scholarly journals Biomass burning aerosols in most climate models are too absorbing

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Hunter Brown ◽  
Xiaohong Liu ◽  
Rudra Pokhrel ◽  
Shane Murphy ◽  
Zheng Lu ◽  
...  

AbstractUncertainty in the representation of biomass burning (BB) aerosol composition and optical properties in climate models contributes to a range in modeled aerosol effects on incoming solar radiation. Depending on the model, the top-of-the-atmosphere BB aerosol effect can range from cooling to warming. By relating aerosol absorption relative to extinction and carbonaceous aerosol composition from 12 observational datasets to nine state-of-the-art Earth system models/chemical transport models, we identify varying degrees of overestimation in BB aerosol absorptivity by these models. Modifications to BB aerosol refractive index, size, and mixing state improve the Community Atmosphere Model version 5 (CAM5) agreement with observations, leading to a global change in BB direct radiative effect of −0.07 W m−2, and regional changes of −2 W m−2 (Africa) and −0.5 W m−2 (South America/Temperate). Our findings suggest that current modeled BB contributes less to warming than previously thought, largely due to treatments of aerosol mixing state.

2009 ◽  
Vol 9 (19) ◽  
pp. 7643-7655 ◽  
Author(s):  
B. I. Magi

Abstract. This study characterizes the aerosol over extratropical and tropical southern Africa during the biomass burning season by presenting an aerosol mass apportionment and aerosol optical properties. Carbonaceous aerosol species account for 54% and 83% of the extratropical and tropical aerosol mass, respectively, which is consistent with the fact that the major source of particulate matter in southern Africa is biomass burning. This mass apportionment implies that carbonaceous species in the form of organic carbon (OC) and black carbon (BC) play a critical role in the aerosol optical properties. By combining the in situ measurements of aerosol mass concentrations with concurrent measurements of aerosol optical properties at a wavelength of 550 nm, it is shown that 80–90% of the aerosol scattering is due to carbonaceous aerosol, and the derived mass scattering cross sections (MSC) for OC and BC are 3.9±0.6 m2/g and 1.6±0.2 m2/g, respectively. Derived values of mass absorption cross sections (MAC) for OC and BC are 0.7±0.6 m2/g and 8.2±1.1 m2/g, respectively. The values of MAC imply that ~26% of the aerosol absorption in southern Africa is due to OC, with the remainder due to BC. The results in this study provide important constraints for aerosol properties in a region dominated by biomass burning and should be integrated into climate models to improve aerosol simulations.


2020 ◽  
Vol 20 (19) ◽  
pp. 11201-11221 ◽  
Author(s):  
Jonathan W. Taylor ◽  
Huihui Wu ◽  
Kate Szpek ◽  
Keith Bower ◽  
Ian Crawford ◽  
...  

Abstract. The optical properties of black carbon (BC) are a major source of uncertainty in regional and global climate studies. In the past, detailed investigation of BC absorption has been hampered by systematic biases in the measurement instrumentation. We present airborne measurements of aerosol absorption and black carbon microphysical properties in highly aged biomass burning plumes measured 4–8 d from their source over the southeast Atlantic Ocean during CLARIFY-2017, using a suite of novel photoacoustic spectrometers to measure aerosol absorption at 405, 514, and 655 nm and a single-particle soot photometer to measure the BC mass concentration, size, and mixing state. These measurements are of sufficient quality and detail to provide constraint on optical schemes used in climate models for the first time in biomass burning plumes far from their source – an aerosol environment that is one of the most important climatically. The average absorption Ångström exponents (AAE) were 1.38 over the wavelength range from 405 to 514 nm and 0.88 over the range from 514 to 655 nm, suggesting that brown carbon (BrC) contributed to 11±2 % of absorption at 405 nm. The effective organic aerosol (OA) mass absorption coefficient (MAC) was 0.31±0.09 m2 g−1 at 405 nm. The BC particles were universally thickly coated, and almost no externally mixed BC particles were detected. The average MAC of BC was 20±4, 15±3, and 12±2 m2g−1 at wavelengths of 405, 514, and 655 nm respectively, with equivalent absorption enhancements of around 1.85±0.45 at all three wavelengths, suggesting that the thick coatings acted as a lens that enhanced light absorption by the BC. We compared the measured MAC and AAE values with those calculated using several optical models and absorption parameterisations that took the measured BC mass and mixing state as inputs. Homogeneous grey-sphere Mie models were only able to replicate MAC for some low (real and imaginary) values of the complex BC refractive index (mBC) at the shortest wavelength, but they would have to use unrealistically low values of mBC to accurately replicate the AAE. A core–shell Mie model was able to generate good agreement for MAC in the green–red end of the visible spectrum for most values of mBC. However, there are no possible values of mBC that produce MAC values that agree with our observations at all three wavelengths, due to a wavelength-dependent underestimation of the MAC of the underlying BC core. Four semiempirical parameterisations from the literature were also tested, linking the BC mixing state to either the MAC or absorption enhancement. Two of these schemes produced results that agreed within a few percent with the measured MAC at all three wavelengths, and the AAE agreed well when discounting the effects of BrC. Our results uniquely demonstrate the validity of absorption parameterisations, as well as the failings of Mie calculations, in this highly aged environment. We recommend that future work should conduct similar analyses in environments where BC has different properties; future studies should also investigate the impact of implementing these types of schemes within climate models as well as the impact of developing equivalent schemes for light scattering by soot particles at visible wavelengths.


