Articles | Volume 17, issue 23
https://doi.org/10.5194/acp-17-14309-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-17-14309-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
04 Dec 2017
Research article |
| 04 Dec 2017
Boreal forest BVOC exchange: emissions versus in-canopy sinks
University of Helsinki, Department of Physics, P.O. Box 64, 00014, University of Helsinki, Helsinki, Finland
Laurens Ganzeveld
Meteorology and Air Quality (MAQ), Department of Environmental Sciences,
Wageningen University and Research Centre, Wageningen, the Netherlands
Ditte Taipale
University of Helsinki, Department of Forest Sciences, P.O. Box 27, 00014, University of Helsinki, Helsinki, Finland
Estonian University of Life Sciences, Department of Plant Physiology, Kreutzwaldi 1, 51014, Estonia
Üllar Rannik
University of Helsinki, Department of Physics, P.O. Box 64, 00014, University of Helsinki, Helsinki, Finland
Pekka Rantala
University of Helsinki, Department of Physics, P.O. Box 64, 00014, University of Helsinki, Helsinki, Finland
Matti Petteri Rissanen
University of Helsinki, Department of Physics, P.O. Box 64, 00014, University of Helsinki, Helsinki, Finland
Dean Chen
University of Helsinki, Department of Physics, P.O. Box 64, 00014, University of Helsinki, Helsinki, Finland
Michael Boy
University of Helsinki, Department of Physics, P.O. Box 64, 00014, University of Helsinki, Helsinki, Finland
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Steven Turnock, Dimitris Akritidis, Larry Horowitz, Mariano Mertens, Andrea Pozzer, Carly Reddington, Hantao Wang, Putian Zhou, and Fiona O'Connor
EGUsphere, https://doi.org/10.5194/egusphere-2024-2732, https://doi.org/10.5194/egusphere-2024-2732, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
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We assess the drivers behind changes in peak season surface zone concentrations and risk to human health between 1850 and 2014. Substantial increases in surface ozone have occurred over this period resulting in a significant increase in the risk to human health, mainly driven by increases in anthropogenic NOx emissions and global CH4 concentrations. Fixing anthropogenic NOx emissions at 1850 values in the near present-day period can eliminate the risk to human health.
Putian Zhou, Zhengyao Lu, Jukka-Pekka Keskinen, Qiong Zhang, Juha Lento, Jianpu Bian, Twan van Noije, Philippe Le Sager, Veli-Matti Kerminen, Markku Kulmala, Michael Boy, and Risto Makkonen
Clim. Past, 19, 2445–2462, https://doi.org/10.5194/cp-19-2445-2023, https://doi.org/10.5194/cp-19-2445-2023, 2023
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A Green Sahara with enhanced rainfall and larger vegetation cover existed in northern Africa about 6000 years ago. Biosphere–atmosphere interactions are found to be critical to explaining this wet period. Based on modeled vegetation reconstruction data, we simulated dust emissions and aerosol formation, which are key factors in biosphere–atmosphere interactions. Our results also provide a benchmark of aerosol climatology for future paleo-climate simulation experiments.
Lukas Pichelstorfer, Pontus Roldin, Matti Rissanen, Noora Hyttinen, Olga Garmash, Carlton Xavier, Putian Zhou, Petri Clusius, Benjamin Foreback, Thomas Golin Almeida, Chenjuan Deng, Metin Baykara, Theo Kurten, and Michael Boy
EGUsphere, https://doi.org/10.5194/egusphere-2023-1415, https://doi.org/10.5194/egusphere-2023-1415, 2023
Preprint archived
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Secondary organic aerosols (SOA) form effectively from gaseous precursors via a process called autoxidation. While key chemical reaction types seem to be known, no general description of autoxidation chemistry exists. In the present work, we present a method to create autoxidation chemistry schemes for any atmospherically relevant hydrocarbon. We exemplarily investigate benzene and its potential to form aerosols. We found that autoxidation, under some conditions, can dominate the SOA formation.
Petri Clusius, Carlton Xavier, Lukas Pichelstorfer, Putian Zhou, Tinja Olenius, Pontus Roldin, and Michael Boy
Geosci. Model Dev., 15, 7257–7286, https://doi.org/10.5194/gmd-15-7257-2022, https://doi.org/10.5194/gmd-15-7257-2022, 2022
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Atmospheric chemistry and aerosol processes form a dynamic and sensitively balanced system, and solving problems regarding air quality or climate requires detailed modelling and coupling of the processes. The models involved are often very complex to use. We have addressed this problem with the new ARCA box model. It puts much of the current knowledge of the nano- and microscale aerosol dynamics and chemistry into usable software and has the potential to become a valuable tool in the community.
Zhuohui Lin, Yonghong Wang, Feixue Zheng, Ying Zhou, Yishuo Guo, Zemin Feng, Chang Li, Yusheng Zhang, Simo Hakala, Tommy Chan, Chao Yan, Kaspar R. Daellenbach, Biwu Chu, Lubna Dada, Juha Kangasluoma, Lei Yao, Xiaolong Fan, Wei Du, Jing Cai, Runlong Cai, Tom V. Kokkonen, Putian Zhou, Lili Wang, Tuukka Petäjä, Federico Bianchi, Veli-Matti Kerminen, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys., 21, 12173–12187, https://doi.org/10.5194/acp-21-12173-2021, https://doi.org/10.5194/acp-21-12173-2021, 2021
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We find that ammonium nitrate and aerosol water content contributed most during low mixing layer height conditions; this may further trigger enhanced formation of sulfate and organic aerosol via heterogeneous reactions. The results of this study contribute towards a more detailed understanding of the aerosol–chemistry–radiation–boundary layer feedback that is likely to be responsible for explosive aerosol mass growth events in urban Beijing.
Yuan Yang, Yonghong Wang, Putian Zhou, Dan Yao, Dongsheng Ji, Jie Sun, Yinghong Wang, Shuman Zhao, Wei Huang, Shuanghong Yang, Dean Chen, Wenkang Gao, Zirui Liu, Bo Hu, Renjian Zhang, Limin Zeng, Maofa Ge, Tuukka Petäjä, Veli-Matti Kerminen, Markku Kulmala, and Yuesi Wang
Atmos. Chem. Phys., 20, 8181–8200, https://doi.org/10.5194/acp-20-8181-2020, https://doi.org/10.5194/acp-20-8181-2020, 2020
Dean Chen, Putian Zhou, Tuomo Nieminen, Pontus Roldin, Ximeng Qi, Petri Clusius, Carlton Xavier, Lukas Pichelstorfer, Markku Kulmala, Pekka Rantala, Juho Aalto, Nina Sarnela, Pasi Kolari, Petri Keronen, Matti P. Rissanen, Metin Baykara, and Michael Boy
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-128, https://doi.org/10.5194/acp-2020-128, 2020
Preprint withdrawn
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Atmospheric oxidants OH, O3 and NO3 dominate the atmospheric oxidation capacity, and sulfuric acid (H2SO4) is considered as a main driver for new particle formation events. We studied how the trends of these atmospheric oxidants and H2SO4 changed in southern Finland during the past 12 years and discussed how these trends related to decreasing emissions of air pollutants in Europe. Our results showed that OH increased by 1.56 % yr−1 at daytime and NO3 decreased by 3.92 % yr−1 at nighttime.
Yonghong Wang, Miao Yu, Yuesi Wang, Guiqian Tang, Tao Song, Putian Zhou, Zirui Liu, Bo Hu, Dongsheng Ji, Lili Wang, Xiaowan Zhu, Chao Yan, Mikael Ehn, Wenkang Gao, Yuepeng Pan, Jinyuan Xin, Yang Sun, Veli-Matti Kerminen, Markku Kulmala, and Tuukka Petäjä
Atmos. Chem. Phys., 20, 45–53, https://doi.org/10.5194/acp-20-45-2020, https://doi.org/10.5194/acp-20-45-2020, 2020
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We found a positive particle matter-mixing layer height feedback at three observation platforms at the 325 m Beijing meteorology tower, which is characterized by a shallower mixing layer height and a higher particle matter concentration. Measurements of solar radiation, aerosol chemical composition, meteorology parameters, trace gases and turbulent kinetic energy (TKE) could explain the feedback mechanism to some extent.
Arnaud P. Praplan, Toni Tykkä, Dean Chen, Michael Boy, Ditte Taipale, Ville Vakkari, Putian Zhou, Tuukka Petäjä, and Heidi Hellén
Atmos. Chem. Phys., 19, 14431–14453, https://doi.org/10.5194/acp-19-14431-2019, https://doi.org/10.5194/acp-19-14431-2019, 2019
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Our study shows that, despite our best efforts and recent progress, our knowledge of the chemical composition of the air under the canopy of a boreal forest still cannot be fully characterized. The discrepancy between the measured total reactivity of the air and the reactivity derived from the known chemical composition highlights the need to better understand the emissions from vegetation, but also other sources, such as the forest soil.
Carlton Xavier, Anton Rusanen, Putian Zhou, Chen Dean, Lukas Pichelstorfer, Pontus Roldin, and Michael Boy
Atmos. Chem. Phys., 19, 13741–13758, https://doi.org/10.5194/acp-19-13741-2019, https://doi.org/10.5194/acp-19-13741-2019, 2019
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Master Chemical Mechanism (MCM) coupled to peroxy radical autoxidation mechanism (PRAM) was used to simulate secondary organic aerosol mass loadings from oxidation of five selected biogenic volatile organic compounds. The simulations were designed to replicate idealized chamber and oxidative flow-tube setups. The mass yields using MCM + PRAM are in good agreement with the experimental yields, thereby allowing us to highlight a few important compounds which contribute to > 95 % of mass loadings.
Yuqin Liu, Jiahua Zhang, Putian Zhou, Tao Lin, Juan Hong, Lamei Shi, Fengmei Yao, Jun Wu, Huadong Guo, and Gerrit de Leeuw
Atmos. Chem. Phys., 18, 18187–18202, https://doi.org/10.5194/acp-18-18187-2018, https://doi.org/10.5194/acp-18-18187-2018, 2018
Ximeng Qi, Aijun Ding, Pontus Roldin, Zhengning Xu, Putian Zhou, Nina Sarnela, Wei Nie, Xin Huang, Anton Rusanen, Mikael Ehn, Matti P. Rissanen, Tuukka Petäjä, Markku Kulmala, and Michael Boy
Atmos. Chem. Phys., 18, 11779–11791, https://doi.org/10.5194/acp-18-11779-2018, https://doi.org/10.5194/acp-18-11779-2018, 2018
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In this study we simulate the HOM concentrations and discuss their roles in NPF at a remote boreal forest site in Finland and a suburban site in eastern China. We found that sulfuric acid and HOM organonitrate concentrations in the gas phase are significantly higher but other HOM monomers and dimers from monoterpene oxidation are lower in eastern China. This study highlights the need for molecular-scale measurements in improving the understanding of NPF mechanisms in polluted areas.
Ben H. Lee, Felipe D. Lopez-Hilfiker, Emma L. D'Ambro, Putian Zhou, Michael Boy, Tuukka Petäjä, Liqing Hao, Annele Virtanen, and Joel A. Thornton
Atmos. Chem. Phys., 18, 11547–11562, https://doi.org/10.5194/acp-18-11547-2018, https://doi.org/10.5194/acp-18-11547-2018, 2018
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Molecular identities and abundances of organic compounds residing in the gas and particle phases above a Finnish boreal forest are presented. We determined that in each phase, the organic components are categorized into three subgroups based on their behavior in time. Some are more enhanced at night, others during midday, and another around sunrise. Identifying such collective behavior can potentially connect the chemical processes that evolve in time to specific distributions of products.
Emilie Öström, Zhou Putian, Guy Schurgers, Mikhail Mishurov, Niku Kivekäs, Heikki Lihavainen, Mikael Ehn, Matti P. Rissanen, Theo Kurtén, Michael Boy, Erik Swietlicki, and Pontus Roldin
Atmos. Chem. Phys., 17, 8887–8901, https://doi.org/10.5194/acp-17-8887-2017, https://doi.org/10.5194/acp-17-8887-2017, 2017
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We used a model to study how biogenic volatile organic compounds (BVOCs) emitted from the boreal forest contribute to the formation and growth of particles in the atmosphere. Some of these particles are important climate forcers, acting as seeds for cloud droplet fomation. We implemented a new gas chemistry mechanism that describes how the BVOCs are oxidized and form low-volatility highly oxidized organic molecules. With the new mechanism we are able to accurately predict the particle growth.
Eero Nikinmaa, Tuomo Kalliokoski, Kari Minkkinen, Jaana Bäck, Michael Boy, Yao Gao, Nina Janasik-Honkela, Janne I. Hukkinen, Maarit Kallio, Markku Kulmala, Nea Kuusinen, Annikki Mäkelä, Brent D. Matthies, Mikko Peltoniemi, Risto Sievänen, Ditte Taipale, Lauri Valsta, Anni Vanhatalo, Martin Welp, Luxi Zhou, Putian Zhou, and Frank Berninger
Biogeosciences Discuss., https://doi.org/10.5194/bg-2017-141, https://doi.org/10.5194/bg-2017-141, 2017
Manuscript not accepted for further review
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We estimated the impact of boreal forest management on climate, considering the effects of carbon, albedo, aerosols, and effects of industrial wood use. We made analyses both in current and warmer climate of 2050. The aerosol effect was comparable to that of carbon sequestration. Deciduous trees may have a large potential for mitigation due to their high albedo and aerosol effects. If the forests will be used more intensively and mainly for pulp and energy, the warming influence is clear.
Yuqin Liu, Gerrit de Leeuw, Veli-Matti Kerminen, Jiahua Zhang, Putian Zhou, Wei Nie, Ximeng Qi, Juan Hong, Yonghong Wang, Aijun Ding, Huadong Guo, Olaf Krüger, Markku Kulmala, and Tuukka Petäjä
Atmos. Chem. Phys., 17, 5623–5641, https://doi.org/10.5194/acp-17-5623-2017, https://doi.org/10.5194/acp-17-5623-2017, 2017
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The aerosol effects on warm cloud parameters over the Yangtze River Delta are systematically examined using multi-sensor retrievals. This study shows that the COT–CDR and CWP–CDR relationships are not unique, but are affected by atmospheric aerosol loading. CDR and cloud fraction show different behaviours for low and high AOD. Aerosol–cloud interaction (ACI) is stronger for clouds mixed with smoke aerosol than for clouds mixed with dust. Meteorological conditions play an important role in ACI.
Putian Zhou, Laurens Ganzeveld, Üllar Rannik, Luxi Zhou, Rosa Gierens, Ditte Taipale, Ivan Mammarella, and Michael Boy
Atmos. Chem. Phys., 17, 1361–1379, https://doi.org/10.5194/acp-17-1361-2017, https://doi.org/10.5194/acp-17-1361-2017, 2017
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We implemented a multi-layer O3 dry deposition model in a 1-D model SOSAA to simulate O3 flux and concentration within and above a boreal forest at SMEAR II in Hyytiälä, Finland, in August 2010. The results showed that when RH > 70 % the O3 uptake on leaf wet skin was ~ 51 % to the total deposition at night and ~ 19 % at daytime. The sub-canopy contribution below 4.2 m was ~ 38 % at daytime. The averaged daily chemical contribution to total O3 alteration inside the canopy was less than 10 %.
Henning Finkenzeller, Jyri Mikkilä, Cecilia Righi, Paxton Juuti, Mikko Sipilä, Matti Rissanen, Douglas Worsnop, Aleksei Shcherbinin, Nina Sarnela, and Juha Kangasluoma
Atmos. Meas. Tech., 17, 5989–6001, https://doi.org/10.5194/amt-17-5989-2024, https://doi.org/10.5194/amt-17-5989-2024, 2024
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Chemical ionisation mass spectrometry is used in the atmospheric sciences to measure trace gas concentrations. Neutral gases require charging in inlets before the mass-to-charge ratio of the resulting ions can be analysed. This study uses multiphysics modelling to investigate how the MION2 and Eisele type inlets work and shows the effect of tuning parameters and their current limitations. The findings are helpful for inlet users and are expected to aid in developing improved inlets.
Steven Turnock, Dimitris Akritidis, Larry Horowitz, Mariano Mertens, Andrea Pozzer, Carly Reddington, Hantao Wang, Putian Zhou, and Fiona O'Connor
EGUsphere, https://doi.org/10.5194/egusphere-2024-2732, https://doi.org/10.5194/egusphere-2024-2732, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
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We assess the drivers behind changes in peak season surface zone concentrations and risk to human health between 1850 and 2014. Substantial increases in surface ozone have occurred over this period resulting in a significant increase in the risk to human health, mainly driven by increases in anthropogenic NOx emissions and global CH4 concentrations. Fixing anthropogenic NOx emissions at 1850 values in the near present-day period can eliminate the risk to human health.
Anam M. Khan, Olivia E. Clifton, Jesse O. Bash, Sam Bland, Nathan Booth, Philip Cheung, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christian Hogrefe, Christopher D. Holmes, Laszlo Horvath, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Perez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Donna Schwede, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamas Weidinger, Zhiyong Wu, Leiming Zhang, and Paul C. Stoy
EGUsphere, https://doi.org/10.5194/egusphere-2024-3038, https://doi.org/10.5194/egusphere-2024-3038, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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Vegetation removes tropospheric ozone through stomatal uptake, and accurately modeling the stomatal uptake of ozone is important for modeling dry deposition and air quality. We evaluated the stomatal component of ozone dry deposition modeled by atmospheric chemistry models at six sites. We find that models and observation-based estimates agree at times during the growing season at all sites, but some models overestimated the stomatal component during the dry summers at a seasonally dry site.
Alex Rowell, James Brean, David C. S. Beddows, Zongbo Shi, Avinash Kumar, Matti Rissanen, Miikka Dal Maso, Peter Mettke, Kay Weinhold, Maik Merkel, and Roy M. Harrison
Atmos. Chem. Phys., 24, 10349–10361, https://doi.org/10.5194/acp-24-10349-2024, https://doi.org/10.5194/acp-24-10349-2024, 2024
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Ions enhance the formation and growth rates of new particles, affecting the Earth's radiation budget. Despite these effects, there is little published data exploring the sources of ions in the urban environment and their role in new particle formation (NPF). Here we show that natural ion sources dominate in urban environments, while traffic is a secondary source. Ions contribute up to 12.7 % of the formation rate of particles, indicating that they are important for forming urban PM.
