The impacts of aerosol loading, composition, and water uptake on aerosol  extinction variability in the Baltimore–Washington, D.C. region

Abstract. In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites) and mass measurements of aerosol loading (PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type – such as composition, size, and hygroscopicity – and to the surrounding atmosphere, such as temperature, relative humidity (RH), and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project, extensive in situ atmospheric profiling in the Baltimore, MD–Washington, D.C. region was performed during 14 flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties, and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 %) and organics (57 %). A distinct difference in composition was observed, with high-loading days having a proportionally larger percentage of sulfate due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity) such that higher relative contributions of inorganics increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity, causing an increase in the water content of the aerosol. Conversely, low-aerosol-loading days had lower sulfate and higher black carbon contributions, causing lower single-scattering albedos (SSAs). The average black carbon concentrations were 240 ng m−3 in the lowest 1 km, decreasing to 35 ng m−3 in the free troposphere (above 3 km). Routine airborne sampling over six locations was used to evaluate the relative contributions of aerosol loading, composition, and relative humidity (the amount of water available for uptake onto aerosols) to variability in mixed-layer aerosol extinction. Aerosol loading (dry extinction) was found to be the predominant source, accounting for 88 % on average of the measured spatial variability in ambient extinction, with lesser contributions from variability in relative humidity (10 %) and aerosol composition (1.3 %). On average, changes in aerosol loading also caused 82 % of the diurnal variability in ambient aerosol extinction. However on days with relative humidity above 60 %, variability in RH was found to cause up to 62 % of the spatial variability and 95 % of the diurnal variability in ambient extinction. This work shows that extinction is driven to first order by aerosol mass loadings; however, humidity-driven hydration effects play an important secondary role. This motivates combined satellite–modeling assimilation products that are able to capture these components of the aerosol optical depth (AOD)–PM2.5 link. Conversely, aerosol hygroscopicity and SSA play a minor role in driving variations both spatially and throughout the day in aerosol extinction and therefore AOD. However, changes in aerosol hygroscopicity from day to day were large and could cause a bias of up to 27 % if not accounted for. Thus it appears that a single daily measurement of aerosol hygroscopicity can be used for AOD-to-PM2.5 conversions over the study region (on the order of 1400 km2). This is complimentary to the results of Chu et al. (2015), who determined that the aerosol vertical distribution from "a single lidar is feasible to cover the range of 100 km" in the same region.

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Aerosol composition and variability in the Baltimore–Washington, DC region

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-15-23317-2015 ◽

2015 ◽

Vol 15 (16) ◽

pp. 23317-23355

Author(s):

A. J. Beyersdorf ◽

L. D. Ziemba ◽

G. Chen ◽

C. A. Corr ◽

J. H. Crawford ◽

...

Keyword(s):

