skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: The effect of acid–base clustering and ions on the growth of atmospheric nano-particles

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms11594· OSTI ID:1270918
 [1];  [2];  [3];  [3];  [3];  [3];  [2];  [4];  [3];  [5];  [6];  [5];  [7]; ORCiD logo [8];  [3];  [9];  [10];  [11]; ORCiD logo [12];  [13] more »;  [6];  [14];  [15];  [14];  [11];  [3];  [16];  [13];  [3];  [3];  [17];  [18]; ORCiD logo [2];  [19];  [3];  [20];  [21];  [2];  [22];  [3];  [3];  [22];  [3];  [1];  [3];  [3];  [11];  [3];  [13];  [2];  [21];  [6];  [23];  [11];  [18];  [3];  [19];  [19];  [2];  [24];  [19];  [18]; ORCiD logo [25];  [26];  [6];  [9];  [2];  [27];  [5] « less
  1. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics; Paul Scherrer Inst., Villigen (Switzerland). Laboratory of Atmospheric Chemistry
  2. Goethe-Univ. of Frankfurt, Frankfurt am Main (Germany). Inst. for Atmospheric and Environmental Sciences
  3. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics
  4. Goethe-Univ. of Frankfurt, Frankfurt am Main (Germany). Inst. for Atmospheric and Environmental Sciences; CERN, Geneva (Switzerland)
  5. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics, Inst. of Physics
  6. Paul Scherrer Inst., Villigen (Switzerland). Laboratory of Atmospheric Chemistry
  7. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics; Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics
  8. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics, Inst. of Physics; CERN, Geneva (Switzerland)
  9. Stockholm Univ., Stockholm (Sweden). Dept. of Environmental Science and Analytical Chemistry (ACES) & Bolin Centre for Climate Research
  10. CERN, Geneva (Switzerland); Univ. of Lisbon and Univ. of Beira Interior, Lisbon (Portugal). SIM
  11. Univ. of Lisbon and Univ. of Beira Interior, Lisbon (Portugal). SIM
  12. Paul Scherrer Inst., Villigen (Switzerland). Laboratory of Atmospheric Chemistry; ETH Zurich, Zurich (Switzerland). Inst. for Atmospheric and Climate Science
  13. TechnikerstraBe 25, Innsbruck (Austria). Inst. for Ion Physics and Applied Physics
  14. California Inst. of Technology, Pasadena, CA (United States). Div. of Chemistry and Chemical Engineering
  15. Univ. of Leeds, Leeds (United Kingdom). School of Earth and Environment;Atmospheric Research Centre of Eastern Finland, Kuopio (Finland). Finnish Meteorological Inst.
  16. TechnikerstraBe 25, Innsbruck (Austria). Inst. for Ion Physics and Applied Physics; Ionicon Analytik GmbH, Innsbruck (Austria)
  17. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics;Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics
  18. Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics
  19. Univ. of Vienna, Vienna (Austria). Faculty of Physics
  20. Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics; Finnish Meteorological Inst., Helsinki (Finland)
  21. Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics; Univ. of California, Irvine, CA (United States). Dept. of Chemistry
  22. CERN, Geneva (Switzerland)
  23. Leibniz Inst. for Tropospheric Research, Leipzig (Germany)
  24. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics; Goethe-Univ. of Frankfurt, Frankfurt am Main (Germany). Inst. for Atmospheric and Environmental Sciences
  25. Carnegie Mellon Univ., Pittsburgh, PA (United States). Center for Atmospheric Particle Studies
  26. Univ. of Leeds, Leeds (United Kingdom). School of Earth and Environment
  27. Univ. of Helsinki, Helsinki (Finland). Dept. of Physics; Univ. of Eastern Finland, Kuopio (Finland). Dept. of Applied Physics; Atmospheric Research Centre of Eastern Finland, Kuopio (Finland). Finnish Meteorological Inst.; Aerodyne Research Inc., Billerica, MA (United States)
+ Show Author Affiliations

The growth of freshly formed aerosol particles can be the bottleneck in their survival to cloud condensation nuclei. It is therefore crucial to understand how particles grow in the atmosphere. Insufficient experimental data has impeded a profound understanding of nano-particle growth under atmospheric conditions. Here we study nano-particle growth in the CLOUD (Cosmics Leaving OUtdoors Droplets) chamber, starting from the formation of molecular clusters. We present measured growth rates at sub-3 nm sizes with different atmospherically relevant concentrations of sulphuric acid, water, ammonia and dimethylamine. We find that atmospheric ions and small acid-base clusters, which are not generally accounted for in the measurement of sulphuric acid vapour, can participate in the growth process, leading to enhanced growth rates. The availability of compounds capable of stabilizing sulphuric acid clusters governs the magnitude of these effects and thus the exact growth mechanism. Furthermore, we bring these observations into a coherent framework and discuss their significance in the atmosphere.

