scholarly journals The potential role of methanesulfonic acid (MSA) in aerosol formation and growth and the associated radiative forcings

2019 ◽  
Vol 19 (5) ◽  
pp. 3137-3160 ◽  
Author(s):  
Anna L. Hodshire ◽  
Pedro Campuzano-Jost ◽  
John K. Kodros ◽  
Betty Croft ◽  
Benjamin A. Nault ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Methanesulfonic Acid ◽  
Aerosol Size Distribution ◽  
Size Distributions ◽  
Global Models ◽  
Cloud Albedo ◽  
Dms Oxidation ◽  
Aerosol Mass ◽  
The Impact ◽  
Model Measurement

Abstract. Atmospheric marine aerosol particles impact Earth's albedo and climate. These particles can be primary or secondary and come from a variety of sources, including sea salt, dissolved organic matter, volatile organic compounds, and sulfur-containing compounds. Dimethylsulfide (DMS) marine emissions contribute greatly to the global biogenic sulfur budget, and its oxidation products can contribute to aerosol mass, specifically as sulfuric acid and methanesulfonic acid (MSA). Further, sulfuric acid is a known nucleating compound, and MSA may be able to participate in nucleation when bases are available. As DMS emissions, and thus MSA and sulfuric acid from DMS oxidation, may have changed since pre-industrial times and may change in a warming climate, it is important to characterize and constrain the climate impacts of both species. Currently, global models that simulate aerosol size distributions include contributions of sulfate and sulfuric acid from DMS oxidation, but to our knowledge, global models typically neglect the impact of MSA on size distributions. In this study, we use the GEOS-Chem-TOMAS (GC-TOMAS) global aerosol microphysics model to determine the impact on aerosol size distributions and subsequent aerosol radiative effects from including MSA in the size-resolved portion of the model. The effective equilibrium vapor pressure of MSA is currently uncertain, and we use the Extended Aerosol Inorganics Model (E-AIM) to build a parameterization for GC-TOMAS of MSA's effective volatility as a function of temperature, relative humidity, and available gas-phase bases, allowing MSA to condense as an ideally nonvolatile or semivolatile species or too volatile to condense. We also present two limiting cases for MSA's volatility, assuming that MSA is always ideally nonvolatile (irreversible condensation) or that MSA is always ideally semivolatile (quasi-equilibrium condensation but still irreversible condensation). We further present simulations in which MSA participates in binary and ternary nucleation with the same efficacy as sulfuric acid whenever MSA is treated as ideally nonvolatile. When using the volatility parameterization described above (both with and without nucleation), including MSA in the model changes the global annual averages at 900 hPa of submicron aerosol mass by 1.2 %, N3 (number concentration of particles greater than 3 nm in diameter) by −3.9 % (non-nucleating) or 112.5 % (nucleating), N80 by 0.8 % (non-nucleating) or 2.1 % (nucleating), the cloud-albedo aerosol indirect effect (AIE) by −8.6 mW m−2 (non-nucleating) or −26 mW m−2 (nucleating), and the direct radiative effect (DRE) by −15 mW m−2 (non-nucleating) or −14 mW m−2 (nucleating). The sulfate and sulfuric acid from DMS oxidation produces 4–6 times more submicron mass than MSA does, leading to an ∼10 times stronger cooling effect in the DRE. But the changes in N80 are comparable between the contributions from MSA and from DMS-derived sulfate/sulfuric acid, leading to comparable changes in the cloud-albedo AIE. Model–measurement comparisons with the Heintzenberg et al. (2000) dataset over the Southern Ocean indicate that the default model has a missing source or sources of ultrafine particles: the cases in which MSA participates in nucleation (thus increasing ultrafine number) most closely match the Heintzenberg distributions, but we cannot conclude nucleation from MSA is the correct reason for improvement. Model–measurement comparisons with particle-phase MSA observed with a customized Aerodyne high-resolution time-of-flight aerosol mass spectrometer (AMS) from the ATom campaign show that cases with the MSA volatility parameterizations (both with and without nucleation) tend to fit the measurements the best (as this is the first use of MSA measurements from ATom, we provide a detailed description of these measurements and their calibration). However, no one model sensitivity case shows the best model–measurement agreement for both Heintzenberg and the ATom campaigns. As there are uncertainties in both MSA's behavior (nucleation and condensation) and the DMS emissions inventory, further studies on both fronts are needed to better constrain MSA's past, current, and future impacts upon the global aerosol size distribution and radiative forcing.

