Mixed Aerosols Research Articles

Climatic–Environmental Effects of Aerosols and Their Sensitivity to Aerosol Mixing States in East Asia in Winter

To establish the direct climatic and environmental effect of anthropogenic aerosols in East Asia in winter under external, internal, and partial internal mixing (EM, IM and PIM) states, a well-developed regional climate–chemical model RegCCMS is used by carrying out sensitive numerical simulations. Different aerosol mixing states yield different aerosol optical and radiative properties. The regional averaged EM aerosol single scattering albedo is approximately 1.4 times that of IM. The average aerosol effective radiative forcing in the atmosphere ranges from −0.35 to +1.40 W/m2 with increasing internal mixed aerosols. Due to the absorption of black carbon aerosol, lower air temperatures are increased, which likely weakens the EAWM circulations and makes the atmospheric boundary more stable. Consequently, substantial accumulations of aerosols further appear in most regions of China. This type of interaction will be intensified when more aerosols are internally mixed. Overall, the aerosol mixing states may be important for regional air pollution and climate change assessments. The different aerosol mixing states in East Asia in winter will result in a variation from 0.04 to 0.11 K for the averaged lower air temperature anomaly and from approximately 0.45 to 2.98 μg/m3 for the aerosol loading anomaly, respectively, due to the different mixing aerosols.

Quantifying the effects of mixing state on aerosol optical properties

Abstract. Calculations of the aerosol direct effect on climate rely on simulated aerosol fields. The model representation of aerosol mixing state potentially introduces large uncertainties into these calculations, since the simulated aerosol optical properties are sensitive to mixing state. In this study, we systematically quantified the impact of aerosol mixing state on aerosol optical properties using an ensemble of 1800 aerosol populations from particle-resolved simulations as a basis for Mie calculations for optical properties. Assuming the aerosol to be internally mixed within prescribed size bins caused overestimations of aerosol absorptivity and underestimations of aerosol scattering. Together, these led to errors in the populations' single scattering albedo of up to −22.3 % with a median of −0.9 %. The mixing state metric χ proved useful in relating errors in the volume absorption coefficient, the volume scattering coefficient and the single scattering albedo to the degree of internally mixing of the aerosol, with larger errors being associated with more external mixtures. At the same time, a range of errors existed for any given value of χ. We attributed this range to the extent to which the internal mixture assumption distorted the particles' black carbon content and the refractive index of the particle coatings. Both can vary for populations with the same value of χ. These results are further evidence of the important yet complicated role of mixing state in calculating aerosol optical properties.

Aerosol Optical Characteristics with Ground-based Measurements via Sun Photometer and Its Relationship with PM Particle Concentration in Chang'an

