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An explanatory model study is presented on semivolatile 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. 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 gasaerosol 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 200m (night) up to 600m (day) is representative for the partitioning of ammonium nitrate at the surface in the beginning of May 2008. [ABSTRACT FROM AUTHOR]

Interpretation of observed diurnal carbon dioxide (CO2) mixing ratios near the surface requires knowledge of the local dynamics of the planetary boundary layer. In this paper, we quantify the relationship between the boundary layer dynamics and the CO2 budget in convective conditions through a newly derived set of analytical equations. From these equations, we are able to quantify how uncertainties in boundary layer dynamical variables or in the morning CO2 distribution in the mixed-layer or in the free atmosphere influence the bulk CO2 mixing ratio. We find that the largest uncertainty incurred on the mid-day CO2 mixing ratio comes from the prescribed early morning CO2 mixing ratios in the stable boundary layer, and in the free atmosphere. Errors in these values influence CO2 mixing ratios inversely proportional to the boundary layer depth (h), just like uncertainties in the assumed initial boundary layer depth and surface CO2 flux. The influence of uncertainties in the boundary layer depth itself are one order of magnitude smaller. If we "invert" the problem and calculate CO2 surface exchange from observed or simulated CO2 mixing ratios, the sensitivities to errors in boundary layer dynamics also invert: they become linearly proportional to the boundary layer depth. We demonstrate these relations for a typical well characterized situation at the Cabauw tower in the Netherlands, and conclude that knowledge of the temperature and carbon dioxide vertical profiles in the early morning are of vital importance to correctly interpret observed CO2 mixing ratios during midday. [ABSTRACT FROM AUTHOR]

The article discusses the extensive description of the physical and numerical formulation of the Dutch Atmospheric Large-Eddy Simulation (DALES). The model can be applied to studies including atmospheric boundary layer, flow over sloping or heterogeneous terrain, and dispersion of inert and chemically active species. The resolution of turbulent scales larger than a certain filter width and the parameterization of smaller, less energetic scales are aimed in Large-Eddy Simulations (LES).