ALBERT

Description: A specific instrument combination was developed to achieve a better microphysical and chemical characterization of atmospheric aerosol particles that have the potential to act as ice nucleating particles (INP). For this purpose a pumped counterflow virtual impactor system called IN-PCVI was set up and characterized to separate ice particles that had been activated on INP in the Fast Ice Nucleus Chamber (FINCH) from interstitial, non-activated particles. This coupled setup consisting of FINCH (ice particle activation and counting), IN-PCVI (INP separation and preparation), and further aerosol instrumentation (INP characterization) had been developed for the application in field experiments. The separated INP were characterized on-line with regard to their total number concentration, number size distribution and chemical composition, especially with the Aircraft-based Laser Ablation Aerosol Mass Spectrometer ALABAMA. Moreover, impactor samples for electron microscopy were taken. Due to the coupling the IN-PCVI had to be operated with different flow settings than known from literature, which required a further characterization of its cut-off-behavior. Taking the changed cut-off-behavior into account, the INP number concentration measured by the IN-PCVI system was in good agreement with the one detected by the FINCH optics for water saturation ratios up to 1.01 (ice saturation ratios between 1.21–1.34 and temperatures between −18 and −26 °C). First field results of INP properties are presented which were gained during the INUIT-JFJ/CLACE 2013 campaign at the high altitude research station Jungfraujoch in the Bernese Alps, Switzerland (3580 m a.s.l.).

Description: A detailed study of the levels, the temporal and diurnal variability of the main compounds involved in the biogenic sulfur cycle was carried out in Crete (Eastern Mediterranean) during the Mediterranean Intensive Oxidant Study (MINOS) field experiment in July-August 2001. Intensive measurements of gaseous dimethylsulfide (DMS), dimethylsulfoxide (DMSO), sulfur dioxide (SO2), sulfuric (H2SO4) and methanesulfonic acids (MSA) and particulate sulfate (SO42-) and methanesulfonate (MS-) have been performed during the campaign. Dimethylsulfide (DMS) levels ranged from 2.9 to 136 pmol·mol-1 (mean value of 21.7 pmol·mol-1) and showed a clear diurnal variation with daytime maximum. During nighttime DMS levels fall close or below the detection limit of 2 pmol·mol-1. Concurrent measurements of OH and NO3 radicals during the campaign indicate that NO3 levels can explain most of the observed diurnal variation of DMS. Dimethylsulfoxide (DMSO) ranged between 0.02 and 10.1 pmol·mol-1 (mean value of 1.7 pmol·mol-1) and presents a diurnal variation similar to that of DMS. SO2 levels ranged from 220 to 2970 pmol·mol-1 (mean value of 1030 pmol·mol-1), while nss-SO42- and MS- ranged from 330 to 7100 pmol·mol-1, (mean value of 1440 pmol·mol-1) and 1.1 to 37.5 pmol·mol-1 (mean value of 11.5 pmol·mol-1) respectively. Of particular interest are the measurements of gaseous MSA and H2SO4. MSA ranged from below the detection limit (3x104) to 3.7x107 molecules cm-3, whereas H2SO4 ranged between 1x105 and 9.0x107 molecules cm-3. The measured H2SO4 maxima are among the highest reported in literature and can be attributed to high insolation, absence of precipitation and increased SO2 levels in the area. From the concurrent SO2, OH, and H2SO4 measurements a sticking coefficient of 0.52±0.28 was calculated for H2SO4. From the concurrent MSA, OH, and DMS measurements the yield of gaseous MSA from the OH-initiated oxidation of DMS was calculated to range between 0.1-0.4%. This low MSA yield implies that gaseous MSA levels can not account for the observed MS- levels. Heterogeneous reactions of DMSO on aerosols should be considered to explain the observed levels of MS-.

