Intense dust and extremely fresh biomass burning outbreak in Barcelona, Spain: characterization of their optical properties and estimation of their direct radiative forcing

Abstract. Atmospheric black carbon (BC) is a leading climate warming agent, yet uncertainties on the global direct radiative forcing (DRF) remain large. Here we expand a global model simulation (GEOS-Chem) of BC to include the absorption enhancement associated with BC coating and separately treat both the aging and physical properties of fossil-fuel and biomass-burning BC. In addition we develop a global simulation of brown carbon (BrC) from both secondary (aromatic) and primary (biomass burning and biofuel) sources. The global mean lifetime of BC in this simulation (4.4 days) is substantially lower compared to the AeroCom I model means (7.3 days), and as a result, this model captures both the mass concentrations measured in near-source airborne field campaigns (ARCTAS, EUCAARI) and surface sites within 30%, and in remote regions (HIPPO) within a factor of 2. We show that the new BC optical properties together with the inclusion of BrC reduces the model bias in absorption aerosol optical depth (AAOD) at multiple wavelengths by more than 50% at AERONET sites worldwide. However our improved model still underestimates AAOD by a factor of 1.4 to 2.8 regionally, with the largest underestimates in regions influenced by fire. Using the RRTMG model integrated with GEOS-Chem we estimate that the all-sky top-of-atmosphere DRF of BC is +0.13 Wm−2 (0.08 Wm−2 from anthropogenic sources and 0.05 Wm−2 from biomass burning). If we scale our model to match AERONET AAOD observations we estimate the DRF of BC is +0.21 Wm−2, with an additional +0.11 Wm−2 of warming from BrC. Uncertainties in size, optical properties, observations, and emissions suggest an overall uncertainty in BC DRF of −80%/+140%. Our estimates are at the lower end of the 0.2–1.0 Wm−2 range from previous studies, and substantially less than the +0.6 Wm−2 DRF estimated in the IPCC 5th Assessment Report. We suggest that the DRF of BC has previously been overestimated due to the overestimation of the BC lifetime (including the effect on the vertical profile) and the incorrect attribution of BrC absorption to BC.

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Exploiting simultaneous observational constraints on mass and absorption to estimate the global direct radiative forcing of black carbon and brown carbon

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-14-17527-2014 ◽

2014 ◽

Vol 14 (11) ◽

pp. 17527-17583 ◽

Cited By ~ 7

Author(s):

X. Wang ◽

C. L. Heald ◽

D. A. Ridley ◽

J. P. Schwarz ◽

J. R. Spackman ◽

...

Keyword(s):

Optical Properties ◽

Black Carbon ◽

Biomass Burning ◽

Radiative Forcing ◽

Model Simulation ◽

Anthropogenic Sources ◽

Absorption Enhancement ◽

Brown Carbon ◽

Direct Radiative Forcing ◽

Improved Model

Abstract. Atmospheric black carbon (BC) is a leading climate warming agent, yet uncertainties on the global direct radiative forcing (DRF) remain large. Here we expand a global model simulation (GEOS-Chem) of BC to include the absorption enhancement associated with BC coating and separately treat both the aging and physical properties of fossil fuel and biomass burning BC. In addition we develop a global simulation of Brown Carbon (BrC) from both secondary (aromatic) and primary (biomass burning and biofuel) sources. The global mean lifetime of BC in this simulation (4.4 days) is substantially lower compared to the AeroCom I model means (7.3 days), and as a result, this model captures both the mass concentrations measured in near-source airborne field campaigns (ARCTAS, EUCAARI) and surface sites within 30%, and in remote regions (HIPPO) within a factor of two. We show that the new BC optical properties together with the inclusion of BrC reduces the model bias in Absorption Aerosol Optical Depth (AAOD) at multiple wavelengths by more than 50% at AERONET sites worldwide. However our improved model still underestimates AAOD by a factor of 1.4 to 2.8 regionally, with largest underestimates in regions influenced by fire. Using the RRTMG model integrated with GEOS-Chem we estimate that the all-sky top-of-atmosphere DRF of BC is +0.13 W m−2 (0.08 W m−2 from anthropogenic sources and 0.05 W m−2 from biomass burning). If we scale our model to match AERONET AAOD observations we estimate the DRF of BC is +0.21 W m−2, with an additional +0.11 W m−2 of warming from BrC. Uncertainties in size, optical properties, observations, and emissions suggest an overall uncertainty in BC DRF of −80% / +140%. Our estimates are at the lower end of the 0.2–1.0 W m−2 range from previous studies, and substantially less than the +0.6 W m−2 DRF estimated in the IPCC 5th Assessment Report. We suggest that the DRF of BC has previously been overestimated due to the overestimation of the BC lifetime and the incorrect attribution of BrC absorption to BC.

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Modelling the optical properties of fresh biomass burning aerosol produced in a smoke chamber: results from the EFEU campaign

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-7-12657-2007 ◽

2007 ◽

Vol 7 (4) ◽

pp. 12657-12686 ◽

Cited By ~ 2

Author(s):

K. Hungershöfer ◽

K. Zeromskiene ◽

Y. Iinuma ◽

G. Helas ◽

J. Trentmann ◽

...

