Photochemical Ozone and Sulphuric Acid Aerosol Formation in the Atmosphere over Southern England

Nature ◽  
1972 ◽  
Vol 235 (5338) ◽  
pp. 372-376 ◽  
Author(s):  
D. H. F. ATKINS ◽  
R. A. COX ◽  
A. E. J. EGGLETON
Keyword(s):  
Sulphuric Acid ◽  
Aerosol Formation ◽  
Southern England ◽  
Photochemical Ozone

scholarly journals Atmospheric sulphuric acid and aerosol formation: implications from atmospheric measurements for nucleation and early growth mechanisms

2006 ◽  
Vol 6 (12) ◽  
pp. 4079-4091 ◽  
Author(s):  
S.-L. Sihto ◽  
M. Kulmala ◽  
V.-M. Kerminen ◽  
M. Dal Maso ◽  
T. Petäjä ◽  
...  
Keyword(s):  
Time Delay ◽  
Sulphuric Acid ◽  
Acid Concentration ◽  
Particle Formation ◽  
Early Growth ◽  
Activation Mechanism ◽  
Aerosol Formation ◽  
Atmospheric Measurements ◽  
Nucleation Mechanisms ◽  
Sulphuric Acid Concentration

Abstract. We have investigated the formation and early growth of atmospheric secondary aerosol particles building on atmospheric measurements. The measurements were part of the QUEST 2 campaign which took place in spring 2003 in Hyytiälä (Finland). During the campaign numerous aerosol particle formation events occurred of which 15 were accompanied by gaseous sulphuric acid measurements. Our detailed analysis of these 15 events is focussed on nucleation and early growth (to a diameter of 3 nm) of fresh particles. It revealed that new particle formation seems to be a function of the gaseous sulphuric acid concentration to the power from one to two when the time delay between the sulphuric acid and particle number concentration is taken into account. From the time delay the growth rates of freshly nucleated particles from 1 nm to 3 nm were determined. The mean growth rate was 1.2 nm/h and it was clearly correlated with the gaseous sulphuric acid concentration. We tested two nucleation mechanisms – recently proposed cluster activation and kinetic type nucleation – as possible candidates to explain the observed dependences, and determined experimental nucleation coefficients. We found that some events are dominated by the activation mechanism and some by the kinetic mechanism. Inferred coefficients for the two nucleation mechanisms are the same order of magnitude as chemical reaction coefficients in the gas phase and they correlate with the product of gaseous sulphuric acid and ammonia concentrations. This indicates that besides gaseous sulphuric acid also ammonia has a role in nucleation.

scholarly journals Results from the CERN pilot CLOUD experiment

2010 ◽  
Vol 10 (4) ◽  
pp. 1635-1647 ◽  
Author(s):  
J. Duplissy ◽  
M. B. Enghoff ◽  
K. L. Aplin ◽  
F. Arnold ◽  
H. Aufmhoff ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Growth Rates ◽  
Formation Rate ◽  
Detection Threshold ◽  
Proton Synchrotron ◽  
Aerosol Formation ◽  
Stringent Requirement ◽  
Pilot Experiment ◽  
Aerosol Chamber ◽  
Ion Recombination