Air Quality ◽

Relative Humidity ◽

Ammonium Sulfate ◽

Washington Dc ◽

Aerosol Extinction ◽

Aerosol Composition ◽

Diurnal Variability ◽

Aerosol Loading ◽

Aerosol Mass ◽

Aerosol Hygroscopicity

Abstract. In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites) and mass measurements of aerosol loading (PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type, such as composition, size and hygroscopicity, and to the surrounding atmosphere, such as temperature, relative humidity (RH) and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project, extensive in-situ atmospheric profiling in the Baltimore, MD–Washington, DC region was performed during fourteen flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 %) and organics (57 %). A distinct difference in composition was observed with high-loading days having a proportionally larger percentage of ammonium sulfate (up to 49 %) due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity) such that higher relative contributions of ammonium sulfate increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity causing an increase in the water content of the aerosol. Conversely, low aerosol loading days had lower ammonium sulfate and higher black carbon contributions causing lower single scattering albedos (SSAs). The average black carbon concentrations were 240 ng m−3 in the lowest 1 km decreasing to 35 ng m−3 in the free troposphere (above 3 km). Routine airborne sampling over six locations was used to evaluate the relative contributions of aerosol loading, composition, and relative humidity (the amount of water available for uptake onto aerosols) to variability in mixed layer aerosol. Aerosol loading was found to be the predominant source accounting for 88 % on average of the measured spatial variability in extinction with lesser contributions from variability in relative humidity (10 %) and aerosol composition (1.3 %). On average, changes in aerosol loading also caused 82 % of the diurnal variability in ambient aerosol extinction. However on days with relative humidity above 60 %, variability in RH was found to cause up to 62 % of the spatial variability and 95 % of the diurnal variability in ambient extinction. This work shows that extinction is driven to first-order by aerosol mass loadings; however, humidity-driven hydration effects play an important secondary role. This motivates combined satellite/modelling assimilation products that are able to capture these components of the AOD-PM2.5 link. Conversely, aerosol hygroscopicity and SSA play a minor role in driving variations both spatially and throughout the day in aerosol extinction and therefore AOD. However, changes in aerosol hygroscopicity from day-to-day were large and could cause a bias of up to 27 % if not accounted for. Thus it appears that a single daily measurement of aerosol hygroscopicity can be used for AOD-to-PM2.5 conversions over the study region (on the order of 1400 km2). This is complimentary to the results of Chu et al. (2015) that determined the aerosol vertical distribution from "a single lidar is feasible to cover the range of 100 km" in the same region.

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Understanding and improving model representation of aerosol optical properties for a Chinese haze event measured during KORUS-AQ

10.5194/acp-2019-1022 ◽

2019 ◽

Cited By ~ 1

Author(s):

Pablo E. Saide ◽

Meng Gao ◽

Zifeng Lu ◽

Dan Goldberg ◽

David G. Streets ◽

...

Keyword(s):

Optical Properties ◽

Air Quality ◽

Data Assimilation ◽

Health Effect ◽

Model Representation ◽

Climate Projections ◽

Hygroscopic Growth ◽

Multiple Sources ◽

Inorganic Aerosols ◽

Aerosol Mass

Abstract. KORUS-AQ was an international cooperative air quality field study in South Korea that measured local and remote sources of air pollution affecting the Korean peninsula during May–June 2016. Some of the largest aerosol mass concentrations were measured during a Chinese haze transport event (May 24th). Air quality forecasts using the WRF-Chem model with aerosol optical depth (AOD) data assimilation captured AOD during this pollution episode but over-predicted surface particulate matter concentrations, especially PM2.5 often by a factor of 2 or larger. Analysis revealed multiple sources of model deficiency related to the calculation of optical properties from aerosol mass that explain these discrepancies. Using in-situ observations of aerosol size and composition as inputs to the optical properties calculations showed that using a low resolution size bin representation under-estimates the efficiency at which aerosols scatter and absorb light (mass extinction efficiency). Besides using finer-resolution size bins, it was also necessary to increase the refractive indices and hygroscopicity of select aerosol species within the range of values reported in the literature to achieve consistency with measured values of mass/volume extinction efficiencies and light scattering enhancement factor (f(RH)) due to aerosol hygroscopic growth. Furthermore, evaluation of optical properties obtained using modeled aerosol properties revealed the inability of sectional and modal aerosol representations in WRF-Chem to properly reproduce the observed size distribution, with the models displaying a much wider accumulation mode. Other model deficiencies included an under-estimate of organic aerosol density and an over-prediction of the fractional contribution of inorganic aerosols other than sulfate, ammonium, nitrate, chloride and sodium (mostly dust). These results illustrate the complexity of achieving an accurate model representation of optical properties and provide potential solutions that are relevant to multiple disciplines and applications such as air quality forecasts, health-effect assessments, climate projections, solar-power forecasts, and aerosol data assimilation.

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Quantification of black carbon mixing state from traffic: implications for aerosol optical properties

Atmospheric Chemistry and Physics ◽

10.5194/acp-16-4693-2016 ◽

2016 ◽

Vol 16 (7) ◽

pp. 4693-4706 ◽

Cited By ~ 22

Author(s):

Megan D. Willis ◽

Robert M. Healy ◽

Nicole Riemer ◽

Matthew West ◽

Jon M. Wang ◽

...

