4.2 Article

Atmospheric gas-to-particle conversion: why NPF events are observed in megacities?

Journal

FARADAY DISCUSSIONS
Volume 200, Issue -, Pages 271-288

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/c6fd00257a

Keywords

-

Funding

  1. Academy of Finland via the Center of Excellence in Atmospheric Sciences and Academy Professor Project
  2. European Commission within ACTRIS2
  3. Royal Society-Newton Advanced Fellowship [NA140106]

Ask authors/readers for more resources

In terms of the global aerosol particle number load, atmospheric new particle formation (NPF) dominates over primary emissions. The key for quantifying the importance of atmospheric NPF is to understand how gas-to-particle conversion (GTP) takes place at sizes below a few nanometers in particle diameter in different environments, and how this nano-GTP affects the survival of small clusters into larger sizes. The survival probability of growing clusters is tied closely to the competition between their growth and scavenging by pre-existing aerosol particles, and the key parameter in this respect is the ratio between the condensation sink (CS) and the cluster growth rate (GR). Here we define their ratio as a dimensionless survival parameter, P, as P = (CS/10(-4) s(-1))/(GR/nm h(-1)). Theoretical arguments and observations in clean and moderately-polluted conditions indicate that P needs to be smaller than about 50 for a notable NPF to take place. However, the existing literature shows that in China, NPF occurs frequently in megacities such as in Beijing, Nanjing and Shanghai, and our analysis shows that the calculated values of P are even larger than 200 in these cases. By combining direct observations and conceptual modelling, we explore the variability of the survival parameter P in different environments and probe the reasons for NPF occurrence under highly-polluted conditions.

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.2
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

Article Environmental Sciences

Measurement of atmospheric nanoparticles: Bridging the gap between gas-phase molecules and larger particles

Chao Peng, Chenjuan Deng, Ting Lei, Jun Zheng, Jun Zhao, Dongbin Wang, Zhijun Wu, Lin Wang, Yan Chen, Mingyuan Liu, Jingkun Jiang, Anpei Ye, Maofa Ge, Weigang Wang

Summary: Atmospheric nanoparticles play a crucial role in fine particulate matter (PM2.5) and have significant impacts on visibility, climate, and human health. Advanced experimental techniques have been developed to monitor and characterize the physical and chemical properties of atmospheric nanoparticles, providing insights into their formation and growth processes.

JOURNAL OF ENVIRONMENTAL SCIENCES (2023)

Article Meteorology & Atmospheric Sciences

Aerosols, Clusters, Greenhouse Gases, Trace Gases and Boundary-Layer Dynamics: on Feedbacks and Interactions

Markku Kulmala, Tom Kokkonen, Ekaterina Ezhova, Alexander Baklanov, Alexander Mahura, Ivan Mammarella, Jaana Back, Hanna K. Lappalainen, Svyatoslav Tyuryakov, Veli-Matti Kerminen, Sergej Zilitinkevich, Tuukka Petaja

Summary: Turbulence is a key process in the atmosphere that transports material and energy, and causes concentration fluctuations. It influences various atmospheric processes and has implications for air pollution and climate change. Understanding the mechanisms of atmospheric turbulence, chemistry, and aerosol dynamics is crucial for analyzing the connections and feedbacks among these processes.

BOUNDARY-LAYER METEOROLOGY (2023)

Article Environmental Sciences

Phenomenology of ultrafine particle concentrations and size distribution across urban Europe

Pedro Trechera, Meritxell Garcia-Marles, Xiansheng Liu, Cristina Reche, Noemi Perez, Marjan Savadkoohi, David Beddows, Imre Salma, Mate Vorosmarty, Andrea Casans, Juan Andres Casquero-Vera, Christoph Hueglin, Nicolas Marchand, Benjamin Chazeau, Gregory Gille, Panayiotis Kalkavouras, Nikos Mihalopoulos, Jakub Ondracek, Nadia Zikova, Jarkko V. Niemi, Hanna E. Manninen, David C. Green, Anja H. Tremper, Michael Norman, Stergios Vratolis, Konstantinos Eleftheriadis, Francisco J. Gomez-Moreno, Elisabeth Alonso-Blanco, Holger Gerwig, Alfred Wiedensohler, Kay Weinhold, Maik Merkel, Susanne Bastian, Jean-Eudes Petit, Olivier Favez, Suzanne Crumeyrolle, Nicolas Ferlay, Sebastiao Martins Dos Santos, Jean-Philippe Putaud, Hilkka Timonen, Janne Lampilahti, Christof Asbach, Carmen Wolf, Heinz Kaminski, Hicran Altug, Barbara Hoffmann, David Q. Rich, Marco Pandolfi, Roy M. Harrison, Philip K. Hopke, Tuukka Petaja, Andres Alastuey, Xavier Querol

