scholarly journals Ambient black carbon particle hygroscopic properties controlled by mixing state and composition

2012 ◽  
Vol 12 (11) ◽  
pp. 28955-28992 ◽  
Author(s):  
D. Liu ◽  
J. Allan ◽  
J. Whitehead ◽  
D. Young ◽  
M. Flynn ◽  
...  
Keyword(s):  
Ammonium Nitrate ◽  
Black Carbon ◽  
Radiative Forcing ◽  
Western Europe ◽  
Carbon Particle ◽  
Chemical Compositions ◽  
Mixing State ◽  
Additional Material ◽  
Considerable Uncertainty ◽  
Hygroscopic Properties

Abstract. The wet removal of black carbon aerosol (BC) in the atmosphere is a crucial factor in determining its atmospheric lifetime and thereby the vertical and horizontal distributions, dispersion on local and regional scales, and the direct, semi-direct and indirect radiative forcing effects. The in-cloud scavenging and wet deposition rate of freshly emitted hydrophobic BC will be increased on acquisition of more-hydrophilic components by coagulation or coating processes. The lifetime of BC is still subject to considerable uncertainty for most of the model inputs, which is largely due to the insufficient constraints on the BC hydrophobic-to-hydrophilic conversion process from observational field data. This study was conducted at a site along UK North Norfolk coastline, where the BC particles were transported from different regions within Western Europe. A hygroscopicity tandem differential mobility analyser (HTDMA) was coupled with a single particle soot photometer (SP2) to measure the hygroscopic properties of BC particles and associated mixing state in real time. In addition, a Soot Particle AMS (SP-AMS) measured the chemical compositions of additional material associated with BC particles. The ensemble of BC particles persistently contained a less-hygroscopic mode at a growth factor (gf) of around 1.05 at 90% RH (dry diameter 163 nm). Importantly, a more-hygroscopic mode of BC particles was observed throughout the experiment, the gf of these BC particles extended up to ~1.4–1.6 with the minimum between this and the less hygroscopic mode at a gf ~1.25, or equivalent effective hygroscopicity parameter κ = ~0.1. The gf of BC particles (gfBC) was highly influenced by the composition of associated soluble material: increases of gfBC were associated with secondary inorganic components, and these increases were more pronounced when ammonium nitrate was in the BC particles; however the presence of secondary organic matter suppressed the gfBC below that of pure inorganics. The Zdanovskii-Stokes-Robinson (ZSR) mixing rule captures the hygroscopicity contributions from different compositions within ±30% compared to the measured results, however is subject to uncertainty due to the complex morphology of BC component and potential artefacts associated with semivolatile particles measured with the HTDMA. This study provides detailed insights on BC hygroscopicity associated with its mixing state, and the results will importantly constrain the microphysical mixing schemes of BC as used by a variety of high level models. In particular, this provides direct evidence to highlight the need to consider ammonium nitrate ageing of BC particles because this will result in particles becoming hydrophilic on much shorter timescales than for sulphate formation, which is often the only mechanism considered.

scholarly journals Ambient black carbon particle hygroscopic properties controlled by mixing state and composition

2013 ◽  
Vol 13 (4) ◽  
pp. 2015-2029 ◽  
Author(s):  
D. Liu ◽  
J. Allan ◽  
J. Whitehead ◽  
D. Young ◽  
M. Flynn ◽  
...  
Keyword(s):  
Ammonium Nitrate ◽  
Black Carbon ◽  
Radiative Forcing ◽  
Western Europe ◽  
Carbon Particle ◽  
Chemical Compositions ◽  
Mixing State ◽  
Additional Material ◽  
Considerable Uncertainty ◽  
Hygroscopic Properties

