Articles | Volume 16, issue 6
https://doi.org/10.5194/acp-16-3727-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Special issue:
https://doi.org/10.5194/acp-16-3727-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
21 Mar 2016
Research article |
| 21 Mar 2016
Simulating the formation of carbonaceous aerosol in a European Megacity (Paris) during the MEGAPOLI summer and winter campaigns
Christos Fountoukis
Institute of Chemical Engineering Sciences, Foundation for Research and
Technology Hellas (FORTH), 26504 Patras, Greece
Athanasios G. Megaritis
Department of Chemical Engineering, University of Patras, 26500 Patras,
Greece
Ksakousti Skyllakou
Department of Chemical Engineering, University of Patras, 26500 Patras,
Greece
Panagiotis E. Charalampidis
Institute of Chemical Engineering Sciences, Foundation for Research and
Technology Hellas (FORTH), 26504 Patras, Greece
Department of Environment, University of the Aegean, 81100 Mytilene,
Greece
Hugo A. C. Denier van der Gon
TNO Climate, Air and Sustainability, P.O. Box 80015, 3508 TA Utrecht, the
Netherlands
Monica Crippa
European Commission, Joint Research Centre (JRC), Institute for Environment
and Sustainability (IES), Air and Climate Unit, Via Fermi, 2749, 21027 Ispra, Italy
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI
Villigen, Switzerland
André S. H. Prévôt
Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, PSI
Villigen, Switzerland
Friederike Fachinger
Max Planck Institute for Chemistry, Particle Chemistry Department,
Mainz, Germany
Alfred Wiedensohler
Leibniz Institute for Tropospheric Research, Leipzig, Germany
Christodoulos Pilinis
Department of Environment, University of the Aegean, 81100 Mytilene,
Greece
Spyros N. Pandis
CORRESPONDING AUTHOR
Institute of Chemical Engineering Sciences, Foundation for Research and
Technology Hellas (FORTH), 26504 Patras, Greece
Department of Chemical Engineering, University of Patras, 26500 Patras,
Greece
Department of Chemical Engineering, Carnegie Mellon University,
Pittsburgh, Pennsylvania, USA
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CoCO2-MOSAIC 1.0 is a global mosaic of regional bottom-up inventories providing gridded (0.1˚×0.1˚) monthly CO2 emissions fluxes. Regional datasets include country-specific information and finer spatial resolution than global inventories. Therefore, CoCO2-MOSAIC can be considered as a regionally accepted reference to assess the quality of global emission inventories and to evaluate the sensitivity of inverse models to the bottom-up emissions used as priors.
Samira Atabakhsh, Laurent Poulain, Gang Chen, Francesco Canonaco, André S. H. Prévôt, Mira Pöhlker, Alfred Wiedensohler, and Hartmut Herrmann
Atmos. Chem. Phys., 23, 6963–6988, https://doi.org/10.5194/acp-23-6963-2023, https://doi.org/10.5194/acp-23-6963-2023, 2023
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The study focuses on the aerosol chemical variations found in the rural-background station of Melpitz based on ACSM and MAAP measurements. Source apportionment on both organic aerosol (OA) and black carbon (eBC) was performed, and source seasonality was also linked to air mass trajectories. Overall, three anthropogenic sources were identified in OA and eBC plus two additional aged OA. Our results demonstrate the influence of transported coal-combustion-related OA even during summer time.
Andreas Forstmaier, Jia Chen, Florian Dietrich, Juan Bettinelli, Hossein Maazallahi, Carsten Schneider, Dominik Winkler, Xinxu Zhao, Taylor Jones, Carina van der Veen, Norman Wildmann, Moritz Makowski, Aydin Uzun, Friedrich Klappenbach, Hugo Denier van der Gon, Stefan Schwietzke, and Thomas Röckmann
Atmos. Chem. Phys., 23, 6897–6922, https://doi.org/10.5194/acp-23-6897-2023, https://doi.org/10.5194/acp-23-6897-2023, 2023
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Large cities emit greenhouse gases which contribute to global warming. In this study, we measured the release of one important green house gas, methane, in Hamburg. Multiple sources that contribute to methane emissions were located and quantified. Methane sources were found to be mainly caused by human activity (e.g., by release from oil and gas refineries). Moreover, potential natural sources have been located, such as the Elbe River and lakes.
Fabian Manuel Maier, Ingeborg Levin, Sébastien Conil, Maksym Gachkivskyi, Hugo Denier van der Gon, and Samuel Hammer
EGUsphere, https://doi.org/10.5194/egusphere-2023-1237, https://doi.org/10.5194/egusphere-2023-1237, 2023
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We assess the uncertainty of continuous fossil fuel carbon dioxide (ffCO2) estimates derived from carbon monoxide (CO) observations and radiocarbon (14CO2) flask measurements from an urban and a rural site. This study provides the basis for using continuous CO-based ffCO2 observations in atmospheric transport inversion frameworks to derive ffCO2 emissions estimates. We also compare the flask-based CO / ffCO2 ratios with modelled ratios to validate an emission inventory for Central Europe.
Christina N. Vasilakopoulou, Kalliopi Florou, Christos Kaltsonoudis, Iasonas Stavroulas, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Meas. Tech., 16, 2837–2850, https://doi.org/10.5194/amt-16-2837-2023, https://doi.org/10.5194/amt-16-2837-2023, 2023
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The offline aerosol mass spectrometry technique is a useful tool for the source apportionment of organic aerosol in areas and periods during which an aerosol mass spectrometer is not available. In this work, an improved offline technique was developed and evaluated in an effort to capture most of the partially soluble and insoluble organic aerosol material, reducing the uncertainty of the corresponding source apportionment significantly.
Jun Zhang, Kun Li, Tiantian Wang, Erlend Gammelsæter, Ka Yuen Cheung, Mihnea Surdu, Sophie Bogler, Deepika Bhattu, Dongyu S. Wang, Tianqu Cui, Lu Qi, Houssni Lamkaddam, Imad El Haddad, Jay G. Slowik, Andre S. H. Prevot, and David M. Bell
EGUsphere, https://doi.org/10.5194/egusphere-2023-1102, https://doi.org/10.5194/egusphere-2023-1102, 2023
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We conducted burning experiments to simulate various types of solid fuel combustion, including residential burning, wildfires, agricultural burning, cow dung, and plastic bags burning. The chemical composition of the particles was characterized using mass spectrometers, and new potential markers for different fuels were identified using statistical analysis. This work improves our understanding of emissions from solid fuel burning and offers support for refined source apportionment.
Marc Guevara, Santiago Enciso, Carles Tena, Oriol Jorba, Stijn Dellaert, Hugo Denier van der Gon, and Carlos Pérez García-Pando
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2023-95, https://doi.org/10.5194/essd-2023-95, 2023
Preprint under review for ESSD
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A global dataset of emissions from thermal power plants was created for the year 2018. The resulting catalogue reports annual emissions of CO2 and co-emitted species (NOx, CO, SO2 and CH4) for more than 16000 individual facilities at their exact geographical location. Information on the temporal and vertical distribution of the emissions is also provided at the facility level. The dataset is intended to support current and future satellite emission monitoring and inverse modelling efforts.
Ana Maria Roxana Petrescu, Chunjing Qiu, Matthew J. McGrath, Philippe Peylin, Glen P. Peters, Philippe Ciais, Rona L. Thompson, Aki Tsuruta, Dominik Brunner, Matthias Kuhnert, Bradley Matthews, Paul I. Palmer, Oksana Tarasova, Pierre Regnier, Ronny Lauerwald, David Bastviken, Lena Höglund-Isaksson, Wilfried Winiwarter, Giuseppe Etiope, Tuula Aalto, Gianpaolo Balsamo, Vladislav Bastrikov, Antoine Berchet, Patrick Brockmann, Giancarlo Ciotoli, Giulia Conchedda, Monica Crippa, Frank Dentener, Christine D. Groot Zwaaftink, Diego Guizzardi, Dirk Günther, Jean-Matthieu Haussaire, Sander Houweling, Greet Janssens-Maenhout, Massaer Kouyate, Adrian Leip, Antti Leppänen, Emanuele Lugato, Manon Maisonnier, Alistair J. Manning, Tiina Markkanen, Joe McNorton, Marilena Muntean, Gabriel D. Oreggioni, Prabir K. Patra, Lucia Perugini, Isabelle Pison, Maarit T. Raivonen, Marielle Saunois, Arjo J. Segers, Pete Smith, Efisio Solazzo, Hanqin Tian, Francesco N. Tubiello, Timo Vesala, Guido R. van der Werf, Chris Wilson, and Sönke Zaehle
Earth Syst. Sci. Data, 15, 1197–1268, https://doi.org/10.5194/essd-15-1197-2023, https://doi.org/10.5194/essd-15-1197-2023, 2023
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This study updates the state-of-the-art scientific overview of CH4 and N2O emissions in the EU27 and UK in Petrescu et al. (2021a). Yearly updates are needed to improve the different respective approaches and to inform on the development of formal verification systems. It integrates the most recent emission inventories, process-based model and regional/global inversions, comparing them with UNFCCC national GHG inventories, in support to policy to facilitate real-time verification procedures.
Vaishali Jain, Nidhi Tripathi, Sachchida N. Tripathi, Mansi Gupta, Lokesh K. Sahu, Vishnu Murari, Sreenivas Gaddamidi, Ashutosh K. Shukla, and Andre S. H. Prevot
Atmos. Chem. Phys., 23, 3383–3408, https://doi.org/10.5194/acp-23-3383-2023, https://doi.org/10.5194/acp-23-3383-2023, 2023
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This research chemically characterises 173 different NMVOCs (non-methane volatile organic compounds) measured in real time for three seasons in the city of the central Indo-Gangetic basin of India, Lucknow. Receptor modelling is used to analyse probable sources of NMVOCs and their crucial role in forming ozone and secondary organic aerosols. It is observed that vehicular emissions and solid fuel combustion are the highest contributors to the emission of primary and secondary NMVOCs.
Matthew Joseph McGrath, Ana Maria Roxana Petrescu, Philippe Peylin, Robbie M. Andrew, Bradley Matthews, Frank Dentener, Juraj Balkovič, Vladislav Bastrikov, Meike Becker, Gregoire Broquet, Philippe Ciais, Audrey Fortems, Raphael Ganzenmüller, Giacomo Grassi, Ian Harris, Matthew Jones, Juergen Knauer, Matthias Kuhnert, Guillaume Monteil, Saqr Munassar, Paul I. Palmer, Glen P. Peters, Chunjing Qiu, Mart-Jan Schelhaas, Oksana Tarasova, Matteo Vizzarri, Karina Winkler, Gianpaolo Balsamo, Antoine Berchet, Peter Briggs, Patrick Brockmann, Frédéric Chevallier, Giulia Conchedda, Monica Crippa, Stijn Dellaert, Hugo A. C. Denier van der Gon, Sara Filipek, Pierre Friedlingstein, Richard Fuchs, Michael Gauss, Christoph Gerbig, Diego Guizzardi, Dirk Günther, Richard A. Houghton, Greet Janssens-Maenhout, Ronny Lauerwald, Bas Lerink, Ingrid T. Luijkx, Géraud Moulas, Marilena Muntean, Gert-Jan Nabuurs, Aurélie Paquirissamy, Lucia Perugini, Wouter Peters, Roberto Pilli, Julia Pongratz, Pierre Regnier, Marko Scholze, Yusuf Serengil, Pete Smith, Efisio Solazzo, Rona L. Thompson, Francesco N. Tubiello, Timo Vesala, and Sophia Walther
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2022-412, https://doi.org/10.5194/essd-2022-412, 2023
Revised manuscript accepted for ESSD
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Accurate estimation of fluxes of carbon dioxide from the land surface is essential to understanding future impacts of greenhouse gas emissions on the climate system. A wide variety of methods currently exist to estimate these sources and sinks. We are continuing work to develop annual comparisons of these diverse methods in order to clarify what they all actually calculate and resolve apparent disagreement, in addition to highlighting opportunities for increased understanding.
Tingting Feng, Yingkun Wang, Weiwei Hu, Ming Zhu, Wei Song, Wei Chen, Yanyan Sang, Zheng Fang, Wei Deng, Hua Fang, Xu Yu, Cheng Wu, Bin Yuan, Shan Huang, Min Shao, Xiaofeng Huang, Lingyan He, Young Ro Lee, Lewis Gregory Huey, Francesco Canonaco, Andre S. H. Prevot, and Xinming Wang
Atmos. Chem. Phys., 23, 611–636, https://doi.org/10.5194/acp-23-611-2023, https://doi.org/10.5194/acp-23-611-2023, 2023
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To investigate the impact of aging processes on organic aerosols (OA), we conducted a comprehensive field study at a continental remote site using an on-line mass spectrometer. The results show that OA in the Chinese outflows were strongly influenced by upwind anthropogenic emissions. The aging processes can significantly decrease the OA volatility and result in a varied viscosity of OA under different circumstances, signifying the complex physiochemical properties of OA in aged plumes.
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
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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.
Spiro D. Jorga, Kalliopi Florou, David Patoulias, and Spyros N. Pandis
Atmos. Chem. Phys., 23, 85–97, https://doi.org/10.5194/acp-23-85-2023, https://doi.org/10.5194/acp-23-85-2023, 2023
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We take advantage of this unexpected low, new particle formation frequency in Greece and use a dual atmospheric simulation chamber system with starting point ambient air in an effort to gain insight about the chemical species that is limiting nucleation in this area. A potential nucleation precursor, ammonia, was added in one of the chambers while the other one was used as a reference. The addition of ammonia assisted new particle formation in almost 50 % of the experiments conducted.
Srijana Lama, Sander Houweling, K. Folkert Boersma, Ilse Aben, Hugo A. C. Denier van der Gon, and Maarten C. Krol
Atmos. Chem. Phys., 22, 16053–16071, https://doi.org/10.5194/acp-22-16053-2022, https://doi.org/10.5194/acp-22-16053-2022, 2022
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Hydroxyl radical (OH) is the important chemical species that determines the lifetime of some greenhouse gases and trace gases. OH plays a vital role in air pollution chemistry. OH has a short lifetime and is extremely difficult to measure directly. OH concentrations derived from the chemistry transport model (CTM) have uncertainties of >50 %. Therefore, in this study, OH is derived indirectly using satellite date in urban plumes.
Yandong Tong, Lu Qi, Giulia Stefenelli, Dongyu Simon Wang, Francesco Canonaco, Urs Baltensperger, André Stephan Henry Prévôt, and Jay Gates Slowik
Atmos. Meas. Tech., 15, 7265–7291, https://doi.org/10.5194/amt-15-7265-2022, https://doi.org/10.5194/amt-15-7265-2022, 2022
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We present a method for positive matrix factorisation (PMF) analysis on a single dataset that includes measurements from both EESI-TOF and AMS in Zurich, Switzerland. For the first time, we resolved and quantified secondary organic aerosol (SOA) sources. Meanwhile, we also determined the retrieved EESI-TOF factor-dependent sensitivities. This method provides a framework for exploiting semi-quantitative, high-resolution instrumentation for quantitative source apportionment.
Brian T. Dinkelacker, Pablo Garcia Rivera, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Geosci. Model Dev., 15, 8899–8912, https://doi.org/10.5194/gmd-15-8899-2022, https://doi.org/10.5194/gmd-15-8899-2022, 2022
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The performance of a chemical transport model in reproducing PM2.5 concentrations and composition was evaluated at the finest scale using measurements from regulatory sites as well as a network of low-cost monitors. Total PM2.5 mass is reproduced well by the model during the winter when compared to regulatory measurements, but in the summer PM2.5 is underpredicted, mainly due to difficulties in reproducing regional secondary organic aerosol levels.
Christina Vasilakopoulou, Iasonas Stavroulas, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Meas. Tech., 15, 6419–6431, https://doi.org/10.5194/amt-15-6419-2022, https://doi.org/10.5194/amt-15-6419-2022, 2022
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Offline aerosol mass spectrometer (AMS) measurements can provide valuable information about ambient organic aerosols when online AMS measurements are not available. In this study, we examine whether and how the low time resolution (usually 24 h) of the offline technique affects source apportionment results. We concluded that use of the daily averages resulted in estimated average contributions that were within 8 % of the total OA compared with the high-resolution analysis.
Stella E. I. Manavi and Spyros N. Pandis
Geosci. Model Dev., 15, 7731–7749, https://doi.org/10.5194/gmd-15-7731-2022, https://doi.org/10.5194/gmd-15-7731-2022, 2022
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The paper describes the first step towards the development of a simulation framework for the chemistry and secondary organic aerosol production of intermediate-volatility organic compounds (IVOCs). These compounds can be a significant source of organic particulate matter. Our approach treats IVOCs as lumped compounds that retain their chemical characteristics. Estimated IVOC emissions from road transport were a factor of 8 higher than emissions used in previous applications.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, Thomas J. Bannan, Michael Flynn, Spyros N. Pandis, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 13677–13693, https://doi.org/10.5194/acp-22-13677-2022, https://doi.org/10.5194/acp-22-13677-2022, 2022
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The addition of a low-yield precursor to the reactive mixture of aVOC and bVOC can increase or decrease the SOA volatility that is system-dependent. Therefore, the SOA volatility of the mixtures cannot always be predicted based on the additivity. In complex mixtures the formation of lower-volatility products likely outweighs the formation of products with higher volatility. The unique products of each mixture contribute significantly to the signal, suggesting interactions can be important.
David M. Bell, Cheng Wu, Amelie Bertrand, Emelie Graham, Janne Schoonbaert, Stamatios Giannoukos, Urs Baltensperger, Andre S. H. Prevot, Ilona Riipinen, Imad El Haddad, and Claudia Mohr
Atmos. Chem. Phys., 22, 13167–13182, https://doi.org/10.5194/acp-22-13167-2022, https://doi.org/10.5194/acp-22-13167-2022, 2022
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A series of studies designed to investigate the evolution of organic aerosol were performed in an atmospheric simulation chamber, using a common oxidant found at night (NO3). The chemical composition steadily changed from its initial composition via different chemical reactions that were taking place inside of the aerosol particle. These results show that the composition of organic aerosol steadily changes during its lifetime in the atmosphere.
Marta Via, Gang Chen, Francesco Canonaco, Kaspar R. Daellenbach, Benjamin Chazeau, Hasna Chebaicheb, Jianhui Jiang, Hannes Keernik, Chunshui Lin, Nicolas Marchand, Cristina Marin, Colin O'Dowd, Jurgita Ovadnevaite, Jean-Eudes Petit, Michael Pikridas, Véronique Riffault, Jean Sciare, Jay G. Slowik, Leïla Simon, Jeni Vasilescu, Yunjiang Zhang, Olivier Favez, André S. H. Prévôt, Andrés Alastuey, and María Cruz Minguillón
Atmos. Meas. Tech., 15, 5479–5495, https://doi.org/10.5194/amt-15-5479-2022, https://doi.org/10.5194/amt-15-5479-2022, 2022
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This work presents the differences resulting from two techniques (rolling and seasonal) of the positive matrix factorisation model that can be run for organic aerosol source apportionment. The current state of the art suggests that the rolling technique is more accurate, but no proof of its effectiveness has been provided yet. This paper tackles this issue in the context of a synthetic dataset and a multi-site real-world comparison.
Brian T. Dinkelacker, Pablo Garcia Rivera, Ksakousti Skyllakou, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-648, https://doi.org/10.5194/acp-2022-648, 2022
Revised manuscript not accepted
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A number of factors have influenced the biogenic secondary organic aerosol (SOA) levels in the southeastern US from 2001 to 2010. The increases in temperature have led to an increase of the emissions of biogenic volatile organic compounds by trees and a corresponding increase of the SOA. However, this increase has been balanced by the reductions in the anthropogenic emissions of organic gases and particulate matter as well as of the oxides of nitrogen keeping the biogenic SOA roughly constant.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Josef Dommen, Mao Xiao, Xueqin Zhou, Andrea Baccarini, Stamatios Giannoukos, Günther Wehrle, Pascal André Schneider, Andre S. H. Prevot, Jay G. Slowik, Houssni Lamkaddam, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 15, 3747–3760, https://doi.org/10.5194/amt-15-3747-2022, https://doi.org/10.5194/amt-15-3747-2022, 2022
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Real-time detection of both the gas and particle phase is needed to elucidate the sources and chemical reaction pathways of organic vapors and particulate matter. The Dual-EESI was developed to measure gas- and particle-phase species to provide new insights into aerosol sources or formation mechanisms. After characterizing the relative gas and particle response factors of EESI via organic aerosol uptake experiments, the Dual-EESI is more sensitive toward gas-phase analyes.
Varun Kumar, Stamatios Giannoukos, Sophie L. Haslett, Yandong Tong, Atinderpal Singh, Amelie Bertrand, Chuan Ping Lee, Dongyu S. Wang, Deepika Bhattu, Giulia Stefenelli, Jay S. Dave, Joseph V. Puthussery, Lu Qi, Pawan Vats, Pragati Rai, Roberto Casotto, Rangu Satish, Suneeti Mishra, Veronika Pospisilova, Claudia Mohr, David M. Bell, Dilip Ganguly, Vishal Verma, Neeraj Rastogi, Urs Baltensperger, Sachchida N. Tripathi, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 22, 7739–7761, https://doi.org/10.5194/acp-22-7739-2022, https://doi.org/10.5194/acp-22-7739-2022, 2022
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Here we present source apportionment results from the first field deployment in Delhi of an extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF). The EESI-TOF is a recently developed instrument capable of providing uniquely detailed online chemical characterization of organic aerosol (OA), in particular the secondary OA (SOA) fraction. Here, we are able to apportion not only primary OA but also SOA to specific sources, which is performed for the first time in Delhi.
Marc Guevara, Hervé Petetin, Oriol Jorba, Hugo Denier van der Gon, Jeroen Kuenen, Ingrid Super, Jukka-Pekka Jalkanen, Elisa Majamäki, Lasse Johansson, Vincent-Henri Peuch, and Carlos Pérez García-Pando
Earth Syst. Sci. Data, 14, 2521–2552, https://doi.org/10.5194/essd-14-2521-2022, https://doi.org/10.5194/essd-14-2521-2022, 2022
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To control the spread of the COVID-19 disease, European governments implemented mobility restriction measures that resulted in an unprecedented drop in anthropogenic emissions. This work presents a dataset of emission adjustment factors that allows quantifying changes in 2020 European primary emissions per country and pollutant sector at the daily scale. The resulting dataset can be used as input in modelling studies aiming at quantifying the impact of COVID-19 on air quality levels.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Meas. Tech., 15, 2857–2874, https://doi.org/10.5194/amt-15-2857-2022, https://doi.org/10.5194/amt-15-2857-2022, 2022
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While the aerosol mass spectrometer provides high-time-resolution characterization of the overall extent of oxidation, the extensive fragmentation of molecules and specificity of the technique have posed challenges toward deeper understanding of molecular structures in aerosols. This work demonstrates how functional group information can be extracted from a suite of commonly measured mass fragments using collocated infrared spectroscopy measurements.
Hossein Maazallahi, Antonio Delre, Charlotte Scheutz, Anders M. Fredenslund, Stefan Schwietzke, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2022-134, https://doi.org/10.5194/amt-2022-134, 2022
Revised manuscript accepted for AMT
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Measurement methods are increasingly deployed to verify reported methane emissions of gas leaks. This study describes unique advantages and limitations of three methods. Two methods are rapidly deployed, but uncertainties and biases exist for some leak locations. In contrast, the suction method could accurately determine leak rates in principle. However, this method, which provides data for the German emission inventory, creates an overall low-bias in our study due to non-random site selection.
