scholarly journals Multi-year statistical and modeling analysis of submicrometer aerosol number size distributions at a rain forest site in Amazonia

2018 ◽  
Vol 18 (14) ◽  
pp. 10255-10274 ◽  
Author(s):  
Luciana Varanda Rizzo ◽  
Pontus Roldin ◽  
Joel Brito ◽  
John Backman ◽  
Erik Swietlicki ◽  
...  

Abstract. The Amazon Basin is a unique region to study atmospheric aerosols, given their relevance for the regional hydrological cycle and the large uncertainty of their sources. Multi-year datasets are crucial when contrasting periods of natural conditions and periods influenced by anthropogenic emissions. In the wet season, biogenic sources and processes prevail, and the Amazonian atmospheric composition resembles preindustrial conditions. In the dry season, the basin is influenced by widespread biomass burning emissions. This work reports multi-year observations of high time resolution submicrometer (10–600 nm) particle number size distributions at a rain forest site in Amazonia (TT34 tower, 60 km NW from Manaus city), between 2008 and 2010 and 2012 and 2014. The median particle number concentration was 403 cm−3 in the wet season and 1254 cm−3 in the dry season. The Aitken mode (∼ 30–100 nm in diameter) was prominent during the wet season, while the accumulation mode (∼ 100–600 nm in diameter) dominated the particle size spectra during the dry season. Cluster analysis identified groups of aerosol number size distributions influenced by convective downdrafts, nucleation events and fresh biomass burning emissions. New particle formation and subsequent growth was rarely observed during the 749 days of observations, similar to previous observations in the Amazon Basin. A stationary 1-D column model (ADCHEM – Aerosol Dynamics, gas and particle phase CHEMistry and radiative transfer model) was used to assess the importance of the processes behind the observed diurnal particle size distribution trends. Three major particle source types are required in the model to reproduce the observations: (i) a surface source of particles in the evening, possibly related to primary biological emissions; (ii) entrainment of accumulation mode aerosols in the morning; and (iii) convective downdrafts transporting Aitken mode particles into the boundary layer mostly during the afternoon. The latter process has the largest influence on the modeled particle number size distributions. However, convective downdrafts are often associated with rain and, thus, act as both a source of Aitken mode particles and a sink of accumulation mode particles, causing a net reduction in the median total particle number concentrations in the surface layer. Our study shows that the combination of the three mentioned particle sources is essential to sustain particle number concentrations in Amazonia.

2018 ◽  
Author(s):  
Luciana Varanda Rizzo ◽  
Pontus Roldin ◽  
Joel Brito ◽  
John Backman ◽  
Erik Swietlicki ◽  
...  

Abstract. The Amazon Basin is a unique region to study atmospheric aerosols, given their relevance for the regional hydrological cycle and large uncertainty of their sources. Multi-year datasets are crucial when contrasting periods of natural conditions and periods influenced by anthropogenic emissions. In the wet season, biogenic sources and processes prevail, and the Amazonian atmospheric composition resembles pre-industrial conditions. In the dry season, the Basin is influenced by widespread biomass burning emissions. This work reports multi-year observations of high time resolution submicrometer (10–600 nm) particle number size distributions at a rain forest site in Amazonia (TT34 tower, 60 km NW from Manaus city), between years 2008–2010 and 2012–2014. Median particle number concentration was 403 cm−3 in the wet season and 1254 cm−3 in the dry season. The Aitken mode (~ 30–100 nm in diameter) was prominent during the wet season, while accumulation mode (~ 100–600 nm in diameter) dominated the particle size spectra during the dry season. Cluster analysis identified groups of aerosol number size distribution influenced by convective downdrafts, nucleation events and fresh biomass burning emissions. New particle formation and subsequent growth was rarely observed during the 749 days of observations, similar to previous observations in the Amazon Basin. A stationary 1D column model (ADCHEM – Aerosol Dynamics, gas and particle phase CHEMistry and radiative transfer model) was used to assess importance of processes behind the observed diurnal particle size distribution trends. Three major particle source types are required in the model to reproduce the observations: (i) a surface source of particles in the evening, possibly related to primary biological emissions (ii) entrainment of accumulation mode aerosols in the morning, and (iii) convective downdrafts transporting Aitken mode particles into the boundary layer mostly during the afternoon. The latter process has the largest influence on the modelled particle number size distributions. However, convective downdrafts are often associated with rain and thus act both as a source of Aitken mode particles, and as a sink of accumulation mode particles, causing a net reduction in the median total particle number concentrations in the surface layer. Our study shows that the combination of the three mentioned particle sources are essential to sustain particle number concentrations in Amazonia.