Summary: This study evaluated the hourly particle number size distributions (PNSD) from 26 sites in Europe and 1 in the US, focusing on urban background (UB) and traffic (TR) sites. The objective was to describe the characteristics of urban ultrafine particles (UFP) in Europe. The results showed variations in PNC and BC across different regions and site types, with traffic emissions being a major contributor. The study emphasized the need for specific monitoring of PNSD and measurements of <10 nm PNC for assessing the health effects of nanoparticles.

ENVIRONMENT INTERNATIONAL (2023)

Article Multidisciplinary Sciences

Smoke-weather interaction affects extreme wildfires in diverse coastal regions

Xin Huang, Ke Ding, Jingyi Liu, Zilin Wang, Rong Tang, Lian Xue, Haikun Wang, Qiang Zhang, Zhe-Min Tan, Congbin Fu, Steven J. Davis, Meinrat O. Andreae, Aijun Ding

Summary: Extreme wildfires pose threats to human lives, air quality, and ecosystems. The impact of meteorology on wildfire behaviors and the correlation between wildfires and climate are well-studied. However, the influence of fire-weather feedback on short-term wildfire variability remains unclear, hindering fire disaster mitigation. In this study, we demonstrate the dominant role of synoptic-scale feedback in driving extreme fires in Mediterranean and monsoon climate regions. We observed that the radiative effects of smoke aerosols can modify near-surface wind, air dryness, and rainfall, thereby exacerbating air pollution by enhancing fire emissions and weakening dispersion. The complex interactions among wildfires, smoke, and weather create a positive feedback loop that significantly increases air pollution exposure.

SCIENCE (2023)

Article Environmental Sciences

Shift in Peaks of PAH-Associated Health Risks From East Asia to South Asia and Africa in the Future

Sijia Lou, Manish Shrivastava, Aijun Ding, Richard C. Easter, Jerome D. Fast, Philip J. Rasch, Huizhong Shen, Staci Massey L. Simonich, Steven J. Smith, Shu Tao, Alla Zelenyuk

Summary: The lung cancer risk from exposure to ambient polycyclic aromatic hydrocarbons (PAHs) is expected to change significantly by 2050 compared to 2008 due to changes in climate and emissions. Residential biofuel use in East Asia and South Asia contributes to the higher BaP concentrations, exceeding WHO-recommended limits. However, stringent air quality policies in developed countries have led to a substantial decrease in PAH lung cancer risk. Future policies should focus on reducing air pollutant emissions and promoting efficient combustion technologies.

EARTHS FUTURE (2023)

Article Environmental Sciences

Size-dependent chemical composition of atmospheric nanoparticles in urban Beijing during springtime

Yan Chen, Chenjuan Deng, Ting Lei, Junling Li, Chaofan Lian, Yiran Li, Jun Zheng, Jun Zhao, Dongbin Wang, Zhijun Wu, Lin Wang, Lei Li, Hong Li, Jian Gao, Jingkun Jiang, Maofa Ge, Weigang Wang

Summary: By using a custom-made Nanoparticle Chemical Ionization Mass Spectrometer (NPCIMS), we conducted comprehensive field measurements of the size-resolved chemical composition of atmospheric nanoparticles in the size range from 10 to 100 nm. The quantification results showed that CHO organics accounted for around 80% of the newly formed particles in the growth process with diameters from 10 to 25 nm. In contrast to previous observations in urban Mexico, the growth of newly formed particles in urban Beijing was dominated by ammonium, sulfate, and organic components in the size-resolved modes (10-25 nm) during springtime.

