Sources and Transport of Black Carbon number size distribution at Zeppelin Observatory, Svalbard

Author(s):  
Roxana Cremer ◽  
Peter Tunved ◽  
Daniel Partridge ◽  
Johan Ström

<p>Black carbon (BC) particles originate from incomplete combustion of biomass and fossil fuels. They are known to contribute to the warming of Earth’s climate due to radiative effects and aerosol-cloud interactions. The lifetime of sub-micron BC in the troposphere is in the order of days-weeks. Through interaction with other airborne compounds, the hydrophobic nature of BC gradually becomes more hygroscopic and thus available as CCN.</p><p>An assessment of the large-scale impact on clouds and climate requires detailed insights about the lifecycle of BC in the atmosphere, understanding sources for BC, transport, transformation, and removal processes. All these processes are tightly linked to particle size, making knowledge regarding how BC distributes over a given size range substantial.</p><p>In a previous study we explored statistical methods to attribute BC mass according to particle size (in review). Combining these results with cluster analysis of long term record of aerosol number size distribution (NSD) observations from Zeppelin Observatory it was shown that the method produced reasonable results for a majority of observations. However, the cluster characteristic of NSD associated with high level of pollution presented additional challenges as the methodological approach gave an unrealistic average BC size distribution.</p><p>In the current study we focus on these inconsistencies; additional analytical methods are introduced to resolve source-receptor relationships, defining transport characteristics using extensive trajectory analysis. The analysis provides insights of the processes along the travel path to the receptor location and resolves key transport routes for the BC fraction to the Arctic.</p>

2008 ◽  
Vol 5 (2) ◽  
pp. 509-521 ◽  
Author(s):  
A. Engel ◽  
K. G. Schulz ◽  
U. Riebesell ◽  
R. Bellerby ◽  
B. Delille ◽  
...  

Abstract. The influence of seawater carbon dioxide (CO2) concentration on the size distribution of suspended particles (2–60 μm) and on phytoplankton abundance was investigated during a mesocosm experiment at the large scale facility (LFS) in Bergen, Norway, in the frame of the Pelagic Ecosystem CO2 Enrichment study (PeECE II). In nine outdoor enclosures the partial pressure of CO2 in seawater was modified by an aeration system to simulate past (~190 μatm CO2), present (~370 μatm CO2) and future (~700 μatm CO2) CO2 conditions in triplicates. Due to the initial addition of inorganic nutrients, phytoplankton blooms developed in all mesocosms and were monitored over a period of 19 days. Seawater samples were collected daily for analysing the abundance of suspended particles and phytoplankton with the Coulter Counter and with Flow Cytometry, respectively. During the bloom period, the abundance of small particles (<4 μm) significantly increased at past, and decreased at future CO2 levels. At that time, a direct relationship between the total-surface-to-total-volume ratio of suspended particles and DIC concentration was determined for all mesocosms. Significant changes with respect to the CO2 treatment were also observed in the phytoplankton community structure. While some populations such as diatoms seemed to be insensitive to the CO2 treatment, others like Micromonas spp. increased with CO2, or showed maximum abundance at present day CO2 (i.e. Emiliania huxleyi). The strongest response to CO2 was observed in the abundance of small autotrophic nano-plankton that strongly increased during the bloom in the past CO2 mesocosms. Together, changes in particle size distribution and phytoplankton community indicate a complex interplay between the ability of the cells to physiologically respond to changes in CO2 and size selection. Size of cells is of general importance for a variety of processes in marine systems such as diffusion-limited uptake of substrates, resource allocation, predator-prey interaction, and gravitational settling. The observed changes in particle size distribution are therefore discussed with respect to biogeochemical cycling and ecosystem functioning.


2016 ◽  
Vol 9 (1) ◽  
pp. 103-114 ◽  
Author(s):  
G. I. Gkatzelis ◽  
D. K. Papanastasiou ◽  
K. Florou ◽  
C. Kaltsonoudis ◽  
E. Louvaris ◽  
...  