2019 ◽  
Vol 19 (23) ◽  
pp. 14849-14873 ◽  
Author(s):  
Peter Tunved ◽  
Johan Ström

Abstract. Size-resolved aerosol trends were investigated based on a 17-year data set (2000–2017) from the rural background site Aspvreten located in southern Sweden (58.8∘ N, 17.4∘ E). Cluster analysis of the size distributions was performed to aid in the interpretation of the data. The results confirm previous findings of decreasing aerosol mass and number during the last decades as a result of reduced anthropogenic emissions in Europe. We show that both particle modal number concentration and size have substantially been reduced during the last 17 years. Negative trends in particle number concentration of about 10 cm−3 yr−1 are present for nuclei, Aitken, and accumulation modes. In total, integral particle number concentration has decreased by 30 %, from 1860 to ca. 1300 cm−3. The reduction in modal number concentration is accompanied by a decrease in modal size, and this decrease is largest for the accumulation mode (2 nm yr−1 or about 17 % for the whole period). These reductions have resulted in a decrease in submicron particle mass (< 390 nm) by more than 50 % over the period 2000–2017. These decreases are similar to observations found at other stations in northern Europe. Although all size classes show a downward trend as annual averages, we also show that observed trends are not evenly distributed over the year and that a rather complex picture emerges where both sign and magnitude of trends vary with season and size. The strongest negative trends are present during spring (accumulation mode) and autumn (Aitken mode). The strongest positive trends are present during summer months (Aitken mode). The combined trajectory and data analyses do not present evidence for an increase in new particle formation formed locally, although some evidence of increased new particle formation some distance away from the receptor is present. Observed aerosol size distribution data, together with an adiabatic cloud parcel model, were further used to estimate the change in cloud droplet concentration for various assumptions of updraught velocities and aerosol chemical composition. The results indicate a substantial increase in the atmospheric brightening effect due to a reduction in cloud reflectivity corresponding to 10 %–12 % reduction in cloud albedo over the period 2000–2017.


2005 ◽  
Vol 21 (4) ◽  
pp. 451-460 ◽  
Author(s):  
Eduardo Jacusiel Miranda ◽  
George L. Vourlitis ◽  
Nicolau Priante Filho ◽  
Pedro Correto Priante ◽  
José Holanda Campelo ◽  
...  

The photosynthetic light response of Amazonian semi-deciduous forest trees of the rain forest–savanna transition near Sinop Mato Grosso, Brazil was measured between July 2000 and September 2003 to test the hypothesis that the photosynthetic capacity of trees acclimated to different growth light environments will decline during the dry season. Maximum photosynthesis (Amax) and stomatal conductance (gmax) were significantly higher during the wet season; however, the physiological response to drought was not a clear function of growth light environment. For some species, such as Psychotria sp. growing in the mid-canopy, internal leaf CO2 concentration (Ci) was >30% lower during the dry season suggesting that declines in Amax were caused in part by stomatal limitations to CO2 diffusion. For other species, such as Brosimum lactescens growing at the top of the canopy, Tovomita schomburgkii growing in the mid-canopy, and Dinizia excelsa growing in the understorey, dry season Ci declined by <20% suggesting that factors independent of CO2 diffusion were more important in limiting Amax. Dry-season declines in gmax appeared to be important for maintaining a more consistent leaf water potential for some species (T. schomburgkii and D. excelsa) but not others (Psychotria sp.). These results indicate that while seasonal drought exerts an important limitation on the physiological capacity of semi-deciduous Amazonian forest trees, the mechanism of this limitation may differ between species.


