.
Mallory L. Hinks, Julia Montoya-Aguilera, Lucas Ellison, Peng Lin, Alexander Laskin, Julia Laskin, Manabu Shiraiwa, Donald Dabdub, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 18, 1643–1652, https://doi.org/10.5194/acp-18-1643-2018, https://doi.org/10.5194/acp-18-1643-2018, 2018
Short summary
Short summary
We have observed a strong effect of relative humidity on the composition of particulate matter produced from the oxidation of toluene in clean air. At higher relative humidity, there was a significant reduction in the fraction of high-molecular-weight compounds present in the particles. The amount of particulate matter also decreased at higher relative humidity. The main implication of this study is that water vapor participates in the photooxidation of toluene in a complicated way.
Julia Montoya-Aguilera, Jeremy R. Horne, Mallory L. Hinks, Lauren T. Fleming, Véronique Perraud, Peng Lin, Alexander Laskin, Julia Laskin, Donald Dabdub, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 17, 11605–11621, https://doi.org/10.5194/acp-17-11605-2017, https://doi.org/10.5194/acp-17-11605-2017, 2017
Short summary
Short summary
Various plant species emit a chemical compound called indole under stressed conditions or during flowering events. Our experiments show that indole can be oxidized in the atmosphere to produce a brownish haze containing well-known indole-derived dyes, such as indigo dye. An airshed model that includes indole chemistry shows that indole aerosol makes a significant contribution to the total aerosol burden and to visibility.
Xianda Gong, Ci Zhang, Hong Chen, Sergey A. Nizkorodov, Jianmin Chen, and Xin Yang
Atmos. Chem. Phys., 16, 5399–5411, https://doi.org/10.5194/acp-16-5399-2016, https://doi.org/10.5194/acp-16-5399-2016, 2016
Short summary
Short summary
In this study, we used a Single Particle Aerosol Mass Spectrometer and a Single Particle Soot Photometer to investigate the chemical and physical properties of black carbon (BC) aerosols during a regional air pollution episode in urban Shanghai. BC containing particles were mainly attributed to biomass burning and traffic emissions. We observed a group of highly aged traffic emitted particles with a relatively small BC core (~ 60–80 nm) and a very thick absolute coating thickness (~ 130–300 nm).
Related subject area
Subject: Aerosols | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Substantially positive contributions of new particle formation to cloud condensation nuclei under low supersaturation in China based on numerical model improvements
Evolution of atmospheric age of particles and its implications for the formation of a severe haze event in eastern China
A multimodel evaluation of the potential impact of shipping on particle species in the Mediterranean Sea
How does tropospheric VOC chemistry affect climate? An investigation of preindustrial control simulations using the Community Earth System Model version 2
Anthropogenic amplification of biogenic secondary organic aerosol production
A dynamic parameterization of sulfuric acid–dimethylamine nucleation and its application in three-dimensional modeling
Modeling dust mineralogical composition: sensitivity to soil mineralogy atlases and their expected climate impacts
Assessment of the impacts of cloud chemistry on surface SO2 and sulfate levels in typical regions of China
Impact of Landes forest fires on air quality in France during the 2022 summer
Global nitrogen and sulfur deposition mapping using a measurement–model fusion approach
Comprehensive simulations of new particle formation events in Beijing with a cluster dynamics–multicomponent sectional model
Implications of differences between recent anthropogenic aerosol emission inventories for diagnosed AOD and radiative forcing from 1990 to 2019
Unbalanced emission reductions of different species and sectors in China during COVID-19 lockdown derived by multi-species surface observation assimilation
Simulating organic aerosol in Delhi with WRF-Chem using the volatility-basis-set approach: exploring model uncertainty with a Gaussian process emulator
Modelling wintertime sea-spray aerosols under Arctic haze conditions
Impact of solar geoengineering on wildfires in the 21st century in CESM2/WACCM6
Reactive Organic Carbon Air Emissions from Mobile Sources in the United States
Linking gas, particulate, and toxic endpoints to air emissions in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Development and evaluation of processes affecting simulation of diel fine particulate matter variation in the GEOS-Chem model
Dynamics-based estimates of decline trend with fine temporal variations in China's PM2.5 emissions
Contribution of regional aerosol nucleation to low-level CCN in an Amazonian deep convective environment: results from a regionally nested global model
Development of an integrated model framework for multi-air-pollutant exposure assessments in high-density cities and the implications for epidemiological research
Coarse particulate matter air quality in East Asia: implications for fine particulate nitrate
The Emissions Model Intercomparison Project (Emissions-MIP): quantifying model sensitivity to emission characteristics
Foreign emissions exacerbate PM2.5 pollution in China through nitrate chemistry
Analysis of new particle formation events and comparisons to simulations of particle number concentrations based on GEOS-Chem–advanced particle microphysics in Beijing, China
Simulation of organic aerosol, its precursors, and related oxidants in the Landes pine forest in southwestern France: accounting for domain-specific land use and physical conditions
Modelling the European wind-blown dust emissions and their impact on particulate matter (PM) concentrations
Impacts of estimated plume rise on PM2.5 exceedance prediction during extreme wildfire events: a comparison of three schemes (Briggs, Freitas, and Sofiev)
Effects of Secondary Organic Aerosol Water on fine PM levels and composition over US
Strong particle production and condensational growth in the upper troposphere sustained by biogenic VOCs from the canopy of the Amazon Basin
Sources of organic aerosols in eastern China: a modeling study with high-resolution intermediate-volatility and semivolatile organic compound emissions
Composited analyses of the chemical and physical characteristics of co-polluted days by ozone and PM2.5 over 2013–2020 in the Beijing–Tianjin–Hebei region
Observation-based constraints on modeled aerosol surface area: implications for heterogeneous chemistry
Oligomer formation from the gas-phase reactions of Criegee intermediates with hydroperoxide esters: mechanism and kinetics
Modelling SO2 conversion into sulfates in the mid-troposphere with a 3D chemistry transport model: the case of Mount Etna's eruption on 12 April 2012
Global distribution of Asian, Middle Eastern, and North African dust simulated by CESM1/CARMA
Opinion: Coordinated development of emission inventories for climate forcers and air pollutants
Seasonal modeling analysis of nitrate formation pathways in Yangtze River Delta region, China
Modeling radiative and climatic effects of brown carbon aerosols with the ARPEGE-Climat global climate model
Numerical simulation of the impact of COVID-19 lockdown on tropospheric composition and aerosol radiative forcing in Europe
Evaluation of the WRF and CHIMERE models for the simulation of PM2.5 in large East African urban conurbations
Impact of urban heat island on inorganic aerosol in the lower free troposphere: a case study in Hangzhou, China
Statistical and machine learning methods for evaluating trends in air quality under changing meteorological conditions
Simulating the radiative forcing of oceanic dimethylsulfide (DMS) in Asia based on machine learning estimates
Quantifying the effects of mixing state on aerosol optical properties
Secondary organic aerosol formation via multiphase reaction of hydrocarbons in urban atmospheres using CAMx integrated with the UNIPAR model
Contrasting source contributions of Arctic black carbon to atmospheric concentrations, deposition flux, and atmospheric and snow radiative effects
Effect of dust on rainfall over the Red Sea coast based on WRF-Chem model simulations
A new assessment of global and regional budgets, fluxes, and lifetimes of atmospheric reactive N and S gases and aerosols
Chupeng Zhang, Shangfei Hai, Yang Gao, Yuhang Wang, Shaoqing Zhang, Lifang Sheng, Bin Zhao, Shuxiao Wang, Jingkun Jiang, Xin Huang, Xiaojing Shen, Junying Sun, Aura Lupascu, Manish Shrivastava, Jerome D. Fast, Wenxuan Cheng, Xiuwen Guo, Ming Chu, Nan Ma, Juan Hong, Qiaoqiao Wang, Xiaohong Yao, and Huiwang Gao
Atmos. Chem. Phys., 23, 10713–10730, https://doi.org/10.5194/acp-23-10713-2023, https://doi.org/10.5194/acp-23-10713-2023, 2023
Short summary
Short summary
New particle formation is an important source of atmospheric particles, exerting critical influences on global climate. Numerical models are vital tools to understanding atmospheric particle evolution, which, however, suffer from large biases in simulating particle numbers. Here we improve the model chemical processes governing particle sizes and compositions. The improved model reveals substantial contributions of newly formed particles to climate through effects on cloud condensation nuclei.
Xiaodong Xie, Jianlin Hu, Momei Qin, Song Guo, Min Hu, Dongsheng Ji, Hongli Wang, Shengrong Lou, Cheng Huang, Chong Liu, Hongliang Zhang, Qi Ying, Hong Liao, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 10563–10578, https://doi.org/10.5194/acp-23-10563-2023, https://doi.org/10.5194/acp-23-10563-2023, 2023
Short summary
Short summary
The atmospheric age of particles reflects how long particles have been formed and suspended in the atmosphere, which is closely associated with the evolution processes of particles. An analysis of the atmospheric age of PM2.5 provides a unique perspective on the evolution processes of different PM2.5 components. The results also shed lights on how to design effective emission control actions under unfavorable meteorological conditions.
