scholarly journals Boundary layer nucleation as a source of new CCN in savannah environment

2013 ◽  
Vol 13 (4) ◽  
pp. 1957-1972 ◽  
Author(s):  
L. Laakso ◽  
J. Merikanto ◽  
V. Vakkari ◽  
H. Laakso ◽  
M. Kulmala ◽  
...  

Abstract. The South African savannah region is a complex environment of air pollution and natural emissions influenced by a strong seasonal cycle in biomass burning and strong precipitation. However, the scarcity of long-term observations means that the knowledge of controlling aerosol processes in this environment is limited. Here we use a recent dataset of 18 months of aerosol size distribution observations trying to understand the annual cycle of cloud condensation nuclei (CCN). Our observations show that the concentration of CCN-sized particles remains, in line with previous studies, high throughout the year with the highest concentrations during the dry winter and the lowest during the wet summer. During the wet season with reduced anthropogenic and biomass burning primary emissions, this pool of CCN is partly filled by boundary layer nucleation with subsequent growth. The enhanced importance of formation and growth during the wet season is addressed to increased biogenic activity together with enhanced free tropospheric removal decreasing the concentration of pre-existing CCN. During the dry season, while frequent new particle formation takes place, particle growth is reduced due to reduced condensing vapour concentrations. Thus in the dry season particles are not able to grow to sizes where they may act as CCN nearly as efficiently as during the wet season. The observations are compared to simulations by a global aerosol model GLOMAP. To our surprise, the global aerosol model utilized to explain the observations was not capable of re-producing the characteristics of particle formation and the annual CCN cycle, despite earlier good performance in predicting the particle concentrations in a number of diverse environments, including the South African savannah region. While the average yearly CCN concentrations of modelled CCN is close to observed concentrations, the characteristics of nucleation bursts and subsequent growth are not captured satisfactory by the model. Our sensitivity tests using different nucleation parameterizations and condensing organic vapour production rates show that neither of these is likely to explain the differences between observed and modelled nucleation and growth rates. A sensitivity study varying 28 modelling parameters indicates that the main uncertainties in the result are due to uncertainties in biomass burning emissions during the dry season, and anthropogenic sulphur emissions during the wet season, both in terms or emitted mass and particle sizes. The uncertainties appear to be mostly related to uncertainties in primary particle emissions, including the emissions variability not captured by monthly emission inventories. The results of this paper also highlights the fact that deficiencies in emissions estimates may result in deficiencies in particle production fluxes, while the end product such as modelled CCN concentration may be in line with observations.

2012 ◽  
Vol 12 (3) ◽  
pp. 8503-8531 ◽  
Author(s):  
L. Laakso ◽  
J. Merikanto ◽  
V. Vakkari, ◽  
H. Laakso ◽  
M. Kulmala ◽  
...  

Abstract. The South African savannah region is complex environment of air pollution and natural emissions influenced by a strong seasonal cycle in biomass burning and strong precipitation. However, the scarcity of long-term observations means that our knowledge of controlling aerosol processes in this environment is very poor. Here we use a new dataset of 18 months of aerosol observations to understand the factors that control aerosol properties, and in particular cloud condensation nuclei. We find that biomass burning produces a strong source of primary CCN-sized particles during the dry winter season. However, measured CCN-sized particle concentrations remain high during the wet summer season despite the lack of burning and high wet removal rates. We show that during the wet season, a substantial fraction of CCN-sized particles originate from boundary layer new particle formation, whereas primary sources dominate during the dry winter season. The large contribution of boundary layer nucleation to CCN concentrations during the wet season is found to be due to high particle formation and growth rates and low pre-existing particle concentration in the beginning of particle formation. Based on the estimated seasonal cycle of condensable sulphuric acid and organic vapours, higher growth rates during the wet season are attributed to vapours of biogenic origin. Global model results for this region have the same seasonal cycle in nuclei growth rates but the opposite cycle in particle formation rates, and both rates are much lower than observed. In contrast, the same model tends to capture the seasonal cycle in particle concentrations at many other global sites where nucleation is an important process. These results point to deficiencies in our understanding of biogenic emissions and the factors controlling nucleation and growth in such dynamic environments.