Keyword(s):

Optical Properties ◽

Black Carbon ◽

Chemical Properties ◽

Mixing State ◽

Aerosol Optical Properties ◽

Aerosol Composition ◽

Average Mass ◽

Measurement Capability ◽

Aerosol Mass ◽

Physical And Chemical

Abstract. The climatic impacts of black carbon (BC) aerosol, an important absorber of solar radiation in the atmosphere, remain poorly constrained and are intimately related to its particle-scale physical and chemical properties. Using particle-resolved modelling informed by quantitative measurements from a soot-particle aerosol mass spectrometer, we confirm that the mixing state (the distribution of co-emitted aerosol amongst fresh BC-containing particles) at the time of emission significantly affects BC-aerosol optical properties even after a day of atmospheric processing. Both single particle and ensemble aerosol mass spectrometry observations indicate that BC near the point of emission co-exists with hydrocarbon-like organic aerosol (HOA) in two distinct particle types: HOA-rich and BC-rich particles. The average mass fraction of black carbon in HOA-rich and BC-rich particle classes was < 0.1 and 0.8, respectively. Notably, approximately 90 % of BC mass resides in BC-rich particles. This new measurement capability provides quantitative insight into the physical and chemical nature of BC-containing particles and is used to drive a particle-resolved aerosol box model. Significant differences in calculated single scattering albedo (an increase of 0.1) arise from accurate treatment of initial particle mixing state as compared to the assumption of uniform aerosol composition at the point of BC injection into the atmosphere.

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Modeling the smoky troposphere of the southeast Atlantic: a comparison to ORACLES airborne observations from September of 2016

Atmospheric Chemistry and Physics ◽

10.5194/acp-20-11491-2020 ◽

2020 ◽

Vol 20 (19) ◽

pp. 11491-11526 ◽

Cited By ~ 2

Author(s):

Yohei Shinozuka ◽

Pablo E. Saide ◽

Gonzalo A. Ferrada ◽

Sharon P. Burton ◽

Richard Ferrare ◽

...

Keyword(s):

Boundary Layer ◽

Optical Properties ◽

Black Carbon ◽

Marine Boundary Layer ◽

Organic Aerosol ◽

Airborne Lidar ◽

Aerosol Mass ◽

Wide Range ◽

Smoke Layer ◽

Mass Concentrations

Abstract. In the southeast Atlantic, well-defined smoke plumes from Africa advect over marine boundary layer cloud decks; both are most extensive around September, when most of the smoke resides in the free troposphere. A framework is put forth for evaluating the performance of a range of global and regional atmospheric composition models against observations made during the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) airborne mission in September 2016. A strength of the comparison is a focus on the spatial distribution of a wider range of aerosol composition and optical properties than has been done previously. The sparse airborne observations are aggregated into approximately 2∘ grid boxes and into three vertical layers: 3–6 km, the layer from cloud top to 3 km, and the cloud-topped marine boundary layer. Simulated aerosol extensive properties suggest that the flight-day observations are reasonably representative of the regional monthly average, with systematic deviations of 30 % or less. Evaluation against observations indicates that all models have strengths and weaknesses, and there is no single model that is superior to all the others in all metrics evaluated. Whereas all six models typically place the top of the smoke layer within 0–500 m of the airborne lidar observations, the models tend to place the smoke layer bottom 300–1400 m lower than the observations. A spatial pattern emerges, in which most models underestimate the mean of most smoke quantities (black carbon, extinction, carbon monoxide) on the diagonal corridor between 16∘ S, 6∘ E, and 10∘ S, 0∘ E, in the 3–6 km layer, and overestimate them further south, closer to the coast, where less aerosol is present. Model representations of the above-cloud aerosol optical depth differ more widely. Most models overestimate the organic aerosol mass concentrations relative to those of black carbon, and with less skill, indicating model uncertainties in secondary organic aerosol processes. Regional-mean free-tropospheric model ambient single scattering albedos vary widely, between 0.83 and 0.93 compared with in situ dry measurements centered at 0.86, despite minimal impact of humidification on particulate scattering. The modeled ratios of the particulate extinction to the sum of the black carbon and organic aerosol mass concentrations (a mass extinction efficiency proxy) are typically too low and vary too little spatially, with significant inter-model differences. Most models overestimate the carbonaceous mass within the offshore boundary layer. Overall, the diversity in the model biases suggests that different model processes are responsible. The wide range of model optical properties requires further scrutiny because of their importance for radiative effect estimates.