Abstract. During a 4-week run in October–November 2006, a pilot experiment was performed at the CERN Proton Synchrotron in preparation for the Cosmics Leaving OUtdoor Droplets (CLOUD) experiment, whose aim is to study the possible influence of cosmic rays on clouds. The purpose of the pilot experiment was firstly to carry out exploratory measurements of the effect of ionising particle radiation on aerosol formation from trace H2SO4 vapour and secondly to provide technical input for the CLOUD design. A total of 44 nucleation bursts were produced and recorded, with formation rates of particles above the 3 nm detection threshold of between 0.1 and 100 cm−3s−1, and growth rates between 2 and 37 nm h−1. The corresponding H2O concentrations were typically around 106 cm−3 or less. The experimentally-measured formation rates and H2SO4 concentrations are comparable to those found in the atmosphere, supporting the idea that sulphuric acid is involved in the nucleation of atmospheric aerosols. However, sulphuric acid alone is not able to explain the observed rapid growth rates, which suggests the presence of additional trace vapours in the aerosol chamber, whose identity is unknown. By analysing the charged fraction, a few of the aerosol bursts appear to have a contribution from ion-induced nucleation and ion-ion recombination to form neutral clusters. Some indications were also found for the accelerator beam timing and intensity to influence the aerosol particle formation rate at the highest experimental SO2 concentrations of 6 ppb, although none was found at lower concentrations. Overall, the exploratory measurements provide suggestive evidence for ion-induced nucleation or ion-ion recombination as sources of aerosol particles. However in order to quantify the conditions under which ion processes become significant, improvements are needed in controlling the experimental variables and in the reproducibility of the experiments. Finally, concerning technical aspects, the most important lessons for the CLOUD design include the stringent requirement of internal cleanliness of the aerosol chamber, as well as maintenance of extremely stable temperatures (variations below 0.1 °C

scholarly journals Marine aerosol production: a review of the current knowledge

2007 ◽  
Vol 365 (1856) ◽  
pp. 1753-1774 ◽  
Author(s):  
Colin D O'Dowd ◽  
Gerrit de Leeuw
Keyword(s):  
Sulphuric Acid ◽  
Current Knowledge ◽  
Oxidation Products ◽  
Marine Aerosol ◽  
Aerosol Formation ◽  
Multistep Process ◽  
Isoprene Oxidation ◽  
Iodine Oxides ◽  
20 Nm ◽  
Isoprene Oxidation Products

The current knowledge in primary and secondary marine aerosol formation is reviewed. For primary marine aerosol source functions, recent source functions have demonstrated a significant flux of submicrometre particles down to radii of 20 nm. Moreover, the source functions derived from different techniques up to 10 μm have come within a factor of two of each other. For secondary marine aerosol formation, recent advances have identified iodine oxides and isoprene oxidation products, in addition to sulphuric acid, as contributing to formation and growth, although the exact roles remains to be determined. While a multistep process seems to be required, isoprene oxidation products are more likely to participate in growth and sulphuric acid is more likely to participate in nucleation. Iodine oxides are likely to participate in both nucleation and growth.

scholarly journals Modelling the formation of organic particles in the atmosphere

2003 ◽  
Vol 3 (6) ◽  
pp. 6147-6178 ◽  
Author(s):  
T. Anttila ◽  
V.-M. Kerminen ◽  
M. Kulmala ◽  
A. Laaksonen ◽  
C. O’Dowd
Keyword(s):  
Sulphuric Acid ◽  
Particle Formation ◽  
Water Soluble ◽  
Forest Site ◽  
Initial Growth ◽  
Aerosol Formation ◽  
Stable Clusters ◽  
Kohler Theory ◽  
Organic Particles ◽  
Organic Particle

Abstract. A modelling study investigating the formation of organic particles from inorganic, thermodynamically stable clusters was carried out. A recently-developed theory, the so-called nano-Köhler theory, which describes a thermodynamic equilibrium between a nanometer-size cluster, water and water-soluble organic compound, was implemented in a dynamical model along with a treatment of the appropriate aerosol and gas-phase processes. The obtained results suggest that both gaseous sulphuric acid and organic vapours contribute to organic particle formation. The initial growth of freshly-nucleated clusters having a diameter around 1 nm is driven by condensation of gaseous sulphuric acid and by a lesser extent cluster self-coagulation. After the clusters have reached sizes of around 2 nm in diameter, low-volatile organic vapours start to condense spontaneously into the clusters, thereby accelerating their growth to detectable sizes. A shortage of gaseous sulphuric acid or organic vapours limit, or suppress altogether, the particle formation, since freshly-nucleated clusters are rapidly coagulated away by pre-existing particles. The obtained modelling results were applied to explaining the observed seasonal cycle in the number of aerosol formation events in a continental forest site.

