A semi-analytical method for calculating rates of new sulfate aerosol formation from the gas phase

Kazil, J.; Lovejoy, Edward R.

doi:10.5194/acp-7-3447-2007

Cited by 77 publications

(81 citation statements)

References 34 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Switching from Vehkamäki et al (2002) to the Kazil and Lovejoy (2007) parameterization leads to an upward shift of the highest concentrations of fine particles ( Fig. 2a-b), due to a strong reduction of nucleation at altitudes of 400-150 hPa and a moderate increase at 150-50 hPa (not shown).…”

Section: Sulfuric Acid Gas and Aerosol Nucleationmentioning

confidence: 99%

See 1 more Smart Citation

The global aerosol-climate model ECHAM-HAM, version 2: sensitivity to improvements in process representations

et al. 2012

Self Cite

View full text Add to dashboard Cite

Abstract. This paper introduces and evaluates the second version of the global aerosol-climate model ECHAM-HAM. Major changes have been brought into the model, including new parameterizations for aerosol nucleation and water uptake, an explicit treatment of secondary organic aerosols, modified emission calculations for sea salt and mineral dust, the coupling of aerosol microphysics to a two-moment stratiform cloud microphysics scheme, and alternative wet scavenging parameterizations. These revisions extend the model's capability to represent details of the aerosol lifecycle and its interaction with climate. Nudged simulations of the year 2000 are carried out to compare the aerosol properties and global distribution in HAM1 and HAM2, and to evaluate them against various observations. Sensitivity experiments are performed to help identify the impact of each individual update in model formulation.Results indicate that from HAM1 to HAM2 there is a marked weakening of aerosol water uptake in the lower troposphere, reducing the total aerosol water burden from 75 Tg to 51 Tg. The main reason is the newly introduced κ-Köhler-theory-based water uptake scheme uses a lower value for the maximum relative humidity cutoff. Particulate organic matter loading in HAM2 is considerably higher in the upper troposphere, because the explicit treatment of secondary organic aerosols allows highly volatile oxidation products of the precursors to be vertically transported to regions of very low temperature and to form aerosols there. Sulfate, black carbon, particulate organic matter and mineral dust in HAM2 have longer lifetimes than in HAM1 because of weaker incloud scavenging, which is in turn related to lower autoconversion efficiency in the newly introduced two-moment cloud microphysics scheme. Modification in the sea salt emission scheme causes a significant increase in the ratio (from 1.6 to 7.7) between accumulation mode and coarse mode emission fluxes of aerosol number concentration. This leads to a general increase in the number concentration of smaller particles over the oceans in HAM2, as reflected by the higher Angström parameters.Evaluation against observation reveals that in terms of model performance, main improvements in HAM2 include a marked decrease of the systematic negative bias in the absorption aerosol optical depth, as well as smaller biases over the oceans inÅngström parameter and in the accumulation mode number concentration. The simulated geographical distribution of aerosol optical depth (AOD) is better correlated with the MODIS data, while the surface aerosol mass concentrations are very similar to those in the old version. The total aerosol water content in HAM2 is considerably Published by Copernicus Publications on behalf of the European Geosciences Union. K. Zhang et al.: Aerosol properties in ECHAM-HAM2closer to the multi-model average from Phase I of the AeroCom intercomparison project. Model deficiencies that require further efforts in the future include (i) positive biases in AOD over the ocean, (ii) n...

show abstract

Section: Sulfuric Acid Gas and Aerosol Nucleationmentioning

confidence: 99%

“…Table 5). Kazil et al (2010) implemented the scheme of Kazil and Lovejoy (2007) for neutral and charged nucleation of H 2 SO 4 and H 2 O. This parameterization is based on laboratory measurements using a semianalytical approach to calculate aerosol formation rates.…”

Section: Sulfuric Acid Gas and Aerosol Nucleationmentioning

confidence: 99%

The global aerosol-climate model ECHAM-HAM, version 2: sensitivity to improvements in process representations

et al. 2012

Self Cite

View full text Add to dashboard Cite

show abstract

“…In SAWNUC, evaporation rates of small, negatively charged clusters are based on measured thermodynamics and partly on quantum chemical calculations Froyd and Lovejoy, 2003). More detailed information on SAWNUC can be found in Lovejoy et al (2004), Kazil and Lovejoy (2007), and Ehrhart and Curtius (2013).…”

Section: Sawnuc Modelmentioning

confidence: 99%

Thermodynamics of the formation of sulfuric acid dimers in the binary (H2SO4–H2O) and ternary (H2SO4–H2O–NH3) system

Kürten¹,

Münch

Rondo

et al. 2015

Atmos. Chem. Phys.