The simultaneous quantitative investigation of aerosol ground observation data and particle concentration data is important for a better understanding of the vertical distribution characteristics of air pollution and formulating reasonable air pollution control measures in Chang'an, Xi'an. CE-318 measurements from October 2018 to April 2021 were systematically analyzed to reveal the seasonal and yearly variations in atmospheric aerosols in Chang'an. Then, the relationship between AOD and particle concentration in different seasons and different pollution degrees was explored. The obtained results were as follows:① the seasonal variation in AOD in Chang'an was determined, whereby autumn (1.02)>winter (1.00)>summer (0.63)>spring (0.47). Distinct monthly and inter-annual differences in AOD were observed, showing that the annual average of AOD in 2019 was higher than that in 2020. ② Obvious seasonal and monthly differences in aerosol main control modes were observed; the dominant mode of aerosols gradually changed from coarse mode to fine mode from spring to winter. The seasonal variation in the main control mode of aerosols in 2019 was similar to that in the whole observation period. The seasonal aerosol Angstrom wavelength index (Angstrom) was evenly distributed in 2020, and aerosol particles existed in coarse mode form. Generally speaking, the aerosol type in Chang'an was mostly mixed aerosol throughout the whole observation period. ③ Significant seasonal variations in the relationship between AOD and Angstrom was shown, in which the air pollution in spring was dominated by coarse mode aerosol particles. The local pollution in summer was caused by coarse and fine mode aerosol particles, and the fine mode particles were dominant when the pollution was obvious. The characteristic distribution of Angstrom in autumn and winter was similar; in case of local pollution, the coarse mode aerosol particles were dominant, and in case of obvious pollution, the fine mode aerosol particles were dominant. ④ The monthly concentration variation trend of PM2.5 and PM10 in Chang'an consistent with the maximum and minimum values appeared in January and summer, respectively. Seasonal variation in the concentration of PM2.5 and PM10 was apparent, with the highest values in winter. ⑤ A positive correlation between AOD and particulate matter concentration in different seasons and pollution levels was obtained during the observation periods, but the correlation coefficient differed. The specific characteristics were as follows:the correlation between AOD and PM2.5 concentration was greater than that with PM10 concentration; the correlation between AOD and particle concentration in autumn and winter was greater than that in spring and summer; and the correlation between AOD and particulate matter concentration was greater in polluted weather. Particle concentration was the most important determinant of AOD change, followed by relative humidity, which was the meteorological factor with the highest interpretation rate of AOD change in Chang'an. This indicates that a higher correlation between AOD and particle concentration would benefit from a reasonable humidity correction of AOD.

Performance of MODIS Deep Blue Collection 6.1 Aerosol Optical Depth Products Over Indonesia: Spatiotemporal Variations and Aerosol Types

This study aims to evaluate the performance of the long-term Terra Moderate Resolution Imaging Spectroradiometer (MODIS) Deep Blue (DB) Collection 6.1 (C6.1) in determining the spatiotemporal variation of aerosol optical depth (AOD) and aerosol types over Indonesia. For this purpose, monthly MODIS DB AOD datasets are directly compared with Aerosol Robotic Network (AERONET) Version 3 Level 2.0 (cloud-screened and quality-assured) monthly measurements at 8 sites throughout Indonesia. The results indicate that MODIS DB AOD retrievals and AERONET AOD measurements have a high correlation in Sumatra Island (i.e., Kototabang (r = 0.88) and Jambi (r = 0.9)) and Kalimantan Island (i.e., Palangkaraya (r = 0.89) and Pontianak (r = 0.92)). However, the correlations are low in Bandung, Palu, and Sorong. In general, MODIS DB AOD tends to overestimate AERONET AOD at all sites by 16 to 61% and can detect extreme fire events in Sumatra and Kalimantan Islands quite well. Aerosol types in Indonesia mostly consist of clean continental, followed by biomass burning/urban industrial and mixed aerosols. Palu and Sorong had the highest clean continental aerosol contribution (90%), while Bandung had the highest biomass burning/urban-industrial aerosol contribution to atmospheric composition (93.7%). For mixed aerosols, the highest contribution was found in Pontianak, with a proportion of 48.4%. Spatially, the annual mean AOD in the western part of Indonesia is higher than in the eastern part. Seasonally, the highest AOD is observed during the period of September–November, which is associated with the emergence of fire events.

Optical and Microphysical Properties of the Aerosol Field over Sofia, Bulgaria, Based on AERONET Sun-Photometer Measurements