Andrea Pozzer, Simon F. Reifenberg, Vinod Kumar, Bruno Franco, Matthias Kohl, Domenico Taraborrelli, Sergey Gromov, Sebastian Ehrhart, Patrick Jöckel, Rolf Sander, Veronica Fall, Simon Rosanka, Vlassis Karydis, Dimitris Akritidis, Tamara Emmerichs, Monica Crippa, Diego Guizzardi, Johannes W. Kaiser, Lieven Clarisse, Astrid Kiendler-Scharr, Holger Tost, and Alexandra Tsimpidi
Geosci. Model Dev., 15, 2673–2710, https://doi.org/10.5194/gmd-15-2673-2022, https://doi.org/10.5194/gmd-15-2673-2022, 2022
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A newly developed setup of the chemistry general circulation model EMAC (ECHAM5/MESSy for Atmospheric Chemistry) is evaluated here. A comprehensive organic degradation mechanism is used and coupled with a volatility base model.
The results show that the model reproduces most of the tracers and aerosols satisfactorily but shows discrepancies for oxygenated organic gases. It is also shown that this model configuration can be used for further research in atmospheric chemistry.
Pablo Garcia Rivera, Brian T. Dinkelacker, Ioannis Kioutsioukis, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 22, 2011–2027, https://doi.org/10.5194/acp-22-2011-2022, https://doi.org/10.5194/acp-22-2011-2022, 2022
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The contribution of various pollution sources to the variability of fine PM in an urban area was examined using as an example the city of Pittsburgh. Biomass burning aerosol shows the largest variability during the winter with local maxima within the city and in the suburbs. During both periods the largest contributing source to the average PM2.5 is particles from outside the modeling domain. The average population-weighted PM2.5 concentration does not change significantly with resolution.
Jeroen Kuenen, Stijn Dellaert, Antoon Visschedijk, Jukka-Pekka Jalkanen, Ingrid Super, and Hugo Denier van der Gon
Earth Syst. Sci. Data, 14, 491–515, https://doi.org/10.5194/essd-14-491-2022, https://doi.org/10.5194/essd-14-491-2022, 2022
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This paper presents an 18-year time series for anthropogenic emissions for the main air pollutants in Europe, distinguishing 15 main source categories. It provides a complete overview of emissions to air and is designed to support air quality modelling. The data build where possible on official country total emissions used in the policy processes, but where necessary alternative data were used. The emission data are spatially distributed at high resolution (~ 6 km x 6 km) in a consistent way.
David Patoulias and Spyros N. Pandis
Atmos. Chem. Phys., 22, 1689–1706, https://doi.org/10.5194/acp-22-1689-2022, https://doi.org/10.5194/acp-22-1689-2022, 2022
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Our simulations indicate that the recently identified production and subsequent condensation effect of extremely low-volatility organic compounds have a smaller-than-expected effect on the total concentration of atmospheric particles. On the other hand, the oxidation of intermediate-volatility organic compounds leads to decreases in the ultrafine-particle concentrations. These results improve our understanding of the links between secondary organic aerosol formation and ultrafine particles.
Nicolás Álamos, Nicolás Huneeus, Mariel Opazo, Mauricio Osses, Sebastián Puja, Nicolás Pantoja, Hugo Denier van der Gon, Alejandra Schueftan, René Reyes, and Rubén Calvo
Earth Syst. Sci. Data, 14, 361–379, https://doi.org/10.5194/essd-14-361-2022, https://doi.org/10.5194/essd-14-361-2022, 2022
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This study presents the first high-resolution national inventory of anthropogenic emissions for Chile (Inventario Nacional de Emisiones Antropogénicas, INEMA). Emissions for vehicular, industrial, energy, mining and residential sectors are estimated for the period 2015–2017 and spatially distributed onto a high-resolution grid (1 × 1 km). This inventory will support policies seeking to mitigate climate change and improve air quality by providing qualified scientific spatial emission information.
Miska Olin, David Patoulias, Heino Kuuluvainen, Jarkko V. Niemi, Topi Rönkkö, Spyros N. Pandis, Ilona Riipinen, and Miikka Dal Maso
Atmos. Chem. Phys., 22, 1131–1148, https://doi.org/10.5194/acp-22-1131-2022, https://doi.org/10.5194/acp-22-1131-2022, 2022
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An emission factor particle size distribution was determined from the measurements at an urban traffic site. It was used in updating a pre-existing emission inventory, and regional modeling was performed after the update. Emission inventories typically underestimate nanoparticle emissions due to challenges in determining them with high certainty. This update reveals that the simulated aerosol levels have previously been underestimated especially for urban areas and for sub-50 nm particles.
Ksakousti Skyllakou, Pablo Garcia Rivera, Brian Dinkelacker, Eleni Karnezi, Ioannis Kioutsioukis, Carlos Hernandez, Peter J. Adams, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 17115–17132, https://doi.org/10.5194/acp-21-17115-2021, https://doi.org/10.5194/acp-21-17115-2021, 2021
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Significant reductions in pollutant emissions took place in the US from 1990 to 2010. The reductions in sulfur dioxide emissions from electric-generating units have dominated the reductions in fine particle mass. The reductions in transportation emissions have led to a 30 % reduction of elemental concentrations and of organic particulate matter by a factor of 3. On the other hand, changes in biomass burning and biogenic secondary organic aerosol have been modest.
Margarita Choulga, Greet Janssens-Maenhout, Ingrid Super, Efisio Solazzo, Anna Agusti-Panareda, Gianpaolo Balsamo, Nicolas Bousserez, Monica Crippa, Hugo Denier van der Gon, Richard Engelen, Diego Guizzardi, Jeroen Kuenen, Joe McNorton, Gabriel Oreggioni, and Antoon Visschedijk
Earth Syst. Sci. Data, 13, 5311–5335, https://doi.org/10.5194/essd-13-5311-2021, https://doi.org/10.5194/essd-13-5311-2021, 2021
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People worry that growing man-made carbon dioxide (CO2) concentrations lead to climate change. Global models, use of observations, and datasets can help us better understand behaviour of CO2. Here a tool to compute uncertainty in man-made CO2 sources per country per year and month is presented. An example of all sources separated into seven groups (intensive and average energy, industry, humans, ground and air transport, others) is presented. Results will be used to predict CO2 concentrations.
Jan C. Minx, William F. Lamb, Robbie M. Andrew, Josep G. Canadell, Monica Crippa, Niklas Döbbeling, Piers M. Forster, Diego Guizzardi, Jos Olivier, Glen P. Peters, Julia Pongratz, Andy Reisinger, Matthew Rigby, Marielle Saunois, Steven J. Smith, Efisio Solazzo, and Hanqin Tian
Earth Syst. Sci. Data, 13, 5213–5252, https://doi.org/10.5194/essd-13-5213-2021, https://doi.org/10.5194/essd-13-5213-2021, 2021
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We provide a synthetic dataset on anthropogenic greenhouse gas (GHG) emissions for 1970–2018 with a fast-track extension to 2019. We show that GHG emissions continued to rise across all gases and sectors. Annual average GHG emissions growth slowed, but absolute decadal increases have never been higher in human history. We identify a number of data gaps and data quality issues in global inventories and highlight their importance for monitoring progress towards international climate goals.
Dongyu S. Wang, Chuan Ping Lee, Jordan E. Krechmer, Francesca Majluf, Yandong Tong, Manjula R. Canagaratna, Julia Schmale, André S. H. Prévôt, Urs Baltensperger, Josef Dommen, Imad El Haddad, Jay G. Slowik, and David M. Bell
Atmos. Meas. Tech., 14, 6955–6972, https://doi.org/10.5194/amt-14-6955-2021, https://doi.org/10.5194/amt-14-6955-2021, 2021
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To understand the sources and fate of particulate matter in the atmosphere, the ability to quantitatively describe its chemical composition is essential. In this work, we developed a calibration method for a state-of-the-art measurement technique without the need for chemical standards. Statistical analyses identified the driving factors behind instrument sensitivity variability towards individual components of particulate matter.
Spiro D. Jorga, Kalliopi Florou, Christos Kaltsonoudis, John K. Kodros, Christina Vasilakopoulou, Manuela Cirtog, Axel Fouqueau, Bénédicte Picquet-Varrault, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 15337–15349, https://doi.org/10.5194/acp-21-15337-2021, https://doi.org/10.5194/acp-21-15337-2021, 2021
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We test the hypothesis that significant secondary organic aerosol production can take place even during winter nights through the oxidation of the emitted organic vapors by the nitrate radicals produced during the reaction of ozone and nitrogen oxides. Our experiments, using as a starting point the ambient air of an urban area with high biomass burning activity, demonstrate that, even with sunlight, there is 20 %–70 % additional organic aerosol formed in a few hours.
Gang Chen, Yulia Sosedova, Francesco Canonaco, Roman Fröhlich, Anna Tobler, Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Christoph Hueglin, Peter Graf, Urs Baltensperger, Jay G. Slowik, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 15081–15101, https://doi.org/10.5194/acp-21-15081-2021, https://doi.org/10.5194/acp-21-15081-2021, 2021
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A novel, advanced source apportionment technique was applied to a dataset measured in Magadino. Rolling positive matrix factorisation (PMF) allows for retrieving more realistic, time-dependent, and detailed information on organic aerosol sources. The strength of the rolling PMF mechanism is highlighted by comparing it with results derived from conventional seasonal PMF. Overall, this comprehensive interpretation of aerosol chemical speciation monitor data could be a role model for similar work.
Wenfei Zhu, Song Guo, Zirui Zhang, Hui Wang, Ying Yu, Zheng Chen, Ruizhe Shen, Rui Tan, Kai Song, Kefan Liu, Rongzhi Tang, Yi Liu, Shengrong Lou, Yuanju Li, Wenbin Zhang, Zhou Zhang, Shijin Shuai, Hongming Xu, Shuangde Li, Yunfa Chen, Min Hu, Francesco Canonaco, and Andre S. H. Prévôt
Atmos. Chem. Phys., 21, 15065–15079, https://doi.org/10.5194/acp-21-15065-2021, https://doi.org/10.5194/acp-21-15065-2021, 2021
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The experiments of primary emissions and secondary organic aerosol (SOA) formation from urban lifestyle sources (cooking and vehicles) were conducted. The mass spectral features of primary organic aerosol (POA) and SOA were characterized by using a high-resolution time-of-flight aerosol mass spectrometer. This work, for the first time, establishes the vehicle and cooking SOA source profiles and can be further used as source constraints in the OA source apportionment in the ambient atmosphere.
Anna K. Tobler, Alicja Skiba, Francesco Canonaco, Griša Močnik, Pragati Rai, Gang Chen, Jakub Bartyzel, Miroslaw Zimnoch, Katarzyna Styszko, Jaroslaw Nęcki, Markus Furger, Kazimierz Różański, Urs Baltensperger, Jay G. Slowik, and Andre S. H. Prevot
Atmos. Chem. Phys., 21, 14893–14906, https://doi.org/10.5194/acp-21-14893-2021, https://doi.org/10.5194/acp-21-14893-2021, 2021
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Kraków is among the cities with the highest particulate matter levels within Europe. We conducted long-term and highly time-resolved measurements of the chemical composition of submicron particlulate matter (PM1). Combined with advanced source apportionment techniques, which allow for time-dependent factor profiles, our results elucidate that traffic and residential heating (biomass burning and coal combustion) as well as oxygenated organic aerosol are the key PM sources in Kraków.
Cheng Wu, David M. Bell, Emelie L. Graham, Sophie Haslett, Ilona Riipinen, Urs Baltensperger, Amelie Bertrand, Stamatios Giannoukos, Janne Schoonbaert, Imad El Haddad, Andre S. H. Prevot, Wei Huang, and Claudia Mohr
Atmos. Chem. Phys., 21, 14907–14925, https://doi.org/10.5194/acp-21-14907-2021, https://doi.org/10.5194/acp-21-14907-2021, 2021
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Night-time reactions of biogenic volatile organic compounds and nitrate radicals can lead to the formation of secondary organic aerosol (BSOANO3). Here, we study the impacts of light exposure on the BSOANO3 from three biogenic precursors. Our results suggest that photolysis causes photodegradation of a substantial fraction of BSOANO3, changes the chemical composition and bulk volatility, and might be a potentially important loss pathway of BSOANO3 during the night-to-day transition.
Mehliyar Sadiq, Paul I. Palmer, Mark F. Lunt, Liang Feng, Ingrid Super, Stijn N. C. Dellaert, and Hugo A. C. Denier van der Gon
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-816, https://doi.org/10.5194/acp-2021-816, 2021
Publication in ACP not foreseen
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We make use of high-resolution emission inventory of CO2 and co-emitted tracers, satellite measurements, together with nested atmospheric transport model simulation, to investigate how reactive trace gases such as nitrogen dioxide and carbon monoxide can be used as proxies to determine the combustion contribution to atmospheric CO2 over Europe. We find stronger correlation in ratios of nitrogen dioxide and carbon dioxide between emission and satellite observed and modelled column concentration.
Aristeidis Voliotis, Yu Wang, Yunqi Shao, Mao Du, Thomas J. Bannan, Carl J. Percival, Spyros N. Pandis, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 21, 14251–14273, https://doi.org/10.5194/acp-21-14251-2021, https://doi.org/10.5194/acp-21-14251-2021, 2021
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Secondary organic aerosol (SOA) formation from mixtures of volatile precursors can be affected by the molecular interactions of the products. Composition and volatility measurements of SOA formed from mixtures of anthropogenic and biogenic precursors reveal processes that can increase or decrease the SOA volatility. The unique products of the mixture were more oxygenated and less volatile than those from either precursor. Analytical context is provided to explore the SOA volatility in mixtures.
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Houssni Lamkaddam, Mingyi Wang, Farnoush Ataei, Victoria Hofbauer, Brandon Lopez, Neil M. Donahue, Josef Dommen, Andre S. H. Prevot, Jay G. Slowik, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
Atmos. Meas. Tech., 14, 5913–5923, https://doi.org/10.5194/amt-14-5913-2021, https://doi.org/10.5194/amt-14-5913-2021, 2021
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Extractive electrospray ionization mass spectrometry (EESI-MS) has been deployed for high throughput online detection of particles with minimal fragmentation. Our study elucidates the extraction mechanism between the particles and electrospray (ES) droplets of different properties. The results show that the extraction rate is likely affected by the coagulation rate between the particles and ES droplets. Once coagulated, the particles undergo complete extraction within the ES droplet.
Vaios Moschos, Martin Gysel-Beer, Robin L. Modini, Joel C. Corbin, Dario Massabò, Camilla Costa, Silvia G. Danelli, Athanasia Vlachou, Kaspar R. Daellenbach, Sönke Szidat, Paolo Prati, André S. H. Prévôt, Urs Baltensperger, and Imad El Haddad
Atmos. Chem. Phys., 21, 12809–12833, https://doi.org/10.5194/acp-21-12809-2021, https://doi.org/10.5194/acp-21-12809-2021, 2021
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This study provides a holistic approach to studying the spectrally resolved light absorption by atmospheric brown carbon (BrC) and black carbon using long time series of daily samples from filter-based measurements. The obtained results provide (1) a better understanding of the aerosol absorption profile and its dependence on BrC and on lensing from less absorbing coatings and (2) an estimation of the most important absorbers at typical European locations.
Evelyn Freney, Karine Sellegri, Alessia Nicosia, Leah R. Williams, Matteo Rinaldi, Jonathan T. Trueblood, André S. H. Prévôt, Melilotus Thyssen, Gérald Grégori, Nils Haëntjens, Julie Dinasquet, Ingrid Obernosterer, France Van Wambeke, Anja Engel, Birthe Zäncker, Karine Desboeufs, Eija Asmi, Hilkka Timonen, and Cécile Guieu
Atmos. Chem. Phys., 21, 10625–10641, https://doi.org/10.5194/acp-21-10625-2021, https://doi.org/10.5194/acp-21-10625-2021, 2021
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In this work, we present observations of the organic aerosol content in primary sea spray aerosols (SSAs) continuously generated along a 5-week cruise in the Mediterranean. This information is combined with seawater biogeochemical properties also measured continuously along the ship track to develop a number of parametrizations that can be used in models to determine SSA organic content in oligotrophic waters that represent 60 % of the oceans from commonly measured seawater variables.
Amir Yazdani, Nikunj Dudani, Satoshi Takahama, Amelie Bertrand, André S. H. Prévôt, Imad El Haddad, and Ann M. Dillner
Atmos. Chem. Phys., 21, 10273–10293, https://doi.org/10.5194/acp-21-10273-2021, https://doi.org/10.5194/acp-21-10273-2021, 2021
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Functional group compositions of primary and aged aerosols from wood burning and coal combustion sources from chamber experiments are interpreted through compounds present in the fuels and known gas-phase oxidation products. Infrared spectra of aged wood burning in the chamber and ambient biomass burning samples reveal striking similarities, and a new method for identifying burning-impacted samples in monitoring network measurements is presented.
Yandong Tong, Veronika Pospisilova, Lu Qi, Jing Duan, Yifang Gu, Varun Kumar, Pragati Rai, Giulia Stefenelli, Liwei Wang, Ying Wang, Haobin Zhong, Urs Baltensperger, Junji Cao, Ru-Jin Huang, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 21, 9859–9886, https://doi.org/10.5194/acp-21-9859-2021, https://doi.org/10.5194/acp-21-9859-2021, 2021
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We investigate SOA sources and formation processes by a field deployment of the EESI-TOF-MS and L-TOF AMS in Beijing in late autumn and early winter. Our study shows that the sources and processes giving rise to haze events in Beijing are variable and seasonally dependent: (1) in the heating season, SOA formation is driven by oxidation of aromatics from solid fuel combustion; and (2) under high-NOx and RH conditions, aqueous-phase chemistry can be a major contributor to SOA formation.
Siqi Hou, Di Liu, Jingsha Xu, Tuan V. Vu, Xuefang Wu, Deepchandra Srivastava, Pingqing Fu, Linjie Li, Yele Sun, Athanasia Vlachou, Vaios Moschos, Gary Salazar, Sönke Szidat, André S. H. Prévôt, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 21, 8273–8292, https://doi.org/10.5194/acp-21-8273-2021, https://doi.org/10.5194/acp-21-8273-2021, 2021
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This study provides a newly developed method which combines radiocarbon (14C) with organic tracers to enable source apportionment of primary and secondary fossil vs. non-fossil sources of carbonaceous aerosols at an urban and a rural site of Beijing. The source apportionment results were compared with those by chemical mass balance and AMS/ACSM-PMF methods. Correlations of WINSOC and WSOC with different sources of OC were also performed to elucidate the formation mechanisms of SOC.
Ana Maria Roxana Petrescu, Chunjing Qiu, Philippe Ciais, Rona L. Thompson, Philippe Peylin, Matthew J. McGrath, Efisio Solazzo, Greet Janssens-Maenhout, Francesco N. Tubiello, Peter Bergamaschi, Dominik Brunner, Glen P. Peters, Lena Höglund-Isaksson, Pierre Regnier, Ronny Lauerwald, David Bastviken, Aki Tsuruta, Wilfried Winiwarter, Prabir K. Patra, Matthias Kuhnert, Gabriel D. Oreggioni, Monica Crippa, Marielle Saunois, Lucia Perugini, Tiina Markkanen, Tuula Aalto, Christine D. Groot Zwaaftink, Hanqin Tian, Yuanzhi Yao, Chris Wilson, Giulia Conchedda, Dirk Günther, Adrian Leip, Pete Smith, Jean-Matthieu Haussaire, Antti Leppänen, Alistair J. Manning, Joe McNorton, Patrick Brockmann, and Albertus Johannes Dolman
Earth Syst. Sci. Data, 13, 2307–2362, https://doi.org/10.5194/essd-13-2307-2021, https://doi.org/10.5194/essd-13-2307-2021, 2021
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This study is topical and provides a state-of-the-art scientific overview of data availability from bottom-up and top-down CH4 and N2O emissions in the EU27 and UK. The data integrate recent emission inventories with process-based model data and regional/global inversions for the European domain, aiming at reconciling them with official country-level UNFCCC national GHG inventories in support to policy and to facilitate real-time verification procedures.
Ana Maria Roxana Petrescu, Matthew J. McGrath, Robbie M. Andrew, Philippe Peylin, Glen P. Peters, Philippe Ciais, Gregoire Broquet, Francesco N. Tubiello, Christoph Gerbig, Julia Pongratz, Greet Janssens-Maenhout, Giacomo Grassi, Gert-Jan Nabuurs, Pierre Regnier, Ronny Lauerwald, Matthias Kuhnert, Juraj Balkovič, Mart-Jan Schelhaas, Hugo A. C. Denier van der
Gon, Efisio Solazzo, Chunjing Qiu, Roberto Pilli, Igor B. Konovalov, Richard A. Houghton, Dirk Günther, Lucia Perugini, Monica Crippa, Raphael Ganzenmüller, Ingrid T. Luijkx, Pete Smith, Saqr Munassar, Rona L. Thompson, Giulia Conchedda, Guillaume Monteil, Marko Scholze, Ute Karstens, Patrick Brockmann, and Albertus Johannes Dolman
Earth Syst. Sci. Data, 13, 2363–2406, https://doi.org/10.5194/essd-13-2363-2021, https://doi.org/10.5194/essd-13-2363-2021, 2021
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This study is topical and provides a state-of-the-art scientific overview of data availability from bottom-up and top-down CO2 fossil emissions and CO2 land fluxes in the EU27+UK. The data integrate recent emission inventories with ecosystem data, land carbon models and regional/global inversions for the European domain, aiming at reconciling CO2 estimates with official country-level UNFCCC national GHG inventories in support to policy and facilitating real-time verification procedures.
Karl Espen Yttri, Francesco Canonaco, Sabine Eckhardt, Nikolaos Evangeliou, Markus Fiebig, Hans Gundersen, Anne-Gunn Hjellbrekke, Cathrine Lund Myhre, Stephen Matthew Platt, André S. H. Prévôt, David Simpson, Sverre Solberg, Jason Surratt, Kjetil Tørseth, Hilde Uggerud, Marit Vadset, Xin Wan, and Wenche Aas
Atmos. Chem. Phys., 21, 7149–7170, https://doi.org/10.5194/acp-21-7149-2021, https://doi.org/10.5194/acp-21-7149-2021, 2021
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Carbonaceous aerosol sources and trends were studied at the Birkenes Observatory. A large decrease in elemental carbon (EC; 2001–2018) and a smaller decline in levoglucosan (2008–2018) suggest that organic carbon (OC)/EC from traffic/industry is decreasing, whereas the abatement of OC/EC from biomass burning has been less successful. Positive matrix factorization apportioned 72 % of EC to fossil fuel sources and 53 % (PM2.5) and 78 % (PM10–2.5) of OC to biogenic sources.