Research Organization:
Univ. of California, Irvine, CA (United States)
Sponsoring Organization:
USDOE; CERN; European Union (EU); German Federal Ministry of Education and Research (BMBF); Swiss National Science Foundation (SNSF); Academy of Finland, Center of Excellence program; Austrian Science Fund (FWF); Portuguese Foundation for Science and Technology; Swedish Research Council (SRC); Russian Foundation for Basic Research; National Science Foundation (NSF); Vaisala foundation; EC Seventh Framework Programme (Marie Curie Initial Training Network 'CLOUD-ITN'); EC Seventh Framework Programme (Marie Curie Initial Training Network 'CLOUD-TRAIN'); EC Seventh Framework Programme (ERC grant 'ATMOGAIN'); EC Seventh Framework Programme (ERC grant 'MOCAPAF'; EC Seventh Framework Programme (ERC grant 'NANODYNAMITE'); EC Seventh Framework Programme (ERC grant 'ATMNUCLE')
Grant/Contract Number:
SC0014469
OSTI ID:
1270918
Journal Information:
Nature Communications, Vol. 7; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 103 works
Citation information provided by
Web of Science

References (47)

Impact of nucleation on global CCN journal January 2009
Role of sulphuric acid, ammonia and galactic cosmic rays in atmospheric aerosol nucleation journal August 2011
Molecular understanding of sulphuric acid–amine particle nucleation in the atmosphere journal October 2013
Molecular understanding of atmospheric particle formation from sulfuric acid and large oxidized organic molecules journal October 2013
Connections between atmospheric sulphuric acid and new particle formation during QUEST III–IV campaigns in Heidelberg and Hyytiälä journal January 2007
Nanoparticles in boreal forest and coastal environment: a comparison of observations and implications of the nucleation mechanism journal January 2010
Size and time-resolved growth rate measurements of 1 to 5 nm freshly formed atmospheric nuclei journal January 2012
The Role of Sulfuric Acid in Atmospheric Nucleation journal March 2010
Sub-10 nm particle growth by vapor condensation – effects of vapor molecule size and particle thermal speed journal January 2010
Evidence for the role of organics in aerosol particle formation under atmospheric conditions journal January 2010
The contribution of organics to atmospheric nanoparticle growth journal June 2012
Quantitative and time-resolved nanoparticle composition measurements during new particle formation journal January 2013
Observations of aminium salts in atmospheric nanoparticles and possible climatic implications journal January 2010
The effect of trimethylamine on atmospheric nucleation involving H 2 SO 4 journal January 2011
Acid-base chemical reaction model for nucleation rates in the polluted atmospheric boundary layer journal October 2012
Effect of condensation rate enhancement factor on 3-nm (diameter) particle formation in binary ion-induced and homogeneous nucleation journal January 2003
Uptake of neutral polar vapor molecules by charged clusters/particles: Enhancement due to dipole-charge interaction journal January 2003
Atmospheric new particle formation: real and apparent growth of neutral and charged particles journal January 2011
On-line determination of ammonia at low pptv mixing ratios in the CLOUD chamber journal January 2012
Dimethylamine and ammonia measurements with ion chromatography during the CLOUD4 campaign journal January 2012