2021 ◽  
Author(s):  
Marco A. Franco ◽  
Florian Ditas ◽  
Leslie Ann Kremper ◽  
Luiz A. T. Machado ◽  
Meinrat O. Andreae ◽  
...  

Abstract. New particle formation (NPF), referring to the nucleation of molecular clusters and their subsequent growth into the cloud condensation nuclei (CCN) size range, is a globally significant and climate-relevant source of atmospheric aerosols. Classical NPF exhibiting continuous growth from a few nanometers to the Aitken mode around 60–70 nm is widely observed in the planetary boundary layer (PBL) around the world, but not in central Amazonia. Here, classical NPF events are rarely observed in the PBL, but instead, NPF begins in the upper troposphere (UT), followed by downdraft injection of sub-50 nm (CN< 50) particles into the PBL and their subsequent growth. Central aspects of our understanding of these processes in the Amazon have remained enigmatic, however. Based on more than six years of aerosol and meteorological data from the Amazon Tall Tower Observatory (ATTO, Feb 2014 to Sep 2020), we analyzed the diurnal and seasonal patterns as well as meteorological conditions during 254 of such Amazonian growth events on 217 event days, which show a sudden occurrence of particles between 10 and 50 nm in the PBL, followed by their growth to CCN sizes. The occurrence of events was significantly higher during the wet season, with 88 % of all events from January to June, than during the dry season, with 12 % from July to December, probably due to differences in the condensation sink (CS), atmospheric aerosol load, and meteorological conditions. Across all events, a median growth rate (GR) of 5.2 nm h−1 and a median CS of 0.0011 s−1 were observed. The growth events were more frequent during the daytime (74 %) and showed higher GR (5.9 nm h−1) compared to nighttime events (4.0 nm h−1), emphasizing the role of photochemistry and PBL evolution in particle growth. About 70 % of the events showed a negative anomaly of the equivalent potential temperature (∆θ'e) – as a marker for downdrafts – and a low satellite brightness temperature (Tir) – as a marker for deep convective clouds – in good agreement with particle injection from the UT in the course of strong convective activity. About 30 % of the events, however, occurred in the absence of deep convection, partly under clear sky conditions, and with a positive ∆θ'e anomaly. Therefore, these events do not appear to be related to downdraft injection and suggest the existence of other currently unknown sources of the sub-50 nm particles.


2018 ◽  
Vol 18 (14) ◽  
pp. 10773-10797 ◽  
Author(s):  
John E. Shilling ◽  
Mikhail S. Pekour ◽  
Edward C. Fortner ◽  
Paulo Artaxo ◽  
Suzane de Sá ◽  
...  