scholarly journals The potential role of methanesulfonic acid (MSA) in aerosol formation and growth and the associated radiative forcings

2018 ◽  
Author(s):  
Anna L. Hodshire ◽  
Pedro Campuzano-Jost ◽  
John K. Kodros ◽  
Betty Croft ◽  
Benjamin A. Nault ◽  
...  
Keyword(s):  
Sulfuric Acid ◽  
Methanesulfonic Acid ◽  
Climate Impacts ◽  
Aerosol Size Distribution ◽  
Size Distributions ◽  
Global Models ◽  
Dms Oxidation ◽  
Aerosol Mass ◽  
The Impact ◽  
Model Measurement

Abstract. Atmospheric marine aerosol particles impact Earth's albedo and climate. These particles can be primary or secondary and come from a variety of sources, including sea salt, dissolved organic matter, volatile organic compounds, and sulfur-containing compounds. Dimethylsulfide (DMS) marine emissions contribute greatly to the global biogenic sulfur budget, and its oxidation products can contribute to aerosol mass, specifically as sulfuric acid and methanesulfonic acid (MSA). Further, sulfuric acid is a known nucleating compound, and MSA may be able to participate in nucleation when bases are available. As DMS emissions, and thus MSA and sulfuric acid from DMS oxidation, may have changed since pre-industrial times and may change in a warming climate, it is important to characterize and constrain the climate impacts of both species. Currently, global models that simulate aerosol size distributions include contributions of sulfate and sulfuric acid from DMS oxidation, but to our knowledge, global models typically neglect the impact of MSA on size distributions. In this study, we use the GEOS-Chem-TOMAS (GC-TOMAS) global aerosol microphysics model to determine the impact on aerosol size distributions and subsequent aerosol radiative effects from including MSA in the size-resolved portion of the model. The effective equilibrium vapor pressure of MSA is currently uncertain, and we use the Extended Aerosol Inorganics Model (E-AIM) to build a parameterization for GC-TOMAS of MSA's effective volatility as a function of temperature, relative humidity, and available gas-phase bases, allowing MSA to condense as an ideally nonvolatile or semivolatile species or too volatile to condense. We also present two limiting cases for MSA's volatility, assuming that MSA is always ideally nonvolatile (irreversible condensation) or that MSA is always ideally semivolatile (quasi-equilibrium condensation but still irreversible condensation). We further present simulations in which MSA participates in binary and ternary nucleation with the same efficacy as sulfuric acid whenever MSA is treated as ideally nonvolatile. When using the volatility parameterization described above (both with and without nucleation), including MSA in the model changes the global annual averages at 900 hPa of submicron aerosol mass by 1.2 %, N3 (number concentration of particles greater than 3 nm in diameter) by −3.9 % (non-nucleating) or 112.5 % (nucleating), N80 by 0.8 % (non-nucleating) or 2.1 % (nucleating), the aerosol indirect effect (AIE) by −8.6 mW m−2 (non-nucleating) or −26 mW m−2 (nucleating), and the direct radiative effect (DRE) by −15 mW m−2 (non-nucleating) or −14 mW m−2 (nucleating). The sulfate and sulfuric acid from DMS oxidation produces 4–6 times more submicron mass than MSA does, leading to ~ 10 times a stronger cooling effect in the DRE. But the changes in N80 are comparable between the contributions from MSA and from DMS-derived sulfate/sulfuric acid, leading to comparable changes in the AIE. Model-measurement comparisons with the Heintzenberg et al. (2000) dataset over the Southern Ocean indicate that the default model has a missing source or sources of ultrafine particles: the cases in which MSA participates in nucleation (thus increasing ultrafine number) most closely match the Heintzenberg distributions, but we cannot conclude nucleation from MSA is the correct reason for improvement. Model-measurement comparisons with particle-phase MSA observed with a customized Aerodyne high-resolution time-of-flight aerosol mass spectrometer (AMS) from the ATom campaign show that cases with the MSA volatility parameterizations (both with and without nucleation) tend to fit the measurements the best (as this is the first use of MSA measurements from ATom, we provide a detailed description of these measurements and their calibration). However, no one model sensitivity case shows the best model-measurement agreement for both Heintzenberg and the ATom campaigns. As there are uncertainties in both MSA's behavior (nucleation and condensation) and the DMS emissions inventory, further studies on both fronts are needed to better constrain MSA's past, current and future impacts upon the global aerosol size distribution and radiative forcing.