Neutral molecular cluster formation of sulfuric acid–dimethylamine observed in real time under atmospheric conditions journal October 2014
Toward Reconciling Measurements of Atmospherically Relevant Clusters by Chemical Ionization Mass Spectrometry and Mobility Classification/Vapor Condensation journal December 2014
Atmospheric sulphuric acid and neutral cluster measurements using CI-APi-TOF journal January 2012
Atmospheric Cluster Dynamics Code: a flexible method for solution of the birth-death equations journal January 2012
Photochemical aerosol formation from SO2: A theoretical analysis of smog chamber data journal December 1980
Effect of dimethylamine on the gas phase sulfuric acid concentration measured by Chemical Ionization Mass Spectrometry journal March 2016
A large source of low-volatility secondary organic aerosol journal February 2014
Oxidation Products of Biogenic Emissions Contribute to Nucleation of Atmospheric Particles journal May 2014
Effect of ions on sulfuric acid-water binary particle formation: 2. Experimental data and comparison with QC-normalized classical nucleation theory: BINARY PARTICLE FORMATION EXPERIMENTS journal February 2016
Particle Size Magnifier for Nano-CN Detection journal March 2011
Molecular monodisperse mobility and mass standards from electrosprays of tetra-alkyl ammonium halides journal October 2005
Remarks on Ion Generation for CPC Detection Efficiency Studies in Sub-3-nm Size Range journal May 2013
Performance of diethylene glycol-based particle counters in the sub-3 nm size range journal January 2013
A high-resolution mass spectrometer to measure atmospheric ion composition journal January 2010
Measurement of the gas phase concentration of H 2 SO 4 and methane sulfonic acid and estimates of H 2 SO 4 production and loss in the atmosphere journal May 1993
Performance of a corona ion source for measurement of sulfuric acid by chemical ionization mass spectrometry journal January 2011
Calibration of a Chemical Ionization Mass Spectrometer for the Measurement of Gaseous Sulfuric Acid journal February 2012
Gas-Phase Ozonolysis of Selected Olefins: The Yield of Stabilized Criegee Intermediate and the Reactivity toward SO 2 journal September 2012
The effect of H 2 SO 4 – amine clustering on chemical ionization mass spectrometry (CIMS) measurements of gas-phase sulfuric acid journal January 2011
Atmospheric sub-3 nm particles at high altitudes journal January 2010
O2+ as reagent ion in the PTR-MS instrument: Detection of gas-phase ammonia journal September 2007
High resolution PTR-TOF: Quantification and formula confirmation of VOC in real time journal June 2010
Characterisation of organic contaminants in the CLOUD chamber at CERN journal January 2014
Growth rates of nucleation mode particles in Hyytiälä during 2003−2009: variation with particle size, season, data analysis method and ambient conditions journal January 2011
Contribution of sulfuric acid and oxidized organic compounds to particle formation and growth journal January 2012
Growth rates of atmospheric molecular clusters based on appearance times and collision–evaporation fluxes: Growth by monomers journal December 2014
An Instrumental Comparison of Mobility and Mass Measurements of Atmospheric Small Ions journal March 2011

Cited By (42)