Dandan Li, Dongyu Wang, Lucia Caudillo, Wiebke Scholz, Mingyi Wang, Sophie Tomaz, Guillaume Marie, Mihnea Surdu, Elias Eccli, Xianda Gong, Loic Gonzalez-Carracedo, Manuel Granzin, Joschka Pfeifer, Birte Rörup, Benjamin Schulze, Pekka Rantala, Sébastien Perrier, Armin Hansel, Joachim Curtius, Jasper Kirkby, Neil M. Donahue, Christian George, Imad El-Haddad, and Matthieu Riva
Atmos. Meas. Tech., 17, 5413–5428, https://doi.org/10.5194/amt-17-5413-2024, https://doi.org/10.5194/amt-17-5413-2024, 2024
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Due to the analytical challenges of measuring organic vapors, it remains challenging to identify and quantify organic molecules present in the atmosphere. Here, we explore the performance of the Orbitrap chemical ionization mass spectrometer (CI-Orbitrap) using ammonium ion chemistry. This study shows that ammonium-ion-based chemistry associated with the high mass resolution of the Orbitrap mass analyzer can measure almost all inclusive compounds.
Stéphanie Alage, Vincent Michoud, Sergio Harb, Bénédicte Picquet-Varrault, Manuela Cirtog, Avinash Kumar, Matti Rissanen, and Christopher Cantrell
Atmos. Meas. Tech., 17, 4709–4724, https://doi.org/10.5194/amt-17-4709-2024, https://doi.org/10.5194/amt-17-4709-2024, 2024
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Calibration exercises are essential for determining the accuracy of instruments. We performed calibrations on a NO3¯ ToFCIMS instrument to determine its sensitivity and linearity for detecting various organic compounds. Our findings revealed significant variability, over several orders of magnitude, in the calibration factors obtained. The results suggest that relying on a single calibration factor from H2SO4 for the quantification of all compounds detected by this technique is not appropriate.
Federica Bortolussi, Hilda Sandström, Fariba Partovi, Joona Mikkilä, Patrick Rinke, and Matti Rissanen
EGUsphere, https://doi.org/10.5194/egusphere-2024-1846, https://doi.org/10.5194/egusphere-2024-1846, 2024
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Chemical ionization mass spectrometry (CIMS) is widely used in atmospheric chemistry studies. We still have a limited understanding of the complex functioning of the instrument, therefore, we applied machine learning to provide insights from CIMS analyses. We were able to predict both detection and signal intensity with a fair error and we found out the most important structural fragments for negative ionization schemes (NH and OH) and positive ones (nitrogen-containing groups).
Romain Salignat, Matti Rissanen, Siddharth Iyer, Jean-Luc Baray, Pierre Tulet, Jean-Marc Metzger, Jérôme Brioude, Karine Sellegri, and Clémence Rose
Atmos. Chem. Phys., 24, 3785–3812, https://doi.org/10.5194/acp-24-3785-2024, https://doi.org/10.5194/acp-24-3785-2024, 2024
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Using mass spectrometry data collected at the Maïdo Observatory (2160 m a.s.l., Réunion), we provide the first detailed analysis of molecular cluster chemical composition specifically in the marine free troposphere. The abundance of the identified species is related both to in situ meteorological parameters and air mass history, which also provide insight into their origin. Our work makes an important contribution to documenting the chemistry and physics of the marine free troposphere.
Putian Zhou, Zhengyao Lu, Jukka-Pekka Keskinen, Qiong Zhang, Juha Lento, Jianpu Bian, Twan van Noije, Philippe Le Sager, Veli-Matti Kerminen, Markku Kulmala, Michael Boy, and Risto Makkonen
Clim. Past, 19, 2445–2462, https://doi.org/10.5194/cp-19-2445-2023, https://doi.org/10.5194/cp-19-2445-2023, 2023
Short summary
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A Green Sahara with enhanced rainfall and larger vegetation cover existed in northern Africa about 6000 years ago. Biosphere–atmosphere interactions are found to be critical to explaining this wet period. Based on modeled vegetation reconstruction data, we simulated dust emissions and aerosol formation, which are key factors in biosphere–atmosphere interactions. Our results also provide a benchmark of aerosol climatology for future paleo-climate simulation experiments.
Xu-Cheng He, Jiali Shen, Siddharth Iyer, Paxton Juuti, Jiangyi Zhang, Mrisha Koirala, Mikko M. Kytökari, Douglas R. Worsnop, Matti Rissanen, Markku Kulmala, Norbert M. Maier, Jyri Mikkilä, Mikko Sipilä, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 4461–4487, https://doi.org/10.5194/amt-16-4461-2023, https://doi.org/10.5194/amt-16-4461-2023, 2023
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In this study, the upgraded multi-scheme chemical ionisation inlet 2 is presented. Sulfuric acid, hypoiodous acid, iodine, sulfur dioxide, and hydroperoxyl radicals are calibrated, and the improved ion optics allow us to detect sulfuric acid and iodine-containing molecules at as low as a few parts per quadrillion by volume. Additionally, we confirm the reliable detection of iodic acid using both the nitrate and bromide chemical ionisation methods under atmospherically relevant conditions.
Shawon Barua, Siddharth Iyer, Avinash Kumar, Prasenjit Seal, and Matti Rissanen
Atmos. Chem. Phys., 23, 10517–10532, https://doi.org/10.5194/acp-23-10517-2023, https://doi.org/10.5194/acp-23-10517-2023, 2023
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This work illustrates how a common volatile hydrocarbon, hexanal, has the potential to undergo atmospheric autoxidation that leads to prompt formation of condensable material that subsequently contributes to aerosol formation, deteriorating the air quality of urban atmospheres. We used the combined state-of-the-art quantum chemical modeling and experimental flow reactor experiments under atmospheric conditions to resolve the autoxidation mechanism of hexanal initiated by a common oxidant.
Olivia E. Clifton, Donna Schwede, Christian Hogrefe, Jesse O. Bash, Sam Bland, Philip Cheung, Mhairi Coyle, Lisa Emberson, Johannes Flemming, Erick Fredj, Stefano Galmarini, Laurens Ganzeveld, Orestis Gazetas, Ignacio Goded, Christopher D. Holmes, László Horváth, Vincent Huijnen, Qian Li, Paul A. Makar, Ivan Mammarella, Giovanni Manca, J. William Munger, Juan L. Pérez-Camanyo, Jonathan Pleim, Limei Ran, Roberto San Jose, Sam J. Silva, Ralf Staebler, Shihan Sun, Amos P. K. Tai, Eran Tas, Timo Vesala, Tamás Weidinger, Zhiyong Wu, and Leiming Zhang
Atmos. Chem. Phys., 23, 9911–9961, https://doi.org/10.5194/acp-23-9911-2023, https://doi.org/10.5194/acp-23-9911-2023, 2023
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A primary sink of air pollutants is dry deposition. Dry deposition estimates differ across the models used to simulate atmospheric chemistry. Here, we introduce an effort to examine dry deposition schemes from atmospheric chemistry models. We provide our approach’s rationale, document the schemes, and describe datasets used to drive and evaluate the schemes. We also launch the analysis of results by evaluating against observations and identifying the processes leading to model–model differences.
Lukas Pichelstorfer, Pontus Roldin, Matti Rissanen, Noora Hyttinen, Olga Garmash, Carlton Xavier, Putian Zhou, Petri Clusius, Benjamin Foreback, Thomas Golin Almeida, Chenjuan Deng, Metin Baykara, Theo Kurten, and Michael Boy
EGUsphere, https://doi.org/10.5194/egusphere-2023-1415, https://doi.org/10.5194/egusphere-2023-1415, 2023
Preprint archived
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Secondary organic aerosols (SOA) form effectively from gaseous precursors via a process called autoxidation. While key chemical reaction types seem to be known, no general description of autoxidation chemistry exists. In the present work, we present a method to create autoxidation chemistry schemes for any atmospherically relevant hydrocarbon. We exemplarily investigate benzene and its potential to form aerosols. We found that autoxidation, under some conditions, can dominate the SOA formation.
Melissa Meder, Otso Peräkylä, Jonathan G. Varelas, Jingyi Luo, Runlong Cai, Yanjun Zhang, Theo Kurtén, Matthieu Riva, Matti Rissanen, Franz M. Geiger, Regan J. Thomson, and Mikael Ehn
Atmos. Chem. Phys., 23, 4373–4390, https://doi.org/10.5194/acp-23-4373-2023, https://doi.org/10.5194/acp-23-4373-2023, 2023
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We discuss and show the viability of a method where multiple isotopically labelled precursors are used for probing the formation pathways of highly oxygenated organic molecules (HOMs) from the oxidation of the monoterpene a-pinene. HOMs are very important for secondary organic aerosol (SOA) formation in forested regions, and monoterpenes are the single largest source of SOA globally. The fast reactions forming HOMs have thus far remained elusive despite considerable efforts over the last decade.
Lejish Vettikkat, Pasi Miettinen, Angela Buchholz, Pekka Rantala, Hao Yu, Simon Schallhart, Tuukka Petäjä, Roger Seco, Elisa Männistö, Markku Kulmala, Eeva-Stiina Tuittila, Alex B. Guenther, and Siegfried Schobesberger
Atmos. Chem. Phys., 23, 2683–2698, https://doi.org/10.5194/acp-23-2683-2023, https://doi.org/10.5194/acp-23-2683-2023, 2023
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Wetlands cover a substantial fraction of the land mass in the northern latitudes, from northern Europe to Siberia and Canada. Yet, their isoprene and terpene emissions remain understudied. Here, we used a state-of-the-art measurement technique to quantify ecosystem-scale emissions from a boreal wetland during an unusually warm spring/summer. We found that the emissions from this wetland were (a) higher and (b) even more strongly dependent on temperature than commonly thought.
Petri Clusius, Carlton Xavier, Lukas Pichelstorfer, Putian Zhou, Tinja Olenius, Pontus Roldin, and Michael Boy
Geosci. Model Dev., 15, 7257–7286, https://doi.org/10.5194/gmd-15-7257-2022, https://doi.org/10.5194/gmd-15-7257-2022, 2022
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Atmospheric chemistry and aerosol processes form a dynamic and sensitively balanced system, and solving problems regarding air quality or climate requires detailed modelling and coupling of the processes. The models involved are often very complex to use. We have addressed this problem with the new ARCA box model. It puts much of the current knowledge of the nano- and microscale aerosol dynamics and chemistry into usable software and has the potential to become a valuable tool in the community.
Benjamin Foreback, Lubna Dada, Kaspar R. Daellenbach, Chao Yan, Lili Wang, Biwu Chu, Ying Zhou, Tom V. Kokkonen, Mona Kurppa, Rosaria E. Pileci, Yonghong Wang, Tommy Chan, Juha Kangasluoma, Lin Zhuohui, Yishou Guo, Chang Li, Rima Baalbaki, Joni Kujansuu, Xiaolong Fan, Zemin Feng, Pekka Rantala, Shahzad Gani, Federico Bianchi, Veli-Matti Kerminen, Tuukka Petäjä, Markku Kulmala, Yongchun Liu, and Pauli Paasonen
Atmos. Chem. Phys., 22, 11089–11104, https://doi.org/10.5194/acp-22-11089-2022, https://doi.org/10.5194/acp-22-11089-2022, 2022
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This study analyzed air quality in Beijing during the Chinese New Year over 7 years, including data from a new in-depth measurement station. This is one of few studies to look at long-term impacts, including the outcome of firework restrictions starting in 2018. Results show that firework pollution has gone down since 2016, indicating a positive result from the restrictions. Results of this study may be useful in making future decisions about the use of fireworks to improve air quality.
Carlton Xavier, Metin Baykara, Robin Wollesen de Jonge, Barbara Altstädter, Petri Clusius, Ville Vakkari, Roseline Thakur, Lisa Beck, Silvia Becagli, Mirko Severi, Rita Traversi, Radovan Krejci, Peter Tunved, Mauro Mazzola, Birgit Wehner, Mikko Sipilä, Markku Kulmala, Michael Boy, and Pontus Roldin
Atmos. Chem. Phys., 22, 10023–10043, https://doi.org/10.5194/acp-22-10023-2022, https://doi.org/10.5194/acp-22-10023-2022, 2022
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The focus of this work is to study and improve our understanding of processes involved in the formation and growth of new particles in a remote Arctic marine environment. We run the 1D model ADCHEM along air mass trajectories arriving at Ny-Ålesund in May 2018. The model finds that ion-mediated H2SO4–NH3 nucleation can explain the observed new particle formation at Ny-Ålesund. The growth of particles is driven via H2SO4 condensation and formation of methane sulfonic acid in the aqueous phase.
Hannele Hakola, Ditte Taipale, Arnaud Praplan, Simon Schallhart, Steven Thomas, Toni Tykkä, Aku Helin, Jaana Bäck, and Heidi Hellén
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-478, https://doi.org/10.5194/acp-2022-478, 2022
Revised manuscript not accepted
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Norway spruce is one of the main tree species growing in the boreal area. We show that volatile organic compound emission potentials and compound composition vary a lot. We have investigated if e.g. growing location or age of a tree could explain the variations. Recognizing this observed large variability in spruce BVOC emissions (precursors for new particle formation processes), we also tested the consequences of this variability in simulations of aerosol formation.
Miska Olin, Magdalena Okuljar, Matti P. Rissanen, Joni Kalliokoski, Jiali Shen, Lubna Dada, Markus Lampimäki, Yusheng Wu, Annalea Lohila, Jonathan Duplissy, Mikko Sipilä, Tuukka Petäjä, Markku Kulmala, and Miikka Dal Maso
Atmos. Chem. Phys., 22, 8097–8115, https://doi.org/10.5194/acp-22-8097-2022, https://doi.org/10.5194/acp-22-8097-2022, 2022
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Atmospheric new particle formation is an important source of the total particle number concentration in the atmosphere. Several parameters for predicting new particle formation events have been suggested before, but the results have been inconclusive. This study proposes an another predicting parameter, related to a specific type of highly oxidized organic molecules, especially for similar locations to the measurement site in this study, which was a coastal agricultural site in Finland.
Ruochong Xu, Joel A. Thornton, Ben H. Lee, Yanxu Zhang, Lyatt Jaeglé, Felipe D. Lopez-Hilfiker, Pekka Rantala, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 5477–5494, https://doi.org/10.5194/acp-22-5477-2022, https://doi.org/10.5194/acp-22-5477-2022, 2022
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Monoterpenes are emitted into the atmosphere by vegetation and by the use of certain consumer products. Reactions of monoterpenes in the atmosphere lead to low-volatility products that condense to grow particulate matter or participate in new particle formation and, thus, affect air quality and climate. We use a model of atmospheric chemistry and transport to evaluate the global-scale importance of recent updates to our understanding of monoterpene chemistry in particle formation and growth.
Hanna K. Lappalainen, Tuukka Petäjä, Timo Vihma, Jouni Räisänen, Alexander Baklanov, Sergey Chalov, Igor Esau, Ekaterina Ezhova, Matti Leppäranta, Dmitry Pozdnyakov, Jukka Pumpanen, Meinrat O. Andreae, Mikhail Arshinov, Eija Asmi, Jianhui Bai, Igor Bashmachnikov, Boris Belan, Federico Bianchi, Boris Biskaborn, Michael Boy, Jaana Bäck, Bin Cheng, Natalia Chubarova, Jonathan Duplissy, Egor Dyukarev, Konstantinos Eleftheriadis, Martin Forsius, Martin Heimann, Sirkku Juhola, Vladimir Konovalov, Igor Konovalov, Pavel Konstantinov, Kajar Köster, Elena Lapshina, Anna Lintunen, Alexander Mahura, Risto Makkonen, Svetlana Malkhazova, Ivan Mammarella, Stefano Mammola, Stephany Buenrostro Mazon, Outi Meinander, Eugene Mikhailov, Victoria Miles, Stanislav Myslenkov, Dmitry Orlov, Jean-Daniel Paris, Roberta Pirazzini, Olga Popovicheva, Jouni Pulliainen, Kimmo Rautiainen, Torsten Sachs, Vladimir Shevchenko, Andrey Skorokhod, Andreas Stohl, Elli Suhonen, Erik S. Thomson, Marina Tsidilina, Veli-Pekka Tynkkynen, Petteri Uotila, Aki Virkkula, Nadezhda Voropay, Tobias Wolf, Sayaka Yasunaka, Jiahua Zhang, Yubao Qiu, Aijun Ding, Huadong Guo, Valery Bondur, Nikolay Kasimov, Sergej Zilitinkevich, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 22, 4413–4469, https://doi.org/10.5194/acp-22-4413-2022, https://doi.org/10.5194/acp-22-4413-2022, 2022
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We summarize results during the last 5 years in the northern Eurasian region, especially from Russia, and introduce recent observations of the air quality in the urban environments in China. Although the scientific knowledge in these regions has increased, there are still gaps in our understanding of large-scale climate–Earth surface interactions and feedbacks. This arises from limitations in research infrastructures and integrative data analyses, hindering a comprehensive system analysis.
Dalrin Ampritta Amaladhasan, Claudia Heyn, Christopher R. Hoyle, Imad El Haddad, Miriam Elser, Simone M. Pieber, Jay G. Slowik, Antonio Amorim, Jonathan Duplissy, Sebastian Ehrhart, Vladimir Makhmutov, Ugo Molteni, Matti Rissanen, Yuri Stozhkov, Robert Wagner, Armin Hansel, Jasper Kirkby, Neil M. Donahue, Rainer Volkamer, Urs Baltensperger, Martin Gysel-Beer, and Andreas Zuend
Atmos. Chem. Phys., 22, 215–244, https://doi.org/10.5194/acp-22-215-2022, https://doi.org/10.5194/acp-22-215-2022, 2022
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We use a combination of models for gas-phase chemical reactions and equilibrium gas–particle partitioning of isoprene-derived secondary organic aerosols (SOAs) informed by dark ozonolysis experiments conducted in the CLOUD chamber. Our predictions cover high to low relative humidities (RHs) and quantify how SOA mass yields are enhanced at high RH as well as the impact of inorganic seeds of distinct hygroscopicities and acidities on the coupled partitioning of water and semi-volatile organics.
Auke J. Visser, Laurens N. Ganzeveld, Ignacio Goded, Maarten C. Krol, Ivan Mammarella, Giovanni Manca, and K. Folkert Boersma
Atmos. Chem. Phys., 21, 18393–18411, https://doi.org/10.5194/acp-21-18393-2021, https://doi.org/10.5194/acp-21-18393-2021, 2021
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Dry deposition is an important sink for tropospheric ozone that affects ecosystem carbon uptake, but process understanding remains incomplete. We apply a common deposition representation in atmospheric chemistry models and a multi-layer canopy model to multi-year ozone deposition observations. The multi-layer canopy model performs better on diurnal timescales compared to the common approach, leading to a substantially improved simulation of ozone deposition and vegetation ozone impact metrics.
