Peter Tunved

Hygroscopic properties of submicrometer atmospheric aerosol particles measured with H-TDMA instruments in various environments—a review

The hygroscopic properties play a vital role for the direct and indirect effects of aerosols on climate, as well as the health effects of particulate matter (PM) by modifying the deposition pattern of inhaled particles in the humid human respiratory tract. Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA) instruments have been used in field campaigns in various environments globally over the last 25 yr to determine the water uptake on submicrometre particles at subsaturated conditions. These investigations have yielded valuable and comprehensive information regarding the particle hygroscopic properties of the atmospheric aerosol, including state of mixing. These properties determine the equilibrium particle size at ambient relative humidities and have successfully been used to calculate the activation of particles at water vapour supersaturation. This paper summarizes the existing published H-TDMA results on the sizeresolved submicrometre aerosol particle hygroscopic properties obtained from ground-based measurements at multiple marine, rural, urban and free tropospheric measurement sites. The data is classified into groups of hygroscopic growth indicating the external mixture, and providing clues to the sources and processes controlling the aerosol. An evaluation is given on how different chemical and physical properties affect the hygroscopic growth.

Aerosol characteristics of air masses in northern Europe: Influences of location, transport, sinks, and sources

Synoptic-scale air masses at different stations were classified following a definition based on Berliner Wetterkarte. This air mass classification has been related to 1 year of aerosol number siz ...

Annual and interannual variation in boreal forest aerosol particle number and volume concentration and their connection to particle formation

We investigated size-resolved submicrometre aerosol particle number and volume concentration time series as well as aerosol dynamic parameters derived from Differential Mobility Particle Sizer (DMPS) measurements at five background stations in the Nordic boreal forest area. The stations in question were Aspvreten, Hyytiälä and Utö in southern Finland and Sweden, and Värriö and Pallas in the Finnish Lapland. The objective of our investigation was to identify and quantify annual and interannual variation observable in the time series. We found that the total number and mass concentrations were much lower at the Lapland stations than at the southern stations and that the total particle number was strongly correlated to particle formation event frequency. The annual total number concentration followed the annual distribution of particle formation events at the southern stations but much less clearly at the Lapland stations. The volume concentration was highest during summer, in line with higher condensation growth rates; this is in line with the assumption that a large part of the particle volume is produced by oxidized plant emissions. The decrease of sulphate emissions in Europe was not visible in our data set. Aerosol dynamic parameters such as condensation sink, condensation sink diameter and the power law exponent linking coagulation losses and condensation sink are presented to characterize the submicron Nordic background aerosol.

Is nucleation capable of explaining observed aerosol integral number increase during southerly transport over Scandinavia

Using a pseudo-Lagrangian approach, changes in aerosol size distribution was investigated during southerly transport under clear sky conditions from Finnish Lapland to Hyytiälä. Seventy-nine individual transport cases were considered. The mean transport distance was 700 km and mean transport time 66 h. On average, a sevenfold increase in Aitken mode number concentration could be observed. An increase in number concentration was observed in virtually all the cases. Several of the studied cases were associated with indications of nucleation at the receptor site. Six of the cases were simulated in detail utilizing a box-model approach. Aerosol dynamics was evaluated using the University of Helsinki Multi-component Aerosol model. Particle formation was assumed to be controlled by a kinetic nucleation mechanism. Growth of particles was suggested to be controlled by, except water and ammonia, sulphuric acid, and some unknown species with saturation vapour pressure of 3 × 106 cm-3. This product was supposed to derive from terpene oxidation by hydroxyl radical, ozone, and nitrate radical. The investigation strongly suggests nucleation events occurring over large scales to be responsible for the observed number increase during transport under modelled conditions. Using a simplified two layer structure of the lowermost troposphere, we highlight the role of vertical exchange. Modelled growth rates were found to be in agreement with observational data, in the order of 1–2 nm h–1. In order to reproduce the observed growth rates, a molar yield of condensable products from terpene oxidation of 10% was required. Concentration of sulphuric acid and condensable organic vapours were on average 3 × 106 and 1.5 × 107 cm-3, respectively.

Observational signature of the direct radiative effect by natural boreal forest aerosols and its relation to the corresponding first indirect effect

By using a screened set of long-term aerosol measurement data, the contribution of natural boreal forest aerosols to the direct radiative effect (DRE) was observed at a remote continental site in n ...

