Aged boreal biomass-burning aerosol size distributions  from BORTAS 2011

Abstract. Biomass-burning aerosols contribute to aerosol radiative forcing on the climate system. The magnitude of this effect is partially determined by aerosol size distributions, which are functions of source fire characteristics (e.g. fuel type, MCE) and in-plume microphysical processing. The uncertainties in biomass-burning emission number–size distributions in climate model inventories lead to uncertainties in the CCN (cloud condensation nuclei) concentrations and forcing estimates derived from these models. The BORTAS-B (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellite) measurement campaign was designed to sample boreal biomass-burning outflow over eastern Canada in the summer of 2011. Using these BORTAS-B data, we implement plume criteria to isolate the characteristic size distribution of aged biomass-burning emissions (aged ~ 1–2 days) from boreal wildfires in northwestern Ontario. The composite median size distribution yields a single dominant accumulation mode with Dpm = 230 nm (number-median diameter) and σ = 1.5, which are comparable to literature values of other aged plumes of a similar type. The organic aerosol enhancement ratios (ΔOA / ΔCO) along the path of Flight b622 show values of 0.09–0.17 μg m−3 ppbv−1 (parts per billion by volume) with no significant trend with distance from the source. This lack of enhancement ratio increase/decrease with distance suggests no detectable net OA (organic aerosol) production/evaporation within the aged plume over the sampling period (plume age: 1–2 days), though it does not preclude OA production/loss at earlier stages. A Lagrangian microphysical model was used to determine an estimate of the freshly emitted size distribution corresponding to the BORTAS-B aged size distributions. The model was restricted to coagulation and dilution processes based on the insignificant net OA production/evaporation derived from the ΔOA / ΔCO enhancement ratios. We estimate that the young-plume median diameter was in the range of 59–94 nm with modal widths in the range of 1.7–2.8 (the ranges are due to uncertainty in the entrainment rate). Thus, the size of the freshly emitted particles is relatively unconstrained due to the uncertainties in the plume dilution rates.

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Aged boreal biomass burning aerosol size distributions from BORTAS 2011

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-14-24349-2014 ◽

2014 ◽

Vol 14 (17) ◽

pp. 24349-24385 ◽

Cited By ~ 2

Author(s):

K. M. Sakamoto ◽

J. D. Allan ◽

H. Coe ◽

J. W. Taylor ◽

T. J. Duck ◽

...

Keyword(s):

Size Distribution ◽

Biomass Burning ◽

Radiative Forcing ◽

Climate Model ◽

Sampling Period ◽

Characteristic Size ◽

Entrainment Rate ◽

Size Distributions ◽

Eastern Canada ◽

Median Diameter

Abstract. Biomass-burning aerosols contribute to aerosol radiative forcing on the climate system. The magnitude of this effect is partially determined by aerosol size distributions, which are functions of source fire characteristics (e.g. fuel type, MCE) and in-plume microphysical processing. The uncertainties in biomass-burning emission number size-distributions in climate model inventories lead to uncertainties in the CCN concentrations and forcing estimates derived from these models. The BORTAS-B measurement campaign was designed to sample boreal biomass-burning outflow over Eastern Canada in the summer of 2011. Using these BORTAS-B data, we implement plume criteria to isolate the characteristic size-distribution of aged biomass-burning emissions (aged ∼1–2 days) from boreal wildfires in Northwestern Ontario. The composite median size-distribution yields a single dominant accumulation mode with Dpm = 230 nm (number-median diameter), σ = 1.7, which are comparable to literature values of other aged plumes of a similar type. The organic aerosol enhancement ratios (ΔOA / ΔCO) along the path of Flight b622 show values of 0.05–0.18 μg m−3 ppbv−1 with no significant trend with distance from the source. This lack of enhancement ratio increase/decrease with distance suggests no detectable net OA production/evaporation within the aged plume over the sampling period. A Lagrangian microphysical model was used to determine an estimate of the freshly emitted size distribution corresponding to the BORTAS-B aged size-distributions. The model was restricted to coagulation and dilution processes based on the insignificant net OA production/evaporation derived from the ΔOA / ΔCO enhancement ratios. We estimate that the fresh-plume median diameter was in the range of 59–94 nm with modal widths in the range of 1.7–2.8 (the ranges are due to uncertainty in the entrainment rate). Thus, the size of the freshly emitted particles is relatively unconstrained due to the uncertainties in the plume dilution rates.