An analysis of the optical and microphysical characteristics of aerosol passages over Sofia City, Bulgaria, was performed on the basis of data provided by the AErosol RObotic NETwork (AERONET). The data considered are the result of two nearly complete annual cycles of passive optical remote sensing of the atmosphere above the Sofia Site using a Cimel CE318-TS9 sun/sky/lunar photometer functioning since 5 May 2020. The values of the Aerosol Optical Depth (AOD) and the Ångström Exponent (AE) measured during each annual cycle and the overall two-year cycle exhibited similar statistics. The two-year mean AODs were 0.20 (±0.11) and 0.17 (±0.10) at the wavelengths of 440 nm (AOD440) and 500 nm, respectively. The two-year mean AEs at the wavelength pairs 440/870 nm (AE440/870) and 380/500 nm were 1.45 (±0.35) and 1.32 (±0.29). The AOD values obtained reach maxima in winter-to-spring and summer and were about two times smaller than those obtained 15 years ago using a hand-held Microtops II sun photometer. The AOD440 and AE440/870 frequency distributions outline two AOD and three AE modes, i.e., 3 × 2 groups of aerosol events identifiable using AOD–AE-based aerosol classifications, additional aerosol characteristics, and aerosol migration models. The aerosol load over the city was estimated to consist most frequently of urban (63.4%) aerosols. The relative occurrences of desert dust, biomass-burning aerosols, and mixed aerosols were, respectively, 8.0%, 9.1% and 19.5%.

Severe Biomass-Burning Aerosol Pollution during the 2019 Amazon Wildfire and Its Direct Radiative-Forcing Impact: A Space Perspective from MODIS Retrievals

An extreme biomass burning event occurred in the Amazonian rainforest from July through September 2019 due to the extensive wildfires used to clear the land, which allowed for more significant forest burning than previously occurred. In this study, we reclustered the clear-sky ambient aerosols to adapt the black carbon (BC) aerosol retrieval algorithm to Amazonia. This not only isolated the volumetric fraction of BC (fbc) from moderate-resolution imaging spectroradiometer (MODIS) aerosol data, but also facilitated the use of aerosol mixing and scattering models to estimate the absorption properties of smoke plumes. The retrieved MODIS aerosol dataset provided a space perspective on characterizing the aerosol changes and trends of the 2019 pollution event. A very high aerosol optical depth (AOD) was found to affect the source areas continuously, with higher and thus stronger aerosol absorption. These pollutants also affected the atmosphere downwind due to the transport of air masses. In addition, properties of aerosols emitted from the 2019 Amazonian wildfire events visualized a significant year-to-year enhancement, with the averaged AOD at 550 nm increased by 150%. A 200% increase in the aerosol-absorption optical depth (AAOD) at 550 nm was recognized due to the low single-scattering albedo (SSA) caused by the explosive BC emissions during the pollution peak. Further simulations of aerosol radiative forcing (ARF) showed that the biomass-burning aerosols emitted during the extreme Amazonian wildfires event in 2019 forced a significant change in the radiative balance, which not only produced greater heating of the atmospheric column through strong absorption of BC, but also reduced the radiation reaching the top-of-atmosphere (TOA) and surface level. The negative radiative forcing at the TOA and surface level, as well as the positive radiative forcing in the atmosphere, were elevated by ~30% across the whole of South America compared to 2018. These radiative effects of the absorbing aerosol could have the ability to accelerate the deterioration cycle of drought and fire over the Amazonian rainforest.

Wintertime Observations of Tropical Northwest Atlantic Aerosol Properties During ATOMIC: Varying Mixtures of Dust and Biomass Burning

AbstractThe Atlantic Tradewind Ocean‐Atmosphere Mesoscale Campaign (ATOMIC) took place from 7 January to 11 July 2020 in the tropical North Atlantic between the east coast of Barbados and the Northwest Tropical Atlantic Station (NTAS) mooring. Measurements of aerosol chemical, microphysical, optical, and cloud‐nucleating properties were made during boreal winter onboard the NOAA RV Ronald H. Brown from 7 January to 13 February 2020. Observed aerosol properties indicate there were distinct periods when the aerosol was typical of clean marine conditions (particle number concentrations <400 cm−3, light absorption levels <1 Mm−1, and 222Rn concentrations <500 mBq m−3) and when there were intrusions of dust mixed to varying degrees with biomass burning aerosol. In comparison to the long‐term dust record at the Barbados Atmospheric Chemistry Observatory, the fraction of samples collected during ATOMIC with dust concentrations greater than 20 μg m−3 exceeded all years of the Barbados January to February record with the exception of 1983. The degree of mixing of the dust with biomass burning aerosol was modulated by the location of the North Atlantic subtropical high. A high located to the west of Africa led to a more northerly transport route and more dust‐like (MDL) aerosol arriving at the ship. A location of the high further to the east over northern Africa led to a more southerly transport route and more biomass burning aerosol mixed with the dust. Properties for the marine, MDL, and mixed dust and biomass burning aerosol are presented.