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Amplification of black carbon light absorption induced by atmospheric aging: temporal variation at seasonal and diel scales in urban Guangzhou

10.5194/acp-2019-654 ◽

2019 ◽

Author(s):

Jia Yin Sun ◽

Cheng Wu ◽

Dui Wu ◽

Chunlei Cheng ◽

Mei Li ◽

...

Keyword(s):

Optical Properties ◽

Organic Carbon ◽

Black Carbon ◽

Light Absorption ◽

Dry Season ◽

Diurnal Fluctuation ◽

Absorption Enhancement ◽

Wet Season ◽

Diurnal Variability ◽

The Impact

Abstract. Black carbon (BC) is an important climate forcer in the atmosphere. Amplification of light absorption can occur by coatings on BC aerosols, an effect that remains one of the major sources of uncertainties for accessing the radiative forcing of BC. In this study, the absorption enhancement factor (Eabs) was quantified by the minimum R squared (MRS) method using elemental carbon (EC) as the tracer. Two field campaigns were conducted in urban Guangzhou at the Jinan university super site during both wet season (July 31–September 10, 2017) and dry season (November 15, 2017–January 15, 2018) to explore the temporal dynamics of BC optical properties. The average concentration of EC was 1.94 ± 0.93 and 2.81 ± 2.01 μgC m−3 in the wet and dry seasons, respectively. Mass absorption efficiency at 520 nm by primary aerosols (MAEp520) determined by MRS exhibit a strong seasonality (8.6 m2g−1 in the wet season and 16.8 m2g−1 in the dry season). Eabs520 was higher in the wet season (1.51 ± 0.50) and lower in the dry season (1.29 ± 0.28). Absorption Ångström exponent (AAE470-660) in the dry season (1.46 ± 0.12) were higher than that in the wet season (1.37 ± 0.10). Collective evidence showed that the active biomass burning (BB) in dry season effectively altered optical properties of BC, leading to elevated MAE, MAEp and AAE in dry season comparing to those in wet season. Diurnal Eabs520 was positively correlated with AAE470-660 (R2 = 0.71) and negatively correlated with the AE33 aerosol loading compensation parameter (k) (R2 = 0.74) in the wet season, but these correlations were significantly weaker in the dry season, which may be related to the impact of BB. This result suggests that lensing effect was dominating the AAE diurnal variability during the wet season. The effect of secondary processing on Eabs diurnal dynamic were also investigated. The Eabs520 exhibit a clear dependency on secondary organic carbon to organic carbon ratio (SOC/OC). Eabs520 correlated well with nitrate, implying that gas-particle partitioning of semi-volatile compounds may potentially play an important role in steering the diurnal fluctuation of Eabs520. In dry season, the diurnal variability of Eabs520 was associated with photochemical aging as evidenced by the good correlation (R2 = 0.69) between oxidant concentrations (Ox=O3+NO2) and Eabs520.

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Measurement-based climatology of aerosol direct radiative effect, its sensitivities, and uncertainties from a background southeast US site

Atmospheric Chemistry and Physics ◽

10.5194/acp-18-4131-2018 ◽

2018 ◽

Vol 18 (6) ◽

pp. 4131-4152 ◽

Cited By ~ 3

Author(s):

James P. Sherman ◽

Allison McComiskey

Keyword(s):

