S. Romakkaniemi

Adsorptive uptake of water by semisolid secondary organic aerosols

Aerosol climate effects are intimately tied to interactions with water. Here we combine hygroscopicity measurements with direct observations about the phase of secondary organic aerosol (SOA) particles to show that water uptake by slightly oxygenated SOA is an adsorption-dominated process under subsaturated conditions, where low solubility inhibits water uptake until the humidity is high enough for dissolution to occur. This reconciles reported discrepancies in previous hygroscopicity closure studies. We demonstrate that the difference in SOA hygroscopic behavior in subsaturated and supersaturated conditions can lead to an effect up to about 30% in the direct aerosol forcinghighlighting the need to implement correct descriptions of these processes in atmospheric models. Obtaining closure across the water saturation point is therefore a critical issue for accurate climate modeling.

Direct and indirect effects of sea spray geoengineering and the role of injected particle size

[1] Climate-aerosol model ECHAM5.5-HAM2 was used to investigate how geoengineering with artificial sea salt emissions would affect marine clouds and the Earth’s radiative balance. Prognostic cloud droplet number concentration and interaction of aerosol particles with clouds and radiation were calculated explicitly, thus making this the first time that aerosol direct effects of sea spray geoengineering are considered. When a wind speed dependent baseline geoengineering flux was applied over all oceans (total annual emissions 443.9 Tg), we predicted a radiative flux perturbation (RFP) of 5.1 W m , which is enough to counteract warming from doubled CO2 concentration. When the baseline flux was limited to three persistent stratocumulus regions (3.3% of Earth’s surface, total annual emissions 20.6 Tg), the RFP was 0.8 Wm 2 resulting mainly from a 74–80% increase in cloud droplet number concentration and a 2.5–4.4 percentage point increase in cloud cover. Multiplying the baseline mass flux by 5 or reducing the injected particle size from 250 to 100 nm had comparable effects on the geoengineering efficiency with RFPs 2.2 and 2.1 Wm , respectively. Within regions characterized with persistent stratocumulus decks, practically all of the radiative effect originated from aerosol indirect effects. However, when all oceanic regions were seeded, the direct effect with the baseline flux was globally about 29% of the total radiative effect. Together with previous studies, our results indicate that there are still large uncertainties associated with the sea spray geoengineering efficiency due to variations in e.g., background aerosol concentration, updraft velocity, cloud altitude and onset of precipitation.

Climate impacts of changing aerosol emissions since 1996

Increases in Asian aerosol emissions have been suggested as one possible reason for the hiatus in global temperature increase during the past 15 years. We study the effect of sulphur and black carbon (BC) emission changes between 1996 and 2010 on the global energy balance. We find that the increased Asian emissions have had very little regional or global effects, while the emission reductions in Europe and the U.S. have caused a positive radiative forcing. In our simulations, the global-mean aerosol direct radiative effect changes by 0.06 W/m2 during 1996 to 2010, while the effective radiative forcing (ERF) is 0.42 W/m2. The rather large ERF arises mainly from changes in cloudiness, especially in Europe. In Asia, the BC warming due to sunlight absorption has largely offset the cooling caused by sulphate aerosols. Asian BC concentrations have increased by a nearly constant fraction at all altitudes, and thus, they warm the atmosphere also in cloudy conditions.

Long-term measurements of cloud droplet concentrations and aerosol–cloud interactions in continental boundary layer clouds

The effects of aerosol on cloud droplet effective radius (R eff), cloud optical thickness and cloud droplet number concentration (N d) are analysed both from long-term direct ground-based in situ measurements conducted at the Puijo measurement station in Eastern Finland and from the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument onboard the Terra and Aqua satellites. The mean in situ N d during the period of study was 217 cm−3, while the MODIS-based N d was 171 cm−3. The absolute values, and the dependence of both N d observations on the measured aerosol number concentration in the accumulation mode (N acc), are quite similar. In both data sets N d is clearly dependent on N acc, for N acc values lower than approximately 450 cm−3. Also, the values of the aerosol–cloud-interaction parameter [ACI=(1/3)*d ln(N d)/d ln(N acc)] are quite similar for N acc<400 cm−3 with values of 0.16 and 0.14 from in situ and MODIS measurements, respectively. With higher N acc (>450 cm−3) N d increases only slowly. Similarly, the effect of aerosol on MODIS-retrieved R eff is visible only at low N acc values. In a sub set of data, the cloud and aerosol properties were measured simultaneously. For that data the comparison between MODIS-derived N d and directly measured N d, or the cloud droplet number concentration estimated from N acc values (N d,p), shows a correlation, which is greatly improved after careful screening using a ceilometer to make sure that only single cloud layers existed. This suggests that such determination of the number of cloud layers is very important when trying to match ground-based measurements to MODIS measurements.