Dust Aerosol Vertical Profiles in the Hinterland of Taklimakan Desert During Summer 2019

Dust aerosol vertical profiles are very essential to accurately evaluate their climate forcing and trans-subcontinental transportation to downstream areas. We initiated a joint comprehensive field experiment to investigate the vertical profiles and optical characteristics of dust aerosol in the hinterland of Taklimakan Desert (TD) during summer 2019. After smoothing the raw signals, the CHM15k ceilometer could distinctly detect a moderate intensity of dust layer, cloud layer, and subsequent rainfall process. The results showed that dust events frequently occurred in TD during the entire period; the overall mean PM2.5, PM10, PM2.5/PM10, and Ångström exponent are 110.4 ± 121.0 μg/m3, 317.2 ± 340.0 μg/m3, 0.35 ± 0.07, and 0.28 ± 0.12, respectively, suggesting that dust particles are predominant aerosol types in TD. There was an obvious summertime dust stagnation layer persistently hanged over the desert at 1.5–3.0-km height. A deep and intense daytime convective structure was also detected by the ceilometer, with maximum aerosol mixing layer height of ∼3 km that appeared at 12:00 UTC, which was in favor of lifting the ground-generated dust particles into the upper atmosphere. The normalized range-corrected signal log10(RCS), aerosol extinction σ(z), and backscattering coefficient β(z) of the ceilometer were higher than 6.2, 0.5 km−1, and 0.01 km−1 sr−1 for heavy dust storms, respectively, and the corresponding vertical optical range was smaller than 1.0 km. The aerosol lidar ratio was equal to 50 sr, which was greatly different from those of clear-sky cases. The retrieved σ(z) values were about 2.0, 0.5, 0.14, and 0.10 km−1 at 200-m height, respectively, under strong dust storm, blowing dust, floating dust, and clear-sky conditions. This indicated that the aerosol extinction coefficients under dust events were about 3–10 times greater than those of clear-sky cases. The statistics of the aerosol optical parameters under different dust intensities in TD were very helpful to explore and validate dust aerosols in the application of climate models or satellite remote sensing.

Impact of Aerosol Mixing State and Hygroscopicity on the Lidar Ratio

The lidar ratio (LR) is a key parameter for the retrieval of atmospheric optical parameters from lidar equations. In this study, we simulated the optical parameters to investigate the impact factors of the LR using a three-component optical aerosol assumption based on the Mie model. The simulated LR was generally related to the overall particle size of the aerosols, the proportion of elemental carbon (EC), as well as aerosol mixing states and hygroscopicity. The LR was positively correlated with the particle size and volume fraction of elemental carbon (fEC). The LR increased more than three-fold with the increase in fEC from 0% to 40%. The LR of the core-shell (CS) mixing state and homogeneously internal (INT) mixing state was greater than that of the external (EXT) mixing state. The LR of all mixing states increased monotonically with hygroscopicity when the fEC was below 10%, while the LR of the core-shell mixing state (homogeneously internal mixing state) initially decreased (increased) and then increased (decreased) with increasing hygroscopicity when the fEC was more than 20%. These results will help in selecting a reasonable LR for practical applications.