Lea Fink, Matthias Karl, Volker Matthias, Sonia Oppo, Richard Kranenburg, Jeroen Kuenen, Sara Jutterström, Jana Moldanova, Elisa Majamäki, and Jukka-Pekka Jalkanen
Atmos. Chem. Phys., 23, 10163–10189, https://doi.org/10.5194/acp-23-10163-2023, https://doi.org/10.5194/acp-23-10163-2023, 2023
Short summary
Short summary
The Mediterranean Sea is a heavily trafficked shipping area, and air quality monitoring stations in numerous cities along the Mediterranean coast have detected high levels of air pollutants originating from shipping emissions. The current study investigates how existing restrictions on shipping-related emissions to the atmosphere ensure compliance with legislation. Focus was laid on fine particles and particle species, which were simulated with five different chemical transport models.
Noah A. Stanton and Neil F. Tandon
Atmos. Chem. Phys., 23, 9191–9216, https://doi.org/10.5194/acp-23-9191-2023, https://doi.org/10.5194/acp-23-9191-2023, 2023
Short summary
Short summary
Chemistry in Earth’s atmosphere has a potentially strong but very uncertain impact on climate. Past attempts to fully model chemistry in Earth’s troposphere (the lowest layer of the atmosphere) typically simplified the representation of Earth’s surface, which in turn limited the ability to simulate changes in climate. The cutting-edge model that we use in this study does not require such simplification, and we use it to examine the climate effects of chemical interactions in the troposphere.
Yiqi Zheng, Larry W. Horowitz, Raymond Menzel, David J. Paynter, Vaishali Naik, Jingyi Li, and Jingqiu Mao
Atmos. Chem. Phys., 23, 8993–9007, https://doi.org/10.5194/acp-23-8993-2023, https://doi.org/10.5194/acp-23-8993-2023, 2023
Short summary
Short summary
Biogenic secondary organic aerosols (SOAs) account for a large fraction of fine aerosol at the global scale. Using long-term measurements and a climate model, we investigate anthropogenic impacts on biogenic SOA at both decadal and centennial timescales. Results show that despite reductions in biogenic precursor emissions, SOA has been strongly amplified by anthropogenic emissions since the preindustrial era and exerts a cooling radiative forcing.
Yuyang Li, Jiewen Shen, Bin Zhao, Runlong Cai, Shuxiao Wang, Yang Gao, Manish Shrivastava, Da Gao, Jun Zheng, Markku Kulmala, and Jingkun Jiang
Atmos. Chem. Phys., 23, 8789–8804, https://doi.org/10.5194/acp-23-8789-2023, https://doi.org/10.5194/acp-23-8789-2023, 2023
Short summary
Short summary
We set up a new parameterization for 1.4 nm particle formation rates from sulfuric acid–dimethylamine (SA–DMA) nucleation, fully including the effects of coagulation scavenging and cluster stability. Incorporating the new parameterization into 3-D chemical transport models, we achieved better consistencies between simulation results and observation data. This new parameterization provides new insights into atmospheric nucleation simulations and its effects on atmospheric pollution or health.
María Gonçalves Ageitos, Vincenzo Obiso, Ron L. Miller, Oriol Jorba, Martina Klose, Matt Dawson, Yves Balkanski, Jan Perlwitz, Sara Basart, Enza Di Tomaso, Jerónimo Escribano, Francesca Macchia, Gilbert Montané, Natalie M. Mahowald, Robert O. Green, David R. Thompson, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 8623–8657, https://doi.org/10.5194/acp-23-8623-2023, https://doi.org/10.5194/acp-23-8623-2023, 2023
Short summary
Short summary
Dust aerosols affect our climate differently depending on their mineral composition. We include dust mineralogy in an atmospheric model considering two existing soil maps, which still have large associated uncertainties. The soil data and the distribution of the minerals in different aerosol sizes are key to our model performance. We find significant regional variations in climate-relevant variables, which supports including mineralogy in our current models and the need for improved soil maps.
Jianyan Lu, Sunling Gong, Jian Zhang, Jianmin Chen, Lei Zhang, and Chunhong Zhou
Atmos. Chem. Phys., 23, 8021–8037, https://doi.org/10.5194/acp-23-8021-2023, https://doi.org/10.5194/acp-23-8021-2023, 2023
Short summary
Short summary
WRF/CUACE was used to assess the cloud chemistry contribution in China. Firstly, the CUACE cloud chemistry scheme was found to reproduce well the cloud processing and consumption of H2O2, O3, and SO2, as well as the increase of sulfate. Secondly, during cloud availability in December under a heavy pollution episode, sulfate production increased 60–95 % and SO2 was reduced by over 80 %. This study provides a way to analyze the phenomenon of overestimation of SO2 in many chemical transport models.
Laurent Menut, Arineh Cholakian, Guillaume Siour, Rémy Lapere, Romain Pennel, Sylvain Mailler, and Bertrand Bessagnet
Atmos. Chem. Phys., 23, 7281–7296, https://doi.org/10.5194/acp-23-7281-2023, https://doi.org/10.5194/acp-23-7281-2023, 2023
Short summary
Short summary
This study is about the wildfires occurring in France during the summer 2022. We study the forest fires that took place in the Landes during the summer of 2022. We show the direct impact of these fires on the air quality, especially downstream of the smoke plume towards the Paris region. We quantify the impact of these fires on the pollutants peak concentrations and the possible exceedance of thresholds.
Hannah J. Rubin, Joshua S. Fu, Frank Dentener, Rui Li, Kan Huang, and Hongbo Fu
Atmos. Chem. Phys., 23, 7091–7102, https://doi.org/10.5194/acp-23-7091-2023, https://doi.org/10.5194/acp-23-7091-2023, 2023
Short summary
Short summary
We update the 2010 global deposition budget for nitrogen (N) and sulfur (S) with new regional wet deposition measurements, improving the ensemble results of 11 global chemistry transport models from HTAP II. Our study demonstrates that a global measurement–model fusion approach can substantially improve N and S deposition model estimates at a regional scale and represents a step forward toward the WMO goal of global fusion products for accurately mapping harmful air pollution.
Chenxi Li, Yuyang Li, Xiaoxiao Li, Runlong Cai, Yaxin Fan, Xiaohui Qiao, Rujing Yin, Chao Yan, Yishuo Guo, Yongchun Liu, Jun Zheng, Veli-Matti Kerminen, Markku Kulmala, Huayun Xiao, and Jingkun Jiang
Atmos. Chem. Phys., 23, 6879–6896, https://doi.org/10.5194/acp-23-6879-2023, https://doi.org/10.5194/acp-23-6879-2023, 2023
Short summary
Short summary
New particle formation and growth in polluted environments are not fully understood despite intensive research. We applied a cluster dynamics–multicomponent sectional model to simulate the new particle formation events observed in Beijing, China. The simulation approximately captures how the events evolve. Further diagnosis shows that the oxygenated organic molecules may have been under-detected, and modulating their abundance leads to significantly improved simulation–observation agreement.
Marianne Tronstad Lund, Gunnar Myhre, Ragnhild Bieltvedt Skeie, Bjørn Hallvard Samset, and Zbigniew Klimont
Atmos. Chem. Phys., 23, 6647–6662, https://doi.org/10.5194/acp-23-6647-2023, https://doi.org/10.5194/acp-23-6647-2023, 2023
Short summary
Short summary
Here we show that differences, in magnitude and trend, between recent global anthropogenic emission inventories have a notable influence on simulated regional abundances of anthropogenic aerosol over the 1990–2019 period. This, in turn, affects estimates of radiative forcing. Our findings form a basis for comparing existing and upcoming studies on anthropogenic aerosols using different emission inventories.
Lei Kong, Xiao Tang, Jiang Zhu, Zifa Wang, Yele Sun, Pingqing Fu, Meng Gao, Huangjian Wu, Miaomiao Lu, Qian Wu, Shuyuan Huang, Wenxuan Sui, Jie Li, Xiaole Pan, Lin Wu, Hajime Akimoto, and Gregory R. Carmichael
Atmos. Chem. Phys., 23, 6217–6240, https://doi.org/10.5194/acp-23-6217-2023, https://doi.org/10.5194/acp-23-6217-2023, 2023
Short summary
Short summary
A multi-air-pollutant inversion system has been developed in this study to estimate emission changes in China during COVID-19 lockdown. The results demonstrate that the lockdown is largely a nationwide road traffic control measure with NOx emissions decreasing by ~40 %. Emissions of other species only decreased by ~10 % due to smaller effects of lockdown on other sectors. Assessment results further indicate that the lockdown only had limited effects on the control of PM2.5 and O3 in China.
Ernesto Reyes-Villegas, Douglas Lowe, Jill S. Johnson, Kenneth S. Carslaw, Eoghan Darbyshire, Michael Flynn, James D. Allan, Hugh Coe, Ying Chen, Oliver Wild, Scott Archer-Nicholls, Alex Archibald, Siddhartha Singh, Manish Shrivastava, Rahul A. Zaveri, Vikas Singh, Gufran Beig, Ranjeet Sokhi, and Gordon McFiggans
Atmos. Chem. Phys., 23, 5763–5782, https://doi.org/10.5194/acp-23-5763-2023, https://doi.org/10.5194/acp-23-5763-2023, 2023
Short summary
Short summary
Organic aerosols (OAs), their sources and their processes remain poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem, can be a useful tool to describe primary OA (POA) production and aging. However, the main disadvantage is its complexity. We used a Gaussian process simulator to reproduce model results and to estimate the sources of model uncertainty. We do this by comparing the outputs with OA observations made at Delhi, India, in 2018.