Description: The influence of aerosols, both natural and anthropogenic, remains a major area of uncertainty when predicting the properties and behaviour of clouds and their influence on climate. In an attempt to better understand warm cloud formation in a tropical marine environment, a period of intensive measurements took place in December 2004 in Puerto Rico, using some of the latest developments in online instrumentation such as aerosol mass spectrometers, cloud condensation nuclei counters and a hygroscopicity tandem differential mobility analyser. Simultaneous online measurements of aerosol size distributions, composition, hygroscopicity and optical properties were made near the lighthouse of Cape San Juan in the north-eastern corner of the island and at the top of East Peak mountain (1040 m a.s.l.), the two sites separated by 17 km. Additional measurements of the cloud droplet residual and interstitial aerosol properties were made at the mountain site, accompanied by measurements of cloud droplet size distributions, liquid water content and the chemical composition of cloud and rain water samples. Both aerosol composition and cloud properties were found to be sensitive to wind sector. Air from the east-northeast (ENE) was mostly free of anthropogenic influences, the submicron fraction being mainly composed of non-sea salt sulphate, while that from the east-southeast (ESE) was found to be moderately influenced by populated islands upwind, adding smaller (

Description: Within the framework of the POLARCAT-France campaign, aerosol physical, chemical and optical properties over Greenland were measured onboard the French ATR-42 research aircraft. The origins of CO excess peaks detected in the aircraft measurements then have been identified through FLEXPART simulations. The study presented here focuses particularly on the characterization of air masses transported from the North American continent to Greenland. Air masses that picked up emissions from Canadian boreal forest fires as well as from the cities on the American east coast were identified and selected for a detailed study. Measurements of CO concentrations, aerosol chemical composition, aerosol number size distributions, aerosol volume volatile fractions and aerosol light absorption (mainly from black carbon) are used in order to study the relationship between CO enhancement (ΔCO), aerosol particle concentrations and number size distributions. Aerosol number size distributions (normalised with their respective ΔCO) are in good agreement with previous studies. Nonetheless, wet scavenging may have occurred along the pathway between the emission sources and Greenland leading to a less pronounced accumulation mode in the POLARCAT data. Chemical analyses from mass spectrometry show that submicrometer aerosol particles are mainly composed of sulphate and organics. The observed bimodal (Aitken and accumulation) aerosol number size distributions show a significant enhancement in Aitken mode particles. Furthermore, results from the thermodenuder analysis demonstrate the external mixture of boreal fire (BF) air masses from North America (NA). This is particularly observed in the accumulation mode, containing a volume fraction of up to 25–30% of refractory material at the applied temperature of 280 °C. NA anthropogenic air masses with only 6% refractory material in the accumulation mode can be clearly distinguished from BF air masses. Overall, during the campaign rather small amounts of black carbon from the North American continent were transported towards Greenland during the summer POLARCAT observation period, which also is a valuable finding with respect to potential climate impacts of black carbon in the Arctic.

Description: Mass spectrometric analysis of volatile and semi-volatile (=non-refractory) aerosol particles have been performed during a field study in the summer Eastern Mediterranean. A size-resolved, quantitative mass spectrometric technique (the Aerodyne Aerosol Mass Spectrometer, AMS) has been used, and the results are compared to filter sampling methods and particle sizing techniques. The different techniques agree with the finding that the fine particle mode (D

Description: We have performed a three-year series of routine lidar measurements at preselected times. The measurements were performed between 1 December 1997, and 30 November 2000, at Kühlungsborn, Germany (54°07' N, 11°46' E). Using a Rayleigh/Mie/Raman lidar system, we measured the aerosol backscatter coefficients at three wavelengths and the extinction coefficient at one wavelength. The present data analysis focuses on after-sunset Raman measurements obtained on cloud-free days. Aerosol backscatter profiles are available for altitudes above 100 m, while the majority of the extinction measurements has been restricted to heights above the residual layer. The residual layer shows an annual cycle with its maximum height in summer (2000 m) and minimum height in winter (850 m). The backscatter coefficients in the residual layer were found to be about 10 times higher than above. The mean aerosol optical depth above the residual layer and below 5 km is 0.3(±1.0) x10-2 in summer, and 1.5(±1.0) x10-2 in winter, which almost is negligible compared to values measured in during daytime in the planetary boundary layer. A cluster analysis of the backward trajectories yielded two major directions of air mass origin above the residual layer and 4 major directions inside. A marked difference between the aerosol properties dependent on the air mass origin could be found for air masses originating from the west and travelling at high wind speeds. Comparing the measured spectral dependence of the backscatter coefficients with data from the Global Aerosol Data Set, we found a general agreement, but only a few conclusions with respect to the aerosol type could be drawn due to the high variability of the measured backscatter coefficients.