Athanasios Nenes, Spyros N. Pandis, Maria Kanakidou, Armistead G. Russell, Shaojie Song, Petros Vasilakos, and Rodney J. Weber
Atmos. Chem. Phys., 21, 6023–6033, https://doi.org/10.5194/acp-21-6023-2021, https://doi.org/10.5194/acp-21-6023-2021, 2021
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Ecosystems and air quality are affected by the dry deposition of inorganic reactive nitrogen (Nr, the sum of ammonium and nitrate). Its large variability is driven by the large difference in deposition velocity of N when in the gas or particle phase. Here we show that aerosol liquid water and acidity, by affecting gas–particle partitioning, modulate the dry deposition velocity of NH3, HNO3, and Nr worldwide. These effects explain the rapid accumulation of nitrate aerosol during haze events.
Georgia N. Theodoritsi, Giancarlo Ciarelli, and Spyros N. Pandis
Geosci. Model Dev., 14, 2041–2055, https://doi.org/10.5194/gmd-14-2041-2021, https://doi.org/10.5194/gmd-14-2041-2021, 2021
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Two schemes based on the volatility basis set were used for the simulation of biomass burning organic aerosol (bbOA) in the continental US. The first is the default scheme of the PMCAMx-SR model, and the second is a recently developed scheme based on laboratory experiments. The alternative bbOA scheme predicts much higher concentrations. The default scheme performed better during summer and fall, while the alternative scheme was a little better during spring.
Efisio Solazzo, Monica Crippa, Diego Guizzardi, Marilena Muntean, Margarita Choulga, and Greet Janssens-Maenhout
Atmos. Chem. Phys., 21, 5655–5683, https://doi.org/10.5194/acp-21-5655-2021, https://doi.org/10.5194/acp-21-5655-2021, 2021
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We conducted an extensive analysis of the structural uncertainty of the Emissions Database for Global Atmospheric Research (EDGAR) emission inventory of greenhouse gases, which adds a much needed reliability dimension to the accuracy of the emission estimates. The study undertakes in-depth analyses of the implication of aggregating emissions from different sources and/or countries on the accuracy. Results are presented for all emissions sectors according to IPCC definitions.
Weiqi Xu, Chun Chen, Yanmei Qiu, Ying Li, Zhiqiang Zhang, Eleni Karnezi, Spyros N. Pandis, Conghui Xie, Zhijie Li, Jiaxing Sun, Nan Ma, Wanyun Xu, Pingqing Fu, Zifa Wang, Jiang Zhu, Douglas R. Worsnop, Nga Lee Ng, and Yele Sun
Atmos. Chem. Phys., 21, 5463–5476, https://doi.org/10.5194/acp-21-5463-2021, https://doi.org/10.5194/acp-21-5463-2021, 2021
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Here aerosol volatility and viscosity at a rural site (Gucheng) and an urban site (Beijing) in the North China Plain (NCP) were investigated in summer and winter. Our results showed that organic aerosol (OA) in winter in the NCP is more volatile than that in summer due to enhanced primary emissions from coal combustion and biomass burning. We also found that OA existed mainly as a solid in winter in Beijing but as semisolids in Beijing in summer and Gucheng in winter.
Jianhui Jiang, Imad El Haddad, Sebnem Aksoyoglu, Giulia Stefenelli, Amelie Bertrand, Nicolas Marchand, Francesco Canonaco, Jean-Eudes Petit, Olivier Favez, Stefania Gilardoni, Urs Baltensperger, and André S. H. Prévôt
Geosci. Model Dev., 14, 1681–1697, https://doi.org/10.5194/gmd-14-1681-2021, https://doi.org/10.5194/gmd-14-1681-2021, 2021
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We developed a box model with a volatility basis set to simulate organic aerosol (OA) from biomass burning and optimized the vapor-wall-loss-corrected OA yields with a genetic algorithm. The optimized parameterizations were then implemented in the air quality model CAMx v6.5. Comparisons with ambient measurements indicate that the vapor-wall-loss-corrected parameterization effectively improves the model performance in predicting OA, which reduced the mean fractional bias from −72.9 % to −1.6 %.
Xiaohui Lin, Wen Zhang, Monica Crippa, Shushi Peng, Pengfei Han, Ning Zeng, Lijun Yu, and Guocheng Wang
Earth Syst. Sci. Data, 13, 1073–1088, https://doi.org/10.5194/essd-13-1073-2021, https://doi.org/10.5194/essd-13-1073-2021, 2021
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CH4 is a potent greenhouse gas, and China’s anthropogenic CH4 emissions account for a large proportion of global total emissions. However, the existing estimates either focus on a specific sector or lag behind real time by several years. We collected and analyzed 12 datasets and compared them to reveal the spatiotemporal changes and their uncertainties. We further estimated the emissions from 1990–2019, and the estimates showed a robust trend in recent years when compared to top-down results.
Marc Guevara, Oriol Jorba, Carles Tena, Hugo Denier van der Gon, Jeroen Kuenen, Nellie Elguindi, Sabine Darras, Claire Granier, and Carlos Pérez García-Pando
Earth Syst. Sci. Data, 13, 367–404, https://doi.org/10.5194/essd-13-367-2021, https://doi.org/10.5194/essd-13-367-2021, 2021
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The temporal variability of atmospheric emissions is linked to changes in activity patterns, emission processes and meteorology. Accounting for the change in temporal emission characteristics is a key aspect for modelling the trends of air pollutants. This work presents a dataset of global and European emission temporal profiles to be used for air quality modelling purposes. The profiles were constructed considering the influences of local sociodemographic factors and climatological conditions.
Francesco Canonaco, Anna Tobler, Gang Chen, Yulia Sosedova, Jay Gates Slowik, Carlo Bozzetti, Kaspar Rudolf Daellenbach, Imad El Haddad, Monica Crippa, Ru-Jin Huang, Markus Furger, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Meas. Tech., 14, 923–943, https://doi.org/10.5194/amt-14-923-2021, https://doi.org/10.5194/amt-14-923-2021, 2021
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Long-term ambient aerosol mass spectrometric data were analyzed with a statistical model (PMF) to obtain source contributions and fingerprints. The new aspects of this paper involve time-dependent source fingerprints by a rolling technique and the replacement of the full visual inspection of each run by a user-defined set of criteria to monitor the quality of each of these runs more efficiently. More reliable sources will finally provide better instruments for political mitigation strategies.
Stylianos Kakavas, David Patoulias, Maria Zakoura, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 21, 799–811, https://doi.org/10.5194/acp-21-799-2021, https://doi.org/10.5194/acp-21-799-2021, 2021
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The dependence of aerosol acidity on particle size, location, and altitude over Europe during a summertime period is investigated. Differences of up to 1–4 pH units are predicted between sub- and supermicron particles in northern and southern Europe. Particles of all sizes become increasingly acidic with altitude (0.5–2.5 pH units decrease over 2.5 km). The size-dependent pH differences carry important implications for pH-sensitive processes in the aerosol.
Marc Guevara, Oriol Jorba, Albert Soret, Hervé Petetin, Dene Bowdalo, Kim Serradell, Carles Tena, Hugo Denier van der Gon, Jeroen Kuenen, Vincent-Henri Peuch, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 21, 773–797, https://doi.org/10.5194/acp-21-773-2021, https://doi.org/10.5194/acp-21-773-2021, 2021
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Most European countries have imposed lockdowns to combat the spread of the COVID-19 pandemic. Such a socioeconomic disruption has resulted in a sudden drop of atmospheric emissions and air pollution levels. This study quantifies the daily reductions in national emissions and associated levels of nitrogen dioxide (NO2) due to the COVID-19 lockdowns in Europe, by making use of multiple open-access measured activity data as well as artificial intelligence and modelling techniques.
Pragati Rai, Jay G. Slowik, Markus Furger, Imad El Haddad, Suzanne Visser, Yandong Tong, Atinderpal Singh, Günther Wehrle, Varun Kumar, Anna K. Tobler, Deepika Bhattu, Liwei Wang, Dilip Ganguly, Neeraj Rastogi, Ru-Jin Huang, Jaroslaw Necki, Junji Cao, Sachchida N. Tripathi, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 21, 717–730, https://doi.org/10.5194/acp-21-717-2021, https://doi.org/10.5194/acp-21-717-2021, 2021
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We present a simple conceptual framework based on elemental size distributions and enrichment factors that allows for a characterization of major sources, site-to-site similarities, and local differences and the identification of key information required for efficient policy development. Absolute concentrations are by far the highest in Delhi, followed by Beijing, and then the European cities.
Sebnem Aksoyoglu, Jianhui Jiang, Giancarlo Ciarelli, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 15665–15680, https://doi.org/10.5194/acp-20-15665-2020, https://doi.org/10.5194/acp-20-15665-2020, 2020
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We investigated the role of ammonia in European air quality between 1990 and 2030 under varying land and ship emissions. If ship emissions will be regulated more strictly in the future, particulate nitrate will decrease in coastal areas in northern Europe, while sulfate aerosol will decrease in the Mediterranean region. We predict a shift in the sensitivity of aerosol formation from NH3 towards NOx emissions between 1990 and 2030 in most of Europe except the eastern part of the model domain.
Erin E. McDuffie, Steven J. Smith, Patrick O'Rourke, Kushal Tibrewal, Chandra Venkataraman, Eloise A. Marais, Bo Zheng, Monica Crippa, Michael Brauer, and Randall V. Martin
Earth Syst. Sci. Data, 12, 3413–3442, https://doi.org/10.5194/essd-12-3413-2020, https://doi.org/10.5194/essd-12-3413-2020, 2020
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Global emission inventories are vital to understanding the impacts of air pollution on the environment, human health, and society. We update the open-source Community Emissions Data System (CEDS) to provide global gridded emissions of seven key air pollutants from 1970–2017 for 11 source sectors and multiple fuel types, including coal, solid biofuel, and liquid oil and natural gas. This dataset includes both monthly global gridded emissions and annual national totals.
Hossein Maazallahi, Julianne M. Fernandez, Malika Menoud, Daniel Zavala-Araiza, Zachary D. Weller, Stefan Schwietzke, Joseph C. von Fischer, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 14717–14740, https://doi.org/10.5194/acp-20-14717-2020, https://doi.org/10.5194/acp-20-14717-2020, 2020
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Methane accounts for ∼ 25 % of current climate warming. The current lack of methane measurements is a barrier for tracking major sources, which are key for near-term climate mitigation. We use mobile measurements to identify and quantify methane emission sources in Utrecht (NL) and Hamburg (DE) with a focus on natural gas pipeline leaks. The measurements resulted in fixing the major leaks by the local utility, but coordinated efforts are needed at national levels for further emission reductions.
Antonios Tasoglou, Evangelos Louvaris, Kalliopi Florou, Aikaterini Liangou, Eleni Karnezi, Christos Kaltsonoudis, Ningxin Wang, and Spyros N. Pandis
Atmos. Chem. Phys., 20, 11625–11637, https://doi.org/10.5194/acp-20-11625-2020, https://doi.org/10.5194/acp-20-11625-2020, 2020
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A month-long set of summertime measurements in a remote area in the Mediterranean is used to quantify aerosol absorption. The measured light absorption was two or more times higher than that of fresh black carbon. The absorption enhancement due to the coating of black carbon cores by other aerosol components could explain only part of this absorption enhancement. The rest was due to brown carbon, mostly in the form of extremely low volatility organic compounds.
Anna K. Tobler, Alicja Skiba, Dongyu S. Wang, Philip Croteau, Katarzyna Styszko, Jarosław Nęcki, Urs Baltensperger, Jay G. Slowik, and André S. H. Prévôt
Atmos. Meas. Tech., 13, 5293–5301, https://doi.org/10.5194/amt-13-5293-2020, https://doi.org/10.5194/amt-13-5293-2020, 2020
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Some quadrupole aerosol chemical speciation monitors (Q-ACSMs) have had issues with the quantification of particulate chloride, resulting in apparent negative chloride concentrations. We can show that this is due to the different behavior of Cl+ and HCl+, and we present a correction for the more accurate quantification of chloride. The correction can be applied to measurements in environments where the particulate chloride is dominated by NH4Cl.
Pengfei Han, Ning Zeng, Tom Oda, Xiaohui Lin, Monica Crippa, Dabo Guan, Greet Janssens-Maenhout, Xiaolin Ma, Zhu Liu, Yuli Shan, Shu Tao, Haikun Wang, Rong Wang, Lin Wu, Xiao Yun, Qiang Zhang, Fang Zhao, and Bo Zheng
Atmos. Chem. Phys., 20, 11371–11385, https://doi.org/10.5194/acp-20-11371-2020, https://doi.org/10.5194/acp-20-11371-2020, 2020
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An accurate estimation of China’s fossil-fuel CO2 emissions (FFCO2) is significant for quantification of carbon budget and emissions reductions towards the Paris Agreement goals. Here we assessed 9 global and regional inventories. Our findings highlight the significance of using locally measured coal emission factors. We call on the enhancement of physical measurements for validation and provide comprehensive information for inventory, monitoring, modeling, assimilation, and reducing emissions.
Srijana Lama, Sander Houweling, K. Folkert Boersma, Henk Eskes, Ilse Aben, Hugo A. C. Denier van der Gon, Maarten C. Krol, Han Dolman, Tobias Borsdorff, and Alba Lorente
Atmos. Chem. Phys., 20, 10295–10310, https://doi.org/10.5194/acp-20-10295-2020, https://doi.org/10.5194/acp-20-10295-2020, 2020
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Rapid urbanization has increased the consumption of fossil fuel, contributing the degradation of urban air quality. Burning efficiency is a major factor determining the impact of fuel burning on the environment. We quantify the burning efficiency of fossil fuel use over six megacities using satellite remote sensing data. City governance can use these results to understand air pollution scenarios and to formulate effective air pollution control strategies.
Liwei Wang, Jay G. Slowik, Nidhi Tripathi, Deepika Bhattu, Pragati Rai, Varun Kumar, Pawan Vats, Rangu Satish, Urs Baltensperger, Dilip Ganguly, Neeraj Rastogi, Lokesh K. Sahu, Sachchida N. Tripathi, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 9753–9770, https://doi.org/10.5194/acp-20-9753-2020, https://doi.org/10.5194/acp-20-9753-2020, 2020
Martin Rigler, Luka Drinovec, Gašper Lavrič, Athanasia Vlachou, André S. H. Prévôt, Jean Luc Jaffrezo, Iasonas Stavroulas, Jean Sciare, Judita Burger, Irena Kranjc, Janja Turšič, Anthony D. A. Hansen, and Griša Močnik
Atmos. Meas. Tech., 13, 4333–4351, https://doi.org/10.5194/amt-13-4333-2020, https://doi.org/10.5194/amt-13-4333-2020, 2020
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Carbonaceous aerosols are a large fraction of fine particulate matter. They are extremely diverse, and they directly impact air quality, visibility, cloud formation and public health. In this paper we present a new instrument and new method to measure carbon content in particulate matter in real time and at a high time resolution. The new method was validated in a 1-month winter field campaign in Ljubljana, Slovenia.
Eirini Boleti, Christoph Hueglin, Stuart K. Grange, André S. H. Prévôt, and Satoshi Takahama
Atmos. Chem. Phys., 20, 9051–9066, https://doi.org/10.5194/acp-20-9051-2020, https://doi.org/10.5194/acp-20-9051-2020, 2020
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Long-term temporal evolution of ozone concentrations between 2000 and 2015 in Europe was estimated using a signal decomposition technique. The seasonal cycles are correlated with local climate conditions and vary according to geographic region, while ozone levels are indicative of distance to emission sources. The site's environment plays a key role in ozone trends, with the most polluted environments showing the least reduction in ozone, while in less polluted areas ozone has decreased.
Tuukka Petäjä, Ella-Maria Duplissy, Ksenia Tabakova, Julia Schmale, Barbara Altstädter, Gerard Ancellet, Mikhail Arshinov, Yurii Balin, Urs Baltensperger, Jens Bange, Alison Beamish, Boris Belan, Antoine Berchet, Rossana Bossi, Warren R. L. Cairns, Ralf Ebinghaus, Imad El Haddad, Beatriz Ferreira-Araujo, Anna Franck, Lin Huang, Antti Hyvärinen, Angelika Humbert, Athina-Cerise Kalogridis, Pavel Konstantinov, Astrid Lampert, Matthew MacLeod, Olivier Magand, Alexander Mahura, Louis Marelle, Vladimir Masloboev, Dmitri Moisseev, Vaios Moschos, Niklas Neckel, Tatsuo Onishi, Stefan Osterwalder, Aino Ovaska, Pauli Paasonen, Mikhail Panchenko, Fidel Pankratov, Jakob B. Pernov, Andreas Platis, Olga Popovicheva, Jean-Christophe Raut, Aurélie Riandet, Torsten Sachs, Rosamaria Salvatori, Roberto Salzano, Ludwig Schröder, Martin Schön, Vladimir Shevchenko, Henrik Skov, Jeroen E. Sonke, Andrea Spolaor, Vasileios K. Stathopoulos, Mikko Strahlendorff, Jennie L. Thomas, Vito Vitale, Sterios Vratolis, Carlo Barbante, Sabine Chabrillat, Aurélien Dommergue, Konstantinos Eleftheriadis, Jyri Heilimo, Kathy S. Law, Andreas Massling, Steffen M. Noe, Jean-Daniel Paris, André S. H. Prévôt, Ilona Riipinen, Birgit Wehner, Zhiyong Xie, and Hanna K. Lappalainen
Atmos. Chem. Phys., 20, 8551–8592, https://doi.org/10.5194/acp-20-8551-2020, https://doi.org/10.5194/acp-20-8551-2020, 2020
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The role of polar regions is increasing in terms of megatrends such as globalization, new transport routes, demography, and the use of natural resources with consequent effects on regional and transported pollutant concentrations. Here we summarize initial results from our integrative project exploring the Arctic environment and pollution to deliver data products, metrics, and indicators for stakeholders.
Yunle Chen, Masayuki Takeuchi, Theodora Nah, Lu Xu, Manjula R. Canagaratna, Harald Stark, Karsten Baumann, Francesco Canonaco, André S. H. Prévôt, L. Gregory Huey, Rodney J. Weber, and Nga L. Ng
Atmos. Chem. Phys., 20, 8421–8440, https://doi.org/10.5194/acp-20-8421-2020, https://doi.org/10.5194/acp-20-8421-2020, 2020
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Two online mass spectrometry instruments, an aerosol mass spectrometer and a chemical ionization mass spectrometer equipped with a filter inlet for gases and aerosols, were deployed at Yorkville, GA, for a comprehensive characterization of organic aerosol. We observed notable secondary organic aerosol formation from isoprene and monoterpenes via different pathways during both day and night, and a series of highly oxidized acid-like compounds was found to be closely related to aged SOA.
Philippe Thunis, Monica Crippa, Cornelis Cuvelier, Diego Guizzardi, Alexander De Meij, Gabriel Oreggioni, and Enrico Pisoni
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2020-144, https://doi.org/10.5194/essd-2020-144, 2020
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A comparison of emissions inventories for air quality modelling, in Europe, is presented. Among these inventories, EDGAR v5.0 for air pollutants is introduced and validated, through a simulation with the EMEP model.
Lu Qi, Alexander L. Vogel, Sepideh Esmaeilirad, Liming Cao, Jing Zheng, Jean-Luc Jaffrezo, Paola Fermo, Anne Kasper-Giebl, Kaspar R. Daellenbach, Mindong Chen, Xinlei Ge, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 20, 7875–7893, https://doi.org/10.5194/acp-20-7875-2020, https://doi.org/10.5194/acp-20-7875-2020, 2020
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We present the first application of this online and offline strategy using the new extractive electrospray ionization time-of-flight mass spectrometer (EESI-TOF), which achieves increased chemical specificity relative to other online techniques. Measurement and source apportionment of 1 year of filter samples collected in Zurich, Switzerland, show seasonal contributions from fresh and aged wood combustion in winter and biogenic emission-derived SOA in summer, as well as other sources.
Ingrid Super, Hugo A. C. Denier van der Gon, Michiel K. van der Molen, Stijn N. C. Dellaert, and Wouter Peters
Geosci. Model Dev., 13, 2695–2721, https://doi.org/10.5194/gmd-13-2695-2020, https://doi.org/10.5194/gmd-13-2695-2020, 2020
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Understanding urban CO2 fluxes is increasingly important to support emission reduction policies. In this work we extended an existing framework for emission verification to increase its suitability for urban areas and source-sector-based decision-making by using a dynamic emission model. We find that the dynamic emission model provides a better understanding of emissions at small scales and their uncertainties. By including co-emitted species, emission can be related to specific source sectors.
Siddika Celik, Frank Drewnick, Friederike Fachinger, James Brooks, Eoghan Darbyshire, Hugh Coe, Jean-Daniel Paris, Philipp G. Eger, Jan Schuladen, Ivan Tadic, Nils Friedrich, Dirk Dienhart, Bettina Hottmann, Horst Fischer, John N. Crowley, Hartwig Harder, and Stephan Borrmann
Atmos. Chem. Phys., 20, 4713–4734, https://doi.org/10.5194/acp-20-4713-2020, https://doi.org/10.5194/acp-20-4713-2020, 2020
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Analysis of 252 ship emission plumes in the Mediterranean Sea and around the Arabian Peninsula examined particulate- and gas-phase characteristics. By identifying the corresponding ships, source features and plume age were determined. Emission factors (amount of pollutant per kilogram of fuel burned) were calculated and investigated for dependencies on source characteristics, atmospheric conditions, and transport time, providing insight into the most relevant influences on ship emissions.
Jia Chen, Florian Dietrich, Hossein Maazallahi, Andreas Forstmaier, Dominik Winkler, Magdalena E. G. Hofmann, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 3683–3696, https://doi.org/10.5194/acp-20-3683-2020, https://doi.org/10.5194/acp-20-3683-2020, 2020
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We demonstrate for the first time that large festivals can be significant methane sources, though they are not included in emission inventories. We combined in situ measurements with a Gaussian plume model to determine the Oktoberfest emissions and show that they are not due solely to human biogenic emissions, but are instead primarily fossil fuel related. Our study provides the foundation to develop reduction policies for such events and new pathways to mitigate fossil fuel methane emissions.
Athanasios Nenes, Spyros N. Pandis, Rodney J. Weber, and Armistead Russell
Atmos. Chem. Phys., 20, 3249–3258, https://doi.org/10.5194/acp-20-3249-2020, https://doi.org/10.5194/acp-20-3249-2020, 2020
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We show that aerosol acidity (pH) and liquid water content naturally emerge as previously ignored parameters that drive particulate matter formation in the atmosphere, and its sensitivity to emissions of ammonia and nitric acid. The simple framework presented is easily applied to ambient measurements or model output, and it provides the
chemical regimeof PM sensitivity to ammonia and nitric acid availability.
Ingrid Super, Stijn N. C. Dellaert, Antoon J. H. Visschedijk, and Hugo A. C. Denier van der Gon
Atmos. Chem. Phys., 20, 1795–1816, https://doi.org/10.5194/acp-20-1795-2020, https://doi.org/10.5194/acp-20-1795-2020, 2020
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Emission data contain uncertainties introduced by the methodology and the data used. We quantified uncertainties in gridded emissions using the uncertainty in underlying data, showing that disaggregation in space and time significantly increases the uncertainty. Understanding uncertainties helps to interpret atmospheric measurements and the gap with modelled concentrations. Moreover, our analyses help identify regions with large uncertainties, which require further scrutiny.