Retrieval of refractive index of ultrafine single particle using hygroscopic growth factor obtained by high sensitive surface plasmon resonance microscopy

When exposed to different relative humidities (RHs), the optical properties of atmospheric aerosols will change because of changes in the aerosol particle size and complex refractive index (RI), which will affect haze formation and global climate change. The potential contributions of ultrafine particles to the atmospheric optical characteristics and to haze spreading cannot be ignored because of their high particle number concentrations and strong diffusibility; measurement of the optical properties of wet ultrafine particles is thus highly important for environmental assessment. Therefore, a surface plasmon resonance microscopy with azimuthal rotation illumination (SPRM-ARI) system is designed to determine the RIs of single particle aerosols with diameters of less than 100 nm in the hygroscopic growth process. Measurements are taken using mixed single particles with different mass ratios. The RIs of mixed single aerosols at different RHs are retrieved by measuring the scattering light intensity using the SPRM-ARI system and almost all the RIs of the bicomponent particles with different mass ratios decrease with increasing water content under high RH conditions. Finally, for each of the bicomponent particles, the maximum standard deviations for the retrieved RI values are only 2.06×10−3, 3.08×10−3 and 3.83×10−3, corresponding to the NaCl and NaNO3 bicomponent particles with a 3:1 mass ratio at 76.0% RH, the NaCl and glucose particles with a 1:3 mass ratio at 89.0% RH, and the NaCl and OA particles with a 1:1 mass ratio at 78.0% RH, respectively; these results indicate that the high-sensitivity SPRM-ARI system can measure the RI effectively and accurately.

The 2019 Raikoke volcanic eruption – Part 2: Particle-phase dispersion and concurrent wildfire smoke emissions

Abstract. Between 27 June and 14 July 2019 aerosol layers were observed by the United Kingdom (UK) Raman lidar network in the upper troposphere and lower stratosphere. The arrival of these aerosol layers in late June caused some concern within the London Volcanic Ash Advisory Centre (VAAC) as according to dispersion simulations the volcanic plume from the 21 June 2019 eruption of Raikoke was not expected over the UK until early July. Using dispersion simulations from the Met Office Numerical Atmospheric-dispersion Modelling Environment (NAME), and supporting evidence from satellite and in situ aircraft observations, we show that the early arrival of the stratospheric layers was not due to aerosols from the explosive eruption of the Raikoke volcano but due to biomass burning smoke aerosols associated with intense forest fires in Alberta, Canada, that occurred 4 d prior to the Raikoke eruption. We use the observations and model simulations to describe the dispersion of both the volcanic and forest fire aerosol clouds and estimate that the initial Raikoke ash aerosol cloud contained around 15 Tg of volcanic ash and that the forest fires produced around 0.2 Tg of biomass burning aerosol. The operational monitoring of volcanic aerosol clouds is a vital capability in terms of aviation safety and the synergy of NAME dispersion simulations, and lidar data with depolarising capabilities allowed scientists at the Met Office to interpret the various aerosol layers over the UK and attribute the material to their sources. The use of NAME allowed the identification of the observed stratospheric layers that reached the UK on 27 June as biomass burning aerosol, characterised by a particle linear depolarisation ratio of 9 %, whereas with the lidar alone the latter could have been identified as the early arrival of a volcanic ash–sulfate mixed aerosol cloud. In the case under study, given the low concentration estimates, the exact identification of the aerosol layers would have made little substantive difference to the decision-making process within the London VAAC. However, our work shows how the use of dispersion modelling together with multiple observation sources enabled us to create a more complete description of atmospheric aerosol loading.

Evaluation of a new internally-mixed aerosol optics scheme in the weather research and forecasting model