Mikko Sipilä, Nina Sarnela, Kimmo Neitola, Totti Laitinen, Deniz Kemppainen, Lisa Beck, Ella-Maria Duplissy, Salla Kuittinen, Tuuli Lehmusjärvi, Janne Lampilahti, Veli-Matti Kerminen, Katrianne Lehtipalo, Pasi P. Aalto, Petri Keronen, Erkki Siivola, Pekka A. Rantala, Douglas R. Worsnop, Markku Kulmala, Tuija Jokinen, and Tuukka Petäjä
Atmos. Chem. Phys., 21, 17559–17576, https://doi.org/10.5194/acp-21-17559-2021, https://doi.org/10.5194/acp-21-17559-2021, 2021
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Metallurgical industry in Kola peninsula is a large source of air pollution in the (sub-)Arctic domain. Sulfur dioxide emissions from the ore smelters are transported across large areas. We investigated sulfur dioxide and its transformation to sulfuric acid aerosol particles during winter months in Finnish Lapland, close to Kola industrial areas. We observed intense formation of new aerosol particles despite the low solar radiation intensity, often required for new particle formation elsewhere.
Ditte Taipale, Veli-Matti Kerminen, Mikael Ehn, Markku Kulmala, and Ülo Niinemets
Atmos. Chem. Phys., 21, 17389–17431, https://doi.org/10.5194/acp-21-17389-2021, https://doi.org/10.5194/acp-21-17389-2021, 2021
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Larval feeding and fungal infections of leaves can greatly change the emission of volatile compounds from plants and thereby influence aerosol processes in the air. We developed a model that considers the dynamics of larvae and fungi and the dependency of the emission on the severity of stress. We show that the infections can be highly atmospherically relevant during long periods of time and at times more important to consider than the parameters that are currently used in emission models.
Yang Liu, Simon Schallhart, Ditte Taipale, Toni Tykkä, Matti Räsänen, Lutz Merbold, Heidi Hellén, and Petri Pellikka
Atmos. Chem. Phys., 21, 14761–14787, https://doi.org/10.5194/acp-21-14761-2021, https://doi.org/10.5194/acp-21-14761-2021, 2021
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We studied the mixing ratio of biogenic volatile organic compounds (BVOCs) in a humid highland and dry lowland African ecosystem in Kenya. The mixing ratio of monoterpenoids was similar to that measured in the relevant ecosystems in western and southern Africa, while that of isoprene was lower. Modeling the emission factors (EFs) for BVOCs from the lowlands, the EFs for isoprene and β-pinene agreed well with what is assumed in the MEGAN, while those of α-pinene and limonene were higher.
Mao Xiao, Christopher R. Hoyle, Lubna Dada, Dominik Stolzenburg, Andreas Kürten, Mingyi Wang, Houssni Lamkaddam, Olga Garmash, Bernhard Mentler, Ugo Molteni, Andrea Baccarini, Mario Simon, Xu-Cheng He, Katrianne Lehtipalo, Lauri R. Ahonen, Rima Baalbaki, Paulus S. Bauer, Lisa Beck, David Bell, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, António Dias, Jonathan Duplissy, Henning Finkenzeller, Hamish Gordon, Victoria Hofbauer, Changhyuk Kim, Theodore K. Koenig, Janne Lampilahti, Chuan Ping Lee, Zijun Li, Huajun Mai, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Serge Mathot, Roy L. Mauldin, Wei Nie, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti Rissanen, Siegfried Schobesberger, Simone Schuchmann, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Robert Wagner, Yonghong Wang, Lena Weitz, Daniela Wimmer, Yusheng Wu, Chao Yan, Penglin Ye, Qing Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Ken Carslaw, Joachim Curtius, Armin Hansel, Rainer Volkamer, Paul M. Winkler, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Jasper Kirkby, Neil M. Donahue, Urs Baltensperger, Imad El Haddad, and Josef Dommen
Atmos. Chem. Phys., 21, 14275–14291, https://doi.org/10.5194/acp-21-14275-2021, https://doi.org/10.5194/acp-21-14275-2021, 2021
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Experiments at CLOUD show that in polluted environments new particle formation (NPF) is largely driven by the formation of sulfuric acid–base clusters, stabilized by amines, high ammonia concentrations or lower temperatures. While oxidation products of aromatics can nucleate, they play a minor role in urban NPF. Our experiments span 4 orders of magnitude variation of observed NPF rates in ambient conditions. We provide a framework based on NPF and growth rates to interpret ambient observations.
Zhuohui Lin, Yonghong Wang, Feixue Zheng, Ying Zhou, Yishuo Guo, Zemin Feng, Chang Li, Yusheng Zhang, Simo Hakala, Tommy Chan, Chao Yan, Kaspar R. Daellenbach, Biwu Chu, Lubna Dada, Juha Kangasluoma, Lei Yao, Xiaolong Fan, Wei Du, Jing Cai, Runlong Cai, Tom V. Kokkonen, Putian Zhou, Lili Wang, Tuukka Petäjä, Federico Bianchi, Veli-Matti Kerminen, Yongchun Liu, and Markku Kulmala
Atmos. Chem. Phys., 21, 12173–12187, https://doi.org/10.5194/acp-21-12173-2021, https://doi.org/10.5194/acp-21-12173-2021, 2021
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We find that ammonium nitrate and aerosol water content contributed most during low mixing layer height conditions; this may further trigger enhanced formation of sulfate and organic aerosol via heterogeneous reactions. The results of this study contribute towards a more detailed understanding of the aerosol–chemistry–radiation–boundary layer feedback that is likely to be responsible for explosive aerosol mass growth events in urban Beijing.
Toprak Aslan, Olli Peltola, Andreas Ibrom, Eiko Nemitz, Üllar Rannik, and Ivan Mammarella
Atmos. Meas. Tech., 14, 5089–5106, https://doi.org/10.5194/amt-14-5089-2021, https://doi.org/10.5194/amt-14-5089-2021, 2021
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Vertical turbulent fluxes of gases measured by the eddy covariance (EC) technique are subject to high-frequency losses. There are different methods used to describe this low-pass filtering effect and to correct the measured fluxes. In this study, we analysed the systematic uncertainty related to this correction for various attenuation and signal-to-noise ratios. A new and robust transfer function method is finally proposed.
Olli Peltola, Toprak Aslan, Andreas Ibrom, Eiko Nemitz, Üllar Rannik, and Ivan Mammarella
Atmos. Meas. Tech., 14, 5071–5088, https://doi.org/10.5194/amt-14-5071-2021, https://doi.org/10.5194/amt-14-5071-2021, 2021
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Gas fluxes measured by the eddy covariance (EC) technique are subject to filtering due to non-ideal instrumentation. For linear first-order systems this filtering causes also a time lag between vertical wind speed and gas signal which is additional to the gas travel time in the sampling line. The effect of this additional time lag on EC fluxes is ignored in current EC data processing routines. Here we show that this oversight biases EC fluxes and hence propose an approach to rectify this bias.
Johannes G. M. Barten, Laurens N. Ganzeveld, Gert-Jan Steeneveld, and Maarten C. Krol
Atmos. Chem. Phys., 21, 10229–10248, https://doi.org/10.5194/acp-21-10229-2021, https://doi.org/10.5194/acp-21-10229-2021, 2021
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We present an evaluation of ocean and snow/ice O3 deposition in explaining observed hourly surface O3 at 25 pan-Arctic sites using an atmospheric meteorology/chemistry model. The model includes a mechanistic representation of ocean O3 deposition as a function of ocean biogeochemical and mixing conditions. The mechanistic representation agrees better with O3 observations in terms of magnitude and temporal variability especially in the High Arctic (> 70° N).
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
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Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Meri Räty, Otso Peräkylä, Matthieu Riva, Lauriane Quéléver, Olga Garmash, Matti Rissanen, and Mikael Ehn
Atmos. Chem. Phys., 21, 7357–7372, https://doi.org/10.5194/acp-21-7357-2021, https://doi.org/10.5194/acp-21-7357-2021, 2021
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Cyclohexene resembles certain relatively complex compounds in the atmosphere that through oxidation produce vapours that take part in aerosol formation. We studied the highly oxygenated organic molecules (HOMs) formed in cyclohexene ozonolysis, the relationship between their chemical composition and their tendency to condense onto seed aerosol, as well as the effect of NOx pollutants on their signals. Two existing models were also tested for their ability to predict the volatility of the HOMs.
Clémence Rose, Matti P. Rissanen, Siddharth Iyer, Jonathan Duplissy, Chao Yan, John B. Nowak, Aurélie Colomb, Régis Dupuy, Xu-Cheng He, Janne Lampilahti, Yee Jun Tham, Daniela Wimmer, Jean-Marc Metzger, Pierre Tulet, Jérôme Brioude, Céline Planche, Markku Kulmala, and Karine Sellegri
Atmos. Chem. Phys., 21, 4541–4560, https://doi.org/10.5194/acp-21-4541-2021, https://doi.org/10.5194/acp-21-4541-2021, 2021
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Sulfuric acid (H2SO4) is commonly accepted as a key precursor for atmospheric new particle formation. However, direct measurements of [H2SO4] remain challenging, motivating the development of proxies. Using data collected in two different volcanic plumes, we show, under these specific conditions, the good performance of a proxy from the literature and also highlight the benefit of the newly developed proxies for the prediction of the highest [H2SO4] values.
Haiyan Li, Manjula R. Canagaratna, Matthieu Riva, Pekka Rantala, Yanjun Zhang, Steven Thomas, Liine Heikkinen, Pierre-Marie Flaud, Eric Villenave, Emilie Perraudin, Douglas Worsnop, Markku Kulmala, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 21, 4123–4147, https://doi.org/10.5194/acp-21-4123-2021, https://doi.org/10.5194/acp-21-4123-2021, 2021
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For the first time, we performed binPMF analysis on the complex mass spectra acquired with the Vocus PTR-TOF in two European pine forests and identified various primary emission sources and secondary oxidation processes of atmospheric organic vapors, i.e., terpenes and their oxidation products, with varying oxidation degrees. Further insights were gained regarding monoterpene and sesquiterpene reactions based on the interpretation results.
Ilona Ylivinkka, Santeri Kaupinmäki, Meri Virman, Maija Peltola, Ditte Taipale, Tuukka Petäjä, Veli-Matti Kerminen, Markku Kulmala, and Ekaterina Ezhova
Atmos. Meas. Tech., 13, 5595–5619, https://doi.org/10.5194/amt-13-5595-2020, https://doi.org/10.5194/amt-13-5595-2020, 2020
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In this study, we developed a new algorithm for cloud classification using solar radiation and cloud base height measurements. Our objective was to develop a simple and inexpensive but effective algorithm for the needs of studies related to ecosystem and atmosphere interactions. In the present study, we used the algorithm for obtaining cloud statistics at a measurement station in southern Finland, and we discuss the advantages and shortcomings of the algorithm.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Wei Wang, Laurens Ganzeveld, Samuel Rossabi, Jacques Hueber, and Detlev Helmig
Atmos. Chem. Phys., 20, 11287–11304, https://doi.org/10.5194/acp-20-11287-2020, https://doi.org/10.5194/acp-20-11287-2020, 2020
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Trees exchange with the atmosphere nitrogen oxides and ozone, affecting the tropospheric composition and consequently air quality and ecosystem health. We examined the leaf-level gas exchanges for four typical tree species (pine, maple, oak, aspen) found in northern Michigan, US. The leaves largely absorb the gases, showing little evidence of emission. We measured the uptake rates that can be used to improve model studies of the source and sink processes controlling these gases in forests.
Johannes G. M. Barten, Laurens N. Ganzeveld, Auke J. Visser, Rodrigo Jiménez, and Maarten C. Krol
Atmos. Chem. Phys., 20, 9441–9458, https://doi.org/10.5194/acp-20-9441-2020, https://doi.org/10.5194/acp-20-9441-2020, 2020
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Combining satellite and urban air pollution measurements with a meteorology and air quality model, we present the state of air quality in Colombia. We found four distinctly different emission regimes. The simulated pollution levels compare well with satellite data, but the comparison also indicates misrepresentation of prescribed fire emissions and simulated lightning emissions. Comparison of urban measurements requires careful consideration of (nocturnal) boundary layer dynamics and advection.
Mario Simon, Lubna Dada, Martin Heinritzi, Wiebke Scholz, Dominik Stolzenburg, Lukas Fischer, Andrea C. Wagner, Andreas Kürten, Birte Rörup, Xu-Cheng He, João Almeida, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Lisa Beck, Anton Bergen, Federico Bianchi, Steffen Bräkling, Sophia Brilke, Lucia Caudillo, Dexian Chen, Biwu Chu, António Dias, Danielle C. Draper, Jonathan Duplissy, Imad El-Haddad, Henning Finkenzeller, Carla Frege, Loic Gonzalez-Carracedo, Hamish Gordon, Manuel Granzin, Jani Hakala, Victoria Hofbauer, Christopher R. Hoyle, Changhyuk Kim, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Bernhard Mentler, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Lauriane L. J. Quéléver, Ananth Ranjithkumar, Matti P. Rissanen, Simon Schallhart, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee J. Tham, António R. Tomé, Miguel Vazquez-Pufleau, Alexander L. Vogel, Robert Wagner, Mingyi Wang, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, Yusheng Wu, Mao Xiao, Chao Yan, Penglin Ye, Qing Ye, Marcel Zauner-Wieczorek, Xueqin Zhou, Urs Baltensperger, Josef Dommen, Richard C. Flagan, Armin Hansel, Markku Kulmala, Rainer Volkamer, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 9183–9207, https://doi.org/10.5194/acp-20-9183-2020, https://doi.org/10.5194/acp-20-9183-2020, 2020
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Highly oxygenated organic compounds (HOMs) have been identified as key vapors involved in atmospheric new-particle formation (NPF). The molecular distribution, HOM yield, and NPF from α-pinene oxidation experiments were measured at the CLOUD chamber over a wide tropospheric-temperature range. This study shows on a molecular scale that despite the sharp reduction in HOM yield at lower temperatures, the reduced volatility counteracts this effect and leads to an overall increase in the NPF rate.
Yuan Yang, Yonghong Wang, Putian Zhou, Dan Yao, Dongsheng Ji, Jie Sun, Yinghong Wang, Shuman Zhao, Wei Huang, Shuanghong Yang, Dean Chen, Wenkang Gao, Zirui Liu, Bo Hu, Renjian Zhang, Limin Zeng, Maofa Ge, Tuukka Petäjä, Veli-Matti Kerminen, Markku Kulmala, and Yuesi Wang
Atmos. Chem. Phys., 20, 8181–8200, https://doi.org/10.5194/acp-20-8181-2020, https://doi.org/10.5194/acp-20-8181-2020, 2020
Dominik Stolzenburg, Mario Simon, Ananth Ranjithkumar, Andreas Kürten, Katrianne Lehtipalo, Hamish Gordon, Sebastian Ehrhart, Henning Finkenzeller, Lukas Pichelstorfer, Tuomo Nieminen, Xu-Cheng He, Sophia Brilke, Mao Xiao, António Amorim, Rima Baalbaki, Andrea Baccarini, Lisa Beck, Steffen Bräkling, Lucía Caudillo Murillo, Dexian Chen, Biwu Chu, Lubna Dada, António Dias, Josef Dommen, Jonathan Duplissy, Imad El Haddad, Lukas Fischer, Loic Gonzalez Carracedo, Martin Heinritzi, Changhyuk Kim, Theodore K. Koenig, Weimeng Kong, Houssni Lamkaddam, Chuan Ping Lee, Markus Leiminger, Zijun Li, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Tatjana Müller, Wei Nie, Eva Partoll, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Matti P. Rissanen, Birte Rörup, Siegfried Schobesberger, Simone Schuchmann, Jiali Shen, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, António Tomé, Miguel Vazquez-Pufleau, Andrea C. Wagner, Mingyi Wang, Yonghong Wang, Stefan K. Weber, Daniela Wimmer, Peter J. Wlasits, Yusheng Wu, Qing Ye, Marcel Zauner-Wieczorek, Urs Baltensperger, Kenneth S. Carslaw, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Armin Hansel, Markku Kulmala, Jos Lelieveld, Rainer Volkamer, Jasper Kirkby, and Paul M. Winkler
Atmos. Chem. Phys., 20, 7359–7372, https://doi.org/10.5194/acp-20-7359-2020, https://doi.org/10.5194/acp-20-7359-2020, 2020
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Sulfuric acid is a major atmospheric vapour for aerosol formation. If new particles grow fast enough, they can act as cloud droplet seeds or affect air quality. In a controlled laboratory set-up, we demonstrate that van der Waals forces enhance growth from sulfuric acid. We disentangle the effects of ammonia, ions and particle hydration, presenting a complete picture of sulfuric acid growth from molecular clusters onwards. In a climate model, we show its influence on the global aerosol budget.
Dean Chen, Putian Zhou, Tuomo Nieminen, Pontus Roldin, Ximeng Qi, Petri Clusius, Carlton Xavier, Lukas Pichelstorfer, Markku Kulmala, Pekka Rantala, Juho Aalto, Nina Sarnela, Pasi Kolari, Petri Keronen, Matti P. Rissanen, Metin Baykara, and Michael Boy
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-128, https://doi.org/10.5194/acp-2020-128, 2020
Preprint withdrawn
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Atmospheric oxidants OH, O3 and NO3 dominate the atmospheric oxidation capacity, and sulfuric acid (H2SO4) is considered as a main driver for new particle formation events. We studied how the trends of these atmospheric oxidants and H2SO4 changed in southern Finland during the past 12 years and discussed how these trends related to decreasing emissions of air pollutants in Europe. Our results showed that OH increased by 1.56 % yr−1 at daytime and NO3 decreased by 3.92 % yr−1 at nighttime.
Liine Heikkinen, Mikko Äijälä, Matthieu Riva, Krista Luoma, Kaspar Dällenbach, Juho Aalto, Pasi Aalto, Diego Aliaga, Minna Aurela, Helmi Keskinen, Ulla Makkonen, Pekka Rantala, Markku Kulmala, Tuukka Petäjä, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 20, 3151–3180, https://doi.org/10.5194/acp-20-3151-2020, https://doi.org/10.5194/acp-20-3151-2020, 2020
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Atmospheric aerosols are solid or liquid particles suspended in the air. They are known as a health risk, but they also influence the Earth's climate. The composition of aerosols becomes important when predicting their effect on climate. We show both seasonal and year-to-year variability of aerosol chemical composition in the boreal forest of Finland. We observed a consistent bimodal seasonal trend: a biogenic summertime maximum and an anthropogenic wintertime maximum in the mass concentration.
Haiyan Li, Matthieu Riva, Pekka Rantala, Liine Heikkinen, Kaspar Daellenbach, Jordan E. Krechmer, Pierre-Marie Flaud, Douglas Worsnop, Markku Kulmala, Eric Villenave, Emilie Perraudin, Mikael Ehn, and Federico Bianchi
Atmos. Chem. Phys., 20, 1941–1959, https://doi.org/10.5194/acp-20-1941-2020, https://doi.org/10.5194/acp-20-1941-2020, 2020
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We deployed the recently developed Vocus PTR-TOF in the French Landes forest during summertime to gain insights into terpene chemistry. In addition to isoprene, monoterpenes, sesquiterpenes, and the low-volatility diterpenes, various terpene reaction products are characterized. Through the analysis of terpene chemistry, we demonstrate the capability of the Vocus PTR-TOF for the detection of oxidized reaction products, highlighting its importance in investigating atmospheric oxidation processes.