ATMOSPHERIC ENVIRONMENT (2023)

Article Meteorology & Atmospheric Sciences

Development and characterization of the Portable Ice Nucleation Chamber 2 (PINCii)

Dimitri Castarede, Zoe Brasseur, Yusheng Wu, Zamin A. Kanji, Markus Hartmann, Lauri Ahonen, Merete Bilde, Markku Kulmala, Tuukka Petaja, Jan B. C. Pettersson, Berko Sierau, Olaf Stetzer, Frank Stratmann, Birgitta Svenningsson, Erik Swietlicki, Quynh Thu Nguyen, Jonathan Duplissy, Erik S. Thomson

Summary: The Portable Ice Nucleation Chamber 2 (PINCii) is a new continuous flow diffusion chamber (CFDC) that can measure ice nucleating particles (INPs). PINCii has been engineered to improve upon the limitations of previous CFDCs and offers several possibilities for improved INP measurements. It features low background particle counts, high-spatial-resolution wall-temperature mapping, and a new method for analyzing CFDC data. Additionally, it can be used to study droplet activation processes and extend ice crystal growth. The instrument's capabilities have been demonstrated through a series of experiments. The sources of uncertainty in CFDCs, including particle background, particle loss, and variations in aerosol lamina temperature and relative humidity, have also been quantified and discussed for PINCii. Overall, the importance of this work in developing a more advanced instrument for measuring INPs is rated 9 out of 10.

ATMOSPHERIC MEASUREMENT TECHNIQUES (2023)

Article Environmental Sciences

A dynamic parameterization of sulfuric acid-dimethylamine nucleation and its application in three-dimensional modeling

Yuyang Li, Jiewen Shen, Bin Zhao, Runlong Cai, Shuxiao Wang, Yang Gao, Manish Shrivastava, Da Gao, Jun Zheng, Markku Kulmala, Jingkun Jiang

Summary: Sulfuric acid (SA) is a major precursor for atmospheric new particle formation (NPF), and the formation of SA-dimethylamine (DMA) clusters initiates intense NPF events in polluted urban atmospheres. We developed a parameterization of SA-DMA nucleation based on cluster dynamic simulations and quantum chemistry calculations, which successfully reproduced the dependence of particle formation rates on temperature and condensation sinks (CSs). The parameterization was incorporated into a 3-D chemical transport model and showed good agreement with observations in wintertime Beijing, contributing significantly to nucleation rates and aerosol population during the simulations.

ATMOSPHERIC CHEMISTRY AND PHYSICS (2023)

Article Meteorology & Atmospheric Sciences

SMEARcore - modular data infrastructure for atmospheric measurement stations

Anton Rusanen, Kristo Horrak, Lauri R. Ahonen, Tuomo Nieminen, Pasi P. Aalto, Pasi Kolari, Markku Kulmala, Tuukka Petaja, Heikki Junninen

Summary: We introduce SMEARcore, a framework for real-time data analysis and management intended for measurement stations. It allows integration of new SMEAR stations with existing ones and facilitates easier problem diagnosis through robust data pipelines. Unlike previous similar concepts, SMEARcore keeps processing under data owners' control, provides tools for general data interoperability, and is extensible to new instruments. It is meant to supplement existing infrastructures and promote structured data curation in more measurement stations.

ATMOSPHERIC MEASUREMENT TECHNIQUES (2023)

Article Environmental Sciences

Dynamics of aerosol, humidity, and clouds in air masses travelling over Fennoscandian boreal forests

Meri Raty, Larisa Sogacheva, Helmi-Marja Keskinen, Veli-Matti Kerminen, Tuomo Nieminen, Tuukka Petaja, Ekaterina Ezhova, Markku Kulmala

Summary: Boreal forests in the Northern Hemisphere have a complex interaction with the atmosphere, including a feedback process that may produce a cooling effect through increased cloud reflectance due to aerosol-cloud interactions. This study investigates the impact of the boreal forest environment on cloud-related properties during the growing season. Results show that air masses with longer exposure to the forest have different properties compared to those with shorter land transport times. The study also reveals changes in cloud condensation nuclei concentrations, specific humidity, and precipitation frequency after a certain threshold of land transport time.