Abstract. The wet removal of black carbon aerosol (BC) in the atmosphere is a crucial factor in determining its atmospheric lifetime and thereby the vertical and horizontal distributions, dispersion on local and regional scales, and the direct, semi-direct and indirect radiative forcing effects. The in-cloud scavenging and wet deposition rate of freshly emitted hydrophobic BC will be increased on acquisition of more-hydrophilic components by coagulation or coating processes. The lifetime of BC is still subject to considerable uncertainty for most of the model inputs, which is largely due to the insufficient constraints on the BC hydrophobic-to-hydrophilic conversion process from observational field data. This study was conducted at a site along UK North Norfolk coastline, where the BC particles were transported from different regions within Western Europe. A hygroscopicity tandem differential mobility analyser (HTDMA) was coupled with a single particle soot photometer (SP2) to measure the hygroscopic properties of BC particles and associated mixing state in real time. In addition, a Soot Particle AMS (SP-AMS) measured the chemical compositions of additional material associated with BC particles. The ensemble of BC particles persistently contained a less-hygroscopic mode at a growth factor (gf) of around 1.05 at 90% RH (dry diameter 163 nm). Importantly, a more-hygroscopic mode of BC particles was observed throughout the experiment, the gf of these BC particles extended up to ~1.4–1.6 with the minimum between this and the less hygroscopic mode at a gf ~1.25, or equivalent effective hygroscopicity parameter κ ~0.1. The gf of BC particles (gfBC) was highly influenced by the composition of associated soluble material: increases of gfBC were associated with secondary inorganic components, and these increases were more pronounced when ammonium nitrate was in the BC particles; however the presence of secondary organic matter suppressed the gfBC below that of pure inorganics. The Zdanovskii-Stokes-Robinson (ZSR) mixing rule captures the hygroscopicity contributions from different compositions within ±30% compared to the measured results, however is subject to uncertainty due to the complex morphology of BC component and potential artefacts associated with semivolatile particles measured with the HTDMA. This study provides detailed insights on BC hygroscopicity associated with its mixing state, and the results will importantly constrain the microphysical mixing schemes of BC as used by a variety of high level models. In particular, this provides direct evidence to highlight the need to consider ammonium nitrate ageing of BC particles because this will result in particles becoming hydrophilic on much shorter timescales than for sulphate formation, which is often the only mechanism considered.

scholarly journals Droplet activation behaviour of atmospheric black carbon particles in fog as a function of their size and mixing state

2018 ◽  
Author(s):  
Ghislain Motos ◽  
Julia Schmale ◽  
Joel Christopher Corbin ◽  
Marco Zanatta ◽  
Urs Baltensperger ◽  
...  
Keyword(s):  
Black Carbon ◽  
Single Particle ◽  
Radiative Forcing ◽  
Cloud Condensation Nuclei ◽  
Mixing State ◽  
Scanning Mobility Particle Sizer ◽  
Carbon Particles ◽  
Hygroscopic Properties ◽  
Droplet Activation ◽  
Aerosol Cloud Interactions

Abstract. Among the variety of particle types present in the atmosphere, black carbon (BC), emitted by combustion processes, is uniquely associated with harmful effects to the human body and substantial radiative forcing of the Earth. Pure BC is known to be non-hygroscopic, but its ability to acquire a coating of hygroscopic organic and inorganic material leads to increased hygroscopicity as well as diameter, facilitating droplet activation. This affects BC radiative forcing through aerosol-cloud interactions (aci) and BC life cycle. To gain insights into these processes, we performed a field campaign in winter 2015/16 in a residential area of Zurich which aimed at distinguishing different particle mixing states regarding hygroscopic properties in the cloud condensation nuclei (CCN)-activated fraction spectrum of urban aerosol and establishing relations between the mixing state of BC and its activation to form droplets in fog. This was achieved by operating a CCN counter (CCNC), a scanning mobility particle sizer (SMPS), a single particle soot photometer (SP2) and an aerosol chemical speciation monitor (ACSM) behind a combination of a total- and an interstitial-aerosol inlet. Our results indicate that, depending on the time of the day, we sampled both heavily aged internally mixed BC from background air advected to the site and freshly emitted externally mixed BC from local or regional traffic sources. During rush hours in the morning of weekdays, we found clear evidence that the enhanced traffic emissions caused peaks in the number fraction of externally mixed BC particles which do not act as CCN within the CCNC. The mixing state of BC particles was also found to play a key role in their ability to form fog droplets. The very low effective peak supersaturations (SSpeak) occurring in fog (between approximately 0.03 and 0.06 % during this campaign) restrict droplet activation to a minor fraction of the aerosol burden (around 0.5 to 1 % of total particle number concentration between 20 and 593 nm) leading to very selective criteria on diameter and chemical composition. We show that bare BC cores are unable to activate to fog droplets at such low SSpeak, while BC particles surrounded by thick coating have a very similar activation behavior as BC-free particles. The threshold coating thickness required for activation was shown to decrease with increasing BC core size. Using simplified κ-Köhler theory combined with the ZSR mixing rule assuming spherical core-shell particle geometry constrained with single particle measurements of respective volumes, we found good agreement between the predicted and the directly observed size and mixing state resolved droplet activation behaviour of BC-containing particles in fog. This successful closure demonstrates the predictability of their droplet activation in fog with a simplified theoretical model only requiring size and mixing state information, which can also be applied in a consistent manner in model simulations.

