Aerosol–cloud interactions (ACI) constitute the single largest uncertainty
in anthropogenic radiative forcing. To reduce the uncertainties and gain
more confidence in the simulation of ACI, models ...need to be evaluated
against observations, in particular against measurements of cloud
condensation nuclei (CCN). Here we present a data set – ready to be used for
model validation – of long-term observations of CCN number concentrations,
particle number size distributions and chemical composition from 12
sites on 3 continents. Studied environments include coastal background,
rural background, alpine sites, remote forests and an urban surrounding.
Expectedly, CCN characteristics are highly variable across site categories.
However, they also vary within them, most strongly in the coastal background
group, where CCN number concentrations can vary by up to a factor of 30
within one season. In terms of particle activation behaviour, most
continental stations exhibit very similar activation ratios (relative to
particles > 20 nm) across the range of 0.1 to 1.0 %
supersaturation. At the coastal sites the transition from particles being
CCN inactive to becoming CCN active occurs over a wider range of the
supersaturation spectrum. Several stations show strong seasonal cycles of CCN number concentrations
and particle number size distributions, e.g. at Barrow (Arctic haze in
spring), at the alpine stations (stronger influence of polluted boundary
layer air masses in summer), the rain forest (wet and dry season) or
Finokalia (wildfire influence in autumn). The rural background and urban
sites exhibit relatively little variability throughout the year, while
short-term variability can be high especially at the urban site. The average hygroscopicity parameter, κ, calculated from the
chemical composition of submicron particles was highest at the coastal site
of Mace Head (0.6) and lowest at the rain forest station ATTO (0.2–0.3).
We performed closure studies based on κ–Köhler theory
to predict CCN number concentrations. The ratio of predicted to measured CCN
concentrations is between 0.87 and 1.4 for five different types of κ.
The temporal variability is also well captured, with Pearson
correlation coefficients exceeding 0.87. Information on CCN number concentrations at many locations is important to
better characterise ACI and their radiative forcing. But long-term
comprehensive aerosol particle characterisations are labour intensive and
costly. Hence, we recommend operating “migrating-CCNCs” to conduct
collocated CCN number concentration and particle number size distribution
measurements at individual locations throughout one year at least to derive
a seasonally resolved hygroscopicity parameter. This way, CCN number
concentrations can only be calculated based on continued particle number size
distribution information and greater spatial coverage of long-term
measurements can be achieved.
The nucleation of atmospheric vapours is an important source of new aerosol particles that can subsequently grow to form cloud condensation nuclei in the atmosphere. Most field studies of atmospheric ...aerosols over continents are influenced by atmospheric vapours of anthropogenic origin (for example, ref. 2) and, in consequence, aerosol processes in pristine, terrestrial environments remain poorly understood. The Amazon rainforest is one of the few continental regions where aerosol particles and their precursors can be studied under near-natural conditions, but the origin of small aerosol particles that grow into cloud condensation nuclei in the Amazon boundary layer remains unclear. Here we present aircraft- and ground-based measurements under clean conditions during the wet season in the central Amazon basin. We find that high concentrations of small aerosol particles (with diameters of less than 50 nanometres) in the lower free troposphere are transported from the free troposphere into the boundary layer during precipitation events by strong convective downdrafts and weaker downward motions in the trailing stratiform region. This rapid vertical transport can help to maintain the population of particles in the pristine Amazon boundary layer, and may therefore influence cloud properties and climate under natural conditions.
Size-resolved long-term measurements of atmospheric aerosol and cloud condensation nuclei (CCN) concentrations and hygroscopicity were conducted at the remote Amazon Tall Tower Observatory (ATTO) in ...the central Amazon Basin over a 1-year period and full seasonal cycle (March 2014–February 2015). The measurements provide a climatology of CCN properties characteristic of a remote central Amazonian rain forest site.The CCN measurements were continuously cycled through 10 levels of supersaturation (S = 0.11 to 1.10 %) and span the aerosol particle size range from 20 to 245 nm. The mean critical diameters of CCN activation range from 43 nm at S = 1.10 % to 172 nm at S = 0.11 %. The particle hygroscopicity exhibits a pronounced size dependence with lower values for the Aitken mode (κAit = 0.14 ± 0.03), higher values for the accumulation mode (κAcc = 0.22 ± 0.05), and an overall mean value of κmean = 0.17 ± 0.06, consistent with high fractions of organic aerosol.The hygroscopicity parameter, κ, exhibits remarkably little temporal variability: no pronounced diurnal cycles, only weak seasonal trends, and few short-term variations during long-range transport events. In contrast, the CCN number concentrations exhibit a pronounced seasonal cycle, tracking the pollution-related seasonality in total aerosol concentration. We find that the variability in the CCN concentrations in the central Amazon is mostly driven by aerosol particle number concentration and size distribution, while variations in aerosol hygroscopicity and chemical composition matter only during a few episodes.For modeling purposes, we compare different approaches of predicting CCN number concentration and present a novel parametrization, which allows accurate CCN predictions based on a small set of input data.