2011 ◽  
Vol 11 (17) ◽  
pp. 8899-8912 ◽  
Author(s):  
L. V. Rizzo ◽  
A. L. Correia ◽  
P. Artaxo ◽  
A. S. Procópio ◽  
M. O. Andreae

Abstract. In this study, we examine the spectral dependence of aerosol absorption at different sites and seasons in the Amazon Basin. The analysis is based on measurements performed during three intensive field experiments at a pasture site (Fazenda Nossa Senhora, Rondônia) and at a primary forest site (Cuieiras Reserve, Amazonas), from 1999 to 2004. Aerosol absorption spectra were measured using two Aethalometers: a 7-wavelength Aethalometer (AE30) that covers the visible (VIS) to near-infrared (NIR) spectral range, and a 2-wavelength Aethalometer (AE20) that measures absorption in the UV and in the NIR. As a consequence of biomass burning emissions, about 10 times greater absorption values were observed in the dry season in comparison to the wet season. Power law expressions were fitted to the measurements in order to derive the absorption Ångström exponent, defined as the negative slope of absorption versus wavelength in a log-log plot. At the pasture site, about 70 % of the absorption Ångström exponents fell between 1.5 and 2.5 during the dry season, indicating that biomass burning aerosols have a stronger spectral dependence than soot carbon particles. Ångström exponents decreased from the dry to the wet season, in agreement with the shift from biomass burning aerosols, predominant in the fine mode, to biogenic and dust aerosols, predominant in the coarse mode. The lowest absorption Ångström exponents (90 % of data below 1.5) were observed at the forest site during the dry season. Also, results indicate that low absorption coefficients were associated with low Ångström exponents. This finding suggests that biogenic aerosols from Amazonia have a weaker spectral dependence for absorption than biomass burning aerosols, contradicting our expectations of biogenic particles behaving as brown carbon. In a first order assessment, results indicate a small (<1 %) effect of variations in absorption Ångström exponents on 24-h aerosol forcings, at least in the spectral range of 450–880 nm. Further studies should be taken to assess the corresponding impact in the UV spectral range. The assumption that soot spectral properties represent all ambient light absorbing particles may cause a misjudgment of absorption towards the UV, especially in remote areas. Therefore, it is recommended to measure aerosol absorption at several wavelengths to accurately assess the impact of non-soot aerosols on climate and on photochemical atmospheric processes.


2006 ◽  
Vol 6 (2) ◽  
pp. 471-491 ◽  
Author(s):  
J. Rissler ◽  
A. Vestin ◽  
E. Swietlicki ◽  
G. Fisch ◽  
J. Zhou ◽  
...  

Abstract. Aerosol particle number size distributions and hygroscopic properties were measured at a pasture site in the southwestern Amazon region (Rondonia). The measurements were performed 11 September-14 November 2002 as part of LBA-SMOCC (Large scale Biosphere atmosphere experiment in Amazonia - SMOke aerosols, Clouds, rainfall and Climate), and cover the later part of the dry season (with heavy biomass burning), a transition period, and the onset of the wet period. Particle number size distributions were measured with a DMPS (Differential Mobility Particle Sizer, 3-850nm) and an APS (Aerodynamic Particle Sizer), extending the distributions up to 3.3 µm in diameter. An H-TDMA (Hygroscopic Tandem Differential Mobility Analyzer) measured the hygroscopic diameter growth factors (Gf) at 90% relative humidity (RH), for particles with dry diameters (dp) between 20-440 nm, and at several occasions RH scans (30-90% RH) were performed for 165nm particles. These data provide the most extensive characterization of Amazonian biomass burning aerosol, with respect to particle number size distributions and hygroscopic properties, presented until now. The evolution of the convective boundary layer over the course of the day causes a distinct diel variation in the aerosol physical properties, which was used to get information about the properties of the aerosol at higher altitudes. The number size distributions averaged over the three defined time periods showed three modes; a nucleation mode with geometrical median diameters (GMD) of ~12 nm, an Aitken mode (GMD=61-92 nm) and an accumulation mode (GMD=128-190 nm). The two larger modes were shifted towards larger GMD with increasing influence from biomass burning. The hygroscopic growth at 90% RH revealed a somewhat external mixture with two groups of particles; here denoted nearly hydrophobic (Gf~1.09 for 100 nm particles) and moderately hygroscopic (Gf~1.26). While the hygroscopic growth factors were surprisingly similar over the periods, the number fraction of particles belonging to each hygroscopic group varied more, with the dry period aerosol being more dominated by nearly hydrophobic particles. As a result the total particle water uptake rose going into the cleaner period. The fraction of moderately hygroscopic particles was consistently larger for particles in the accumulation mode compared to the Aitken mode for all periods. Scanning the H-TDMA over RH (30-90% RH) showed no deliquescence behavior. A parameterization of both Gf(RH) and Gf(dp), is given.