Ditte Taipale, Juho Aalto, Pauliina Schiestl-Aalto, Markku Kulmala, and Jaana Bäck
Biogeosciences Discuss., https://doi.org/10.5194/bg-2019-502, https://doi.org/10.5194/bg-2019-502, 2020
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Olga Garmash, Matti P. Rissanen, Iida Pullinen, Sebastian Schmitt, Oskari Kausiala, Ralf Tillmann, Defeng Zhao, Carl Percival, Thomas J. Bannan, Michael Priestley, Åsa M. Hallquist, Einhard Kleist, Astrid Kiendler-Scharr, Mattias Hallquist, Torsten Berndt, Gordon McFiggans, Jürgen Wildt, Thomas F. Mentel, and Mikael Ehn
Atmos. Chem. Phys., 20, 515–537, https://doi.org/10.5194/acp-20-515-2020, https://doi.org/10.5194/acp-20-515-2020, 2020
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Highly oxygenated organic molecules (HOMs) facilitate aerosol formation in the atmosphere. Using NO3− chemical ionization mass spectrometry we investigated HOM composition and yield in oxidation of aromatic compounds at different reactant concentrations, in the presence of NOx and seed aerosol. Higher OH concentrations increased HOM yield, suggesting multiple oxidation steps, and affected HOM composition, potentially explaining in part discrepancies in published secondary organic aerosol yields.
Yonghong Wang, Miao Yu, Yuesi Wang, Guiqian Tang, Tao Song, Putian Zhou, Zirui Liu, Bo Hu, Dongsheng Ji, Lili Wang, Xiaowan Zhu, Chao Yan, Mikael Ehn, Wenkang Gao, Yuepeng Pan, Jinyuan Xin, Yang Sun, Veli-Matti Kerminen, Markku Kulmala, and Tuukka Petäjä
Atmos. Chem. Phys., 20, 45–53, https://doi.org/10.5194/acp-20-45-2020, https://doi.org/10.5194/acp-20-45-2020, 2020
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We found a positive particle matter-mixing layer height feedback at three observation platforms at the 325 m Beijing meteorology tower, which is characterized by a shallower mixing layer height and a higher particle matter concentration. Measurements of solar radiation, aerosol chemical composition, meteorology parameters, trace gases and turbulent kinetic energy (TKE) could explain the feedback mechanism to some extent.
Matti P. Rissanen, Jyri Mikkilä, Siddharth Iyer, and Jani Hakala
Atmos. Meas. Tech., 12, 6635–6646, https://doi.org/10.5194/amt-12-6635-2019, https://doi.org/10.5194/amt-12-6635-2019, 2019
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A novel chemical ionization methodology for rapid gas–phase environmental monitoring is presented. The usefulness of the new inlet design is demonstrated by measuring various aerosol precursor compounds that are present at very low concentrations by using two consecutive ionization schemes. This new inlet enables the detection of a wide range of compounds of interest with a minimum of effort and at a fast repetition rate.
Arnaud P. Praplan, Toni Tykkä, Dean Chen, Michael Boy, Ditte Taipale, Ville Vakkari, Putian Zhou, Tuukka Petäjä, and Heidi Hellén
Atmos. Chem. Phys., 19, 14431–14453, https://doi.org/10.5194/acp-19-14431-2019, https://doi.org/10.5194/acp-19-14431-2019, 2019
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Our study shows that, despite our best efforts and recent progress, our knowledge of the chemical composition of the air under the canopy of a boreal forest still cannot be fully characterized. The discrepancy between the measured total reactivity of the air and the reactivity derived from the known chemical composition highlights the need to better understand the emissions from vegetation, but also other sources, such as the forest soil.
Carlton Xavier, Anton Rusanen, Putian Zhou, Chen Dean, Lukas Pichelstorfer, Pontus Roldin, and Michael Boy
Atmos. Chem. Phys., 19, 13741–13758, https://doi.org/10.5194/acp-19-13741-2019, https://doi.org/10.5194/acp-19-13741-2019, 2019
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Master Chemical Mechanism (MCM) coupled to peroxy radical autoxidation mechanism (PRAM) was used to simulate secondary organic aerosol mass loadings from oxidation of five selected biogenic volatile organic compounds. The simulations were designed to replicate idealized chamber and oxidative flow-tube setups. The mass yields using MCM + PRAM are in good agreement with the experimental yields, thereby allowing us to highlight a few important compounds which contribute to > 95 % of mass loadings.
Auke J. Visser, K. Folkert Boersma, Laurens N. Ganzeveld, and Maarten C. Krol
Atmos. Chem. Phys., 19, 11821–11841, https://doi.org/10.5194/acp-19-11821-2019, https://doi.org/10.5194/acp-19-11821-2019, 2019
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Health and ecosystem impacts of O3 generally occur when O3 concentrations are highest, but most air quality models underestimate peak O3. We derived European NOx emissions based on satellite NO2 column data and evaluated the impact on model-simulated NO2 and ozone. We show that a simulation with satellite-derived NOx emissions leads to better agreement with independent in situ observations of surface NO2 and O3, which helps to reduce the model underestimations of peak ozone concentrations.
Matthieu Riva, Pekka Rantala, Jordan E. Krechmer, Otso Peräkylä, Yanjun Zhang, Liine Heikkinen, Olga Garmash, Chao Yan, Markku Kulmala, Douglas Worsnop, and Mikael Ehn
Atmos. Meas. Tech., 12, 2403–2421, https://doi.org/10.5194/amt-12-2403-2019, https://doi.org/10.5194/amt-12-2403-2019, 2019
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The impact of aerosol particles on climate and air quality remains poorly understood due to multiple factors. One of the current limitations is the incomplete understanding of the contribution of oxygenated species, formed from the oxidation of volatile organic compounds (VOCs) to aerosol formation. Taking advantage of recent mass spectrometric developments, we have evaluated and compared the capability of multiple state-of-the-art mass spectrometers to detect a wide variety of oxygenated VOCs.
Nikos Kalivitis, Veli-Matti Kerminen, Giorgos Kouvarakis, Iasonas Stavroulas, Evaggelia Tzitzikalaki, Panayiotis Kalkavouras, Nikos Daskalakis, Stelios Myriokefalitakis, Aikaterini Bougiatioti, Hanna E. Manninen, Pontus Roldin, Tuukka Petäjä, Michael Boy, Markku Kulmala, Maria Kanakidou, and Nikolaos Mihalopoulos
Atmos. Chem. Phys., 19, 2671–2686, https://doi.org/10.5194/acp-19-2671-2019, https://doi.org/10.5194/acp-19-2671-2019, 2019
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New particle formation (NPF) is an important source of atmospheric aerosols. For the Mediterranean atmosphere, only few studies exist. In this study we present one of the longest series of NPF by analyzing 10 years of data from Crete, Greece. NPF took place on 27 % of the available days; it was more frequent in spring and less so in late summer. Model simulations showed that NPF in the subtropical environment may differ greatly from that in the boreal environment.
Michael Boy, Erik S. Thomson, Juan-C. Acosta Navarro, Olafur Arnalds, Ekaterina Batchvarova, Jaana Bäck, Frank Berninger, Merete Bilde, Zoé Brasseur, Pavla Dagsson-Waldhauserova, Dimitri Castarède, Maryam Dalirian, Gerrit de Leeuw, Monika Dragosics, Ella-Maria Duplissy, Jonathan Duplissy, Annica M. L. Ekman, Keyan Fang, Jean-Charles Gallet, Marianne Glasius, Sven-Erik Gryning, Henrik Grythe, Hans-Christen Hansson, Margareta Hansson, Elisabeth Isaksson, Trond Iversen, Ingibjorg Jonsdottir, Ville Kasurinen, Alf Kirkevåg, Atte Korhola, Radovan Krejci, Jon Egill Kristjansson, Hanna K. Lappalainen, Antti Lauri, Matti Leppäranta, Heikki Lihavainen, Risto Makkonen, Andreas Massling, Outi Meinander, E. Douglas Nilsson, Haraldur Olafsson, Jan B. C. Pettersson, Nønne L. Prisle, Ilona Riipinen, Pontus Roldin, Meri Ruppel, Matthew Salter, Maria Sand, Øyvind Seland, Heikki Seppä, Henrik Skov, Joana Soares, Andreas Stohl, Johan Ström, Jonas Svensson, Erik Swietlicki, Ksenia Tabakova, Throstur Thorsteinsson, Aki Virkkula, Gesa A. Weyhenmeyer, Yusheng Wu, Paul Zieger, and Markku Kulmala
Atmos. Chem. Phys., 19, 2015–2061, https://doi.org/10.5194/acp-19-2015-2019, https://doi.org/10.5194/acp-19-2015-2019, 2019
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The Nordic Centre of Excellence CRAICC (Cryosphere–Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011–2016, is the largest joint Nordic research and innovation initiative to date and aimed to strengthen research and innovation regarding climate change issues in the Nordic region. The paper presents an overview of the main scientific topics investigated and provides a state-of-the-art comprehensive summary of what has been achieved in CRAICC.
Yuqin Liu, Jiahua Zhang, Putian Zhou, Tao Lin, Juan Hong, Lamei Shi, Fengmei Yao, Jun Wu, Huadong Guo, and Gerrit de Leeuw
Atmos. Chem. Phys., 18, 18187–18202, https://doi.org/10.5194/acp-18-18187-2018, https://doi.org/10.5194/acp-18-18187-2018, 2018
Ekaterina Ezhova, Ilona Ylivinkka, Joel Kuusk, Kaupo Komsaare, Marko Vana, Alisa Krasnova, Steffen Noe, Mikhail Arshinov, Boris Belan, Sung-Bin Park, Jošt Valentin Lavrič, Martin Heimann, Tuukka Petäjä, Timo Vesala, Ivan Mammarella, Pasi Kolari, Jaana Bäck, Üllar Rannik, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 18, 17863–17881, https://doi.org/10.5194/acp-18-17863-2018, https://doi.org/10.5194/acp-18-17863-2018, 2018
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Understanding the connections between aerosols, solar radiation and photosynthesis in terrestrial ecosystems is important for estimates of the CO2 balance in the atmosphere. Atmospheric aerosols and clouds influence solar radiation. In this study, we quantify the aerosol effect on solar radiation in boreal forests and study forest ecosystems response to this change in the radiation conditions. The analysis is based on atmospheric observations from several remote stations in Eurasian forests.
Leena Järvi, Üllar Rannik, Tom V. Kokkonen, Mona Kurppa, Ari Karppinen, Rostislav D. Kouznetsov, Pekka Rantala, Timo Vesala, and Curtis R. Wood
Atmos. Meas. Tech., 11, 5421–5438, https://doi.org/10.5194/amt-11-5421-2018, https://doi.org/10.5194/amt-11-5421-2018, 2018
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Identical EC systems on two sides of a building in central Helsinki were used to assess the uncertainty of the vertical fluxes on the single measurement point from July 2013 to September 2015. Sampling at only one point yielded up to 12% underestimation in the cumulative carbon fluxes; for sensible and latent heat the respective values were up to 5 and 8%. The commonly used statistics, kurtosis and skewness, are not necessarily suitable for filtering out data in a densely built urban area.
Ximeng Qi, Aijun Ding, Pontus Roldin, Zhengning Xu, Putian Zhou, Nina Sarnela, Wei Nie, Xin Huang, Anton Rusanen, Mikael Ehn, Matti P. Rissanen, Tuukka Petäjä, Markku Kulmala, and Michael Boy
Atmos. Chem. Phys., 18, 11779–11791, https://doi.org/10.5194/acp-18-11779-2018, https://doi.org/10.5194/acp-18-11779-2018, 2018
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In this study we simulate the HOM concentrations and discuss their roles in NPF at a remote boreal forest site in Finland and a suburban site in eastern China. We found that sulfuric acid and HOM organonitrate concentrations in the gas phase are significantly higher but other HOM monomers and dimers from monoterpene oxidation are lower in eastern China. This study highlights the need for molecular-scale measurements in improving the understanding of NPF mechanisms in polluted areas.
Ben H. Lee, Felipe D. Lopez-Hilfiker, Emma L. D'Ambro, Putian Zhou, Michael Boy, Tuukka Petäjä, Liqing Hao, Annele Virtanen, and Joel A. Thornton
Atmos. Chem. Phys., 18, 11547–11562, https://doi.org/10.5194/acp-18-11547-2018, https://doi.org/10.5194/acp-18-11547-2018, 2018
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Molecular identities and abundances of organic compounds residing in the gas and particle phases above a Finnish boreal forest are presented. We determined that in each phase, the organic components are categorized into three subgroups based on their behavior in time. Some are more enhanced at night, others during midday, and another around sunrise. Identifying such collective behavior can potentially connect the chemical processes that evolve in time to specific distributions of products.
Ana María Yáñez-Serrano, Anke Christine Nölscher, Efstratios Bourtsoukidis, Eliane Gomes Alves, Laurens Ganzeveld, Boris Bonn, Stefan Wolff, Marta Sa, Marcia Yamasoe, Jonathan Williams, Meinrat O. Andreae, and Jürgen Kesselmeier
Atmos. Chem. Phys., 18, 3403–3418, https://doi.org/10.5194/acp-18-3403-2018, https://doi.org/10.5194/acp-18-3403-2018, 2018
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This study shows the measurements of concentration of different monoterpene species in terms of height, time of day and season. Speciation seems similar during the dry seasons but changes with season. Furthermore, reactivity with the different oxidants demonstrated that a higher abundance of a monoterpene species does not automatically imply higher reactivity and that the most abundant monoterpene may not be the most atmospheric chemically relevant compound.
Nina Sarnela, Tuija Jokinen, Jonathan Duplissy, Chao Yan, Tuomo Nieminen, Mikael Ehn, Siegfried Schobesberger, Martin Heinritzi, Sebastian Ehrhart, Katrianne Lehtipalo, Jasmin Tröstl, Mario Simon, Andreas Kürten, Markus Leiminger, Michael J. Lawler, Matti P. Rissanen, Federico Bianchi, Arnaud P. Praplan, Jani Hakala, Antonio Amorim, Marc Gonin, Armin Hansel, Jasper Kirkby, Josef Dommen, Joachim Curtius, James N. Smith, Tuukka Petäjä, Douglas R. Worsnop, Markku Kulmala, Neil M. Donahue, and Mikko Sipilä
Atmos. Chem. Phys., 18, 2363–2380, https://doi.org/10.5194/acp-18-2363-2018, https://doi.org/10.5194/acp-18-2363-2018, 2018
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Atmospheric trace gases can form small molecular clusters, which can grow to larger sizes through the condensation of vapours. This process is called new particle formation. In this paper we studied the formation of sulfuric acid and highly oxygenated molecules, the key compounds in atmospheric new particle formation, in chamber experiments and introduced a way to simulate these ozonolysis products of α-pinene in a simple manner.
Simon Schallhart, Pekka Rantala, Maija K. Kajos, Juho Aalto, Ivan Mammarella, Taina M. Ruuskanen, and Markku Kulmala
Atmos. Chem. Phys., 18, 815–832, https://doi.org/10.5194/acp-18-815-2018, https://doi.org/10.5194/acp-18-815-2018, 2018
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Emissions of volatile organic compounds (VOCs) have impact to air quality, human health and climate. We investigated the development of VOC exchange in a boreal forest between April and June 2013. VOC exchange and diversity increased towards summer, but over 75 % of the biogenic net exchange was driven by methanol, monoterpenes and acetone only. The boreal forest emitted less than 0.2 % carbon in form of VOCs in relation to the carbon uptake.
Andreas Kürten, Chenxi Li, Federico Bianchi, Joachim Curtius, António Dias, Neil M. Donahue, Jonathan Duplissy, Richard C. Flagan, Jani Hakala, Tuija Jokinen, Jasper Kirkby, Markku Kulmala, Ari Laaksonen, Katrianne Lehtipalo, Vladimir Makhmutov, Antti Onnela, Matti P. Rissanen, Mario Simon, Mikko Sipilä, Yuri Stozhkov, Jasmin Tröstl, Penglin Ye, and Peter H. McMurry
Atmos. Chem. Phys., 18, 845–863, https://doi.org/10.5194/acp-18-845-2018, https://doi.org/10.5194/acp-18-845-2018, 2018
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A recent laboratory study (CLOUD) showed that new particles nucleate efficiently from sulfuric acid and dimethylamine (DMA). The reanalysis of previously published data reveals that the nucleation rates are even faster than previously assumed, i.e., nucleation can proceed at rates that are compatible with collision-controlled new particle formation for atmospheric conditions. This indicates that sulfuric acid–DMA nucleation is likely an important source of particles in the boundary layer.
Carla Frege, Ismael K. Ortega, Matti P. Rissanen, Arnaud P. Praplan, Gerhard Steiner, Martin Heinritzi, Lauri Ahonen, António Amorim, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Martin Breitenlechner, Lubna Dada, António Dias, Jonathan Duplissy, Sebastian Ehrhart, Imad El-Haddad, Lukas Fischer, Claudia Fuchs, Olga Garmash, Marc Gonin, Armin Hansel, Christopher R. Hoyle, Tuija Jokinen, Heikki Junninen, Jasper Kirkby, Andreas Kürten, Katrianne Lehtipalo, Markus Leiminger, Roy Lee Mauldin, Ugo Molteni, Leonid Nichman, Tuukka Petäjä, Nina Sarnela, Siegfried Schobesberger, Mario Simon, Mikko Sipilä, Dominik Stolzenburg, António Tomé, Alexander L. Vogel, Andrea C. Wagner, Robert Wagner, Mao Xiao, Chao Yan, Penglin Ye, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Markku Kulmala, Douglas R. Worsnop, Paul M. Winkler, Josef Dommen, and Urs Baltensperger
Atmos. Chem. Phys., 18, 65–79, https://doi.org/10.5194/acp-18-65-2018, https://doi.org/10.5194/acp-18-65-2018, 2018
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It was recently shown that biogenic highly oxygenated molecules (HOMs) form particles in the absence of sulfuric acid and ions enhance the nucleation rate. Here we compare the molecular composition of positive and negative HOM clusters at 25, 5 and −25 °C. At lower temperatures the HOM average oxygen-to-carbon ratio decreases indicating a reduction in the rate of autoxidation due to rather high activation energy. The experimental findings are supported by quantum chemical calculations.
Xuemeng Chen, Lauriane L. J. Quéléver, Pak L. Fung, Jutta Kesti, Matti P. Rissanen, Jaana Bäck, Petri Keronen, Heikki Junninen, Tuukka Petäjä, Veli-Matti Kerminen, and Markku Kulmala
Atmos. Chem. Phys., 18, 49–63, https://doi.org/10.5194/acp-18-49-2018, https://doi.org/10.5194/acp-18-49-2018, 2018
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We analysed a 20-year-long dataset collected in a Finnish boreal forest at SMEAR II station to investigate the frequency and strength of ozone depletion events. We could identify a number of ozone depletion events that lasted for more than 3 h, mainly in the autumn and winter months. Their occurrence was likely related to the formation of a low mixing layer under the conditions of low temperatures, low wind speeds, high relative humidities and limited intensity of solar radiation.