Optical Properties ◽

Surface Reflectance ◽

Radiative Effect ◽

Aerosol Optical Properties ◽

Diurnal Variability ◽

Clear Sky ◽

Aerosol Loading ◽

Measurement Uncertainties ◽

Southeast Us ◽

Seasonal Dependence

Abstract. Aerosol optical properties measured at Appalachian State University's co-located NASA AERONET and NOAA ESRL aerosol network monitoring sites over a nearly four-year period (June 2012–Feb 2016) are used, along with satellite-based surface reflectance measurements, to study the seasonal variability of diurnally averaged clear sky aerosol direct radiative effect (DRE) and radiative efficiency (RE) at the top-of-atmosphere (TOA) and at the surface. Aerosol chemistry and loading at the Appalachian State site are likely representative of the background southeast US (SE US), home to high summertime aerosol loading and one of only a few regions not to have warmed during the 20th century. This study is the first multi-year ground truth DRE study in the SE US, using aerosol network data products that are often used to validate satellite-based aerosol retrievals. The study is also the first in the SE US to quantify DRE uncertainties and sensitivities to aerosol optical properties and surface reflectance, including their seasonal dependence.Median DRE for the study period is −2.9 W m−2 at the TOA and −6.1 W m−2 at the surface. Monthly median and monthly mean DRE at the TOA (surface) are −1 to −2 W m−2 (−2 to −3 W m−2) during winter months and −5 to −6 W m−2 (−10 W m−2) during summer months. The DRE cycles follow the annual cycle of aerosol optical depth (AOD), which is 9 to 10 times larger in summer than in winter. Aerosol RE is anti-correlated with DRE, with winter values 1.5 to 2 times more negative than summer values. Due to the large seasonal dependence of aerosol DRE and RE, we quantify the sensitivity of DRE to aerosol optical properties and surface reflectance, using a calendar day representative of each season (21 December for winter; 21 March for spring, 21 June for summer, and 21 September for fall). We use these sensitivities along with measurement uncertainties of aerosol optical properties and surface reflectance to calculate DRE uncertainties. We also estimate uncertainty in calculated diurnally-averaged DRE due to diurnal aerosol variability. Aerosol DRE at both the TOA and surface is most sensitive to changes in AOD, followed by single-scattering albedo (ω0). One exception is under the high summertime aerosol loading conditions (AOD  ≥  0.15 at 550 nm), when sensitivity of TOA DRE to ω0 is comparable to that of AOD. Aerosol DRE is less sensitive to changes in scattering asymmetry parameter (g) and surface reflectance (R). While DRE sensitivity to AOD varies by only ∼ 25 to 30 % with season, DRE sensitivity to ω0, g, and R largely follow the annual AOD cycle at APP, varying by factors of 8 to 15 with season. Since the measurement uncertainties of AOD, ω0, g, and R are comparable at Appalachian State, their relative contributions to DRE uncertainty are largely influenced by their (seasonally dependent) DRE sensitivity values, which suggests that the seasonal dependence of DRE uncertainty must be accounted for. Clear sky aerosol DRE uncertainty at the TOA (surface) due to measurement uncertainties ranges from 0.45 (0.75 W m−2) for December to 1.1 (1.6 W m−2) for June. Expressed as a fraction of DRE computed using monthly median aerosol optical properties and surface reflectance, the DRE uncertainties at TOA (surface) are 20 to 24 % (15 to 22 %) for March, June, and September and 49 (50 %) for DEC. The relatively low DRE uncertainties are largely due to the low uncertainty in AOD measured by AERONET. Use of satellite-based AOD measurements by MODIS in the DRE calculations increases DRE uncertainties by a factor of 2 to 5 and DRE uncertainties are dominated by AOD uncertainty for all seasons. Diurnal variability in AOD (and to a lesser extent g) contributes to uncertainties in DRE calculated using daily-averaged aerosol optical properties that are slightly larger (by ∼ 20 to 30 %) than DRE uncertainties due to measurement uncertainties during summer and fall, with comparable uncertainties during winter and spring.

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Retrieval of Aerosol Optical Properties over East Asia from TROPOMI using GEMS Aerosol Algorithm

10.5194/egusphere-egu21-6841 ◽

2021 ◽

Author(s):

Yeseul Cho ◽

Jhoon Kim ◽

Sujung Go ◽

Mijin Kim ◽

Hyunkwang Lim ◽

...