Pragati Rai, Markus Furger, Jay G. Slowik, Francesco Canonaco, Roman Fröhlich, Christoph Hüglin, María Cruz Minguillón, Krag Petterson, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 20, 1657–1674, https://doi.org/10.5194/acp-20-1657-2020, https://doi.org/10.5194/acp-20-1657-2020, 2020
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A source apportionment study of hourly resolved elements in PM10 measured at a traffic-influenced site in Härkingen, Switzerland, using positive matrix factorization (PMF) and multilinear engine-2 (ME-2) offered resolution of robust and unambiguous factor profiles and contributions. We show that the rotational control available in ME-2 provides a means for treating extreme events such as fireworks within a PMF analysis.
Leyang Feng, Steven J. Smith, Caleb Braun, Monica Crippa, Matthew J. Gidden, Rachel Hoesly, Zbigniew Klimont, Margreet van Marle, Maarten van den Berg, and Guido R. van der Werf
Geosci. Model Dev., 13, 461–482, https://doi.org/10.5194/gmd-13-461-2020, https://doi.org/10.5194/gmd-13-461-2020, 2020
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We describe the methods used for generating gridded emission datasets produced for use by the modeling community, particularly for the Coupled Model Intercomparison Project Phase 6 (CMIP6). The development of three sets of gridded data (historical open burning, historical anthropogenic, and future scenarios) was coordinated to produce consistent data over 1750–2100. We discuss the methodologies used to produce these data along with limitations and potential for future work.
Marco Paglione, Stefania Gilardoni, Matteo Rinaldi, Stefano Decesari, Nicola Zanca, Silvia Sandrini, Lara Giulianelli, Dimitri Bacco, Silvia Ferrari, Vanes Poluzzi, Fabiana Scotto, Arianna Trentini, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Francesco Canonaco, André S. H. Prévôt, Paola Massoli, Claudio Carbone, Maria Cristina Facchini, and Sandro Fuzzi
Atmos. Chem. Phys., 20, 1233–1254, https://doi.org/10.5194/acp-20-1233-2020, https://doi.org/10.5194/acp-20-1233-2020, 2020
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Our multi-year observational study regarding organic aerosol (OA) in the Po Valley indicates that more than half of OA is of secondary origin (SOA) through all the year and at both urban and rural sites. Within the SOA, the measurements show the importance of biomass burning (BB) aging products during cold seasons and indicate aqueous-phase processing of BB emissions as a fundamental driver of SOA formation in wintertime, with important consequences for air quality policy at the global level.
Ying Chen, Yafang Cheng, Nan Ma, Chao Wei, Liang Ran, Ralf Wolke, Johannes Größ, Qiaoqiao Wang, Andrea Pozzer, Hugo A. C. Denier van der Gon, Gerald Spindler, Jos Lelieveld, Ina Tegen, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 20, 771–786, https://doi.org/10.5194/acp-20-771-2020, https://doi.org/10.5194/acp-20-771-2020, 2020
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Particulate nitrate is one of the most important climate cooling agents. Our results show that interaction with sea-salt aerosol can shift nitrate to larger sized particles (redistribution effect), weakening its direct cooling effect. The modelling results indicate strong redistribution over coastal and offshore regions worldwide as well as continental Europe. Improving the consideration of the redistribution effect in global models fosters a better understanding of climate change.
Jianhui Jiang, Sebnem Aksoyoglu, Imad El-Haddad, Giancarlo Ciarelli, Hugo A. C. Denier van der Gon, Francesco Canonaco, Stefania Gilardoni, Marco Paglione, María Cruz Minguillón, Olivier Favez, Yunjiang Zhang, Nicolas Marchand, Liqing Hao, Annele Virtanen, Kalliopi Florou, Colin O'Dowd, Jurgita Ovadnevaite, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 15247–15270, https://doi.org/10.5194/acp-19-15247-2019, https://doi.org/10.5194/acp-19-15247-2019, 2019
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We use an air quality model with a modified organic aerosol (OA) module based on chamber experiments to identify the OA sources and their contributions in Europe. Comparisons with long-term measurements at nine sites in 2011 show an improvement in OA simulation. Our results suggest that the biomass burning and biogenic emissions are the dominant sources in winter and summer, respectively. Contributions of diesel and gasoline vehicles are relatively small compared to a previous study in the US.
Giulia Stefenelli, Veronika Pospisilova, Felipe D. Lopez-Hilfiker, Kaspar R. Daellenbach, Christoph Hüglin, Yandong Tong, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 19, 14825–14848, https://doi.org/10.5194/acp-19-14825-2019, https://doi.org/10.5194/acp-19-14825-2019, 2019
Yunjiang Zhang, Olivier Favez, Jean-Eudes Petit, Francesco Canonaco, Francois Truong, Nicolas Bonnaire, Vincent Crenn, Tanguy Amodeo, Andre S. H. Prévôt, Jean Sciare, Valerie Gros, and Alexandre Albinet
Atmos. Chem. Phys., 19, 14755–14776, https://doi.org/10.5194/acp-19-14755-2019, https://doi.org/10.5194/acp-19-14755-2019, 2019
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We present 6-year source apportionment of organic aerosol (OA) achieved with near-continuous online measurements and subsequent receptor model analysis in the Paris region, France. The OA factors presented distinct seasonal patterns, associated with different atmospheric formation processes and roles in air pollution. Limited year-round trends for two primary anthropogenic factors and a biogenic-like secondary factor were observed, while a more oxidized secondary OA showed a decreasing feature.
Jun Zhou, Miriam Elser, Ru-Jin Huang, Manuel Krapf, Roman Fröhlich, Deepika Bhattu, Giulia Stefenelli, Peter Zotter, Emily A. Bruns, Simone M. Pieber, Haiyan Ni, Qiyuan Wang, Yichen Wang, Yaqing Zhou, Chunying Chen, Mao Xiao, Jay G. Slowik, Samuel Brown, Laure-Estelle Cassagnes, Kaspar R. Daellenbach, Thomas Nussbaumer, Marianne Geiser, André S. H. Prévôt, Imad El-Haddad, Junji Cao, Urs Baltensperger, and Josef Dommen
Atmos. Chem. Phys., 19, 14703–14720, https://doi.org/10.5194/acp-19-14703-2019, https://doi.org/10.5194/acp-19-14703-2019, 2019
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Reactive oxygen species (ROS) are believed to contribute to the adverse health effects of aerosols. We measured particle-bound ROS (PB-ROS) with an online instrument in two distinct environments, i.e., Beijing (China) and Bern (Switzerland). In both cities these exogenic ROS are predominantly related to secondary organic aerosol (SOA). PB-ROS content in SOA from various anthropogenic emission sources tested in the laboratory was comparable to that in the ambient measurements.
Alcide Zhao, Massimo A. Bollasina, Monica Crippa, and David S. Stevenson
Atmos. Chem. Phys., 19, 14517–14533, https://doi.org/10.5194/acp-19-14517-2019, https://doi.org/10.5194/acp-19-14517-2019, 2019
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Emissions of aerosols over the recent past have been regulated largely by two policy-relevant drivers: energy-use growth and technology advances. These generate large and competing impacts on global radiation balance and climate, particularly over Asia, Europe, and the Arctic. This may help better assess and interpret future climate projections, and hence inform future climate change impact reduction strategies. Yet, it is pressing to better constrain various uncertainties related to aerosols.
Xiaoli Shen, Heike Vogel, Bernhard Vogel, Wei Huang, Claudia Mohr, Ramakrishna Ramisetty, Thomas Leisner, André S. H. Prévôt, and Harald Saathoff
Atmos. Chem. Phys., 19, 13189–13208, https://doi.org/10.5194/acp-19-13189-2019, https://doi.org/10.5194/acp-19-13189-2019, 2019
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This study provides good insight into the chemical nature and complex origin of aerosols by combining comprehensive field observations and transport modelling. We suggest that factors related to topography, metrological conditions, local emissions, in situ formation and growth, regional transport, and the interaction of biogenic and anthropogenic compounds need to be considered for a comprehensive understanding of aerosol processes.
Philipp G. Eger, Nils Friedrich, Jan Schuladen, Justin Shenolikar, Horst Fischer, Ivan Tadic, Hartwig Harder, Monica Martinez, Roland Rohloff, Sebastian Tauer, Frank Drewnick, Friederike Fachinger, James Brooks, Eoghan Darbyshire, Jean Sciare, Michael Pikridas, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 19, 12121–12140, https://doi.org/10.5194/acp-19-12121-2019, https://doi.org/10.5194/acp-19-12121-2019, 2019
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Shipborne measurements of nitryl chloride (ClNO2) were made during the AQABA (Air Quality and climate change in the Arabian BAsin) ship campaign in summer 2017. The dataset includes measurements over the Mediterranean Sea and around the Arabian Peninsula with observed mixing ratios ranging from the limit of detection to 600 pptv. We examined the regional variability in the generation of ClNO2 and its importance for Cl atom generation in a marine boundary layer influenced by ships and industry.
Giulia Stefenelli, Jianhui Jiang, Amelie Bertrand, Emily A. Bruns, Simone M. Pieber, Urs Baltensperger, Nicolas Marchand, Sebnem Aksoyoglu, André S. H. Prévôt, Jay G. Slowik, and Imad El Haddad
Atmos. Chem. Phys., 19, 11461–11484, https://doi.org/10.5194/acp-19-11461-2019, https://doi.org/10.5194/acp-19-11461-2019, 2019
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Box model simulations, based on the volatility basis set approach, of smog chamber wood combustion experiments conducted at different temperatures (−10 °C, 2 °C, 15 °C), emission loads, combustion conditions (flaming and smoldering) and residential stoves fabricated in the last 2 decades. Novel parameterization methods based on a genetic algorithm approach allowed estimation of precursor class contributions to SOA and evaluation of the effect of emission variability on SOA yield predictions.
Felipe D. Lopez-Hilfiker, Veronika Pospisilova, Wei Huang, Markus Kalberer, Claudia Mohr, Giulia Stefenelli, Joel A. Thornton, Urs Baltensperger, Andre S. H. Prevot, and Jay G. Slowik
Atmos. Meas. Tech., 12, 4867–4886, https://doi.org/10.5194/amt-12-4867-2019, https://doi.org/10.5194/amt-12-4867-2019, 2019
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We present a novel, field-deployable extractive electrospray time-of-flight mass spectrometer (EESI-TOF), which provides real-time, near-molecular measurements of organic aerosol at atmospherically relevant concentrations, addressing a critical gap in existing measurement capabilities. Successful deployments of the EESI-TOF for laboratory measurements, ground-based ambient sampling, and aboard a research aircraft highlight the versatility and potential of the EESI-TOF system.
Weiqi Xu, Conghui Xie, Eleni Karnezi, Qi Zhang, Junfeng Wang, Spyros N. Pandis, Xinlei Ge, Jingwei Zhang, Junling An, Qingqing Wang, Jian Zhao, Wei Du, Yanmei Qiu, Wei Zhou, Yao He, Ying Li, Jie Li, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 19, 10205–10216, https://doi.org/10.5194/acp-19-10205-2019, https://doi.org/10.5194/acp-19-10205-2019, 2019
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We present the first aerosol volatility measurements in Beijing in summer using a thermodenuder coupled with aerosol mass spectrometers. Our results showed that organic aerosol (OA) comprised mainly semi-volatile organic compounds in summer, and the freshly oxidized secondary OA was the most volatile component. We also found quite different volatility distributions in black-carbon-containing primary and secondary OA, ambient OA, ambient secondary OA and the WRF-Chem model.
Greet Janssens-Maenhout, Monica Crippa, Diego Guizzardi, Marilena Muntean, Edwin Schaaf, Frank Dentener, Peter Bergamaschi, Valerio Pagliari, Jos G. J. Olivier, Jeroen A. H. W. Peters, John A. van Aardenne, Suvi Monni, Ulrike Doering, A. M. Roxana Petrescu, Efisio Solazzo, and Gabriel D. Oreggioni
Earth Syst. Sci. Data, 11, 959–1002, https://doi.org/10.5194/essd-11-959-2019, https://doi.org/10.5194/essd-11-959-2019, 2019
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In support of the Paris Agreement, EDGARv4.3.2 provides global annual estimates, broken down into IPCC-compliant source-sector levels, from 1970 to 2012. The anthropogenic CO2, CH4 and N2O emissions were calculated bottom up with international statistics and emission factors for 226 countries and spatially distributed. EDGARv4.3.2 is input for the top-down modelling of the Global Carbon Project and EU policy-making, needing GHG emission estimates for each country at the climate negotiations.
Lu Qi, Mindong Chen, Giulia Stefenelli, Veronika Pospisilova, Yandong Tong, Amelie Bertrand, Christoph Hueglin, Xinlei Ge, Urs Baltensperger, André S. H. Prévôt, and Jay G. Slowik
Atmos. Chem. Phys., 19, 8037–8062, https://doi.org/10.5194/acp-19-8037-2019, https://doi.org/10.5194/acp-19-8037-2019, 2019
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Current understanding of OA sources is limited by the chemical resolution of existing real-time measurement technology. We describe the first wintertime deployment of a novel extractive electrospray ionization time-of-flight mass spectrometer, which provides near-molecular OA measurements with high time resolution. We show that biomass combustion strongly influences winter OA. Via factor analysis, aging-dependent signatures and time contributions of biomass-combustion-derived OA are resolved.
Athanasia Vlachou, Anna Tobler, Houssni Lamkaddam, Francesco Canonaco, Kaspar R. Daellenbach, Jean-Luc Jaffrezo, María Cruz Minguillón, Marek Maasikmets, Erik Teinemaa, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 7279–7295, https://doi.org/10.5194/acp-19-7279-2019, https://doi.org/10.5194/acp-19-7279-2019, 2019
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The resolution of rotational ambiguity in positive matrix factorization (PMF) models is a major challenge. Here, we developed a method based on bootstrapping and correlations to extract environmentally meaningful solutions from PMF analysis based on offline aerosol mass spectrometry data. The method has been tested on a dataset that covers 1 full year of filter samples collected at three different sites in Estonia.
Christos Kaltsonoudis, Spiro D. Jorga, Evangelos Louvaris, Kalliopi Florou, and Spyros N. Pandis
Atmos. Meas. Tech., 12, 2733–2743, https://doi.org/10.5194/amt-12-2733-2019, https://doi.org/10.5194/amt-12-2733-2019, 2019
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A portable dual-smog-chamber system was developed using two identical pillow-shaped smog chambers surrounded by UV lamps. The system has been designed to use ambient air as the starting point of the experiments. It can be easily disassembled and transported, enabling the study of various atmospheric environments and it can be used with natural sunlight. The results of test experiments using ambient air are discussed as examples of applications of this system.
Kaspar R. Daellenbach, Ivan Kourtchev, Alexander L. Vogel, Emily A. Bruns, Jianhui Jiang, Tuukka Petäjä, Jean-Luc Jaffrezo, Sebnem Aksoyoglu, Markus Kalberer, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 5973–5991, https://doi.org/10.5194/acp-19-5973-2019, https://doi.org/10.5194/acp-19-5973-2019, 2019
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Here we present the molecular composition of the organic aerosol (OA) at an urban site in Central Europe (Zurich, Switzerland) and compare it to smog chamber wood smoke and ambient biogenic secondary OA (SOA) (Orbitrap analyses). Accordingly, we are able to explain the strong seasonality of the molecular composition by aged wood smoke and biogenic SOA during winter and summer. Our results could also explain the predominance of non-fossil organic carbon at European locations throughout the year.
Katerina S. Karadima, Vlasis G. Mavrantzas, and Spyros N. Pandis
Atmos. Chem. Phys., 19, 5571–5587, https://doi.org/10.5194/acp-19-5571-2019, https://doi.org/10.5194/acp-19-5571-2019, 2019
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We explore the morphologies of multicomponent nanoparticles through atomistic molecular dynamics simulations under atmospherically relevant conditions. Phase separation is predicted for almost all simulated nanoparticles either between organics and inorganics or between hydrophobic and hydrophilic constituents. Three main particle types were identified: organic islands at the surface, inorganic core-organic shell morphologies and complex structures with hydrophobic and hydrophilic domains.
Georgia N. Theodoritsi and Spyros N. Pandis
Atmos. Chem. Phys., 19, 5403–5415, https://doi.org/10.5194/acp-19-5403-2019, https://doi.org/10.5194/acp-19-5403-2019, 2019
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The chemical transport model PMCAMx was extended to investigate the effects of partitioning and photochemical aging of biomass burning emissions on organic aerosol (OA) concentrations and was applied in Europe. During the summer, the contribution of biomass burning to total OA levels over continental Europe was 16 % and during winter 47 %. Intermediate volatility organic compounds are predicted to be important precursors of secondary OA from biomass burning.
Monica Crippa, Greet Janssens-Maenhout, Diego Guizzardi, Rita Van Dingenen, and Frank Dentener
Atmos. Chem. Phys., 19, 5165–5186, https://doi.org/10.5194/acp-19-5165-2019, https://doi.org/10.5194/acp-19-5165-2019, 2019
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In this work we evaluate the contribution of the major anthropogenic emission sources to global air quality and human health, focusing on particulate matter (PM) concentrations because of their importance in populated areas and the proven cumulative negative effects on human health. We show that in order to improve air quality, regional policies should be implemented due to the transboundary features of PM pollution.
Karl Espen Yttri, David Simpson, Robert Bergström, Gyula Kiss, Sönke Szidat, Darius Ceburnis, Sabine Eckhardt, Christoph Hueglin, Jacob Klenø Nøjgaard, Cinzia Perrino, Ignazio Pisso, Andre Stephan Henry Prevot, Jean-Philippe Putaud, Gerald Spindler, Milan Vana, Yan-Lin Zhang, and Wenche Aas
Atmos. Chem. Phys., 19, 4211–4233, https://doi.org/10.5194/acp-19-4211-2019, https://doi.org/10.5194/acp-19-4211-2019, 2019
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Carbonaceous aerosols from natural sources were abundant regardless of season. Residential wood burning (RWB) emissions were occasionally equally as large as or larger than of fossil-fuel sources, depending on season and region. RWB emissions are poorly constrained; thus emissions inventories need improvement. Harmonizing emission factors between countries is likely the most important step to improve model calculations for biomass burning emissions and European PM2.5 concentrations in general.
Debra Wunch, Dylan B. A. Jones, Geoffrey C. Toon, Nicholas M. Deutscher, Frank Hase, Justus Notholt, Ralf Sussmann, Thorsten Warneke, Jeroen Kuenen, Hugo Denier van der Gon, Jenny A. Fisher, and Joannes D. Maasakkers
Atmos. Chem. Phys., 19, 3963–3980, https://doi.org/10.5194/acp-19-3963-2019, https://doi.org/10.5194/acp-19-3963-2019, 2019
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We used five atmospheric observatories in Europe measuring total column dry-air mole fractions of methane and carbon monoxide to infer methane emissions in the area between the observatories. We find that the methane emissions are overestimated by the state-of-the-art inventories, and that this is likely due, at least in part, to the inventory disaggregation. We find that there is significant uncertainty in the carbon monoxide inventories that requires further investigation.
Jianhui Jiang, Sebnem Aksoyoglu, Giancarlo Ciarelli, Emmanouil Oikonomakis, Imad El-Haddad, Francesco Canonaco, Colin O'Dowd, Jurgita Ovadnevaite, María Cruz Minguillón, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 19, 3747–3768, https://doi.org/10.5194/acp-19-3747-2019, https://doi.org/10.5194/acp-19-3747-2019, 2019
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Biogenic volatile organic compound (BVOC) emissions from vegetation are essential inputs for air quality models but their uncertainties are very high. In this study we show the importance of BVOC emissions for modelled ozone and aerosol concentrations in Europe. Using different biogenic emissions from MEGAN and PSI models significantly affected organic aerosols (smaller effect on ozone), indicating the importance of harmonising the BVOC emissions in the model inter-comparison studies.
Mikko Äijälä, Kaspar R. Daellenbach, Francesco Canonaco, Liine Heikkinen, Heikki Junninen, Tuukka Petäjä, Markku Kulmala, André S. H. Prévôt, and Mikael Ehn
Atmos. Chem. Phys., 19, 3645–3672, https://doi.org/10.5194/acp-19-3645-2019, https://doi.org/10.5194/acp-19-3645-2019, 2019
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Aerosol mass spectrometry produces large amounts of complex data, the analysis of which necessitates chemometrics – the application of advanced statistical and mathematical tools to chemical data. Here, we perform a data-driven analysis of multiple aerosol mass spectrometric data sets, to show that the traditional separation of organics and inorganics is not necessary. The resulting 7-component aerosol speciation explains 83 % to 96 % of observed variability at our boreal forest experiment site.
Li Xing, Jiarui Wu, Miriam Elser, Shengrui Tong, Suixin Liu, Xia Li, Lang Liu, Junji Cao, Jiamao Zhou, Imad El-Haddad, Rujin Huang, Maofa Ge, Xuexi Tie, André S. H. Prévôt, and Guohui Li
Atmos. Chem. Phys., 19, 2343–2359, https://doi.org/10.5194/acp-19-2343-2019, https://doi.org/10.5194/acp-19-2343-2019, 2019
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We used the WRF-CHEM model to simulate wintertime secondary organic aerosol (SOA) concentrations over Beijing–Tianjin–Hebei (BTH), China. Heterogeneous HONO sources increased the near-surface SOA by 46.3 % in BTH. Direct emissions of glyoxal and methylglyoxal from residential sources contributed 25.5 % to the total SOA mass. Our study highlights the importance of heterogeneous HONO sources and primary residential emissions of glyoxal and methylglyoxal to SOA formation in winter over BTH.
Ru-Jin Huang, Yichen Wang, Junji Cao, Chunshui Lin, Jing Duan, Qi Chen, Yongjie Li, Yifang Gu, Jin Yan, Wei Xu, Roman Fröhlich, Francesco Canonaco, Carlo Bozzetti, Jurgita Ovadnevaite, Darius Ceburnis, Manjula R. Canagaratna, John Jayne, Douglas R. Worsnop, Imad El-Haddad, André S. H. Prévôt, and Colin D. O'Dowd
Atmos. Chem. Phys., 19, 2283–2298, https://doi.org/10.5194/acp-19-2283-2019, https://doi.org/10.5194/acp-19-2283-2019, 2019
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We found that in wintertime Shijiazhuang fine PM was mostly from primary emissions without sufficient atmospheric aging. In addition, secondary inorganic and organic aerosol dominated in pollution events under high-RH conditions, likely due to enhanced aqueous-phase chemistry, whereas primary organic aerosol dominated in pollution events under low-RH and stagnant conditions. Our results also highlighted the importance of meteorological conditions for PM pollution in this highly polluted city.
Anthoula D. Drosatou, Ksakousti Skyllakou, Georgia N. Theodoritsi, and Spyros N. Pandis
Atmos. Chem. Phys., 19, 973–986, https://doi.org/10.5194/acp-19-973-2019, https://doi.org/10.5194/acp-19-973-2019, 2019
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The ability of positive matrix factorization (PMF) factor analysis to identify and quantify the organic aerosol (OA) sources accurately is tested in this modeling study. The estimated uncertainty of the contribution of fresh biomass burning is less than 30 % and of the other primary sources is less than 40 %, when these sources contribute more than 20 % to the OA. Τhe first oxygenated OA factor includes mainly highly aged OA, while the second oxygenated OA factor contains fresher secondary OA.
