scholarly journals Separating refractory and non-refractory particulate chloride and estimating chloride depletion by aerosol mass spectrometry in a marine environment

2015 ◽  
Vol 15 (2) ◽  
pp. 2085-2118 ◽  
Author(s):  
I. Nuaaman ◽  
S.-M. Li ◽  
K. L. Hayden ◽  
T. B. Onasch ◽  
P. Massoli ◽  
...  
Keyword(s):  
Scaling Factor ◽  
Sea Salt ◽  
Lower Sensitivity ◽  
Aerosol Composition ◽  
Ambient Aerosols ◽  
Sea Salt Aerosols ◽  
Aerosol Mass ◽  
Chloride Depletion ◽  
Good Tracer ◽  
Continental Outflow

Abstract. Aerosol composition and concentration measurements along the coast of California were obtained using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) onboard the research vessel Atlantis during the CalNex study in 2010. This paper focuses on the measurement of aerosol chloride using the HR-AMS that can be ambiguous in regions with significant quantities of sea salt aerosols. This ambiguity arises due to large differences in the sensitivity of the HR-AMS to refractory chloride species (i.e., NaCl) and non refractory chloride species (i.e., NH4Cl, HCl, etc.). Using the HR-AMS, the aerosol chloride signal is typically quantified using ion signals for 35Cl+, H35Cl+, 37Cl+ and H37Cl+ (HxCl+). During this study, the highest aerosol chloride signal was observed during sea sweep experiments when the source of the aerosol chloride was NaCl present in artificially generated sea salt aerosols even though the HR-AMS has significantly lower sensitivity to such refractory species. Other prominent ion signals that arise from NaCl salt were also observed at m/z 22.99 for Na+ and m/z 57.96 for Na35Cl+ during both sea sweep experiments and during periods of ambient measurements. Thus, refractory NaCl contributes significantly to the HxCl+ signal, interfering with attempts to quantify non sea salt chloride (nssCl). It was found that during ambient aerosol measurements, the interference in the HxCl+ signal from sea salt chloride (ssCl) was as high as 89%, but with a study wide average of 10%. The Na35Cl+ ion signal was found to be a good tracer for NaCl. We outline a method to establish nssCl in the ambient aerosols by subtracting the sea salt chloride (ssCl) signal from the HxCl+ signal. The ssCl signal is derived from the Na35Cl+ ion tracer signal and the HxCl+ to Na35Cl+ ratio established from the sea sweep experiments. Ambient submicron concentrations of ssCl were also established using the Na35Cl+ ion tracer signal and a scaling factor determined through simultaneous measurements of submicron aerosol chloride on filters. This scaling factor accounts for the low vaporization response of the AMS heater to ssCl, although regular calibration of this response is recommended in future applications. It follows that true total particulate chloride (pCl) is the sum of nssCl and ssCl. In this study, the median levels observed for the concentrations of pCl, nssCl and ssCl were 0.052, 0.017 and 0.024 μg m−3 respectively. The average contributions of nssCl and ssCl to pCl were 48 and 52% respectively, with nssCl dominating in periods of continental outflow and ssCl dominating during other periods. Finally, we propose a method to measure percentage chloride depletion of NaCl in ambient submicron sea salt aerosols, strictly using the AMS measurements of Na+ and Na35Cl+ ion signals. The median chloride depletion in submicron aerosols in this study was found to be 78%.

scholarly journals Change in global aerosol composition since preindustrial times

2006 ◽  
Vol 6 (3) ◽  
pp. 5585-5628 ◽  
Author(s):  
K. Tsigaridis ◽  
M. Krol ◽  
F. J. Dentener ◽  
Y. Balkanski ◽  
J. Lathière ◽  
...  
Keyword(s):  
Chemical Composition ◽  
Atmospheric Aerosols ◽  
Transport Model ◽  
Sea Salt ◽  
Carbonaceous Aerosol ◽  
Aerosol Formation ◽  
Aerosol Composition ◽  
Aerosol Mass ◽  
Composition Changes ◽  
Aerosol Chemical Composition