We present long-term (5-year) measurements of particulate matter with an upper diameter limit of ∼ 10 µm (PM10), elemental carbon (EC), organic carbon (OC), and water-soluble organic carbon (WSOC) in ...aerosol filter samples collected at the Zotino Tall Tower Observatory in the middle-taiga subzone (Siberia). The data are complemented with carbon monoxide (CO) measurements. Air mass back trajectory analysis and satellite image analysis were used to characterise potential source regions and the transport pathway of haze plumes. Polluted and background periods were selected using a non-parametric statistical approach and analysed separately. In addition, near-pristine air masses were selected based on their EC concentrations being below the detection limit of our thermal–optical instrument. Over the entire sampling campaign, 75 and 48 % of air masses in winter and in summer, respectively, and 42 % in spring and fall are classified as polluted. The observed background concentrations of CO and EC showed a sine-like behaviour with a period of 365 ± 4 days, mostly due to different degrees of dilution and the removal of polluted air masses arriving at the Zotino Tall Tower Observatory (ZOTTO) from remote sources. Our analysis of the near-pristine conditions shows that the longest periods with clean air masses were observed in summer, with a frequency of 17 %, while in wintertime only 1 % can be classified as a clean. Against a background of low concentrations of CO, EC, and OC in the near-pristine summertime, it was possible to identify pollution plumes that most likely came from crude-oil production sites located in the oil-rich regions of Western Siberia. Overall, our analysis indicates that most of the time the Siberian region is impacted by atmospheric pollution arising from biomass burning and anthropogenic emissions. A relatively clean atmosphere can be observed mainly in summer, when polluted species are removed by precipitation and the aerosol burden returns to near-pristine conditions.
During the Observations and Modeling of the Green Ocean Amazon (GoAmazon2014/5) campaign, size-resolved cloud condensation nuclei (CCN) spectra were characterized at a research site (T3) 60 km ...downwind of the city of Manaus, Brazil, in central Amazonia for 1 year (12 March 2014 to 3 March 2015). Particle hygroscopicity (κCCN) and mixing state were derived from the size-resolved CCN spectra, and the hygroscopicity of the organic component of the aerosol (κorg) was then calculated from κCCN and concurrent chemical composition measurements. The annual average κCCN increased from 0.13 at 75 nm to 0.17 at 171 nm, and the increase was largely due to an increase in sulfate volume fraction. During both wet and dry seasons, κCCN, κorg, and particle composition under background conditions exhibited essentially no diel variations. The constant κorg of ∼ 0. 15 is consistent with the largely uniform and high O : C value (∼ 0. 8), indicating that the aerosols under background conditions are dominated by the aged regional aerosol particles consisting of highly oxygenated organic compounds. For air masses strongly influenced by urban pollution and/or local biomass burning, lower values of κorg and organic O : C atomic ratio were observed during night, due to accumulation of freshly emitted particles, dominated by primary organic aerosol (POA) with low hygroscopicity, within a shallow nocturnal boundary layer. The O : C, κorg, and κCCN increased from the early morning hours and peaked around noon, driven by the formation and aging of secondary organic aerosol (SOA) and dilution of POA emissions into a deeper boundary layer, while the development of the boundary layer, which leads to mixing with aged particles from the residual layer aloft, likely also contributed to the increases. The hygroscopicities associated with individual organic factors, derived from PMF (positive matrix factorization) analysis of AMS (aerosol mass spectrometry) spectra, were estimated through multivariable linear regression. For the SOA factors, the variation of the κ value with O : C agrees well with the linear relationship reported from earlier laboratory studies of SOA hygroscopicity. On the other hand, the variation in O : C of ambient aerosol organics is largely driven by the variation in the volume fractions of POA and SOA factors, which have very different O : C values. As POA factors have hygroscopicity values well below the linear relationship between SOA hygroscopicity and O : C, mixtures with different POA and SOA fractions exhibit a steeper slope for the increase in κorg with O : C, as observed during this and earlier field studies. This finding helps better understand and reconcile the differences in the relationships between κorg and O : C observed in laboratory and field studies, therefore providing a basis for improved parameterization in global models, especially in a tropical context.
