| 11. |
- Ahlm, Lars, 1976-, et al.
(författare)
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A comparison of dry and wet season aerosol number fluxes over the Amazon rain forest
- 2010
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 10:6, s. 3063-3079
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Tidskriftsartikel (refereegranskat)abstract
- Vertical number fluxes of aerosol particles and vertical fluxes of CO2 were measured with the eddy covariance method at the top of a 53m high tower in the Amazon rain forest as part of the LBA (The Large Scale Biosphere Atmosphere Experiment in Amazonia) experiment. The observed aerosol number fluxes included particles with sizes down to 10 nm in diameter. The measurements were carried out during the wet and dry season in 2008. In this study focus is on the dry season aerosol fluxes, with significant influence from biomass burning, and these are compared with aerosol fluxes measured during the wet season. Net particle deposition fluxes dominated in daytime in both seasons and the deposition flux was considerably larger in the dry season due to the much higher dry season particle concentration. The particle transfer velocity increased linearly with increasing friction velocity in both seasons. The difference in transfer velocity between the two seasons was small, indicating that the seasonal change in aerosol number size distribution is not enough for causing any significant change in deposition velocity. In general, particle transfer velocities in this study are low compared to studies over boreal forests. The reasons are probably the high percentage of accumulation mode particles and the low percentage of nucleation mode particles in the Amazon boundary layer, both in the dry and wet season, and low wind speeds in the tropics compared to the midlatitudes. In the dry season, nocturnal particle fluxes behaved very similar to the nocturnal CO2 fluxes. Throughout the night, the measured particle flux at the top of the tower was close to zero, but early in the morning there was an upward particle flux peak that is not likely a result of entrainment or local pollution. It is possible that these morning upward particle fluxes are associated with emission of primary biogenic particles from the rain forest. Emitted particles may be stored within the canopy during stable conditions at nighttime, similarly to CO2, and being released from the canopy when conditions become more turbulent in the morning.
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| 12. |
- Ahlm, Lars, 1976-, et al.
(författare)
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Aerosol number fluxes over the Amazon rain forest during the wet season
- 2009
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Ingår i: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 9:24, s. 9381-9400
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Tidskriftsartikel (refereegranskat)abstract
- Number fluxes of particles with diameter larger than 10 nm were measured with the eddy covariance method over the Amazon rain forest during the wet season as part of the LBA (The Large Scale Biosphere Atmosphere Experiment in Amazonia) campaign 2008. The primary goal was to investigate whether sources or sinks dominate the aerosol number flux in the tropical rain forest-atmosphere system. During the measurement campaign, from 12 March to 18 May, 60% of the particle fluxes pointed downward, which is a similar fraction to what has been observed over boreal forests. The net deposition flux prevailed even in the absolute cleanest atmospheric conditions during the campaign and therefore cannot be explained only by deposition of anthropogenic particles. The particle transfer velocity vt increased with increasing friction velocity and the relation is described by the equation vt=2.4×10−3×u* where u* is the friction velocity. Upward particle fluxes often appeared in the morning hours and seem to a large extent to be an effect of entrainment fluxes into a growing mixed layer rather than primary aerosol emission. In general, the number source of primary aerosol particles within the footprint area of the measurements was small, possibly because the measured particle number fluxes reflect mostly particles less than approximately 200 nm. This is an indication that the contribution of primary biogenic aerosol particles to the aerosol population in the Amazon boundary layer may be low in terms of number concentrations. However, the possibility of horizontal variations in primary aerosol emission over the Amazon rain forest cannot be ruled out.
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| 13. |
- Ahlm, Lars, et al.
