Andreas Veira

Microphysical and optical properties of dust and tropical biomass burning aerosol layers in the Cape Verde region—an overview of the airborne in situ and lidar measurements during SAMUM-2

In the framework of the Saharan Mineral Dust Experiment (SAMUM) airborne High Spectral Resolution Lidar and in situ measurements of the particle size, aerosol mixing state and absorption coefficient were conducted. Here, the properties of mineral dust and tropical biomass burning layers in the Cape Verde region in January/February 2008 are investigated and compared with the properties of fresh dust observed in May/June 2006 close the Sahara. In the Cape Verde area, we found a complex stratification with dust layers covering the altitude range below 2 km and biomass burning layers aloft. The aerosol type of the individual layers was classified based on depolarization and lidar ratios and, in addition, on in situ measured Ångström exponents of absorption åap. The dust layers had a depth of 1.3 ± 0.4 km and showed a median åap of 3.95. The median effective diameter Deff was 2.5 μm and the dust layers over Cape Verde yielded clear signals of aging: large particles were depleted due to gravitational settling and the accumulation mode diameter was shifted towards larger sizes as a result of coagulation. The tropical biomass layers had a depth of 2.0 ± 1.1 km and were characterized by a median åap of 1.34. They always contained a certain amount of large dust particles and showed a median Deff of 1.1 μm and a fine mode Deff,fine of 0.33. The dust and biomass burning layers had a median aerosol optical depth (AOD) of 0.23 and 0.09, respectively. The median contributions to the AOD of the total atmospheric column below 10 km were 75 and 37%, respectively.

Optical and microphysical properties of smoke over Cape Verde inferred from multiwavelength lidar measurements

Lidar measurements of mixed dust/smoke plumes over the tropical Atlantic ocean were carried out during the winter campaign of SAMUM-2 at Cape Verde. Profiles of backscatter and extinction coefficients, lidar ratios, and Ångstr¨om exponents related to pure biomass-burning aerosol from southern West Africa were extracted from these observations. Furthermore, these findings were used as input for an inversion algorithm to retrieve microphysical properties of pure smoke. Seven measurement days were found suitable for the procedure of aerosol-type separation and successive inversion of optical data that describe biomass-burning smoke. We inferred high smoke lidar ratios of 87 ± 17 sr at 355 nm and 79 ± 17 sr at 532 nm. Smoke lidar ratios and Ångström exponents are higher compared to the ones for the dust/smoke mixture. These numbers indicate higher absorption and smaller sizes for pure smoke particles compared to the dust/smoke mixture. Inversion of the smoke data set results in mean effective radii of 0.22 ± 0.08 μm with individual results varying between 0.10 and 0.36 μm. The single-scattering albedo for pure biomass-burning smoke was found to vary between 0.63 and 0.89 with a very low mean value of 0.75 ± 0.07. This is in good agreement with findings of airborne in situ measurements which showed values of 0.77 ± 0.03. Effective radii from the inversion were similar to the ones found for the fine mode of the in situ size distributions.

Particle chemical properties in the vertical column based on aircraft observations in the vicinity of Cape Verde Islands

During the second Saharan Mineral Dust Experiment (SAMUM-2) field campaign, particles with geometric diameters (d) between ∼0.1 and 25 μm were collected on board of the Deutsches Zentrum f¨ur Luft- und Raumfahrt (German Aerospace Center, DLR) Falcon aircraft. Size, chemical composition and mixing state of aerosols sampled (spatially and vertically resolved) along theWest African coastline and in the Cape Verde Islands region were determined by electron microscopy. A pronounced layer structure of biomass-burning aerosol and desert dust was present for all days during the sampling period from 23 January to 6 February. The aerosol composition of the small particles (d < 0.5 μm) was highly variable and in cases of biomass burning strongly dominated by soot with up to 90% relative number abundance. Internal mixtures of soot particles with mineral dust were not detected. Soot was only observed to mix with secondary sulphate. The coarse particles (d > 0.5 μm) were dominated by silicates. In the Cape Verde Islands region mineral dust is well mixed. The determination of source regions by elemental or mineralogical composition was generally not possible, except for air masses which were transported over the Gulf of Guinea. The real part of the refractive index showed little variation. In contrast, the imaginary part strongly depended on the abundance of soot (biomass-burning aerosol) and haematite (mineral dust).

