Anthropogenic pollution elevates the peak height of new particle formation from planetary boundary layer to lower free troposphere
Abstract
New particle formation (NPF) and subsequent growth are primary sources of atmospheric aerosol particles and cloud condensation nuclei. Previous studies have been conducted in relatively clean environments; investigation of NPF events over highly polluted megacities is still lacking. Here in this paper we show, based on a recent yearlong aircraft campaign conducted over Beijing, China, from April 2011 to June 2012, that NPF occurrence peaks in the lower free troposphere (LT), instead of planetary boundary layer (PBL), as most previous studies have found and that the distance of NPF peak to PBL top increases with increasing aerosol loading. Further analysis reveals that increased aerosols suppress NPF in PBL, but enhance NPF in LT due to a complex chain of aerosol-radiation-photochemistry interactions that affect both NPF sources and sinks. These findings shed new light on our understanding of NPF occurrence, NPF vertical distribution, and thus their effects on atmospheric photochemistry, clouds, and climate.
- Authors:
-
- Chinese Meteorological Administration, Beijing (China). Inst. of Urban Meteorology; Beijing Key Lab. of Cloud, Precipitation, and Atmospheric Water Resources, Beijing (China); Brookhaven National Lab. (BNL), Upton, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Chinese Meteorological Administration, Beijing (China). Inst. of Urban Meteorology; Beijing Key Lab. of Cloud, Precipitation, and Atmospheric Water Resources, Beijing (China)
- Beijing Key Lab. of Cloud, Precipitation, and Atmospheric Water Resources, Beijing (China)
- Chinese Academy of Sciences (CAS), Beijing (China). Inst. of Atmospheric Physics
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1376169
- Report Number(s):
- BNL-114144-2017-JA
Journal ID: ISSN 0094-8276; R&D Project: 2016-BNL-EE630EECA-Budg; KP1701000
- Grant/Contract Number:
- SC0012704; 2017YFC0209604; 2016YFA0602001; 2014BAC06B03
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Geophysical Research Letters
- Additional Journal Information:
- Journal Volume: 44; Journal Issue: 14; Journal ID: ISSN 0094-8276
- Publisher:
- American Geophysical Union
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; new particle formation; pollution; troposphere; planetary boundary layer; China
Citation Formats
Quan, Jiannong, Liu, Yangang, Liu, Quan, Jia, Xingcan, Li, Xia, Gao, Yang, Ding, Deping, Li, Jie, and Wang, Zifa. Anthropogenic pollution elevates the peak height of new particle formation from planetary boundary layer to lower free troposphere. United States: N. p., 2017.
Web. doi:10.1002/2017GL074553.
Quan, Jiannong, Liu, Yangang, Liu, Quan, Jia, Xingcan, Li, Xia, Gao, Yang, Ding, Deping, Li, Jie, & Wang, Zifa. Anthropogenic pollution elevates the peak height of new particle formation from planetary boundary layer to lower free troposphere. United States. https://doi.org/10.1002/2017GL074553
Quan, Jiannong, Liu, Yangang, Liu, Quan, Jia, Xingcan, Li, Xia, Gao, Yang, Ding, Deping, Li, Jie, and Wang, Zifa. Fri .
"Anthropogenic pollution elevates the peak height of new particle formation from planetary boundary layer to lower free troposphere". United States. https://doi.org/10.1002/2017GL074553. https://www.osti.gov/servlets/purl/1376169.