Photochemical Ozone Formation in the Atmosphere over Southern England

Nature ◽  
1973 ◽  
Vol 241 (5388) ◽  
pp. 341-342 ◽  
Author(s):  
E. H. STEINBERGER ◽  
Y. BALMOR
Keyword(s):  
Ozone Formation ◽  
Southern England ◽  
Photochemical Ozone

The influence of volcano activity on aerosol formation over the Andes

2020 ◽  
Author(s):  
Federico Bianchi ◽  
Diego Aliaga ◽  
Qiaozhi Zha ◽  
Liine Heikkinen ◽  
Marcos Andrade ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Sulphuric Acid ◽  
Negative Ions ◽  
Particle Formation ◽  
Amazon Forest ◽  
Particle Nucleation ◽  
New Particle Formation ◽  
Aerosol Formation ◽  
Air Masses ◽  
Particle Sizer

<p>A significant fraction (>50%) of cloud condensation nuclei (CCN) in the atmosphere arises from new particle formation (Dunne et al., 2016). While particle nucleation has been observed almost everywhere in the atmosphere, the mechanisms governing this process are still poorly understood and subject of on-going research. For example, it is still largely unknown which components participate in new-particle formation. Laboratory experiments and quantum chemical calculations have identified potential candidates that may play a role, including sulphuric acid, ions, ammonia, amines and highly oxygenated organic molecules (Kirkby et al., 2011; Almeida et al., 2013; Bianchi et al., 2016; Bianchi et al., 2019).</p><p>Here we present observations of the formation and growth of newly formed particles measured during intense volcano activities.</p><p>The measurements were conducted at Chacaltaya mountain station (5240 m a.s.l.) in Bolivia. The station is located on top of the Cordillera Real. It has air masses coming from the Amazon forest, La Paz and the Bolivian altiplano.</p><p>With the Chemical Ionization Atmospheric Pressure interface Time-Of-Light mass spectrometers (CI-APi-TOF) we measured H<sub>2</sub>SO<sub>4</sub>, the APi-TOF retrieved the chemical composition of positive and negative ions. Ion and particle size distributions were measured with the NAIS (Neutral cluster and Air Ion Spectrometer) and the SMPS (Scanning Mobility Particle Sizer), respectively. The PSM (Particle Sizer Magnifier) measured particles with a cut off that varied from 1-4 nm. Finally, with the ACSM (Aerosol Chemical Speciation Monitor) and the FIGAERO (Filter Inlet for Gases and AEROsols) we retrieved the aerosol chemical composition. Besides this set of instruments, other parameters were measured at the Chacaltaya GAW station.</p><p>During the intensive measurement campaign, air masses coming directly from volcano eruptions were detected by all our instruments. We were therefore able to determine the gas and particle chemical composition of the air mass. In addition to that, we observed several NPF events triggered by air masses coming from volcanic emissions. With this set of instruments, we were able to retrieve the chemical composition of the vapours leading to the formation of new particles. It was found that all the nucleation event observed during the volcano activity were triggered by sulphuric acid and ammonia. In the presentation we will show more details on the chemical and physical mechanism behind this process.</p><p> </p><p>Almeida, J., et al., (2013) Nature 502, 359-363.</p><p>Bianchi, F., et al., (2016) Science 6289, 1109-1112.</p><p>Bianchi, F., et al., (2019) Chemical Review 119, 3472−3509</p><p>Dunne et al., (2016) Science 354, 1119-1124.</p><p>Kirkby, J., et al., (2011) Nature 476, (7361), 429-433.</p>

scholarly journals Radiative forcing from particle emissions by future supersonic aircraft