Abstract. The Green Ocean Amazon (GoAmazon 2014/5) campaign, conducted from January 2014 to December 2015 in the vicinity of Manaus, Brazil, was designed to study the aerosol life cycle and aerosol–cloud interactions in both pristine and anthropogenically influenced conditions. As part of this campaign, the U.S. Department of Energy (DOE) Gulfstream 1 (G-1) research aircraft was deployed from 17 February to 25 March 2014 (wet season) and 6 September to 5 October 2014 (dry season) to investigate aerosol and cloud properties aloft. Here, we present results from the G-1 deployments focusing on measurements of the aerosol chemical composition and secondary organic aerosol (SOA) formation and aging. In the first portion of the paper, we provide an overview of the data and compare and contrast the data from the wet and dry season. Organic aerosol (OA) dominates the deployment-averaged chemical composition, comprising 80 % of the non-refractory PM1 aerosol mass, with sulfate comprising 14 %, nitrate 2 %, and ammonium 4 %. This product distribution was unchanged between seasons, despite the fact that total aerosol loading was significantly higher in the dry season and that regional and local biomass burning was a significant source of OA mass in the dry, but not wet, season. However, the OA was more oxidized in the dry season, with the median of the mean carbon oxidation state increasing from −0.45 in the wet season to −0.02 in the dry season. In the second portion of the paper, we discuss the evolution of the Manaus plume, focusing on 13 March 2014, one of the exemplary days in the wet season. On this flight, we observe a clear increase in OA concentrations in the Manaus plume relative to the background. As the plume is transported downwind and ages, we observe dynamic changes in the OA. The mean carbon oxidation state of the OA increases from −0.6 to −0.45 during the 4–5 h of photochemical aging. Hydrocarbon-like organic aerosol (HOA) mass is lost, with ΔHOA∕ΔCO values decreasing from 17.6 µg m−3 ppmv−1 over Manaus to 10.6 µg m−3 ppmv−1 95 km downwind. Loss of HOA is balanced out by formation of oxygenated organic aerosol (OOA), with ΔOOA∕ΔCO increasing from 9.2 to 23.1 µg m−3 ppmv−1. Because hydrocarbon-like organic aerosol (HOA) loss is balanced by OOA formation, we observe little change in the net Δorg∕ΔCO values; Δorg∕ΔCO averages 31 µg m−3 ppmv−1 and does not increase with aging. Analysis of the Manaus plume evolution using data from two additional flights in the wet season showed similar trends in Δorg∕ΔCO to the 13 March flight; Δorg∕ΔCO values averaged 34 µg m−3 ppmv−1 and showed little change over 4–6.5 h of aging. Our observation of constant Δorg∕ΔCO are in contrast to literature studies of the outflow of several North American cities, which report significant increases in Δorg∕ΔCO for the first day of plume aging. These observations suggest that SOA formation in the Manaus plume occurs, at least in part, by a different mechanism than observed in urban outflow plumes in most other literature studies. Constant Δorg∕ΔCO with plume aging has been observed in many biomass burning plumes, but we are unaware of reports of fresh urban emissions aging in this manner. These observations show that urban pollution emitted from Manaus in the wet season forms less particulate downwind as it ages than urban pollution emitted from North American cities.


2019 ◽  
Author(s):  
Chauvigné Aurélien ◽  
Diego Aliaga ◽  
Marcos Andrade ◽  
Patrick Ginot ◽  
Radovan Krejci ◽  
...  

Abstract. We present the variability of aerosol particle optical properties measured at the global Atmosphere Watch (GAW) station Chacaltaya (5240 m a.s.l.). The in-situ mountain site is ideally located to study regional impacts of the densely populated urban area of La Paz/El Alto, and the intensive activity in the Amazonian basin. Four year measurements allow to study aerosol particle properties for distinct atmospheric conditions as stable and turbulent layers, different airmass origins, as well as for wet and dry seasons, including biomass-burning influenced periods. The absorption, scattering and extinction coefficients (median annual values of 0.74, 12.14 and 12.96 Mm−1 respectively) show a clear seasonal variation with low values during the wet season (0.57, 7.94 and 8.68 Mm−1 respectively) and higher values during the dry season (0.80, 11.23 and 14.51 Mm−1 respectively). These parameters also show a pronounced diurnal variation (maximum during daytime, minimum during night-time, as a result of the dynamic and convective effects of leading to lower atmospheric layers reaching the site during daytime. Retrieved intensive optical properties are significantly different from one season to the other, showing the influence of different sources of aerosols according to the season. Both intensive and extensive optical properties of aerosols were found to be different among the different atmospheric layers. The particle light absorption, scattering and extinction coefficients are in average 1.94, 1.49 and 1.55 times higher, respectively, in the turbulent layer compared to the stable layer. We observe that the difference is highest during the wet season and lowest during the dry season. Using wavelength dependence of aerosol particle optical properties, we discriminated contributions from natural (mainly mineral dust) and anthropogenic (mainly biomass-burning and urban transport or industries) emissions according to seasons and tropospheric layers. The main sources influencing measurements at CHC are arising from the urban area of La Paz/El Alto, and regional biomass-burning from the Amazonian basin. Results show a 28 % to 80 % increase of the extinction coefficients during the biomass-burning season with respect to the dry season, which is observed in both tropospheric layers. From this analyse, long-term observations at CHC provides the first direct evidence of the impact of emissions in the Amazonian basin on atmospheric optical properties far away from their sources, all the way to the stable layer.


