Analysis of new particle formation events and comparisons to simulations of particle number concentrations based on GEOS-Chem–advanced particle microphysics in Beijing, China

Abstract. Aerosol particles play important roles in air quality and global climate change. In this study, we analyze the measurements of particle size distribution from 12 March to 6 April 2016 in Beijing to characterize new particle formation (NPF) using the observational data of sulfuric acid, meteorological parameters, solar radiation, and the mass concentration of fine particles (PM2.5, particulate matter with diameters less than 2.5 µm). During this 26 d campaign, 11 new particle formation events are identified with obvious bursts of sub-3 nm particle number concentrations and subsequent growth of these nucleated particles. It is found that sulfuric acid concentration in Beijing does not have a significant difference between NPF event and non-event days. Low relative humidity (RH) and high daily total solar radiation appear to be favorable for the occurrence of NPF events, which is quite obvious in this campaign. The simulations using four nucleation schemes, i.e., H2SO4–H2O binary homogeneous nucleation (BHN), H2SO4–H2O–NH3 ternary homogeneous nucleation (THN), H2SO4–H2O–ion binary ion-mediated nucleation (BIMN), and H2SO4–H2O–NH3–ion ternary ion-mediated nucleation (TIMN), based on a global chemistry transport model (GEOS-Chem) coupled with an advanced particle microphysics (APM) model, are conducted to study the particle number concentrations and new particle formation process. Our comparisons between measurements and simulations indicate that the BHN scheme and BIMN scheme significantly underestimate the observed particle number concentrations, and the THN scheme captures the total particle number concentration on most NPF event days well but fails to capture the noticeable increase in particle number concentrations on 18 March and 1 April. The TIMN scheme has obvious improvement in terms of total and sub-3 nm particle number concentrations and nucleation rates. This study provides a basis for further understanding of the nucleation mechanism in Beijing.

[1]  T. Petäjä,et al.  The missing base molecules in atmospheric acid–base nucleation , 2022, National science review.

[2]  Wei You,et al.  Optimization and Evaluation of SO2 Emissions Based on WRF-Chem and 3DVAR Data Assimilation , 2022, Remote. Sens..

[3]  D. Worsnop,et al.  Contribution of Atmospheric Oxygenated Organic Compounds to Particle Growth in an Urban Environment. , 2021, Environmental science & technology.

[4]  L. Ahonen,et al.  The driving factors of new particle formation and growth in the polluted boundary layer , 2021, Atmospheric Chemistry and Physics.

[5]  T. Petäjä,et al.  Supplementary material to "Measurement Report: A Multi-Year Study on the Impacts of Chinese New Year Celebrations on Air Quality in Beijing, China" , 2021 .

[6]  Junying Sun,et al.  Enhancement of nanoparticle formation and growth during the COVID-19 lockdown period in urban Beijing , 2021, Atmospheric Chemistry and Physics.

[7]  D. Worsnop,et al.  Sulfuric acid–amine nucleation in urban Beijing , 2021, Atmospheric Chemistry and Physics.

[8]  Zhanqing Li,et al.  The impact of the atmospheric turbulence-development tendency on new particle formation: a common finding on three continents , 2020, National science review.

[9]  A. Ding,et al.  Seasonal Characteristics of New Particle Formation and Growth in Urban Beijing. , 2020, Environmental science & technology.

[10]  F. Yu,et al.  H2SO4–H2O binary and H2SO4–H2O–NH3 ternary homogeneous and ion-mediated nucleation: lookup tables version 1.0 for 3-D modeling application , 2020, Geoscientific Model Development.

[11]  T. Petäjä,et al.  Variation of size-segregated particle number concentrations in wintertime Beijing , 2020 .

[12]  Min Hu,et al.  Improving new particle formation simulation by coupling a volatility-basis set (VBS) organic aerosol module in NAQPMS+APM , 2019, Atmospheric Environment.

[13]  K. M. Nazarenko,et al.  H2SO4–H2O–NH3 ternary ion-mediated nucleation (TIMN): kinetic-based model and comparison with CLOUD measurements , 2018, Atmospheric Chemistry and Physics.

[14]  T. Petäjä,et al.  Atmospheric new particle formation in China , 2018, Atmospheric Chemistry and Physics.

[15]  Jun Zheng,et al.  Atmospheric new particle formation from sulfuric acid and amines in a Chinese megacity , 2018, Science.

[16]  Jingkun Jiang,et al.  Aerosol surface area concentration: a governing factor in new particle formation in Beijing , 2017 .

[17]  R. Jayaratne,et al.  Observations of particles at their formation sizes in Beijing, China , 2017 .

[18]  J. Hao,et al.  A miniature cylindrical differential mobility analyzer for sub-3 nm particle sizing , 2017 .

