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

2016 ◽  
Vol 16 (7) ◽  
pp. 4693-4706 ◽  
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.

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

2015 ◽  
Vol 15 (22) ◽  
pp. 33555-33582 ◽  
Author(s):  
M. D. Willis ◽  
R. M. Healy ◽  
N. Riemer ◽  
M. West ◽  
J. 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 in two distinct particle types: HOA-rich and BC-rich particles. The average mass fraction of black carbon in HOA-rich and BC-rich particles was 0.02–0.08 and 0.72–0.93, 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.

scholarly journals Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the UK

2011 ◽  
Vol 11 (5) ◽  
pp. 14991-15027 ◽  
Author(s):  
G. R. McMeeking ◽  
W. T. Morgan ◽  
M. Flynn ◽  
E. J. Highwood ◽  
K. Turnbull ◽  
...  
Keyword(s):  
Optical Properties ◽  
Black Carbon ◽  
Radiative Forcing ◽  
Organic Aerosols ◽  
Mixing State ◽  
Aerosol Composition ◽  
Air Masses ◽  
Aerosol Mass ◽  
The Uk ◽  
Urban Plumes

Abstract. Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the UK. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA observed in urban plumes compared to regional aerosol (0.85 versus 0.9–0.95). We attribute these differences to the presence of relatively rapidly formed secondary aerosol, primarily OOA and ammonium nitrate, which must be taken into account in radiative forcing calculations.

scholarly journals Closure on the single scattering albedo in the WRF-Chem framework using data from the MILAGRO campaign

2009 ◽  
Vol 9 (1) ◽  
pp. 5009-5054
Author(s):  
J. C. Barnard ◽  
J. D. Fast ◽  
G. Paredes-Miranda ◽  
W. P. Arnott
Keyword(s):  
Optical Properties ◽  
Black Carbon ◽  
Chemical Properties ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Aerosol Optical Properties ◽  
Mean Values ◽  
Coarse Mode ◽  
Fine Mode ◽  
Using Data

Abstract. Data from the MILAGRO field campaign, which took place in the Mexico City Metropolitan Area (MCMA) during March 2006, is used to perform a closure experiment between aerosol chemical properties and aerosol optical properties. Measured aerosol chemical properties, obtained from the MILAGRO T1 site, are fed to two different "chemical to optical properties" modules. One module uses a sectional approach and is identical to that used in the WRF-Chem model, while the other is based on a modal approach. This modal code is employed as an independent check on the WRF-Chem module. Both modules compute aerosol optical properties and, in particular, the single-scattering albedo, ϖ0, as a function of time. The single-scattering albedos are compared to independent measurements obtained from a photoacoustic spectrometer (PAS). Because chemical measurements of the aerosol coarse mode were not available, and the inlet of the PAS could not ingest aerosols larger than about 2 to 3 μm, we focus here on the fine-mode ϖ0. At 870 nm, the wavelength of the PAS measurements, the agreement between the computed (modal and WRF-Chem) and observed fine-mode ϖ0, averaged over the course of the campaign, is reasonably good. The observed ϖ0 value is 0.77, while for both modules, the calculated value was 0.75 resulting in a difference of 0.02 between observations and both computational approaches. This difference is less than the uncertainty of the observed ϖ0 values (6%, or 0.05), and therefore "closure" is achieved, at least for mean values. After adjusting some properties of black carbon absorption and mass concentration within plausible uncertainty limits, the two modules simulate well the diurnal variation of ϖ0, and the absorption coefficient, Babs, but are less successful in calculating the variation of the scattering coefficient, Bscat. This difficulty is probably caused by the presence of larger particles during the day when windblown dust is ubiquitous; this dust likely increases the proportion of large particles introduced into the PAS. The dust also contributes to a very large aerosol mass loading in the coarse mode, and neglect of the coarse mode may cause significant errors, estimated to be as large as 0.07, in the calculation and measurement of ambient ϖ0. Finally, the observed ϖ0 is compared to the ϖ0 computed by the full WRF-Chem model, which includes prognostic aerosol chemistry. Unlike the results discussed above, a comparison between observed and simulated ϖ0 values reveals major differences. This large discrepancy is probably due, in part, to poor characterization of emissions near the T1 site, particularly black carbon emissions.

scholarly journals Black carbon aerosol mixing state, organic aerosols and aerosol optical properties over the United Kingdom

2011 ◽  
Vol 11 (17) ◽  
pp. 9037-9052 ◽  
Author(s):  
G. R. McMeeking ◽  
W. T. Morgan ◽  
M. Flynn ◽  
E. J. Highwood ◽  
K. Turnbull ◽  
...  
Keyword(s):  
Optical Properties ◽  
United Kingdom ◽  
Radiative Forcing ◽  
Organic Aerosols ◽  
Mixing State ◽  
Aerosol Composition ◽  
Air Masses ◽  
The United Kingdom ◽  
Aerosol Mass ◽  
Urban Plumes

