1Meteorology and Air Quality Section, Wageningen University, Wageningen, The Netherlands
2TNO, Earth, Environment and Life Sciences, Research Group Climate, Air and Sustainability, Utrecht, The Netherlands
3Centre for Atmospheric Science, University of Manchester, Manchester, UK
4Max Planck Institute for Meteorology, Hamburg, Germany
5Energy research Centre of the Netherlands (ECN), P.O. Box 1, 1755 LE Petten, The Netherlands
6Institute for Marine and Atmospheric Research Utrecht, The Netherlands
Received: 07 Oct 2011 – Discussion started: 20 Oct 2011
Abstract. An explanatory model study is presented on semi-volatile secondary inorganic aerosols on three clear days in May 2008 during the IMPACT campaign at the Cabauw tower in the Netherlands. A single column model in combination with the equilibrium aerosol model ISORROPIA is used. This model uses surface observations from IMPACT and calculates the gas-aerosol partitioning of ammonium nitrate. The calculated gas-aerosol equilibrium overestimates the gas phase fraction during daytime, and overestimates the aerosol phase fraction during night-time. This discrepancy can partly be solved when the approach of the gas-aerosol equilibrium is forced to proceed with a delay timescale of up to two hours. Although it is shown that the delay itself has a small effect, the most important effect is caused by the mixing of air from higher altitudes at which the equilibrium is shifted to the aerosol phase. Thus, vertical mixing is shown to have a significant influence on the calculated partitioning at the surface. On some occasions, the correspondence to the observed partitioning improves dramatically.
Revised: 06 Mar 2012 – Accepted: 19 Mar 2012 – Published: 27 Mar 2012
Even though gas-aerosol partitioning of ammonium nitrate is not instantaneous, observations show that a different equilibrium in the upper boundary layer causes aerosol ammonium nitrate concentrations to increase with altitude. Our model calculates similar vertical gradients depending on the assumed speed of gas-aerosol equilibrium. The calculated optical properties of the aerosol show a similar behaviour. The aerosol optical properties depend on the aerosol size distribution both directly, because light scattering depends on particle size, and indirectly, because the equilibration timescale depends on the aerosol sizes. Future studies should therefore focus on a fully size-resolved treatment of the gas-aerosol partitioning.
Finally, coarser-resolution models may treat the gas-aerosol equilibrium of ammonium nitrate by calculating the equilibrium with a temperature and humidity sampled at a different altitude. We found that the equilibrium at an altitude of 200 m (night) up to 600 m (day) is representative for the partitioning of ammonium nitrate at the surface in the beginning of May 2008.
Aan de Brugh, J. M. J., Henzing, J. S., Schaap, M., Morgan, W. T., van Heerwaarden, C. C., Weijers, E. P., Coe, H., and Krol, M. C.: Modelling the partitioning of ammonium nitrate in the convective boundary layer, Atmos. Chem. Phys., 12, 3005-3023, doi:10.5194/acp-12-3005-2012, 2012.