The Amazon rainforest is a sensitive ecosystem experiencing the combined pressures of progressing deforestation and climate change. Its atmospheric conditions oscillate between biogenic and biomass ...burning (BB) dominated states. The Amazon further represents one of the few remaining continental places where the atmosphere approaches pristine conditions during occasional wet season episodes. The Amazon Tall Tower Observatory (ATTO) has been established in central Amazonia to investigate the complex interactions between the rainforest ecosystem and the atmosphere. Physical and chemical aerosol properties have been analyzed continuously since 2012. This paper provides an in-depth analysis of the aerosol's optical properties at ATTO based on data from 2012 to 2017. The following key results have been obtained. The aerosol scattering and absorption coefficients at 637 nm, σsp,637 and σap,637, show a pronounced seasonality with lowest values in the clean wet season (mean ± SD: σsp,637=7.5±9.3 M m−1; σap,637=0.68±0.91 M m−1) and highest values in the BB-polluted dry season (σsp,637=33±25 M m−1; σap,637=4.0±2.2 M m−1). The single scattering albedo at 637 nm, ω0, is lowest during the dry season (ω0=0.87±0.03) and highest during the wet season (ω0=0.93±0.04). The retrieved BC mass absorption cross sections, αabs, are substantially higher than values widely used in the literature (i.e., 6.6 m2 g−1 at 637 nm wavelength), likely related to thick organic or inorganic coatings on the BC cores. Wet season values of αabs=11.4±1.2 m2 g−1 (637 nm) and dry season values of αabs=12.3±1.3 m2 g−1 (637 nm) were obtained. The BB aerosol during the dry season is a mixture of rather fresh smoke from local fires, somewhat aged smoke from regional fires, and strongly aged smoke from African fires. The African influence appears to be substantial, with its maximum from August to October. The interplay of African vs. South American BB emissions determines the aerosol optical properties (e.g., the fractions of black vs. brown carbon, BC vs. BrC). By analyzing the diel cycles, it was found that particles from elevated aerosol-rich layers are mixed down to the canopy level in the early morning and particle number concentrations decrease towards the end of the day. Brown carbon absorption at 370 nm, σap,BrC,370, was found to decrease earlier in the day, likely due to photo-oxidative processes. BC-to-CO enhancement ratios, ERBC, reflect the variability of burnt fuels, combustion phases, and atmospheric removal processes. A wide range of ERBC between 4 and 15 ng m−3 ppb−1 was observed with higher values during the dry season, corresponding to the lowest ω0 levels (0.86–0.93). The influence of the 2009/2010 and 2015/2016 El Niño periods and the associated increased fire activity on aerosol optical properties was analyzed by means of 9-year σsp and σap time series (combination of ATTO and ZF2 data). Significant El Niño-related enhancements were observed: in the dry season, σsp,637 increased from 24±18 to 48±33 M m−1 and σap, 637 from 3.8±2.8 to 5.3±2.5 M m−1. The absorption Ångström exponent, åabs, representing the aerosol absorption wavelength dependence, was mostly <1.0 with episodic increases upon smoke advection. A parameterization of åabs as a function of the BC-to-OA mass ratio for Amazonian aerosol ambient measurements is presented. The brown carbon (BrC) contribution to σap at 370 nm was obtained by calculating the theoretical BC åabs, resulting in BrC contributions of 17 %–29 % (25th and 75th percentiles) to σap 370 for the entire measurement period. The BrC contribution increased to 27 %–47 % during fire events under El Niño-related drought conditions from September to November 2015. The results presented here may serve as a basis to understand Amazonian atmospheric aerosols in terms of their interactions with solar radiation and the physical and chemical-aging processes that they undergo during transport. Additionally, the analyzed aerosol properties during the last two El Niño periods in 2009/2010 and 2015/2016 offer insights that could help to assess the climate change-related potential for forest-dieback feedbacks under warmer and drier conditions.
Natural aerosol feedbacks are expected to become more important in the future, as anthropogenic aerosol emissions decrease due to air quality policy. One such feedback is initiated by the increase in ...biogenic volatile organic compound (BVOC) emissions with higher temperatures, leading to higher secondary organic aerosol (SOA) production and a cooling of the surface via impacts on cloud radiative properties. Motivated by the considerable spread in feedback strength in Earth System Models (ESMs), we here use two long-term observational datasets from boreal and tropical forests, together with satellite data, for a process-based evaluation of the BVOC-aerosol-cloud feedback in four ESMs. The model evaluation shows that the weakest modelled feedback estimates can likely be excluded, but highlights compensating errors making it difficult to draw conclusions of the strongest estimates. Overall, the method of evaluating along process chains shows promise in pin-pointing sources of uncertainty and constraining modelled aerosol feedbacks.