Anthropogenic aerosol effects on convective cloud microphysical properties in southern Sweden

In this study, we look for anthropogenic aerosol effects in southern Scandinavia’s clouds under the influence of moderate levels of pollution and relatively weak dynamic forcing. This was done by comparing surface aerosol measurements with convective cloud microphysical profiles produced from satellite image analyses. The results show that the clouds associated with the anthropogenic-affected air with high PM0.5, had to acquire a vertical development of ∼3.5 km before forming precipitation-sized particles, compared to less than 1 km for the clouds associated with low PM0.5 air-masses. Additionally, a comparison of profiles with precipitation was done with regard to different potentially important parameters. For precipitating clouds the variability of the cloud thickness needed to produce the precipitation (Δh14) is directly related to PM0.5 concentrations, even without considering atmospheric stability, the specific aerosol size distribution or the aerosols’ chemical composition. Each additional 1 μg m−3 of PM0.5 was found to increase Δh14 by ∼200–250 m. Our conclusion is that it is indeed possible to detect the effects of anthropogenic aerosol on the convective clouds in southern Scandinavia despite modest aerosol masses. It also emphasizes the importance of including aerosol processes in climate-radiation models and in numerical weather prediction models.

Indirect evidence of the composition of nucleation mode atmospheric particles in the high Arctic

Previous long-term observations have shown that nanoparticle formation events are common in the summer-time high Arctic and linked to local photochemical activity. However, current knowledge is limited with respect to the chemical precursors of resulting nanoparticles and the compounds involved in their subsequent growth. Here we report case-study measurements during new particle formation (NPF) events of the particle size distribution (diameter > 7 nm) and for the first time the volatility of monodisperse particles having diameter ≤40 nm, providing indirect information about their composition. Volatility measurements provide indirect evidence that a predominant fraction of the 12 nm particle population is ammoniated sulfates in the summertime high Arctic. Our observations further suggest that the majority of the sub-40 nm particle population during NPF events does not exist in the form of sulfuric acid but rather as partly or fully neutralized ammoniated sulfates.

Arctic sea ice melt leads to atmospheric new particle formation

Atmospheric new particle formation (NPF) and growth significantly influences climate by supplying new seeds for cloud condensation and brightness. Currently, there is a lack of understanding of whether and how marine biota emissions affect aerosol-cloud-climate interactions in the Arctic. Here, the aerosol population was categorised via cluster analysis of aerosol size distributions taken at Mt Zeppelin (Svalbard) during a 11 year record. The daily temporal occurrence of NPF events likely caused by nucleation in the polar marine boundary layer was quantified annually as 18%, with a peak of 51% during summer months. Air mass trajectory analysis and atmospheric nitrogen and sulphur tracers link these frequent nucleation events to biogenic precursors released by open water and melting sea ice regions. The occurrence of such events across a full decade was anti-correlated with sea ice extent. New particles originating from open water and open pack ice increased the cloud condensation nuclei concentration background by at least ca. 20%, supporting a marine biosphere-climate link through sea ice melt and low altitude clouds that may have contributed to accelerate Arctic warming. Our results prompt a better representation of biogenic aerosol sources in Arctic climate models.

The radiative effect of an aged, internally mixed Arctic aerosol originating from lower-latitude biomass burning

Arctic-haze layers and their radiative effects have been investigated previously in numerous studies as they are known to have an impact on the regional climate. In this study, we report on an event of an elevated aerosol layer, notably consisting of high-absorbing soot particles, observed in the European Arctic free troposphere the 2007 April 14 during the ASTAR 2007 campaign. The ca. 0.5 km vertically thick aerosol layer located at an altitude of around 3 km had a particle-size distribution mode around 250 nm diameter. In this study, we quantify the radiative effect aerosol layers have on the Arctic atmosphere by using in situ observations. Measurements of particles size segregated temperature stability using thermal denuders, indicate that the aerosol in the optically active size range was chemically internally mixed. In the plume, maximum observed absorption and scattering coefficients were 3 × 10−6 and 20 × 10−6 m−1, respectively. Observed microphysical and optical properties were used to constrain calculations of heating rates of an internally mixed aerosol assuming two different surface albedos that represent snow/ice covered and open ocean. The average profile resulted in a heating rate in the layer of 0.2 K d−1 for the high-albedo case and 0.15 K d−1 for the low albedo case. This calculated dependence on albedo based on actual observations corroborates previous numerical simulations. The heating within the plume resulted in a measurable signal shown as an enhancement in the temperature of a few tenths of a degree. Although the origin of the aerosol plume could not unambiguously be determined, the microphysical properties of the aerosol had strong similarities with previously reported biomass burning plumes. With a changing climate, short-lived pollutants such as biomass plumes may become more frequent in the Arctic and have important radiative effects at regional scale.

Evaluation of ground‐based black carbon measurements by filter‐based photometers at two Arctic sites

Long-term measurements of the light absorption coefficient (b(abs)) obtained with a particle soot absorption photometer (PSAP), b(abs) (PSAP), have been previously reported for Barrow, Alaska, and ...