Description: We deployed an aerosol mass spectrometer during the POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols, and Transport) summer campaign in Greenland in June/July 2008 on the research aircraft ATR-42. Online size resolved chemical composition data of submicron aerosol were collected up to 7.6 km altitude in the region 60 to 71° N and 40 to 60° W. Biomass burning (BB) and fossil fuel combustion (FF) plumes originating from North America, Asia, Siberia and Europe were sampled. Transport pathways of detected plumes included advection below 700 hPa, air mass uplifting in warm conveyor belts, and high altitude transport in the upper troposphere. By means of the Lagrangian particle dispersion model FLEXPART, trace gas analysis of O3 and CO, particle size distributions and aerosol chemical composition 48 pollution events were identified and classified into five chemically distinct categories. Aerosol from North American BB consisted of 22% particulate sulphate, while with increasing anthropogenic and Asian influence aerosol in Asian FF dominated plumes was composed of up to 37% sulphate category mean value. Overall, it was found that the organic matter fraction was larger (85%) in pollution plumes than for background conditions (71%). Despite different source regions and emission types the particle oxygen to carbon ratio of all plume classes was around 1 indicating low-volatility highly oxygenated aerosol. The volume size distribution of out-of-plume aerosol showed markedly smaller modes than all other distributions with two Aitken mode diameters of 24 and 43 nm and a geometric standard deviation σg of 1.12 and 1.22, respectively, while another very broad mode was found at 490 nm (σg = 2.35). Nearly pure BB particles from North America exhibited an Aitken mode at 66 nm (σg = 1.46) and an accumulation mode diameter of 392 nm (σg = 1.76). An aerosol lifetime, including all processes from emission to detection, in the range between 7 and 11 days was derived for North American emissions.

Description: Real-time measurements of non-refractory submicron aerosols (NR-PM1) were conducted within the greater Alpine region (Switzerland, Germany, Austria, France and Liechtenstein) during several week-long field campaigns in 2002–2009. This region represents one of the most important economic and recreational spaces in Europe. A large variety of sites was covered including urban backgrounds, motorways, rural, remote, and high-alpine stations, and also mobile on-road measurements were performed. Inorganic and organic aerosol (OA) fractions were determined by means of aerosol mass spectrometry (AMS). The data originating from 13 different field campaigns and the combined data have been utilized for providing an improved temporal and spatial data coverage. The average mass concentration of NR-PM1 for the different campaigns typically ranged between 10 and 30 μg m−3. Overall, the organic portion was most abundant, ranging from 36% to 81% of NR-PM1. Other main constituents comprised ammonium (5–15%), nitrate (8–36%), sulfate (3–26%), and chloride (0–5%). These latter anions were, on average, fully neutralized by ammonium. As a major result, time of the year (winter vs. summer) and location of the site (Alpine valleys vs. Plateau) could largely explain the variability in aerosol chemical composition for the different campaigns and were found to be better descriptors for aerosol composition than the type of site (urban, rural etc.). Thus, a reassessment of classifications of measurements sites might be considered in the future, possibly also for other regions of the world. The OA data was further analyzed using positive matrix factorization (PMF) and the multi-linear engine ME (factor analysis) separating the total OA into its underlying components, such as oxygenated (mostly secondary) organic aerosol (OOA), hydrocarbon-like and freshly emitted organic aerosol (HOA), as well as OA from biomass burning (BBOA). OOA was ubiquitous, ranged between 36% and 94% of OA, and could be separated into a low-volatility and a semi-volatile fraction (LV-OOA and SV-OOA) for all summer campaigns at low altitude sites. Wood combustion (BBOA) accounted for a considerable fraction during wintertime (17–49% OA), particularly in narrow Alpine valleys BBOA was often the most abundant OA component. HOA/OA ratios were comparatively low for all campaigns (6–16%) with the exception of on-road, mobile measurements (23%) in the Rhine Valley. The abundance of the aerosol components and the retrievability of SV-OOA and LV-OOA are discussed in the light of atmospheric chemistry and physics.