Mixing of mineral dust with urban pollution aerosol over Dakar (Senegal): impact on dust physico-chemical and radiative properties

In the framework of the Saharan Mineral Dust Experiment (SAMUM) in 2008, the mixing of the urban pollution plume of Dakar (Senegal) with mineral dust was studied in detail using the German research aircraft Falcon which was equipped with a nadir-looking high spectral resolution lidar (HSRL) and extensive aerosol in situ instrumentation. The mineral dust layer as well as the urban pollution plume were probed remotely by the HSRL and in situ. Back trajectory analyses were used to attribute aerosol samples to source regions.We found that the emission from the region of Dakar increased the aerosol optical depth (532 nm) from approximately 0.30 over sea and over land east of Dakar to 0.35 in the city outflow. In the urban area, local black carbon (BC) emissions, or soot respectively, contributed more than 75% to aerosol absorption at 530 nm. In the dust layer, the single-scattering albedo at 530 nm was 0.96 − 0.99, whereas we found a value of 0.908 ± 0.018 for the aerosol dominated by urban pollution. After 6 h of transport over the North Atlantic, the externally mixed mode of secondary aerosol particles had almost completely vanished, whereas the BC agglomerates (soot) were still externally mixed with mineral dust particles.

Wildfires in a warmer climate: Emission fluxes, emission heights and black carbon concentrations in 2090-2099

Global warming is expected to considerably impact wildfire activity and aerosol emission release in the future. Due to their complexity, the future interactions between climate change, wildfire activity, emission release, and atmospheric aerosol processes are still uncertain. Here we use the process-based fire model SPITFIRE within the global vegetation model JSBACH to simulate wildfire activity for present-day climate conditions and future Representative Concentration Pathways (RCPs). The modeled fire emission fluxes and fire radiative power serve as input for the aerosol-climate model ECHAM6-HAM2, which has been extended by a semiempirical plume height parametrization. Our results indicate a general increase in extratropical and a decrease in tropical wildfire activity at the end of the 21st century. Changes in emission fluxes are most pronounced for the strongest warming scenario RCP8.5 (+49% in the extratropics, −37% in the tropics). Tropospheric black carbon (BC) concentrations are similarly affected by changes in emission fluxes and changes in climate conditions with regional variations of up to −50% to +100%. In the Northern Hemispheric extratropics, we attribute a mean increase in aerosol optical thickness of +0.031±0.002 to changes in wildfire emissions. Due to the compensating effects of fire intensification and more stable atmospheric conditions, global mean emission heights change by at most 0.3 km with only minor influence on BC long-range transport. The changes in wildfire emission fluxes for the RCP8.5 scenario, however, may largely compensate the projected reduction in anthropogenic BC emissions by the end of the 21st century.

Assessment of background particulate matter concentrations in small cities and rural locations—Prince George, Canada