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

Environmental Science: Atmospheres ◽

10.1039/d1ea00025j ◽

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...

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Effects of near-source coagulation of biomass burning aerosols on global predictions of aerosol size distributions and implications for aerosol radiative effects

Atmospheric Chemistry and Physics ◽

10.5194/acp-19-6561-2019 ◽

2019 ◽

Vol 19 (9) ◽

pp. 6561-6577 ◽

Cited By ~ 11

Author(s):

Emily Ramnarine ◽

John K. Kodros ◽

Anna L. Hodshire ◽

Chantelle R. Lonsdale ◽

Matthew J. Alvarado ◽

...

Keyword(s):

Size Distribution ◽

Biomass Burning ◽

Indirect Effect ◽

Size Distributions ◽

Aerosol Indirect Effect ◽

Fresh Biomass ◽

Biomass Burning Aerosol ◽

Aerosol Radiative Effects ◽

The Impact ◽

Aerosol Radiative

Abstract. Biomass burning is a significant global source of aerosol number and mass. In fresh biomass burning plumes, aerosol coagulation reduces aerosol number and increases the median size of aerosol size distributions, impacting aerosol radiative effects. Near-source biomass burning aerosol coagulation occurs at spatial scales much smaller than the grid boxes of global and many regional models. To date, these models have ignored sub-grid coagulation and instantly mixed fresh biomass burning emissions into coarse grid boxes. A previous study found that the rate of particle growth by coagulation within an individual smoke plume can be approximated using the aerosol mass emissions rate, initial size distribution median diameter and modal width, plume mixing depth, and wind speed. In this paper, we use this parameterization of sub-grid coagulation in the GEOS-Chem–TOMAS (TwO-Moment Aerosol Sectional) global aerosol microphysics model to quantify the impacts on global aerosol size distributions, the direct radiative effect, and the cloud-albedo aerosol indirect effect. We find that inclusion of biomass burning sub-grid coagulation reduces the biomass burning impact on the number concentration of particles larger than 80 nm (a proxy for CCN-sized particles) by 37 % globally. This cloud condensation nuclei (CCN) reduction causes our estimated global biomass burning cloud-albedo aerosol indirect effect to decrease from −76 to −43 mW m−2. Further, as sub-grid coagulation moves mass to sizes with more efficient scattering, including it increases our estimated biomass burning all-sky direct effect from −224 to −231 mW m−2, with assumed external mixing of black carbon and from −188 to −197 mW m−2 and with assumed internal mixing of black carbon with core-shell morphology. However, due to differences in fire and meteorological conditions across regions, the impact of sub-grid coagulation is not globally uniform. We also test the sensitivity of the impact of sub-grid coagulation to two different biomass burning emission inventories to various assumptions about the fresh biomass burning aerosol size distribution and to two different timescales of sub-grid coagulation. The impacts of sub-grid coagulation are qualitatively the same regardless of these assumptions.

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Mexico city aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) – Part 2: Analysis of the biomass burning contribution and the non-fossil carbon fraction

Atmospheric Chemistry and Physics ◽

10.5194/acp-10-5315-2010 ◽

2010 ◽

Vol 10 (12) ◽

pp. 5315-5341 ◽

Cited By ~ 152

Author(s):

A. C. Aiken ◽

B. de Foy ◽

C. Wiedinmyer ◽

P. F. DeCarlo ◽

I. M. Ulbrich ◽

...