Description: Biogenic influences on the composition and characteristics of aerosol were investigated on Bird Island (54°00' S, 38°03' W) in the South Atlantic during November and December 2010. This remote marine environment is characterised by large seabird and seal colonies. The chemical composition of the submicron particles, measured by an aerosol mass spectrometer (AMS), was 21% non-sea-salt sulfate, 2% nitrate, 8% ammonium, 22% organics and 47% sea salt including sea salt sulfate. A new method to isolate the sea spray signature from the high-resolution AMS data was applied. Generally, the aerosol was found to be less acidic than in other marine environments due to the high availability of ammonia, from local fauna emissions. By positive matrix factorisation five different organic aerosol (OA) profiles could be isolated: an amino acid/amine factor (AA-OA, 18% of OA mass), a methanesulfonic acid OA factor (MSA-OA, 25%), a marine oxygenated OA factor (M-OOA, 41%), a sea spray OA fraction (SS-OA, 7%) and locally produced hydrocarbon-like OA (HOA, 9%). The AA-OA was dominant during the first two weeks of November and found to be related with the hatching of penguins in a nearby colony. This factor, rich in nitrogen (N : C ratio = 0.13), has implications for the biogeochemical cycling of nitrogen in the area as particulate matter is often transported over longer distances than gaseous N-rich compounds. The MSA-OA was mainly transported from more southerly latitudes where phytoplankton bloomed. The bloom was identified as one of three sources for particulate sulfate on Bird Island, next to sea salt sulfate and sulfate transported from South America. M-OOA was the dominant organic factor and found to be similar to marine OA observed at Mace Head, Ireland. An additional OA factor highly correlated with sea spray aerosol was identified (SS-OA). However, based on the available data the type of mixture, internal or external, could not be determined. Potassium was not associated with sea salt particles during 19% of the time, indicating the presence of biogenic particles in addition to the MSA-OA and AA-OA factors.

Description: The detection of primary biological material in submicron aerosol by means of thermal desorption/electron impact ionization aerosol mass spectrometry was investigated. Mass spectra of amino acids, carbohydrates, small peptides, and proteins, all of which are key building blocks of biological particles, were recorded in laboratory experiments. Several characteristic marker fragments were identified. The intensity of the marker signals relative to the total organic mass spectrum allows for an estimation of the content of primary biological material in ambient organic aerosol. The developed method was applied to mass spectra recorded during AMAZE-08, a field campaign conducted in the pristine rainforest of the central Amazon Basin, Brazil, during the wet season of February and March 2008. The low abundance of identified marker fragments places upper limits of 7.5% for amino acids and 5.6% for carbohydrates on the contribution of primary biological aerosol particles (PBAP) to the submicron organic aerosol mass concentration during this time period. Upper limits for the absolute submicron concentrations for both compound classes range from 0.01 to 0.1 μg m−3. Carbohydrates and proteins (composed of amino acids) make up for about two thirds of the dry mass of a biological cell. Thus, our findings suggest an upper limit for the PBAP mass fraction of about 20% to the submicron organic aerosol measured in Amazonia during AMAZE-08.