Anthropogenic aerosols may have increased upper tropospheric humidity in the 20th century

Recent simulations of deep convection with a spectral microphysics cloud model show that an increase in aerosol concentration can have a significant effect on the nature of convection with more ice precipitation and less warm rain in polluted air. The cloud lifetime and the area covered by cloud anvils of deep convection are also larger for polluted air. Therefore, it is possible that the increase of anthropogenic aerosols in most of the 20th century has increased humidity and perhaps also cloudiness in the mid- to upper troposphere. Satellite data of upper tropospheric relative humidity in 1979–1997 and observed changes in cloudiness support this hypothesis. As changes in upper tropospheric humidity strongly affect longwave radiation, it is possible that anthropogenic aerosols have had a significant warming effect in addition to their other known effects on radiation

Influence of spectral solar irradiance on the formation of new particles in the continental boundary layer

International audienceThe relationship between nucleation events and spectral solar irradiance was analysed using two years of data collected at the Station for Measuring Forest Ecosystem-Atmosphere Relations (SMEAR II) in Hyytiälä, Finland. We analysed the data in two different ways. In the first step we calculated ten nanometer average values from the irradiance measurements between 280 and 580 nm and explored if any special wavelengths groups showed higher values on event days compared to a spectral reference curve for all the days for 2 years or to reference curves for every month. The results indicated that short wavelength irradiance between 300 and 340 nm is higher on event days in winter (February and March) compared to the monthly reference graph but quantitative much smaller than in spring or summer. By building the ratio between the average values of different event classes and the yearly reference graph we obtained peaks between 1.17 and 1.6 in the short wavelength range (300--340 nm). In the next step we included number concentrations of particles between 3 and 10 nm and calculated correlation coefficients between the different wavelengths groups and the particles. The results were quite similar to those obtained previously; the highest correlation coefficients were reached for the spectral irradiance groups 3--5 (300--330 nm) with average values for the single event classes around 0.6 and a nearly linear decrease towards higher wavelengths groups by 30%. Both analyses indicate quite clearly that short wavelength irradiance between 300 and 330 or 340 nm is the most important solar spectral radiation for the formation of newly formed aerosols. In the end we introduce a photochemical mechanism as the probable responsible pathway by calculating the production rate of excited oxygen. This mechanism shows in which way short wavelength irradiance can influence the formation of new particles even though the absolute values are one to two magnitudes smaller compared to irradiance between 400 and 500 nm

The part of the solar spectrum with the highest influence on the formation of SOA in the continental boundary layer

International audienceThe relationship between nucleation events and spectral solar irradiance was analysed using two years of data collected at the Station for Measuring Forest Ecosystem-Atmosphere Relations (SMEAR II) in Hyytiälä, Finland. We analysed the data in two different ways. In the first step we calculated ten nanometer average values from the irradiance measurements between 280 and 580 nm and explored if any special wavelengths groups showed higher values on event days compared to a spectral reference curve for all the days for 2 years or to reference curves for every month. The results indicated that short wavelength irradiance between 300 and 340 nm is higher on event days in winter (February and March) compared to the monthly reference graph but quantitative much smaller than in spring or summer. By building the ratio between the average values of different event classes and the yearly reference graph we obtained peaks between 1.17 and 1.6 in the short wavelength range (300--340 nm). In the next step we included number concentrations of particles between 3 and 10 nm and calculated correlation coefficients between the different wavelengths groups and the particles. The results were quite similar to those obtained previously; the highest correlation coefficients were reached for the spectral irradiance groups 3--5 (300--330 nm) with average values for the single event classes around 0.6 and a nearly linear decrease towards higher wavelengths groups by 30%. Both analyses indicate quite clearly that short wavelength irradiance between 300 and 330 or 340 nm is the most important solar spectral radiation for the formation of newly formed aerosols. In the end we introduce a photochemical mechanism as one possible pathway how short wavelength irradiance can influence the formation of SOA by calculating the production rate of excited oxygen. This mechanism shows in which way short wavelength irradiance can influence the formation of new particles even though the absolute values are one to two magnitudes smaller compared to irradiance between 400 and 500 nm

Estimating seasonal variations in cloud droplet number concentration over the boreal forest from satellite observations

Seasonal variations in cloud droplet number concentration (NCD) in low-level stratiform clouds over the boreal forest are estimated from MODIS observations of cloud optical and microphysical properties, using a sub-adiabatic cloud model to interpret vertical profiles of cloud properties. An uncertainty analysis of the cloud model is included to reveal the main sensitivities of the cloud model. We compared the seasonal cycle in NCD, obtained using 9 yr of satellite data, to surface concentrations of potential cloud activating aerosols, measured at the SMEAR II station at Hyytiälä in Finland. The results show that NCD and cloud condensation nuclei (CCN) concentrations have no clear correlation at seasonal time scale. The fraction of aerosols that actually activate as cloud droplet decreases sharply with increasing aerosol concentrations. Furthermore, information on the stability of the atmosphere shows that low NCD is linked to stable atmospheric conditions. Combining these findings leads to the conclusion that cloud droplet activation for the studied clouds over the boreal forest is limited by convection. Our results suggest that it is important to take the strength of convection into account when studying the influence of aerosols from the boreal forest on cloud formation, although they do not rule out the possibility that aerosols from the boreal forest affect other types of clouds with a closer coupling to the surfac

Aerosol formation over the Boreal forest in Hyytiälä, Finland: monthly frequency and annual cycles ? the roles of air mass characteristics and synoptic scale meteorology