Keyword(s):

High Resolution ◽

Mexico City ◽

Biomass Burning ◽

Forest Fires ◽

Organic Aerosol ◽

Total Carbon ◽

Fire Emissions ◽

Fossil Carbon ◽

Aerosol Mass ◽

The Impact

Abstract. Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Aerosol Mass Spectrometer (AMS) and complementary instrumentation. Positive Matrix Factorization (PMF) of high resolution AMS spectra identified a biomass burning organic aerosol (BBOA) component, which includes several large plumes that appear to be from forest fires within the region. Here, we show that the AMS BBOA concentration at T0 correlates with fire counts in the vicinity of Mexico City and that most of the BBOA variability is captured when the FLEXPART model is used for the dispersion of fire emissions as estimated from satellite fire counts. The resulting FLEXPART fire impact factor (FIF) correlates well with the observed BBOA, acetonitrile (CH3CN), levoglucosan, and potassium, indicating that wildfires in the region surrounding Mexico City are the dominant source of BBOA at T0 during MILAGRO. The impact of distant BB sources such as the Yucatan is small during this period. All fire tracers are correlated, with BBOA and levoglucosan showing little background, acetonitrile having a well-known tropospheric background of ~100–150 pptv, and PM2.5 potassium having a background of ~160 ng m−3 (two-thirds of its average concentration), which does not appear to be related to BB sources. We define two high fire periods based on satellite fire counts and FLEXPART-predicted FIFs. We then compare these periods with a low fire period when the impact of regional fires is about a factor of 5 smaller. Fire tracers are very elevated in the high fire periods whereas tracers of urban pollution do not change between these periods. Dust is also elevated during the high BB period but this appears to be coincidental due to the drier conditions and not driven by direct dust emission from the fires. The AMS oxygenated organic aerosol (OA) factor (OOA, mostly secondary OA or SOA) does not show an increase during the fire periods or a correlation with fire counts, FLEXPART-predicted FIFs or fire tracers, indicating that it is dominated by urban and/or regional sources and not by the fires near the MCMA. A new 14C aerosol dataset is presented. Both this new and a previously published dataset of 14C analysis suggest a similar BBOA contribution as the AMS and chemical mass balance (CMB), resulting in 13% higher non-fossil carbon during the high vs. low regional fire periods. The new dataset has ~15% more fossil carbon on average than the previously published one, and possible reasons for this discrepancy are discussed. During the low regional fire period, 38% of organic carbon (OC) and 28% total carbon (TC) are from non-fossil sources, suggesting the importance of urban and regional non-fossil carbon sources other than the fires, such as food cooking and regional biogenic SOA. The ambient BBOA/ΔCH3CN ratio is much higher in the afternoon when the wildfires are most intense than during the rest of the day. Also, there are large differences in the contributions of the different OA components to the surface concentrations vs. the integrated column amounts. Both facts may explain some apparent disagreements between BB impacts estimated from afternoon aircraft flights vs. those from 24-h ground measurements. We show that by properly accounting for the non-BB sources of K, all of the BB PM estimates from MILAGRO can be reconciled. Overall, the fires from the region near the MCMA are estimated to contribute 15–23% of the OA and 7–9% of the fine PM at T0 during MILAGRO, and 2–3% of the fine PM as an annual average. The 2006 MCMA emissions inventory contains a substantially lower impact of the forest fire emissions, although a fraction of these emissions occur just outside of the MCMA inventory area.

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Properties and evolution of biomass burning organic aerosol from Canadian boreal forest fires

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-14-25095-2014 ◽

2014 ◽

Vol 14 (18) ◽

pp. 25095-25138 ◽

Cited By ~ 3

Author(s):

M. D. Jolleys ◽

H. Coe ◽

G. McFiggans ◽

J. W. Taylor ◽

S. J. O'Shea ◽

...

Keyword(s):