Keyword(s):

Optical Properties ◽

Biomass Burning ◽

Atmospheric Chemistry ◽

Absorption Efficiency ◽

Max Planck ◽

Fresh Biomass ◽

Biomass Burning Aerosol ◽

Smoke Chamber ◽

The Impact ◽

Mass Absorption Efficiency

Abstract. A better characterisation of the optical properties of biomass burning aerosol as a function of the burning conditions is required in order to quantify their effects on climate and atmospheric chemistry. Controlled laboratory combustion experiments with different fuel types were carried out at the combustion facility of the Max Planck Institute for Chemistry (Mainz, Germany) as part of the 'Impact of Vegetation Fires on the Composition and Circulation of the Atmosphere' (EFEU) project. Using the measured size distributions as well as mass scattering and absorption efficiencies, Mie calculations provided mean effective refractive indices of 1.60−0.010i and 1.56−0.010i (λ=0.55 μm) for smoke particles emitted from the combustion of savanna grass and an African hardwood (musasa), respectively. The relatively low imaginary parts suggest that the light-absorbing carbon of the investigated fresh biomass burning aerosol is only partly graphitized, resulting in strongly scattering and less absorbing particles. While the observed variability in mass scattering efficiencies was consistent with changes in particle size, the changes in the mass absorption efficiency can only be explained, if the chemical composition of the particles varies with combustion conditions.

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Seasonal Variation of Aerosol Direct Radiative Forcing and Optical Properties Estimated from Ground-Based Solar Radiation Measurements

Journal of the Atmospheric Sciences ◽

10.1175/1520-0469(2004)061<0057:svoadr>2.0.co;2 ◽

2004 ◽

Vol 61 (1) ◽

pp. 57-72 ◽

Cited By ~ 13

Author(s):

Tomoaki Nishizawa ◽

Shoji Asano ◽

Akihiro Uchiyama ◽

Akihiro Yamazaki

Keyword(s):

Optical Properties ◽

Seasonal Variation ◽

Solar Radiation ◽

Radiative Forcing ◽

Direct Radiative Forcing ◽

Radiation Measurements

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Intercomparison of biomass burning aerosol optical properties from in situ and remote-sensing instruments in ORACLES-2016

Atmospheric Chemistry and Physics ◽

10.5194/acp-19-9181-2019 ◽

2019 ◽

Vol 19 (14) ◽

pp. 9181-9208 ◽

Cited By ~ 16

Author(s):

Kristina Pistone ◽

Jens Redemann ◽

Sarah Doherty ◽

Paquita Zuidema ◽

Sharon Burton ◽

...

Keyword(s):

Optical Properties ◽

Case Studies ◽

Biomass Burning ◽

Radiative Forcing ◽

Measurement Techniques ◽

Single Scattering ◽

Single Scattering Albedo ◽

Aerosol Optical Properties ◽

Biomass Burning Aerosol

Abstract. The total effect of aerosols, both directly and on cloud properties, remains the biggest source of uncertainty in anthropogenic radiative forcing on the climate. Correct characterization of intensive aerosol optical properties, particularly in conditions where absorbing aerosol is present, is a crucial factor in quantifying these effects. The southeast Atlantic Ocean (SEA), with seasonal biomass burning smoke plumes overlying and mixing with a persistent stratocumulus cloud deck, offers an excellent natural laboratory to make the observations necessary to understand the complexities of aerosol–cloud–radiation interactions. The first field deployment of the NASA ORACLES (ObseRvations of Aerosols above CLouds and their intEractionS) campaign was conducted in September of 2016 out of Walvis Bay, Namibia. Data collected during ORACLES-2016 are used to derive aerosol properties from an unprecedented number of simultaneous measurement techniques over this region. Here, we present results from six of the eight independent instruments or instrument combinations, all applied to measure or retrieve aerosol absorption and single-scattering albedo. Most but not all of the biomass burning aerosol was located in the free troposphere, in relative humidities typically ranging up to 60 %. We present the single-scattering albedo (SSA), absorbing and total aerosol optical depth (AAOD and AOD), and absorption, scattering, and extinction Ångström exponents (AAE, SAE, and EAE, respectively) for specific case studies looking at near-coincident and near-colocated measurements from multiple instruments, and SSAs for the broader campaign average over the month-long deployment. For the case studies, we find that SSA agrees within the measurement uncertainties between multiple instruments, though, over all cases, there is no strong correlation between values reported by one instrument and another. We also find that agreement between the instruments is more robust at higher aerosol loading (AOD400>0.4). The campaign-wide average and range shows differences in the values measured by each instrument. We find the ORACLES-2016 campaign-average SSA at 500 nm (SSA500) to be between 0.85 and 0.88, depending on the instrument considered (4STAR, AirMSPI, or in situ measurements), with the interquartile ranges for all instruments between 0.83 and 0.89. This is consistent with previous September values reported over the region (between 0.84 and 0.90 for SSA at 550nm). The results suggest that the differences observed in the campaign-average values may be dominated by instrument-specific spatial sampling differences and the natural physical variability in aerosol conditions over the SEA, rather than fundamental methodological differences.

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