International audienceNew atmospheric particles with diameters of 3?10 nm and their subsequent growth to cloud condensation nucleus have been observed at various places in the European boundary layer. These events have been observed simultaneously within wide geographical areas (over 1000 km) in connection to specific weather systems, the cold air behind cyclones. Here we show that atmospheric aerosol formation (i.e. nucleation and initial growth) is favoured by the outbreak of cold Arctic air over northern Europe. Aerosol formation was about twice as common in Arctic air as in sub-Polar air, and even more so compared to other air masses. The most important general factor favouring aerosol formation in Arctic air and marine air was weaker competing condensational sink (CS) for the precursor gases (less pre-existing aerosols), while high CS prevented aerosol formation in heated sub-Polar air and mid-latitude air. High SO2 levels favoured nucleation in continental air and high UV-B radiation in sub-tropical air. The critical factor that determined if aerosol formation would start on a day with Arctic air was the UV-B radiation. The same applied to sub-Polar air and continental air, while increased SO2 concentration could trigger formation in heated sub-Polar and mid-latitude air, and reduced CS could cause formation in mid-latitude, marine or mixed/transient air. We speculate that strong emissions of volatile organic compounds from the Boreal forest and strong boundary layer dynamics may have caused aerosol formation in sub-Polar air masses and air in transition from a marine to a continental character. The monthly frequency of Arctic air masses and the probability for photo-chemically driven aerosol formation explains the observed annual cycle in monthly particle formation frequency as well as much of the inter annual variability. The same cyclones that transport cold, clean air from the Arctic to Europe will also transport warm polluted air in the other direction, which help cause the Arctic Haze phenomena. The cyclones have a key role for the atmospheric aerosol life cycle in mid to high latitudes. Due to the observed growth to the size of CCN in one to two days, there is a potential feed back from the effects on the CCN population and cloud albedo even within the same weather system, but also on the climatic time scale

Ternary nucleation of H_2SO_4, NH_3 and H_2O

A classical theory of the ternary homogeneous nucleation of sulfuric acid—ammonia—water is presented. For NH3 mixing ratios exceeding 1 ppt, the presence of ammonia enhances the binary (sulfuric acid—water) nucleation rate by several orders of magnitude. However, the limiting component for ternary nucleation—as for binary nucleation—is sulfuric acid. The sulfuric acid concentration needed for significant ternary nucleation is several orders of magnitude below that required in binary case

A model for particle formation and growth in the atmosphere with molecular resolution in size

International audienceThe formation and growth of atmospheric aerosol particles is considered using an exact discrete method with molecular resolution in size space. The method is immune to numerical diffusion problems that are a nuisance for typical simulation methods using a sectional representation for the particle size distribution. For condensational growth, a slight modification is proposed for the Fuchs-Sutugin expression, which improves the prediction of the growth rate of nano-sized particles by as much as a factor of two. The presented method is applied to particle formation in a Finnish Boreal forest and is shown to capture the essential features of the dynamics quite nicely. Furthermore, it is shown that the growth of the particles is roughly linear, which means that the amount of condensable vapour is constant (of the order 1013 1/m3)

Field measurements of hygroscopic properties and state of mixing of nucleation mode particles

International audienceAn Ultrafine Tandem Differential Mobility Analyser (UF-TDMA) has been used in several field campaigns over the last few years. The investigations were focused on the origin and properties of nucleation event aerosols, which are observed frequently in various environments. This paper gives a summary of the results of 10 nm and 20 nm particle hygroscopic properties from different measurement sites: an urban site, an urban background site and a forest site in Finland and a coastal site in western Ireland. The data can be classified in four hygroscopic growth classes: hydrofobic, less-hygroscopic, more-hygroscopic and sea-salt. Similar classification has been earlier presented for Aitken and accumulation mode particles. In urban air, the summertime 10 nm particles showed varying less-hygroscopic growth behaviour, while winter time 10 nm and 20 nm particles were externally mixed with two different hygroscopic growth modes. The forest measurements revealed diurnal behaviour of hygroscopic growth, with high growth factors at day time and lower during night. The urban background particles had growth behaviour similar to the urban and forest measurement sites depending on the origin of the observed particles. The coastal measurements were strongly affected by air mass history. Both 10 nm and 20 nm particles were hygroscopic in marine background air. The 10 nm particles produced during clean nucleation burst periods were hydrofobic. Diurnal variation and higher growth factors of 10 nm particles were observed in air affected by other source regions. External mixing was occasionally observed at all the sites, but incidents with more than two growth modes were extremely rare

Field measurements of hygroscopic properties and state of mixing of nucleation mode particles

An Ultrafine Tandem Differential Mobility Analyser (UF-TDMA) has been used in several field campaigns over the last few years. The investigations were focused on the origin and properties of nucleation event aerosols, which are observed frequently in various environments. This paper gives a summary of the results of 10 nm and 20 nm particle hygroscopic properties from different measurement sites: an urban site, an urban background site and a forest site in Finland and a coastal site in western Ireland. The data can be classified in four hygroscopic growth classes: hydrofobic, less-hygroscopic, more-hygroscopic and sea-salt. Similar classification has been earlier presented for Aitken and accumulation mode particles. In urban air, the summertime 10 nm particles showed varying less-hygroscopic growth behaviour, while winter time 10 nm and 20 nm particles were externally mixed with two different hygroscopic growth modes. The forest measurements revealed diurnal behaviour of hygroscopic growth, with high growth factors at day time and lower during night. The urban background particles had growth behaviour similar to the urban and forest measurement sites depending on the origin of the observed particles. The coastal measurements were strongly affected by air mass history. Both 10 nm and 20 nm particles were hygroscopic in marine background air. The 10 nm particles produced during clean nucleation burst periods were hydrofobic. Diurnal variation and higher growth factors of 10 nm particles were observed in air affected by other source regions. External mixing was occasionally observed at all the sites, but incidents with more than two growth modes were extremely rare