scholarly journals Characterization of the South Atlantic marine boundary layer aerosol using an Aerodyne Aerosol Mass Spectrometer

2008 ◽  
Vol 8 (2) ◽  
pp. 4831-4876 ◽  
Author(s):  
S. R. Zorn ◽  
F. Drewnick ◽  
M. Schott ◽  
T. Hoffmann ◽  
S. Borrmann
Keyword(s):  
Boundary Layer ◽  
Sulfuric Acid ◽  
Marine Boundary Layer ◽  
Methanesulfonic Acid ◽  
Field Measurements ◽  
Size Distributions ◽  
Air Masses ◽  
Aerosol Mass ◽  
Mass Size ◽  
Mass Concentrations

Abstract. Measurements of the submicron fraction of the atmospheric aerosol in the marine boundary layer were performed from January to March 2007 (Southern Hemisphere summer) onboard the French research vessel Marion Dufresne in the Southern Atlantic and Indian Ocean (20° S–60° S, 70° W–60° E). For chemical composition measurements an Aerodyne High-Resolution-Time-of-Flight AMS was used to measure mass concentrations and species-resolved size distributions of non-refractory aerosol components in the submicron range. Within the "standard" AMS compounds (ammonium, chloride, nitrate, sulfate, organics) "sulfate" is the dominating species in the marine boundary layer reaching concentrations between 50 ng m−3 and 3 μg m−3. Furthermore, what is seen as "sulfate" by the AMS seems to be mostly sulfuric acid. Another sulfur containing species that can ubiquitously be found in marine environments is methanesulfonic acid (MSA). Since MSA has not been directly measured before with an AMS, and is not part of the standard AMS analysis, laboratory experiments needed to be performed in order to be able to identify it within the AMS raw data and to extract mass concentrations for MSA from the field measurements. To identify characteristic air masses and their source regions backwards trajectories were used and averaged concentrations for AMS standard compounds were calculated for each air mass type. Sulfate mass size distributions were measured for these periods showing a distinct difference between oceanic air masses and those from African outflow. While the peak size in the mass distribution was roughly 250 nm in marine air masses it was shifted to 470 nm in African outflow air. Correlations between the mass concentrations of sulfate, organics and MSA were calculated which show a narrow correlation for MSA with sulfate/sulfuric acid coming from the ocean but not with continental sulfate.

scholarly journals Characterization of the South Atlantic marine boundary layer aerosol using an aerodyne aerosol mass spectrometer

2008 ◽  
Vol 8 (16) ◽  
pp. 4711-4728 ◽  
Author(s):  
S. R. Zorn ◽  
F. Drewnick ◽  
M. Schott ◽  
T. Hoffmann ◽  
S. Borrmann
Keyword(s):  
Boundary Layer ◽  
Sulfuric Acid ◽  
High Resolution ◽  
Marine Boundary Layer ◽  
Methanesulfonic Acid ◽  
Field Measurements ◽  
Size Distributions ◽  
Air Masses ◽  
Unit Mass Resolution ◽  
Mass Concentrations

Abstract. Measurements of the submicron fraction of the atmospheric aerosol in the marine boundary layer were performed from January to March 2007 (Southern Hemisphere summer) onboard the French research vessel Marion Dufresne in the Southern Atlantic and Indian Ocean (20° S–60° S, 70° W–60° E). We used an Aerodyne High-Resolution-Time-of-Flight AMS to characterize the chemical composition and to measure species-resolved size distributions of non-refractory aerosol components in the submicron range. Within the "standard" AMS compounds (ammonium, chloride, nitrate, sulfate, organics) "sulfate" is the dominant species in the marine boundary layer with concentrations ranging between 50 ng m−3 and 3 μg m−3. Furthermore, what is seen as "sulfate" by the AMS is likely comprised mostly of sulfuric acid. Another sulfur containing species that is produced in marine environments is methanesulfonic acid (MSA). There have been previously measurements of MSA using an Aerodyne AMS. However, due to the use of an instrument equipped with a quadrupole detector with unit mass resolution it was not possible to physically separate MSA from other contributions to the same m/z. In order to identify MSA within the HR-ToF-AMS raw data and to extract mass concentrations for MSA from the field measurements the standard high-resolution MSA fragmentation patterns for the measurement conditions during the ship campaign (e.g. vaporizer temperature) needed to be determined. To identify characteristic air masses and their source regions backwards trajectories were used and averaged concentrations for AMS standard compounds were calculated for each air mass type. Sulfate mass size distributions were measured for these periods showing a distinct difference between oceanic air masses and those from African outflow. While the peak in the mass distribution was roughly at 250 nm (vacuum aerodynamic diameter) in marine air masses, it was shifted to 470 nm in African outflow air. Correlations between the mass concentrations of sulfate, organics and MSA show a narrow correlation for MSA with sulfate/sulfuric acid coming from the ocean, but not with continental sulfate.