2008 ◽  
Vol 8 (2) ◽  
pp. 5091-5135 ◽  
Author(s):  
G. Pitari ◽  
D. Iachetti ◽  
E. Mancini ◽  
V. Montanaro ◽  
C. Marizy ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Radiative Forcing ◽  
Stratospheric Ozone ◽  
Aerosol Formation ◽  
Aircraft Emissions ◽  
Number Range ◽  
Supersonic Aircraft ◽  
Ozone Sensitivity ◽  
The Impact ◽  
Aircraft Emission

Abstract. In this work we focus on the direct radiative forcing (RF) of black carbon (BC) and sulphuric acid particles emitted by future supersonic aircraft, as well as on the ozone RF due to changes produced by emissions of both gas species (NOx, H2O) and aerosol particles capable of affecting stratospheric ozone chemistry. Heterogeneous chemical reactions on the surface of sulphuric acid stratospheric particles (SSA-SAD) are the main link between ozone chemistry and supersonic aircraft emissions of sulphur precursors (SO2) and particles (H2O-H2SO4). Photochemical O3 changes are compared from four independent 3-D atmosphere-chemistry models (ACMs), using as input the perturbation of SSA-SAD calculated in the University of L'Aquila model, which includes on-line a microphysics code for aerosol formation and growth. The ACMs in this study use aircraft emission scenarios for the year 2050 developed by AIRBUS as a part of the EU project SCENIC, assessing options for fleet size, engine technology (NOx emission index), Mach number, range and cruising altitude. From our baseline modelling simulation, the impact of supersonic aircraft on sulphuric acid aerosol and BC mass burdens is 53 and 1.5 μg/m2, respectively, with a direct RF of −11.4 and 4.6 mW/m2 (net RF=−6.8 mW/m2). This paper discusses the similarities and differences amongst the participating models in terms of O3 precursors changes due to aircraft emissions (NOx, HOx,Clx,Brx) and stratospheric ozone sensitivity to them. In the baseline case, the calculated global ozone change is −0.4±0.3 DU, with a net radiative forcing (IR+UV) of −2.5±2 mW/m2. The fraction of this O3-RF attributable to SSA-SAD changes is, however, highly variable among the models, depending on the NOx removal efficiency from the aircraft emission regions by large scale transport.

scholarly journals Atmospheric sulphuric acid and aerosol formation: implications from atmospheric measurements for nucleation and early growth mechanisms

2006 ◽  
Vol 6 (3) ◽  
pp. 3845-3882 ◽  
Author(s):  
S.-L. Sihto ◽  
M. Kulmala ◽  
V.-M. Kerminen ◽  
M. Dal Maso ◽  
T. Petäjä ◽  
...  
Keyword(s):  
Sulphuric Acid ◽  
Acid Concentration ◽  
Kinetic Mechanism ◽  
Particle Formation ◽  
Early Growth ◽  
Nucleation Theory ◽  
Activation Mechanism ◽  
Aerosol Formation ◽  
Atmospheric Measurements ◽  
Sulphuric Acid Concentration

Abstract. We have investigated the formation and early growth of atmospheric secondary aerosol particles building on atmospheric measurements. The measurements were part of the QUEST 2 campaign which took place in spring 2003 in Hyytiälä (Finland). During the campaign numerous new aerosol particle formation events occurred of which 15 were accompanied by gaseous sulphuric acid measurements. Our detailed analysis of these 15 events is focussed on nucleation and early growth (to a diameter of 3 nm) of fresh particles. It revealed that new particle formation seems to be a function of the gaseous sulphuric acid concentration to the power from one to two. The former would be consistent with the recently developed activation theory while the latter would be consistent with the kinetic nucleation theory. We find that some events are dominated by the activation mechanism and some are dominated by the kinetic mechanism. Inferred coefficients for the two nucleation mechanisms are correlated with the product of gaseous sulphuric acid and ammonia concentrations. This indicates that besides gaseous sulphuric acid also ammonia has a role in nucleation. Early growth of fresh particles to a diameter of 3 nm has a mean rate of 1.2 nm/h and is clearly correlated with the gaseous sulphuric acid concentration.

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