2019 ◽  
Vol 19 (12) ◽  
pp. 7973-8001 ◽  
Author(s):  
Suzane S. de Sá ◽  
Luciana V. Rizzo ◽  
Brett B. Palm ◽  
Pedro Campuzano-Jost ◽  
Douglas A. Day ◽  
...  

Abstract. Urbanization and deforestation have important impacts on atmospheric particulate matter (PM) over Amazonia. This study presents observations and analysis of PM1 concentration, composition, and optical properties in central Amazonia during the dry season, focusing on the anthropogenic impacts. The primary study site was located 70 km downwind of Manaus, a city of over 2 million people in Brazil, as part of the GoAmazon2014/5 experiment. A high-resolution time-of-flight aerosol mass spectrometer (AMS) provided data on PM1 composition, and aethalometer measurements were used to derive the absorption coefficient babs,BrC of brown carbon (BrC) at 370 nm. Non-refractory PM1 mass concentrations averaged 12.2 µg m−3 at the primary study site, dominated by organics (83 %), followed by sulfate (11 %). A decrease in babs,BrC was observed as the mass concentration of nitrogen-containing organic compounds decreased and the organic PM1 O:C ratio increased, suggesting atmospheric bleaching of the BrC components. The organic PM1 was separated into six different classes by positive-matrix factorization (PMF), and the mass absorption efficiency Eabs associated with each factor was estimated through multivariate linear regression of babs,BrC on the factor loadings. The largest Eabs values were associated with urban (2.04±0.14 m2 g−1) and biomass-burning (0.82±0.04 to 1.50±0.07 m2 g−1) sources. Together, these sources contributed at least 80 % of babs,BrC while accounting for 30 % to 40 % of the organic PM1 mass concentration. In addition, a comparison of organic PM1 composition between wet and dry seasons revealed that only part of the 9-fold increase in mass concentration between the seasons can be attributed to biomass burning. Biomass-burning factor loadings increased by 30-fold, elevating its relative contribution to organic PM1 from about 10 % in the wet season to 30 % in the dry season. However, most of the PM1 mass (>60 %) in both seasons was accounted for by biogenic secondary organic sources, which in turn showed an 8-fold seasonal increase in factor loadings. A combination of decreased wet deposition and increased emissions and oxidant concentrations, as well as a positive feedback on larger mass concentrations are thought to play a role in the observed increases. Furthermore, fuzzy c-means clustering identified three clusters, namely “baseline”, “event”, and “urban” to represent different pollution influences during the dry season. The baseline cluster, representing the dry season background, was associated with a mean mass concentration of 9±3 µg m−3. This concentration increased on average by 3 µg m−3 for both the urban and the event clusters. The event cluster, representing an increased influence of biomass burning and long-range transport of African volcanic emissions, was characterized by remarkably high sulfate concentrations. The urban cluster, representing the influence of Manaus emissions on top of the baseline, was characterized by an organic PM1 composition that differed from the other two clusters. The differences discussed suggest a shift in oxidation pathways as well as an accelerated oxidation cycle due to urban emissions, in agreement with findings for the wet season.


2006 ◽  
Vol 6 (10) ◽  
pp. 2911-2925 ◽  
Author(s):  
D. Chand ◽  
P. Guyon ◽  
P. Artaxo ◽  
O. Schmid ◽  
G. P. Frank ◽  
...  