@article{osti_1376169,
title = {Anthropogenic pollution elevates the peak height of new particle formation from planetary boundary layer to lower free troposphere},
author = {Quan, Jiannong and Liu, Yangang and Liu, Quan and Jia, Xingcan and Li, Xia and Gao, Yang and Ding, Deping and Li, Jie and Wang, Zifa},
abstractNote = {New particle formation (NPF) and subsequent growth are primary sources of atmospheric aerosol particles and cloud condensation nuclei. Previous studies have been conducted in relatively clean environments; investigation of NPF events over highly polluted megacities is still lacking. Here in this paper we show, based on a recent yearlong aircraft campaign conducted over Beijing, China, from April 2011 to June 2012, that NPF occurrence peaks in the lower free troposphere (LT), instead of planetary boundary layer (PBL), as most previous studies have found and that the distance of NPF peak to PBL top increases with increasing aerosol loading. Further analysis reveals that increased aerosols suppress NPF in PBL, but enhance NPF in LT due to a complex chain of aerosol-radiation-photochemistry interactions that affect both NPF sources and sinks. These findings shed new light on our understanding of NPF occurrence, NPF vertical distribution, and thus their effects on atmospheric photochemistry, clouds, and climate.},
doi = {10.1002/2017GL074553},
journal = {Geophysical Research Letters},
number = 14,
volume = 44,
place = {United States},
year = {Fri Jul 21 00:00:00 EDT 2017},
month = {Fri Jul 21 00:00:00 EDT 2017}
}
Web of Science
Works referenced in this record:
Free troposphere as a major source of CCN for the equatorial pacific boundary layer: long-range transport and teleconnections
journal, January 2013
- Clarke, A. D.; Freitag, S.; Simpson, R. M. C.
- Atmospheric Chemistry and Physics, Vol. 13, Issue 15
New particle formation events measured on board the ATR-42 aircraft during the EUCAARI campaign
journal, January 2010
- Crumeyrolle, S.; Manninen, H. E.; Sellegri, K.
- Atmospheric Chemistry and Physics, Vol. 10, Issue 14
An improved criterion for new particle formation in diverse atmospheric environments
journal, January 2010
- Kuang, C.; Riipinen, I.; Sihto, S. -L.
- Atmospheric Chemistry and Physics, Vol. 10, Issue 17
Nucleation and Growth of Nanoparticles in the Atmosphere
journal, November 2011
- Zhang, Renyi; Khalizov, Alexei; Wang, Lin
- Chemical Reviews, Vol. 112, Issue 3
Global atmospheric particle formation from CERN CLOUD measurements
journal, October 2016
- Dunne, E. M.; Gordon, H.; Kurten, A.
- Science, Vol. 354, Issue 6316
Spatial Mapping of Ozone and SO2 Trends in Europe
journal, September 2010
- Denby, Bruce; Sundvor, Ingrid; Cassiani, Massimo
- Science of The Total Environment, Vol. 408, Issue 20
Sulfuric acid and OH concentrations in a boreal forest site
journal, January 2009
- Petäjä, T.; Mauldin, III, R. L.; Kosciuch, E.
- Atmospheric Chemistry and Physics, Vol. 9, Issue 19
Impact of nucleation on global CCN
journal, January 2009
- Merikanto, J.; Spracklen, D. V.; Mann, G. W.
- Atmospheric Chemistry and Physics, Vol. 9, Issue 21
Assessment of the global impact of aerosols on tropospheric oxidants
journal, January 2005
- Tie, Xuexi
- Journal of Geophysical Research, Vol. 110, Issue D3
In situ observations of new particle formation in the tropical upper troposphere: the role of clouds and the nucleation mechanism
journal, January 2011
- Weigel, R.; Borrmann, S.; Kazil, J.
- Atmospheric Chemistry and Physics, Vol. 11, Issue 18
Stable sulphate clusters as a source of new atmospheric particles
journal, March 2000
- Kulmala, Markku; Pirjola, Liisa; Mäkelä, Jyrki M.
- Nature, Vol. 404, Issue 6773
Simulation of particle size distribution with a global aerosol model: contribution of nucleation to aerosol and CCN number concentrations
journal, January 2009
- Yu, F.; Luo, G.
- Atmospheric Chemistry and Physics, Vol. 9, Issue 20
New-particle formation events in a continental boundary layer: first results from the SATURN experiment
journal, January 2003
- Stratmann, F.; Siebert, H.; Spindler, G.
- Atmospheric Chemistry and Physics, Vol. 3, Issue 5
High frequency new particle formation in the Himalayas
journal, October 2008
- Venzac, H.; Sellegri, K.; Laj, P.