scholarly journals SALSA2.0: The sectional aerosol module of the aerosol-chemistry-climate model ECHAM6.3.0-HAM2.3-MOZ1.0

2018 ◽  
Author(s):  
Harri Kokkola ◽  
Thomas Kühn ◽  
Anton Laakso ◽  
Tommi Bergman ◽  
Kari E. J. Lehtinen ◽  
...  
Keyword(s):  
Climate Model ◽  
Stratospheric Aerosol ◽  
Aerosol Size Distribution ◽  
Global Burden ◽  
Size Distributions ◽  
Aerosol Chemistry ◽  
Microphysics Scheme ◽  
Size Dependent ◽  
Aerosol Mass ◽  
Aerosol Module

Abstract. In this paper, we present the implementation and evaluation of the aerosol microphysics module SALSA2.0 in the framework of the aerosol-chemistry-climate model ECHAM-HAMMOZ. It is an alternative microphysics module to the default modal microphysics scheme M7 in ECHAM-HAMMOZ. The SALSA2.0 implementation is evaluated against the observations of aerosol optical properties, aerosol mass, and size distributions. We also compare the skill of SALSA2.0 in reproducing the observed quantities to the skill of the M7 implementation. The largest differences between SALSA2.0 and M7 are evident over regions where the aerosol size distribution is heavily modified by the microphysical processing of aerosol particles. Such regions are, for example, highly polluted regions and regions strongly affected by biomass burning. In addition, in a simulation of the 1991 Mt Pinatubo eruption in which a stratospheric sulfate plume was formed, the global burden and the effective radii of the stratospheric aerosol are very different in SALSA2.0 and M7. While SALSA2.0 was able to reproduce the observed time evolution of the global burden of sulfate and the effective radii of stratospheric aerosol, M7 strongly overestimates the removal of coarse stratospheric particles and thus underestimates the effective radius of stratospheric aerosol. As the mode widths of M7 have been optimized for the troposphere and were not designed to represent stratospheric aerosol the ability of M7 to simulate the volcano plume was improved by modifying the mode widths decreasing the standard deviations of the accumulation and coarse modes from 1.59 and 2.0, respectively, to 1.2. Overall, SALSA2.0 shows promise in improving the aerosol description of ECHAM-HAMMOZ and can be further improved by implementing methods for aerosol processes that are more suitable for the sectional method, e.g size dependent emissions for aerosol species and size resolved wet deposition.

scholarly journals An investigation of processes controlling the evolution of the boundary layer aerosol size distribution properties at the Swedish background station Aspvreten

2004 ◽  
Vol 4 (11/12) ◽  
pp. 2581-2592 ◽  
Author(s):  
P. Tunved ◽  
J. Ström ◽  
H.-C. Hansson
Keyword(s):  
Size Distribution ◽  
Wet Deposition ◽  
Source Area ◽  
Aerosol Size Distribution ◽  
Back Trajectory ◽  
Main Process ◽  
Size Distributions ◽  
Back Trajectory Analysis ◽  
Aerosol Mass ◽  
The One

Abstract. Aerosol size distributions have been measured at the Swedish background station Aspvreten (58.8° N, 17.4° E). Different states of the aerosol were determined using a novel application of cluster analysis. The analysis resulted in eight different clusters capturing different stages of the aerosol lifecycle. The atmospheric aerosol size distributions were interpreted as belonging to fresh, intermediate and aged types of size distribution. With aid of back trajectory analysis we present statistics concerning the relation of source area and different meteorological parameters using a non-Lagrangian approach. Source area is argued to be important although not sufficient to describe the observed aerosol properties. Especially processing by clouds and precipitation is shown to be crucial for the evolution of the aerosol size distribution. As much as 60% of the observed size distributions present features that are likely to be related to cloud processes or wet deposition. The lifetime properties of different sized aerosols are discussed by means of measured variability of the aerosol size distribution. Processing by clouds and precipitation is shown to be especially crucial in the size range 100 nm and larger. This indicates an approximate limit for activation in clouds to 100 nm in this type of environment. The aerosol lifecycle is discussed. Size distributions indicating signs of recent new particle formation (~30% of the observed size distributions) represent the first stage in the lifecycle. Aging of the aerosol size distribution may follow two branches: either growth by condensation and coagulation or processing by non-precipitating clouds. In both cases mass is accumulated. Wet removal is the main process capable of removing aerosol mass. Wet deposition is argued to be an important mechanism in reaching a state where nucleation may occur (i.e. sufficiently low aerosol surface area) in environments similar to the one studied.