Nivedita K. Kumar, Joel C. Corbin, Emily A. Bruns, Dario Massabó, Jay G. Slowik, Luka Drinovec, Griša Močnik, Paolo Prati, Athanasia Vlachou, Urs Baltensperger, Martin Gysel, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 17843–17861, https://doi.org/10.5194/acp-18-17843-2018, https://doi.org/10.5194/acp-18-17843-2018, 2018
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It is clear that considerable uncertainties still exist in understanding the magnitude of aerosol absorption on a global scale and its contribution to global warming. This manuscript provides a comprehensive assessment of the optical absorption by organic aerosols (brown carbon) from residential wood combustion as a function of atmospheric aging.
Ningxin Wang, Spiro D. Jorga, Jeffery R. Pierce, Neil M. Donahue, and Spyros N. Pandis
Atmos. Meas. Tech., 11, 6577–6588, https://doi.org/10.5194/amt-11-6577-2018, https://doi.org/10.5194/amt-11-6577-2018, 2018
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The interaction of particles with the chamber walls has been a significant source of uncertainty when analyzing results of secondary organic aerosol formation experiments performed in Teflon chambers. We evaluated the performance of several particle wall-loss correction methods for aging experiments of α-pinene ozonolysis products. Experimental procedures are proposed for the characterization of particle losses during different stages of these experiments.
Rita Van Dingenen, Frank Dentener, Monica Crippa, Joana Leitao, Elina Marmer, Shilpa Rao, Efisio Solazzo, and Luana Valentini
Atmos. Chem. Phys., 18, 16173–16211, https://doi.org/10.5194/acp-18-16173-2018, https://doi.org/10.5194/acp-18-16173-2018, 2018
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The evaluation of air pollution impacts, including on human health, vegetation, climate, and ecosystem health, is an essential component in the design of policies that affect air quality directly or indirectly. We have developed a tool that allows for a fast screening of relevant air pollution impacts from given emission scenarios at the regional to global scale, bypassing expensive numerical modelling of complex atmospheric processes. This paper provides a full documentation of the methodology.
Monica Crippa, Diego Guizzardi, Marilena Muntean, Edwin Schaaf, Frank Dentener, John A. van Aardenne, Suvi Monni, Ulrike Doering, Jos G. J. Olivier, Valerio Pagliari, and Greet Janssens-Maenhout
Earth Syst. Sci. Data, 10, 1987–2013, https://doi.org/10.5194/essd-10-1987-2018, https://doi.org/10.5194/essd-10-1987-2018, 2018
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EDGAR v4.3.2 is a global bottom-up emission inventory providing consistent anthropogenic emissions of gaseous and particulate air pollutants for 1970–2012 (with annual and monthly resolution) and grid maps with 0.1° × 0.1° resolution. We compare world regions using per capita and per GDP emissions, implied emissions per unit of energy, and emission ratios of co-emitted pollutants. We also show the growth of high-emitting areas (e.g. China, India) and the implications for global air quality.
Rocío Baró, Pedro Jiménez-Guerrero, Martin Stengel, Dominik Brunner, Gabriele Curci, Renate Forkel, Lucy Neal, Laura Palacios-Peña, Nicholas Savage, Martijn Schaap, Paolo Tuccella, Hugo Denier van der Gon, and Stefano Galmarini
Atmos. Chem. Phys., 18, 15183–15199, https://doi.org/10.5194/acp-18-15183-2018, https://doi.org/10.5194/acp-18-15183-2018, 2018
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Particles in the atmosphere, such as pollution, desert dust, and volcanic ash, have an impact on meteorology. They interact with incoming radiation resulting in a cooling effect of the atmosphere. Today, the use of meteorology and chemistry models help us to understand these processes, but there are a lot of uncertainties. The goal of this work is to evaluate how these interactions are represented in the models by comparing them to satellite data to see how close they are to reality.
Yingjie Zhang, Wei Du, Yuying Wang, Qingqing Wang, Haofei Wang, Haitao Zheng, Fang Zhang, Hongrong Shi, Yuxuan Bian, Yongxiang Han, Pingqing Fu, Francesco Canonaco, André S. H. Prévôt, Tong Zhu, Pucai Wang, Zhanqing Li, and Yele Sun
Atmos. Chem. Phys., 18, 14637–14651, https://doi.org/10.5194/acp-18-14637-2018, https://doi.org/10.5194/acp-18-14637-2018, 2018
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We have a comprehensive characterization of aerosol chemistry and particle growth events at a downwind site of a highly polluted city in the North China Plain. Aerosol particles at the urban downwind site were highly aged and mainly from secondary formation. New particle growth events were also frequently observed on both clean and polluted days. While both sulfate and SOA played important roles in particle growth during clean periods, SOA was more important than sulfate during polluted events.
David Patoulias, Christos Fountoukis, Ilona Riipinen, Ari Asmi, Markku Kulmala, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 13639–13654, https://doi.org/10.5194/acp-18-13639-2018, https://doi.org/10.5194/acp-18-13639-2018, 2018
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PMCAMx-UF, a 3-D chemical transport model focusing on the simulation of ultrafine particles, has been extended with the addition of the volatility basis set (VBS) approach for the simulation of organic aerosol. The model was applied in Europe and its predictions were evaluated against field observations collected during the PEGASOS 2012 campaign. The condensation of organics led to an increase (50–120 %) in the larger particles but the total number concentration decreased by 10–30 %.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Andrea Pozzer, Spyros N. Pandis, and Jos Lelieveld
Geosci. Model Dev., 11, 3369–3389, https://doi.org/10.5194/gmd-11-3369-2018, https://doi.org/10.5194/gmd-11-3369-2018, 2018
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A new module, ORACLE 2-D, that calculates the concentrations of surrogate organic species in two-dimensional space defined by volatility and oxygen-to-carbon ratio has been developed and evaluated. ORACLE 2-D uses a simple photochemical aging scheme that efficiently simulates the net effects of fragmentation and functionalization. ORACLE 2-D can be used to compute the ability of organic particles to act as cloud condensation nuclei and serves as a tool to quantify their climatic impact.
Xiao-Feng Huang, Bei-Bing Zou, Ling-Yan He, Min Hu, André S. H. Prévôt, and Yuan-Hang Zhang
Atmos. Chem. Phys., 18, 11563–11580, https://doi.org/10.5194/acp-18-11563-2018, https://doi.org/10.5194/acp-18-11563-2018, 2018
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A novel multilinear engine (ME-2) model was applied to the PM2.5 dataset observed in the Pearl River Delta (PRD) of China in 2015 and identified the sources of secondary sulfate (21 %), vehicle emissions (14 %), industrial emissions (13 %), secondary nitrate (11 %), biomass burning (11 %), secondary organic aerosol (7 %), coal burning (6 %), fugitive dust (5 %), ship emissions (3 %) and aged sea salt (2 %). The central PRD area was clearly identified as the key emission area in the PRD.
Antoon J. H. Visschedijk, Hugo A. C. Denier van der Gon, Hans C. Doornenbal, and Lorenzo Cremonese
Adv. Geosci., 45, 125–131, https://doi.org/10.5194/adgeo-45-125-2018, https://doi.org/10.5194/adgeo-45-125-2018, 2018
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Electricity produced by gas instead of coal is more climate-friendly as it emits 2 times less CO2 but with methane leakage rates > 3 % of production this advantage is lost. Ethane in (shale)gas can be used to identify gas leakage. The ratio of ethane/methane for European shale gas plays is derived and emission under different production and leakage scenarios is quantified. This can be used to design an atmospheric monitoring system that alerts competent authorities if unacceptable leakage occurs.
Amelie Bertrand, Giulia Stefenelli, Simone M. Pieber, Emily A. Bruns, Brice Temime-Roussel, Jay G. Slowik, Henri Wortham, André S. H. Prévôt, Imad El Haddad, and Nicolas Marchand
Atmos. Chem. Phys., 18, 10915–10930, https://doi.org/10.5194/acp-18-10915-2018, https://doi.org/10.5194/acp-18-10915-2018, 2018
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We model the evolution of several BBOA markers including levoglucosan during aging experiments conducted in an atmospheric Teflon chamber, in order to evaluate the influence of vapor wall loss on the determination of the rate constants of the compounds with hydroxyl radicals (OH).
Eleni Karnezi, Benjamin N. Murphy, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Florian Rubach, Astrid Kiendler-Scharr, Thomas F. Mentel, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 10759–10772, https://doi.org/10.5194/acp-18-10759-2018, https://doi.org/10.5194/acp-18-10759-2018, 2018
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Different parameterizations of the organic aerosol (OA) formation and evolution are evaluated using ground and airborne measurements collected in the 2012 PEGASOS field campaign in the Po Valley (Italy). Total OA concentration and O : C ratios were reproduced within experimental error by a number of schemes. Anthropogenic secondary OA (SOA) contributed 15–25 % of the total OA, 20–35 % of SOA from intermediate volatility compounds oxidation, and 15–45 % of biogenic SOA depending on the scheme.
Xia Li, Jiarui Wu, Miriam Elser, Tian Feng, Junji Cao, Imad El-Haddad, Rujin Huang, Xuexi Tie, André S. H. Prévôt, and Guohui Li
Atmos. Chem. Phys., 18, 10675–10691, https://doi.org/10.5194/acp-18-10675-2018, https://doi.org/10.5194/acp-18-10675-2018, 2018
Filippo Xausa, Pauli Paasonen, Risto Makkonen, Mikhail Arshinov, Aijun Ding, Hugo Denier Van Der Gon, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 18, 10039–10054, https://doi.org/10.5194/acp-18-10039-2018, https://doi.org/10.5194/acp-18-10039-2018, 2018
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Our project describes the feasibility of implementing particle number emissions taken from the GAINS model in global climate modeling through a simulation with the ECHAM-HAM global climate model. The results from the simulations have important implications regarding modeled particle number concentrations and future climate effects. Our findings represent an important starting point for further simulations concerning climate effects derived from anthropogenic particle emissions on a global scale.
Simone M. Pieber, Nivedita K. Kumar, Felix Klein, Pierre Comte, Deepika Bhattu, Josef Dommen, Emily A. Bruns, Doǧuşhan Kılıç, Imad El Haddad, Alejandro Keller, Jan Czerwinski, Norbert Heeb, Urs Baltensperger, Jay G. Slowik, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 9929–9954, https://doi.org/10.5194/acp-18-9929-2018, https://doi.org/10.5194/acp-18-9929-2018, 2018
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We studied primary emissions and secondary organic aerosol (SOA) from gasoline direct injection (GDI) vehicles including GDIs retrofitted with gasoline particle filters (GPF). GPF retrofitting significantly decreased the primary particulate matter, particularly through removal of refractory black carbon and, to a lesser extent, of non-refractory organic particulates. SOA experiments were conducted in a batch and flow reactor. GPF retrofitting did not significantly affect precursors or yields.
Emmanouil Oikonomakis, Sebnem Aksoyoglu, Martin Wild, Giancarlo Ciarelli, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Chem. Phys., 18, 9741–9765, https://doi.org/10.5194/acp-18-9741-2018, https://doi.org/10.5194/acp-18-9741-2018, 2018
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We report a model sensitivity study on the impact of aerosol–radiation interaction (ARI) changes in Europe between 1990 and 2010 on summer surface ozone via effects on photolysis rates and biogenic emissions. The overall impact of ARI changes on ozone was relatively small when compared to the total ozone concentrations, but it was more important when compared to the order of magnitude of ozone trends, indicating a potential partial damping of the effects of ozone precursor emissions' reduction.
Yele Sun, Weiqi Xu, Qi Zhang, Qi Jiang, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Jie Li, John Jayne, Douglas R. Worsnop, and Zifa Wang
Atmos. Chem. Phys., 18, 8469–8489, https://doi.org/10.5194/acp-18-8469-2018, https://doi.org/10.5194/acp-18-8469-2018, 2018
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We present a 2–year analysis of organic aerosol (OA) from highly time–resolved measurements by an aerosol chemical speciation monitor in the megacity of Beijing. The sources of OA were analyzed with the advanced factor analysis of a multilinear engine (ME-2). Our results showed very different seasonal patterns, relative humidity and temperature dependence, and sources regions among different OA factors. The sources and processes of OA factors, and their roles in haze pollution are elucidated.
Amelie Bertrand, Giulia Stefenelli, Coty N. Jen, Simone M. Pieber, Emily A. Bruns, Haiyan Ni, Brice Temime-Roussel, Jay G. Slowik, Allen H. Goldstein, Imad El Haddad, Urs Baltensperger, André S. H. Prévôt, Henri Wortham, and Nicolas Marchand
Atmos. Chem. Phys., 18, 7607–7624, https://doi.org/10.5194/acp-18-7607-2018, https://doi.org/10.5194/acp-18-7607-2018, 2018
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A thermal desorption aerosol gas chromatograph coupled to an aerosol mass spectrometer (TAG–AMS) is connected to an atmospheric chamber. The setup serves the quantitative study of the impact of combustion conditions and atmospheric aging on the chemical fingerprint at the molecular level of biomass burning organic aerosol.
Doğuşhan Kılıç, Imad El Haddad, Benjamin T. Brem, Emily Bruns, Carlo Bozetti, Joel Corbin, Lukas Durdina, Ru-Jin Huang, Jianhui Jiang, Felix Klein, Avi Lavi, Simone M. Pieber, Theo Rindlisbacher, Yinon Rudich, Jay G. Slowik, Jing Wang, Urs Baltensperger, and Andre S. H. Prévôt
Atmos. Chem. Phys., 18, 7379–7391, https://doi.org/10.5194/acp-18-7379-2018, https://doi.org/10.5194/acp-18-7379-2018, 2018
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We study primary emissions and secondary aerosol (SA) from an aircraft turbofan. By monitoring the chemical composition of both gaseous and particulate emissions at different engine loads, we explained SA formed in an oxidation flow reactor (PAM) by the oxidation of gaseous species. At idle, more than 90 % of the secondary particle mass was organic and could be explained by the oxidation of gaseous aromatic species, while at an approximated cruise load sulfates comprised 85 % of the total SA.
Arineh Cholakian, Matthias Beekmann, Augustin Colette, Isabelle Coll, Guillaume Siour, Jean Sciare, Nicolas Marchand, Florian Couvidat, Jorge Pey, Valerie Gros, Stéphane Sauvage, Vincent Michoud, Karine Sellegri, Aurélie Colomb, Karine Sartelet, Helen Langley DeWitt, Miriam Elser, André S. H. Prévot, Sonke Szidat, and François Dulac
Atmos. Chem. Phys., 18, 7287–7312, https://doi.org/10.5194/acp-18-7287-2018, https://doi.org/10.5194/acp-18-7287-2018, 2018
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In this work, four schemes for the simulation of organic aerosols in the western Mediterranean basin are added to the CHIMERE chemistry–transport model; the resulting simulations are then compared to measurements obtained from ChArMEx. It is concluded that the scheme taking into account the fragmentation and the formation of nonvolatile organic aerosols corresponds better to measurements; the major source of this aerosol in the western Mediterranean is found to be of biogenic origin.
Jun Zhou, Peter Zotter, Emily A. Bruns, Giulia Stefenelli, Deepika Bhattu, Samuel Brown, Amelie Bertrand, Nicolas Marchand, Houssni Lamkaddam, Jay G. Slowik, André S. H. Prévôt, Urs Baltensperger, Thomas Nussbaumer, Imad El-Haddad, and Josef Dommen
Atmos. Chem. Phys., 18, 6985–7000, https://doi.org/10.5194/acp-18-6985-2018, https://doi.org/10.5194/acp-18-6985-2018, 2018
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We thoroughly studied the reactive oxygen species (ROS) generation potential of particulate wood combustion emissions, from different combustion technologies, fuel types, operation methods, combustion regimes and phases. ROS from automatically operated combustion devices under optimal conditions were much lower than those from manually operated appliances. We examined the impact of atmospheric aging on ROS content in SOA and determined the controlling parameters, by using an online ROS analyzer.
Athanasia Vlachou, Kaspar R. Daellenbach, Carlo Bozzetti, Benjamin Chazeau, Gary A. Salazar, Soenke Szidat, Jean-Luc Jaffrezo, Christoph Hueglin, Urs Baltensperger, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 6187–6206, https://doi.org/10.5194/acp-18-6187-2018, https://doi.org/10.5194/acp-18-6187-2018, 2018
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Carbonaceous aerosols are related to adverse human health effects, which depend on the aerosol chemical composition and size. Here, we combine aerosol mass spectrometry and radiocarbon measurements of size-resolved samples collected over a long term to identify the origins of primary and secondary carbonaceous aerosols in the fine and coarse modes.
Evangelia Kostenidou, Eleni Karnezi, James R. Hite Jr., Aikaterini Bougiatioti, Kate Cerully, Lu Xu, Nga L. Ng, Athanasios Nenes, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 5799–5819, https://doi.org/10.5194/acp-18-5799-2018, https://doi.org/10.5194/acp-18-5799-2018, 2018
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The volatility distribution of organic aerosol (OA) and its sources during the Southern Oxidant and Aerosol Study (SOAS) was estimated. The volatility distribution of all components covered a wide range including both semi-volatile and low-volatility components. The oxygen content of the factors can be combined with their estimated volatility and hygroscopicity to provide a better view of their physical properties.
Yan-Lin Zhang, Imad El-Haddad, Ru-Jin Huang, Kin-Fai Ho, Jun-Ji Cao, Yongming Han, Peter Zotter, Carlo Bozzetti, Kaspar R. Daellenbach, Jay G. Slowik, Gary Salazar, André S. H. Prévôt, and Sönke Szidat
Atmos. Chem. Phys., 18, 4005–4017, https://doi.org/10.5194/acp-18-4005-2018, https://doi.org/10.5194/acp-18-4005-2018, 2018
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Here we present a quantitative source apportionment of WSOC, isolated from aerosols in China using radiocarbon (14C) and offline high-resolution time of flight aerosol mass spectrometer measurements. We demonstrate a dominant contribution of non-fossil emissions to WSOC aerosols in the Northern Hemisphere. However, the fossil fraction is substantially larger in aerosols from East Asia and the east Asian pollution outflow, especially during winter, due to increasing coal combustion.
Wei Zhou, Qingqing Wang, Xiujuan Zhao, Weiqi Xu, Chen Chen, Wei Du, Jian Zhao, Francesco Canonaco, André S. H. Prévôt, Pingqing Fu, Zifa Wang, Douglas R. Worsnop, and Yele Sun
Atmos. Chem. Phys., 18, 3951–3968, https://doi.org/10.5194/acp-18-3951-2018, https://doi.org/10.5194/acp-18-3951-2018, 2018
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We present a 3-month analysis of submicron aerosols that were measured at 260 m on a meteorological tower in Beijing, China. The sources of organic aerosol (OA) were analyzed by using a multi-linear engine (ME-2). Our results showed significant changes in both primary and secondary OA composition from the non-heating season to the heating season. We also observed a considerable contribution (10–13%) of cooking OA at 260 m and very different OA composition between ground level and 260 m.
Ningxin Wang, Evangelia Kostenidou, Neil M. Donahue, and Spyros N. Pandis
Atmos. Chem. Phys., 18, 3589–3601, https://doi.org/10.5194/acp-18-3589-2018, https://doi.org/10.5194/acp-18-3589-2018, 2018
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This study investigates aging in the α-pinene ozonolysis system with hydroxyl radicals (OH) through smog chamber experiments. After an equivalent of 2–4 days of typical atmospheric oxidation conditions, homogeneous OH oxidation of the α-pinene ozonolysis products resulted in a 20–40 % net increase in the organic aerosol concentration and an increase in aerosol O : C by up to 0.04. The relative humidity in the 5–50 % range had a minimum effect on aging.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
Qiao Zhu, Xiao-Feng Huang, Li-Ming Cao, Lin-Tong Wei, Bin Zhang, Ling-Yan He, Miriam Elser, Francesco Canonaco, Jay G. Slowik, Carlo Bozzetti, Imad El-Haddad, and André S. H. Prévôt
Atmos. Meas. Tech., 11, 1049–1060, https://doi.org/10.5194/amt-11-1049-2018, https://doi.org/10.5194/amt-11-1049-2018, 2018
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Organic aerosol constitutes one of the major components of atmospheric particulate matter globally and is emitted from various sources. Therefore, identifying and quantifying the sources of organic aerosol accurately is a key task in the field. In this study, we applied a rather novel procedure for an improved source apportionment method (ME-2) to resolve the
less meaningful or mixed factorsproblems for organic aerosol using the traditional method (PMF).
Kaspar R. Daellenbach, Imad El-Haddad, Lassi Karvonen, Athanasia Vlachou, Joel C. Corbin, Jay G. Slowik, Maarten F. Heringa, Emily A. Bruns, Samuel M. Luedin, Jean-Luc Jaffrezo, Sönke Szidat, Andrea Piazzalunga, Raquel Gonzalez, Paola Fermo, Valentin Pflueger, Guido Vogel, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 18, 2155–2174, https://doi.org/10.5194/acp-18-2155-2018, https://doi.org/10.5194/acp-18-2155-2018, 2018
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A novel offline LDI-MS method was developed to analyse particulate matter (PM) collected at multiple sites in central Europe during the entire year of 2013. PM sources were identified by positive matrix factorization. Wood burning emissions were separated according to the burning conditions; inefficient burns had a larger impact on air quality in southern Alpine valleys than in northern Switzerland. Moreover, primary tailpipe exhaust was distinguished from aged/secondary traffic emissions.
Emmanouil Oikonomakis, Sebnem Aksoyoglu, Giancarlo Ciarelli, Urs Baltensperger, and André Stephan Henry Prévôt
Atmos. Chem. Phys., 18, 2175–2198, https://doi.org/10.5194/acp-18-2175-2018, https://doi.org/10.5194/acp-18-2175-2018, 2018
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We report a modeling study investigating the uncertainties in ozone production in Europe. Using various methods for different emission and meteorological scenarios, we searched for the possible reasons for underestimation of high ozone levels in Europe by models. Our results suggest that emissions, especially NOx, might be too low in the European inventories. Improvement of the modeled ozone production will contribute to more consistent and effective ozone mitigation strategies for the future.
Jun Zhou, Emily A. Bruns, Peter Zotter, Giulia Stefenelli, André S. H. Prévôt, Urs Baltensperger, Imad El-Haddad, and Josef Dommen
Atmos. Meas. Tech., 11, 65–80, https://doi.org/10.5194/amt-11-65-2018, https://doi.org/10.5194/amt-11-65-2018, 2018
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Reactive oxygen species (ROS) in the particle phase may induce oxidative stress in the human lungs upon inhalation. Here we present and thoroughly characterize a modified online and offline ROS analyzer. Selected model organic compounds were tested and potential interferences from gas-phase and matrix effects of particulate constituents were evaluated. ROS measurements of filter samples revealed the rapid decay of a substantial ROS fraction, supporting the application of online measurements.
Kerrigan P. Cain and Spyros N. Pandis
Atmos. Meas. Tech., 10, 4865–4876, https://doi.org/10.5194/amt-10-4865-2017, https://doi.org/10.5194/amt-10-4865-2017, 2017
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Hygroscopicity, oxidation level, and volatility of organic pollutants are three crucial properties that determine their fate in the atmosphere. This study assesses the feasibility of a novel measurement and analysis technique to determine these properties of organic aerosol
components at the same time and to establish their relationship.
