References

ACP

Atmospheric Chemistry and Physics

ACP

1680-7324

Copernicus GmbH

Göttingen, Germany

10.5194/acp-12-4227-2012

A coupled observation – modeling approach for studying activation kinetics from measurements of CCN activity

Raatikainen

¹ Moore

R. H.

² ³ Lathem

T. L.

¹ Nenes

¹ ²

School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta, Georgia, USA

School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia, USA

currently at: NASA Langley Research Center, Hampton, VA, USA

11 05 2012

12 9 4227 4243

This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited.

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The full text article is available as a PDF file from http://www.atmos-chem-phys.net/12/4227/2012/acp-12-4227-2012.pdf

This paper presents an approach to study droplet activation kinetics from measurements of CCN activity by the Continuous Flow Streamwise Thermal Gradient CCN Chamber (CFSTGC) and a comprehensive model of the instrument and droplet growth. The model, which can be downloaded from <a href="http://nenes.eas.gatech.edu/Experiments/CFSTGC.html "target="_blank">http://nenes.eas.gatech.edu/Experiments/CFSTGC.html </a>, is evaluated against a series of experiments with ammonium sulfate calibration aerosol. Observed and modeled droplet sizes are in excellent agreement for a water vapor uptake coefficient ~0.2, which is consistent with theoretical expectations. The model calculations can be considerably accelerated without significant loss of accuracy by assuming simplified instrument geometry and constant parabolic flow velocity profiles. With these assumptions, the model can be applied to large experimental data sets to infer kinetic growth parameters while fully accounting for water vapor depletion effects and changes in instrument operation parameters such as the column temperature, flow rates, sheath and sample flow relative humidities, and pressure. When the effects of instrument operation parameters, water vapor depletion and equilibrium dry particle properties on droplet size are accounted for, the remaining variations in droplet size are most likely due to non-equilibrium processes such as those caused by organic surface films, slow solute dissociation and glassy or highly viscous particle states. As an example of model application, data collected during a research flight in the ARCTAS 2008 campaign are analyzed. The model shows that water vapor depletion effects can explain changes in the observed average droplet size.

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