Boreal Forest ◽

Biomass Burning ◽

Forest Fires ◽

Spatial Scales ◽

Near Field ◽

Organic Aerosol ◽

Charge Ratio ◽

Far Field ◽

Airborne Measurements ◽

The Impact

Abstract. Airborne measurements of biomass burning organic aerosol (BBOA) from boreal forest fires reveal highly contrasting properties for plumes of different ages. These measurements, performed using an Aerodyne Research Inc. compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) during the BORTAS (quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) experiment in the summer of 2011, have been used to derive normalised excess organic aerosol (OA) mass concentrations (ΔOA/ΔCO), with higher average ratios observed closer to source (0.190 ± 0.010) than in the far-field (0.097 ± 0.002). The difference in ΔOA/ΔCO between fresh and aged plumes is influenced by a change in dominant combustion conditions throughout the campaign. Measurements at source sampled largely smouldering fires, while plumes encountered in the far-field originated from fires occurring earlier in the campaign when fire activity had been more intense. Changing combustion conditions also affect the vertical distribution of biomass burning emissions, as aged plumes from more flaming-dominated fires are injected to higher altitudes of up to 6000 m. Proportional contributions of the mass-to-charge ratio (m/z) 60 and 44 peaks in the AMS mass spectra to the total OA mass (denoted f60 and f44) are used as tracers for primary and oxidized BBOA, respectively. Given the shorter aging times associated with near-field plumes, f44 is lower on average than in more aged, transported plumes. However, high levels of ΔO3/ΔCO and -log(NOx/NOy) close to source indicate that emissions can be subject to very rapid oxidation over short timescales. Conversely, the lofting of plumes into the upper troposphere can lead to the retention of source profiles after transportation over extensive temporal and spatial scales, with f60 also higher on average in aged plumes. Evolution of OA composition with aging is comparable to observations of BB tracers in previous studies, revealing a consistent progression from f60 to f44. The elevated levels of oxygenation in aged plumes, and their association with lower average ΔOA/ΔCO, highlight the influence of OA losses during aging, although there remain considerable uncertainties regarding the role of combustion processes on BBOA production and composition.

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Effects of Near-Source Coagulation of Biomass Burning Aerosols on Global Predictions of Aerosol Size Distributions and Implications for Aerosol Radiative Effects

10.5194/acp-2018-1084 ◽

2018 ◽

Cited By ~ 1

Author(s):

Emily Ramnarine ◽

John K. Kodros ◽

Anna L. Hodshire ◽

Chantelle R. Lonsdale ◽

Matthew J. Alvarado ◽

...

Keyword(s):

Size Distribution ◽

Biomass Burning ◽

Indirect Effect ◽

Size Distributions ◽

Aerosol Indirect Effect ◽

Fresh Biomass ◽

Biomass Burning Aerosol ◽

Aerosol Radiative Effects ◽

The Impact ◽

Aerosol Radiative

Abstract. Biomass burning is a significant global source of aerosol number and mass. In fresh biomass burning plumes, aerosol coagulation reduces aerosol number and increases the median size of aerosol size distributions, impacting aerosol radiative effects. Near-source biomass burning aerosol coagulation occurs at spatial scales much smaller than the grid boxes of global and many regional models. To date, these models ignore sub-grid coagulation and instantly mix fresh biomass burning emissions into coarse grid boxes. A previous study found that the rate of particle growth by coagulation within an individual smoke plume can be approximated using the aerosol mass emissions rate, initial size distribution median diameter and modal width, plume mixing depth, and wind speed. In this paper, we use this parameterization of sub-grid coagulation in the GEOS-Chem-TOMAS global aerosol microphysics model to quantify the impacts on global aerosol size distributions, the direct radiative effect, and the cloud-albedo aerosol indirect effect. We find that inclusion of biomass burning sub-grid coagulation reduces the biomass burning impact on the number concentration of particles larger than 80 nm (a proxy for CCN-sized particles) by 37 % globally. This CCN reduction causes our estimated global biomass burning cloud-albedo aerosol indirect effect to decrease from −76 to −43 mW m−2. Further, as sub-grid coagulation moves mass to sizes with more efficient scattering, including it increases our estimated biomass burning all-sky direct effect from −224 to −231 mW m−2 with assumed external mixing and from −188 to −197 mW m−2 with assumed internal mixing with core-shell morphology. However, due to differences in fire and meteorological conditions across regions, the impact of sub-grid coagulation is not globally uniform. We also test the sensitivity of the impact of sub-grid coagulation to two different biomass burning emission inventories, to various assumptions about the fresh biomass burning aerosol size distribution, and to two different timescales of sub-grid coagulation. The impacts of sub-grid coagulation are qualitatively the same regardless of these assumptions.

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ACE-FTS observations of pyrogenic trace species in boreal biomass burning plumes during BORTAS

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-12-31629-2012 ◽

2012 ◽

Vol 12 (12) ◽

pp. 31629-31661 ◽

Cited By ~ 7

Author(s):

K. A. Tereszchuk ◽

G. González Abad ◽

C. Clerbaux ◽

J. Hadji-Lazaro ◽

D. Hurtmans ◽

...