Abstract. To elucidate human induced changes of aerosol load and composition in the atmosphere, a coupled aerosol and gas-phase chemistry transport model of the troposphere and lower stratosphere has been used. This is the first 3-d modeling study that focuses on aerosol chemical composition change since preindustrial times considering the secondary organic aerosol formation together with all other main aerosol components including nitrate. In particular, we evaluate non-sea-salt sulfate (nss-SO4=), ammonium (NH4+), nitrate (NO3-), black carbon (BC), sea-salt, dust, primary and secondary organics (POA and SOA) with a focus on the importance of secondary organic aerosols. Our calculations show that the aerosol optical depth (AOD) has increased by about 21% since preindustrial times. This enhancement of AOD is attributed to a rise in the atmospheric load of BC, nss-SO4=, NO3-, POA and SOA by factors of 3.3, 2.6, 2.7, 2.3 and 1.2, respectively, whereas we assumed that the natural dust and sea-salt sources remained constant. The nowadays increase in carbonaceous aerosol loading is dampened by a 34–42% faster conversion of hydrophobic to hydrophilic carbonaceous aerosol leading to higher removal rates. These changes between the various aerosol components resulted in significant modifications of the aerosol chemical composition. The relative importance of the various aerosol components is critical for the aerosol climatic effect, since atmospheric aerosols behave differently when their chemical composition changes. According to this study, the aerosol composition changed significantly over the different continents and with height since preindustrial times. The presence of anthropogenically emitted primary particles in the atmosphere facilitates the condensation of the semi-volatile species that form SOA onto the aerosol phase, particularly in the boundary layer. The SOA burden that is dominated by the natural component has increased by 24% while its contribution to the AOD has increased by 11%. The increase in oxidant levels and preexisting aerosol mass since preindustrial times is the reason of the burden change, since emissions have not changed significantly. The computed aerosol composition changes translate into about 2.5 times more water associated with non sea-salt aerosol. Additionally, aerosols contain 2.7 times more inorganic components nowadays than during the preindustrial times. We find that the increase in emissions of inorganic aerosol precursors is much larger than the corresponding aerosol increase, reflecting a non-linear atmospheric response.

scholarly journals Tropospheric aerosol microphysics simulation with assimilated meteorology: model description and intermodel comparison

2008 ◽  
Vol 8 (12) ◽  
pp. 3149-3168 ◽  
Author(s):  
W. Trivitayanurak ◽  
P. J. Adams ◽  
D. V. Spracklen ◽  
K. S. Carslaw
Keyword(s):  
Marine Boundary Layer ◽  
Model System ◽  
Sea Salt ◽  
Model Description ◽  
Emission Inventories ◽  
Size Distributions ◽  
Model Intercomparison ◽  
Sea Salt Aerosols ◽  
Aerosol Mass ◽  
Tropospheric Aerosol

Abstract. We implement the TwO-Moment Aerosol Sectional (TOMAS) microphysics module into GEOS-CHEM, a CTM driven by assimilated meteorology. TOMAS has 30 size sections covering 0.01–10 μm diameter with conservation equations for both aerosol mass and number. The implementation enables GEOS-CHEM to simulate aerosol microphysics, size distributions, mass and number concentrations. The model system is developed for sulfate and sea-salt aerosols, a year-long simulation has been performed, and results are compared to observations. Additionally model intercomparison was carried out involving global models with sectional microphysics: GISS GCM-II' and GLOMAP. Comparison with marine boundary layer observations of CN10 and CCN(0.2%) shows that all models perform well with average errors of 30–50%. However, all models underpredict CN10 by up to 42% between 15° S and 45° S while overpredicting CN10 up to 52% between 45° N and 60° N, which could be due to the sea-salt emission parameterization and the assumed size distribution of primary sulfate emission, in each case respectively. Model intercomparison at the surface shows that GISS GCM-II' and GLOMAP, each compared against GEOS-CHEM, both predict 40% higher CN10 and predict 20% and 30% higher CCN(0.2%) on average, respectively. Major discrepancies are due to different emission inventories and transport. Budget comparison shows GEOS-CHEM predicts the lowest global CCN(0.2%) due to microphysical growth being a factor of 2 lower than other models because of lower SO2 availability. These findings stress the need for accurate meteorological inputs, updated emission inventories, and realistic clouds and oxidant fields when evaluating global aerosol microphysics models.