Abstract. As part of the Large Scale Biosphere-Atmosphere Experiment in Amazonia – Smoke, Aerosols, Clouds, Rainfall and Climate (LBA-SMOCC) campaign, detailed surface and airborne aerosol measurements were performed over the Amazon Basin during the dry to wet season from 16 September to 14 November 2002. Optical and physical properties of aerosols at the surface, and in the boundary layer (BL) and free troposphere (FT) during the dry season are discussed in this article. Carbon monoxide (CO) is used as a tracer for biomass burning emissions. At the surface, good correlation among the light scattering coefficient (σs at 545 nm), PM2.5, and CO indicates that biomass burning is the main source of aerosols. Accumulation of haze during some of the large-scale biomass burning events led to high PM2.5 (225 μg m−3), σs (1435 Mm−1), aerosol optical depth at 500 nm (3.0), and CO (3000 ppb). A few rainy episodes reduced the PM2.5, number concentration (CN) and CO concentration by two orders of magnitude. The correlation analysis between σs and aerosol optical thickness shows that most of the optically active aerosols are confined to a layer with a scale height of 1617 m during the burning season. This is confirmed by aircraft profiles. The average mass scattering and absorption efficiencies (545 nm) for small particles (diameter Dp<1.5 μm) at surface level are found to be 5.0 and 0.33 m2 g−1, respectively, when relating the aerosol optical properties to PM2.5 aerosols. The observed mean single scattering albedo (ωo at 545 nm) for submicron aerosols at the surface is 0.92±0.02. The light scattering by particles (Δσs/Δ CN) increase 2–10 times from the surface to the FT, most probably due to the combined affects of coagulation and condensation.


2005 ◽  
Vol 5 (2) ◽  
pp. 311-335 ◽  
Author(s):  
B. Sauvage ◽  
V. Thouret ◽  
J.-P. Cammas ◽  
F. Gheusi ◽  
G. Athier ◽  
...  

Abstract. We analyze ozone observations recorded over Equatorial Africa between April 1997 and March 2003 by the MOZAIC programme, providing the first ozone climatology deriving from continental in-situ data over this region. Three-dimensional streamlines strongly suggests connections between the characteristics of the ozone monthly mean vertical profiles, the most persistent circulation patterns in the troposphere over Equatorial Africa (on a monthly basis) such as the Harmattan, the African Easterly Jet, the Trades and the regions of ozone precursors emissions by biomass burning. During the biomass burning season in each hemisphere, the lower troposphere exhibits layers of enhanced ozone (i.e. 70 ppbv over the coast of Gulf of Guinea in December-February and 85 ppbv over Congo in June-August). The characteristics of the ozone monthly mean vertical profiles are clearly connected to the regional flow regime determined by seasonal dynamic forcing. The mean ozone profile over the coast of Gulf of Guinea in the burning season is characterized by systematically high ozone below 650hPa ; these are due to the transport by the Harmattan and the AEJ of the pollutants originating from upwind fires. The confinement of high ozone to the lower troposphere is due to the high stability of the Harmattan and the blocking Saharan anticyclone which prevents efficient vertical mixing. In contrast, ozone enhancements observed over Central Africa during the local dry season (June-August) are not only found in the lower troposphere but throughout the troposphere. Moreover, this study highlights a connection between the regions of the coast of Gulf of Guinea and regions of Congo to the south that appears on a semi annual basis. Vertical profiles in wet-season regions exhibit ozone enhancements in the lower troposphere due to biomass burning products transport from fires situated in the opposite dry-season hemisphere.


2014 ◽  
Vol 110 (5/6) ◽  
pp. 1-12 ◽  
Author(s):  
Lauri Laakso ◽  
Ditte Mogensen ◽  
Ville Vakkari ◽  
Johan P. Beukes ◽  
Pieter G. van Zyl ◽  
...  