(författare)
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Emission and dry deposition of accumulation mode particles in the Amazon Basin
- 2010
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 10:21, s. 10237-10253
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Tidskriftsartikel (refereegranskat)abstract
- Size-resolved vertical aerosol number fluxes of particles in the diameter range 0.25–2.5 μm were measured with the eddy covariance method from a 53 m high tower over the Amazon rain forest, 60 km NNW of Manaus, Brazil. This study focuses on data measured during the relatively clean wet season, but a shorter measurement period from the more polluted dry season is used as a comparison. Size-resolved net particle fluxes of the five lowest size bins, representing 0.25–0.45 μm in diameter, pointed downward in more or less all wind sectors in the wet season. This is an indication that the source of primary biogenic aerosol particles may be small in this particle size range. In the diameter range 0.5–2.5 μm, vertical particle fluxes were highly dependent on wind direction. In wind sectors where anthropogenic influence was low, net emission fluxes dominated. However, in wind sectors associated with higher anthropogenic influence, net deposition fluxes dominated. The net emission fluxes were interpreted as primary biogenic aerosol emission, but deposition of anthropogenic particles seems to have masked this emission in wind sectors with higher anthropogenic influence. The emission fluxes were at maximum in the afternoon when the mixed layer is well developed, and these emissions were best correlated with horizontal wind speed by the equation log10F=0.47·U+2.26 where F is the emission number flux of 0.5–2.5 μm particles [m−2s−1] and U is the horizontal wind speed [ms−1] at the top of the tower.
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| 14. |
- Ahlm, Lars, et al.
(författare)
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Marine cloud brightening - as effective without clouds
- 2017
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:21, s. 13071-13087
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Tidskriftsartikel (refereegranskat)abstract
- Marine cloud brightening through sea spray injection has been proposed as a climate engineering method for avoiding the most severe consequences of global warming. A limitation of most of the previous modelling studies on marine cloud brightening is that they have either considered individual models or only investigated the effects of a specific increase in the number of cloud droplets. Here we present results from coordinated simulations with three Earth system models (ESMs) participating in the Geoengineering Model Intercomparison Project (GeoMIP) G4sea-salt experiment. Injection rates of accumulation-mode sea spray aerosol particles over ocean between 30 degrees N and 30 degrees S are set in each model to generate a global-mean effective radiative forcing (ERF) of -2.0 W m(-2) at the top of the atmosphere. We find that the injection increases the cloud droplet number concentration in lower layers, reduces the cloud-top effective droplet radius, and increases the cloud optical depth over the injection area. We also find, however, that the global-mean clear-sky ERF by the injected particles is as large as the corresponding total ERF in all three ESMs, indicating a large potential of the aerosol direct effect in regions of low cloudiness. The largest enhancement in ERF due to the presence of clouds occur as expected in the subtropical stratocumulus regions off the west coasts of the American and African continents. However, outside these regions, the ERF is in general equally large in cloudy and clear-sky conditions. These findings suggest a more important role of the aerosol direct effect in sea spray climate engineering than previously thought.
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| 15. |
- Alastuey, Andres, et al.
(författare)
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Geochemistry of PM10 over Europe during the EMEP intensive measurement periods in summer 2012 and winter 2013
- 2016
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:10, s. 6107-6129
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Tidskriftsartikel (refereegranskat)abstract
- The third intensive measurement period (IMP) organised by the European Monitoring and Evaluation Programme (EMEP) under the UNECE CLTRAP took place in summer 2012 and winter 2013, with PM10 filter samples concurrently collected at 20 (16 EMEP) regional background sites across Europe for subsequent analysis of their mineral dust content. All samples were analysed by the same or a comparable methodology. Higher PM10 mineral dust loadings were observed at most sites in summer (0.5-10aEuro-A mu gaEuro-m(-3)) compared to winter (0.2-2aEuro-A mu gaEuro-m(-3)), with the most elevated concentrations in the southern- and easternmost countries, accounting for 20-40aEuro-% of PM10. Saharan dust outbreaks were responsible for the high summer dust loadings at western and central European sites, whereas regional or local sources explained the elevated concentrations observed at eastern sites. The eastern Mediterranean sites experienced elevated levels due to African dust outbreaks during both summer and winter. The mineral dust composition varied more in winter than in summer, with a higher relative contribution of anthropogenic dust during the former period. A relatively high contribution of K from non-mineral and non-sea-salt sources, such as biomass burning, was evident in winter at some of the central and eastern European sites. The spatial distribution of some components and metals reveals the influence of specific anthropogenic sources on a regional scale: shipping emissions (V, Ni, and SO42-) in the Mediterranean region, metallurgy (Cr, Ni, and Mn) in central and eastern Europe, high temperature processes (As, Pb, and SO42-) in eastern countries, and traffic (Cu) at sites affected by emissions from nearby cities.