scholarly journals Tropospheric aerosol microphysics simulation with assimilated meteorology: model description and intermodel comparison

2007 ◽  
Vol 7 (5) ◽  
pp. 14369-14411 ◽  
Author(s):  
W. Trivitayanurak ◽  
P. J. Adams ◽  
D. V. Spracklen ◽  
K. S. Carslaw
Keyword(s):  
Marine Boundary Layer ◽  
Model System ◽  
Sea Salt ◽  
Model Description ◽  
Emission Inventories ◽  
Size Distributions ◽  
Model Intercomparison ◽  
Sea Salt Aerosols ◽  
Aerosol Mass ◽  
Tropospheric Aerosol

Abstract. We implement the TwO-Moment Aerosol Sectional (TOMAS) microphysics module into GEOS-CHEM, a CTM driven by assimilated meteorology. TOMAS has 30 size sections covering 0.01–10 μm diameter with conservation equations for both aerosol mass and number. The implementation enables GEOS-CHEM to simulate aerosol microphysics, size distributions, mass and number concentrations. The model system is developed for sulfate and sea-salt aerosols, a year-long simulation has been performed, and results are compared to observations. Additionally model intercomparison was carried out involving global models with sectional microphysics: GISS GCM-II' and GLOMAP. Comparison with marine boundary layer observations of CN and CCN(0.2%) shows that all models perform well with average errors of 30–50%. However, all models underpredict CN by up to 42% between 15° S and 45° S while overpredicting CN up to 52% between 45° N and 60° N, which could be due to the sea-salt emission parameterization and the assumed size distribution of primary sulfate emission, in each case respectively. Model intercomparison at the surface shows that GISS GCM-II' and GLOMAP, each compared against GEOS-CHEM, both predict 40% higher CN and predict 20% and 30% higher CCN(0.2%) on average, respectively. Major discrepancies are due to different emission inventories and transport. Budget comparison shows GEOS-CHEM predicts the lowest global CCN(0.2%) due to microphysical growth being a factor of 2 lower than other models because of lower SO2 availability. These findings stress the need for accurate meteorological inputs and updated emission inventories when evaluating global aerosol microphysics models.

scholarly journals Impact of the particle mixing state on the hygroscopicity of internally mixed sodium chloride-ammonium sulfate single droplets: A theoretical and experimental study

2021 ◽  
Author(s):  
Yeny A. Tobon ◽  
Danielle El Hajj ◽  
Samantha Seng ◽  
Ferdaous Bengrad ◽  
Myriam Moreau ◽  
...  
Keyword(s):  
Experimental Study ◽  
Sodium Chloride ◽  
Ammonium Sulfate ◽  
Atmospheric Transport ◽  
Sea Salt ◽  
Main Constituent ◽  
Sea Salt Aerosols ◽  
Particle Mixing ◽  
Secondary Aerosols ◽  
Single Droplets

Sodium chloride (NaCl) is the main constituent of sea-salt aerosols. During atmospheric transport, sea-salt aerosols can interact with gases and other particles including secondary aerosols containing ammonium sulfate ((NH4)2SO4). This...

scholarly journals Linking variations in sea spray aerosol particle hygroscopicity to composition during two microcosm experiments

2016 ◽  
Author(s):  
Sara D. Forestieri ◽  
Gavin C. Cornwell ◽  
Taylor M. Helgestad ◽  
Kathryn A. Moore ◽  
Christopher Lee ◽  
...  
Keyword(s):  
Light Scattering ◽  
Relative Humidity ◽  
Salt Content ◽  
Sea Salt ◽  
Sea Spray ◽  
Hygroscopic Growth ◽  
Phytoplankton Blooms ◽  
Aerosol Composition ◽  
Sea Spray Aerosol ◽  
Indoor And Outdoor