Keyword(s):

Optical Properties ◽

Air Quality ◽

East Asia ◽

Spatial Resolution ◽

High Spatial Resolution ◽

Visible Range ◽

Fine Scale ◽

Aerosol Optical Properties ◽

Aerosol Loading

<p>To better understanding the role of aerosols in climate change and their direct effects on human health, aerosol optical properties have been monitored by various satellite sensors. Successful operations of the Tropospheric Monitoring Instrument (TROPOMI) onboard the Copernicus Sentinel-5 Precursor satellite allow an improved understanding of the wide-ranging variation in aerosol distribution and properties with high spatial resolution since 2018. The Geostationary Environmental Monitoring Spectrometer (GEMS), onboard Geokompsat-2B (GK-2B) satellites, is the first air quality monitoring sensor in geostationary earth orbit and was successfully launched on February 19, 2020. GEMS measures hourly hyperspectral radiances with the spectral resolution of 0.6 nm in UV and visible range (300 &#8211; 500 nm) and the spatial resolution of 3.5 x 8 km<sup>2</sup> over Asia during the daytime to provide air quality information. TROPOMI which has similar specifications to GEMS, has the advantages of the sensitivity of aerosol absorption and aerosol height information in UV-Vis wavelengths. GEMS aerosol algorithm was applied to the Level 1B data of TROPOMI to retrieve aerosol optical properties such as aerosol optical depth (AOD), UV aerosol index (UVAI), single scattering albedo (SSA), and aerosol loading height (ALH). We present GEMS aerosol retrieval results to discuss high aerosol loading cases over East Asia and analysis results as a case study. Our results show that the GEMS aerosol products have the advantage to capture the fine-scale features of aerosol properties in high spatial resolution. Further, the results are compared to other aerosol products obtained from the Advanced Himawari Imager (AHI) onboard Himawari-8. Qualitatively good agreements and fine-scale features are shown in this case study.</p>

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Black carbon in the Lower Fraser Valley, British Columbia: Impact of 2017 wildfires on local air quality and aerosol optical properties

Atmospheric Environment ◽

10.1016/j.atmosenv.2019.116976 ◽

2019 ◽

Vol 217 ◽

pp. 116976 ◽

Cited By ~ 2

Author(s):

Robert M. Healy ◽

Jonathan M. Wang ◽

Uwayemi Sofowote ◽

Yushan Su ◽

Jerzy Debosz ◽

...

Keyword(s):

British Columbia ◽

Optical Properties ◽

Air Quality ◽

Black Carbon ◽

Aerosol Optical Properties ◽

Lower Fraser Valley ◽

Fraser Valley

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Understanding and improving model representation of aerosol optical properties for a Chinese haze event measured during KORUS-AQ

Atmospheric Chemistry and Physics ◽

10.5194/acp-20-6455-2020 ◽

2020 ◽

Vol 20 (11) ◽

pp. 6455-6478 ◽

Cited By ~ 1

Author(s):

Pablo E. Saide ◽

Meng Gao ◽

Zifeng Lu ◽

Daniel L. Goldberg ◽

David G. Streets ◽

...

Keyword(s):

Optical Properties ◽

Air Quality ◽

Data Assimilation ◽

South Korea ◽

Mass Extinction ◽

Model Representation ◽

Climate Projections ◽

Extinction Efficiency ◽

Aerosol Mass ◽

Mass Extinction Efficiency

Abstract. KORUS-AQ was an international cooperative air quality field study in South Korea that measured local and remote sources of air pollution affecting the Korean Peninsula during May–June 2016. Some of the largest aerosol mass concentrations were measured during a Chinese haze transport event (24 May). Air quality forecasts using the WRF-Chem model with aerosol optical depth (AOD) data assimilation captured AOD during this pollution episode but overpredicted surface particulate matter concentrations in South Korea, especially PM2.5, often by a factor of 2 or larger. Analysis revealed multiple sources of model deficiency related to the calculation of optical properties from aerosol mass that explain these discrepancies. Using in situ observations of aerosol size and composition as inputs to the optical properties calculations showed that using a low-resolution size bin representation (four bins) underestimates the efficiency with which aerosols scatter and absorb light (mass extinction efficiency). Besides using finer-resolution size bins (8–16 bins), it was also necessary to increase the refractive indices and hygroscopicity of select aerosol species within the range of values reported in the literature to achieve better consistency with measured values of the mass extinction efficiency (6.7 m2 g−1 observed average) and light-scattering enhancement factor (f(RH)) due to aerosol hygroscopic growth (2.2 observed average). Furthermore, an evaluation of the optical properties obtained using modeled aerosol properties revealed the inability of sectional and modal aerosol representations in WRF-Chem to properly reproduce the observed size distribution, with the models displaying a much wider accumulation mode. Other model deficiencies included an underestimate of organic aerosol density (1.0 g cm−3 in the model vs. observed average of 1.5 g cm−3) and an overprediction of the fractional contribution of submicron inorganic aerosols other than sulfate, ammonium, nitrate, chloride, and sodium corresponding to mostly dust (17 %–28 % modeled vs. 12 % estimated from observations). These results illustrate the complexity of achieving an accurate model representation of optical properties and provide potential solutions that are relevant to multiple disciplines and applications such as air quality forecasts, health impact assessments, climate projections, solar power forecasts, and aerosol data assimilation.