Eleftherios Ioannidis, Kathy S. Law, Jean-Christophe Raut, Louis Marelle, Tatsuo Onishi, Rachel M. Kirpes, Lucia M. Upchurch, Thomas Tuch, Alfred Wiedensohler, Andreas Massling, Henrik Skov, Patricia K. Quinn, and Kerri A. Pratt
Atmos. Chem. Phys., 23, 5641–5678, https://doi.org/10.5194/acp-23-5641-2023, https://doi.org/10.5194/acp-23-5641-2023, 2023
Short summary
Short summary
Remote and local anthropogenic emissions contribute to wintertime Arctic haze, with enhanced aerosol concentrations, but natural sources, which also contribute, are less well studied. Here, modelled wintertime sea-spray aerosols are improved in WRF-Chem over the wider Arctic by including updated wind speed and temperature-dependent treatments. As a result, anthropogenic nitrate aerosols are also improved. Open leads are confirmed to be the main source of sea-spray aerosols over northern Alaska.
Wenfu Tang, Simone Tilmes, David M. Lawrence, Fang Li, Cenlin He, Louisa K. Emmons, Rebecca R. Buchholz, and Lili Xia
Atmos. Chem. Phys., 23, 5467–5486, https://doi.org/10.5194/acp-23-5467-2023, https://doi.org/10.5194/acp-23-5467-2023, 2023
Short summary
Short summary
Globally, total wildfire burned area is projected to increase over the 21st century under scenarios without geoengineering and decrease under the two geoengineering scenarios. Geoengineering reduces fire by decreasing surface temperature and wind speed and increasing relative humidity and soil water. However, geoengineering also yields reductions in precipitation, which offset some of the fire reduction.
Benjamin N. Murphy, Darrell Sonntag, Karl M. Seltzer, Havala O. T. Pye, Christine Allen, Evan Murray, Claudia Toro, Drew R. Gentner, Cheng Huang, Shantanu H. Jathar, Li Li, Andrew A. May, and Allen L. Robinson
EGUsphere, https://doi.org/10.5194/egusphere-2023-855, https://doi.org/10.5194/egusphere-2023-855, 2023
Short summary
Short summary
We update methods for calculating organic particle and vapor emissions from mobile sources in the U.S. Conventionally, particulate matter (PM) and volatile organic carbon (VOC) are speciated without consideration of primary semivolatile emissions. Our methods integrate state-of-the-science speciation profiles and correct for common artifacts when sampling emissions in a laboratory. We quantify impacts of the emission updates on ambient pollution with the Community Multiscale Air Quality model.
Havala O. T. Pye, Bryan K. Place, Benjamin N. Murphy, Karl M. Seltzer, Emma L. D'Ambro, Christine Allen, Ivan R. Piletic, Sara Farrell, Rebecca H. Schwantes, Matthew M. Coggon, Emily Saunders, Lu Xu, Golam Sarwar, William T. Hutzell, Kristen M. Foley, George Pouliot, Jesse Bash, and William R. Stockwell
Atmos. Chem. Phys., 23, 5043–5099, https://doi.org/10.5194/acp-23-5043-2023, https://doi.org/10.5194/acp-23-5043-2023, 2023
Short summary
Short summary
Chemical mechanisms describe how emissions from vehicles, vegetation, and other sources are chemically transformed in the atmosphere to secondary products including criteria and hazardous air pollutants. The Community Regional Atmospheric Chemistry Multiphase Mechanism integrates gas-phase radical chemistry with pathways to fine-particle mass. New species were implemented, resulting in a bottom-up representation of organic aerosol, which is required for accurate source attribution of pollutants.
Yanshun Li, Randall V. Martin, Chi Li, Brian L. Boys, Aaron van Donkelaar, Jun Meng, and Jeffrey R. Pierce
EGUsphere, https://doi.org/10.5194/egusphere-2023-704, https://doi.org/10.5194/egusphere-2023-704, 2023
Short summary
Short summary
We developed and evaluated processes affecting within-day (diel) variability in fine particulate matter (PM2.5) concentrations in a chemical transport model (GEOS-Chem) over the US. We find that diel variability in PM2.5 is driven by 1) early morning accumulation into a shallow mixed layer, 2) decreases from mid-morning through afternoon with mixed-layer growth, 3) increases from mid-afternoon through evening as the mixed-layer collapses, and 4) decreases overnight as emissions decrease.
Zhen Peng, Lili Lei, Zhe-Min Tan, Meigen Zhang, Aijun Ding, and Xingxia Kou
EGUsphere, https://doi.org/10.5194/egusphere-2023-755, https://doi.org/10.5194/egusphere-2023-755, 2023
Short summary
Short summary
Annual PM2.5 emission in China consistently decreases about 3 % to 5 % from 2017 to 2020 with spatial variations and seasonal dependences. High temporal-resolution and dynamics-based PM2.5 emission estimates provide quantitative diurnal variations for each season. Significant reduction of PM2.5 emissions in the north China plain and northeast of China in 2020 are caused by COVID-19.
Xuemei Wang, Hamish Gordon, Daniel P. Grosvenor, Meinrat O. Andreae, and Ken S. Carslaw
Atmos. Chem. Phys., 23, 4431–4461, https://doi.org/10.5194/acp-23-4431-2023, https://doi.org/10.5194/acp-23-4431-2023, 2023
Short summary
Short summary
New particle formation in the upper troposphere is important for the global boundary layer aerosol population, and they can be transported downward in Amazonia. We use a global and a regional model to quantify the number of aerosols that are formed at high altitude and transported downward in a 1000 km region. We find that the majority of the aerosols are from outside the region. This suggests that the 1000 km region is unlikely to be a
closed loopfor aerosol formation, transport and growth.
Zhiyuan Li, Kin-Fai Ho, Harry Fung Lee, and Steve Hung Lam Yim
EGUsphere, https://doi.org/10.5194/egusphere-2023-513, https://doi.org/10.5194/egusphere-2023-513, 2023
Short summary
Short summary
This study developed an integrated model framework for accurate multi-air-pollutant exposure assessments in high-density and high-rise cities. Following the proposed integrated model framework, we established multi-air-pollutant exposure models for four major PM10 chemical species as well as four criteria air pollutants with R2 values ranging from 0.73 to 0.93. The proposed framework serves an important tool for combined exposure assessment and the corresponding epidemiological studies.
Shixian Zhai, Daniel J. Jacob, Drew C. Pendergrass, Nadia K. Colombi, Viral Shah, Laura Hyesung Yang, Qiang Zhang, Shuxiao Wang, Hwajin Kim, Yele Sun, Jin-Soo Choi, Jin-Soo Park, Gan Luo, Fangqun Yu, Jung-Hun Woo, Younha Kim, Jack E. Dibb, Taehyoung Lee, Jin-Seok Han, Bruce E. Anderson, Ke Li, and Hong Liao
Atmos. Chem. Phys., 23, 4271–4281, https://doi.org/10.5194/acp-23-4271-2023, https://doi.org/10.5194/acp-23-4271-2023, 2023
Short summary
Short summary
Anthropogenic fugitive dust in East Asia not only causes severe coarse particulate matter air pollution problems, but also affects fine particulate nitrate. Due to emission control efforts, coarse PM decreased steadily. We find that the decrease of coarse PM is a major driver for a lack of decrease of fine particulate nitrate, as it allows more nitric acid to form fine particulate nitrate. The continuing decrease of coarse PM requires more stringent ammonia and nitrogen oxides emission controls.
Hamza Ahsan, Hailong Wang, Jingbo Wu, Mingxuan Wu, Steven J. Smith, Susanne Bauer, Harrison Suchyta, Dirk Olivié, Gunnar Myhre, Hitoshi Matsui, Huisheng Bian, Jean-François Lamarque, Ken Carslaw, Larry Horowitz, Leighton Regayre, Mian Chin, Michael Schulz, Ragnhild Bieltvedt Skeie, Toshihiko Takemura, and Vaishali Naik
EGUsphere, https://doi.org/10.5194/egusphere-2023-604, https://doi.org/10.5194/egusphere-2023-604, 2023
Short summary
Short summary
We examine the impact of the assumed effective height of SO2 injection, SO2 and BC emissions seasonality, and the assumed fraction of SO2 emissions injected as SO4 on climate and chemistry model results. We find that the SO2 injection height has a large impact on surface SO2 concentrations and, in some models, radiative flux. These assumptions are a “hidden” source of inter-model variability and may be leading to bias in some climate model results.
Jun-Wei Xu, Jintai Lin, Gan Luo, Jamiu Adeniran, and Hao Kong
Atmos. Chem. Phys., 23, 4149–4163, https://doi.org/10.5194/acp-23-4149-2023, https://doi.org/10.5194/acp-23-4149-2023, 2023
Short summary
Short summary
Research on the sources of Chinese PM2.5 pollution has focused on the contributions of China’s domestic emissions. However, the impact of foreign anthropogenic emissions has typically been simplified or neglected. Here we find that foreign anthropogenic emissions play an important role in Chinese PM2.5 pollution through chemical interactions between foreign-transported pollutants and China’s local emissions. Thus, foreign emission reductions are essential for improving Chinese air quality.