Naifang Bei, Jiarui Wu, Miriam Elser, Tian Feng, Junji Cao, Imad El-Haddad, Xia Li, Rujin Huang, Zhengqiang Li, Xin Long, Li Xing, Shuyu Zhao, Xuexi Tie, André S. H. Prévôt, and Guohui Li
Atmos. Chem. Phys., 17, 14579–14591, https://doi.org/10.5194/acp-17-14579-2017, https://doi.org/10.5194/acp-17-14579-2017, 2017
Yunjiang Zhang, Lili Tang, Philip L. Croteau, Olivier Favez, Yele Sun, Manjula R. Canagaratna, Zhuang Wang, Florian Couvidat, Alexandre Albinet, Hongliang Zhang, Jean Sciare, André S. H. Prévôt, John T. Jayne, and Douglas R. Worsnop
Atmos. Chem. Phys., 17, 14501–14517, https://doi.org/10.5194/acp-17-14501-2017, https://doi.org/10.5194/acp-17-14501-2017, 2017
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We conducted the first field measurements of non-refractory fine aerosols (NR-PM2.5) in a megacity of eastern China using a PM2.5-ACSM along with a PM1-ACSM measurement. Inter-comparisons demonstrated that the NR-PM2.5 components can be characterized. Substantial mass fractions of aerosol species were observed in the size range of 1–2.5 μm, with sulfate and SOA being the two largest contributors. The impacts of aerosol water driven by secondary inorganic aerosols on SOA formation were explored.
Hugo A. C. Denier van der Gon, Jeroen J. P. Kuenen, Greet Janssens-Maenhout, Ulrike Döring, Sander Jonkers, and Antoon Visschedijk
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2017-124, https://doi.org/10.5194/essd-2017-124, 2017
Revised manuscript has not been submitted
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A gridded European emission inventory for CO2 from fossil fuels and biofuels (2000–2014) is made to support carbon cycle modelling and city-scale identification of emissions. Future projections following a “business as usual” and a climate change scenario are included to study possible CO2 emission changes between Paris Agreement stocktake years (2023-2028-2033). The data can be used for testing GHG verification modelling and sensitivity tests for designing a future observational system.
Astrid M. M. Manders, Peter J. H. Builtjes, Lyana Curier, Hugo A. C. Denier van der Gon, Carlijn Hendriks, Sander Jonkers, Richard Kranenburg, Jeroen J. P. Kuenen, Arjo J. Segers, Renske M. A. Timmermans, Antoon J. H. Visschedijk, Roy J. Wichink Kruit, W. Addo J. van Pul, Ferd J. Sauter, Eric van der Swaluw, Daan P. J. Swart, John Douros, Henk Eskes, Erik van Meijgaard, Bert van Ulft, Peter van Velthoven, Sabine Banzhaf, Andrea C. Mues, Rainer Stern, Guangliang Fu, Sha Lu, Arnold Heemink, Nils van Velzen, and Martijn Schaap
Geosci. Model Dev., 10, 4145–4173, https://doi.org/10.5194/gmd-10-4145-2017, https://doi.org/10.5194/gmd-10-4145-2017, 2017
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The regional-scale air quality model LOTOS–EUROS has been developed by a consortium of Dutch institutes. Recently, version 2.0 of the model was released as an open-source version. Next to a technical description and model evaluation for 2012, this paper presents the model developments in context of the history of air quality modelling and provides an outlook for future directions. Key and innovative applications of LOTOS–EUROS are also highlighted.
Ingrid Super, Hugo A. C. Denier van der Gon, Michiel K. van der Molen, Hendrika A. M. Sterk, Arjan Hensen, and Wouter Peters
Atmos. Chem. Phys., 17, 13297–13316, https://doi.org/10.5194/acp-17-13297-2017, https://doi.org/10.5194/acp-17-13297-2017, 2017
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In this research we examined the use of different models to simulate CO2 concentrations in and around urban areas. We find that in the presence of large stack emissions in a gridded model is insufficient to represent the small dimensions of the CO2 plumes. A plume model improves this representation up to 10–14 km from the stack. Better model results can improve the estimate of CO2 emissions from urban areas and assist in identifying efficient emission reduction policies.
Kaspar R. Daellenbach, Giulia Stefenelli, Carlo Bozzetti, Athanasia Vlachou, Paola Fermo, Raquel Gonzalez, Andrea Piazzalunga, Cristina Colombi, Francesco Canonaco, Christoph Hueglin, Anne Kasper-Giebl, Jean-Luc Jaffrezo, Federico Bianchi, Jay G. Slowik, Urs Baltensperger, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 13265–13282, https://doi.org/10.5194/acp-17-13265-2017, https://doi.org/10.5194/acp-17-13265-2017, 2017
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We present offline AMS analyses for the organic aerosol (OA) in PM10 at nine sites in central Europe for 2013. Primary OA is separated into traffic, cooking, and wood-burning components. A factor explaining sulfur-containing ions, with an event-driven time series, is also separated. We observe enhanced production of secondary OA (SOA) in summer, following biogenic emissions with temperature. In winter a SOA component is dominant, which correlates with anthropogenic inorganic species.
Evangelos E. Louvaris, Eleni Karnezi, Evangelia Kostenidou, Christos Kaltsonoudis, and Spyros N. Pandis
Atmos. Meas. Tech., 10, 3909–3918, https://doi.org/10.5194/amt-10-3909-2017, https://doi.org/10.5194/amt-10-3909-2017, 2017
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A method for the determination of the organic aerosol volatility distribution combining thermodenuder and isothermal dilution measurements is developed. The approach was tested in experiments that were conducted in a smog chamber using organic aerosol produced during meat charbroiling. Addition of the dilution measurements to the thermodenuder data results in a lower uncertainty of the estimated vaporization enthalpy as well as the semivolatile content of the aerosol.
Vitali Fioletov, Chris A. McLinden, Shailesh K. Kharol, Nickolay A. Krotkov, Can Li, Joanna Joiner, Michael D. Moran, Robert Vet, Antoon J. H. Visschedijk, and Hugo A. C. Denier van der Gon
Atmos. Chem. Phys., 17, 12597–12616, https://doi.org/10.5194/acp-17-12597-2017, https://doi.org/10.5194/acp-17-12597-2017, 2017
Laura-Hélèna Rivellini, Isabelle Chiapello, Emmanuel Tison, Marc Fourmentin, Anaïs Féron, Aboubacry Diallo, Thierno N'Diaye, Philippe Goloub, Francesco Canonaco, André Stephan Henry Prévôt, and Véronique Riffault
Atmos. Chem. Phys., 17, 10291–10314, https://doi.org/10.5194/acp-17-10291-2017, https://doi.org/10.5194/acp-17-10291-2017, 2017
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A 3-month field campaign was conducted in March–June 2015 in Senegal, as part of the SHADOW (SaHAran Dust Over West Africa) project. This article presents the time variability of the chemical composition of submicron particles. Organics (sulfates) were predominant for days under continental (marine) influence. Half the organic sources were identified as local, including one due to open waste-burning, and half were linked to regional air masses and enhanced photochemical processes.
Yi Ming Qin, Hao Bo Tan, Yong Jie Li, Misha I. Schurman, Fei Li, Francesco Canonaco, André S. H. Prévôt, and Chak K. Chan
Atmos. Chem. Phys., 17, 10245–10258, https://doi.org/10.5194/acp-17-10245-2017, https://doi.org/10.5194/acp-17-10245-2017, 2017
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Freshly emitted HOA contributed significantly to the high concentrations of organics at night as heavy-duty vehicles enter downtown Guangzhou, while SOA contributed to the daytime high concentration. The large input of NOx, from automobile emissions, resulted in the significant formation of nitrate in both daytime and nighttime. Mitigating the PM pollution in urbanized areas such as Guangzhou can potentially benefit their peripheral cities, by reductions in traffic-related pollutants.
Greet Janssens-Maenhout, Monica Crippa, Diego Guizzardi, Marilena Muntean, Edwin Schaaf, Frank Dentener, Peter Bergamaschi, Valerio Pagliari, Jos G. J. Olivier, Jeroen A. H. W. Peters, John A. van Aardenne, Suvi Monni, Ulrike Doering, and A. M. Roxana Petrescu
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2017-79, https://doi.org/10.5194/essd-2017-79, 2017
Revised manuscript not accepted
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The Emissions Database for Global Atmospheric Research supports climate policy making with a global dataset at disaggregated country & source-sector level for 1970–2012. This dataset is not only unique in its space/time coverage, but also in its completeness & consistency of CO2, CH4 & N2O emissions compilation for all anthropogenic activities except land use. Comparison with UNFCCC values show that estimates are within the uncertainty range, but have an annual variation smaller than this range.
Prettiny K. Ma, Yunliang Zhao, Allen L. Robinson, David R. Worton, Allen H. Goldstein, Amber M. Ortega, Jose L. Jimenez, Peter Zotter, André S. H. Prévôt, Sönke Szidat, and Patrick L. Hayes
Atmos. Chem. Phys., 17, 9237–9259, https://doi.org/10.5194/acp-17-9237-2017, https://doi.org/10.5194/acp-17-9237-2017, 2017
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Airborne particulate matter (PM) negatively impacts air quality in cities throughout the world. An important fraction of PM is organic aerosol. We have evaluated and developed several new models for secondary organic aerosol (SOA), which is formed from the chemical processing of gaseous precursors. Using our model results, we have quantified important SOA sources and precursors and also identified possible model parameterizations that could be used for air quality predictions.
Carlo Bozzetti, Imad El Haddad, Dalia Salameh, Kaspar Rudolf Daellenbach, Paola Fermo, Raquel Gonzalez, María Cruz Minguillón, Yoshiteru Iinuma, Laurent Poulain, Miriam Elser, Emanuel Müller, Jay Gates Slowik, Jean-Luc Jaffrezo, Urs Baltensperger, Nicolas Marchand, and André Stephan Henry Prévôt
Atmos. Chem. Phys., 17, 8247–8268, https://doi.org/10.5194/acp-17-8247-2017, https://doi.org/10.5194/acp-17-8247-2017, 2017
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We present the first long-term organic aerosol source apportionment in an environment influenced by anthropogenic emissions including biomass burning and industrial processes and an active photochemistry. Online and offline aerosol mass spectrometry were used to characterize these emissions and their transformation. Measurements of organic markers provided insights into the origin of biomass smoke in this area, with different seasonal contributions from domestic heating and agricultural burning.
Reza Shaiganfar, Steffen Beirle, Hugo Denier van der Gon, Sander Jonkers, Jeroen Kuenen, Herve Petetin, Qijie Zhang, Matthias Beekmann, and Thomas Wagner
Atmos. Chem. Phys., 17, 7853–7890, https://doi.org/10.5194/acp-17-7853-2017, https://doi.org/10.5194/acp-17-7853-2017, 2017
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We determine NOx emissions for Paris in summer 2009 and winter 2009/2010 by combining car MAX-DOAS measurements of NO2 with wind fields. We compare the results with simulations from the CHIMERE model. We derive daily average NOx emissions for Paris of 4.0 × 1025 molecules s−1 for summer and of 6.9 × 1025 molecules s−1 in winter. These values are a factor of about 1.4 and 2.0 larger than the corresponding emissions in the MACC-III emission inventory.
Sebnem Aksoyoglu, Giancarlo Ciarelli, Imad El-Haddad, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 7757–7773, https://doi.org/10.5194/acp-17-7757-2017, https://doi.org/10.5194/acp-17-7757-2017, 2017
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Sources of inorganic aerosols in Europe were investigated using a regional air quality model. Results of this study suggested that biogenic volatile organic coumpounds emitted from vegetation had a significant effect on inorganic aerosols, especially on ammonium nitrate concentrations. Sensitivity analyses showed that it is mainly terpene reactions with nitrate radical at night that lead to a decrease in ammonium nitrate.
Ganlin Huang, Rosie Brook, Monica Crippa, Greet Janssens-Maenhout, Christian Schieberle, Chris Dore, Diego Guizzardi, Marilena Muntean, Edwin Schaaf, and Rainer Friedrich
Atmos. Chem. Phys., 17, 7683–7701, https://doi.org/10.5194/acp-17-7683-2017, https://doi.org/10.5194/acp-17-7683-2017, 2017
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In this study, a global speciated non-methane volatile organic compound (NMVOC) emission data set is developed by compiling and allocating region- and source-specific speciation profiles, i.e. distributions of NMVOC species, to the revised and extended Emissions Database for Global Atmospheric Research emission inventory, which can serve as input data for chemical transport models and health impact assessments. Species time series and high-resolution global grid maps for 1970–2012 are produced.
Giancarlo Ciarelli, Imad El Haddad, Emily Bruns, Sebnem Aksoyoglu, Ottmar Möhler, Urs Baltensperger, and André S. H. Prévôt
Geosci. Model Dev., 10, 2303–2320, https://doi.org/10.5194/gmd-10-2303-2017, https://doi.org/10.5194/gmd-10-2303-2017, 2017
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In Europe, residential wood-burning emissions constitute one of the main anthropogenic sources of air pollution. Novel wood-burning experiments performed in a state-of-the-art smog chamber provide valuable information on the chemical properties of wood-burning emissions and the transformation in the atmosphere. In this study, these new data were used in a box model to constrain a parameterization suitable for predicting the contribution of wood burning to air pollution with large-scale models.
Giancarlo Ciarelli, Sebnem Aksoyoglu, Imad El Haddad, Emily A. Bruns, Monica Crippa, Laurent Poulain, Mikko Äijälä, Samara Carbone, Evelyn Freney, Colin O'Dowd, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 7653–7669, https://doi.org/10.5194/acp-17-7653-2017, https://doi.org/10.5194/acp-17-7653-2017, 2017
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Organic aerosol (OA) comprises the main fraction of fine particulate matter (PM1). Using a new VBS parameterization, we performed model-based source apportionment studies to assess the importance of different emission sources to the total OA loads in Europe during winter periods. Our results indicate that residential wood burning emissions represent the major source of OA, followed by non-residential emission sources (i.e. traffic and industries).
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 17, 7345–7364, https://doi.org/10.5194/acp-17-7345-2017, https://doi.org/10.5194/acp-17-7345-2017, 2017
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We analyzed the sensitivity of model-predicted global-scale OA to parameters and assumptions that control primary emissions, photochemical aging, and the scavenging efficiency of LVOCs, SVOCs, and IVOCs. The simulated OA concentrations were evaluated against a global dataset of AMS measurements. According to our analysis, a combination of increased IVOCs and decreased hygroscopicity of the freshly emitted IVOCs can help reduce discrepancies between simulated SOA and observed OOA concentrations.
Christos Kaltsonoudis, Evangelia Kostenidou, Evangelos Louvaris, Magda Psichoudaki, Epameinondas Tsiligiannis, Kalliopi Florou, Aikaterini Liangou, and Spyros N. Pandis
Atmos. Chem. Phys., 17, 7143–7155, https://doi.org/10.5194/acp-17-7143-2017, https://doi.org/10.5194/acp-17-7143-2017, 2017
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Cooking emissions can be a significant source of particulate matter in urban areas. In this study the aerosol- and gas-phase emissions from meat charbroiling were characterized. More than 99% of the aerosol emitted was composed of organic compounds. The fresh particles were similar to the cooking organic aerosol over Greek cities during the winter, while the reacted particles were similar to those found in the atmosphere during the summer.
Markus Furger, María Cruz Minguillón, Varun Yadav, Jay G. Slowik, Christoph Hüglin, Roman Fröhlich, Krag Petterson, Urs Baltensperger, and André S. H. Prévôt
Atmos. Meas. Tech., 10, 2061–2076, https://doi.org/10.5194/amt-10-2061-2017, https://doi.org/10.5194/amt-10-2061-2017, 2017
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An Xact 625 Ambient Metals Monitor was tested during a 3-week summer field campaign at a rural, traffic-influenced site in Switzerland. The objective was to characterize the operation of the instrument, evaluate the data quality by intercomparison with other independent measurements, and test its applicability for aerosol source quantification. The results demonstrate significant advantages compared to traditional elemental analysis methods, with some desirable improvements.
Johannes R. W. Fachinger, Stéphane J. Gallavardin, Frank Helleis, Friederike Fachinger, Frank Drewnick, and Stephan Borrmann
Atmos. Meas. Tech., 10, 1623–1637, https://doi.org/10.5194/amt-10-1623-2017, https://doi.org/10.5194/amt-10-1623-2017, 2017
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The design of an ion trap aerosol mass spectrometer was improved, allowing for the instrument's first field deployment. Detection limits were found to be sufficiently low for ambient measurements. Via MS-MS measurements the instrument is capable of differentiating ion fragments of different elemental compositions, but also fragments which only differ in their molecular structures. This could allow for e.g. the differentiation between sugars and carboxylic acids by MS–MS studies on m/z 60 and 73.
Lisa Stirnweis, Claudia Marcolli, Josef Dommen, Peter Barmet, Carla Frege, Stephen M. Platt, Emily A. Bruns, Manuel Krapf, Jay G. Slowik, Robert Wolf, Andre S. H. Prévôt, Urs Baltensperger, and Imad El-Haddad
Atmos. Chem. Phys., 17, 5035–5061, https://doi.org/10.5194/acp-17-5035-2017, https://doi.org/10.5194/acp-17-5035-2017, 2017
Haiyan Li, Qi Zhang, Qiang Zhang, Chunrong Chen, Litao Wang, Zhe Wei, Shan Zhou, Caroline Parworth, Bo Zheng, Francesco Canonaco, André S. H. Prévôt, Ping Chen, Hongliang Zhang, Timothy J. Wallington, and Kebin He
Atmos. Chem. Phys., 17, 4751–4768, https://doi.org/10.5194/acp-17-4751-2017, https://doi.org/10.5194/acp-17-4751-2017, 2017
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The sources and aerosol evolution processes of severe pollution episodes were investigated in Handan during wintertime using real-time measurements. An in-depth analysis of the data uncovered that primary emissions from coal combustion and biomass burning together with secondary formation of sulfate (mainly from SO2 emitted by coal combustion) are important driving factors for haze evolution. Our findings provide useful insights into air pollution control in heavily polluted regions.
Peter Zotter, Hanna Herich, Martin Gysel, Imad El-Haddad, Yanlin Zhang, Griša Močnik, Christoph Hüglin, Urs Baltensperger, Sönke Szidat, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 4229–4249, https://doi.org/10.5194/acp-17-4229-2017, https://doi.org/10.5194/acp-17-4229-2017, 2017
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Most studies use a single Ångström exponent for wood burning (αWB) and traffic (αTR) emissions in the Aethalometer model, used for source apportionment of black carbon, derived from previous work. However, accurate determination of the α values is currently lacking. Comparing radiocarbon measurements (14C) with the Aehtalometer model, good agreement was found, indicating that the Aethalometer model reproduces reasonably well the 14C results using our best estimate of a single αWB and αTR.
Luka Drinovec, Asta Gregorič, Peter Zotter, Robert Wolf, Emily Anne Bruns, André S. H. Prévôt, Jean-Eudes Petit, Olivier Favez, Jean Sciare, Ian J. Arnold, Rajan K. Chakrabarty, Hans Moosmüller, Agnes Filep, and Griša Močnik
Atmos. Meas. Tech., 10, 1043–1059, https://doi.org/10.5194/amt-10-1043-2017, https://doi.org/10.5194/amt-10-1043-2017, 2017
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Black carbon measurements are usually conducted with absorption filter photometers, which are prone to the filter-loading effect – a saturation of the instrumental response due to the accumulation of the sample in the filter matrix. In this paper, we conducted several field campaigns to investigate the hypothesis that this filter-loading effect depends on the optical properties of particles present in the filter matrix, especially on the coating of black carbon particles.
Mikko Äijälä, Liine Heikkinen, Roman Fröhlich, Francesco Canonaco, André S. H. Prévôt, Heikki Junninen, Tuukka Petäjä, Markku Kulmala, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 17, 3165–3197, https://doi.org/10.5194/acp-17-3165-2017, https://doi.org/10.5194/acp-17-3165-2017, 2017
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Mass spectrometric measurements commonly yield data on hundreds of variables over thousands of points in time. Refining and synthesising this “raw” data into chemical information necessitates the use of advanced, statistics-based data analysis techniques. Here we present an example of combining data dimensionality reduction (factorisation) with exploratory classification (clustering) and show that the results complement and broaden our current perspectives on aerosol chemical classification.
Kalliopi Florou, Dimitrios K. Papanastasiou, Michael Pikridas, Christos Kaltsonoudis, Evangelos Louvaris, Georgios I. Gkatzelis, David Patoulias, Nikolaos Mihalopoulos, and Spyros N. Pandis
Atmos. Chem. Phys., 17, 3145–3163, https://doi.org/10.5194/acp-17-3145-2017, https://doi.org/10.5194/acp-17-3145-2017, 2017
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The composition of fine particulate matter (PM) in two major Greek cities (Athens and Patras) was measured during two wintertime campaigns in 2012 and 2013. Residential wood burning has dramatically increased due to the Greek financial crisis, contributing around 50 % of the fine PM on average and more than 80 % during nighttime. Cooking is also an important source during both midday and evening, while transportation dominates only during the morning rush hour.
Emily A. Bruns, Jay G. Slowik, Imad El Haddad, Dogushan Kilic, Felix Klein, Josef Dommen, Brice Temime-Roussel, Nicolas Marchand, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 705–720, https://doi.org/10.5194/acp-17-705-2017, https://doi.org/10.5194/acp-17-705-2017, 2017
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We characterize primary and aged gaseous emissions from residential wood combustion using proton transfer reaction time-of-flight mass spectrometry. This approach allows for improved characterization, particularly of oxygenated gases, which are a considerable fraction of the total gaseous mass emitted during residential wood combustion. This study is the first thorough characterization of organic gases from this source and provides a benchmark for future studies.
Carlo Bozzetti, Yuliya Sosedova, Mao Xiao, Kaspar R. Daellenbach, Vidmantas Ulevicius, Vadimas Dudoitis, Genrik Mordas, Steigvilė Byčenkienė, Kristina Plauškaitė, Athanasia Vlachou, Benjamin Golly, Benjamin Chazeau, Jean-Luc Besombes, Urs Baltensperger, Jean-Luc Jaffrezo, Jay G. Slowik, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 117–141, https://doi.org/10.5194/acp-17-117-2017, https://doi.org/10.5194/acp-17-117-2017, 2017
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In this study we present the offline-AMS source apportionment of the submicron organic aerosol (OA) sources conducted over 1 year at three locations in the south east Baltic region, which has so far received small attention. Offline-AMS enabled broadening the AMS spatial and temporal coverage, and provided a full characterization of the OA sources. Source apportionment results revealed that biomass burning and biogenic secondary emissions were the major OA sources during winter and summer.
Ioannis Kioutsioukis, Ulas Im, Efisio Solazzo, Roberto Bianconi, Alba Badia, Alessandra Balzarini, Rocío Baró, Roberto Bellasio, Dominik Brunner, Charles Chemel, Gabriele Curci, Hugo Denier van der Gon, Johannes Flemming, Renate Forkel, Lea Giordano, Pedro Jiménez-Guerrero, Marcus Hirtl, Oriol Jorba, Astrid Manders-Groot, Lucy Neal, Juan L. Pérez, Guidio Pirovano, Roberto San Jose, Nicholas Savage, Wolfram Schroder, Ranjeet S. Sokhi, Dimiter Syrakov, Paolo Tuccella, Johannes Werhahn, Ralf Wolke, Christian Hogrefe, and Stefano Galmarini
Atmos. Chem. Phys., 16, 15629–15652, https://doi.org/10.5194/acp-16-15629-2016, https://doi.org/10.5194/acp-16-15629-2016, 2016
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Four ensemble methods are applied to two annual AQMEII datasets and their performance is compared for O3, NO2 and PM10. The goal of the study is to quantify to what extent we can extract predictable signals from an ensemble with superior skill at each station over the single models and the ensemble mean. The promotion of the right amount of accuracy and diversity within the ensemble results in an average additional skill of up to 31 % compared to using the full ensemble in an unconditional way.