2016 ◽  
Vol 16 (15) ◽  
pp. 9727-9743 ◽  
Author(s):  
James D. Whitehead ◽  
Eoghan Darbyshire ◽  
Joel Brito ◽  
Henrique M. J. Barbosa ◽  
Ian Crawford ◽  
...  

Abstract. The Amazon basin is a vast continental area in which atmospheric composition is relatively unaffected by anthropogenic aerosol particles. Understanding the properties of the natural biogenic aerosol particles over the Amazon rainforest is key to understanding their influence on regional and global climate. While there have been a number of studies during the wet season, and of biomass burning particles in the dry season, there has been relatively little work on the transition period – the start of the dry season in the absence of biomass burning. As part of the Brazil–UK Network for Investigation of Amazonian Atmospheric Composition and Impacts on Climate (BUNIAACIC) project, aerosol measurements, focussing on unpolluted biogenic air masses, were conducted at a remote rainforest site in the central Amazon during the transition from wet to dry season in July 2013. This period marks the start of the dry season but before significant biomass burning occurs in the region. Median particle number concentrations were 266 cm−3, with size distributions dominated by an accumulation mode of 130–150 nm. During periods of low particle counts, a smaller Aitken mode could also be seen around 80 nm. While the concentrations were similar in magnitude to those seen during the wet season, the size distributions suggest an enhancement in the accumulation mode compared to the wet season, but not yet to the extent seen later in the dry season, when significant biomass burning takes place. Submicron nonrefractory aerosol composition, as measured by an aerosol chemical speciation monitor (ACSM), was dominated by organic material (around 81 %). Aerosol hygroscopicity was probed using measurements from a hygroscopicity tandem differential mobility analyser (HTDMA), and a quasi-monodisperse cloud condensation nuclei counter (CCNc). The hygroscopicity parameter, κ, was found to be low, ranging from 0.12 for Aitken-mode particles to 0.18 for accumulation-mode particles. This was consistent with previous studies in the region, but lower than similar measurements conducted in Borneo, where κ ranged 0.17–0.37. A wide issue bioaerosol sensor (WIBS-3M) was deployed at ground level to probe the coarse mode, detecting primary biological aerosol by fluorescence (fluorescent biological aerosol particles, or FBAPs). The mean FBAP number concentration was 400 ± 242 L−1; however, this ranged from around 200 L−1 during the day to as much as 1200 L−1 at night. FBAPs dominated the coarse-mode particles, comprising between 55 and 75 % of particles during the day to more than 90 % at night. Non-FBAPs did not show a strong diurnal pattern. Comparison with previous FBAP measurements above canopy at the same location suggests there is a strong vertical gradient in FBAP concentrations through the canopy. Cluster analysis of the data suggests that FBAPs were dominated (around 70 %) by fungal spores. Further, long-term measurements will be required in order to fully examine the seasonal variability and distribution of primary biological aerosol particles through the canopy. This is the first time that such a suite of measurements has been deployed at this site to investigate the chemical composition and properties of the biogenic contributions to Amazonian aerosol during the transition period from the wet to the dry season, and thus provides a unique comparison to the aerosol properties observed during the wet season in previous similar campaigns. This was also the first deployment of a WIBS in the Amazon rainforest to study coarse-mode particles, particularly primary biological aerosol particles, which are likely to play an important role as ice nuclei in the region.