[19]  D. Ceburnis,et al.  Molecular scale evidence of new particle formation via sequential addition of HIO3 , 2016, Nature.

[20]  A. Ding,et al.  On secondary new particle formation in China , 2016, Frontiers of Environmental Science & Engineering.

[21]  I. Riipinen,et al.  The role of low-volatility organic compounds in initial particle growth in the atmosphere , 2016, Nature.

[22]  J. Seinfeld,et al.  Ion-induced nucleation of pure biogenic particles , 2016, Nature.

[23]  Qiang Zhang,et al.  A spectrometer for measuring particle size distributions in the range of 3 nm to 10 μm , 2016, Frontiers of Environmental Science & Engineering.

[24]  A. Ding,et al.  Aerosol size distribution and new particle formation in the western Yangtze River Delta of China: 2 years of measurements at the SORPES station , 2015 .

[25]  Mindong Chen,et al.  Development of a new corona discharge based ion source for high resolution time-of-flight chemical ionization mass spectrometer to measure gaseous H2SO4 and aerosol sulfate , 2015 .

[26]  Han-qing Kang,et al.  Characteristics of new particle formation events in Nanjing, China: Effect of water-soluble ions , 2015 .

[27]  Dingli Yue,et al.  Connection of organics to atmospheric new particle formation and growth at an urban site of Beijing , 2015 .

[28]  M. Molina,et al.  Elucidating severe urban haze formation in China , 2014, Proceedings of the National Academy of Sciences.

[29]  D. Worsnop,et al.  Strong atmospheric new particle formation in winter in urban Shanghai, China , 2014 .

[30]  A. Ding,et al.  Aerosols and nucleation in eastern China: first insights from the new SORPES-NJU station , 2013 .

[31]  I. Riipinen,et al.  Direct Observations of Atmospheric Aerosol Nucleation , 2013, Science.

[32]  Min Hu,et al.  Nucleation and growth of nanoparticles in the atmosphere. , 2012, Chemical reviews.

[33]  F. Yu,et al.  Simulation of particle formation and number concentration over the Eastern United States with the WRF-Chem + APM model , 2011 .

[34]  R. Turco,et al.  The size-dependent charge fraction of sub-3-nm particles as a key diagnostic of competitive nucleation mechanisms under atmospheric conditions , 2011 .

[35]  Dingli Yue,et al.  Measurements of gaseous H 2 SO 4 by AP-ID-CIMS during CAREBeijing 2008 Campaign , 2011 .

[36]  F. Yu.  A secondary organic aerosol formation model considering successive oxidation aging and kinetic condensation of organic compounds: global scale implications , 2011 .

[37]  F. Yu,et al.  Oceanic Dimethyl Sulfide Emission and New Particle Formation around the Coast of Antarctica: A Modeling Study of Seasonal Variations and Comparison with Measurements , 2010 .

[38]  H. Kalesse,et al.  Competition of coagulation sink and source rate: New particle formation in the Pearl River Delta of China , 2010 .

[39]  T. Petäjä,et al.  The Role of Sulfuric Acid in Atmospheric Nucleation , 2010, Science.

[40]  I. Riipinen,et al.  Evidence for the role of organics in aerosol particle formation under atmospheric conditions , 2010, Proceedings of the National Academy of Sciences.

[41]  G. Mann,et al.  Impact of nucleation on global CCN , 2009 .

[42]  F. Yu,et al.  Simulation of particle size distribution with a global aerosol model: contribution of nucleation to aerosol and CCN number concentrations , 2009 .

[43]  I. Riipinen,et al.  Connection of sulfuric acid to atmospheric nucleation in boreal forest. , 2009, Environmental science & technology.

[44]  Alfred Wiedensohler,et al.  Particle number size distribution in the urban atmosphere of Beijing, China , 2008 .

[45]  R. Turco,et al.  Ion-mediated nucleation as an important global source of tropospheric aerosols , 2007 .

[46]  F. Yu.  Improved quasi-unary nucleation model for binary H2SO4-H2O homogeneous nucleation. , 2007, The Journal of chemical physics.

[47]  F. Yu.  From molecular clusters to nanoparticles: second-generation ion-mediated nucleation model , 2006 .

[48]  Jocelyn Kaiser,et al.  How Dirty Air Hurts the Heart , 2005, Science.

[49]  C. O'Dowd,et al.  Physical characterization of aerosol particles during nucleation events , 2001 .

[50]  L. Pirjola,et al.  Stable sulphate clusters as a source of new atmospheric particles , 2000, Nature.

[51]  W. Stockwell,et al.  The mechanism of the HO-SO2 reaction , 1983 .