Abstract. An experimental methodology was developed to measure the nonvolatile particle number concentration using a thermodenuder (TD). The TD was coupled with a high-resolution time-of-flight aerosol mass spectrometer, measuring the chemical composition and mass size distribution of the submicrometer aerosol and a scanning mobility particle sizer (SMPS) that provided the number size distribution of the aerosol in the range from 10 to 500 nm. The method was evaluated with a set of smog chamber experiments and achieved almost complete evaporation (> 98 %) of secondary organic as well as freshly nucleated particles, using a TD temperature of 400 °C and a centerline residence time of 15 s. This experimental approach was applied in a winter field campaign in Athens and provided a direct measurement of number concentration and size distribution for particles emitted from major pollution sources. During periods in which the contribution of biomass burning sources was dominant, more than 80 % of particle number concentration remained after passing through the thermodenuder, suggesting that nearly all biomass burning particles had a nonvolatile core. These remaining particles consisted mostly of black carbon (60 % mass contribution) and organic aerosol (OA; 40 %). Organics that had not evaporated through the TD were mostly biomass burning OA (BBOA) and oxygenated OA (OOA) as determined from AMS source apportionment analysis. For periods during which traffic contribution was dominant 50–60 % of the particles had a nonvolatile core while the rest evaporated at 400 °C. The remaining particle mass consisted mostly of black carbon with an 80 % contribution, while OA was responsible for another 15–20 %. Organics were mostly hydrocarbon-like OA (HOA) and OOA. These results suggest that even at 400 °C some fraction of the OA does not evaporate from particles emitted from common combustion processes, such as biomass burning and car engines, indicating that a fraction of this type of OA is of extremely low volatility.


2019 ◽  
Vol 19 (5) ◽  
pp. 2787-2812 ◽  
Author(s):  
Betty Croft ◽  
Randall V. Martin ◽  
W. Richard Leaitch ◽  
Julia Burkart ◽  
Rachel Y.-W. Chang ◽  
...  

Abstract. Summertime Arctic aerosol size distributions are strongly controlled by natural regional emissions. Within this context, we use a chemical transport model with size-resolved aerosol microphysics (GEOS-Chem-TOMAS) to interpret measurements of aerosol size distributions from the Canadian Arctic Archipelago during the summer of 2016, as part of the “NETwork on Climate and Aerosols: Addressing key uncertainties in Remote Canadian Environments” (NETCARE) project. Our simulations suggest that condensation of secondary organic aerosol (SOA) from precursor vapors emitted in the Arctic and near Arctic marine (ice-free seawater) regions plays a key role in particle growth events that shape the aerosol size distributions observed at Alert (82.5∘ N, 62.3∘ W), Eureka (80.1∘ N, 86.4∘ W), and along a NETCARE ship track within the Archipelago. We refer to this SOA as Arctic marine SOA (AMSOA) to reflect the Arctic marine-based and likely biogenic sources for the precursors of the condensing organic vapors. AMSOA from a simulated flux (500 µgm-2day-1, north of 50∘ N) of precursor vapors (with an assumed yield of unity) reduces the summertime particle size distribution model–observation mean fractional error 2- to 4-fold, relative to a simulation without this AMSOA. Particle growth due to the condensable organic vapor flux contributes strongly (30 %–50 %) to the simulated summertime-mean number of particles with diameters larger than 20 nm in the study region. This growth couples with ternary particle nucleation (sulfuric acid, ammonia, and water vapor) and biogenic sulfate condensation to account for more than 90 % of this simulated particle number, which represents a strong biogenic influence. The simulated fit to summertime size-distribution observations is further improved at Eureka and for the ship track by scaling up the nucleation rate by a factor of 100 to account for other particle precursors such as gas-phase iodine and/or amines and/or fragmenting primary particles that could be missing from our simulations. Additionally, the fits to the observed size distributions and total aerosol number concentrations for particles larger than 4 nm improve with the assumption that the AMSOA contains semi-volatile species: the model–observation mean fractional error is reduced 2- to 3-fold for the Alert and ship track size distributions. AMSOA accounts for about half of the simulated particle surface area and volume distributions in the summertime Canadian Arctic Archipelago, with climate-relevant simulated summertime pan-Arctic-mean top-of-the-atmosphere aerosol direct (−0.04 W m−2) and cloud-albedo indirect (−0.4 W m−2) radiative effects, which due to uncertainties are viewed as an order of magnitude estimate. Future work should focus on further understanding summertime Arctic sources of AMSOA.