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

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.

scholarly journals The filter loading effect by ambient aerosols in filter absorption photometers depends on the mixing state of the sampled particles

2016 ◽  
Author(s):  
Luka Drinovec ◽  
Asta Gregorič ◽  
Peter Zotter ◽  
Robert Wolf ◽  
Emily Anne Bruns ◽  
...  
Keyword(s):  
Black Carbon ◽  
Carbon Particle ◽  
Mixing State ◽  
Ambient Aerosols ◽  
Loading Effect ◽  
Particle Mixing ◽  
Filter Loading ◽  
Ångström Exponent ◽  
Loading Parameter ◽  
Black Carbon Particle

Abstract. Black carbon is a primary aerosol tracer for high-temperature combustion emissions and can be used to characterize the time evolution of its sources. It is correlated with a decrease in public health and contributes to atmospheric warming. Black carbon measurements are usually conducted with absorption filter photometers, which are prone to the filter-loading effect – a saturation of the instrumental response due to the accumulation of the sample in the filter matrix. In this paper, we investigate the hypothesis that this filter-loading effect depends on the optical properties of particles present in the filter matrix, especially on the black carbon particle mixing state. We conducted field campaigns in contrasting environments to determine the influence of source characteristics, particle age and coating on the magnitude of the filter-loading effect. High time resolution measurements of the filter-loading parameter in filter absorption photometers show daily and seasonal variations of the effect. The variation is most pronounced in the near-infrared region, where the black carbon mass concentration is determined. During winter, the filter-loading parameter value increases with the absorption Ångström exponent. It is suggested that this effect is related to the size of the black carbon particle core as the wood burning (with higher values of the absorption Ångström exponent) produces soot particles with larger diameters. A reduction of the filter-loading effect is correlated with the availability of the coating material. As the coating of ambient aerosols is reduced or removed, the filter-loading parameter increases. Coatings composed of ammonium sulfate and secondary organics seem to be responsible for the variation of the loading effect. The potential source contribution function analysis shows that high values of the filter-loading parameter in the infrared are indicative of local pollution, whereas low values of the filter-loading parameter result from ageing and coating during long range transport. Our results show that the filter-loading parameter can be used as proxy for determination of the particle mixing state, thus allowing for differentiation between local/fresh and transported/aged particles.

scholarly journals Single particle diversity and mixing state measurements

2014 ◽  
Vol 14 (12) ◽  
pp. 6289-6299 ◽  
Author(s):  
R. M. Healy ◽  
N. Riemer ◽  
J. C. Wenger ◽  
M. Murphy ◽  
M. West ◽  
...  
Keyword(s):  
Species Diversity ◽  
Ammonium Nitrate ◽  
Black Carbon ◽  
Mass Spectrometer ◽  
Single Particle ◽  
Organic Aerosol ◽  
Particle Mass ◽  
Mixing State ◽  
Mass Fractions ◽  
State Index

Abstract. A newly developed framework for quantifying aerosol particle diversity and mixing state based on information-theoretic entropy is applied for the first time to single particle mass spectrometry field data. Single particle mass fraction estimates for black carbon, organic aerosol, ammonium, nitrate and sulfate, derived using single particle mass spectrometer, aerosol mass spectrometer and multi-angle absorption photometer measurements are used to calculate single particle species diversity (Di). The average single particle species diversity (Dα) is then related to the species diversity of the bulk population (Dγ) to derive a mixing state index value (χ) at hourly resolution. The mixing state index is a single parameter representation of how internally/externally mixed a particle population is at a given time. The index describes a continuum, with values of 0 and 100% representing fully external and internal mixing, respectively. This framework was applied to data collected as part of the MEGAPOLI winter campaign in Paris, France, 2010. Di values are low (~ 2) for fresh traffic and wood-burning particles that contain high mass fractions of black carbon and organic aerosol but low mass fractions of inorganic ions. Conversely, Di values are higher (~ 4) for aged carbonaceous particles containing similar mass fractions of black carbon, organic aerosol, ammonium, nitrate and sulfate. Aerosol in Paris is estimated to be 59% internally mixed in the size range 150–1067 nm, and mixing state is dependent both upon time of day and air mass origin. Daytime primary emissions associated with vehicular traffic and wood-burning result in low χ values, while enhanced condensation of ammonium nitrate on existing particles at night leads to higher χ values. Advection of particles from continental Europe containing ammonium, nitrate and sulfate leads to increases in Dα, Dγ and χ. The mixing state index represents a useful metric by which to compare and contrast ambient particle mixing state at other locations globally.