Kun Wang, Xiaoyan Ma, Rong Tian, and Fangqun Yu
Atmos. Chem. Phys., 23, 4091–4104, https://doi.org/10.5194/acp-23-4091-2023, https://doi.org/10.5194/acp-23-4091-2023, 2023
Short summary
Short summary
From 12 March to 6 April 2016 in Beijing, there were 11 typical new particle formation days, 13 non-event days, and 2 undefined days. We first analyzed the favorable background of new particle formation in Beijing and then conducted the simulations using four nucleation schemes based on a global chemistry transport model (GEOS-Chem) to understand the nucleation mechanism.
Arineh Cholakian, Matthias Beekmann, Guillaume Siour, Isabelle Coll, Manuela Cirtog, Elena Ormeño, Pierre-Marie Flaud, Emilie Perraudin, and Eric Villenave
Atmos. Chem. Phys., 23, 3679–3706, https://doi.org/10.5194/acp-23-3679-2023, https://doi.org/10.5194/acp-23-3679-2023, 2023
Short summary
Short summary
This article revolves around the simulation of biogenic secondary organic aerosols in the Landes forest (southwestern France). Several sensitivity cases involving biogenic emission factors, land cover data, anthropogenic emissions, and physical or meteorological parameters were performed and each compared to measurements both in the forest canopy and around the forest. The chemistry behind the formation of these aerosols and their production and transport in the forest canopy is discussed.
Marina Liaskoni, Peter Huszar, Lukáš Bartík, Alvaro Patricio Prieto Perez, Jan Karlický, and Ondřej Vlček
Atmos. Chem. Phys., 23, 3629–3654, https://doi.org/10.5194/acp-23-3629-2023, https://doi.org/10.5194/acp-23-3629-2023, 2023
Short summary
Short summary
Wind-blown dust (WBD) emissions emitted from European soils are estimated for the 2007–2016 period, and their impact on the total particulate matter (PM) concentration is calculated. We found a considerable increase in PM concentrations due to such emissions, especially on selected days (rather than on a seasonal average). We also found that WBD emissions are strongest over western Europe, and the highest impacts on PM are calculated for this region.
Yunyao Li, Daniel Tong, Siqi Ma, Saulo R. Freitas, Ravan Ahmadov, Mikhail Sofiev, Xiaoyang Zhang, Shobha Kondragunta, Ralph Kahn, Youhua Tang, Barry Baker, Patrick Campbell, Rick Saylor, Georg Grell, and Fangjun Li
Atmos. Chem. Phys., 23, 3083–3101, https://doi.org/10.5194/acp-23-3083-2023, https://doi.org/10.5194/acp-23-3083-2023, 2023
Short summary
Short summary
Plume height is important in wildfire smoke dispersion and affects air quality and human health. We assess the impact of plume height on wildfire smoke dispersion and the exceedances of the National Ambient Air Quality Standards. A higher plume height predicts lower pollution near the source region, but higher pollution in downwind regions, due to the faster spread of the smoke once ejected, affects pollution exceedance forecasts and the early warning of extreme air pollution events.
Stylianos Kakavas, Spyros Pandis, and Athanasios Nenes
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-815, https://doi.org/10.5194/acp-2022-815, 2023
Revised manuscript accepted for ACP
Short summary
Short summary
Water uptake from organic species in aerosol can affect the partitioning of semi-volatile inorganic compounds, but are not considered in global and chemical transport models. We address this with a version of the PM-CAMx model that considers such organic water effects and use it to carry out year-long aerosol simulations over the continental US. We show that such organic water impacts can have an important impact on dry PM1 levels when RH levels and PM1 concentrations are high.
Yunfan Liu, Hang Su, Siwen Wang, Chao Wei, Wei Tao, Mira L. Pöhlker, Christopher Pöhlker, Bruna A. Holanda, Ovid O. Krüger, Thorsten Hoffmann, Manfred Wendisch, Paulo Artaxo, Ulrich Pöschl, Meinrat O. Andreae, and Yafang Cheng
Atmos. Chem. Phys., 23, 251–272, https://doi.org/10.5194/acp-23-251-2023, https://doi.org/10.5194/acp-23-251-2023, 2023
Short summary
Short summary
The origins of the abundant cloud condensation nuclei (CCN) in the upper troposphere (UT) of the Amazon remain unclear. With model developments of new secondary organic aerosol schemes and constrained by observation, we show that strong aerosol nucleation and condensation in the UT is triggered by biogenic organics, and organic condensation is key for UT CCN production. This UT CCN-producing mechanism may prevail over broader vegetation canopies and deserves emphasis in aerosol–climate feedback.
Jingyu An, Cheng Huang, Dandan Huang, Momei Qin, Huan Liu, Rusha Yan, Liping Qiao, Min Zhou, Yingjie Li, Shuhui Zhu, Qian Wang, and Hongli Wang
Atmos. Chem. Phys., 23, 323–344, https://doi.org/10.5194/acp-23-323-2023, https://doi.org/10.5194/acp-23-323-2023, 2023
Short summary
Short summary
This paper aims to build up an approach to establish a high-resolution emission inventory of intermediate-volatility and semi-volatile organic compounds in city-scale and detailed source categories and incorporate it into the CMAQ model. We believe this approach can be widely applied to improve the simulation of secondary organic aerosol and its source contributions.
Huibin Dai, Hong Liao, Ke Li, Xu Yue, Yang Yang, Jia Zhu, Jianbing Jin, Baojie Li, and Xingwen Jiang
Atmos. Chem. Phys., 23, 23–39, https://doi.org/10.5194/acp-23-23-2023, https://doi.org/10.5194/acp-23-23-2023, 2023
Short summary
Short summary
We apply the 3-D global chemical transport model (GEOS-Chem) to simulate co-polluted days by O3 and PM2.5 (O3–PM2.5PDs) in Beijing–Tianjin–Hebei in 2013–2020 and investigate the chemical and physical characteristics of O3–PM2.5PDs by composited analyses of such days that are captured by both the observations and the model. We report for the first time the unique features in vertical distributions of aerosols during O3–PM2.5PDs and the physical and chemical characteristics of O3–PM2.5PDs.
Rachel A. Bergin, Monica Harkey, Alicia Hoffman, Richard H. Moore, Bruce Anderson, Andreas Beyersdorf, Luke Ziemba, Lee Thornhill, Edward Winstead, Tracey Holloway, and Timothy H. Bertram
Atmos. Chem. Phys., 22, 15449–15468, https://doi.org/10.5194/acp-22-15449-2022, https://doi.org/10.5194/acp-22-15449-2022, 2022
Short summary
Short summary
Correctly predicting aerosol surface area concentrations is important for determining the rate of heterogeneous reactions in chemical transport models. Here, we compare aircraft measurements of aerosol surface area with a regional model. In polluted air masses, we show that the model underpredicts aerosol surface area by a factor of 2. Despite this disagreement, the representation of heterogeneous chemistry still dominates the overall uncertainty in the loss rate of molecules such as N2O5.
Long Chen, Yu Huang, Yonggang Xue, Zhihui Jia, and Wenliang Wang
Atmos. Chem. Phys., 22, 14529–14546, https://doi.org/10.5194/acp-22-14529-2022, https://doi.org/10.5194/acp-22-14529-2022, 2022
Short summary
Short summary
Quantum chemical methods are applied to gain insight into the oligomerization reaction mechanisms and kinetics of distinct stabilized Criegee intermediate (SCI) reactions with hydroperoxide esters, where calculations show that SCI addition reactions with hydroperoxide esters proceed through the successive insertion of SCIs to form oligomers that involve SCIs as the repeating unit. The saturated vapor pressure of the formed oligomers decreases monotonically with the increasing number of SCIs.
Mathieu Lachatre, Sylvain Mailler, Laurent Menut, Arineh Cholakian, Pasquale Sellitto, Guillaume Siour, Henda Guermazi, Giuseppe Salerno, and Salvatore Giammanco
Atmos. Chem. Phys., 22, 13861–13879, https://doi.org/10.5194/acp-22-13861-2022, https://doi.org/10.5194/acp-22-13861-2022, 2022
Short summary
Short summary
In this study, we have evaluated the predominance of various pathways of volcanic SO2 conversion to sulfates in the upper troposphere. We show that the main conversion pathway was gaseous oxidation by OH, although the liquid pathways were expected to be predominant. These results are interesting with respect to a better understanding of sulfate formation in the middle and upper troposphere and are an important component to help evaluate particulate matter radiative forcing.
Siying Lian, Luxi Zhou, Daniel M. Murphy, Karl D. Froyd, Owen B. Toon, and Pengfei Yu
Atmos. Chem. Phys., 22, 13659–13676, https://doi.org/10.5194/acp-22-13659-2022, https://doi.org/10.5194/acp-22-13659-2022, 2022
Short summary
Short summary
Parameterizations of dust lifting and microphysical properties of dust in climate models are still subject to large uncertainty. Here we use a sectional aerosol climate model to investigate the global vertical distributions of the dust. Constrained by a suite of observations, the model suggests that, although North African dust dominates global dust mass loading at the surface, the relative contribution of Asian dust increases with altitude and becomes dominant in the upper troposphere.
Steven J. Smith, Erin E. McDuffie, and Molly Charles
Atmos. Chem. Phys., 22, 13201–13218, https://doi.org/10.5194/acp-22-13201-2022, https://doi.org/10.5194/acp-22-13201-2022, 2022
Short summary
Short summary
Emissions into the atmosphere of greenhouse gases (GHGs) and air pollutants, quantified in emission inventories, impact human health, ecosystems, and the climate. We review how air pollutant and GHG inventory activities have historically been structured and their different uses and requirements. We discuss the benefits of increasing coordination between air pollutant and GHG inventory development efforts, but also caution that there are differences in appropriate methodologies and applications.