2003 ◽  
Vol 3 (5) ◽  
pp. 5139-5184 ◽  
Author(s):  
T. Hussein ◽  
A. Puustinen ◽  
P. P. Aalto ◽  
J. M. Mäkelä ◽  
K. Hämeri ◽  
...  

Abstract. Aerosol number size distributions were measured continuously in Helsinki, Finland from 5 May 1997 to 28 February 2003. The daily, monthly and annual patterns were investigated. The temporal variation of the particle number concentration was seen to follow the traffic density. The highest total particle number concentrations were usually observed during workdays; especially on Fridays, and the lower concentrations occurred during weekends; especially Sundays. Seasonally, the highest total number concentrations were usually observed during winter and spring and the lowest during June and July. More than 80\\% of the particle number size distributions were tri-modal: nucleation mode (Dp < 30 nm), Aitken mode (20–100 nm) and accumulation mode (Dp > 90 nm). Less than 20% of the particle number size distributions have either two modes or consisted of more than three modes. Two different measurement sites are used; in the first place (Siltavuori, 5 May 1997–5 March 2001), the overall means of the integrated particle number concentrations were 7100 cm−3, 6320 cm−3, and 960 cm−3, respectively, for nucleation, Aitken, and accumulation modes. In the second site (Kumpula, 6 March 2001–28 February 2003) they were 5670 cm−3, 4050 cm−3, and 900 cm−3. The total number concentration in nucleation and Aitken modes were usually significantly higher during weekdays than during weekends. The variations in accumulation mode were less pronounced. The smaller concentrations in Kumpula were mainly due to building construction and also slight overall decreasing trend during these years. During the site changing a period of simultaneous measurements over two weeks were performed showing nice correlation in both sites.


2011 ◽  
Vol 11 (7) ◽  
pp. 3319-3332 ◽  
Author(s):  
T. Schmeissner ◽  
R. Krejci ◽  
J. Ström ◽  
W. Birmili ◽  
A. Wiedensohler ◽  
...  

Abstract. The first long-term measurements of aerosol number and size distributions in South-American tropical free troposphere (FT) were performed from March 2007 until March 2009. The measurements took place at the high altitude Atmospheric Research Station Alexander von Humboldt. The station is located on top of the Sierra Nevada mountain ridge at 4765 m a.s.l. nearby the city of Mérida, Venezuela. Aerosol size distribution and number concentration data was obtained with a custom-built Differential Mobility Particle Sizer (DMPS) system and a Condensational Particle Counter (CPC). The analysis of the annual and diurnal variability of the tropical FT aerosol focused mainly on possible links to the atmospheric general circulation in the tropics. Considerable annual and diurnal cycles of the particle number concentration were observed. Highest total particle number concentrations were measured during the dry season (January–March, 519 ± 613 cm−3), lowest during the wet season (July–September, 318 ± 194 cm−3). The more humid FT (relative humidity (RH) range 50–95 %) contained generally higher aerosol particle number concentrations (573 ± 768 cm−3 during dry season, 320 ± 195 cm−3 during wet season) than the dry FT (RH < 50 %, 454 ± 332 cm−3 during dry season, 275 ± 172 cm−3 during wet season), indicating the importance of convection for aerosol distributions in the tropical FT. The diurnal cycle in the variability of the particle number concentration was mainly driven by local orography.