2004 ◽  
Vol 4 (8) ◽  
pp. 2119-2143 ◽  
Author(s):  
J. Rissler ◽  
E. Swietlicki ◽  
J. Zhou ◽  
G. Roberts ◽  
M. O. Andreae ◽  
...  

Abstract. Sub-micrometer atmospheric aerosol particles were studied in the Amazon region, 125 km northeast of Manaus, Brazil (-1°55.2'S, 59°28.1'W). The measurements were performed during the wet-to-dry transition period, 4-28 July 2001 as part of the LBA (Large-Scale Biosphere Atmosphere Experiment in Amazonia) CLAIRE-2001 (Cooperative LBA Airborne Regional Experiment) experiment. The number size distribution was measured with two parallel differential mobility analyzers, the hygroscopic growth at 90% RH with a Hygroscopic Tandem Mobility Analyzer (H-TDMA) and the concentrations of cloud condensation nuclei (CCN) with a cloud condensation nuclei counter. A model was developed that uses the H-TDMA data to predict the number of soluble molecules or ions in the individual particles and the corresponding minimum particle diameter for activation into a cloud droplet at a certain supersaturation. Integrating the number size distribution above this diameter, CCN concentrations were predicted with a time resolution of 10 min and compared to the measured concentrations. During the study period, three different air masses were identified and compared: clean background, air influenced by aged biomass burning, and moderately polluted air from recent local biomass burning. For the clean period 2001, similar number size distributions and hygroscopic behavior were observed as during the wet season at the same site in 1998, with mostly internally mixed particles of low diameter growth factor (~1.3 taken from dry to 90% RH). During the periods influenced by biomass burning the hygroscopic growth changed slightly, but the largest difference was seen in the number size distribution. The CCN model was found to be successful in predicting the measured CCN concentrations, typically within 25%. A sensitivity study showed relatively small dependence on the assumption of which model salt that was used to predict CCN concentrations from H-TDMA data. One strength of using H-TDMA data to predict CCN concentrations is that the model can also take into account soluble organic compounds, insofar as they go into solution at 90% RH. Another advantage is the higher time resolution compared to using size-resolved chemical composition data.


2011 ◽  
Vol 8 (6) ◽  
pp. 11405-11452 ◽  
Author(s):  
A. Forest ◽  
L. Stemmann ◽  
M. Picheral ◽  
L. Burdorf ◽  
D. Robert ◽  
...  