This study investigates the development and application of a simple method to calculate annual and seasonal PM2.5 and PM10 background concentrations in small cities and rural areas. The Low Pollution Sectors and Conditions (LPSC) method is based on existing measured long-term data sets and is designed for locations where particulate matter (PM) monitors are only influenced by local anthropogenic emission sources from particular wind sectors. The LPSC method combines the analysis of measured hourly meteorological data, PM concentrations, and geographical emission source distributions. PM background levels emerge from measured data for specific wind conditions, where air parcel trajectories measured at a monitoring station are assumed to have passed over geographic sectors with negligible local emissions. Seasonal and annual background levels were estimated for two monitoring stations in Prince George, Canada, and the method was also applied to four other small cities (Burns Lake, Houston, Quesnel, Smithers) in northern British Columbia. The analysis showed reasonable background concentrations for both monitoring stations in Prince George, whereas annual PM10 background concentrations at two of the other locations and PM2.5 background concentrations at one other location were implausibly high. For those locations where the LPSC method was successful, annual background levels ranged between 1.8 ± 0.1 µg/m3 and 2.5 ± 0.1 µg/m3 for PM2.5 and between 6.3 ± 0.3 µg/m3 and 8.5 ± 0.3 µg/m3 for PM10. Precipitation effects and patterns of seasonal variability in the estimated background concentrations were detectable for all locations where the method was successful. Overall the method was dependent on the configuration of local geography and sources with respect to the monitoring location, and may fail at some locations and under some conditions. Where applicable, the LPSC method can provide a fast and cost-efficient way to estimate background PM concentrations for small cities in sparsely populated regions like northern British Columbia. Implications: In rural areas like northern British Columbia, particulate matter (PM) monitoring stations are usually located close to emission sources and residential areas in order to assess the PM impact on human health. Thus there is a lack of accurate PM background concentration data that represent PM ambient concentrations in the absence of local emissions. The background calculation method developed in this study uses observed meteorological data as well as local source emission locations and provides annual, seasonal and precipitation-related PM background concentrations that are comparable to literature values for four out of six monitoring stations.

Quantifying the present and future climate impact of wildfire emission heights in an Earth System Model

Wildfires represent a major source for aerosol particles impacting atmospheric radiative transfer, atmospheric chemistry and cloud micro-physical properties. Compared to other emission sources, wildfires are unique in the sense that they are the only widespread source which can release emissions at high altitudes. Previous studies indicate that the height of the aerosol-radiation interaction crucially affects its climate impact. But the sensitivity to emission heights, i.e., the altitude at which emissions are injected into the atmosphere, has been examined only by a few case studies. In Earth system models (ESMs), the release of wildfire emissions is usually prescribed at the surface or at fixed heights. In this study, a semi-empirical plume height parametrization is implemented and advanced in the aerosol-climate model ECHAM6-HAM2 to investigate the impact of wildfire emission heights on the atmospheric long-range transport of black carbon (BC) particles and radiation. The modified plume height parametrization simulates a reasonable global plume height distribution representing a major improvement over a prescribed emission release. However, the comparison to observational aerosol optical thickness (AOT) data shows that the improved plume height implementation only slightly enhances the model performance in AOT regionally, while large biases remain globally. Free-tropospheric BC concentrations are mainly determined by tropical convection and differences in emission inventories rather than by differences between parametrized and prescribed emission heights. Using the plume height parametrization, wildfire aerosol emissions cause a top of atmosphere radiative forcing (TOA RF) of -0.20±0.07 Wm−2. A prescribed emission release at the surface entails a comparable TOA RF of -0.16±0.06 Wm−2. Overall, substantial improvements in wildfire aerosol modeling likely rely on better emission inventories and aerosol process modeling rather than on improved emission heights. In addition to the plume height sensitivity experiments, future wildfire emission fluxes and emission heights are simulated for Representative Concentration Pathway (RCP) scenarios. For this purpose, the process-based fire model SPITFIRE within the global vegetation model JSBACH is modified and run. The simulated fire emission fluxes and fire intensities serve as input for an ensemble of ECHAM6-HAM2 experiments. Compared to present day, fire emission fluxes are simulated to significantly increase in the extra-tropics by 2090-2099 due to enhanced fuel availability. The strongest changes in emission fluxes are found for the strongest warming scenario RCP8.5. In the tropics, fire emissions generally decrease due to land-use changes. While the increased atmospheric stability tends to decrease plume heights for RCP2.6 and RCP4.5, the enhanced fire intensity overcompensates the stability effects in RCP8.5. Nevertheless, mean global emission heights differ only by a few hundred meters. Changes in atmospheric BC concentrations and AOT are primarily driven by changes in fire emission fluxes and large-scale circulation patterns. In summary, this PhD thesis for the first time assesses the importance of the wildfire emission height representation in an ESM for present and future climate conditions. Although emission heights are of limited importance globally, they may be key parameters for aspects such as regional aerosol-cloud interaction. The new implementations, which link global vegetation-fire and atmospheric aerosol modeling, provide a novel framework to investigate these regional aerosol-climate interactions in future high-resolution ESMs.