- Proceedings of the National Academy of Sciences, Vol. 105, Issue 41
Airborne measurements of nucleation mode particles II: boreal forest nucleation events
journal, January 2009
- O'Dowd, C. D.; Yoon, Y. J.; Junkermann, W.
- Atmospheric Chemistry and Physics, Vol. 9, Issue 3
Characteristics of heavy aerosol pollution during the 2012–2013 winter in Beijing, China
journal, May 2014
- Quan, Jiannong; Tie, Xuexi; Zhang, Qiang
- Atmospheric Environment, Vol. 88
ISORROPIA: A New Thermodynamic Equilibrium Model for Multiphase Multicomponent Inorganic Aerosols
journal, March 1998
- Nenes, Athanasios; Pandis, Spyros N.; Pilinis, Christodoulos
- Aquatic Geochemistry, Vol. 4, Issue 1, p. 123-152
Rapid changes in biomass burning aerosols by atmospheric oxidation: RAPID CHANGES IN BIOMASS BURNING PLUMES
journal, April 2014
- Vakkari, Ville; Kerminen, Veli-Matti; Beukes, Johan Paul
- Geophysical Research Letters, Vol. 41, Issue 7
Influence of clouds on aerosol particle number concentrations in the upper troposphere: INFLUENCE OF CLOUDS ON AEROSOL IN THE UT
journal, January 2009
- Weigelt, A.; Hermann, M.; van Velthoven, P. F. J.
- Journal of Geophysical Research: Atmospheres, Vol. 114, Issue D1
Ground-based remote sensing of the atmospheric boundary layer: 25 years of progress
journal, March 1996
- Wilczak, J. M.; Gossard, E. E.; Neff, W. D.
- Boundary-Layer Meteorology, Vol. 78, Issue 3-4
Particle Formation by Ion Nucleation in the Upper Troposphere and Lower Stratosphere
journal, September 2003
- Lee, S. -H.
- Science, Vol. 301, Issue 5641
New particle formation in the free troposphere: A question of chemistry and timing
journal, May 2016
- Bianchi, F.; Trostl, J.; Junninen, H.
- Science, Vol. 352, Issue 6289
Photodissociation in the atmosphere: 1. Actinic flux and the effects of ground reflections and clouds
journal, January 1987
- Madronich, Sasha
- Journal of Geophysical Research, Vol. 92, Issue D8
Atmospheric sub-3 nm particles at high altitudes
journal, January 2010
- Mirme, S.; Mirme, A.; Minikin, A.
- Atmospheric Chemistry and Physics, Vol. 10, Issue 2
Enhanced new particle formation observed in the northern midlatitude tropopause region: MIDLATITUDE TROPOPAUSE NEW PARTICLE FORMATION
journal, May 2007
- Young, Li-Hao; Benson, David R.; Montanaro, William M.
- Journal of Geophysical Research: Atmospheres, Vol. 112, Issue D10
Ozone photochemistry in boreal biomass burning plumes
journal, January 2013
- Parrington, M.; Palmer, P. I.; Lewis, A. C.
- Atmospheric Chemistry and Physics, Vol. 13, Issue 15
New particle formation in the presence of an aerosol
journal, January 1979
- McMurry, P. H.; Friedlander, S. K.
- Atmospheric Environment (1967), Vol. 13, Issue 12
On the formation, growth and composition of nucleation mode particles
journal, January 2001
- Kulmala, M.; Maso, M. Dal; Mäkelä, J. M.
- Tellus B: Chemical and Physical Meteorology, Vol. 53, Issue 4
Observations of NO y , CO, and SO 2 and the origin of reactive nitrogen in the eastern United States
journal, February 2000
- Stehr, J. W.; Dickerson, R. R.; Hallock-Waters, K. A.
- Journal of Geophysical Research: Atmospheres, Vol. 105, Issue D3
Horizontal homogeneity and vertical extent of new particle formation events
journal, January 2007
- Wehner, Birgit; Siebert, Holger; Stratmann, Frank
- Tellus B: Chemical and Physical Meteorology, Vol. 59, Issue 3
Airborne measurements of new particle formation in the free troposphere above the Mediterranean Sea during the HYMEX campaign
journal, January 2015
- Rose, C.; Sellegri, K.; Freney, E.