Abstract. The size distribution and mean spatial trends of large particles (>100 μm, in equivalent spherical diameter, ESD) and mesozooplankton were investigated across the Mackenzie Shelf (Southeast Beaufort Sea, Arctic Ocean) in July–August 2009. Our main objective was to combine results from an Underwater Vision Profiler 5 (UVP5) and traditional net tows (200 μm mesh size) to characterize the structural diversity and functioning of the Arctic shelf-basin ecosystem and to assess the large-scale correspondence between the two methodological approaches. The core dataset comprised 154 UVP5 profiles and 29 net tows conducted in the shelf (<100 m isobath), slope (100–1000 m) and basin (>1000 m) regions of the study area. The mean abundance of total particles and zooplankton in the upper water column (<75 m depth) declined exponentially with increasing distance from shore. Vertical and latitudinal patterns in total particle concentration followed those of chlorophyll-a (chl-a) concentration, with maximum values between 30 and 70 m depth. Based on the size-spectra derived from the UVP5 dataset, living organisms (0.1–10 mm ESD) accounted for an increasingly large proportion of total particle abundance (from 0.1% to > 50 %) when progressing offshore and as the ESD of particles was increasing. Both the UVP5 and net tows determined that copepods dominated the zooplankton community (~78–94 % by numbers) and that appendicularians were generally the second most abundant group (~1–11 %). The vertical distribution patterns of copepods and appendicularians indicated a close association between primary production and the main grazers. Manual taxonomic counts and ZooScan image analyses shed further light on the size-structure and composition of the copepod community – which was dominated at ~95 % by a guild of 10 typical taxa. The size distributions of copepods, as evaluated with the 3 methods (manual counts, ZooScan and UVP5), showed consistent patterns co-varying in the same order of magnitude over the upper size range (>1 mm ESD). Copepods < 1 mm were not well quantified by the UVP5, which estimated that only ~13–25 % of the assemblage was composed of copepods < 1 mm ESD compared with ~77–89 % from the net tow estimates. However, the biovolume of copepods was overwhelmingly dominated (~93–97 %) by copepods >1 mm ESD. Our results illustrate that the combination of traditional sampling methods and automated imaging techniques is a powerful approach that enabled us to conclude on the prevalence of a relatively high productivity regime and dominant herbivorous food web over the shelf when compared with the low-productive recycling system detected offshore.


2018 ◽  
Author(s):  
Betty Croft ◽  
Randall V. Martin ◽  
W. Richard Leaitch ◽  
Julia Burkart ◽  
Rachel Y.-W. Chang ◽  
...  

Abstract. Summertime Arctic aerosol size distributions are strongly controlled by natural regional emissions. Within this context, we use a chemical transport model with size-resolved aerosol microphysics (GEOS-Chem-TOMAS) to interpret measurements of aerosol size distributions from the Canadian Arctic Archipelago during the summer of 2016, as part of the NETwork on Climate and Aerosols: addressing key uncertainties in Remote Canadian Environments (NETCARE). Our simulations suggest that condensation of secondary organic aerosol (SOA) from precursor vapors emitted in the Arctic and near Arctic marine (open ocean and coastal) regions plays a key role in particle growth events that shape the aerosol size distributions observed at Alert (82.5° N, 62.3° W), Eureka (80.1° N, 86.4° W), and along a NETCARE ship track within the Archipelago. We refer to this SOA as Arctic marine SOA (Arctic MSOA) to reflect the Arctic marine-based and likely biogenic sources for the precursors of the condensing organic vapors. Arctic MSOA from a simulated flux (500 μg m−2 d−1, north of 50° N) of precursor vapors (assumed yield of unity) reduces the summertime particle size distribution model-observation mean fractional error by 2- to 4-fold, relative to a simulation without this Arctic MSOA. Particle growth due to the condensable organic vapor flux contributes strongly (30–50 %) to the simulated summertime-mean number of particles with diameters larger than 20 nm in the study region, and couples with ternary particle nucleation (sulfuric acid, ammonia, and water vapor) and biogenic sulfate condensation to account for more than 90 % of this simulated particle number, a strong biogenic influence. The simulated fit to summertime size-distribution observations is further improved at Eureka and for the ship track by scaling up the nucleation rate by a factor of 100 to account for other particle precursors such as gas-phase iodine and/or amines and/or fragmenting primary particles that could be missing from our simulations. Additionally, the fits to observed size distributions and total aerosol number concentrations for particles larger than 4 nm improve with the assumption that the Arctic MSOA contains semi-volatile species; reducing model-observation mean fractional error by 2- to 3-fold for the Alert and ship track size distributions. Arctic MSOA accounts for more than half of the simulated total particulate organic matter mass concentrations in the summertime Canadian Arctic Archipelago, and this Arctic MSOA has strong simulated summertime pan-Arctic-mean top-of-the-atmosphere aerosol direct (−0.04 W m−2) and cloud-albedo indirect (−0.4 W m−2) radiative effects. Future work should focus on further understanding summertime Arctic sources of Arctic MSOA.


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