2011 ◽  
Vol 11 (4) ◽  
pp. 11547-11577 ◽  
Author(s):  
L. V. Rizzo ◽  
A. L. Correia ◽  
P. Artaxo ◽  
A. S. Procópio ◽  
M. O. Andreae

Abstract. In this study, we examine the spectral dependence of aerosol absorption at different sites and seasons in the Amazon Basin. The analysis is based on measurements performed during three intensive field experiments at a pasture site (Fazenda Nossa Senhora, Rondônia) and at a primary forest site (Cuieiras Reserve, Amazonas), from 1999 to 2004. Aerosol absorption spectra were measured using two Aethalometers: a 7-wavelength Aethalometer (AE30) that covers the visible (VIS) to near-infrared (NIR) spectral range, and a 2-wavelength Aethalometer (AE20) that measures absorption in the UV and in the visible. As a consequence of biomass burning emissions, about 10 times greater absorption values were observed in the dry season in comparison to the wet season. Power law expressions were fitted to the measurements in order to derive the Ångström exponent for absorption, defined as the negative slope of absorption vs. wavelength in a log-log plot. At the pasture site, about 70% of the Ångström exponents fell between 1.5 and 2.5 during the dry season, indicating that biomass burning aerosols have a stronger spectral dependence than soot carbon particles. Ångström exponents decreased from the dry to the wet season, in agreement with the shift from biomass burning aerosols, predominant in the fine mode, to biogenic and dust aerosols, predominant in the coarse mode. The lowest Ångström exponents (90% of data below 1.5) were observed at the forest site during the dry season. Also, results indicate that low absorption coefficients were associated with Ångström exponents below 1.0. This finding suggests that biogenic aerosols from Amazonia may have a weak spectral dependence for absorption, contradicting our expectations of biogenic particles behaving as brown carbon. Nevertheless, additional measurements should be taken in the future, to provide a complete picture of biogenic aerosol absorption spectral characteristics from different seasons and geographic locations. The assumption that soot spectral properties represent all ambient light absorbing particles may cause a misjudgment of absorption towards the UV, especially in remote areas. Therefore, it is recommended to measure aerosol absorption at several wavelengths from UV to near IR to accurately assess the impact of non-soot aerosols on climate and on photochemical atmospheric processes.


2017 ◽  
Author(s):  
Filippo Xausa ◽  
Pauli Paasonen ◽  
Risto Makkonen ◽  
Mikhail Arshinov ◽  
Aijun Ding ◽  
...  

Abstract. Climate models are important tools that are used for generating climate change projections, in which aerosol-climate interactions are one of the main sources of uncertainties. In order to quantify aerosol-radiation and aerosol-cloud interactions, detailed input of anthropogenic aerosol number emissions is necessary. However, the anthropogenic aerosol number emissions are usually converted from the corresponding mass emissions in precompiled emission inventories through a very simplistic method depending uniquely on chemical composition, particle size and density, which are defined for a few very wide main source sectors. In this work, the anthropogenic particle number emissions converted from the AeroCom mass in the ECHAM-HAM climate model were replaced with the recently-formulated number emissions from the Greenhouse Gas and Air Pollution Interactions and Synergies (GAINS)-model, where the emission number size distributions vary, for example, with respect to the fuel and technology. A special attention in our analysis was put on accumulation mode particles (particle diameter dp > 100 nm) because of (i) their capability of acting as cloud condensation nuclei (CCN), thus forming cloud droplets and affecting Earth's radiation budget, and (ii) their dominant role in forming the coagulation sink and thus limiting the concentration of sub-100 nanometers particles. In addition, the estimates of anthropogenic CCN formation, and thus the forcing from aerosol-climate interactions are expected to be affected. Analysis of global particle number concentrations and size distributions reveal that GAINS implementation increases CCN concentration compared with AeroCom, with regional enhancement factors reaching values as high as 10. A comparison between modeled and observed concentrations shows that the increase in number concentration for accumulation mode particle agrees well with measurements, but it leads to a consistent underestimation of both nucleation mode and Aitken mode (dp > 100 nm) particle number concentrations. This suggests that revisions are needed in the new particle formation and growth schemes currently applied in global modeling frameworks.


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