Jinjin Sun, Momei Qin, Xiaodong Xie, Wenxing Fu, Yang Qin, Li Sheng, Lin Li, Jingyi Li, Ishaq Dimeji Sulaymon, Lei Jiang, Lin Huang, Xingna Yu, and Jianlin Hu
Atmos. Chem. Phys., 22, 12629–12646, https://doi.org/10.5194/acp-22-12629-2022, https://doi.org/10.5194/acp-22-12629-2022, 2022
Short summary
Short summary
NO3- has become the dominant and the least reduced chemical component of fine particulate matter in China. NO3- formation is mostly in the NH3-rich regime in the Yangtze River Delta (YRD). OH + NO2 contributes 60 %–83 % of the TNO3 production rates, and the N2O5 heterogeneous pathway contributes 10 %–36 %. The N2O5 heterogeneous pathway becomes more important in cold seasons. Local emissions and regional transportation contribute 50 %–62 % and 38 %–50 % to YRD NO3- concentrations, respectively.
Thomas Drugé, Pierre Nabat, Marc Mallet, Martine Michou, Samuel Rémy, and Oleg Dubovik
Atmos. Chem. Phys., 22, 12167–12205, https://doi.org/10.5194/acp-22-12167-2022, https://doi.org/10.5194/acp-22-12167-2022, 2022
Short summary
Short summary
This study presents the implementation of brown carbon in the atmospheric component of the CNRM global climate model and particularly in its aerosol scheme TACTIC. Several simulations were carried out with this climate model, over the period 2000–2014, to evaluate the model by comparison with different reference datasets (PARASOL-GRASP, OMI-OMAERUVd, MACv2, FMI_SAT, AERONET) and to analyze the brown carbon radiative and climatic effects.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
Short summary
Short summary
In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Andrea Mazzeo, Michael Burrow, Andrew Quinn, Eloise A. Marais, Ajit Singh, David Ng'ang'a, Michael J. Gatari, and Francis D. Pope
Atmos. Chem. Phys., 22, 10677–10701, https://doi.org/10.5194/acp-22-10677-2022, https://doi.org/10.5194/acp-22-10677-2022, 2022
Short summary
Short summary
A modelling system for meteorology and chemistry transport processes, WRF–CHIMERE, has been tested and validated for three East African conurbations using the most up-to-date anthropogenic emissions available. Results show that the model is able to reproduce hourly and daily temporal variabilities in aerosol concentrations that are close to observations in both urban and rural environments, encouraging the adoption of numerical modelling as a tool for air quality management in East Africa.
Hanqing Kang, Bin Zhu, Gerrit de Leeuw, Bu Yu, Ronald J. van der A, and Wen Lu
Atmos. Chem. Phys., 22, 10623–10634, https://doi.org/10.5194/acp-22-10623-2022, https://doi.org/10.5194/acp-22-10623-2022, 2022
Short summary
Short summary
This study quantified the contribution of each urban-induced meteorological effect (temperature, humidity, and circulation) to aerosol concentration. We found that the urban heat island (UHI) circulation dominates the UHI effects on aerosol. The UHI circulation transports aerosol and its precursor gases from the warmer lower boundary layer to the colder lower free troposphere and promotes the secondary formation of ammonium nitrate aerosol in the cold atmosphere.
Minghao Qiu, Corwin Zigler, and Noelle E. Selin
Atmos. Chem. Phys., 22, 10551–10566, https://doi.org/10.5194/acp-22-10551-2022, https://doi.org/10.5194/acp-22-10551-2022, 2022
Short summary
Short summary
Evaluating impacts of emission changes on air quality requires accounting for meteorological variability. Many studies use simple regression methods to correct for meteorology, but little is known about their performance. Using cases in the US and China, we show that widely used regression models do not perform well and can lead to biased estimates of emission-driven trends. We propose a novel machine learning method with lower bias and provide recommendations to policymakers and researchers.
Junri Zhao, Weichun Ma, Kelsey R. Bilsback, Jeffrey R. Pierce, Shengqian Zhou, Ying Chen, Guipeng Yang, and Yan Zhang
Atmos. Chem. Phys., 22, 9583–9600, https://doi.org/10.5194/acp-22-9583-2022, https://doi.org/10.5194/acp-22-9583-2022, 2022
Short summary
Short summary
Marine dimethylsulfide (DMS) emissions play important roles in atmospheric sulfur cycle and climate effects. In this study, DMS emissions were estimated by using the machine learning method and drove the global 3D chemical transport model to simulate their climate effects. To our knowledge, this is the first study in the Asian region that quantifies the combined impacts of DMS on sulfate, particle number concentration, and radiative forcings.
Yu Yao, Jeffrey H. Curtis, Joseph Ching, Zhonghua Zheng, and Nicole Riemer
Atmos. Chem. Phys., 22, 9265–9282, https://doi.org/10.5194/acp-22-9265-2022, https://doi.org/10.5194/acp-22-9265-2022, 2022
Short summary
Short summary
Investigating the impacts of aerosol mixing state on aerosol optical properties has a long history from both the modeling and experimental perspective. In this study, we used particle-resolved simulations as a benchmark to determine the error in optical properties when using simplified aerosol representations. We found that errors in single scattering albedo due to the internal mixture assumptions can have substantial effects on calculating aerosol direct radiative forcing.
Zechen Yu, Myoseon Jang, Soontae Kim, Kyuwon Son, Sanghee Han, Azad Madhu, and Jinsoo Park
Atmos. Chem. Phys., 22, 9083–9098, https://doi.org/10.5194/acp-22-9083-2022, https://doi.org/10.5194/acp-22-9083-2022, 2022
Short summary
Short summary
The UNIPAR model was incorporated into CAMx to predict the ambient concentration of organic matter in urban atmospheres during the KORUS-AQ campaign. CAMx–UNIPAR significantly improved the simulation of SOA formation under the wet aerosol condition through the consideration of aqueous reactions of reactive organic species and gas–aqueous partitioning into the wet inorganic aerosol.
Hitoshi Matsui, Tatsuhiro Mori, Sho Ohata, Nobuhiro Moteki, Naga Oshima, Kumiko Goto-Azuma, Makoto Koike, and Yutaka Kondo
Atmos. Chem. Phys., 22, 8989–9009, https://doi.org/10.5194/acp-22-8989-2022, https://doi.org/10.5194/acp-22-8989-2022, 2022
Short summary
Short summary
Using a global aerosol model, we find that the source contributions to radiative effects of black carbon (BC) in the Arctic are quite different from those to mass concentrations and deposition flux of BC in the Arctic. This is because microphysical properties (e.g., mixing state), altitudes, and seasonal variations of BC in the atmosphere differ among emissions sources. These differences need to be considered for accurate simulations of Arctic BC and its source contributions and climate impacts.
Sagar P. Parajuli, Georgiy L. Stenchikov, Alexander Ukhov, Suleiman Mostamandi, Paul A. Kucera, Duncan Axisa, William I. Gustafson Jr., and Yannian Zhu
Atmos. Chem. Phys., 22, 8659–8682, https://doi.org/10.5194/acp-22-8659-2022, https://doi.org/10.5194/acp-22-8659-2022, 2022
Short summary
Short summary
Rainfall affects the distribution of surface- and groundwater resources, which are constantly declining over the Middle East and North Africa (MENA) due to overexploitation. Here, we explored the effects of dust on rainfall using WRF-Chem model simulations. Although dust is considered a nuisance from an air quality perspective, our results highlight the positive fundamental role of dust particles in modulating rainfall formation and distribution, which has implications for cloud seeding.
Yao Ge, Massimo Vieno, David S. Stevenson, Peter Wind, and Mathew R. Heal
Atmos. Chem. Phys., 22, 8343–8368, https://doi.org/10.5194/acp-22-8343-2022, https://doi.org/10.5194/acp-22-8343-2022, 2022
Short summary
Short summary
Reactive N and S gases and aerosols are critical determinants of air quality. We report a comprehensive analysis of the concentrations, wet and dry deposition, fluxes, and lifetimes of these species globally as well as for 10 world regions. We used the EMEP MSC-W model coupled with WRF meteorology and 2015 global emissions. Our work demonstrates the substantial regional variation in these quantities and the need for modelling to simulate atmospheric responses to precursor emissions.
Cited articles
Albaladejo, J., Ballesteros, B., Jimenez, E., Martin, P., and Martinez, E.: A PLP-LIF kinetic study of the atmospheric reactivity of a series of C4-C7 saturated and unsaturated aliphatic aldehydes with OH, Atmos. Environ., 36, 3231–3239, 2002.
Albinet, A., Minero, C., and Vione, D.: Photochemical generation of reactive species upon irradiation of rainwater: Negligible photoactivity of dissolved organic matter, Sci. Total Environ., 408, 3367–3373, https://doi.org/10.1016/j.scitotenv.2010.04.011, 2010a.
Albinet, A., Minero, C., and Vione, D.: Phototransformation processes of 2,4-dinitrophenol, relevant to atmospheric water droplets, Chemosphere, 80, 753–758, 2010b.