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| 16. |
- Aliaga, Diego, et al.
(författare)
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Identifying source regions of air masses sampled at the tropical high-altitude site of Chacaltaya using WRF-FLEXPART and cluster analysis
- 2021
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:21, s. 16453-16477
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Tidskriftsartikel (refereegranskat)abstract
- Observations of aerosol and trace gases in the remote troposphere are vital to quantify background concentrations and identify long-term trends in atmospheric composition on large spatial scales. Measurements made at high altitude are often used to study free-tropospheric air; however such high-altitude sites can be influenced by boundary layer air masses. Thus, accurate information on air mass origin and transport pathways to high-altitude sites is required. Here we present a new method, based on the source-receptor relationship (SRR) obtained from backwards WRF-FLEXPART simulations and a k-means clustering approach, to identify source regions of air masses arriving at measurement sites. Our method is tailored to areas of complex terrain and to stations influenced by both local and long-range sources. We have applied this method to the Chacaltaya (CHC) GAW station (5240 m a.s.l.; 16.35 degrees S, 68.13 degrees W) for the 6-month duration of the Southern Hemisphere high-altitude experiment on particle nucleation and growth (SALILNA) to identify where sampled air masses originate and to quantify the influence of the surface and the free troposphere. A key aspect of our method is that it is probabilistic, and for each observation time, more than one air mass (cluster) can influence the station, and the percentage influence of each air mass can be quantified. This is in contrast to binary methods, which label each observation time as influenced by either boundary layer or free-troposphere air masses. Air sampled at CHC is a mix of different provenance. We find that on average 9 % of the air, at any given observation time, has been in contact with the surface within 4 d prior to arriving at CHC. Furthermore, 24 % of the air has been located within the first 1.5 km above ground level (surface included). Consequently, 76 % of the air sampled at CHC originates from the free troposphere. However, pure free-tropospheric influences are rare, and often samples are concurrently influenced by both boundary layer and free-tropospheric air masses. A clear diurnal cycle is present, with very few air masses that have been in contact with the surface being detected at night. The 6-month analysis also shows that the most dominant air mass (cluster) originates in the Amazon and is responsible for 29 % of the sampled air. Furthermore, short-range clusters (origins within 100 km of CHC) have high temporal frequency modulated by local meteorology driven by the diurnal cycle, whereas the mid- and long-range clusters' (> 200 km) variability occurs on timescales governed by synoptic-scale dynamics. To verify the reliability of our method, in situ sulfate observations from CHC are combined with the SRR clusters to correctly identify the (pre-known) source of the sulfate: the Sabancaya volcano located 400 km north-west from the station.
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| 17. |
- Allen, G., et al.