View full text Add to dashboard Cite

Abstract. Sulfuric acid is an important gas influencing atmospheric new particle formation (NPF). Both the binary (H 2 SO 4 -H 2 O) system and the ternary system involving ammonia (H 2 SO 4 -H 2 O-NH 3 ) may be important in the free troposphere. An essential step in the nucleation of aerosol particles from gas-phase precursors is the formation of a dimer, so an understanding of the thermodynamics of dimer formation over a wide range of atmospheric conditions is essential to describe NPF. We have used the CLOUD chamber to conduct nucleation experiments for these systems at temperatures from 208 to 248 K. Neutral monomer and dimer concentrations of sulfuric acid were measured using a chemical ionization mass spectrometer (CIMS). From these measurements, dimer evaporation rates in the binary system were derived for temperatures of 208 and 223 K. We compare these results to literature data from a previous study that was conducted at higher temperatures but is in good agreement with the present study. For the ternary system the formation of Published by Copernicus Publications on behalf of the European Geosciences Union. A. Kürten et al.: Thermodynamics of the formation of sulfuric acid dimersH 2 SO 4 q NH 3 is very likely an essential step in the formation of sulfuric acid dimers, which were measured at 210, 223, and 248 K. We estimate the thermodynamic properties (dH and dS) of the H 2 SO 4 q NH 3 cluster using a simple heuristic model and the measured data. Furthermore, we report the first measurements of large neutral sulfuric acid clusters containing as many as 10 sulfuric acid molecules for the binary system using chemical ionization-atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometry.

show abstract

“…While the parametrization by Kazil and Lovejoy (2007) is based on theory and numerous laboratory experiments, the parametrization by Riipinen et al (2007) is based on observations at two (European) sites only. See also Kazil et al (2010) for an evaluation of nucleation processes in ECHAM-HAM.…”

Section: Nucleation Of H 2 So 4 Gasmentioning

confidence: 99%

“…In ECHAM-HAM, two parametrization schemes are used to calculate the formation of new nucleation mode sulfate aerosol based on environmental conditions. Binary homogenous nucleation is parametrized according to Kazil and Lovejoy (2007) and is the main nucleation mechanism yielding large particle numbers at the top of the troposphere. Boundary layer nucleation events over forest areas is modeled according to cluster activation theory (Kulmala et al, 2006) and parametrized as in Riipinen et al (2007).…”

Section: Nucleation Of H 2 So 4 Gasmentioning

confidence: 99%

A pathway analysis of global aerosol processes

Schutgens

Stier

2014

Atmos. Chem. Phys.

View full text Add to dashboard Cite

Abstract. We present a detailed budget of the changes in atmospheric aerosol mass and numbers due to various processes: emission (including instant condensation of soluble biogenic emissions), nucleation, coagulation, H 2 SO 4 condensation and in-cloud production, aging and deposition. The budget is created from monthly averaged tracer tendencies calculated by the global aerosol model ECHAM5.5-HAM2 and allows us to investigate process contributions at various length-scales and timescales. As a result, we show in unprecedented detail what processes drive the evolution of aerosol. In particular, we show that the processes that affect aerosol masses are quite different from those that affect aerosol numbers. Condensation of H 2 SO 4 gas onto preexisting particles is an important process, dominating the growth of small particles in the nucleation mode to the Aitken mode and the aging of hydrophobic matter. Together with in-cloud production of H 2 SO 4 , it significantly contributes to (and often dominates) the mass burden (and hence composition) of the hydrophilic Aitken and accumulation mode particles. Particle growth itself is the leading source of number densities in the hydrophilic Aitken and accumulation modes, with their hydrophobic counterparts contributing (even locally) relatively little. As expected, the coarse mode is dominated by primary emissions and mostly decoupled from the smaller modes. Our analysis also suggests that coagulation serves mainly as a loss process for number densities and that, relative to other processes, it is a rather unimportant contributor to composition changes of aerosol. The analysis is extended with sensitivity studies where the impact of a lower model resolution or pre-industrial emissions is shown to be small. We discuss the use of the current budget for model simplification, prioritization of model improvements, identification of potential structural model errors and model evaluation against observations.

show abstract

A semi-analytical method for calculating rates of new sulfate aerosol formation from the gas phase

Cited by 77 publications

References 34 publications

The global aerosol-climate model ECHAM-HAM, version 2: sensitivity to improvements in process representations

The global aerosol-climate model ECHAM-HAM, version 2: sensitivity to improvements in process representations

Thermodynamics of the formation of sulfuric acid dimers in the binary (H<sub>2</sub>SO<sub>4</sub>–H<sub>2</sub>O) and ternary (H<sub>2</sub>SO<sub>4</sub>–H<sub>2</sub>O–NH<sub>3</sub>) system

A pathway analysis of global aerosol processes

Contact Info

Product

Resources

About

A semi-analytical method for calculating rates of new sulfate aerosol formation from the gas phase

Cited by 77 publications

References 34 publications

The global aerosol-climate model ECHAM-HAM, version 2: sensitivity to improvements in process representations

The global aerosol-climate model ECHAM-HAM, version 2: sensitivity to improvements in process representations

Thermodynamics of the formation of sulfuric acid dimers in the binary (H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;–H&lt;sub&gt;2&lt;/sub&gt;O) and ternary (H&lt;sub&gt;2&lt;/sub&gt;SO&lt;sub&gt;4&lt;/sub&gt;–H&lt;sub&gt;2&lt;/sub&gt;O–NH&lt;sub&gt;3&lt;/sub&gt;) system

A pathway analysis of global aerosol processes

Contact Info

Product

Resources

About

Thermodynamics of the formation of sulfuric acid dimers in the binary (H<sub>2</sub>SO<sub>4</sub>–H<sub>2</sub>O) and ternary (H<sub>2</sub>SO<sub>4</sub>–H<sub>2</sub>O–NH<sub>3</sub>) system