A new internally-mixed aerosol optics scheme was developed. Aerosols (organic carbon, sea salt, aerosol water, sulfate, and nitrate) were assumed to be internally mixed with black carbon and soil dust (BC and SD, respectively), both of which are treated as cores. In the SD-containing particles, the particle non-sphericity was incorporated. Aerosol optical properties were computed from the invariant imbedding T-matrix method and the Lorenz–Mie theory and then parameterized using a novel method involving artificial neural networks (ANN). The new scheme was evaluated using the Weather Research and Forecasting (WRF) model. A case study involving East Asia was performed on Dec 3-4, 2010. Compared to uniformly mixed aerosols, inhomogeneous mixed aerosols had lower absorbability and stronger solar backscattering, causing a positive aerosol direct radiative effect (DRE) bias at the surface (3.0 and 2.6 W/m2 for the Sichuan Basin and Northern China, respectively) and negative DRE bias at the top of atmosphere ([TOA], −3.5 and −2.2 W/m2, respectively). Inhomogeneity effects caused a large reduction (up to 0.2K) in the atmospheric warming above the planetary boundary layer (PBL) and caused a northerly anomaly at 850 hPa on the order of 0.3 m/s. The non-sphericity effect was only significant over the Tarim Basin. DREs related to non-sphericity decreased at both the surface and TOA (−1.0 and −0.6 W/m2, respectively) due to stronger extinction. Non-sphericity caused more surface dimming and more solar heating, which had opposite effects on temperature perturbation, producing a more obvious impact within the PBL than in the free atmosphere.

Genesis of a Severe Dust Storm Over the Indian Subcontinent: Dynamics and Impacts

AbstractThe genesis, dynamics, and impacts of a severe dust storm over the central Himalaya during June 13–17, 2018 have been investigated using in situ measurements, satellite data, and model reanalysis. A low‐pressure system over northern India and prevalence of strong winds (∼20 ms−1) triggered the dust storm leading to poor visibility conditions and five‐fold enhancement in the fine particulate matter (PM2.5) over the central Himalaya. Enhancements in Aerosol Optical Depth (AOD) were observed to be stronger over the Himalayan foothills site (Lumbini) than that over the Indo‐Gangetic Plain (IGP) site‐Gandhi College. The sharp reductions in Angstrom exponent (α) from about 1.2 to 0.3 indicated the dominance of coarse‐mode aerosols during the dust episode. Model results show an enhancement in the dust from 1.5 to 2.5 Tg (∼70%) over the northern Indian subcontinent, with about half of the contribution from the regional source (Thar Desert). Interestingly, dust storm also had significant impacts on turbulent kinetic energy (2.9–9.6 m2 s−2), vertical momentum flux (0.9–3.3 Nm−2), and sensible heat flux (34.8 to −33.9 Wm−2), suggesting turbulent mixing of aerosols and cooling near the surface over the Himalayas. Our study highlights that the large‐scale dust storms exposed to additional dust and pollution from regional sources can profoundly impact the air quality, heat fluxes, and radiative balance over the northern Indian subcontinent. The study would also help in evaluating the results of climate models and to assess the impacts of dust on the hydrological processes and melting Himalayan glaciers.

Aerosols over the Foothills of the Eastern Himalayan Region during Post-monsoon and Winter Seasons

In this study a Microtops II sunphotometer is used for the first time over Birtamode, a rapidly growing city located in the eastern Himalayan foothills of Nepal, to measure aerosol optical depth (AOD). The average AOD for the observation period (October 2018–February 2019) was 0.68 ± 0.39 with the post-monsoon season having a higher value (0.74 ± 0.43) compared to the winter season (0.60 ± 0.32). The Angstrom exponent (α) for post-monsoon and winter are found to be 1.08 ± 0.10 and 1.11 ± 0.16 respectively. During the monitoring period, the majority of AOD values (47%) are above 0.60, indicating moderately polluted conditions in the region. Anthropogenic, biomass burning, and mixed aerosols are identified as the prevalent aerosol types in the study region. The observed aerosol classification is also explained in terms of CAMS near-real-time model datasets. The AOD values retrieved by MODIS, VIIRS, Himawari-8, and CAMS show a good correlation with the observed Microtops AOD with R2 values ranging from 0.60 to 0.94. Moreover, different MODIS aerosol products (DB, DT, and combined DB-DT) are evaluated based on a comparison of Collection 6.1 AOD with the ground truth obtained from Microtops. The spatial distribution of AOD as observed by various satellites are compared and the vertical distribution of aerosol is also explained with the extinction coefficient provided by the CALIOP lidar onboard CALIPSO and aerosol types provided by CAMS.