Amyes, T. L. and Richard, J. P.: Enzymatic catalysis of proton transfer at carbon: Activation of triosephosphate isomerase by phosphite dianion, Biochemistry, 46, 5841–5854, https://doi.org/10.1021/bi700409b, 2007.
Atkinson, R.: A structure-activity relationship for the estimation of rate constants for the gas-phase reactions of OH radicals with organic compounds, Int. J. Chem. Kinet., 19, 799–828, https://doi.org/10.1002/kin.550190903, 1987.
Atkinson, R., Tuazon, E. C., and Aschmann, S. M.: Atmospheric chemistry of 2-pentanone and 2-heptanone, Environ. Sci. Technol., 34, 623–631, https://doi.org/10.1021/es9909374, 2000.
Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F., Hynes, R. G., Jenkin, M. E., Rossi, M. J., and Troe, J.: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume II; gas phase reactions of organic species, Atmos. Chem. Phys., 6, 3625–4055, https://doi.org/10.5194/acp-6-3625-2006, 2006.
Bacher, C., Tyndall, G., and Orlando, J.: The atmospheric chemistry of glycolaldehyde, J. Atmos. Chem., 39, 171–189, https://doi.org/10.1023/a:1010689706869, 2001.
Bayliss, N. S. and McRae, E. G.: Solvent effects in the spectra of acetone, crotonaldehyde, nitromethane and nitrobenzene, J. Phys. Chem., 58, 1006–1011, https://doi.org/10.1021/j150521a018, 1954.
Bayrakçeken, F.: Sensitized phosphorescence studies of p-xylene + biacetyl system, an optical antenna, Spectrochim. Acta A, 66, 1267–1270, https://doi.org/10.1016/j.saa.2006.06.018, 2007.
Bell, R. P. and Gold, V.: The reversible hydration of carbonyl compounds, in: Adv. Phys. Org. Chem., Academic Press, 1–29, 1966.
Berger, R., Fischer, C., and Klessinger, M.: Calculation of the vibronic fine structure in electronic spectra at higher temperatures. 1. Benzene and pyrazine, J. Phys. Chem. A, 102, 7157–7167, https://doi.org/10.1021/jp981597w, 1998.
Betterton, E. A., and Hoffmann, M. R.: Henry's law constants of some environmentally important aldehydes, Environ. Sci. Technol., 22, 1415–1418, https://doi.org/10.1021/es00177a004, 1988.
Bowman, J. H., Barket, D. J., and Shepson, P. B.: Atmospheric chemistry of nonanal, Environ. Sci. Technol., 37, 2218–2225, 2003.
Brown, H. C., McDaniel, D. H., and Hãfliger, O.: Determination of organic structures by physical methods, Dissociation Constants, edited by: Braude, E. A. and Nachod, F. C., v. 1, Academic Press, 1955.
Bunce, N. J., Lamarre, J., and Vaish, S. P.: Photorearrangement of azoxybenzene to 2-hydroxyazobenzene: A convenient chemical actinometer, Photochem. Photobiol., 39, 531–533, https://doi.org/10.1111/j.1751-1097.1984.tb03888.x, 1984.
Buschmann, H.-J., Füldner, H.-H., and Knoche, W.: The reversible hydration of carbonyl compounds in aqueous solution. Part i, the keto/gem-diol equilibrium, Berichte der Bunsengesellschaft für physikalische Chemie, 84, 41–44, https://doi.org/10.1002/bbpc.19800840109, 1980.
Buttery, R. G., Bomben, J. L., Guadagni, D. G., and Ling, L. C.: Volatilities of organic flavor compounds in foods, J. Agric. Food. Chem., 19, 1045–1048, https://doi.org/10.1021/jf60178a004, 1971.
Buxton, G. V., Greenstock, C. L., Helman, W. P., and Ross, A. B.: Critical review of rate constants for reactions of hydrated electrons, hydrogen atoms and hydroxyl radicals in aqueous solution, J. Phys. Chem. Ref. Data, 17, 513–886, 1988.
Buxton, G. V., Malone, N. T., and Salmon, G. A.: Oxidation of glyoxal initiated by OH in oxygenated aqueous solution, J. Chem. Soc., Faraday Trans., 93, 2889–2891, 1997.
Calvert, J. G. and Pitts, J. N.: Photochemistry, Wiley, New York, NY, 625–626, 1966.
Cederstav, A. K. and Novak, B. M.: Investigations into the chemistry of thermodynamically unstable species. The direct polymerization of vinyl alcohol, the enolic tautomer of acetaldehyde, J. Am. Chem. Soc., 116, 4073–4074, https://doi.org/10.1021/ja00088a051, 1994.
Chen, J., Peijnenburg, W. J. G. M., Quan, X., and Yang, F.: Quantitative structure property relationships for direct photolysis quantum yields of selected polycyclic aromatic hydrocarbons, Sci. Total Environ., 246, 11–20, 2000.
Dagaut, P., Wallington, T. J., Liu, R., and Kurylo, M. J.: A kinetics investigation of the gas-phase reactions of OH radicals with cyclic ketones and diones: Mechanistic insights, J. Phys. Chem., 92, 4375–4377, 1988.
Dawson, R. M. C., Elliott, D. C., and Elliott, W. H.: Data for biochemical research, Oxford University Press on Demand, 1989.
Dearden, J. C. and Schüürmann, G.: Quantitative structure-property relationships for predicting Henry's law constant from molecular structure, Environ. Toxicol. Chem., 22, 1755–1770, https://doi.org/10.1897/01-605, 2003.
Dierksen, M. and Grimme, S.: Density functional calculations of the vibronic structure of electronic absorption spectra, J. Chem. Phys., 120, 3544–3554, 2004.
Doussin, J. F. and Monod, A.: Structure-activity relationship for the estimation of OH-oxidation rate constants of carbonyl compounds in the aqueous phase, Atmos. Chem. Phys. Discuss., 13, 15949–15991, https://doi.org/10.5194/acpd-13-15949-2013, 2013.
Encinas, M. V., Rufs, A. M., and Lissi, E. A.: Photochemistry of hydroxyalkanones in solution, J. Chem. Soc., Perkin Trans. 2, 457–460, 1985.
Epstein, S. A. and Nizkorodov, S. A.: A comparison of the chemical sinks of atmospheric organics in the gas and aqueous phase, Atmos. Chem. Phys., 12, 8205–8222, https://doi.org/10.5194/acp-12-8205-2012, 2012.
Epstein, S. A., Shemesh, D., Tran, V. T., Nizkorodov, S. A., and Gerber, R. B.: Absorption spectra and photolysis of methyl peroxide in liquid and frozen water, J. Phys. Chem. A, 24, 6068–6077, 2012.
Ervens, B. and Volkamer, R.: Glyoxal processing by aerosol multiphase chemistry: Towards a kinetic modeling framework of secondary organic aerosol formation in aqueous particles, Atmos. Chem. Phys., 10, 8219–8244, https://doi.org/10.5194/acp-10-8219-2010, 2010.
Ervens, B., George, C., Williams, J. E., Buxton, G. V., Salmon, G. A., Bydder, M., Wilkinson, F., Dentener, F., Mirabel, P., Wolke, R., and Herrmann, H.: Capram 2.4 (modac mechanism): An extended and condensed tropospheric aqueous phase mechanism and its application, J. Geophys. Res., 108, 4426, https://doi.org/10.1029/2002jd002202, 2003a.
Ervens, B., Gligorovski, S., and Herrmann, H.: Temperature-dependent rate constants for hydroxyl radical reactions with organic compounds in aqueous solutions, Phys. Chem. Chem. Phys., 5, 1811–1824, 2003b.
Ervens, B., Turpin, B. J., and Weber, R. J.: Secondary organic aerosol formation in cloud droplets and aqueous particles (aqSOA): A review of laboratory, field and model studies, Atmos. Chem. Phys., 11, 11069–11102, https://doi.org/10.5194/acp-11-11069-2011, 2011.
Esposito, A., Lukas, A., Meany, J. E., and Pocker, Y.: The reversible enolization and hydration of pyruvate: Possible roles of keto, enol, and hydrated pyruvate in lactate dehydrogenase catalysis, Can. J. Chem., 77, 1108–1117, https://doi.org/10.1139/v99-071, 1999.
Facchini, M. C., Fuzzi, S., Zappoli, S., Andracchio, A., Gelencsér, A., Kiss, G., Krivácsy, Z., Mészáros, E., Hansson, H.-C., Alsberg, T., and Zebühr, Y.: Partitioning of the organic aerosol component between fog droplets and interstitial air, J. Geophys. Res., 104, 26821–26832, https://doi.org/10.1029/1999jd900349, 1999.
Fang, W., Gong, L., Zhang, Q., Cao, M., Li, Y., and Sheng, L.: Measurements of secondary organic aerosol formed from OH-initiated photo-oxidation of isoprene using online photoionization aerosol mass spectrometry, Environ. Sci. Tech., 46, 3898–3904, https://doi.org/10.1021/es204669d, 2012.
Finlayson-Pitts, B. J. and Pitts, J. N.: Chemistry of the upper and lower atmosphere, Academic Press, San Diego, CA, USA, 93–128, 2000.
Fischer, M. and Warneck, P.: The dissociation constant of pyruvic acid: Determination by spectrophotometric measurements, Berichte der Bunsengesellschaft für physikalische Chemie, 95, 523–527, https://doi.org/10.1002/bbpc.19910950414, 1991.