Traffic-related pollution is a major concern in urban areas due to its deleterious effects on human health. The characteristics of the traffic emissions on four highway environments in the Helsinki ...metropolitan area were measured with a mobile laboratory, equipped with state-of-the-art instrumentation. Concentration gradients were observed for all traffic-related pollutants, particle number (CN), particulate mass (PM1), black carbon (BC), organics, and nitrogen oxides (NO and NO2). Flow dynamics in different environments appeared to be an important factor for the dilution of the pollutants. For example, the half-decay distances for the traffic-related CN concentrations varied from 8 to 83 m at different sites. The PM1 emissions from traffic mostly consisted of organics and BC. At the most open site, the ratio of organics to BC increased with distance to the highway, indicating condensation of volatile and semi-volatile organics on BC particles. These condensed organics were shown to be hydrocarbons as the fraction of hydrocarbon fragments in organics increased. Regarding the CN size distributions, particle growth during the dilution was not observed; however the mass size distributions measured with a soot particle aerosol mass spectrometer (SP-AMS), showed a visible shift of the mode, detected at ∼ 100 nm at the roadside, to a larger size when the distance to the roadside increased. The fleet average emission factors appeared to be lower for the CN and higher for the NO2 than ten years ago. The reason is likely to be the increased fraction of light-duty (LD) diesel vehicles in the past ten years. The fraction of heavy-duty (HD) traffic, although constituting less than 10 % of the total traffic flow, was found to have a large impact on the emissions.
The Sao Paulo Metropolitan Area is a unique case worldwide due to the extensive use of biofuel, particularly ethanol, by its large fleet of nearly 8 million cars. Based on source apportionment ...analysis of Organic Aerosols in downtown Sao Paulo, and using ethanol as tracer of passenger vehicles, we have identified primary emissions from light-duty-vehicles (LDV) and heavy-duty-vehicles (HDV), as well as secondary process component. Each of those factors mirror a relevant primary source or secondary process in this densely occupied area. Using those factors as predictors in a multiple linear regression analysis of a wide range of pollutants, we have quantified the role of primary LDV or HDV emissions, as well as atmospheric secondary processes, on air quality degradation. Results show a significant contribution of HDV emissions, despite contributing only about 5% of vehicles number in the region. The latter is responsible, for example, of 40% and 47% of benzene and black carbon atmospheric concentration, respectively. This work describes an innovative use of biofuel as a tracer of passenger vehicle emissions, allowing to better understand the role of vehicular sources on air quality degradation in one of most populated megacities worldwide.
In this study the characteristics, sources and water-solubility of submicron organic aerosol (OA) were investigated in Helsinki, Finland. An Aerodyne high-resolution time-of-flight aerosol mass ...spectrometer (HR-ToF-AMS) was used to determine the submicron non-refractory aerosol components nitrate, sulfate, ammonium, chloride and organics between April 9 and May 8, 2009. The concentrations of the major water-soluble ions and water-soluble organic carbon (WSOC) were measured by a particle-into-liquid sampler (PILS) combined with a total organic carbon (TOC) analyzer and two ion chromatographs (IC) between April 25 and May 28, 2009. Parallel measurements of the submicron particulate matter (PM1), organic carbon (OC), black carbon (BC), meteorological quantities and trace gases were used to complement and validate the AMS and PILS-TOC-IC data.
Sources or atmospheric processes affecting the organic aerosol were investigated by applying the Positive Matrix Factorization (PMF) analysis to the high-resolution mass spectra of the HR-ToF-AMS organics. All together seven factors were needed to describe the variation in the obtained dataset. The factors consisted of two different types of low-volatility oxygenated OA (LV-OOA), local and long-range-transported (LRT) biomass burning OA (BBOA), semi-volatile OA (SV-OOA), hydrocarbon-like OA (HOA), and one local source (coffee roastery). These factors were interpretable and could be connected to specific sources or chemical characteristics (biomass burning, traffic, biogenic emissions, oxidized long-range-transported aerosols, marine-processed aerosols and nearby industrial activity) of ambient aerosols. In order to study the organic fraction and PMF factors further, the elemental ratios OM:OC, O:C, H:C and N:C were calculated. The value of the OM:OC ratio varied between 1.4 and 2.1. A high OM:OC ratio (1.5–2.1) was observed for the highly-oxidized and water-soluble fraction, whereas this ratio was clearly lower (1.2–1.4) for local and fresh sources such as traffic. Two different factors representing local and long-range-transported biomass burning were observed. Local biomass burning emissions had a lower OM:OC ratio, indicating that this factor was less aged and had a different source area compared with the LRT BBOA. The water-solubilities of the OA factors were studied by investigating the correlation between these factors and WSOC and by reconstructing the concentration of water-soluble particulate organic matter (WSPOM) from the OA factors. The reconstructed WSPOM had a good correlation with the measured concentration of WSPOM.
► PILS-TOC-IC and AMS were used for chemical characterization of ambient aerosol. ► Positive matrix factorization was used for source analysis. ► Water-solubility of organic fractions from different sources was evaluated. ► Water-soluble organic carbon was found to have high (1.5–2) OM:OC-ratios. ► Two separate biomass burning (local and long-range transport) fractions were found.
PDF