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Amplification of black carbon light absorption induced by atmospheric aging: temporal variation at seasonal and diel scales in urban Guangzhou

Atmospheric Chemistry and Physics ◽

10.5194/acp-20-2445-2020 ◽

2020 ◽

Vol 20 (4) ◽

pp. 2445-2470 ◽

Cited By ~ 6

Author(s):

Jia Yin Sun ◽

Cheng Wu ◽

Dui Wu ◽

Chunlei Cheng ◽

Mei Li ◽

...

Keyword(s):

Optical Properties ◽

Organic Carbon ◽

Black Carbon ◽

Light Absorption ◽

Dry Season ◽

Diurnal Fluctuation ◽

Absorption Enhancement ◽

Wet Season ◽

Diurnal Variability ◽

Atmospheric Aging

Abstract. Black carbon (BC) aerosols have been widely recognized as a vital climate forcer in the atmosphere. Amplification of light absorption can occur due to coatings on BC during atmospheric aging, an effect that remains uncertain in accessing the radiative forcing of BC. Existing studies on the absorption enhancement factor (Eabs) have poor coverage on both seasonal and diurnal scales. In this study, we applied a recently developed minimum R squared (MRS) method, which can cover both seasonal and diurnal scales, for Eabs quantification. Using field measurement data in Guangzhou, the aims of this study are to explore (1) the temporal dynamics of BC optical properties at seasonal (wet season, 31 July–10 September; dry season, 15 November 2017–15 January 2018) and diel scales (1 h time resolution) in the typical urban environment and (2) the influencing factors on Eabs temporal variability. Mass absorption efficiency at 520 nm by primary aerosols (MAEp520) determined by the MRS method exhibited a strong seasonality (8.6 m2 g−1 in the wet season and 16.8 m2 g−1 in the dry season). Eabs520 was higher in the wet season (1.51±0.50) and lower in the dry season (1.29±0.28). Absorption Ångström exponent (AAE470–660) in the dry season (1.46±0.12) was higher than that in the wet season (1.37±0.10). Collective evidence showed that the active biomass burning (BB) in the dry season effectively altered the optical properties of BC, leading to elevated MAE, MAEp and AAE in the dry season compared to those in the wet season. Diurnal Eabs520 was positively correlated with AAE470–660 (R2=0.71) and negatively correlated with the AE33 aerosol loading compensation parameter (k) (R2=0.74) in the wet season, but these correlations were significantly weaker in the dry season, which may be related to the impact of BB. This result suggests that during the wet season, the lensing effect was more likely dominating the AAE diurnal variability rather than the contribution from brown carbon (BrC). Secondary processing can affect Eabs diurnal dynamics. The Eabs520 exhibited a clear dependency on the ratio of secondary organic carbon to organic carbon (SOC∕OC), confirming the contribution of secondary organic aerosols to Eabs; Eabs520 correlated well with nitrate and showed a clear dependence on temperature. This new finding implies that gas–particle partitioning of semivolatile compounds may potentially play an important role in steering the diurnal fluctuation of Eabs520. In the dry season, the diurnal variability in Eabs520 was associated with photochemical aging as evidenced by the good correlation (R2=0.69) between oxidant concentrations (Ox=O3+NO2) and Eabs520.

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