Robert Wagner, Chao Yan, Katrianne Lehtipalo, Jonathan Duplissy, Tuomo Nieminen, Juha Kangasluoma, Lauri R. Ahonen, Lubna Dada, Jenni Kontkanen, Hanna E. Manninen, Antonio Dias, Antonio Amorim, Paulus S. Bauer, Anton Bergen, Anne-Kathrin Bernhammer, Federico Bianchi, Sophia Brilke, Stephany Buenrostro Mazon, Xuemeng Chen, Danielle C. Draper, Lukas Fischer, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Jani Hakala, Liine Heikkinen, Martin Heinritzi, Victoria Hofbauer, Christopher R. Hoyle, Jasper Kirkby, Andreas Kürten, Alexander N. Kvashnin, Tiia Laurila, Michael J. Lawler, Huajun Mai, Vladimir Makhmutov, Roy L. Mauldin III, Ugo Molteni, Leonid Nichman, Wei Nie, Andrea Ojdanic, Antti Onnela, Felix Piel, Lauriane L. J. Quéléver, Matti P. Rissanen, Nina Sarnela, Simon Schallhart, Kamalika Sengupta, Mario Simon, Dominik Stolzenburg, Yuri Stozhkov, Jasmin Tröstl, Yrjö Viisanen, Alexander L. Vogel, Andrea C. Wagner, Mao Xiao, Penglin Ye, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Richard C. Flagan, Martin Gallagher, Armin Hansel, James N. Smith, António Tomé, Paul M. Winkler, Douglas Worsnop, Mikael Ehn, Mikko Sipilä, Veli-Matti Kerminen, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 17, 15181–15197, https://doi.org/10.5194/acp-17-15181-2017, https://doi.org/10.5194/acp-17-15181-2017, 2017
Federico Bianchi, Olga Garmash, Xucheng He, Chao Yan, Siddharth Iyer, Ida Rosendahl, Zhengning Xu, Matti P. Rissanen, Matthieu Riva, Risto Taipale, Nina Sarnela, Tuukka Petäjä, Douglas R. Worsnop, Markku Kulmala, Mikael Ehn, and Heikki Junninen
Atmos. Chem. Phys., 17, 13819–13831, https://doi.org/10.5194/acp-17-13819-2017, https://doi.org/10.5194/acp-17-13819-2017, 2017
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Naturally charged highly oxidised molecules (HOMs) were characterized using advanced mass spectrometers. Two different classes of compounds, clustered with the nitrate and bisulfate ions, were identified: HOMs containing only carbon, hydrogen and oxygen and nitrogen-containing HOMs or organonitrates (ONs). They exhibit strong diurnal variations where HOMs peak during night and ONs during day. Finally, large clusters containing up to 40 carbon atoms (four oxidized
α-pinene units) were observed.
Mikko Auvinen, Leena Järvi, Antti Hellsten, Üllar Rannik, and Timo Vesala
Geosci. Model Dev., 10, 4187–4205, https://doi.org/10.5194/gmd-10-4187-2017, https://doi.org/10.5194/gmd-10-4187-2017, 2017
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Correct spatial interpretation of a micrometeorological measurement requires the determination of its effective source area, or footprint. In urban areas the use of analytical models becomes highly questionable. This work introduces a computational methodology that enables the generation of footprints for complex urban sites. The methodology is based on conducting high-resolution flow and particle analysis on a model that features a detailed topographic description of a real city environment.
Georgios Tsagkogeorgas, Pontus Roldin, Jonathan Duplissy, Linda Rondo, Jasmin Tröstl, Jay G. Slowik, Sebastian Ehrhart, Alessandro Franchin, Andreas Kürten, Antonio Amorim, Federico Bianchi, Jasper Kirkby, Tuukka Petäjä, Urs Baltensperger, Michael Boy, Joachim Curtius, Richard C. Flagan, Markku Kulmala, Neil M. Donahue, and Frank Stratmann
Atmos. Chem. Phys., 17, 8923–8938, https://doi.org/10.5194/acp-17-8923-2017, https://doi.org/10.5194/acp-17-8923-2017, 2017
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The H2SO4 vapour pressure plays key role in Earth's and Venus' atmospheres. In regions where RH is low and stabilising bases are scarce, H2SO4 can evaporate from particles; however the H2SO4 vapour pressure at low RH is uncertain. To address this, we measured H2SO4 evaporation versus T and RH in the CLOUD chamber and constrained the equilibrium constants for dissociation and dehydration of H2SO4. This study is important for nucleation, particle growth and H2SO4 formation occurring in atmosphere.
Emilie Öström, Zhou Putian, Guy Schurgers, Mikhail Mishurov, Niku Kivekäs, Heikki Lihavainen, Mikael Ehn, Matti P. Rissanen, Theo Kurtén, Michael Boy, Erik Swietlicki, and Pontus Roldin
Atmos. Chem. Phys., 17, 8887–8901, https://doi.org/10.5194/acp-17-8887-2017, https://doi.org/10.5194/acp-17-8887-2017, 2017
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We used a model to study how biogenic volatile organic compounds (BVOCs) emitted from the boreal forest contribute to the formation and growth of particles in the atmosphere. Some of these particles are important climate forcers, acting as seeds for cloud droplet fomation. We implemented a new gas chemistry mechanism that describes how the BVOCs are oxidized and form low-volatility highly oxidized organic molecules. With the new mechanism we are able to accurately predict the particle growth.
Eero Nikinmaa, Tuomo Kalliokoski, Kari Minkkinen, Jaana Bäck, Michael Boy, Yao Gao, Nina Janasik-Honkela, Janne I. Hukkinen, Maarit Kallio, Markku Kulmala, Nea Kuusinen, Annikki Mäkelä, Brent D. Matthies, Mikko Peltoniemi, Risto Sievänen, Ditte Taipale, Lauri Valsta, Anni Vanhatalo, Martin Welp, Luxi Zhou, Putian Zhou, and Frank Berninger
Biogeosciences Discuss., https://doi.org/10.5194/bg-2017-141, https://doi.org/10.5194/bg-2017-141, 2017
Manuscript not accepted for further review
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We estimated the impact of boreal forest management on climate, considering the effects of carbon, albedo, aerosols, and effects of industrial wood use. We made analyses both in current and warmer climate of 2050. The aerosol effect was comparable to that of carbon sequestration. Deciduous trees may have a large potential for mitigation due to their high albedo and aerosol effects. If the forests will be used more intensively and mainly for pulp and energy, the warming influence is clear.
Yuqin Liu, Gerrit de Leeuw, Veli-Matti Kerminen, Jiahua Zhang, Putian Zhou, Wei Nie, Ximeng Qi, Juan Hong, Yonghong Wang, Aijun Ding, Huadong Guo, Olaf Krüger, Markku Kulmala, and Tuukka Petäjä
Atmos. Chem. Phys., 17, 5623–5641, https://doi.org/10.5194/acp-17-5623-2017, https://doi.org/10.5194/acp-17-5623-2017, 2017
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The aerosol effects on warm cloud parameters over the Yangtze River Delta are systematically examined using multi-sensor retrievals. This study shows that the COT–CDR and CWP–CDR relationships are not unique, but are affected by atmospheric aerosol loading. CDR and cloud fraction show different behaviours for low and high AOD. Aerosol–cloud interaction (ACI) is stronger for clouds mixed with smoke aerosol than for clouds mixed with dust. Meteorological conditions play an important role in ACI.
Putian Zhou, Laurens Ganzeveld, Üllar Rannik, Luxi Zhou, Rosa Gierens, Ditte Taipale, Ivan Mammarella, and Michael Boy
Atmos. Chem. Phys., 17, 1361–1379, https://doi.org/10.5194/acp-17-1361-2017, https://doi.org/10.5194/acp-17-1361-2017, 2017
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We implemented a multi-layer O3 dry deposition model in a 1-D model SOSAA to simulate O3 flux and concentration within and above a boreal forest at SMEAR II in Hyytiälä, Finland, in August 2010. The results showed that when RH > 70 % the O3 uptake on leaf wet skin was ~ 51 % to the total deposition at night and ~ 19 % at daytime. The sub-canopy contribution below 4.2 m was ~ 38 % at daytime. The averaged daily chemical contribution to total O3 alteration inside the canopy was less than 10 %.
Michael J. Lawler, Paul M. Winkler, Jaeseok Kim, Lars Ahlm, Jasmin Tröstl, Arnaud P. Praplan, Siegfried Schobesberger, Andreas Kürten, Jasper Kirkby, Federico Bianchi, Jonathan Duplissy, Armin Hansel, Tuija Jokinen, Helmi Keskinen, Katrianne Lehtipalo, Markus Leiminger, Tuukka Petäjä, Matti Rissanen, Linda Rondo, Mario Simon, Mikko Sipilä, Christina Williamson, Daniela Wimmer, Ilona Riipinen, Annele Virtanen, and James N. Smith
Atmos. Chem. Phys., 16, 13601–13618, https://doi.org/10.5194/acp-16-13601-2016, https://doi.org/10.5194/acp-16-13601-2016, 2016
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We present chemical observations of newly formed particles as small as ~ 10 nm from new particle formation experiments using sulfuric acid, dimethylamine, ammonia, and water vapor as gas phase reactants. The nanoparticles were more acidic than expected based on thermodynamic expectations, particularly at the smallest measured sizes. The results suggest rapid surface conversion of SO2 to sulfate and show a marked composition change between 10 and 15 nm, possibly indicating a phase change.
Jenni Kontkanen, Pauli Paasonen, Juho Aalto, Jaana Bäck, Pekka Rantala, Tuukka Petäjä, and Markku Kulmala
Atmos. Chem. Phys., 16, 13291–13307, https://doi.org/10.5194/acp-16-13291-2016, https://doi.org/10.5194/acp-16-13291-2016, 2016
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We developed proxies for estimating the concentrations of monoterpenes and their oxidation products at a boreal forest site in Hyytiälä, Finland. The proxies for the monoterpene concentration include temperature-controlled emissions, dilution and different oxidation processes. The proxies were observed to capture the seasonal and diurnal variation of the monoterpene concentration reasonably well. Our proxies can be used in the analysis of new particle formation and growth in boreal environments.
Üllar Rannik, Olli Peltola, and Ivan Mammarella
Atmos. Meas. Tech., 9, 5163–5181, https://doi.org/10.5194/amt-9-5163-2016, https://doi.org/10.5194/amt-9-5163-2016, 2016
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We review available methods for the random error estimation of turbulent fluxes that are widely used by the flux community. Flux errors are evaluated theoretically as well as via numerical calculations by using measured and simulated records. We recommend two flux random errors with clear physical meaning: the total error resulting from stochastic nature of turbulence, well approximated by the method of Finkelstein and Sims (2001), and the error of the flux due to the instrumental noise.
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.
Ivan Mammarella, Olli Peltola, Annika Nordbo, Leena Järvi, and Üllar Rannik
Atmos. Meas. Tech., 9, 4915–4933, https://doi.org/10.5194/amt-9-4915-2016, https://doi.org/10.5194/amt-9-4915-2016, 2016
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In this study we have performed an inter-comparison between EddyUH and EddyPro, two public and commonly used software packages for eddy covariance data processing and calculation. The aims are to estimate the flux uncertainty due to the use of different software packages, and to assess the most critical processing steps, determining the largest deviations in the calculated fluxes. We focus not only on water vapour and carbon dioxide fluxes, but also on the methane flux.
Mari Pihlatie, Üllar Rannik, Sami Haapanala, Olli Peltola, Narasinha Shurpali, Pertti J. Martikainen, Saara Lind, Niina Hyvönen, Perttu Virkajärvi, Mark Zahniser, and Ivan Mammarella
Biogeosciences, 13, 5471–5485, https://doi.org/10.5194/bg-13-5471-2016, https://doi.org/10.5194/bg-13-5471-2016, 2016
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The sources and sinks of carbon monoxide (CO) in the biosphere are poorly understood. We report the first continuous data series of CO fluxes measured by eddy covariance method in an agricultural bioenergy crop. The CO fluxes were seasonally and diurnally variable demonstrating the parallel consumption and production processes. Radiation was the main driver of CO emissions, and the eddy covariance method was demonstrated as suitable for linking short-term flux dynamics to environmental drivers.
Andrey Glazunov, Üllar Rannik, Victor Stepanenko, Vasily Lykosov, Mikko Auvinen, Timo Vesala, and Ivan Mammarella
Geosci. Model Dev., 9, 2925–2949, https://doi.org/10.5194/gmd-9-2925-2016, https://doi.org/10.5194/gmd-9-2925-2016, 2016
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Large-eddy simulation (LES) and Lagrangian stochastic modeling of passive particle dispersion were applied to the scalar flux footprint determination in the stable atmospheric boundary layer. The footprint functions obtained in LES were compared with the functions calculated with the use of first-order single-particle Lagrangian stochastic models (LSMs) and zeroth-order Lagrangian stochastic models - the random displacement models (RDMs).
Pekka Rantala, Leena Järvi, Risto Taipale, Terhi K. Laurila, Johanna Patokoski, Maija K. Kajos, Mona Kurppa, Sami Haapanala, Erkki Siivola, Tuukka Petäjä, Taina M. Ruuskanen, and Janne Rinne
Atmos. Chem. Phys., 16, 7981–8007, https://doi.org/10.5194/acp-16-7981-2016, https://doi.org/10.5194/acp-16-7981-2016, 2016
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Fluxes of volatile organic compounds (VOCs) were measured above an urban landscape in Helsinki, northern Europe. We found that traffic was a major source for many oxygenated and aromatic VOCs, whereas isoprene originated mostly from the urban vegetation. Overall, the VOC fluxes were quite small in comparison with the earlier urban VOC flux measurements.
Natalia Babkovskaia, Ullar Rannik, Vaughan Phillips, Holger Siebert, Birgit Wehner, and Michael Boy
Atmos. Chem. Phys., 16, 7889–7898, https://doi.org/10.5194/acp-16-7889-2016, https://doi.org/10.5194/acp-16-7889-2016, 2016
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Turbulence, aerosol growth and microphysics of hydrometeors in clouds are intimately coupled. A new modelling approach was applied to quantify this linkage. We study the interaction in the cloud area under transient, high supersaturation conditions, using direct numerical simulations. Analysing the effect of aerosol dynamics on the turbulent kinetic energy and on vertical velocity, we conclude that the presence of aerosol has an effect on vertical motion and tends to reduce downward velocity.
Simon Schallhart, Pekka Rantala, Eiko Nemitz, Ditte Taipale, Ralf Tillmann, Thomas F. Mentel, Benjamin Loubet, Giacomo Gerosa, Angelo Finco, Janne Rinne, and Taina M. Ruuskanen
Atmos. Chem. Phys., 16, 7171–7194, https://doi.org/10.5194/acp-16-7171-2016, https://doi.org/10.5194/acp-16-7171-2016, 2016
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We present ecosystem exchange fluxes from a mixed oak–hornbeam forest in the Po Valley, Italy. Detectable fluxes were observed for 29 compounds, dominated by isoprene, which comprised over 60 % of the upward flux. Methanol seemed to be deposited to dew, as the deposition happened in the early morning. We estimated that up to 30 % of the upward flux of methyl vinyl ketone and methacrolein originated from atmospheric oxidation of isoprene.
W. Joe F. Acton, Simon Schallhart, Ben Langford, Amy Valach, Pekka Rantala, Silvano Fares, Giulia Carriero, Ralf Tillmann, Sam J. Tomlinson, Ulrike Dragosits, Damiano Gianelle, C. Nicholas Hewitt, and Eiko Nemitz
Atmos. Chem. Phys., 16, 7149–7170, https://doi.org/10.5194/acp-16-7149-2016, https://doi.org/10.5194/acp-16-7149-2016, 2016
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Volatile organic compounds (VOCs) represent a large source of reactive carbon in the atmosphere and hence have a significant impact on air quality. It is therefore important that we can accurately quantify their emission. In this paper we use three methods to determine the fluxes of reactive VOCs from a woodland canopy. We show that two different canopy-scale measurement methods give good agreement, whereas estimates based on leaf-level-based emission underestimate isoprene fluxes.
Üllar Rannik, Luxi Zhou, Putian Zhou, Rosa Gierens, Ivan Mammarella, Andrey Sogachev, and Michael Boy
Atmos. Chem. Phys., 16, 3145–3160, https://doi.org/10.5194/acp-16-3145-2016, https://doi.org/10.5194/acp-16-3145-2016, 2016
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Atmospheric boundary layer (ABL) model coupled with detailed atmospheric chemistry and aerosol dynamical model was used to quantify the role of aerosol and ABL dynamics in the vertical transport of aerosols at a pine forest site in southern Finland. Simulations showed that under dynamical conditions the particle fluxes above canopy can significantly deviate from the dry deposition into the canopy. The deviation can be systematic for certain particle sizes over a period of several days.
Xin Huang, Luxi Zhou, Aijun Ding, Ximeng Qi, Wei Nie, Minghuai Wang, Xuguang Chi, Tuukka Petäjä, Veli-Matti Kerminen, Pontus Roldin, Anton Rusanen, Markku Kulmala, and Michael Boy
Atmos. Chem. Phys., 16, 2477–2492, https://doi.org/10.5194/acp-16-2477-2016, https://doi.org/10.5194/acp-16-2477-2016, 2016
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By combining a regional model and a box model, this study simulates new particle formation in Nanjing, China, when the air masses were affected by anthropogenic activities, biogenic emissions, or mixed ocean and continental sources. The simulations reveal that biogenic organic compounds play a vital role in growth of newly formed clusters. This novel combination of two models makes it possible to accomplish new particle formation simulation without direct measurements of all chemical species.
J. Kim, L. Ahlm, T. Yli-Juuti, M. Lawler, H. Keskinen, J. Tröstl, S. Schobesberger, J. Duplissy, A. Amorim, F. Bianchi, N. M. Donahue, R. C. Flagan, J. Hakala, M. Heinritzi, T. Jokinen, A. Kürten, A. Laaksonen, K. Lehtipalo, P. Miettinen, T. Petäjä, M. P. Rissanen, L. Rondo, K. Sengupta, M. Simon, A. Tomé, C. Williamson, D. Wimmer, P. M. Winkler, S. Ehrhart, P. Ye, J. Kirkby, J. Curtius, U. Baltensperger, M. Kulmala, K. E. J. Lehtinen, J. N. Smith, I. Riipinen, and A. Virtanen
Atmos. Chem. Phys., 16, 293–304, https://doi.org/10.5194/acp-16-293-2016, https://doi.org/10.5194/acp-16-293-2016, 2016
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The hygroscopicity of nucleated nanoparticles was measured in the presence of sulfuric acid, sulfuric acid-dimethylamine, and sulfuric acid-organics derived from α-pinene oxidation during CLOUD7 at CERN in 2012. The hygroscopicity parameter κ decreased with increasing particle size, indicating decreasing acidity of particles.