Abstract. Black carbon (BC) aerosols absorb sunlight thereby leading to a positive radiative forcing and a warming of climate and can also impact human health through their impact on the respiratory system. The state of mixing of BC with other aerosol species, particularly the degree of internal/external mixing, has been highlighted as a major uncertainty in assessing its radiative forcing and hence its climate impact, but few in situ observations of mixing state exist. We present airborne single particle soot photometer (SP2) measurements of refractory BC (rBC) mass concentrations and mixing state coupled with aerosol composition and optical properties measured in urban plumes and regional pollution over the United Kingdom. All data were obtained using instrumentation flown on the UK's BAe-146-301 large Atmospheric Research Aircraft (ARA) operated by the Facility for Airborne Atmospheric Measurements (FAAM). We measured sub-micron aerosol composition using an aerosol mass spectrometer (AMS) and used positive matrix factorization to separate hydrocarbon-like (HOA) and oxygenated organic aerosols (OOA). We found a higher number fraction of thickly coated rBC particles in air masses with large OOA relative to HOA, higher ozone-to-nitrogen oxides (NOx) ratios and large concentrations of total sub-micron aerosol mass relative to rBC mass concentrations. The more ozone- and OOA-rich air masses were associated with transport from continental Europe, while plumes from UK cities had higher HOA and NOx and fewer thickly coated rBC particles. We did not observe any significant change in the rBC mass absorption efficiency calculated from rBC mass and light absorption coefficients measured by a particle soot absorption photometer despite observing significant changes in aerosol composition and rBC mixing state. The contributions of light scattering and absorption to total extinction (quantified by the single scattering albedo; SSA) did change for different air masses, with lower SSA observed in urban plumes compared to regional aerosol (0.85 versus 0.9–0.95). We attribute these differences to the presence of relatively rapidly formed secondary aerosol, primarily OOA and ammonium nitrate, which must be taken into account in radiative forcing calculations.

A new airborne aerosol sampling system: development, validation, and application in vertical measurement of black carbon mixing state

2021 ◽  
Author(s):  
Shaowen Zhu ◽  
Nan Ma ◽  
Linhong Xie ◽  
Nan Lu ◽  
Minglu Li ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Black Carbon ◽  
System Development ◽  
Chemical Properties ◽  
Aerosol Sampling ◽  
Tethered Balloon ◽  
Mixing State ◽  
Sampling System ◽  
Aerosol Mass ◽  
Aerial Vehicle

&lt;p&gt;Vertical measurements of aerosol physical-chemical properties have important significance for better addressing the environment and climate effects of atmospheric aerosol. Traditional in-situ vertical observations of those properties are mainly based on aircraft platforms which are costly and restrictive, and not applicable for near-ground (&lt;500 m) measurements. Within the boundary layer, tethered balloon and unmanned aerial vehicle (UAV) are ideal observation platforms but cannot carry heavy online aerosol instruments due to payload limitations. In this study, a new lightweight airborne aerosol sampling system is developed for tethered balloon and UAV platform. The system can collect airborne aerosol samples at up to 12 heights with conductive bags, and the samples can be analyzed later by online instruments such as aerosol mass spectrometer and single particle soot photometer (SP2). During an intensive field campaign conducted in Lhasa in summer of 2020, the new developed system was applied together with a SP2 to determine the vertical profile of refractory black carbon (rBC) mixing state. Preliminary results show that most rBC containing particles are external mixture and the proportion of internally mixed rBC increases with height. The vertical profiles of rBC mixing state are affected by surface emissions, the development of atmospheric boundary layer and meteorological conditions.&lt;/p&gt;

scholarly journals Modelling black carbon absorption of solar radiation: combining external and internal mixing assumptions

2019 ◽  
Vol 19 (1) ◽  
pp. 181-204 ◽  
Author(s):  
Gabriele Curci ◽  
Ummugulsum Alyuz ◽  
Rocio Barò ◽  
Roberto Bianconi ◽  
Johannes Bieser ◽  
...  
Keyword(s):  
Optical Properties ◽  
Black Carbon ◽  
Single Scattering ◽  
Single Scattering Albedo ◽  
Absorption Enhancement ◽  
Core Shell ◽  
Mixing State ◽  
Aerosol Optical Properties ◽  
Internal Mixing ◽  
Carbon Absorption

Abstract. An accurate simulation of the absorption properties is key for assessing the radiative effects of aerosol on meteorology and climate. The representation of how chemical species are mixed inside the particles (the mixing state) is one of the major uncertainty factors in the assessment of these effects. Here we compare aerosol optical properties simulations over Europe and North America, coordinated in the framework of the third phase of the Air Quality Model Evaluation International Initiative (AQMEII), to 1 year of AERONET sunphotometer retrievals, in an attempt to identify a mixing state representation that better reproduces the observed single scattering albedo and its spectral variation. We use a single post-processing tool (FlexAOD) to derive aerosol optical properties from simulated aerosol speciation profiles, and focus on the absorption enhancement of black carbon when it is internally mixed with more scattering material, discarding from the analysis scenes dominated by dust. We found that the single scattering albedo at 440 nm (ω0,440) is on average overestimated (underestimated) by 3–5 % when external (core-shell internal) mixing of particles is assumed, a bias comparable in magnitude with the typical variability of the quantity. The (unphysical) homogeneous internal mixing assumption underestimates ω0,440 by ∼14 %. The combination of external and core-shell configurations (partial internal mixing), parameterized using a simplified function of air mass aging, reduces the ω0,440 bias to -1/-3 %. The black carbon absorption enhancement (Eabs) in core-shell with respect to the externally mixed state is in the range 1.8–2.5, which is above the currently most accepted upper limit of ∼1.5. The partial internal mixing reduces Eabs to values more consistent with this limit. However, the spectral dependence of the absorption is not well reproduced, and the absorption Ångström exponent AAE675440 is overestimated by 70–120 %. Further testing against more comprehensive campaign data, including a full characterization of the aerosol profile in terms of chemical speciation, mixing state, and related optical properties, would help in putting a better constraint on these calculations.

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