Keyword(s):

Boreal Forest ◽

Biomass Burning ◽

Atmospheric Chemistry ◽

Forest Fires ◽

Atmospheric Composition ◽

Fire Season ◽

Satellite Measurement ◽

Mixing Ratios ◽

Trace Species ◽

The Impact

Abstract. To further our understanding of the effects of biomass burning emissions on atmospheric composition, the Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites (BORTAS) campaign was conducted on 12 July to 3 August 2011 during the Boreal forest fire season in Canada. The simultaneous aerial, ground and satellite measurement campaign sought to record instances of Boreal biomass burning to measure the tropospheric volume mixing ratios (VMRs) of short- and long-lived trace molecular species from biomass burning emissions. The goal was to investigate the connection between the composition and the distribution of these pyrogenic outflows and their resulting perturbation to atmospheric chemistry, with particular focus on oxidant species to determine the overall impact on the oxidizing capacity of the free troposphere. Measurements of pyrogenic trace species in Boreal biomass burning plumes were made by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) onboard the Canadian Space Agency (CSA) SCISAT-1 satellite during the BORTAS campaign. Even though most biomass burning smoke is typically confined to the boundary layer, emissions are often injected directly into the upper troposphere via fire-related convective processes, thus allowing space-borne instruments to measure these pyrogenic outflows. An extensive set of 15 molecules, CH3OH, CH4, C2H2, C2H6, C3H6O, CO, HCN, HCOOH, HNO3, H2CO, NO, NO2, OCS, O3 and PAN have been analyzed. Included in this analysis is the calculation of age-dependent sets of enhancement ratios for each of the species.

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Properties and evolution of biomass burning organic aerosol from Canadian boreal forest fires

Atmospheric Chemistry and Physics ◽

10.5194/acp-15-3077-2015 ◽

2015 ◽

Vol 15 (6) ◽

pp. 3077-3095 ◽

Cited By ~ 29

Author(s):

M. D. Jolleys ◽

H. Coe ◽

G. McFiggans ◽

J. W. Taylor ◽

S. J. O'Shea ◽

...

Keyword(s):

Boreal Forest ◽

Biomass Burning ◽

Forest Fires ◽

Spatial Scales ◽

Near Field ◽

Organic Aerosol ◽

Charge Ratio ◽

Far Field ◽

Airborne Measurements ◽

The Impact

Abstract. Airborne measurements of biomass burning organic aerosol (BBOA) from boreal forest fires reveal highly contrasting properties for plumes of different ages. These measurements, performed using an Aerodyne Research Inc. compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) during the BORTAS (quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) experiment in the summer of 2011, have been used to derive normalised excess organic aerosol (OA) mass concentrations (ΔOA / ΔCO), with higher average ratios observed closer to source (0.190±0.010) than in the far-field (0.097±0.002). The difference in ΔOA / ΔCO between fresh and aged plumes is influenced by a change in dominant combustion conditions throughout the campaign. Measurements at source comprised 3 plume interceptions during a single research flight and sampled largely smouldering fires. Twenty-three interceptions were made across four flights in the far-field, with plumes originating from fires occurring earlier in the campaign when fire activity had been more intense, creating an underlying contrast in emissions prior to any transformations associated with aging. Changing combustion conditions also affect the vertical distribution of biomass burning emissions, as aged plumes from more flaming-dominated fires are injected to higher altitudes of up to 6000 m. Proportional contributions of the mass-to-charge ratio (m/z) 60 and 44 peaks in the AMS mass spectra to the total OA mass (denoted f60 and f44) are used as tracers for primary and oxidised BBOA, respectively. f44 is lower on average in near-field plumes than those sampled in the far-field, in accordance with longer aging times as plumes are transported a greater distance from source. However, high levels of ΔO3 / ΔCO and −log(NOx / NOy) close to source indicate that emissions can be subject to very rapid oxidation over short timescales. Conversely, the lofting of plumes into the upper troposphere can lead to the retention of source profiles after transportation over extensive temporal and spatial scales, with f60 also higher on average in aged plumes. Evolution of OA composition with aging is comparable to observations of BB tracers in previous studies, revealing a consistent progression from f60 to f44. The elevated levels of oxygenation in aged plumes, and their association with lower average ΔOA / ΔCO, are consistent with OA loss through evaporation during aging due to a combination of dilution and chemical processing, while differences in combustion conditions throughout the campaign also have a significant influence on BBOA production and composition.