2005 ◽  
Vol 5 (4) ◽  
pp. 4373-4406 ◽  
Author(s):  
D. Chand ◽  
P. Guyon ◽  
P. Artaxo ◽  
O. Schmid ◽  
G. P. Frank ◽  
...  

Abstract. As part of the Large Scale Biosphere-Atmosphere Experiment in Amazonia – Smoke, Aerosols, Clouds, Rainfall and Climate (LBA-SMOCC) campaign, detailed surface and airborne aerosol measurements were performed over the Amazon Basin during the dry to wet season from 16 September to 14 November 2002. Optical and physical properties of aerosols at the surface, boundary layer (BL) and free troposphere (FT) during the dry season are discussed in this article. Carbon monoxide (CO) is used as a tracer for biomass burning emissions. At the surface, good correlation among the light scattering coefficient (σs at 550 nm), PM2.5, and CO indicates that biomass burning is the main source of aerosols. Accumulation of haze during some of the large-scale biomass burning events led to high mass loadings (PM2.5=200 µgm−3), σs (1400 Mm−1), aerosol optical depth at 500 nm (3.0), and CO (3000 ppb). A few rainy episodes reduced the aerosol mass loading, number concentration (CN) and CO concentration by two orders of magnitude. The correlation analysis between σs and aerosol optical thickness shows that most of the optically active aerosols are confined to a layer with a scale height of 1660 m during the burning season. The average mass scattering and absorption efficiencies (532 nm) for small particles (diameter Dp<1.5 µm) at surface level are found to be 5.3 and 0.42 m2 g−1, respectively, when relating the aerosol optical properties to PM2.5 aerosols. The observed mean single scattering albedo (ωo at ~540 nm) for submicron aerosols at the surface (0.92±0.02) is significantly higher than reported previously. The scattering efficiency (dσs/dCN) of particles increases 2–10 times from the surface to the FT, most probably due to the combined affects of coagulation and condensation.


1990 ◽  
Vol 17 (6) ◽  
pp. 573 ◽  
Author(s):  
SR Morton ◽  
KG Brennan ◽  
MD Armstrong

Aerial surveys between 1981 and 1984 were used to identify monthly trends in the abundance of wandering whistling-duck Dendrocygna arcuata, plumed whistling-duck D. eytoni, radjah shelduck Tadorna radjah, Pacific black duck Anas superciliosa, and grey teal A. gibberifrons on five floodplains of the Alligator Rivers region, 250 km east of Darwin in the monsoonal north of the Northern Territory. Ground surveys were conducted during the same period on one of the floodplains, the Magela plain, to provide more detailed information. The Magela floodplain was inhabited by few ducks during the wet season (November to March), but numbers then increased to dramatic peaks in the late dry season. The Nourlangie floodplain and Boggy Plain (a large backswamp of the South Alligator floodplain) showed similar patterns, but the numbers of ducks were usually fewer. Ducks were uncommon on the shallower East Alligator and Cooper floodplains except for relatively brief periods in the wet season. The ground surveys suggested that ducks sought out the persistent swamps that characterise the Magela floodplain in the dry season. Ground surveys also indicated that aerial surveys underestimated densities; on the basis of correction factors calculated from the ground surveys, peak numbers on the five floodplains were roughly estimated to be 400 000 wandering whistling-ducks, 70 000 plumed whistling-ducks, 20 000 radjah shelducks, 50 000 Pacific black ducks, and 50 000 grey teal. Pink-eared ducks Malacorhynchus membranaceus and hardhead Aythya australis were recorded sporadically in low numbers. The Alligator Rivers region acted as a dry season refuge for large concentrations of ducks because of the atypical persistence of freshwaters on the Magela and Nourlangie floodplains and some of the backswamps of the South Alligator, such as Boggy Plain. The large aggregations appear to be unique in Australia.


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