Abstract. The extent to which water uptake influences the light scattering ability of marine sea spray aerosol (SSA) particles depends critically on SSA chemical composition. The organic fraction of SSA can increase during phytoplankton blooms, decreasing the salt content and therefore the hygroscopicity of the particles. In this study, subsaturated hygroscopic growth factors at 85 % relative humidity (GF(85 %)) of SSA particles were quantified during two induced phytoplankton blooms in marine aerosol reference tanks (MARTs). One MART was illuminated with fluorescent lights and the other was illuminated with sunlight, referred to as the "indoor" and "outdoor" MARTs, respectively. GF(85 %) values for SSA particles were derived from measurements of light scattering and particle size distributions, concurrently with online single particle and bulk aerosol composition measurements. During both microcosm experiments, the observed bulk average GF(85 %) values were depressed substantially relative to pure, inorganic sea salt, by 10 to 19 %, with a one (indoor MART) and six (outdoor MART) day lag between GF(85 %) depression and the peak chlorophyll-a concentrations. The fraction of organiccontaining SSA particles generally increased after the peak of the phytoplankton blooms. The GF(85 %) values were inversely correlated with the fraction of particles containing organic or other biological markers. This indicates these particles were less hygroscopic than the particles identified as predominately sea salt containing and demonstrates a clear relationship between SSA particle composition and the sensitivity of light scattering to variations in relative humidity. The implications of these observations to the direct climate effects of SSA particles are discussed.

scholarly journals Aerosol chemical and optical properties over the Paris area within ESQUIF project

2006 ◽  
Vol 6 (11) ◽  
pp. 3257-3280 ◽  
Author(s):  
A. Hodzic ◽  
R. Vautard ◽  
P. Chazette ◽  
L. Menut ◽  
B. Bessagnet
Keyword(s):  
Optical Properties ◽  
Secondary Organic Aerosols ◽  
Organic Aerosols ◽  
Dust Particles ◽  
Aerosol Size Distribution ◽  
Aerosol Composition ◽  
Aerosol Mass ◽  
Coarse Mode ◽  
Paris Area ◽  
Flight Trajectories

Abstract. Aerosol chemical and optical properties are extensively investigated for the first time over the Paris Basin in July 2000 within the ESQUIF project. The measurement campaign offers an exceptional framework to evaluate the performances of the chemistry-transport model CHIMERE in simulating concentrations of gaseous and aerosol pollutants, as well as the aerosol-size distribution and composition in polluted urban environments against ground-based and airborne measurements. A detailed comparison of measured and simulated variables during the second half of July with particular focus on 19 and 31 pollution episodes reveals an overall good agreement for gas-species and aerosol components both at the ground level and along flight trajectories, and the absence of systematic biases in simulated meteorological variables such as wind speed, relative humidity and boundary layer height as computed by the MM5 model. A good consistency in ozone and NO concentrations demonstrates the ability of the model to reproduce the plume structure and location fairly well both on 19 and 31 July, despite an underestimation of the amplitude of ozone concentrations on 31 July. The spatial and vertical aerosol distributions are also examined by comparing simulated and observed lidar vertical profiles along flight trajectories on 31 July and confirm the model capacity to simulate the plume characteristics. The comparison of observed and modeled aerosol components in the southwest suburb of Paris during the second half of July indicates that the aerosol composition is rather correctly reproduced, although the total aerosol mass is underestimated by about 20%. The simulated Parisian aerosol is dominated by primary particulate matter that accounts for anthropogenic and biogenic primary particles (40%), and inorganic aerosol fraction (40%) including nitrate (8%), sulfate (22%) and ammonium (10%). The secondary organic aerosols (SOA) represent 12% of the total aerosol mass, while the mineral dust accounts for 8%. The comparison demonstrates the absence of systematic errors in the simulated sulfate, ammonium and nitrates total concentrations. However, for nitrates the observed partition between fine and coarse mode is not reproduced. In CHIMERE there is a clear lack of coarse-mode nitrates. This calls for additional parameterizations in order to account for the heterogeneous formation of nitrate onto dust particles. Larger discrepancies are obtained for the secondary organic aerosols due to both inconsistencies in the SOA formation processes in the model leading to an underestimation of their mass and large uncertainties in the determination of the measured aerosol organic fraction. The observed mass distribution of aerosols is not well reproduced, although no clear explanation can be given.

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