Aerosol Chemical Composition in Cloud Events by High Resolution Time-of-Flight Aerosol Mass Spectrometry

This study presents results of direct observations of aerosol chemical composition in clouds. A high-resolution time-of-flight aerosol mass spectrometer was used to make measurements of cloud interstitial particles (INT) and mixed cloud interstitial and droplet residual particles (TOT). The differences between these two are the cloud droplet residuals (RES). Positive matrix factorization analysis of high-resolution mass spectral data sets and theoretical calculations were performed to yield distributions of chemical composition of the INT and RES particles. We observed that less oxidized hydrocarbon-like organic aerosols (HOA) were mainly distributed into the INT particles, whereas more oxidized low-volatile oxygenated OA (LVOOA) mainly in the RES particles. Nitrates existed as organic nitrate and in chemical form of NH(4)NO(3). Organic nitrates accounted for 45% of total nitrates in the INT particles, in clear contrast to 26% in the RES particles. Meanwhile, sulfates coexist in forms of acidic NH(4)HSO(4) and neutralized (NH(4))(2)SO(4). Acidic sulfate made up 64.8% of total sulfates in the INT particles, much higher than 10.7% in the RES particles. The results indicate a possible joint effect of activation ability of aerosol particles, cloud processing, and particle size effects on cloud formation.

On-Line Characterization of Morphology and Water Adsorption on Fumed Silica Nanoparticles

The first wetting layer on solid nanoparticles has direct implications on the roles these particles play in industrial processes and technological applications as well as in the atmosphere. We present a technique for online measurements of the adsorption of the first few water layers onto insoluble aerosol nanoparticles. Atomized fumed silica nanoparticles were dispersed from aqueous suspension and their hygroscopic growth factors (HGF) and number of the adsorbed water layers at subsaturated conditions were measured using a nanometer hygroscopic tandem differential mobility analyzer (HTDMA). Particle morphology was characterized by electron microscopy and particle density was determined by mobility analysis. The HGFs of the size-selected particles at mobility diameters from 10 to 50 nm at 90% relative humidity (RH) varied from 1.05 to 1.24, corresponding to 2–6 layers of adsorbed water. The morphology of the generated fumed silica nanoparticles varied from spheres at 8–10 nm to agglomerates at larger diameters with effective density from 1.7 to 0.8 g/cm3 and fractal dimension of 2.6. The smallest spheres and agglomerates had the highest HGFs. The smallest particles with diameters of 8 and 10 nm adsorbed two to three water layers in subsaturated conditions, which agreed well with the Frenkel, Halsey, and Hill (FHH) isotherm fitting. In comparison to the small spheres or large agglomerates, the compact agglomerate structure containing a few primary particles increased the number of adsorbed water layers by a factor of ∼1.5. This was probably caused by the capillary effect on the small cavities between the primary particles in the agglomerate.

Effect of aerosol size distribution changes on AOD, CCN and cloud droplet concentration: Case studies from Erfurt and Melpitz, Germany

[1] For the period of 1990 to 2000, atmospheric particulate mass concentrations have decreased in Central Europe. Simultaneously, the amount of shortwave radiation reaching the ground increased during clear sky conditions. The aerosol indirect effect has not been seen as clearly, as the radiation reaching the ground during overcast conditions has not increased as much as might be expected. Here we show that this may be caused by the condensation kinetics of water during cloud droplet formation. The decrease in the particulate mass led to a clear decrease in the number concentration of cloud condensation nuclei (CCN). However, in urban areas a relatively larger decrease in the number of particles in the upper end of the accumulation mode has led to slower condensation of water. As a result, a higher maximum supersaturation is reached during the cloud droplet formation. This compensates for the effect of decreased CCN concentrations. For example in Erfurt between 1991 and 1996, the aerosol properties changed so that aerosol optical depth decreased by 58% and CCN concentration decreased by 25 to 50%. These led to a 4 to 12% reduction in cloud droplet number concentration (CDNC) and less than a 2 Wm � 2 increase in shortwave radiation during overcast conditions. These results demonstrate that locally the aerosol direct effect can be much larger than the aerosol indirect effect. Furthermore, even though AOD appears to be a valid proxy for CCN, the correlation between AOD and CDNC is not straightforward and thus AOD cannot be used as a proxy for CDNC.

Correction of Model Reduction Errors in Simulations

In simulations of complex physical phenomena, model reductions are often required to decrease the computation time of the simulation model to a feasible level. Model reduction is often obtained by using a reduced model, which may be based on a reduced numerical approximation and simplifications of the underlying accurate model. The use of a reduced model, however, induces errors to the simulation results. In this paper, we describe and evaluate a novel approach for the correction of the approximation errors in reduced simulation models. The key idea is to model the approximation error between the accurate and reduced simulation model as an additive noise term to the reduced model and construct a low-cost predictor model for the approximation error based on statistical learning. In this paper, the approximation error approach is evaluated with the following problems: correction of spatial and temporal discretization errors in a time-varying heat equation--based evolution model, correction of spatial discre...