ATMOSPHERIC CHEMISTRY AND PHYSICS (2023)

Article Meteorology & Atmospheric Sciences

Characterization of offline analysis of particulate matter with FIGAERO-CIMS

Jing Cai, Kaspar R. Daellenbach, Cheng Wu, Yan Zheng, Feixue Zheng, Wei Du, Sophie L. Haslett, Qi Chen, Markku Kulmala, Claudia Mohr

Summary: The offline application of FIGAERO-CIMS provides a cost-efficient method to analyze the molecular composition of organic aerosols. This study demonstrates the feasibility of using Teflon and quartz fiber filter samples collected in urban Beijing, with high signal-to-noise ratios, repeatability, and linear signal response. It expands the molecular characterization of organic aerosols by FIGAERO-CIMS to situations where the instrument itself cannot be deployed.

ATMOSPHERIC MEASUREMENT TECHNIQUES (2023)

Article Ecology

Spatiotemporal lagging of predictors improves machine learningestimates of atmosphere-forest CO2 exchange

Matti Kamarainen, Juha-Pekka Tuovinen, Markku Kulmala, Ivan Mammarella, Juha Aalto, Henriikka Vekuri, Annalea Lohila, Anna Lintunen

Summary: In this study, machine learning methods (RF and GB) were used to predict the net ecosystem CO2 exchange (NEE) in a pine-dominated boreal forest in southern Finland over 1996-2018. The results showed that both RF and GB were able to explain the temporal variability of NEE using meteorological predictors, but GB was more accurate.

BIOGEOSCIENCES (2023)

Article Environmental Sciences

High emission rates and strong temperature response make boreal wetlands a large source of isoprene and terpenes

Lejish Vettikkat, Pasi Miettinen, Angela Buchholz, Pekka Rantala, Hao Yu, Simon Schallhart, Tuukka Petaja, Roger Seco, Elisa Mannisto, Markku Kulmala, Eeva-Stiina Tuittila, Alex B. Guenther, Siegfried Schobesberger

Summary: Wetlands cover a small portion of the land surface but boreal wetlands are experiencing significant warming and emit climate-relevant volatile organic compounds. This study presents the first-ever measurements of terpene emissions from a boreal fen wetland and found that isoprene was the dominant compound emitted. The emissions showed a strong exponential dependence on temperature and were significantly higher than previous estimates.

ATMOSPHERIC CHEMISTRY AND PHYSICS (2023)

Article Environmental Sciences

Measurement report: Production and loss of atmospheric formaldehyde at a suburban site of Shanghai in summertime

Yizhen Wu, Juntao Huo, Gan Yang, Yuwei Wang, Lihong Wang, Shijian Wu, Lei Yao, Qingyan Fu, Lin Wang

Summary: During a 2021 summer campaign in a suburban area of Shanghai, China, the atmospheric formaldehyde (HCHO) concentration and production were measured. It was found that secondary production accounted for a significant portion of HCHO, with alkenes being key precursors. The study highlighted the importance of secondary pollution in the suburban areas of Shanghai.

ATMOSPHERIC CHEMISTRY AND PHYSICS (2023)

Article Environmental Sciences

A full year of aerosol size distribution data from the central Arctic under an extreme positive Arctic Oscillation: insights from the Multidisciplinarydrifting Observatory for the Study of Arctic Climate (MOSAiC) expedition

Matthew Boyer, Diego Aliaga, Jakob Boyd Pernov, Helene Angot, Lauriane L. J. Quelever, Lubna Dada, Benjamin Heutte, Manuel Dall'Osto, David C. S. Beddows, Zoe Brasseur, Ivo Beck, Silvia Bucci, Marina Duetsch, Andreas Stohl, Tiia Laurila, Eija Asmi, Andreas Massling, Daniel Charles Thomas, Jakob Kleno Nojgaard, Tak Chan, Sangeeta Sharma, Peter Tunved, Radovan Krejci, Hans Christen Hansson, Federico Bianchi, Katrianne Lehtipalo, Alfred Wiedensohler, Kay Weinhold, Markku Kulmala, Tuukka Petaja, Mikko Sipila, Julia Schmale, Tuija Jokinen

Summary: The Arctic environment is undergoing rapid changes due to accelerated warming. This study investigates the annual cycle of aerosol characteristics in the central Arctic Ocean and compares them to land-based sites across the Arctic. The analysis provides important insights into aerosol processes in the changing Arctic environment and their impact on climate change.

ATMOSPHERIC CHEMISTRY AND PHYSICS (2023)

No Data Available