(författare)
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South East Pacific atmospheric composition and variability sampled = ong 20 degrees S during VOCALS-REx
- 2011
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:11, s. 5237-5262
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Tidskriftsartikel (refereegranskat)abstract
- The VAMOS Ocean-Cloud-Atmosphere-Land Regional Experiment (VOCALS-REx) was conducted from 15 October to 15 November 2008 in the South East Pacific (SEP) region to investigate interactions between land, sea and atmosphere in this unique tropical eastern ocean environment and to improve the skill of global and regional models in = presenting the region. This study synthesises selected aircraft, ship = d surface site observations from VOCALS-REx to statistically summarise = d characterise the atmospheric composition and variability of the = rine Boundary Layer (MBL) and Free Troposphere (FT) along the 20 = grees S parallel between 70 degrees W and 85 degrees W. Significant = nal gradients in mean MBL sub-micron aerosol particle size and = mposition, carbon monoxide, sulphur dioxide and ozone were seen over = e campaign, with a generally more variable and polluted coastal = vironment and a less variable, more pristine remote maritime regime. = adients in aerosol and trace gas concentrations were observed to be = sociated with strong gradients in cloud droplet number. The FT was = ten more polluted in terms of trace gases than the MBL in the mean; = wever increased variability in the FT composition suggests an episodic = ture to elevated concentrations. This is consistent with a complex = rtical interleaving of airmasses with diverse sources and hence = llutant concentrations as seen by generalised back trajectory = alysis, which suggests contributions from both local and long-range = urces. Furthermore, back trajectory analysis demonstrates that the = served zonal gradients both in the boundary layer and the free = oposphere are characteristic of marked changes in airmass history with = stance offshore - coastal boundary layer airmasses having been in = cent contact with the local land surface and remote maritime airmasses = ving resided over ocean for in excess of ten days. Boundary layer = mposition to the east of 75 degrees W was observed to be dominated by = astal emissions from sources to the west of the Andes, with evidence = r diurnal pumping of the Andean boundary layer above the height of the = rine capping inversion. Analysis of intra-campaign variability in = mospheric composition was not found to be significantly correlated = th observed low-frequency variability in the large scale flow pattern; = mpaign-average interquartile ranges of CO, SO(2) and O(3) = ncentrations at all longitudes were observed to dominate over much = aller differences in median concentrations calculated between periods = different flow regimes. The campaign climatology presented here aims = provide a valuable dataset to inform model simulation and future = ocess studies, particularly in the context of aerosol-cloud = teraction and further evaluation of dynamical processes in the SEP = gion for conditions analogous to those during VOCALS-REx. To this end, = r results are discussed in terms of coastal, transitional and remote = atial regimes in the MBL and FT and a gridded dataset are provided as = resource.
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| 18. |
- Andersson, August, et al.
(författare)
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Seasonal source variability of carbonaceous aerosols at the Rwanda Climate Observatory
- 2020
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:8, s. 4561-4573
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Tidskriftsartikel (refereegranskat)abstract
- Sub-Saharan Africa (SSA) is a global hot spot for aerosol emissions, which affect the regional climate and air quality. In this paper, we use ground-based observations to address the large uncertainties in the source-resolved emission estimation of carbonaceous aerosols. Ambient fine fraction aerosol was collected on filters at the high-altitude (2590 m a.s.1.) Rwanda Climate Observatory (RCO), a SSA background site, during the dry and wet seasons in 2014 and 2015. The concentrations of both the carbonaceous and inorganic ion components show a strong seasonal cycle, with highly elevated concentrations during the dry season. Source marker ratios, including carbon isotopes, show that the wet and dry seasons have distinct aerosol compositions. The dry season is characterized by elevated amounts of biomass burning products, which approach similar to 95 % for carbonaceous aerosols. An isotopic mass-balance estimate shows that the amount of the carbonaceous aerosol stemming from savanna fires may increase from 0.2 mu g m(-3) in the wet season up to 10 mu g m(-3) during the dry season. Based on these results, we quantitatively show that savanna fire is the key modulator of the seasonal aerosol composition variability at the RCO.
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| 19. |
- Angelbratt, Jon, 1981, et al.