Ernesto Reyes-Villegas, David C. Green, Max Priestman, Francesco Canonaco, Hugh Coe, André S. H. Prévôt, and James D. Allan
Atmos. Chem. Phys., 16, 15545–15559, https://doi.org/10.5194/acp-16-15545-2016, https://doi.org/10.5194/acp-16-15545-2016, 2016
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For the first time in the UK, an Aerosol Chemical Speciation Monitor was used to measure aerosol concentrations in London in March–December 2013, with further organic aerosol (OA) source apportionment using the ME-2 factorization tool. Five OA sources were identified: biomass burning OA, hydrocarbon-like OA, cooking OA, semivolatile oxygenated OA and low-volatility oxygenated OA. This information can be used to take future action on the respective legislation in order to improve the air quality.
Caroline Struckmeier, Frank Drewnick, Friederike Fachinger, Gian Paolo Gobbi, and Stephan Borrmann
Atmos. Chem. Phys., 16, 15277–15299, https://doi.org/10.5194/acp-16-15277-2016, https://doi.org/10.5194/acp-16-15277-2016, 2016
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The characteristics of ambient aerosol during two seasons (spring/autumn) and at two locations (suburban/urban) in Rome were investigated. We distinguished regionally advected and locally produced organic aerosols, including from cooking, traffic and biomass burning, but also from locally emitted cigarette smoke, for which we propose a new marker peak for identification in aerosol mass spectra. The impact of Saharan dust advection events on local aerosol concentration was studied.
Jianzhong Xu, Jinsen Shi, Qi Zhang, Xinlei Ge, Francesco Canonaco, André S. H. Prévôt, Matthias Vonwiller, Sönke Szidat, Jinming Ge, Jianmin Ma, Yanqing An, Shichang Kang, and Dahe Qin
Atmos. Chem. Phys., 16, 14937–14957, https://doi.org/10.5194/acp-16-14937-2016, https://doi.org/10.5194/acp-16-14937-2016, 2016
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This study deployed an AMS field study in Lanzhou, a city in northwestern China, evaluating the chemical composition, sources, and processes of urban aerosols during wintertime. In comparison with the results during summer in Lanzhou, the air pollution during winter was more severe and the sources were more complex. In addition, this paper estimates the contributions of fossil and non-fossil sources of organic carbon to primary and secondary organic carbon using the carbon isotopic method.
Friderike Kuik, Axel Lauer, Galina Churkina, Hugo A. C. Denier van der Gon, Daniel Fenner, Kathleen A. Mar, and Tim M. Butler
Geosci. Model Dev., 9, 4339–4363, https://doi.org/10.5194/gmd-9-4339-2016, https://doi.org/10.5194/gmd-9-4339-2016, 2016
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The study evaluates the performance of a setup of the Weather Research and Forecasting model with chemistry and aerosols (WRF–Chem) for the Berlin–Brandenburg region of Germany. Its sensitivity to updating urban input parameters based on structural data for Berlin is tested, specifying land use classes on a sub-grid scale, downscaling the original emissions to a resolution of ca. 1 km by 1 km for Berlin based on proxy data and model resolution.
Christos Kaltsonoudis, Evangelia Kostenidou, Kalliopi Florou, Magda Psichoudaki, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 14825–14842, https://doi.org/10.5194/acp-16-14825-2016, https://doi.org/10.5194/acp-16-14825-2016, 2016
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Volatile organic compounds (VOCs) were monitored in urban backgrounds sites, in Athens and Patras in Greece. In summer most of the measured VOCs were due to biogenic and traffic emissions. Winter measurements in Athens revealed that biomass burning used for residential heating was the dominant VOC source. The biomass burning VOC emission ratios and emission factors were estimated.
Antigoni Panagiotopoulou, Panagiotis Charalampidis, Christos Fountoukis, Christodoulos Pilinis, and Spyros N. Pandis
Geosci. Model Dev., 9, 4257–4272, https://doi.org/10.5194/gmd-9-4257-2016, https://doi.org/10.5194/gmd-9-4257-2016, 2016
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The ability of chemical transport model PMCAMx to reproduce ground and satellite aerosol optical depth (AOD) measurements over Europe is evaluated. PMCAMx reproduces AOD values over Spain, the UK, central Europe, and Russia with a fractional bias of less than 15 % and a fractional error of less than 30 %. The model overestimates the AOD over northern Europe probably due to an overestimation of organic aerosol and sulfates, and underestimates over the Balkans due to an underestimation of sulfates.
Petri Tiitta, Ari Leskinen, Liqing Hao, Pasi Yli-Pirilä, Miika Kortelainen, Julija Grigonyte, Jarkko Tissari, Heikki Lamberg, Anni Hartikainen, Kari Kuuspalo, Aki-Matti Kortelainen, Annele Virtanen, Kari E. J. Lehtinen, Mika Komppula, Simone Pieber, André S. H. Prévôt, Timothy B. Onasch, Douglas R. Worsnop, Hendryk Czech, Ralf Zimmermann, Jorma Jokiniemi, and Olli Sippula
Atmos. Chem. Phys., 16, 13251–13269, https://doi.org/10.5194/acp-16-13251-2016, https://doi.org/10.5194/acp-16-13251-2016, 2016
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Real-time measurements of OA aging and SOA formation from logwood combustion were conducted under dark and UV oxidation. Substantial SOA formation was observed in all experiments, leading to twice the initial OA mass emphasizing the importance of the burning conditions for the aging processes. The results prove that emissions are subject to intensive chemical processing in the atmosphere; e.g. the most of the POA was found to become oxidized after the ozone addition, forming aged POA.
Michael Bressi, Fabrizia Cavalli, Claudio A. Belis, Jean-Philippe Putaud, Roman Fröhlich, Sebastiao Martins dos Santos, Ettore Petralia, André S. H. Prévôt, Massimo Berico, Antonella Malaguti, and Francesco Canonaco
Atmos. Chem. Phys., 16, 12875–12896, https://doi.org/10.5194/acp-16-12875-2016, https://doi.org/10.5194/acp-16-12875-2016, 2016
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Atmospheric particulate matter (PM) levels and resulting impacts on human health are in the Po Valley (Italy) among the highest in Europe. This study discusses submicron PM chemical composition, sources and atmospheric processes in this region, using state-of-the-art measurement techniques and receptor models. Based on these results, effective PM abatement strategies are suggested in the upper Po Valley.
Bertrand Bessagnet, Guido Pirovano, Mihaela Mircea, Cornelius Cuvelier, Armin Aulinger, Giuseppe Calori, Giancarlo Ciarelli, Astrid Manders, Rainer Stern, Svetlana Tsyro, Marta García Vivanco, Philippe Thunis, Maria-Teresa Pay, Augustin Colette, Florian Couvidat, Frédérik Meleux, Laurence Rouïl, Anthony Ung, Sebnem Aksoyoglu, José María Baldasano, Johannes Bieser, Gino Briganti, Andrea Cappelletti, Massimo D'Isidoro, Sandro Finardi, Richard Kranenburg, Camillo Silibello, Claudio Carnevale, Wenche Aas, Jean-Charles Dupont, Hilde Fagerli, Lucia Gonzalez, Laurent Menut, André S. H. Prévôt, Pete Roberts, and Les White
Atmos. Chem. Phys., 16, 12667–12701, https://doi.org/10.5194/acp-16-12667-2016, https://doi.org/10.5194/acp-16-12667-2016, 2016
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The EURODELTA III exercise allows a very comprehensive intercomparison and evaluation of air quality models' performance. On average, the models provide a rather good picture of the particulate matter (PM) concentrations over Europe even if the highest concentrations are underestimated. The meteorology is responsible for model discrepancies, while the lack of emissions, particularly in winter, is mentioned as the main reason for the underestimations of PM.
Chao Yan, Wei Nie, Mikko Äijälä, Matti P. Rissanen, Manjula R. Canagaratna, Paola Massoli, Heikki Junninen, Tuija Jokinen, Nina Sarnela, Silja A. K. Häme, Siegfried Schobesberger, Francesco Canonaco, Lei Yao, André S. H. Prévôt, Tuukka Petäjä, Markku Kulmala, Mikko Sipilä, Douglas R. Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 16, 12715–12731, https://doi.org/10.5194/acp-16-12715-2016, https://doi.org/10.5194/acp-16-12715-2016, 2016
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Highly oxidized multifunctional compounds (HOMs) are known to have a significant contribution to secondary aerosol formation, yet their dominating formation pathways remain unclear in the atmosphere. We apply positive matrix factorization (PMF) on HOM data, and successfully retrieve factors representing different formation pathways. The results improve our understanding of HOM formation, and provide new perspectives on using PMF to study the variation of short-lived specie.
Ying Chen, Yafang Cheng, Nan Ma, Ralf Wolke, Stephan Nordmann, Stephanie Schüttauf, Liang Ran, Birgit Wehner, Wolfram Birmili, Hugo A. C. Denier van der Gon, Qing Mu, Stefan Barthel, Gerald Spindler, Bastian Stieger, Konrad Müller, Guang-Jie Zheng, Ulrich Pöschl, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 16, 12081–12097, https://doi.org/10.5194/acp-16-12081-2016, https://doi.org/10.5194/acp-16-12081-2016, 2016
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Sea salt aerosol (SSA) is important for primary and secondary aerosols on a global scale. During 10–20 September 2013, the SSA mass concentration was overestimated by a factor of 8–20 over central Europe by WRF-Chem model, stem from the uncertainty of its emission scheme. This could facilitate the coarse-mode nitrate formation (~ 140 % but inhibit the fine-mode nitrate formation (~−20 %). A special long-range transport mechanism could broaden this influence of SSA to a larger downwind region.
Weiwei Hu, Brett B. Palm, Douglas A. Day, Pedro Campuzano-Jost, Jordan E. Krechmer, Zhe Peng, Suzane S. de Sá, Scot T. Martin, M. Lizabeth Alexander, Karsten Baumann, Lina Hacker, Astrid Kiendler-Scharr, Abigail R. Koss, Joost A. de Gouw, Allen H. Goldstein, Roger Seco, Steven J. Sjostedt, Jeong-Hoo Park, Alex B. Guenther, Saewung Kim, Francesco Canonaco, André S. H. Prévôt, William H. Brune, and Jose L. Jimenez
Atmos. Chem. Phys., 16, 11563–11580, https://doi.org/10.5194/acp-16-11563-2016, https://doi.org/10.5194/acp-16-11563-2016, 2016
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IEPOX-SOA is biogenically derived secondary organic aerosol under anthropogenic influence, which has been shown to comprise a substantial fraction of OA globally. We investigated the lifetime of ambient IEPOX-SOA in the SE US and Amazonia, with an oxidation flow reactor and thermodenuder coupled with MS-based instrumentation. The low volatility and long lifetime of IEPOX-SOA against OH radicals' oxidation (> 2 weeks) was observed, which can help to constrain OA impact on air quality and climate.
Ingrid Super, Hugo A. C. Denier van der Gon, Michiel K. van der Molen, Hendrika A. M. Sterk, Arjan Hensen, and Wouter Peters
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2016-807, https://doi.org/10.5194/acp-2016-807, 2016
Revised manuscript not accepted
Elham Baranizadeh, Benjamin N. Murphy, Jan Julin, Saeed Falahat, Carly L. Reddington, Antti Arola, Lars Ahlm, Santtu Mikkonen, Christos Fountoukis, David Patoulias, Andreas Minikin, Thomas Hamburger, Ari Laaksonen, Spyros N. Pandis, Hanna Vehkamäki, Kari E. J. Lehtinen, and Ilona Riipinen
Geosci. Model Dev., 9, 2741–2754, https://doi.org/10.5194/gmd-9-2741-2016, https://doi.org/10.5194/gmd-9-2741-2016, 2016
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The molecular mechanisms through which new ultrafine (< 100 nm) aerosol particles are formed in the atmosphere have puzzled the scientific community for decades. In the past few years, however, significant progress has been made in unraveling these processes through laboratory studies and computational efforts. In this work we have implemented these new developments to an air quality model and study the implications of anthropogenically driven particle formation for European air quality.
Giancarlo Ciarelli, Sebnem Aksoyoglu, Monica Crippa, Jose-Luis Jimenez, Eriko Nemitz, Karine Sellegri, Mikko Äijälä, Samara Carbone, Claudia Mohr, Colin O'Dowd, Laurent Poulain, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 10313–10332, https://doi.org/10.5194/acp-16-10313-2016, https://doi.org/10.5194/acp-16-10313-2016, 2016
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Recent studies based on aerosol mass spectrometer measurements revealed that the organic fraction dominates the non-refractory PM1 composition. However its representation in chemical transport models is still very challenging due to uncertainties in emission sources and formation pathways. In this study, a novel organic aerosol scheme was tested in the regional air quality model CAMx and results were compared with ambient measurements at 11 different sites in Europe.
Alexandra P. Tsimpidi, Vlassis A. Karydis, Spyros N. Pandis, and Jos Lelieveld
Atmos. Chem. Phys., 16, 8939–8962, https://doi.org/10.5194/acp-16-8939-2016, https://doi.org/10.5194/acp-16-8939-2016, 2016
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In this work we use a global chemistry climate model together with a comprehensive global AMS data set in order to provide valuable insights into the temporal and geographical variability of the contribution of the emitted particles and the chemically processed organic material from combustion sources to total OA. This study reveals the high importance of SOA from anthropogenic sources on global OA concentrations and identifies plausible sources of discrepancy between models and measurements.
Patrick Schlag, Astrid Kiendler-Scharr, Marcus Johannes Blom, Francesco Canonaco, Jeroen Sebastiaan Henzing, Marcel Moerman, André Stephan Henry Prévôt, and Rupert Holzinger
Atmos. Chem. Phys., 16, 8831–8847, https://doi.org/10.5194/acp-16-8831-2016, https://doi.org/10.5194/acp-16-8831-2016, 2016
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This work provides chemical composition data of atmospheric aerosols acquired during 1 year in the rural site of Cabauw, the Netherlands. In some periods, we found unexpected high particle mass concentrations exceeding the WHO limits. Using these composition data, we found that reducing ammonia emissions in this region would largely reduce the main aerosol component ammonium nitrate, whereas the local mitigation of the organics turned out to be difficult due to the lack of a designated source.
Swen Metzger, Benedikt Steil, Mohamed Abdelkader, Klaus Klingmüller, Li Xu, Joyce E. Penner, Christos Fountoukis, Athanasios Nenes, and Jos Lelieveld
Atmos. Chem. Phys., 16, 7213–7237, https://doi.org/10.5194/acp-16-7213-2016, https://doi.org/10.5194/acp-16-7213-2016, 2016
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We introduce an unique single parameter framework to efficiently parameterize the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, being entirely based on the single solute specific coefficient introduced in Metzger et al. (2012).
Miriam Elser, Carlo Bozzetti, Imad El-Haddad, Marek Maasikmets, Erik Teinemaa, Rene Richter, Robert Wolf, Jay G. Slowik, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 7117–7134, https://doi.org/10.5194/acp-16-7117-2016, https://doi.org/10.5194/acp-16-7117-2016, 2016
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This work presents the first detailed in-situ measurements of major air pollutants (including NR-PM2.5, eBC, and trace gases) in the two biggest cities in Estonia. The sources of organic aerosols were investigated by means of positive matrix factorization. Highly time-resolved mobile measurements allowed for the identification of source areas and the determination of regional background concentrations as well as urban increments of the individual components.
Pauli Paasonen, Kaarle Kupiainen, Zbigniew Klimont, Antoon Visschedijk, Hugo A. C. Denier van der Gon, and Markus Amann
Atmos. Chem. Phys., 16, 6823–6840, https://doi.org/10.5194/acp-16-6823-2016, https://doi.org/10.5194/acp-16-6823-2016, 2016
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In this paper we show the first results of size-segregated anthropogenic particle number emissions from the GAINS emission scenario model. The shares of different sources and their predicted changes from 2010 to 2030 are described, showing clear difference in sources dominating the particle number and mass emissions. We also point out the main uncertainties in number emissions. The GAINS particle number emissions can be applied in improving the evaluation of aerosol climate and health effects.
Marje Prank, Mikhail Sofiev, Svetlana Tsyro, Carlijn Hendriks, Valiyaveetil Semeena, Xavier Vazhappilly Francis, Tim Butler, Hugo Denier van der Gon, Rainer Friedrich, Johannes Hendricks, Xin Kong, Mark Lawrence, Mattia Righi, Zissis Samaras, Robert Sausen, Jaakko Kukkonen, and Ranjeet Sokhi
Atmos. Chem. Phys., 16, 6041–6070, https://doi.org/10.5194/acp-16-6041-2016, https://doi.org/10.5194/acp-16-6041-2016, 2016
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Aerosol composition in Europe was simulated by four chemistry transport models and compared to observations to identify the most prominent areas for model improvement. Notable differences were found between the models' predictions, attributable to different treatment or omission of aerosol sources and processes. All models underestimated the observed concentrations by 10–60 %, mostly due to under-predicting the carbonaceous and mineral particles and omitting the aerosol-bound water.
Vidmantas Ulevicius, Steigvilė Byčenkienė, Carlo Bozzetti, Athanasia Vlachou, Kristina Plauškaitė, Genrik Mordas, Vadimas Dudoitis, Gülcin Abbaszade, Vidmantas Remeikis, Andrius Garbaras, Agne Masalaite, Jan Blees, Roman Fröhlich, Kaspar R. Dällenbach, Francesco Canonaco, Jay G. Slowik, Josef Dommen, Ralf Zimmermann, Jürgen Schnelle-Kreis, Gary A. Salazar, Konstantinos Agrios, Sönke Szidat, Imad El Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 5513–5529, https://doi.org/10.5194/acp-16-5513-2016, https://doi.org/10.5194/acp-16-5513-2016, 2016
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In early spring the Baltic region is frequently affected by high pollution events due to biomass burning in that area. Here we present a comprehensive study to investigate the impact of biomass/grass burning (BB) on the evolution and composition of aerosol in Preila, Lithuania, during springtime open fires.
Emma Järvinen, Karoliina Ignatius, Leonid Nichman, Thomas B. Kristensen, Claudia Fuchs, Christopher R. Hoyle, Niko Höppel, Joel C. Corbin, Jill Craven, Jonathan Duplissy, Sebastian Ehrhart, Imad El Haddad, Carla Frege, Hamish Gordon, Tuija Jokinen, Peter Kallinger, Jasper Kirkby, Alexei Kiselev, Karl-Heinz Naumann, Tuukka Petäjä, Tamara Pinterich, Andre S. H. Prevot, Harald Saathoff, Thea Schiebel, Kamalika Sengupta, Mario Simon, Jay G. Slowik, Jasmin Tröstl, Annele Virtanen, Paul Vochezer, Steffen Vogt, Andrea C. Wagner, Robert Wagner, Christina Williamson, Paul M. Winkler, Chao Yan, Urs Baltensperger, Neil M. Donahue, Rick C. Flagan, Martin Gallagher, Armin Hansel, Markku Kulmala, Frank Stratmann, Douglas R. Worsnop, Ottmar Möhler, Thomas Leisner, and Martin Schnaiter
Atmos. Chem. Phys., 16, 4423–4438, https://doi.org/10.5194/acp-16-4423-2016, https://doi.org/10.5194/acp-16-4423-2016, 2016
Sascha Pfeifer, Thomas Müller, Kay Weinhold, Nadezda Zikova, Sebastiao Martins dos Santos, Angela Marinoni, Oliver F. Bischof, Carsten Kykal, Ludwig Ries, Frank Meinhardt, Pasi Aalto, Nikolaos Mihalopoulos, and Alfred Wiedensohler
Atmos. Meas. Tech., 9, 1545–1551, https://doi.org/10.5194/amt-9-1545-2016, https://doi.org/10.5194/amt-9-1545-2016, 2016
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15 aerodynamic particle size spectrometers (APS model 3321, TSI Inc., St. Paul, MN, USA) were compared with a focus on flow rates accuracy, particle sizing, and unit-to-unit variability of the particle number size distribution.
Flow rate deviations were relatively small, while the sizing accuracy was found to be within 10 % compared to polystyrene latex reference particles. The unit-to-unit variability in terms of the particle number size distribution during this study was between 10 % and 60 %.
Monica Crippa, Greet Janssens-Maenhout, Frank Dentener, Diego Guizzardi, Katerina Sindelarova, Marilena Muntean, Rita Van Dingenen, and Claire Granier
Atmos. Chem. Phys., 16, 3825–3841, https://doi.org/10.5194/acp-16-3825-2016, https://doi.org/10.5194/acp-16-3825-2016, 2016
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The interplay of European air quality policies and technological advancement to reduce anthropogenic emissions avoided a dramatic deterioration of air quality in Europe and beyond over the last 40 years (e.g. fuel quality directives reduced global SO2 emissions by 88 %, while the EURO standards led to a 50 % reduction of PM2.5). The story told by the EDGAR retrospective scenarios can be informative for designing multi-pollutant abatement policies also in emerging economies.
Miriam Elser, Ru-Jin Huang, Robert Wolf, Jay G. Slowik, Qiyuan Wang, Francesco Canonaco, Guohui Li, Carlo Bozzetti, Kaspar R. Daellenbach, Yu Huang, Renjian Zhang, Zhengqiang Li, Junji Cao, Urs Baltensperger, Imad El-Haddad, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 3207–3225, https://doi.org/10.5194/acp-16-3207-2016, https://doi.org/10.5194/acp-16-3207-2016, 2016
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This work represents the first online chemical characterization of the PM2.5 using a high-resolution time-of flight aerosol mass spectrometer during extreme haze events China. The application of novel source apportionment techniques allowed for an improved identification and quantification of the sources of organic aerosols. The main sources and processes driving the extreme haze events are assessed.
Andrea Paciga, Eleni Karnezi, Evangelia Kostenidou, Lea Hildebrandt, Magda Psichoudaki, Gabriella J. Engelhart, Byong-Hyoek Lee, Monica Crippa, André S. H. Prévôt, Urs Baltensperger, and Spyros N. Pandis
Atmos. Chem. Phys., 16, 2013–2023, https://doi.org/10.5194/acp-16-2013-2016, https://doi.org/10.5194/acp-16-2013-2016, 2016
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We estimate the volatility distribution for the organic aerosol (OA) components during summer and winter field campaigns in Paris, France as part of the collaborative project MEGAPOLI. The OA factors (hydrocarbon like OA, cooking OA, marine OA, oxygenated OA) had a broad spectrum of volatilities with no direct link between the average volatility and average oxygen to carbon of the OA components.
Sebnem Aksoyoglu, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 16, 1895–1906, https://doi.org/10.5194/acp-16-1895-2016, https://doi.org/10.5194/acp-16-1895-2016, 2016
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As a least-regulated source, ship emissions contribute significantly to air pollution. We used an air quality model to determine the effects of international shipping on the annual and seasonal concentrations of ozone, primary and secondary components of PM2.5, and dry and wet deposition of N and S compounds in Europe. The results presented in this paper suggest evolution of NOx emissions from ships and land-based NH3 emissions will play a significant role in the future European air quality.