scholarly journals The potential role of organics in new particle formation and initial growth in the remote tropical upper troposphere

2020 ◽  
Vol 20 (23) ◽  
pp. 15037-15060
Author(s):  
Agnieszka Kupc ◽  
Christina J. Williamson ◽  
Anna L. Hodshire ◽  
Jan Kazil ◽  
Eric Ray ◽  
...  
Keyword(s):  
Spatial Distribution ◽  
Sulfuric Acid ◽  
Nucleation And Growth ◽  
Box Model ◽  
Acid Water ◽  
Size Distributions ◽  
Global Models ◽  
Upper Troposphere ◽  
Organic Species ◽  
Organic Growth

Abstract. Global observations and model studies indicate that new particle formation (NPF) in the upper troposphere (UT) and subsequent particles supply 40 %–60 % of cloud condensation nuclei (CCN) in the lower troposphere, thus affecting the Earth's radiative budget. There are several plausible nucleation mechanisms and precursor species in this atmospheric region, which, in the absence of observational constraints, lead to uncertainties in modeled aerosols. In particular, the type of nucleation mechanism and concentrations of nucleation precursors, in part, determine the spatial distribution of new particles and resulting spatial distribution of CCN from this source. Although substantial advances in understanding NPF have been made in recent years, NPF processes in the UT in pristine marine regions are still poorly understood and are inadequately represented in global models. Here, we evaluate commonly used and state-of-the-art NPF schemes in a Lagrangian box model to assess which schemes and precursor concentrations best reproduce detailed in situ observations. Using measurements of aerosol size distributions (0.003 < Dp < 4.8 µm) in the remote marine troposphere between ∼0.18 and 13 km altitude obtained during the NASA Atmospheric Tomography (ATom) mission, we show that high concentrations of newly formed particles in the tropical UT over both the Atlantic and Pacific oceans are associated with outflow regions of deep convective clouds. We focus analysis on observations over the remote Pacific Ocean, which is a region less perturbed by continental emissions than the Atlantic. Comparing aerosol size distribution measurements over the remote Pacific with box model simulations for 32 cases shows that none of the NPF schemes most commonly used in global models, including binary nucleation of sulfuric acid and water (neutral and ion-assisted) and ternary involving sulfuric acid, water, and ammonia, are consistent with observations, regardless of precursor concentrations. Through sensitivity studies, we find that the nucleation scheme among those tested that is able to explain most consistently (21 of 32 cases) the observed size distributions is that of Riccobono et al. (2014), which involves both organic species and sulfuric acid. The method of Dunne et al. (2016), involving charged sulfuric acid–water–ammonia nucleation, when coupled with organic growth of the nucleated particles, was most consistent with the observations for 5 of 32 cases. Similarly, the neutral sulfuric acid–water–ammonia method of Napari (2002), when scaled with a tuning factor and with organic growth added, was most consistent for 6 of 32 cases. We find that to best reproduce both nucleation and growth rates, the mixing ratios of gas-phase organic precursors generally need to be at least twice that of SO2, a proxy for dimethyl sulfide (DMS). Unfortunately, we have no information on the nature of oxidized organic species that participated in NPF in this region. Global models rarely include organic-driven nucleation and growth pathways in UT conditions where globally significant NPF takes place, which may result in poor estimates of NPF and CCN abundance and contribute to uncertainties in aerosol–cloud–radiation effects. Furthermore, our results indicate that the organic aerosol precursor vapors may be important in the tropical UT above marine regions, a finding that should guide future observational efforts.