Frelek, J., Kowalska, P., Masnyk, M., Kazimierski, A., Korda, A., Wo\'znica, M., Chmielewski, M., and Furche, F.: Circular dichroism and conformational dynamics of cephams and their carba and oxa analogues, Chem.-Eur. J., 13, 6732–6744, https://doi.org/10.1002/chem.200700127, 2007.
Frenkel, D. and Smit, B.: Understanding molecular simulation: From algorithms to applications, Elsevier Science, 153–158, 2001.
Furche, F. and Rappoport, D.: Computational photochemistry, Computational and theoretical chemistry, edited by: Olivucci, M., Elsevier, Amsterdam, 93–128, 2005.
Garcia-Jiminez, F., Zuniga, O. C., Garcia, Y. C., Cardenas, J., and Cuevas, G.: Experimental and theoretical study of the products from the spontaneous dimerization of dl- and d-glyceraldehyde, J. Brazil. Chem. Soc., 16, 467–476, 2005.
Gelencser, A. and Varga, Z.: Evaluation of the atmospheric significance of multiphase reactions in atmospheric secondary organic aerosol formation, Atmos. Chem. Phys., 5, 2823–2831, https://doi.org/10.5194/acp-5-2823-2005, 2005.
Glushonok, G. K., Petryaev, E. P., Turetskaya, E. A., and Shadyro, O. I.: Equilibrium between the molecular forms of glycolaldehyde and of DL-glyceraldehyde in aqueous solutions, Zh. Fiz. Khim., 60, 2960–2970, 1986.
Glushonok, G. K., Glushonok, T. G., Maslovskaya, L. A., and Shadyro, O. I.: A 1h and 13c nmr and uv study of the state of hydroxyacetone in aqueous solutions, Russ. J. Gen. Chem., 73, 1027–1031, https://doi.org/10.1023/b:rugc.0000007604.91106.60, 2003.
Gubina, T. I., Pankratov, A. N., Labunskaya, V. I., and Rogacheva, S. M.: Self-oscillating reaction in the furan series, Chem. Heterocycl. Compd., 40, 1396–1401, https://doi.org/10.1007/s10593-005-0051-5, 2004.
Guthrie, J. P.: Hydration of thioesters. Evaluation of the free-energy changes for the addition of water to some thioesters, rate-equilibrium correlations over very wide ranges in equilibrium constants, and a new mechanistic criterion, J. Am. Chem. Soc., 100, 5892–5904, https://doi.org/10.1021/ja00486a048, 1978.
Guzmán, M. I., Colussi, A. J., and Hoffmann, M. R.: Photoinduced oligomerization of aqueous pyruvic acid, J. Phys. Chem. A, 110, 3619–3626, https://doi.org/10.1021/jp056097z, 2006.
Guzmán, M. I., Hoffmann, M. R., and Colussi, A. J.: Photolysis of pyruvic acid in ice: Possible relevance to co and CO2 ice core record anomalies, J. Geophys. Res., 112, D10123, https://doi.org/10.1029/2006jd007886, 2007.
Hammond, G. S., Borduin, W. G., and Guter, G. A.: Chelates of beta-diketones. I. Enolization, ionization and spectra, J. Am. Chem. Soc., 81, 4682–4686, https://doi.org/10.1021/ja01526a058, 1959.
Hilal, S. H., Bornander, L. L., and Carreira, L. A.: Hydration equilibrium constants of aldehydes, ketones and quinazolines, QSAR Com. Sci., 24, 631–638, https://doi.org/10.1002/qsar.200430913, 2005.
Hine, J. and Mookerjee, P. K.: Structural effects on rates and equilibriums. Xix. Intrinsic hydrophilic character of organic compounds. Correlations in terms of structural contributions, J. Org. Chem., 40, 292–298, https://doi.org/10.1021/jo00891a006, 1975.
Hobbs, P. V.: Aerosol-cloud-climate interactions, Academic Press, San Diego, CA, 98–105, 1993.
Hoover, W. G.: Canonical dynamics: Equilibrium phase-space distributions, Phys. Rev. A: At. Mol. Opt. Phys., 31, 1695–1697, 1985.
Horowitz, A., Meller, R., and Moortgat, G. K.: The uv-vis absorption cross sections of the alpha-dicarbonyl compounds: Pyruvic acid, biacetyl and glyoxal, J. Photochem. Photobiol., A, 146, 19–27, https://doi.org/10.1016/S1010-6030(01)00601-3, 2001.
Hummel, J. R. and Reck, R. A.: A global surface albedo model, J. Appl. Meteorol., 18, 239–253, 1979.
Ip, H. S. S., Huang, X. H. H., and Yu, J. Z.: Effective Henry's law constants of glyoxal, glyoxylic acid, and glycolic acid, Geophys. Res. Lett., 36, L01802, https://doi.org/10.1029/2008gl036212, 2009.
IUPAC, Data, C. O. E., Serjeant, E. P., and Dempsey, B.: Ionisation constants of organic acids in aqueous solution, Pergamon Press, 1979.
Jaoui, M., Corse, E., Kleindienst, T. E., Offenberg, J. H., Lewandowski, M., and Edney, E. O.: Analysis of secondary organic aerosol compounds from the photooxidation of d-limonene in the presence of NOx and their detection in ambient PM2.5, Environ. Sci. Tech., 40, 3819–3828, https://doi.org/10.1021/es052566z, 2006.
Jürgens, M., Jacob, F., Ekici, P., Friess, A., and Parlar, H.: Determination of direct photolysis rate constants and OH radical reactivity of representative odour compounds in brewery broth using a continuous flow-stirred photoreactor, Atmos. Environ., 41, 4571–4584, https://doi.org/10.1016/j.atmosenv.2007.03.053, 2007.
Karickoff, S. W., Carreira, L. A., and Hilal, S. H.: SPARC performs automated reasoning in chemistry, v4.6, 2011.
Klamt, A. and Schurmann, G.: Cosmo: A new approach to dielectric screening in solvents with explicit expressions for the screening energy and its gradient, J. Chem. Soc., Perkin Trans., 2, 799–805, 1993.
Kwok, E. S. C. and Atkinson, R.: Estimation of hydroxyl radical reaction rate constants for gas-phase organic compounds using a structure-reactivity relationship: An update, Atmos. Environ., 29, 1685–1695, 1995.
Larsen, M. C. and Vaida, V.: Near infrared photochemistry of pyruvic acid in aqueous solution, J. Phys. Chem. A, 116, 5840–5846, https://doi.org/10.1021/jp2087972, 2012.
Leermakers, P. A. and Vesley, G. F.: The photochemistry of alpha-keto acids and alpha-keto esters. I. Photolysis of pyruvic acid and benzoylformic acid, J. Am. Chem. Soc., 85, 3776–3779, https://doi.org/10.1021/ja00906a013, 1963.
Li, S.-M., Macdonald, A. M., Leithead, A., Leaitch, W. R., Gong, W., Anlauf, K. G., Toom-Sauntry, D., Hayden, K., Bottenheim, J., and Wang, D.: Investigation of carbonyls in cloudwater during ICARTT, J. Geophys. Res.-Atmos., 113, D17206, https://doi.org/10.1029/2007JD009364, 2008.
Lim, Y. B., Tan, Y., Perri, M. J., Seitzinger, S. P., and Turpin, B. J.: Aqueous chemistry and its role in secondary organic aerosol (SOA) formation, Atmos. Chem. Phys., 10, 10521–10539, https://doi.org/10.5194/acp-10-10521-2010, 2010.
Mackinney, G. and Temmer, O.: The deterioration of dried fruit. Iv. Spectrophotometric and polarographic studies, J. Am. Chem. Soc., 70, 3586–3590, https://doi.org/10.1021/ja01191a013, 1948.
Malik, M. and Joens, J. A.: Temperature dependent near-UV molar absorptivities of glyoxal and gluteraldehyde in aqueous solution, Spectrochim. Acta, Part A, 56, 2653–2658, 2000.
Martinez, A. M., Cushmac, G. E., and Rocek, J.: Chromic acid oxidation of cyclopropanols, J. Am. Chem. Soc., 97, 6502–6510, https://doi.org/10.1021/ja00855a036, 1975.
Mayer, B. and Madronich, S.: Actinic flux and photolysis in water droplets: Mie calculations and geometrical optics limit, Atmos. Chem. Phys., 4, 2241–2250, https://doi.org/10.5194/acp-4-2241-2004, 2004.
Meylan, W. M. and Howard, P. H.: Bond contribution method for estimating Henry's law constants, Environ. Toxicol. Chem., 10, 1283–1293, https://doi.org/10.1002/etc.5620101007, 1991.
Monod, A. and Doussin, J. F.: Structure-activity relationship for the estimation of OH-oxidation rate constants of aliphatic organic compounds in the aqueous phase: Alkanes, alcohols, organic acids and bases, Atmos. Environ., 42, 7611–7622, 2008.
Monod, A., Poulain, L., Grubert, S., Voisin, D., and Wortham, H.: Kinetics of OH-initiated oxidation of oxygenated organic compounds in the aqueous phase: New rate constants, structure activity relationships and atmospheric implications, Atmos. Environ., 39, 7667–7688, 2005.
Nissenson, P., Knox, C. J. H., Finlayson-Pitts, B. J., Phillips, L. F., and Dabdub, D.: Enhanced photolysis in aerosols: Evidence for important surface effects, Phys. Chem. Chem. Phys., 8, 4700–4710, https://doi.org/10.1039/B609219E, 2006.