(författare)
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A new method to detect long term trends of methane (CH4) and nitrous oxide (N2O) total columns measured within the NDACC ground-based high resolution solar FTIR network
- 2011
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:13, s. 6167-6183
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Tidskriftsartikel (refereegranskat)abstract
- Total columns measured with the ground-based solar FTIR technique are highly variable in time due to atmospheric chemistry and dynamics in the atmosphere above the measurement station. In this paper, a multiple regression model with anomalies of air pressure, total columns of hydrogen fluoride (HF) and carbon monoxide (CO) and tropopause height are used to reduce the variability in the methane (CH(4)) and nitrous oxide (N(2)O) total columns to estimate reliable linear trends with as small uncertainties as possible. The method is developed at the Harestua station (60 degrees N, 11 degrees E, 600 ma.s.l.) and used on three other European FTIR stations, i.e. Jungfraujoch (47 degrees N, 8 degrees E, 3600 ma.s.l.), Zugspitze (47 degrees N, 11 degrees E, 3000 ma.s.l.), and Kiruna (68 degrees N, 20 degrees E, 400 ma.s.l.). Linear CH(4) trends between 0.13 +/- 0.01-0.25 +/- 0.02% yr(-1) were estimated for all stations in the 1996-2009 period. A piecewise model with three separate linear trends, connected at change points, was used to estimate the short term fluctuations in the CH(4) total columns. This model shows a growth in 1996-1999 followed by a period of steady state until 2007. From 2007 until 2009 the atmospheric CH(4) amount increases between 0.57 +/- 0.22-1.15 +/- 0.17% yr(-1). Linear N(2)O trends between 0.19 +/- 0.01-0.40 +/- 0.02% yr(-1) were estimated for all stations in the 1996-2007 period, here with the strongest trend at Harestua and Kiruna and the lowest at the Alp stations. From the N(2)O total columns crude tropospheric and stratospheric partial columns were derived, indicating that the observed difference in the N(2)O trends between the FTIR sites is of stratospheric origin. This agrees well with the N(2)O measurements by the SMR instrument onboard the Odin satellite showing the highest trends at Harestua, 0.98 +/- 0.28% yr(-1), and considerably smaller trends at lower latitudes, 0.27 +/- 0.25% yr(-1). The multiple regression model was compared with two other trend methods, the ordinary linear regression and a Bootstrap algorithm. The multiple regression model estimated CH(4) and N(2)O trends that differed up to 31% compared to the other two methods and had uncertainties that were up to 300% lower. Since the multiple regression method were carefully validated this stresses the importance to account for variability in the total columns when estimating trend from solar FTIR data.
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| 20. |
- Angelbratt, Jon, 1981, et al.
(författare)
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Carbon monoxide (CO) and ethane (C2H6) trends from ground-based solar FTIR measurements at six European stations, comparison and sensitivity analysis with the EMEP model
- 2011
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:17, s. 9253-9269
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Tidskriftsartikel (refereegranskat)abstract
- Trends in the CO and C(2)H(6) partial columns (similar to 0-15 km) have been estimated from four European ground-based solar FTIR (Fourier Transform InfraRed) stations for the 1996-2006 time period. The CO trends from the four stations Jungfraujoch, Zugspitze, Harestua and Kiruna have been estimated to -0.45 +/- 0.16%yr(-1), -1.00 +/- 0.24%yr(-1), -0.62 +/- 0.19%yr(-1) and -0.61 +/- 0.16%yr(-1), respectively. The corresponding trends for C(2)H(6) are -1.51 +/- 0.23%yr(-1), -2.11 +/- 0.30%yr(-1), -1.09 +/- 0.25%yr(-1) and -1.14 +/- 0.18%yr(-1). All trends are presented with their 2-sigma confidence intervals. To find possible reasons for the CO trends, the global-scale EMEP MSC-W chemical transport model has been used in a series of sensitivity scenarios. It is shown that the trends are consistent with the combination of a 20% decrease in the anthropogenic CO emissions seen in Europe and North America during the 1996-2006 period and a 20% increase in the anthropogenic CO emissions in East Asia, during the same time period. The possible impacts of CH(4) and biogenic volatile organic compounds (BVOCs) are also considered. The European and global-scale EMEP models have been evaluated against the measured CO and C(2)H(6) partial columns from Jungfraujoch, Zugspitze, Bremen, Harestua, Kiruna and Ny-Alesund. The European model reproduces, on average the measurements at the different sites fairly well and within 10-22% deviation for CO and 14-31% deviation for C(2)H(6). Their seasonal amplitude is captured within 6-35% and 9-124% for CO and C(2)H(6), respectively. However, 61-98% of the CO and C(2)H(6) partial columns in the European model are shown to arise from the boundary conditions, making the global-scale model a more suitable alternative when modeling these two species. In the evaluation of the global model the average partial columns for 2006 are shown to be within 1-9% and 37-50% of the measurements for CO and C(2)H(6), respectively. The global model sensitivity for assumptions made in this paper is also analyzed.
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