2020 ◽  
Author(s):  
Jonathan W. Taylor ◽  
Huihui Wu ◽  
Kate Szpek ◽  
Keith Bower ◽  
Ian Crawford ◽  
...  

Abstract. The optical properties of black carbon (BC) are a major source of uncertainty in regional and global climate studies. In the past, detailed investigation of BC absorption has been hampered by systematic biases in the measurement instrumentation. We present airborne measurements of aerosol absorption and black carbon microphysical properties in highly aged biomass burning plumes measured over the southeast Atlantic ocean during CLARIFY-2017, using a suite of novel photoacoustic spectrometers to measure 5 aerosol absorption at 405 nm, 514 nm, and 655 nm, and a single-particle soot photometer to measure the BC mass concentration, size, and mixing state. These measurements are of sufficient quality and detail to provide constraint on optical schemes used in climate models for the first time in biomass burning plumes far from source, an aerosol environment that is one of the most important climatically. The average absorption Angstrom exponents (AAE) were 1.39 over the wavelength range 405–514 nm, and 0.94 over the range 514–655 nm, suggesting brown carbon (BrC) contributed to 10 ± 2 % of absorption at 405 nm. The effective OA mass absorption coefficient (MAC) was 0.27 ± 0.08 m2 g−1 at 405 nm. The BC particles were universally thickly-coated, and almost no externally-mixed BC particles were detected. The MAC of BC was also high, with equivalent absorption enhancements of around 1.8 at all three wavelengths, suggesting that the thick coatings acted as a lens that enhanced light absorption by the BC. We compared the measured MAC and AAE values with those calculated using several optical models and absorption parametrisations that took the measured BC mass and mixing state as inputs. Homogeneous grey sphere Mie models were only able to replicate MAC for some low (real and imaginary) values of the complex BC refractive index (mBC) at the shortest wavelength, but they would have to use unrealistically low values of mBC to accurately replicate AAE. A core/shell Mie model was able to generate good agreement for MAC in the green/red end of the visible spectrum for most values of mBC. However, there are no possible values of mBC that produce MAC values that agree with our observations at all three wavelengths, due to a wavelength-dependent underestimation of the MAC of the underlying BC core. Four semi-empirical parametrisations from literature were also tested, linking BC mixing state to either MAC or absorption enhancement. Two of these schemes produced results that agreed within a few percent of the measured MAC at all three wavelengths, and AAE agreed well when discounting the effects of BrC. Our results uniquely demonstrate the validity of absorption parametrisations, as well as the failings of Mie calculations, in this highly aged environment. We recommend future work should conduct similar analyses in environments where BC has different properties, and investigate the impact of implementing these types of schemes within climate models, as well as developing equivalent schemes for light scattering by soot particles at visible wavelengths.


2012 ◽  
Vol 12 (21) ◽  
pp. 10239-10255 ◽  
Author(s):  
L. T. Padró ◽  
R. H. Moore ◽  
X. Zhang ◽  
N. Rastogi ◽  
R. J. Weber ◽  
...  