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Detection of Aerosol Particles from Siberian Biomass Burning over the Western North Pacific

Atmosphere ◽

10.3390/atmos11111175 ◽

2020 ◽

Vol 11 (11) ◽

pp. 1175

Author(s):

Momoka Yoshizue ◽

Fumikazu Taketani ◽

Kouji Adachi ◽

Yoko Iwamoto ◽

Yasunori Tohjima ◽

...

Keyword(s):

Biomass Burning ◽

Forest Fires ◽

North Pacific ◽

Radiative Forcing ◽

Western North Pacific ◽

Aerosol Particles ◽

Carbonaceous Aerosol ◽

The Arctic ◽

First Case ◽

The Impact

Carbonaceous aerosol particles emitted from biomass burning (BB) have a large impact on the global climate. In particular, tarball particles (TBs), which are spherical organic aerosol particles, account for a large proportion of aerosol particles from BB. In this study, we collected aerosol particles over the western North Pacific and analyzed them using transmission electron microscopy with energy-dispersive X-ray spectroscopy (TEM-EDX) to reveal their shape and composition. We detected TBs and organic carbon particles originating from Siberian forest fires. To the best of our knowledge, this is the first case in which a large number of TBs have been found over the Pacific Ocean far from the BB source. The spherical shapes of the TBs were maintained even after long-range transport. In addition, our individual analysis of TBs showed that the size and composition of TBs differ depending on the air mass origin. The occurrence and microphysical properties of TBs are important to accurately evaluate the impact of TBs on climate. Our results imply that TBs can be transported to the Arctic and have an influence on radiative forcing over the ocean and in the Arctic.

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Size distribution and coating thickness of black carbon from the Canadian oil sands operations

10.5194/acp-2017-1015 ◽

2017 ◽

Author(s):

Yuan Cheng ◽

Shao-Meng Li ◽

Mark Gordon ◽

Peter Liu

Keyword(s):

Size Distribution ◽

Black Carbon ◽

Coating Thickness ◽

Oil Sands ◽

Radiative Forcing ◽

Climate Models ◽

Source Area ◽

Size Distributions ◽

Mixing State ◽

Earth’S Climate

Abstract. Black carbon (BC) plays an important role in the Earth’s climate system. However, parameterization of BC size and mixing state have not been well addressed in aerosol-climate models, introducing substantial uncertainties into the estimation of radiative forcing by BC. In this study, we focused on BC emissions from the massive oil sands (OS) industry in northern Alberta, based on an aircraft campaign conducted over the Athabasca OS region in 2013. A total of 14 flights were made over the OS source area, in which the aircraft was typically flown in a 4- or 5-sided polygon pattern along flight tracks encircling an OS facility. Another 3 flights were performed downwind of the OS source area, each of which involved at least three intercepting locations where the well-mixed OS plume was measured along flight tracks perpendicular to the wind direction. Comparable size distributions were observed for refractory black carbon (rBC) over and downwind of the OS facilities, with rBC mass median diameters (MMD) between ~ 135 and 145 nm that were characteristic of fresh urban emissions. This MMD range corresponded to rBC number median diameters (NMD) of ~ 60–70 nm, approximately 100 % higher than the NMD settings in some aerosol-climate models. The typical in- and out-of-plume segments of a flight, which had different rBC concentrations and photochemical ages, showed consistent rBC size distributions. Moreover, rBC size distributions remained unchanged at different downwind distances from the source area, suggesting that atmospheric aging would not necessarily change rBC size distribution. However, aging indeed influenced rBC mixing state. Coating thickness for rBC cores in the diameter range of 130–160 nm was nearly doubled within three hours when the OS plume was transported over a distance of 90 km from the source area.

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