Influence of size and mixing state on the wet scavenging of black carbon aerosol in the North China Plain

2020 ◽  
Author(s):  
Xihao Pan ◽  
Nan Ma ◽  
Yaqing Zhou ◽  
Shaowen Zhu ◽  
Long Peng ◽  
...  
Keyword(s):  
Black Carbon ◽  
Radiative Forcing ◽  
North China Plain ◽  
North China ◽  
Mixing State ◽  
Radiation Fog ◽  
The North ◽  
The North China Plain ◽  
Positive Direct ◽  
Scavenging Efficiency

<p>Black carbon (BC) is the most important light-absorbing species in the atmosphere and has a strong positive direct radiative forcing. In-cloud scavenging is the major way to wash out BC from the atmosphere. Understanding the connection between its physico-chemical properties and scavenging efficiency is therefore a key to evaluate its lifetime, atmospheric burden and spatial distribution. During an intensive field campaign conducted in the North China Plain in 2019, a ground-based counterflow virtual impactor was utilized to separate fog droplets in radiation fog events. BC mass and mixing state of fog droplet residues were online measured with a single particle soot photometer (SP2). In a strong radiation fog event with visibility of about 50 m, more than 20% fog droplets are found to contain a BC core. BC scavenging efficiency is found to be strongly determined by its diameter and mixing state. Driven by different mechanisms, higher scavenging efficiencies up to 10% are observed for larger and smaller BC particles, and the minimum efficiency is found at BC diameter of 120 nm. For large core (>120 nm) BC-containing particles, the scavenging efficiency increases significantly with coating thickness (CT), from about 10% for CT<100 nm to 80% for CT>300 nm. Chemical composition may also be a key parameter influencing the scavenging of BC. Based on the observation of 3 fog events, parameterizations of BC scavenging efficiency are also given in this study.</p>

scholarly journals Changes in the aerosol direct radiative forcing from 2001 to 2015: observational constraints and regional mechanisms

2018 ◽  
Author(s):  
Fabien Paulot ◽  
David Paynter ◽  
Paul Ginoux ◽  
Vaishali Naik ◽  
Larry Horowitz
Keyword(s):  
Black Carbon ◽  
Radiative Forcing ◽  
Western Europe ◽  
Climate Model ◽  
Eastern China ◽  
Radiant Energy ◽  
Present Observation ◽  
So2 Emissions ◽  
Clear Sky ◽  
Direct Forcing

Abstract. We present observation and model-based estimates of the changes in the direct shortwave effect of aerosols under clear-sky (SDRECS) from 2001 to 2015. Observation-based estimates are obtained from changes in the outgoing shortwave clear-sky radiation (Rsutcs) measured by the Clouds and the Earth's Radiant Energy System (CERES), accounting for the effect of variability in surface albedo, water vapor, and ozone. We find increases in SDRECS (i.e., less radiation scattered to space by aerosols) over Western Europe (0.7–1 W m−2 dec−1) and the Eastern US (0.9–1.8 W m−2 dec−1), decreases over India (−0.5– −1.9 W m−2 dec−1) and no significant change over Eastern China. Comparisons with the GFDL chemistry climate model AM3, driven by CMIP6 historical emissions, show that changes in SDRECS over Western Europe and the Eastern US are well captured, which largely reflects the mature understanding of the sulfate budget in these regions. In contrast, the model overestimates the trends in SDRECS over India and Eastern China. Over China, this bias can be partly attributed to the decline of SO2 emissions after 2007, which is not captured by the CMIP6 emissions. In both India and Eastern China, we find much larger contributions of nitrate and black carbon to changes in SDRECS than in the US and Europe, which highlights the need to better constrain their precursors and chemistry. Globally, our model shows that changes in the all-sky aerosol direct forcing between 2001 and 2015 (+0.03 W m−2) are dominated by black carbon (+0.12 W m−2) with significant offsets from nitrate (−0.03 W m−2) and sulfate (−0.03 W m−2). Changes in the sulfate (+7 %) and nitrate (+60 %) all-sky direct forcing between 2001 and 2015 are only weakly related to changes in the emissions of their precursors (−12.5 % and 19 % for SO2 and NH3, respectively), due mostly to chemical non linearities.

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