R. L. Mauldin III, M. P. Rissanen, T. Petäjä, and M. Kulmala
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2015-398, https://doi.org/10.5194/amt-2015-398, 2016
Revised manuscript under review for AMT
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The manuscript describes a novel instrument for the measurement of OH, HO2+RO2, and other atmospheric species. The instrument described combines the chemical ionization techniques of nitrate CIMS, OH conversion to H2SO4, HO2+RO2 conversion to H2SO4, and high resolution time of flight mass spectroscopy into one system. By using one instrument to obtain spectra it is possible to compare spectra from the different modes and gain further chemical information towards peak identification.
J. Patokoski, T. M. Ruuskanen, M. K. Kajos, R. Taipale, P. Rantala, J. Aalto, T. Ryyppö, T. Nieminen, H. Hakola, and J. Rinne
Atmos. Chem. Phys., 15, 13413–13432, https://doi.org/10.5194/acp-15-13413-2015, https://doi.org/10.5194/acp-15-13413-2015, 2015
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In this study, main source areas for long-lived VOCs at the boreal forest in SMEAR II were determined. Air masses arriving from eastern and western directions were more polluted than those arriving from the northern direction. The biogenic and anthropogenic influences of three different source profiles were determined. The elevated trace gas concentrations from forest fire episodes were observed clearly in the trajectory analysis.
X. M. Qi, A. J. Ding, W. Nie, T. Petäjä, V.-M. Kerminen, E. Herrmann, Y. N. Xie, L. F. Zheng, H. Manninen, P. Aalto, J. N. Sun, Z. N. Xu, X. G. Chi, X. Huang, M. Boy, A. Virkkula, X.-Q. Yang, C. B. Fu, and M. Kulmala
Atmos. Chem. Phys., 15, 12445–12464, https://doi.org/10.5194/acp-15-12445-2015, https://doi.org/10.5194/acp-15-12445-2015, 2015
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We report 2 years of measurements of submicron particles at the SORPES station and provide a comprehensive understanding of main factors controlling temporal variation of the aerosol size distribution and NPF in eastern China. The number concentrations of total particles at Nanjing were comparable to other Chinese megacities but the frequency of NPF was much higher. Year-to-year differences of meteorological conditions could significantly influence the seasonal cycle of NPF and growth.
M. K. Kajos, P. Rantala, M. Hill, H. Hellén, J. Aalto, J. Patokoski, R. Taipale, C. C. Hoerger, S. Reimann, T. M. Ruuskanen, J. Rinne, and T. Petäjä
Atmos. Meas. Tech., 8, 4453–4473, https://doi.org/10.5194/amt-8-4453-2015, https://doi.org/10.5194/amt-8-4453-2015, 2015
P. Rantala, J. Aalto, R. Taipale, T. M. Ruuskanen, and J. Rinne
Biogeosciences, 12, 5753–5770, https://doi.org/10.5194/bg-12-5753-2015, https://doi.org/10.5194/bg-12-5753-2015, 2015
M. Sipilä, N. Sarnela, T. Jokinen, H. Junninen, J. Hakala, M. P. Rissanen, A. Praplan, M. Simon, A. Kürten, F. Bianchi, J. Dommen, J. Curtius, T. Petäjä, and D. R. Worsnop
Atmos. Meas. Tech., 8, 4001–4011, https://doi.org/10.5194/amt-8-4001-2015, https://doi.org/10.5194/amt-8-4001-2015, 2015
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Atmospheric concentrations of amines are poorly known mainly due to challenges related to their reliable high-sensitivity detection. We have created a method and instrument that is capable for detecting amines with lowest limit of detection of around 0.01 parts per trillion. Application of the instrument in the field study indicates that concentrations of dimethyl amine in a boreal forest site are below 0.03ppt, not enough to account for the observed new particle formation rates.
P. Roldin, L. Liao, D. Mogensen, M. Dal Maso, A. Rusanen, V.-M. Kerminen, T. F. Mentel, J. Wildt, E. Kleist, A. Kiendler-Scharr, R. Tillmann, M. Ehn, M. Kulmala, and M. Boy
Atmos. Chem. Phys., 15, 10777–10798, https://doi.org/10.5194/acp-15-10777-2015, https://doi.org/10.5194/acp-15-10777-2015, 2015
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We used the ADCHAM model to study new particle formation events in the JPAC chamber. The model results show that the new particles may be formed by a kinetic type of nucleation involving both sulphuric acid and organic compounds formed from OH oxidation of volatile organic compounds (VOCs). The observed particle growth may either be controlled by the condensation of semi- and low-volatililty organic compounds or by the formation of low-volatility compounds (oligomers) at the particle surface.
L. Zhou, R. Gierens, A. Sogachev, D. Mogensen, J. Ortega, J. N. Smith, P. C. Harley, A. J. Prenni, E. J. T. Levin, A. Turnipseed, A. Rusanen, S. Smolander, A. B. Guenther, M. Kulmala, T. Karl, and M. Boy
Atmos. Chem. Phys., 15, 8643–8656, https://doi.org/10.5194/acp-15-8643-2015, https://doi.org/10.5194/acp-15-8643-2015, 2015
T. F. Mentel, M. Springer, M. Ehn, E. Kleist, I. Pullinen, T. Kurtén, M. Rissanen, A. Wahner, and J. Wildt
Atmos. Chem. Phys., 15, 6745–6765, https://doi.org/10.5194/acp-15-6745-2015, https://doi.org/10.5194/acp-15-6745-2015, 2015
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We studied a series of cycloalkenes and methyl-substituted alkenes in order to elucidate the structural pre-requisites and chemical pathways to the recently discovered class of highly oxidized molecules ELVOC (Ehn et al., Nature, 2014). ELVOC may totally change the view on (parts of) the mechanism of SOA formation. We present results which support recent observations of H shifts from C-H to peroxy radicals, highlighting the pivotal role of peroxyradicals in organic atmospheric chemistry.
A. P. Praplan, S. Schobesberger, F. Bianchi, M. P. Rissanen, M. Ehn, T. Jokinen, H. Junninen, A. Adamov, A. Amorim, J. Dommen, J. Duplissy, J. Hakala, A. Hansel, M. Heinritzi, J. Kangasluoma, J. Kirkby, M. Krapf, A. Kürten, K. Lehtipalo, F. Riccobono, L. Rondo, N. Sarnela, M. Simon, A. Tomé, J. Tröstl, P. M. Winkler, C. Williamson, P. Ye, J. Curtius, U. Baltensperger, N. M. Donahue, M. Kulmala, and D. R. Worsnop
Atmos. Chem. Phys., 15, 4145–4159, https://doi.org/10.5194/acp-15-4145-2015, https://doi.org/10.5194/acp-15-4145-2015, 2015
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Our study shows, based on data from three atmospheric pressure interface time-of-flight mass spectrometers measuring in parallel charged and neutral molecules and molecular clusters, how oxidised organic compounds bind to inorganic ions (e.g. bisulfate, nitrate, ammonium). This ionisation is selective for compounds with lower molar mass due to their limited amount and variety of functional groups. We also found that extremely low volatile organic compounds (ELVOCs) can be formed immediately.
D. Mogensen, R. Gierens, J. N. Crowley, P. Keronen, S. Smolander, A. Sogachev, A. C. Nölscher, L. Zhou, M. Kulmala, M. J. Tang, J. Williams, and M. Boy
Atmos. Chem. Phys., 15, 3909–3932, https://doi.org/10.5194/acp-15-3909-2015, https://doi.org/10.5194/acp-15-3909-2015, 2015
D. Mogensen and M. Boy
Atmos. Chem. Phys., 15, 3109–3110, https://doi.org/10.5194/acp-15-3109-2015, https://doi.org/10.5194/acp-15-3109-2015, 2015
J. Kaiser, G. M. Wolfe, B. Bohn, S. Broch, H. Fuchs, L. N. Ganzeveld, S. Gomm, R. Häseler, A. Hofzumahaus, F. Holland, J. Jäger, X. Li, I. Lohse, K. Lu, A. S. H. Prévôt, F. Rohrer, R. Wegener, R. Wolf, T. F. Mentel, A. Kiendler-Scharr, A. Wahner, and F. N. Keutsch
Atmos. Chem. Phys., 15, 1289–1298, https://doi.org/10.5194/acp-15-1289-2015, https://doi.org/10.5194/acp-15-1289-2015, 2015
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Using measurements acquired from a Zeppelin airship during the PEGASOS 2012 campaign, we show that VOC oxidation alone cannot account for the formaldehyde concentrations observed in the morning over rural Italy. Vertical profiles suggest a ground-level source of HCHO. Incorporating this additional HCHO source into a photochemical model increases calculated O3 production by as much as 12%.
Ü. Rannik, S. Haapanala, N. J. Shurpali, I. Mammarella, S. Lind, N. Hyvönen, O. Peltola, M. Zahniser, P. J. Martikainen, and T. Vesala
Biogeosciences, 12, 415–432, https://doi.org/10.5194/bg-12-415-2015, https://doi.org/10.5194/bg-12-415-2015, 2015
M. Sipilä, T. Jokinen, T. Berndt, S. Richters, R. Makkonen, N. M. Donahue, R. L. Mauldin III, T. Kurtén, P. Paasonen, N. Sarnela, M. Ehn, H. Junninen, M. P. Rissanen, J. Thornton, F. Stratmann, H. Herrmann, D. R. Worsnop, M. Kulmala, V.-M. Kerminen, and T. Petäjä
Atmos. Chem. Phys., 14, 12143–12153, https://doi.org/10.5194/acp-14-12143-2014, https://doi.org/10.5194/acp-14-12143-2014, 2014
E. Hermansson, P. Roldin, A. Rusanen, D. Mogensen, N. Kivekäs, R. Väänänen, M. Boy, and E. Swietlicki
Atmos. Chem. Phys., 14, 11853–11869, https://doi.org/10.5194/acp-14-11853-2014, https://doi.org/10.5194/acp-14-11853-2014, 2014
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Secondary organic aerosols (SOA), produced through oxidation processes, constitute a large part of the global organic aerosol load and affect the climate. We found that the modeled mass of SOA was highly dependent on how the oxidation processes were explained in models. The results indicated that it was especially important to get the volatility distribution of the products from the first oxidation step right and that fragmentation during the oxidation process played an important role.
S. Smolander, Q. He, D. Mogensen, L. Zhou, J. Bäck, T. Ruuskanen, S. Noe, A. Guenther, H. Aaltonen, M. Kulmala, and M. Boy
Biogeosciences, 11, 5425–5443, https://doi.org/10.5194/bg-11-5425-2014, https://doi.org/10.5194/bg-11-5425-2014, 2014
L. Liao, V.-M. Kerminen, M. Boy, M. Kulmala, and M. Dal Maso
Atmos. Chem. Phys., 14, 8295–8308, https://doi.org/10.5194/acp-14-8295-2014, https://doi.org/10.5194/acp-14-8295-2014, 2014
P. Roldin, A. C. Eriksson, E. Z. Nordin, E. Hermansson, D. Mogensen, A. Rusanen, M. Boy, E. Swietlicki, B. Svenningsson, A. Zelenyuk, and J. Pagels
Atmos. Chem. Phys., 14, 7953–7993, https://doi.org/10.5194/acp-14-7953-2014, https://doi.org/10.5194/acp-14-7953-2014, 2014
J. Kangasluoma, C. Kuang, D. Wimmer, M. P. Rissanen, K. Lehtipalo, M. Ehn, D. R. Worsnop, J. Wang, M. Kulmala, and T. Petäjä
Atmos. Meas. Tech., 7, 689–700, https://doi.org/10.5194/amt-7-689-2014, https://doi.org/10.5194/amt-7-689-2014, 2014
S. P. K. Bowring, L. M. Miller, L. Ganzeveld, and A. Kleidon
Earth Syst. Dynam., 5, 43–53, https://doi.org/10.5194/esd-5-43-2014, https://doi.org/10.5194/esd-5-43-2014, 2014
Z. B. Wang, M. Hu, D. Mogensen, D. L. Yue, J. Zheng, R. Y. Zhang, Y. Liu, B. Yuan, X. Li, M. Shao, L. Zhou, Z. J. Wu, A. Wiedensohler, and M. Boy
Atmos. Chem. Phys., 13, 11157–11167, https://doi.org/10.5194/acp-13-11157-2013, https://doi.org/10.5194/acp-13-11157-2013, 2013
B. Seok, D. Helmig, L. Ganzeveld, M. W. Williams, and C. S. Vogel
Atmos. Chem. Phys., 13, 7301–7320, https://doi.org/10.5194/acp-13-7301-2013, https://doi.org/10.5194/acp-13-7301-2013, 2013
M. Boy, D. Mogensen, S. Smolander, L. Zhou, T. Nieminen, P. Paasonen, C. Plass-Dülmer, M. Sipilä, T. Petäjä, L. Mauldin, H. Berresheim, and M. Kulmala
Atmos. Chem. Phys., 13, 3865–3879, https://doi.org/10.5194/acp-13-3865-2013, https://doi.org/10.5194/acp-13-3865-2013, 2013
Z. B. Wang, M. Hu, Z. J. Wu, D. L. Yue, J. Zheng, R. Y. Zhang, X. Y. Pei, P. Paasonen, M. Dal Maso, M. Boy, and A. Wiedensohler
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-3419-2013, https://doi.org/10.5194/acpd-13-3419-2013, 2013
Revised manuscript not accepted
Ü. Rannik, N. Altimir, I. Mammarella, J. Bäck, J. Rinne, T. M. Ruuskanen, P. Hari, T. Vesala, and M. Kulmala
Atmos. Chem. Phys., 12, 12165–12182, https://doi.org/10.5194/acp-12-12165-2012, https://doi.org/10.5194/acp-12-12165-2012, 2012
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Physics (physical properties and processes)
Observational and model evidence for a prominent stratospheric influence on variability in tropospheric nitrous oxide
Estimation of Canada's methane emissions: inverse modelling analysis using the Environment and Climate Change Canada (ECCC) measurement network
Spatiotemporal source apportionment of ozone pollution over the Greater Bay Area
Potential of 14C-based vs. ΔCO-based ΔffCO2 observations to estimate urban fossil fuel CO2 (ffCO2) emissions
On the uncertainty of anthropogenic aromatic volatile organic compound emissions: model evaluation and sensitivity analysis
A mechanism of stratospheric O3 intrusion into the atmospheric environment: a case study of the North China Plain
Influence of atmospheric circulation on the interannual variability of transport from global and regional emissions into the Arctic
Surface networks in the Arctic may miss a future methane bomb
Flow-dependent observation errors for GHG inversions in an ensemble Kalman smoother
Potential of using CO2 observations over India in a regional carbon budget estimation by improving the modelling system
Tracing the origins of stratospheric ozone intrusions and their impacts on Central and Eastern China: a long-term study of direct and indirect pathways
A bottom-up emission estimate for the 2022 Nord Stream gas leak: derivation, simulations, and evaluation
An improved Trajectory-mapped Ozonesonde dataset for the Stratosphere and Troposphere (TOST): update, validation and applications
European CH4 inversions with ICON-ART coupled to the CarbonTracker Data Assimilation Shell
Extreme weather exacerbates ozone pollution in the Pearl River Delta, China: role of natural processes
Multidecadal ozone trends in China and implications for human health and crop yields: a hybrid approach combining a chemical transport model and machine learning
On the influence of vertical mixing, boundary layer schemes, and temporal emission profiles on tropospheric NO2 in WRF-Chem – comparisons to in situ, satellite, and MAX-DOAS observations
Decreasing trends of ammonia emissions over Europe seen from remote sensing and inverse modelling
The sensitivity of Southern Ocean atmospheric dimethyl sulfide (DMS) to modeled oceanic DMS concentrations and emissions
Impacts of maritime shipping on air pollution along the US East Coast
Understanding greenhouse gas (GHG) column concentrations in Munich using the Weather Research and Forecasting (WRF) model
Impact of transport model resolution and a priori assumptions on inverse modeling of Swiss F-gas emissions
Estimation of power plant SO2 emissions using the HYSPLIT dispersion model and airborne observations with plume rise ensemble runs
Can we use atmospheric CO2 measurements to verify emission trends reported by cities? Lessons from a 6-year atmospheric inversion over Paris
A new steady-state gas–particle partitioning model of polycyclic aromatic hydrocarbons: implication for the influence of the particulate proportion in emissions
An analysis of CMAQ gas-phase dry deposition over North America through grid-scale and land-use-specific diagnostics in the context of AQMEII4
Rethinking the role of transport and photochemistry in regional ozone pollution: insights from ozone concentration and mass budgets
Decreasing seasonal cycle amplitude of methane in the northern high latitudes being driven by lower-latitude changes in emissions and transport
The effect of anthropogenic emission, meteorological factors, and carbon dioxide on the surface ozone increase in China from 2008 to 2018 during the East Asia summer monsoon season
Development of a CMAQ–PMF-based composite index for prescribing an effective ozone abatement strategy: a case study of sensitivity of surface ozone to precursor volatile organic compound species in southern Taiwan
Comment on “Climate consequences of hydrogen emissions” by Ocko and Hamburg (2022)
Constraining emissions of volatile organic compounds from western US wildfires with WE-CAN and FIREX-AQ airborne observations
Satellite quantification of methane emissions and oil–gas methane intensities from individual countries in the Middle East and North Africa: implications for climate action
Coupled mesoscale–microscale modeling of air quality in a polluted city using WRF-LES-Chem
Impact of aerosol optics on vertical distribution of ozone in autumn over Yangtze River Delta
A view of the European carbon flux landscape through the lens of the ICOS atmospheric observation network
Technical note: The CAMS greenhouse gas reanalysis from 2003 to 2020
Evaluation of simulated CO2 power plant plumes from six high-resolution atmospheric transport models
Impacts of urbanization on air quality and the related health risks in a city with complex terrain
Optimizing 4 years of CO2 biospheric fluxes from OCO-2 and in situ data in TM5: fire emissions from GFED and inferred from MOPITT CO data
Development and application of a multi-scale modeling framework for urban high-resolution NO2 pollution mapping
Towards monitoring the CO2 source–sink distribution over India via inverse modelling: quantifying the fine-scale spatiotemporal variability in the atmospheric CO2 mole fraction
Methane emissions from China: a high-resolution inversion of TROPOMI satellite observations
Estimated regional CO2 flux and uncertainty based on an ensemble of atmospheric CO2 inversions
Assessing the representativity of NH3 measurements influenced by boundary-layer dynamics and the turbulent dispersion of a nearby emission source
Analysis of CO2, CH4, and CO surface and column concentrations observed at Réunion Island by assessing WRF-Chem simulations
Technical note: Interpretation of field observations of point-source methane plume using observation-driven large-eddy simulations
Quantifying fossil fuel methane emissions using observations of atmospheric ethane and an uncertain emission ratio
The impact of peripheral circulation characteristics of typhoon on sustained ozone episodes over the Pearl River Delta region, China
Updated Global Fuel Exploitation Inventory (GFEI) for methane emissions from the oil, gas, and coal sectors: evaluation with inversions of atmospheric methane observations
Cynthia D. Nevison, Qing Liang, Paul A. Newman, Britton B. Stephens, Geoff Dutton, Xin Lan, Roisin Commane, Yenny Gonzalez, and Eric Kort
Atmos. Chem. Phys., 24, 10513–10529, https://doi.org/10.5194/acp-24-10513-2024, https://doi.org/10.5194/acp-24-10513-2024, 2024
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This study examines the drivers of interannual variability in tropospheric N2O. New insights are obtained from aircraft data and a chemistry–climate model that explicitly simulates stratospheric N2O. The stratosphere is found to be the dominant driver of N2O variability in the Northern Hemisphere, while both the stratosphere and El Niño cycles are important in the Southern Hemisphere. These results are consistent with known atmospheric dynamics and differences between the hemispheres.