Abstract. Aerosol composition and mixing state near anthropogenic sources can be highly variable and can challenge predictions of cloud condensation nuclei (CCN). The impacts of chemical composition on CCN activation kinetics is also an important, but largely unknown, aspect of cloud droplet formation. Towards this, we present in-situ size-resolved CCN measurements carried out during the 2008 summertime August Mini Intensive Gas and Aerosol Study (AMIGAS) campaign in Atlanta, GA. Aerosol chemical composition was measured by two particle-into-liquid samplers measuring water-soluble inorganic ions and total water-soluble organic carbon. Size-resolved CCN data were collected using the Scanning Mobility CCN Analysis (SMCA) method and were used to obtain characteristic aerosol hygroscopicity distributions, whose breadth reflects the aerosol compositional variability and mixing state. Knowledge of aerosol mixing state is important for accurate predictions of CCN concentrations and that the influence of an externally-mixed, CCN-active aerosol fraction varies with size from 31% for particle diameters less than 40 nm to 93% for accumulation mode aerosol during the day. Assuming size-dependent aerosol mixing state and size-invariant chemical composition decreases the average CCN concentration overprediction (for all but one mixing state and chemical composition scenario considered) from over 190–240% to less than 20%. CCN activity is parameterized using a single hygroscopicity parameter, κ, which averages to 0.16 ± 0.07 for 80 nm particles and exhibits considerable variability (from 0.03 to 0.48) throughout the study period. Particles in the 60–100 nm range exhibited similar hygroscopicity, with a κ range for 60 nm between 0.06–0.076 (mean of 0.18 ± 0.09). Smaller particles (40 nm) had on average greater κ, with a range of 0.20–0.92 (mean of 0.3 ± 0.12). Analysis of the droplet activation kinetics of the aerosol sampled suggests that most of the CCN activate as rapidly as calibration aerosol, suggesting that aerosol composition exhibits a minor (if any) impact on CCN activation kinetics.


2011 ◽  
Vol 11 (3) ◽  
pp. 7291-7319 ◽  
Author(s):  
H. Jethva ◽  
O. Torres

Abstract. We provide satellite-based evidence of the spectral dependence of absorption in biomass burning aerosols over South America using near-UV measurements made by Ozone Monitoring Instrument (OMI) during 2005–2007. Currently, OMAERUV aerosol algorithm characterizes carbonaceous aerosol as "gray" aerosol, meaning no wavelength dependence in aerosol absorption. With this assumption, OMI-derived aerosol optical depth (AOD) is found to be over-estimated significantly compared to that of AERONET at several sites during intense biomass burning events (August–September). The assumption on height of aerosols and other parameters seem to be reasonable and unable to explain large discrepancy in the retrieval. The specific ground-based studies have revealed strong spectral dependence in aerosol absorption in the near-UV region that indicates the presence of organic carbon. A new set of OMI aerosol retrieval with assumed wavelength-dependent aerosol absorption in the near-UV region (Absorption Angstrom Exponent λ−2.5 to −3.0) provided much improved retrieval of AOD with significantly reduced bias. Also, the new retrieval of single-scattering albedo is in better agreement with those of AERONET within the uncertainties (Δω=±0.03). The new smoke aerosol model was also found to be valid over the biomass burning region of central Africa and northern India. Together with suggesting vast improvement in the retrieval of aerosol properties from OMI, present study demonstrates the near-UV capabilities of OMI in separating aerosols containing organics from pure black carbon through OMI-AERONET integrated measurements.


Atmosphere ◽  
2019 ◽  
Vol 10 (4) ◽  
pp. 168 ◽  
Author(s):  
Robin Stevens ◽  
Ashu Dastoor

Aerosol mixing state significantly affects concentrations of cloud condensation nuclei (CCN), wet removal rates, thermodynamic properties, heterogeneous chemistry, and aerosol optical properties, with implications for human health and climate. Over the last two decades, significant research effort has gone into finding computationally-efficient methods for representing the most important aspects of aerosol mixing state in air pollution, weather prediction, and climate models. In this review, we summarize the interactions between mixing-state and aerosol hygroscopicity, optical properties, equilibrium thermodynamics and heterogeneous chemistry. We focus on the effects of simplified assumptions of aerosol mixing state on CCN concentrations, wet deposition, and aerosol absorption. We also summarize previous approaches for representing aerosol mixing state in atmospheric models, and we make recommendations regarding the representation of aerosol mixing state in future modelling studies.


2019 ◽  
Author(s):  
Martin de Graaf ◽  
Ruben Schulte ◽  
Fanny Peers ◽  
Fabien Waquet ◽  
L. Gijsbert Tilstra ◽  
...  