- Atmospheric Chemistry and Physics, Vol. 15, Issue 17
First observations of increased ultrafine particle number concentrations near the inversion of a continental planetary boundary layer and its relation to ground-based measurements: INCREASED PARTICLE CONCENTRATIONS
journal, May 2004
- Siebert, Holger; Stratmann, Frank; Wehner, Birgit
- Geophysical Research Letters, Vol. 31, Issue 9
Vertical and horizontal variation of aerosol number size distribution in the boreal environment
journal, July 2016
- Väänänen, Riikka; Krejci, Radovan; Manninen, Hanna E.
- Atmospheric Chemistry and Physics Discussions
Slip Correction Measurements of Spherical Solid Aerosol Particles in an Improved Millikan Apparatus
journal, January 1985
- Allen, Michael D.; Raabe, Otto G.
- Aerosol Science and Technology, Vol. 4, Issue 3
Formation and growth rates of ultrafine atmospheric particles: a review of observations
journal, March 2004
- Kulmala, M.; Vehkamäki, H.; Petäjä, T.
- Journal of Aerosol Science, Vol. 35, Issue 2
Spatial and vertical extent of nucleation events in the Midwestern USA: insights from the Nucleation In ForesTs (NIFTy) experiment
journal, January 2011
- Pryor, S. C.; Barthelmie, R. J.; Sørensen, L. L.
- Atmospheric Chemistry and Physics, Vol. 11, Issue 4
Amazon boundary layer aerosol concentration sustained by vertical transport during rainfall
journal, October 2016
- Wang, Jian; Krejci, Radovan; Giangrande, Scott
- Nature, Vol. 539, Issue 7629, p. 416-419
Evolution of aerosol properties over the rain forest in Surinam, South America, observed from aircraft during the LBA-CLAIRE 98 experiment
journal, January 2003
- Krejci, Radovan
- Journal of Geophysical Research, Vol. 108, Issue D18
Daytime Atmospheric Oxidation Capacity of Urban Beijing under Polluted Conditions during the 2008 Beijing Olympic Games and the Impact of Aerosols
journal, January 2011
- Li, Jie; Wang, Zifa; Xiang, Weiling
- SOLA, Vol. 7
Evolution of planetary boundary layer under different weather conditions, and its impact on aerosol concentrations
journal, February 2013
- Quan, Jiannong; Gao, Yang; Zhang, Qiang
- Particuology, Vol. 11, Issue 1
Condensation and coagulation sinks and formation of nucleation mode particles in coastal and boreal forest boundary layers
journal, January 2002
- Dal Maso, M.
- Journal of Geophysical Research, Vol. 107, Issue D19
A criterion for new particle formation in the sulfur-rich Atlanta atmosphere
journal, January 2005
- McMurry, P. H.; Fink, M.; Sakurai, H.
- Journal of Geophysical Research, Vol. 110, Issue D22
High-Dispersed Aerosols
book, January 1971
- Fuchs, N. A.; Sutugin, A. G.
- Topics in Current Aerosol Research
Works referencing / citing this record:
Atmospheric new particle formation and growth: review of field observations
journal, September 2018
- Kerminen, Veli-Matti; Chen, Xuemeng; Vakkari, Ville
- Environmental Research Letters, Vol. 13, Issue 10
Aerosol characteristics in the entrainment interface layer in relation to the marine boundary layer and free troposphere
journal, January 2018
- Dadashazar, Hossein; Braun, Rachel A.; Crosbie, Ewan
- Atmospheric Chemistry and Physics, Vol. 18, Issue 3
Atmospheric new particle formation in China
journal, January 2019
- Chu, Biwu; Kerminen, Veli-Matti; Bianchi, Federico
- Atmospheric Chemistry and Physics, Vol. 19, Issue 1
Remote Sensing Observation of New Particle Formation Events with a (UV, VIS) Polarization Lidar
journal, July 2019
- Miffre, Alain; Cholleton, Danaël; Mehri, Tahar
- Remote Sensing, Vol. 11, Issue 15