Misa Ishizawa, Douglas Chan, Doug Worthy, Elton Chan, Felix Vogel, Joe R. Melton, and Vivek K. Arora
Atmos. Chem. Phys., 24, 10013–10038, https://doi.org/10.5194/acp-24-10013-2024, https://doi.org/10.5194/acp-24-10013-2024, 2024
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Methane (CH4) emissions in Canada for 2007–2017 were estimated using Canada’s surface greenhouse gas measurements. The estimated emissions show no significant trend, but emission uncertainty was reduced as more measurement sites became available. Notably for climate change, we find the wetland CH4 emissions show a positive correlation with surface air temperature in summer. Canada’s measurement network could monitor future CH4 emission changes and compliance with climate change mitigation goals.
Yiang Chen, Xingcheng Lu, and Jimmy C. H. Fung
Atmos. Chem. Phys., 24, 8847–8864, https://doi.org/10.5194/acp-24-8847-2024, https://doi.org/10.5194/acp-24-8847-2024, 2024
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This study investigates the contribution of pollutants from different emitting periods to ozone episodes over the Greater Bay Area. The analysis reveals the variation in major spatiotemporal contributors to the O3 pollution under the influence of typhoons and subtropical high pressure. Through temporal contribution analysis, our work offers a new perspective on the evolution of O3 pollution and can aid in developing effective and timely control policies under unfavorable weather conditions.
Fabian Maier, Christian Rödenbeck, Ingeborg Levin, Christoph Gerbig, Maksym Gachkivskyi, and Samuel Hammer
Atmos. Chem. Phys., 24, 8183–8203, https://doi.org/10.5194/acp-24-8183-2024, https://doi.org/10.5194/acp-24-8183-2024, 2024
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We investigate the usage of discrete radiocarbon (14C)-based fossil fuel carbon dioxide (ffCO2) concentration estimates vs. continuous carbon monoxide (CO)-based ffCO2 estimates to evaluate the seasonal cycle of ffCO2 emissions in an urban region with an inverse modeling framework. We find that the CO-based ffCO2 estimates allow us to reconstruct robust seasonal cycles, which show the distinct COVID-19 drawdown in 2020 and can be used to validate emission inventories.
Kevin Oliveira, Marc Guevara, Oriol Jorba, Hervé Petetin, Dene Bowdalo, Carles Tena, Gilbert Montané Pinto, Franco López, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 7137–7177, https://doi.org/10.5194/acp-24-7137-2024, https://doi.org/10.5194/acp-24-7137-2024, 2024
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In this work, we assess and evaluate benzene, toluene, and xylene primary emissions and air quality levels in Spain by combining observations, emission inventories, and air quality modelling techniques. The comparison between modelled and observed levels allows identifying uncertainty sources within the emission input. This contributes to improving air quality models' performance when simulating these compounds, leading to better support for the design of effective pollution control strategies.
Yuehan Luo, Tianliang Zhao, Kai Meng, Jun Hu, Qingjian Yang, Yongqing Bai, Kai Yang, Weikang Fu, Chenghao Tan, Yifan Zhang, Yanzhe Zhang, and Zhikuan Li
Atmos. Chem. Phys., 24, 7013–7026, https://doi.org/10.5194/acp-24-7013-2024, https://doi.org/10.5194/acp-24-7013-2024, 2024
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We reveal a significant mechanism of stratospheric O3 intrusion (SI) into the atmospheric environment induced by an extratropical cyclone system. This system facilitates the downward transport of stratospheric O3 to the near-surface layer by vertical coupling, involving the upper westerly trough, the middle northeast cold vortex, and the lower extratropical cyclone in the troposphere. On average, stratospheric O3 contributed 26.77 % to near-surface O3 levels over the North China Plain.
Cheng Zheng, Yutian Wu, Mingfang Ting, and Clara Orbe
Atmos. Chem. Phys., 24, 6965–6985, https://doi.org/10.5194/acp-24-6965-2024, https://doi.org/10.5194/acp-24-6965-2024, 2024
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Trace gases and aerosols in the Arctic, which typically originate from midlatitude and tropical emission regions, modulate the Arctic climate via their radiative and chemistry impacts. Thus, long-range transport of these substances is important for understanding the current and the future change of Arctic climate. By employing chemistry–climate models, we explore how year-to-year variations in the atmospheric circulation modulate atmospheric long-range transport into the Arctic.
Sophie Wittig, Antoine Berchet, Isabelle Pison, Marielle Saunois, and Jean-Daniel Paris
Atmos. Chem. Phys., 24, 6359–6373, https://doi.org/10.5194/acp-24-6359-2024, https://doi.org/10.5194/acp-24-6359-2024, 2024
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The aim of this work is to analyse how accurately a methane bomb event could be detected with the current and a hypothetically extended stationary observation network in the Arctic. For this, we incorporate synthetically modelled possible future CH4 concentrations based on plausible emission scenarios into an inverse modelling framework. We analyse how well the increase is detected in different Arctic regions and evaluate the impact of additional observation sites in this respect.
Michael Steiner, Luca Cantarello, Stephan Henne, and Dominik Brunner
EGUsphere, https://doi.org/10.5194/egusphere-2024-1426, https://doi.org/10.5194/egusphere-2024-1426, 2024
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Atmospheric GHG inversions have great potential to independently check reported bottom-up emissions, however they are still subject to large uncertainties. It is therefore paramount to address and reduce the largest source of uncertainty stemming from the representation of atmospheric transport in the models. In this study, we show that the use of a temporally varying, flow-dependent atmospheric transport uncertainty can enhance the accuracy of emission estimation through idealized experiment.
Vishnu Thilakan, Dhanyalekshmi Pillai, Jithin Sukumaran, Christoph Gerbig, Haseeb Hakkim, Vinayak Sinha, Yukio Terao, Manish Naja, and Monish Vijay Deshpande
Atmos. Chem. Phys., 24, 5315–5335, https://doi.org/10.5194/acp-24-5315-2024, https://doi.org/10.5194/acp-24-5315-2024, 2024
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This study investigates the usability of CO2 mixing ratio observations over India to infer regional carbon sources and sinks. We demonstrate that a high-resolution modelling system can represent the observed CO2 variations reasonably well by improving the transport and flux variations at a fine scale. Future carbon data assimilation systems can thus benefit from these recently available CO2 observations when fine-scale variations are adequately represented in the models.
Kai Meng, Tianliang Zhao, Yongqing Bai, Le Cao, Ming Wu, Xuewei Hou, and Yuehan Luo
EGUsphere, https://doi.org/10.5194/egusphere-2024-930, https://doi.org/10.5194/egusphere-2024-930, 2024
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We studied the impact of stratospheric intrusions on tropospheric and near-surface ozone in Central and Eastern China from a stratospheric sources tracing perspective. SIs contribute the most in the eastern plains, with a contribution exceeding 15 %, while their contribution to the western and southern parts is small. Western Siberia and Mongolia are the most critical source areas for indirect and direct SIs respectively, with the Rossby wave and NECV being important driving circulation systems.
Rostislav Kouznetsov, Risto Hänninen, Andreas Uppstu, Evgeny Kadantsev, Yalda Fatahi, Marje Prank, Dmitrii Kouznetsov, Steffen Manfred Noe, Heikki Junninen, and Mikhail Sofiev
Atmos. Chem. Phys., 24, 4675–4691, https://doi.org/10.5194/acp-24-4675-2024, https://doi.org/10.5194/acp-24-4675-2024, 2024
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By relying solely on publicly available media reports, we were able to infer the temporal evolution and the injection height for the Nord Stream gas leaks in September 2022. The inventory specifies locations, vertical distributions, and temporal evolution of the methane sources. The inventory can be used to simulate the event with atmospheric transport models. The inventory is supplemented with a set of observational data tailored to evaluate the results of the simulated atmospheric dispersion.
Zhou Zang, Jane Liu, David Tarasick, Omid Moeini, Jianchun Bian, Jinqiang Zhang, Anne M. Thompson, Roeland Van Malderen, Herman G. J. Smit, Ryan M. Stauffer, Bryan J. Johnson, and Debra E. Kollonige
EGUsphere, https://doi.org/10.5194/egusphere-2024-800, https://doi.org/10.5194/egusphere-2024-800, 2024
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The Trajectory-mapped Ozonesonde dataset for the Stratosphere and Troposphere (TOST) provides a global-scale, long-term ozone climatology that is horizontally- and vertically-resolved. In this study, we improved, updated, and validated the TOST from 1970 to 2021. Based on this TOST dataset, we characterized global ozone variations spatially in both the troposphere and stratosphere and temporally by season and decade. We also showed a stagnant stratospheric ozone variation since the late 1990s.
Michael Steiner, Wouter Peters, Ingrid Luijkx, Stephan Henne, Huilin Chen, Samuel Hammer, and Dominik Brunner
Atmos. Chem. Phys., 24, 2759–2782, https://doi.org/10.5194/acp-24-2759-2024, https://doi.org/10.5194/acp-24-2759-2024, 2024
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The Paris Agreement increased interest in estimating greenhouse gas (GHG) emissions of individual countries, but top-down emission estimation is not yet considered policy-relevant. It is therefore paramount to reduce large errors and to build systems that are based on the newest atmospheric transport models. In this study, we present the first application of ICON-ART in the inverse modeling of GHG fluxes with an ensemble Kalman filter and present our results for European CH4 emissions.
Nan Wang, Hongyue Wang, Xin Huang, Xi Chen, Yu Zou, Tao Deng, Tingyuan Li, Xiaopu Lyu, and Fumo Yang
Atmos. Chem. Phys., 24, 1559–1570, https://doi.org/10.5194/acp-24-1559-2024, https://doi.org/10.5194/acp-24-1559-2024, 2024
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This study explores the influence of extreme-weather-induced natural processes on ozone pollution, which is often overlooked. By analyzing meteorological factors, natural emissions, chemistry pathways and atmospheric transport, we discovered that these natural processes could substantially exacerbate ozone pollution. The findings contribute to a deeper understanding of ozone pollution and offer valuable insights for controlling ozone pollution in the context of global warming.
Jia Mao, Amos P. K. Tai, David H. Y. Yung, Tiangang Yuan, Kong T. Chau, and Zhaozhong Feng
Atmos. Chem. Phys., 24, 345–366, https://doi.org/10.5194/acp-24-345-2024, https://doi.org/10.5194/acp-24-345-2024, 2024
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Surface ozone (O3) is well-known for posing great threats to both human health and agriculture worldwide. However, a multidecadal assessment of the impacts of O3 on public health and agriculture in China is lacking without sufficient O3 observations. We used a hybrid approach combining a chemical transport model and machine learning to provide a robust dataset of O3 concentrations over the past 4 decades in China, thereby filling the gap in the long-term O3 trend and impact assessment in China.
Leon Kuhn, Steffen Beirle, Vinod Kumar, Sergey Osipov, Andrea Pozzer, Tim Bösch, Rajesh Kumar, and Thomas Wagner
Atmos. Chem. Phys., 24, 185–217, https://doi.org/10.5194/acp-24-185-2024, https://doi.org/10.5194/acp-24-185-2024, 2024
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NO₂ is an important air pollutant. It was observed that the WRF-Chem model shows significant deviations in NO₂ abundance when compared to measurements. We use a 1-month simulation over central Europe to show that these deviations can be mostly resolved by reparameterization of the vertical mixing routine. In order to validate our results, they are compared to in situ, satellite, and MAX-DOAS measurements.
Ondřej Tichý, Sabine Eckhardt, Yves Balkanski, Didier Hauglustaine, and Nikolaos Evangeliou
Atmos. Chem. Phys., 23, 15235–15252, https://doi.org/10.5194/acp-23-15235-2023, https://doi.org/10.5194/acp-23-15235-2023, 2023
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We show declining trends in NH3 emissions over Europe for 2013–2020 using advanced dispersion and inverse modelling and satellite measurements from CrIS. Emissions decreased by −26% since 2013, showing that the abatement strategies adopted by the European Union have been very efficient. Ammonia emissions are low in winter and peak in summer due to temperature-dependent soil volatilization. The largest decreases were observed in central and western Europe in countries with high emissions.
Yusuf A. Bhatti, Laura E. Revell, Alex J. Schuddeboom, Adrian J. McDonald, Alex T. Archibald, Jonny Williams, Abhijith U. Venugopal, Catherine Hardacre, and Erik Behrens
Atmos. Chem. Phys., 23, 15181–15196, https://doi.org/10.5194/acp-23-15181-2023, https://doi.org/10.5194/acp-23-15181-2023, 2023
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Aerosols are a large source of uncertainty over the Southern Ocean. A dominant source of sulfate aerosol in this region is dimethyl sulfide (DMS), which is poorly simulated by climate models. We show the sensitivity of simulated atmospheric DMS to the choice of oceanic DMS data set and emission scheme. We show that oceanic DMS has twice the influence on atmospheric DMS than the emission scheme. Simulating DMS more accurately in climate models will help to constrain aerosol uncertainty.
Maryam Golbazi and Cristina Archer
Atmos. Chem. Phys., 23, 15057–15075, https://doi.org/10.5194/acp-23-15057-2023, https://doi.org/10.5194/acp-23-15057-2023, 2023
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We use scientific models to study the impact of ship emissions on air quality along the US East Coast. We find an increase in three major pollutants (PM2.5, NO2, and SO2) in coastal regions. However, we detect a reduction in ozone (O3) levels in major coastal cities. This reduction is linked to the significant emissions of nitrogen oxides (NOx) from ships, which scavenged O3, especially in highly polluted urban areas experiencing an NOx-limited regime.
Xinxu Zhao, Jia Chen, Julia Marshall, Michal Gałkowski, Stephan Hachinger, Florian Dietrich, Ankit Shekhar, Johannes Gensheimer, Adrian Wenzel, and Christoph Gerbig
Atmos. Chem. Phys., 23, 14325–14347, https://doi.org/10.5194/acp-23-14325-2023, https://doi.org/10.5194/acp-23-14325-2023, 2023
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We develop a modeling framework using the Weather Research and Forecasting model at a high spatial resolution (up to 400 m) to simulate atmospheric transport of greenhouse gases and interpret column observations. Output is validated against weather stations and column measurements in August 2018. The differential column method is applied, aided by air-mass transport tracing with the Stochastic Time-Inverted Lagrangian Transport (STILT) model, also for an exploratory measurement interpretation.
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
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The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
Tianfeng Chai, Xinrong Ren, Fong Ngan, Mark Cohen, and Alice Crawford
Atmos. Chem. Phys., 23, 12907–12933, https://doi.org/10.5194/acp-23-12907-2023, https://doi.org/10.5194/acp-23-12907-2023, 2023
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The SO2 emissions of three power plants are estimated using aircraft observations and an ensemble of HYSPLIT dispersion simulations with different plume rise parameters. The emission estimates using the runs with the lowest root mean square errors (RMSEs) and the runs with the best correlation coefficients between the predicted and observed mixing ratios both agree well with the Continuous Emissions Monitoring Systems (CEMS) data. The RMSE-based plume rise appears to be more reasonable.
Jinghui Lian, Thomas Lauvaux, Hervé Utard, François-Marie Bréon, Grégoire Broquet, Michel Ramonet, Olivier Laurent, Ivonne Albarus, Mali Chariot, Simone Kotthaus, Martial Haeffelin, Olivier Sanchez, Olivier Perrussel, Hugo Anne Denier van der Gon, Stijn Nicolaas Camiel Dellaert, and Philippe Ciais
Atmos. Chem. Phys., 23, 8823–8835, https://doi.org/10.5194/acp-23-8823-2023, https://doi.org/10.5194/acp-23-8823-2023, 2023
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This study quantifies urban CO2 emissions via an atmospheric inversion for the Paris metropolitan area over a 6-year period from 2016 to 2021. Results show a long-term decreasing trend of about 2 % ± 0.6 % per year in the annual CO2 emissions over Paris. We conclude that our current capacity can deliver near-real-time CO2 emission estimates at the city scale in under a month, and the results agree within 10 % with independent estimates from multiple city-scale inventories.
Fu-Jie Zhu, Peng-Tuan Hu, and Wan-Li Ma
Atmos. Chem. Phys., 23, 8583–8590, https://doi.org/10.5194/acp-23-8583-2023, https://doi.org/10.5194/acp-23-8583-2023, 2023
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A new steady-state gas–particle partitioning model of polycyclic aromatic hydrocarbons was established based on the level-III multimedia fugacity model, which proved that the particulate proportion of PAHs in emissions was a crucial factor for G–P partitioning of PAHs. In addition, gaseous and particulate interference was also derived in the new steady-state model determined by the particulate proportion in emission that could derivate the G–P partitioning quotients from the equilibrium state.
Christian Hogrefe, Jesse O. Bash, Jonathan E. Pleim, Donna B. Schwede, Robert C. Gilliam, Kristen M. Foley, K. Wyat Appel, and Rohit Mathur
Atmos. Chem. Phys., 23, 8119–8147, https://doi.org/10.5194/acp-23-8119-2023, https://doi.org/10.5194/acp-23-8119-2023, 2023
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Under the umbrella of the fourth phase of the Air Quality Model Evaluation International Initiative (AQMEII4), this study applies AQMEII4 diagnostic tools to better characterize how dry deposition removes pollutants from the atmosphere in the widely used CMAQ model. The results illustrate how these tools can provide insights into similarities and differences between the two CMAQ dry deposition options that affect simulated pollutant budgets and ecosystem impacts from atmospheric pollution.