Ying Chen, Ya-Fang Cheng, Stephan Nordmann, Wolfram Birmili, Hugo A. C. Denier van der Gon, Nan Ma, Ralf Wolke, Birgit Wehner, Jia Sun, Gerald Spindler, Qing Mu, Ulrich Pöschl, Hang Su, and Alfred Wiedensohler
Atmos. Chem. Phys., 16, 1823–1835, https://doi.org/10.5194/acp-16-1823-2016, https://doi.org/10.5194/acp-16-1823-2016, 2016
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We evaluated the EC point sources in Germany with high-resolution simulation by WRF-Chem, and find out that point sources contribute too much EC in the coarse mode aerosol mass. The area emissions in Eastern Europe and Russia also allocate too much EC emission in coarse mode in the EUCAARI EC emission inventory. Because of the shorter life time of coarse mode EC, about 20–40 % less EC can be transported to Melpitz from Eastern Europe. Size segregation information is important for EC inventories.
C. R. Hoyle, C. Fuchs, E. Järvinen, H. Saathoff, A. Dias, I. El Haddad, M. Gysel, S. C. Coburn, J. Tröstl, A.-K. Bernhammer, F. Bianchi, M. Breitenlechner, J. C. Corbin, J. Craven, N. M. Donahue, J. Duplissy, S. Ehrhart, C. Frege, H. Gordon, N. Höppel, M. Heinritzi, T. B. Kristensen, U. Molteni, L. Nichman, T. Pinterich, A. S. H. Prévôt, M. Simon, J. G. Slowik, G. Steiner, A. Tomé, A. L. Vogel, R. Volkamer, A. C. Wagner, R. Wagner, A. S. Wexler, C. Williamson, P. M. Winkler, C. Yan, A. Amorim, J. Dommen, J. Curtius, M. W. Gallagher, R. C. Flagan, A. Hansel, J. Kirkby, M. Kulmala, O. Möhler, F. Stratmann, D. R. Worsnop, and U. Baltensperger
Atmos. Chem. Phys., 16, 1693–1712, https://doi.org/10.5194/acp-16-1693-2016, https://doi.org/10.5194/acp-16-1693-2016, 2016
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A significant portion of sulphate, an important constituent of atmospheric aerosols, is formed via the aqueous phase oxidation of sulphur dioxide by ozone. The rate of this reaction has previously only been measured over a relatively small temperature range. Here, we use the state of the art CLOUD chamber at CERN to perform the first measurements of this reaction rate in super-cooled droplets, confirming that the existing extrapolation of the reaction rate to sub-zero temperatures is accurate.
J. Kukkonen, M. Karl, M. P. Keuken, H. A. C. Denier van der Gon, B. R. Denby, V. Singh, J. Douros, A. Manders, Z. Samaras, N. Moussiopoulos, S. Jonkers, M. Aarnio, A. Karppinen, L. Kangas, S. Lützenkirchen, T. Petäjä, I. Vouitsis, and R. S. Sokhi
Geosci. Model Dev., 9, 451–478, https://doi.org/10.5194/gmd-9-451-2016, https://doi.org/10.5194/gmd-9-451-2016, 2016
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For analyzing the health effects of particulate matter, it is necessary to consider not only the mass of particles, but also their sizes and composition. A simple measure for the former is the number concentration of particles. We present particle number concentrations in five major European cities, namely Helsinki, Oslo, London, Rotterdam, and Athens, in 2008, based mainly on modelling. The concentrations of PN were mostly influenced by the emissions from local vehicular traffic.
L. Xu, L. R. Williams, D. E. Young, J. D. Allan, H. Coe, P. Massoli, E. Fortner, P. Chhabra, S. Herndon, W. A. Brooks, J. T. Jayne, D. R. Worsnop, A. C. Aiken, S. Liu, K. Gorkowski, M. K. Dubey, Z. L. Fleming, S. Visser, A. S. H. Prévôt, and N. L. Ng
Atmos. Chem. Phys., 16, 1139–1160, https://doi.org/10.5194/acp-16-1139-2016, https://doi.org/10.5194/acp-16-1139-2016, 2016
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We investigate the spatial distribution of submicron aerosol in the greater London area as part of the Clean Air for London (ClearfLo) project in winter 2012. Although the concentrations of organic aerosol (OA) are similar between a rural and an urban site, the OA sources are different. We also examine the volatility of submicron aerosol at the rural site and find that the non-volatile organics have similar sources or have undergone similar chemical processing as refractory black carbon.
G. I. Gkatzelis, D. K. Papanastasiou, K. Florou, C. Kaltsonoudis, E. Louvaris, and S. N. Pandis
Atmos. Meas. Tech., 9, 103–114, https://doi.org/10.5194/amt-9-103-2016, https://doi.org/10.5194/amt-9-103-2016, 2016
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A method for the measurement of the nonvolatile atmospheric particle size distribution is developed and tested. The tests include laboratory experiments with biogenic and anthropogenic secondary organic aerosol as well as nucleation experiments with ambient air. The method is then further tested during an ambient campaign.
K. R. Daellenbach, C. Bozzetti, A. Křepelová, F. Canonaco, R. Wolf, P. Zotter, P. Fermo, M. Crippa, J. G. Slowik, Y. Sosedova, Y. Zhang, R.-J. Huang, L. Poulain, S. Szidat, U. Baltensperger, I. El Haddad, and A. S. H. Prévôt
Atmos. Meas. Tech., 9, 23–39, https://doi.org/10.5194/amt-9-23-2016, https://doi.org/10.5194/amt-9-23-2016, 2016
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In this study, we developed an offline technique using the AMS for the characterization of the chemical fingerprints of aerosols collected on quartz filters, and evaluated the suitability of the organic mass spectral data for source apportionment. This technique may be used to enhance the AMS capabilities in measuring size-fractionated, spatially resolved long-term data sets.
V. Crenn, J. Sciare, P. L. Croteau, S. Verlhac, R. Fröhlich, C. A. Belis, W. Aas, M. Äijälä, A. Alastuey, B. Artiñano, D. Baisnée, N. Bonnaire, M. Bressi, M. Canagaratna, F. Canonaco, C. Carbone, F. Cavalli, E. Coz, M. J. Cubison, J. K. Esser-Gietl, D. C. Green, V. Gros, L. Heikkinen, H. Herrmann, C. Lunder, M. C. Minguillón, G. Močnik, C. D. O'Dowd, J. Ovadnevaite, J.-E. Petit, E. Petralia, L. Poulain, M. Priestman, V. Riffault, A. Ripoll, R. Sarda-Estève, J. G. Slowik, A. Setyan, A. Wiedensohler, U. Baltensperger, A. S. H. Prévôt, J. T. Jayne, and O. Favez
Atmos. Meas. Tech., 8, 5063–5087, https://doi.org/10.5194/amt-8-5063-2015, https://doi.org/10.5194/amt-8-5063-2015, 2015
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A large intercomparison study of 13 Q-ACSM was conducted for a 3-week period in the region of Paris to evaluate the performance of this instrument and to monitor the major NR-PM1 chemical components. Reproducibility expanded uncertainties of Q-ACSM concentration measurements were found to be 9, 15, 19, 28, and 36% for NR-PM1, NO3, OM, SO4, and NH4, respectively. Some recommendations regarding best calibration practices, standardized data processing and data treatment are also provided.
G. Janssens-Maenhout, M. Crippa, D. Guizzardi, F. Dentener, M. Muntean, G. Pouliot, T. Keating, Q. Zhang, J. Kurokawa, R. Wankmüller, H. Denier van der Gon, J. J. P. Kuenen, Z. Klimont, G. Frost, S. Darras, B. Koffi, and M. Li
Atmos. Chem. Phys., 15, 11411–11432, https://doi.org/10.5194/acp-15-11411-2015, https://doi.org/10.5194/acp-15-11411-2015, 2015
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This paper provides monthly emission grid maps at 0.1deg x 0.1deg resolution with global coverage for air pollutants and aerosols anthropogenic emissions in 2008 and 2010.
Countries are consistently inter-compared with sector-specific implied emission factors, per capita emissions and emissions per unit of GDP.
The emission grid maps compose the reference emissions data set for the community modelling hemispheric transport of air pollution (HTAP).
R. Fröhlich, M. J. Cubison, J. G. Slowik, N. Bukowiecki, F. Canonaco, P. L. Croteau, M. Gysel, S. Henne, E. Herrmann, J. T. Jayne, M. Steinbacher, D. R. Worsnop, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 15, 11373–11398, https://doi.org/10.5194/acp-15-11373-2015, https://doi.org/10.5194/acp-15-11373-2015, 2015
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This manuscript presents the first long-term (14-month) and highly time-resolved (10 min) measurements of NR-PM1 aerosol chemical composition at a high-altitude site (JFJ, Switzerland, 3580m a.s.l.). The elevated location allowed the investigation of free tropospheric aerosol year round. Total and relative mass loadings, diurnal variations as well as seasonal variations are discussed together with geographical origin, organic aerosol sources and the influence of the planetary boundary layer.
E. Kostenidou, K. Florou, C. Kaltsonoudis, M. Tsiflikiotou, S. Vratolis, K. Eleftheriadis, and S. N. Pandis
Atmos. Chem. Phys., 15, 11355–11371, https://doi.org/10.5194/acp-15-11355-2015, https://doi.org/10.5194/acp-15-11355-2015, 2015
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The concentration and chemical composition of fine particulate matter were measured during the summer of 2012 in two Greek cities, Patras and Athens. The composition of PM1 was surprisingly similar in both areas, demonstrating the importance of regional sources. Analysis of the Aerosol Mass Spectrometer data suggested that the contribution of the primary sources to organic aerosol was important (22% in Patras and 35% in Athens) but not dominant.
M. Pikridas, J. Sciare, F. Freutel, S. Crumeyrolle, S.-L. von der Weiden-Reinmüller, A. Borbon, A. Schwarzenboeck, M. Merkel, M. Crippa, E. Kostenidou, M. Psichoudaki, L. Hildebrandt, G. J. Engelhart, T. Petäjä, A. S. H. Prévôt, F. Drewnick, U. Baltensperger, A. Wiedensohler, M. Kulmala, M. Beekmann, and S. N. Pandis
Atmos. Chem. Phys., 15, 10219–10237, https://doi.org/10.5194/acp-15-10219-2015, https://doi.org/10.5194/acp-15-10219-2015, 2015
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Aerosol size distribution measurements from three ground sites, two mobile laboratories, and one airplane are combined to investigate the spatial and temporal variability of ultrafine particles in and around Paris during the summer and winter MEGAPOLI campaigns. The role of nucleation as a particle source and the influence of Paris emissions on their surroundings are examined.
V. Marécal, V.-H. Peuch, C. Andersson, S. Andersson, J. Arteta, M. Beekmann, A. Benedictow, R. Bergström, B. Bessagnet, A. Cansado, F. Chéroux, A. Colette, A. Coman, R. L. Curier, H. A. C. Denier van der Gon, A. Drouin, H. Elbern, E. Emili, R. J. Engelen, H. J. Eskes, G. Foret, E. Friese, M. Gauss, C. Giannaros, J. Guth, M. Joly, E. Jaumouillé, B. Josse, N. Kadygrov, J. W. Kaiser, K. Krajsek, J. Kuenen, U. Kumar, N. Liora, E. Lopez, L. Malherbe, I. Martinez, D. Melas, F. Meleux, L. Menut, P. Moinat, T. Morales, J. Parmentier, A. Piacentini, M. Plu, A. Poupkou, S. Queguiner, L. Robertson, L. Rouïl, M. Schaap, A. Segers, M. Sofiev, L. Tarasson, M. Thomas, R. Timmermans, Á. Valdebenito, P. van Velthoven, R. van Versendaal, J. Vira, and A. Ung
Geosci. Model Dev., 8, 2777–2813, https://doi.org/10.5194/gmd-8-2777-2015, https://doi.org/10.5194/gmd-8-2777-2015, 2015
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This paper describes the air quality forecasting system over Europe put in place in the Monitoring Atmospheric Composition and Climate projects. It provides daily and 4-day forecasts and analyses for the previous day for major gas and particulate pollutants and their main precursors. These products are based on a multi-model approach using seven state-of-the-art models developed in Europe. An evaluation of the performance of the system is discussed in the paper.
H. Petetin, M. Beekmann, A. Colomb, H. A. C. Denier van der Gon, J.-C. Dupont, C. Honoré, V. Michoud, Y. Morille, O. Perrussel, A. Schwarzenboeck, J. Sciare, A. Wiedensohler, and Q. J. Zhang
Atmos. Chem. Phys., 15, 9799–9818, https://doi.org/10.5194/acp-15-9799-2015, https://doi.org/10.5194/acp-15-9799-2015, 2015
M. Beekmann, A. S. H. Prévôt, F. Drewnick, J. Sciare, S. N. Pandis, H. A. C. Denier van der Gon, M. Crippa, F. Freutel, L. Poulain, V. Ghersi, E. Rodriguez, S. Beirle, P. Zotter, S.-L. von der Weiden-Reinmüller, M. Bressi, C. Fountoukis, H. Petetin, S. Szidat, J. Schneider, A. Rosso, I. El Haddad, A. Megaritis, Q. J. Zhang, V. Michoud, J. G. Slowik, S. Moukhtar, P. Kolmonen, A. Stohl, S. Eckhardt, A. Borbon, V. Gros, N. Marchand, J. L. Jaffrezo, A. Schwarzenboeck, A. Colomb, A. Wiedensohler, S. Borrmann, M. Lawrence, A. Baklanov, and U. Baltensperger
Atmos. Chem. Phys., 15, 9577–9591, https://doi.org/10.5194/acp-15-9577-2015, https://doi.org/10.5194/acp-15-9577-2015, 2015
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A detailed characterization of air quality in the Paris (France) agglomeration, a megacity, during two summer and winter intensive campaigns and from additional 1-year observations, revealed that about 70% of the fine particulate matter (PM) at urban background is transported into the megacity from upwind regions. Unexpectedly, a major part of organic PM is of modern origin (woodburning and cooking activities, secondary formation from biogenic VOC).
S. Fuzzi, U. Baltensperger, K. Carslaw, S. Decesari, H. Denier van der Gon, M. C. Facchini, D. Fowler, I. Koren, B. Langford, U. Lohmann, E. Nemitz, S. Pandis, I. Riipinen, Y. Rudich, M. Schaap, J. G. Slowik, D. V. Spracklen, E. Vignati, M. Wild, M. Williams, and S. Gilardoni
Atmos. Chem. Phys., 15, 8217–8299, https://doi.org/10.5194/acp-15-8217-2015, https://doi.org/10.5194/acp-15-8217-2015, 2015
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Particulate matter (PM) constitutes one of the most challenging problems both for air quality and climate change policies. This paper reviews the most recent scientific results on the issue and the policy needs that have driven much of the increase in monitoring and mechanistic research over the last 2 decades. The synthesis reveals many new processes and developments in the science underpinning climate-PM interactions and the effects of PM on human health and the environment.
L. Hildebrandt Ruiz, A. L. Paciga, K. M. Cerully, A. Nenes, N. M. Donahue, and S. N. Pandis
Atmos. Chem. Phys., 15, 8301–8313, https://doi.org/10.5194/acp-15-8301-2015, https://doi.org/10.5194/acp-15-8301-2015, 2015
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Secondary organic aerosol (SOA) is transformed after its initial formation. We explored the effects of this chemical aging on the composition, mass yield, volatility, and hygroscopicity of SOA formed from the photo-oxidation of small aromatic volatile organic compounds. Higher exposure to the hydroxyl radical resulted in different SOA composition, average carbon oxidation state, and mass yield. The vapor pressure of SOA formed under different conditions varied by as much as a factor of 30.
F. Canonaco, J. G. Slowik, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 15, 6993–7002, https://doi.org/10.5194/acp-15-6993-2015, https://doi.org/10.5194/acp-15-6993-2015, 2015
R. Fröhlich, V. Crenn, A. Setyan, C. A. Belis, F. Canonaco, O. Favez, V. Riffault, J. G. Slowik, W. Aas, M. Aijälä, A. Alastuey, B. Artiñano, N. Bonnaire, C. Bozzetti, M. Bressi, C. Carbone, E. Coz, P. L. Croteau, M. J. Cubison, J. K. Esser-Gietl, D. C. Green, V. Gros, L. Heikkinen, H. Herrmann, J. T. Jayne, C. R. Lunder, M. C. Minguillón, G. Močnik, C. D. O'Dowd, J. Ovadnevaite, E. Petralia, L. Poulain, M. Priestman, A. Ripoll, R. Sarda-Estève, A. Wiedensohler, U. Baltensperger, J. Sciare, and A. S. H. Prévôt
Atmos. Meas. Tech., 8, 2555–2576, https://doi.org/10.5194/amt-8-2555-2015, https://doi.org/10.5194/amt-8-2555-2015, 2015
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Source apportionment (SA) of organic aerosol mass spectrometric data measured with the Aerodyne ACSM using PMF/ME2 is a frequently used technique in the AMS/ACSM community. ME2 uncertainties due to instrument-to-instrument variations are elucidated by performing SA on ambient data from 14 individual, co-located ACSMs, recorded during the first ACTRIS ACSM intercomparison study at SIRTA near Paris (France). The mean uncertainty was 17.2%. Recommendations for future studies using ME2 are provided.
H. A. C. Denier van der Gon, R. Bergström, C. Fountoukis, C. Johansson, S. N. Pandis, D. Simpson, and A. J. H. Visschedijk
Atmos. Chem. Phys., 15, 6503–6519, https://doi.org/10.5194/acp-15-6503-2015, https://doi.org/10.5194/acp-15-6503-2015, 2015
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Residential wood combustion (RWC) is increasing in Europe but may cause high emissions of particulate matter (PM). A revised bottom-up emission inventory was made which included the semi-volatile components. The revised RWC emissions are 2–3 times higher than the previous inventory. It significantly improved the modeling of PM and comparison with observations. Our results suggest primary PM2.5 emission from RWC as reported in Europe is underestimated and emission inventories need to be revised.
D. Patoulias, C. Fountoukis, I. Riipinen, and S. N. Pandis
Atmos. Chem. Phys., 15, 6337–6350, https://doi.org/10.5194/acp-15-6337-2015, https://doi.org/10.5194/acp-15-6337-2015, 2015
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A new aerosol dynamics model (DMANx) describing the organic vapor condensation on nanoparticles based on the volatility basis set framework is used to simulate typical nucleation events in two contrasting environments in Hyytiälä (Finland) and Finokalia (Greece). The role of semivolatile, low, and extremely low volatility organics and the corresponding surface energies is investigated.
M. C. Minguillón, A. Ripoll, N. Pérez, A. S. H. Prévôt, F. Canonaco, X. Querol, and A. Alastuey
Atmos. Chem. Phys., 15, 6379–6391, https://doi.org/10.5194/acp-15-6379-2015, https://doi.org/10.5194/acp-15-6379-2015, 2015
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The study focuses on the aerosol variations found in the regional background of the western Mediterranean basin and their relation with atmospheric conditions and scenarios. An Aerosol Chemical Speciation Monitor (ACSM) was deployed for 1 year and the results were validated with co-located PM1 measurements. The organic sources were investigated and the local secondary organic aerosol (SOA) formation was estimated.
I. Riipinen, N. Rastak, and S. N. Pandis
Atmos. Chem. Phys., 15, 6305–6322, https://doi.org/10.5194/acp-15-6305-2015, https://doi.org/10.5194/acp-15-6305-2015, 2015
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Atmospheric organic aerosol is complex and thus a challenge to model. We introduce a theoretical framework (solubility distributions) to represent the solubility of multicomponent mixtures. Using the framework, we evaluate the commonly made assumptions about the cloud condensation nucleus (CCN) activity of organic mixtures. We find that material with water solubilities larger than 0.1-100 g/L can usually be treated as completely soluble, which simplifies the treatment of organic CCN.
A. Tasoglou and S. N. Pandis
Atmos. Chem. Phys., 15, 6035–6046, https://doi.org/10.5194/acp-15-6035-2015, https://doi.org/10.5194/acp-15-6035-2015, 2015
P. L. Hayes, A. G. Carlton, K. R. Baker, R. Ahmadov, R. A. Washenfelder, S. Alvarez, B. Rappenglück, J. B. Gilman, W. C. Kuster, J. A. de Gouw, P. Zotter, A. S. H. Prévôt, S. Szidat, T. E. Kleindienst, J. H. Offenberg, P. K. Ma, and J. L. Jimenez
Atmos. Chem. Phys., 15, 5773–5801, https://doi.org/10.5194/acp-15-5773-2015, https://doi.org/10.5194/acp-15-5773-2015, 2015
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(1) Four different parameterizations for the formation and chemical evolution of secondary organic aerosol (SOA) are evaluated using a box model representing the Los Angeles region during the CalNex campaign.
(2) The SOA formed only from the oxidation of VOCs is insufficient to explain the observed SOA concentrations.
(3) The amount of SOA mass formed from diesel vehicle emissions is estimated to be 16-27%.
(4) Modeled SOA depends strongly on the P-S/IVOC volatility distribution.
L. Drinovec, G. Močnik, P. Zotter, A. S. H. Prévôt, C. Ruckstuhl, E. Coz, M. Rupakheti, J. Sciare, T. Müller, A. Wiedensohler, and A. D. A. Hansen
Atmos. Meas. Tech., 8, 1965–1979, https://doi.org/10.5194/amt-8-1965-2015, https://doi.org/10.5194/amt-8-1965-2015, 2015
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We present a new real-time algorithm for compensation of the filter-loading effect in filter photometers, based on a two parallel spot measurement of optical absorption. This algorithm has been incorporated into the new Aethalometer AE33. Intercomparison studies show excellent reproducibility of the AE33 measurements and very good agreement with post-processed data obtained using earlier aethalometer models and other filter-based absorption photometers.
S. Banzhaf, M. Schaap, R. Kranenburg, A. M. M. Manders, A. J. Segers, A. J. H. Visschedijk, H. A. C. Denier van der Gon, J. J. P. Kuenen, E. van Meijgaard, L. H. van Ulft, J. Cofala, and P. J. H. Builtjes
Geosci. Model Dev., 8, 1047–1070, https://doi.org/10.5194/gmd-8-1047-2015, https://doi.org/10.5194/gmd-8-1047-2015, 2015
L. R. Crilley, W. J. Bloss, J. Yin, D. C. S. Beddows, R. M. Harrison, J. D. Allan, D. E. Young, M. Flynn, P. Williams, P. Zotter, A. S. H. Prevot, M. R. Heal, J. F. Barlow, C. H. Halios, J. D. Lee, S. Szidat, and C. Mohr
Atmos. Chem. Phys., 15, 3149–3171, https://doi.org/10.5194/acp-15-3149-2015, https://doi.org/10.5194/acp-15-3149-2015, 2015
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Wood is a renewable fuel but its combustion for residential heating releases a number of locally acting air pollutants, most notably particulate matter known to have adverse effects on human health. This paper used chemical tracers for wood smoke to estimate the contribution that burning wood makes to concentrations of airborne particles in the atmosphere of southern England and most particularly in London.
B. Gantt, M. S. Johnson, M. Crippa, A. S. H. Prévôt, and N. Meskhidze
Geosci. Model Dev., 8, 619–629, https://doi.org/10.5194/gmd-8-619-2015, https://doi.org/10.5194/gmd-8-619-2015, 2015