Formation Mechanism of Atmospheric Ammonium Bisulfate: Hydrogen-Bond-Promoted Nearly Barrierless Reactions of SO 3 with NH 3 and H 2 O journal February 2018
Mass spectrometry of aerosol particle analogues in molecular beam experiments journal November 2017
Decrease in radiative forcing by organic aerosol nucleation, climate, and land use change journal January 2019
Ion-mediated hydrogen-bond rearrangement through tunnelling in the iodide–dihydrate complex journal March 2019
Robust metric for quantifying the importance of stochastic effects on nanoparticle growth journal September 2018
Atmospheric gas-to-particle conversion: why NPF events are observed in megacities? journal January 2017
Kinetics of the reaction of CO 3 ˙ − (H 2 O) n , n = 0, 1, 2, with nitric acid, a key reaction in tropospheric negative ion chemistry journal January 2018
Hydration motifs of ammonium bisulfate clusters of relevance to atmospheric new particle formation journal January 2019
Integrated experimental and theoretical approach to probe the synergistic effect of ammonia in methanesulfonic acid reactions with small alkylamines journal January 2020
Rapid growth of organic aerosol nanoparticles over a wide tropospheric temperature range journal August 2018
Molecular-resolution simulations of new particle formation: Evaluation of common assumptions made in describing nucleation in aerosol dynamics models journal November 2016
Contribution of the density-functional-based tight-binding scheme to the description of water clusters: methods, applications and extension to bulk systems journal December 2018
Chemical accuracy in modeling halide ion hydration from many-body representations journal January 2019
Atmospheric new particle formation and growth: review of field observations journal September 2018
Multicomponent new particle formation from sulfuric acid, ammonia, and biogenic vapors journal December 2018
Atmospheric new particle formation from sulfuric acid and amines in a Chinese megacity journal July 2018
Photochemistry of the Cloud Aqueous Phase: A Review journal January 2020
Observation of new particle formation and measurement of sulfuric acid, ammonia, amines and highly oxidized organic molecules at a rural site in central Germany journal January 2016
Unexpectedly acidic nanoparticles formed in dimethylamine–ammonia–sulfuric-acid nucleation experiments at CLOUD journal January 2016
Measurements of sub-3 nm particles using a particle size magnifier in different environments: from clean mountain top to polluted megacities journal January 2017
Exploring the potential of nano-Köhler theory to describe the growth of atmospheric molecular clusters by organic vapors using cluster kinetics simulations journal January 2018
Amines in boreal forest air at SMEAR II station in Finland journal January 2018
Influence of temperature on the molecular composition of ions and charged clusters during pure biogenic nucleation journal January 2018
New particle formation in the sulfuric acid–dimethylamine–water system: reevaluation of CLOUD chamber measurements and comparison to an aerosol nucleation and growth model journal January 2018
Errors in nanoparticle growth rates inferred from measurements in chemically reacting aerosol systems journal January 2018
Rate enhancement in collisions of sulfuric acid molecules due to long-range intermolecular forces journal January 2019
Formation and growth of atmospheric nanoparticles in the eastern Mediterranean: results from long-term measurements and process simulations journal January 2019
New particle formation from sulfuric acid and ammonia: nucleation and growth model based on thermodynamics derived from CLOUD measurements for a wide range of conditions journal January 2019
Temperature effects on sulfuric acid aerosol nucleation and growth: initial results from the TANGENT study journal January 2019
Role of base strength, cluster structure and charge in sulfuric-acid-driven particle formation journal January 2019
Size-resolved online chemical analysis of nanoaerosol particles: a thermal desorption differential mobility analyzer coupled to a chemical ionization time-of-flight mass spectrometer journal January 2018
Size Resolved Chemical Composition of Nanoparticles from Reactions of Sulfuric Acid with Ammonia and Dimethylamine text January 2018
Rapid growth of organic aerosol nanoparticles over a wide tropospheric temperature range text January 2018
Ion-mediated hydrogen-bond rearrangement through tunnelling in the iodide–dihydrate complex text January 2019
Molecular-resolution simulations of new particle formation: Evaluation of common assumptions made in describing nucleation in aerosol dynamics models text January 2016
Size resolved chemical composition of nanoparticles from reactions of sulfuric acid with ammonia and dimethylamine text January 2018
Multicomponent new particle formation from sulfuric acid, ammonia, and biogenic vapors text January 2018
Molecular-resolution simulations of new particle formation: Evaluation of common assumptions made in describing nucleation in aerosol dynamics models text January 2016
Size resolved chemical composition of nanoparticles from reactions of sulfuric acid with ammonia and dimethylamine journal August 2018
Size resolved chemical composition of nanoparticles from reactions of sulfuric acid with ammonia and dimethylamine text January 2018
New particle formation at urban and high-altitude remote sites in the south-eastern Iberian Peninsula journal November 2020
Influence of vegetation on occurrence and time distributions of regional new aerosol particle formation and growth journal February 2021

Similar Records

The role of low-volatility organic compounds in initial particle growth in the atmosphere
Journal Article · Wed May 25 00:00:00 EDT 2016 · Nature (London) · OSTI ID:1270918
+67 more
Effect of dimethylamine on the gas phase sulfuric acid concentration measured by Chemical Ionization Mass Spectrometry
Journal Article · Thu Mar 24 00:00:00 EDT 2016 · Journal of Geophysical Research: Atmospheres · OSTI ID:1270918
+37 more
The role of ions in new particle formation in the CLOUD chamber
Journal Article · Thu Dec 21 00:00:00 EST 2017 · Atmospheric Chemistry and Physics (Online) · OSTI ID:1270918
+70 more

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
ionization mass-spectrometry
phase sulfuric-acid
neutral cluster
boreal forest
cloud chamber
size range
nucleation
rates
ammonia
aerosol