Kun Qu, Xuesong Wang, Xuhui Cai, Yu Yan, Xipeng Jin, Mihalis Vrekoussis, Maria Kanakidou, Guy P. Brasseur, Jin Shen, Teng Xiao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 7653–7671, https://doi.org/10.5194/acp-23-7653-2023, https://doi.org/10.5194/acp-23-7653-2023, 2023
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Basic understandings of ozone processes, especially transport and chemistry, are essential to support ozone pollution control, but studies often have different views on their relative importance. We developed a method to quantify their contributions in the ozone mass and concentration budgets based on the WRF-CMAQ model. Results in a polluted region highlight the differences between two budgets. For future studies, two budgets are both needed to fully understand the effects of ozone processes.
Emily Dowd, Chris Wilson, Martyn P. Chipperfield, Emanuel Gloor, Alistair Manning, and Ruth Doherty
Atmos. Chem. Phys., 23, 7363–7382, https://doi.org/10.5194/acp-23-7363-2023, https://doi.org/10.5194/acp-23-7363-2023, 2023
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Surface observations of methane show that the seasonal cycle amplitude (SCA) of methane is decreasing in the northern high latitudes (NHLs) but increased globally (1995–2020). The NHL decrease is counterintuitive, as we expect the SCA to increase with increasing concentrations. We use a chemical transport model to investigate changes in SCA in the NHLs. We find well-mixed methane and changes in emissions from Canada, the Middle East, and Europe are the largest contributors to the SCA in NHLs.
Danyang Ma, Tijian Wang, Hao Wu, Yawei Qu, Jian Liu, Jane Liu, Shu Li, Bingliang Zhuang, Mengmeng Li, and Min Xie
Atmos. Chem. Phys., 23, 6525–6544, https://doi.org/10.5194/acp-23-6525-2023, https://doi.org/10.5194/acp-23-6525-2023, 2023
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Increasing surface ozone (O3) concentrations have long been a significant environmental issue in China, despite the Clean Air Action Plan launched in 2013. Most previous research ignores the contributions of CO2 variations. Our study comprehensively analyzed O3 variation across China from various perspectives and highlighted the importance of considering CO2 variations when designing long-term O3 control policies, especially in high-vegetation-coverage areas.
Jackson Hian-Wui Chang, Stephen M. Griffith, Steven Soon-Kai Kong, Ming-Tung Chuang, and Neng-Huei Lin
Atmos. Chem. Phys., 23, 6357–6382, https://doi.org/10.5194/acp-23-6357-2023, https://doi.org/10.5194/acp-23-6357-2023, 2023
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A novel CMAQ–PMF-based composite index is developed to identify the key VOC source species for an effective ozone abatement strategy. The index provides information as to which VOC species are key to ozone formation and where to reduce sources of these VOC species. Using the composite index, we recommended the VOC control measures in southern Taiwan should prioritize solvent usage, vehicle emissions, and the petrochemical industry.
Lei Duan and Ken Caldeira
Atmos. Chem. Phys., 23, 6011–6020, https://doi.org/10.5194/acp-23-6011-2023, https://doi.org/10.5194/acp-23-6011-2023, 2023
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Ocko and Hamburg (2022) emphasize the short-term climate impact of hydrogen, and we present an analysis that places greater focus on long-term outcomes. We have derived equations that describe the time-evolving impact of hydrogen and show that higher methane leakage is primarily responsible for the warming potential of blue hydrogen, while hydrogen leakage plays a less critical role. Fossil fuels show more prominent longer-term climate impacts than clean hydrogen under all emission scenarios.
Lixu Jin, Wade Permar, Vanessa Selimovic, Damien Ketcherside, Robert J. Yokelson, Rebecca S. Hornbrook, Eric C. Apel, I-Ting Ku, Jeffrey L. Collett Jr., Amy P. Sullivan, Daniel A. Jaffe, Jeffrey R. Pierce, Alan Fried, Matthew M. Coggon, Georgios I. Gkatzelis, Carsten Warneke, Emily V. Fischer, and Lu Hu
Atmos. Chem. Phys., 23, 5969–5991, https://doi.org/10.5194/acp-23-5969-2023, https://doi.org/10.5194/acp-23-5969-2023, 2023
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Air quality in the USA has been improving since 1970 due to anthropogenic emission reduction. Those gains have been partly offset by increased wildfire pollution in the western USA in the past 20 years. Still, we do not understand wildfire emissions well due to limited measurements. Here, we used a global transport model to evaluate and constrain current knowledge of wildfire emissions with recent observational constraints, showing the underestimation of wildfire emissions in the western USA.
Zichong Chen, Daniel J. Jacob, Ritesh Gautam, Mark Omara, Robert N. Stavins, Robert C. Stowe, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Drew C. Pendergrass, and Sarah Hancock
Atmos. Chem. Phys., 23, 5945–5967, https://doi.org/10.5194/acp-23-5945-2023, https://doi.org/10.5194/acp-23-5945-2023, 2023
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We quantify methane emissions from individual countries in the Middle East and North Africa by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We show that the ability to simply relate oil/gas emissions to activity metrics is compromised by stochastic nature of local infrastructure and management practices. We find that the industry target for oil/gas methane intensity is achievable through associated gas capture, modern infrastructure, and centralized operations.
Yuting Wang, Yong-Feng Ma, Domingo Muñoz-Esparza, Jianing Dai, Cathy Wing Yi Li, Pablo Lichtig, Roy Chun-Wang Tsang, Chun-Ho Liu, Tao Wang, and Guy Pierre Brasseur
Atmos. Chem. Phys., 23, 5905–5927, https://doi.org/10.5194/acp-23-5905-2023, https://doi.org/10.5194/acp-23-5905-2023, 2023
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Air quality in urban areas is difficult to simulate in coarse-resolution models. This work exploits the WRF (Weather Research and Forecasting) model coupled with a large-eddy simulation (LES) component and online chemistry to perform high-resolution (33.3 m) simulations of air quality in a large city. The evaluation of the simulations with observations shows that increased model resolution improves the representation of the chemical species near the pollution sources.
Shuqi Yan, Bin Zhu, Shuangshuang Shi, Wen Lu, Jinhui Gao, Hanqing Kang, and Duanyang Liu
Atmos. Chem. Phys., 23, 5177–5190, https://doi.org/10.5194/acp-23-5177-2023, https://doi.org/10.5194/acp-23-5177-2023, 2023
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We analyze ozone response to aerosol mixing states in the vertical direction by WRF-Chem simulations. Aerosols generally lead to turbulent suppression, precursor accumulation, low-level photolysis reduction, and upper-level photolysis enhancement under different underlying surface and pollution conditions. Thus, ozone decreases within the entire boundary layer during the daytime, and the decrease is the least in aerosol external mixing states compared to internal and core shell mixing states.
Ida Storm, Ute Karstens, Claudio D'Onofrio, Alex Vermeulen, and Wouter Peters
Atmos. Chem. Phys., 23, 4993–5008, https://doi.org/10.5194/acp-23-4993-2023, https://doi.org/10.5194/acp-23-4993-2023, 2023
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In this study, we evaluate what is in the influence regions of the ICOS atmospheric measurement stations to gain insight into what land cover types and land-cover-associated fluxes the network represents. Subsequently, insights about strengths, weaknesses, and potential gaps can assist in future network expansion decisions. The network is concentrated in central Europe, which leads to a general overrepresentation of coniferous forest and cropland and underrepresentation of grass and shrubland.
Anna Agustí-Panareda, Jérôme Barré, Sébastien Massart, Antje Inness, Ilse Aben, Melanie Ades, Bianca C. Baier, Gianpaolo Balsamo, Tobias Borsdorff, Nicolas Bousserez, Souhail Boussetta, Michael Buchwitz, Luca Cantarello, Cyril Crevoisier, Richard Engelen, Henk Eskes, Johannes Flemming, Sébastien Garrigues, Otto Hasekamp, Vincent Huijnen, Luke Jones, Zak Kipling, Bavo Langerock, Joe McNorton, Nicolas Meilhac, Stefan Noël, Mark Parrington, Vincent-Henri Peuch, Michel Ramonet, Miha Razinger, Maximilian Reuter, Roberto Ribas, Martin Suttie, Colm Sweeney, Jérôme Tarniewicz, and Lianghai Wu
Atmos. Chem. Phys., 23, 3829–3859, https://doi.org/10.5194/acp-23-3829-2023, https://doi.org/10.5194/acp-23-3829-2023, 2023
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We present a global dataset of atmospheric CO2 and CH4, the two most important human-made greenhouse gases, which covers almost 2 decades (2003–2020). It is produced by combining satellite data of CO2 and CH4 with a weather and air composition prediction model, and it has been carefully evaluated against independent observations to ensure validity and point out deficiencies to the user. This dataset can be used for scientific studies in the field of climate change and the global carbon cycle.
Dominik Brunner, Gerrit Kuhlmann, Stephan Henne, Erik Koene, Bastian Kern, Sebastian Wolff, Christiane Voigt, Patrick Jöckel, Christoph Kiemle, Anke Roiger, Alina Fiehn, Sven Krautwurst, Konstantin Gerilowski, Heinrich Bovensmann, Jakob Borchardt, Michal Galkowski, Christoph Gerbig, Julia Marshall, Andrzej Klonecki, Pascal Prunet, Robert Hanfland, Margit Pattantyús-Ábrahám, Andrzej Wyszogrodzki, and Andreas Fix
Atmos. Chem. Phys., 23, 2699–2728, https://doi.org/10.5194/acp-23-2699-2023, https://doi.org/10.5194/acp-23-2699-2023, 2023
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We evaluated six atmospheric transport models for their capability to simulate the CO2 plumes from two of the largest power plants in Europe by comparing the models against aircraft observations collected during the CoMet (Carbon Dioxide and Methane Mission) campaign in 2018. The study analyzed how realistically such plumes can be simulated at different model resolutions and how well the planned European satellite mission CO2M will be able to quantify emissions from power plants.
Chenchao Zhan, Min Xie, Hua Lu, Bojun Liu, Zheng Wu, Tijian Wang, Bingliang Zhuang, Mengmeng Li, and Shu Li
Atmos. Chem. Phys., 23, 771–788, https://doi.org/10.5194/acp-23-771-2023, https://doi.org/10.5194/acp-23-771-2023, 2023
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With the development of urbanization, urban land use and anthropogenic
emissions increase, affecting urban air quality and, in turn, the health risks associated with air pollutants. In this study, we systematically evaluate the impacts of urbanization on air quality and the corresponding health risks in a highly urbanized city with severe air pollution and complex terrain. This work focuses on the health risks caused by urbanization and can provide valuable insight for air pollution strategies.
Hélène Peiro, Sean Crowell, and Berrien Moore III
Atmos. Chem. Phys., 22, 15817–15849, https://doi.org/10.5194/acp-22-15817-2022, https://doi.org/10.5194/acp-22-15817-2022, 2022
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CO data can provide a powerful constraint on fire fluxes, supporting more accurate estimation of biospheric CO2 fluxes. We converted CO fire flux into CO2 fire prior, which is then used to adjust CO2 respiration. We applied this to two other fire flux products. CO2 inversions constrained by satellites or in situ data are then performed. Results show larger variations among the data assimilated than across the priors, but tropical flux from in situ inversions is sensitive to priors.
Zhaofeng Lv, Zhenyu Luo, Fanyuan Deng, Xiaotong Wang, Junchao Zhao, Lucheng Xu, Tingkun He, Yingzhi Zhang, Huan Liu, and Kebin He
Atmos. Chem. Phys., 22, 15685–15702, https://doi.org/10.5194/acp-22-15685-2022, https://doi.org/10.5194/acp-22-15685-2022, 2022
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This study developed a hybrid model, CMAQ-RLINE_URBAN, to predict the urban NO2 concentrations at a high spatial resolution. To estimate the influence of various street canyons on the dispersion of air pollutants, a new parameterization scheme was established based on computational fluid dynamics and machine learning methods. This work created a new method to identify the characteristics of vehicle-related air pollution at both city and street scales simultaneously and accurately.
Vishnu Thilakan, Dhanyalekshmi Pillai, Christoph Gerbig, Michal Galkowski, Aparnna Ravi, and Thara Anna Mathew
Atmos. Chem. Phys., 22, 15287–15312, https://doi.org/10.5194/acp-22-15287-2022, https://doi.org/10.5194/acp-22-15287-2022, 2022
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This paper demonstrates how we can use atmospheric observations to improve the CO2 flux estimates in India. This is achieved by improving the representation of terrain, mesoscale transport, and flux variations. We quantify the impact of the unresolved variations in the current models on optimally estimated fluxes via inverse modelling and quantify the associated flux uncertainty. We illustrate how a parameterization scheme captures this variability in the coarse models.
Zichong Chen, Daniel J. Jacob, Hannah Nesser, Melissa P. Sulprizio, Alba Lorente, Daniel J. Varon, Xiao Lu, Lu Shen, Zhen Qu, Elise Penn, and Xueying Yu
Atmos. Chem. Phys., 22, 10809–10826, https://doi.org/10.5194/acp-22-10809-2022, https://doi.org/10.5194/acp-22-10809-2022, 2022
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We quantify methane emissions in China and contributions from different sectors by inverse analysis of 2019 TROPOMI satellite observations of atmospheric methane. We find that anthropogenic methane emissions for China are underestimated in the national inventory. Our estimate of emissions indicates a small life-cycle loss rate, implying net climate benefits from the current
coal-to-gasenergy transition in China. However, this small loss rate can be misleading given China's high gas imports.
Naveen Chandra, Prabir K. Patra, Yousuke Niwa, Akihiko Ito, Yosuke Iida, Daisuke Goto, Shinji Morimoto, Masayuki Kondo, Masayuki Takigawa, Tomohiro Hajima, and Michio Watanabe
Atmos. Chem. Phys., 22, 9215–9243, https://doi.org/10.5194/acp-22-9215-2022, https://doi.org/10.5194/acp-22-9215-2022, 2022
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This paper is intended to accomplish two goals: (1) quantify mean and uncertainty in non-fossil-fuel CO2 fluxes estimated by inverse modeling and (2) provide in-depth analyses of regional CO2 fluxes in support of emission mitigation policymaking. CO2 flux variability and trends are discussed concerning natural climate variability and human disturbances using multiple lines of evidence.
Ruben B. Schulte, Margreet C. van Zanten, Bart J. H. van Stratum, and Jordi Vilà-Guerau de Arellano
Atmos. Chem. Phys., 22, 8241–8257, https://doi.org/10.5194/acp-22-8241-2022, https://doi.org/10.5194/acp-22-8241-2022, 2022
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We present a fine-scale simulation framework, utilizing large-eddy simulations, to assess NH3 measurements influenced by boundary-layer dynamics and turbulent dispersion of a nearby emission source. The minimum required distance from an emission source differs for concentration and flux measurements, from 0.5–3.0 km and 0.75–4.5 km, respectively. The simulation framework presented here proves to be a powerful and versatile tool for future NH3 research at high spatio-temporal resolutions.
Sieglinde Callewaert, Jérôme Brioude, Bavo Langerock, Valentin Duflot, Dominique Fonteyn, Jean-François Müller, Jean-Marc Metzger, Christian Hermans, Nicolas Kumps, Michel Ramonet, Morgan Lopez, Emmanuel Mahieu, and Martine De Mazière
Atmos. Chem. Phys., 22, 7763–7792, https://doi.org/10.5194/acp-22-7763-2022, https://doi.org/10.5194/acp-22-7763-2022, 2022
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A regional atmospheric transport model is used to analyze the factors contributing to CO2, CH4, and CO observations at Réunion Island. We show that the surface observations are dominated by local fluxes and dynamical processes, while the column data are influenced by larger-scale mechanisms such as biomass burning plumes. The model is able to capture the measured time series well; however, the results are highly dependent on accurate boundary conditions and high-resolution emission inventories.
Anja Ražnjević, Chiel van Heerwaarden, Bart van Stratum, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, and Maarten Krol
Atmos. Chem. Phys., 22, 6489–6505, https://doi.org/10.5194/acp-22-6489-2022, https://doi.org/10.5194/acp-22-6489-2022, 2022
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Mobile measurement techniques (e.g., instruments placed in cars) are often employed to identify and quantify individual sources of greenhouse gases. Due to road restrictions, those observations are often sparse (temporally and spatially). We performed high-resolution simulations of plume dispersion, with realistic weather conditions encountered in the field, to reproduce the measurement process of a methane plume emitted from an oil well and provide additional information about the plume.
Alice E. Ramsden, Anita L. Ganesan, Luke M. Western, Matthew Rigby, Alistair J. Manning, Amy Foulds, James L. France, Patrick Barker, Peter Levy, Daniel Say, Adam Wisher, Tim Arnold, Chris Rennick, Kieran M. Stanley, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 22, 3911–3929, https://doi.org/10.5194/acp-22-3911-2022, https://doi.org/10.5194/acp-22-3911-2022, 2022
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Quantifying methane emissions from different sources is a key focus of current research. We present a method for estimating sectoral methane emissions that uses ethane as a tracer for fossil fuel methane. By incorporating variable ethane : methane emission ratios into this model, we produce emissions estimates with improved uncertainty characterisation. This method will be particularly useful for studying methane emissions in areas with complex distributions of sources.
Ying Li, Xiangjun Zhao, Xuejiao Deng, and Jinhui Gao
Atmos. Chem. Phys., 22, 3861–3873, https://doi.org/10.5194/acp-22-3861-2022, https://doi.org/10.5194/acp-22-3861-2022, 2022
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This study finds a new phenomenon of weak wind deepening (WWD) associated with the peripheral circulation of typhoon and gives the influence mechanism of WWD on its contribution to daily variation during sustained ozone episodes. The WWD provides the premise for pollution accumulation in the whole PBL and continued enhancement of ground-level ozone via vertical mixing processes. These findings could benefit the daily daytime ozone forecast in the PRD region and other areas.
Tia R. Scarpelli, Daniel J. Jacob, Shayna Grossman, Xiao Lu, Zhen Qu, Melissa P. Sulprizio, Yuzhong Zhang, Frances Reuland, Deborah Gordon, and John R. Worden
Atmos. Chem. Phys., 22, 3235–3249, https://doi.org/10.5194/acp-22-3235-2022, https://doi.org/10.5194/acp-22-3235-2022, 2022
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We present a spatially explicit version of the national inventories of oil, gas, and coal methane emissions as submitted by individual countries to the United Nations Framework Convention on Climate Change (UNFCCC) in 2021. We then use atmospheric modeling to compare our inventory emissions to atmospheric methane observations with the goal of identifying potential under- and overestimates of oil–gas methane emissions in the national inventories.
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Short summary
In boreal forest, there is a large number of gaseous organic compounds called biogenic volatile organic compounds (BVOCs). Within the canopy, they can be emitted from vegetation and soil, react with each other and other gases, be transported in the air, and be removed from vegetation and soil surfaces. We applied a numerical model to simulate these processes and found that these BVOCs can be divided into five categories according to the significance of their sources and sinks.
In boreal forest, there is a large number of gaseous organic compounds called biogenic volatile...
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