Abstract. The Direct Radiative Effect (DRE) of aerosols above clouds has been found to be significant over the south-east Atlantic Ocean during the African biomass burning season due to elevated smoke layers absorbing radiation above the cloud deck. So far, global climate models have been unsuccessful in reproducing the high DRE values measured by various satellite instruments. Meanwhile, the radiative effects by aerosols have been identified as the largest source of uncertainty in global climate models. In this paper, three independent satellite datasets of DRE during the biomass burning season in 2006 are compared to constrain the south-east Atlantic radiation budget. The DRE of aerosols above clouds is derived from the spectrometer SCIAMACHY, the polarimeter POLDER, and from collocated measurements by the spectrometer OMI and imager MODIS. All three confirm the high DRE values during the biomass season, underlining the relevance of local aerosol effects. Differences between the instruments can be attributed mainly to sampling issues. When these are accounted for, the remaining differences can be completely explained by the higher cloud optical thickness derived from POLDER compared to the other instruments. Additionally, a neglect of AOT at SWIR wavelengths in the method used for SCIAMACHY and OMI/MODIS accounts for 26 % of the difference between POLDER and OMI/MODIS DRE.


2020 ◽  
Vol 47 (19) ◽  
Author(s):  
Cyrielle Denjean ◽  
Joel Brito ◽  
Quentin Libois ◽  
Marc Mallet ◽  
Thierry Bourrianne ◽  
...  

2017 ◽  
Vol 98 (5) ◽  
pp. 971-980 ◽  
Author(s):  
Laura Fierce ◽  
Nicole Riemer ◽  
Tami C. Bond

Abstract Atmospheric aerosols affect Earth’s energy budget, and hence its climate, by scattering and absorbing solar radiation and by altering the radiative properties and the lifetime of clouds. These two major aerosol effects depend on the optical properties and the cloud-nucleating ability of individual particles, which, in turn, depend on the distribution of components among individual particles, termed the “aerosol mixing state.” Global models have moved toward including aerosol schemes to represent the evolution of particle characteristics, but individual particle properties cannot be resolved in global-scale simulations. Instead, models approximate the aerosol mixing state. The errors in climate-relevant aerosol properties introduced by such approximations may be large but have not yet been well quantified. This paper quantitatively addresses the question of to what extent the aerosol mixing state must be resolved to adequately represent the optical properties and cloud-nucleating properties of particle populations. Using a detailed benchmarking model to simulate gas condensation and particle coagulation, we show that, after the particles evolve in the atmosphere, simple mixing-state representations are sufficient for modeling cloud condensation nuclei concentrations, and we quantify the mixing time scale that characterizes this transformation. In contrast, a detailed representation of the mixing state is required to model aerosol light absorption, even for populations that are fully mixed with respect to their hygroscopic properties.


2011 ◽  
Vol 11 (12) ◽  
pp. 32723-32768 ◽  
Author(s):  
L. T. Padró ◽  
R. H. Moore ◽  
X. Zhang ◽  
N. Rastogi ◽  
R. J. Weber ◽  
...  

Abstract. Aerosol composition and mixing state near anthropogenic sources can be highly variable and can challenge predictions of cloud condensation nuclei (CCN). We present in-situ size-resolved CCN measurements to quantify this predictive uncertainty, which were carried out during the 2008 summertime August Mini Intensive Gas and Aerosol Study (AMIGAS) campaign in Atlanta, GA. Aerosol chemical composition was measured by two particle-into-liquid samplers measuring water-soluble inorganic ions and total water-soluble organic carbon. Size-resolved CCN data were collected using the Scanning Mobility CCN Analysis (SMCA) method and were used to obtain characteristic aerosol hygroscopicity distributions, whose breadth reflects the aerosol compositional variability and mixing state. We find that knowledge of aerosol mixing state is important for accurate predictions of CCN concentrations and that the influence of an externally-mixed, non-CCN-active aerosol fraction varies with size from 31% for particle diameters less than 40 nm to 93% for accumulation mode aerosol during the day. This is likely indicative of the interactions between biogenic and anthropogenic emissions which contribute to the formation and transformation of aerosols in this heterogeneous environment. Assuming size-dependent aerosol mixing state and size-invariant chemical composition decreased the average CCN concentration overprediction from greater than 50–200% to less than 20%. CCN activity was parameterized using a single hygroscopicity parameter, κ, which averaged 0.16 ± 0.07 for 80 nm particles and exhibited considerable variability (range: 0.03–0.48) throughout the study period.


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