Nissenson, P., Dabdub, D., Das, R., Maurino, V., Minero, C., and Vione, D.: Evidence of the water-cage effect on the photolysis of NO3- and FeOH2+. 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.
Nosé, S.: A molecular dynamics method for simulations in the canonical ensemble, Mol. Phys., 52, 255–268, https://doi.org/10.1080/00268978400101201, 1984.
Pavia, D. L.: Introduction to spectroscopy, Brooks/Cole, Belmont, CA, 390–411, 2009.
Perdew, J. P., Ernzerhof, M., and Burke, K.: Rationale for mixing exact exchange with density functional approximations, J. Chem. Phys., 105, 9982–9985, 1996a.
Perdew, J. P., Burke, K., and Ernzerhof, M.: Generalized gradient approximation made simple, Phys. Rev. Lett., 77, 3865–3868, 1996b.
Pocker, Y., Meany, J. E., Nist, B. J., and Zadorojny, C.: Reversible hydration of pyruvic acid. I. Equilibrium studies, J. Phys. Chem., 73, 2879–2882, https://doi.org/10.1021/j100843a015, 1969.
Raventos-Duran, T., Camredon, M., Valorso, R., Mouchel-Vallon, C., and Aumont, B.: Structure-activity relationships to estimate the effective Henry's law constants of organics of atmospheric interest, Atmos. Chem. Phys., 10, 7643–7654, https://doi.org/10.5194/acp-10-7643-2010, 2010.
Renard, P., Siekmann, F., Gandolfo, A., Socorro, J., Salque, G., Ravier, S., Quivet, E., Clément, J.-L., Traikia, M., Delort, A.-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.
Renzetti, N. A. and Doyle, D. J.: The chemical nature of the particulate in irradiated automobile exhaust, J. Air Pollut. Control Assoc., 8, 293–296, 1959.
Rice, F. O.: The effect of solvent on the ultra violet absorption spectrum of a pure substance, J. Am. Chem. Soc., 42, 727–735, https://doi.org/10.1021/ja01449a009, 1920.
Rogers, J. D.: Rate constant measurements for the reaction of the hydroxyl radical with cyclohexene, cyclopentene, and glutaraldehyde, Environ. Sci. Technol., 23, 177–181, 1989.
Röhrig, U. F., Frank, I., Hutter, J., Laio, A., VandeVondele, J., and Rothlisberger, U.: QM/MM car-parrinello molecular dynamics study of the solvent effects on the ground state and on the first excited singlet state of acetone in water, Chem. Phys. Chem., 4, 1177–1182, https://doi.org/10.1002/cphc.200300650, 2003.
Sander, R.: Compilation of Henry's law constants for inorganic and organic species of potential importance in environmental chemistry (version 3), http://www.henrys-law.org, (last access: 1 June 2013), 1999.
Sander, S. P., Abbatt, J., Barker, J. R., Burkholder, J. B., Friedl, R. R., Golden, D. M., Huie, R. E., Kolb, C. E., Kurylo, M. J., Moortgat, G. K., Orkin, V. L., and Wine, P. H.: Chemical kinetics and photochemical data for use in atmospheric studies: Evaluation number 17. JPL Publication 10-6, Jet Propulsion Laboratory, Pasadena, http://jpldataeval.jpl.nasa.gov 5 June 2013, 2011.
Saxena, P. and Hildemann, L. M.: Water-soluble organics in atmospheric particles: A critical review of the literature and application of thermodynamics to identify candidate compounds, J. Atmos. Chem., 24, 57–109, 1996.
Schaefer, T., Schindelka, J., Hoffmann, D., and Herrmann, H.: Laboratory kinetic and mechanistic studies on the OH-initiated oxidation of acetone in aqueous solution, J. Phys. Chem. A, 116, 6317–6326, https://doi.org/10.1021/jp2120753, 2012.
Schafer, A., Horn, H., and Ahlrichs, R.: Fully optimized contracted gaussian basis sets for atoms Li to Kr, J. Chem. Phys., 97, 2571–2577, 1992.
Schutze, M. and Herrmann, H.: Uptake of acetone, 2-butanone, 2,3-butanedione and 2-oxopropanal on a water surface, Phys. Chem. Chem. Phys., 6, 965–971, 2004.
Seinfeld, J. and Pandis, S.: Atmospheric chemistry and physics, John Wiley and Sons, Inc., New York, 1998.
Sham, Y. Y. and Joens, J. A.: Temperature dependent near uv molar absorptivities of several small aldehydes in aqueous solution, Spectrochim. Acta A, 51, 247–251, 1995.
Staffelbach, T. A., Orlando, J. J., Tyndall, G. S., and Calvert, J. G.: The uv-visible absorption spectrum and photolysis quantum yields of methylglyoxal, J. Geophys. Res. Atmos., 100, 14189–14198, https://doi.org/10.1029/95JD00541, 1995.
Staudinger, J. and Roberts, P. V.: A critical review of Henry's law constants for environmental applications, Crit. Rev. Environ. Sci. Technol., 26, 205–297, https://doi.org/10.1080/10643389609388492, 1996.
Steenken, S., Jaenicke-Zauner, W., and Schulte-Frohlinde, D.: Photofragmentation of hydroxyacetone, 1.3-dihydroxyacetone, and 1.3-dicarboxyacetone in aqueous solution. An EPR study, Photochem. Photobiol., 21, 21–26, https://doi.org/10.1111/j.1751-1097.1975.tb06624.x, 1975.
Sulpizi, M., Carloni, P., Hutter, J., and Rothlisberger, U.: A hybrid TDDFT/MM investigation of the optical properties of aminocoumarins in water and acetonitrile solution, Phys. Chem. Chem. Phys., 5, 4798–4805, https://doi.org/10.1039/B305846H, 2003.
Tan, Y., Lim, Y. B., Altieri, K. E., Seitzinger, S. P., and Turpin, B. J.: Mechanisms leading to oligomers and SOA through aqueous photooxidation: Insights from OH radical oxidation of acetic acid and methylglyoxal, Atmos. Chem. Phys., 12, 801–813, https://doi.org/10.5194/acp-12-801-2012, 2012.
Tapavicza, E., Meyer, A. M., and Furche, F.: Unravelling the details of vitamin d photosynthesis by non-adiabatic molecular dynamics simulations, Phys. Chem. Chem. Phys., 13, 20986–20998, https://doi.org/10.1039/C1CP21292C, 2011.
Tapavicza, E., Vincent, J. C., Bellchambers, G. D., and Furche, F.: Ab initio non-adiabatic molecular dynamics Phys. Chem. Chem. Phys., https://doi.org/10.1039/C3CP51514A, 2013.
Treutler, O. and Ahlrichs, R.: Efficient molecular numerical integration schemes, J. Chem. Phys., 102, 346–354, 1995.
Turýan, Y. I.: Kinetics and equilibrium of the dehydration-hydration and recombination dissociation reactions of glyoxylic acid investigated by electrochemical methods, Croat. Chem. Acta,, 71, 727–743, 1998.
van Pinxteren, D., Plewka, A., Hofmann, D., Müller, K., Kramberger, H., Svrcina, B., Bächmann, K., Jaeschke, W., Mertes, S., Collett Jr, J. L., and Herrmann, H.: Schmücke hill cap cloud and valley stations aerosol characterisation during FEBUKO (ii): Organic compounds, Atmos. Environ., 39, 4305–4320, https://doi.org/10.1016/j.atmosenv.2005.02.014, 2005.
Vione, D., Maurino, V., Minero, C., Pelizzetti, E., Harrison, M. A. J., Olariu, R.-I., and Arsene, C.: Photochemical reactions in the tropospheric aqueous phase and on particulate matter, Chem. Soc. Rev., 35, 441–453, https://doi.org/10.1039/b510796m, 2006.
Wallington, T. J., and Kurylo, M. J.: Flash photolysis resonance fluorescence investigation of the gas-phase reactions of OH radicals with a series of aliphatic ketones over the temperature range 240–440 k, J. Phys. Chem., 91, 1987.
Weigend, F. and Häser, M.: RI-MP2: First derivatives and global consistency, Theor. Chem. Acc., 97, 331–340, https://doi.org/10.1007/s002140050269, 1997.
Winkelman, J. G. M., Voorwinde, O. K., Ottens, M., Beenackers, A. A. C. M., and Janssen, L. P. B. M.: Kinetics and chemical equilibrium of the hydration of formaldehyde, Chem. Eng. Sci., 57, 4067–4076, 2002.
Xu, H., Wentworth, P. J., Howell, N. W., and Joens, J. A.: Temperature dependent near-uv molar absorptivities of aliphatic aldehydes and ketones in aqueous solution, Spectrochim. Acta A, 49, 1171–1178, 1993.
Zhou, S. M., Barnes, I., Zhu, T., Bejan, I., Albu, M., and Benter, T.: Atmospheric chemistry of acetylacetone, Environ. Sci. Technol., 42, 7905–7910, 2008.
Zhou, X. and Mopper, K.: Apparent partition coefficients of 15 carbonyl compounds between air and seawater and between air and freshwater; implications for air-sea exchange, Environ. Sci. Tech., 24, 1864–1869, https://doi.org/10.1021/es00082a013, 1990.
Altmetrics
Final-revised paper
Preprint