The Impact of the Industrial Processing of Oil on the Rainfall Water Quality

2017 ◽  
Vol 68 (1) ◽  
pp. 175-179
Author(s):  
Oana Roxana Chivu ◽  
Augustin Semenescu ◽  
Claudiu Babis ◽  
Catalin Amza ◽  
Gabriel Iacobescu ◽  
...  
Keyword(s):  
Water Quality ◽  
Sulfuric Acid ◽  
Experimental Research ◽  
Air Purification ◽  
High Toxicity ◽  
Industrial Processing ◽  
Mobile Sources ◽  
Specific Activities ◽  
The Impact ◽  
The Ideal

Rainfall is a major component of the environment and the main source of the air purification becouse of many pollutants increases who have the most varied sources: various human activities including industry and agriculture, and some household duties. Air purification by means of precipitation is achieved by numerous highly complex mechanisms. The final products of degradation of the pollutant in the air, which are generally harmless, can be reacted with each other in the presence of water, giving rise to the final compounds with a high toxicity. Thus, exhaust, mobile sources of noxious almost identical to those specific activities in the industrial processing of oil, contain lead which is the ideal catalyst for converting SO2 to sulfuric acid in the presence of rainwater, with all the disadvantages that they create. This paper will present an experimental research oabout how rainfall water quality is influenced by the activity of the industrial processing of oil, in a chemical plant in Constanta County.

scholarly journals Size-resolved characterization of organic aerosol in the North China Plain: new insights from high resolution spectral analysis

2021 ◽  
Author(s):  
Weiqi Xu ◽  
Chun Chen ◽  
Yanmei Qiu ◽  
Conghui Xie ◽  
Yunle Chen ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
North China Plain ◽  
North China ◽  
Fine Particles ◽  
Large Fraction ◽  
Organic Aerosol ◽  
Size Distributions ◽  
The North ◽  
The Impact

Organic aerosol (OA), a large fraction of fine particles, has a large impact on climate radiative forcing and human health, and the impact depends strongly on size distributions. Here we...

scholarly journals A FEM-Based 2D Model for Simulation and Qualitative Assessment of Shot-Peening Processes

Materials ◽  
2021 ◽  
Vol 14 (11) ◽  
pp. 2784
Author(s):  
Georgios Maliaris ◽  
Christos Gakias ◽  
Michail Malikoutsakis ◽  
Georgios Savaidis
Keyword(s):  
Process Parameters ◽  
Material Properties ◽  
Shot Peening ◽  
Qualitative Assessment ◽  
Experimental Investigations ◽  
Elastoplastic Material ◽  
Size Distributions ◽  
User Friendly ◽  
The Impact ◽  
2D Model

Shot peening is one of the most favored surface treatment processes mostly applied on large-scale engineering components to enhance their fatigue performance. Due to the stochastic nature and the mutual interactions of process parameters and the partially contradictory effects caused on the component’s surface (increase in residual stress, work-hardening, and increase in roughness), there is demand for capable and user-friendly simulation models to support the responsible engineers in developing optimal shot-peening processes. The present paper contains a user-friendly Finite Element Method-based 2D model covering all major process parameters. Its novelty and scientific breakthrough lie in its capability to consider various size distributions and elastoplastic material properties of the shots. Therewith, the model is capable to provide insight into the influence of every individual process parameter and their interactions. Despite certain restrictions arising from its 2D nature, the model can be accurately applied for qualitative or comparative studies and processes’ assessments to select the most promising one(s) for the further experimental investigations. The model is applied to a high-strength steel grade used for automotive leaf springs considering real shot size distributions. The results reveal that the increase in shot velocity and the impact angle increase the extent of the residual stresses but also the surface roughness. The usage of elastoplastic material properties for the shots has been proved crucial to obtain physically reasonable results regarding the component’s behavior.

scholarly journals Evaluating model parameterizations of submicron aerosol scattering and absorption with in situ data from ARCTAS 2008

2016 ◽  
Vol 16 (14) ◽  
pp. 9435-9455 ◽  
Author(s):  
Matthew J. Alvarado ◽  
Chantelle R. Lonsdale ◽  
Helen L. Macintyre ◽  
Huisheng Bian ◽  
Mian Chin ◽  
...  
Keyword(s):  
Optical Properties ◽  
Size Distribution ◽  
Aerosol Size Distribution ◽  
Visible Radiation ◽  
Submicron Aerosol ◽  
In Situ Data ◽  
Aerosol Absorption ◽  
Aerosol Scattering ◽  
The Impact

Abstract. Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10–23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction throughout the aerosol size distribution. Using a core-shell mixing rule in ASP overestimates aerosol absorption, especially for the fresh biomass burning aerosol measured in ARCTAS-B, suggesting the need for modeling the time-varying mixing states of aerosols in future versions of ASP.

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