Mie scattering from optically levitated mixed sulfuric acid-silica core-shell aerosols: observation of core-shell morphology for atmospheric science.

Sulfuric acid is shown to form a core-shell particle on a micron-sized, optically-trapped spherical silica bead. The refractive indices of the silica and sulfuric acid, along with the shell thickness and bead radius were determined by reproducing Mie scattered optical white light as a function of wavelength in Mie spectroscopy. Micron-sized silica aerosols (silica beads were used as a proxy for atmospheric silica minerals) were levitated in a mist of sulfuric acid particles; continuous collection of Mie spectra throughout the collision of sulfuric acid aerosols with the optically trapped silica aerosol demonstrated that the resulting aerosol particle had a core-shell morphology. Contrastingly, the collision of aqueous sulfuric acid aerosols with optically trapped polystyrene aerosol resulted in a partially coated system. The light scattering from the optically levitated aerosols was successfully modelled to determine the diameter of the core aerosol (±0.003 μm), the shell thickness (±0.0003 μm) and the refractive index (±0.007). The experiment demonstrated that the presence of a thin film rapidly changed the light scattering of the original aerosol. When a 1.964 μm diameter silica aerosol was covered with a film of sulfuric acid 0.287 μm thick, the wavelength dependent Mie peak positions resembled sulfuric acid. Thus mineral aerosol advected into the stratosphere would likely be coated with sulfuric acid, with a core-shell morphology, and its light scattering properties would be effectively indistinguishable from a homogenous sulfuric acid aerosol if the film thickness was greater than a few 100 s of nm for UV-visible wavelengths.

Method to quantify black carbon aerosol light absorption enhancement with a mixing state index

Abstract. Large uncertainties remain when estimating the warming effects of ambient black carbon (BC) aerosols on climate. One of the key challenges in modeling the radiative effects is predicting the BC light absorption enhancement, which is mainly determined by the mass ratio (MR) of non-BC coating material to BC in the population of BC-containing aerosols. For the same MR, recent research has found that the radiative absorption enhancements by BC are also controlled by its particle-to-particle heterogeneity. In this study, the BC mixing state index (χ) is developed to quantify the dispersion of ambient black carbon aerosol mixing states based on binary systems of BC and other non-black carbon components. We demonstrate that the BC light absorption enhancement increases with χ for the same MR, which indicates that χ can be employed as a factor to constrain the light absorption enhancement of ambient BC. Our framework can be further used in the model to study the radiative effects of black carbon on climate change.

Quantifying the structural uncertainty of the aerosol mixing state representation in a modal model

Abstract. Aerosol mixing state is an important emergent property that affects aerosol radiative forcing and aerosol–cloud interactions, but it has not been easy to constrain this property globally. This study aims to verify the global distribution of aerosol mixing state represented by modal models. To quantify the aerosol mixing state, we used the aerosol mixing state indices for submicron aerosol based on the mixing of optically absorbing and non-absorbing species (χo), the mixing of primary carbonaceous and non-primary carbonaceous species (χc), and the mixing of hygroscopic and non-hygroscopic species (χh). To achieve a spatiotemporal comparison, we calculated the mixing state indices using output from the Community Earth System Model with the four-mode version of the Modal Aerosol Module (MAM4) and compared the results with the mixing state indices from a benchmark machine-learned model trained on high-detail particle-resolved simulations from the particle-resolved stochastic aerosol model PartMC-MOSAIC. The two methods yielded very different spatial patterns of the mixing state indices. In some regions, the yearly averaged χ value computed by the MAM4 model differed by up to 70 percentage points from the benchmark values. These errors tended to be zonally structured, with the MAM4 model predicting a more internally mixed aerosol at low latitudes and a more externally mixed aerosol at high latitudes compared to the benchmark. Our study quantifies potential model bias in simulating mixing state in different regions and provides insights into potential improvements to model process representation for a more realistic simulation of aerosols towards better quantification of radiative forcing and aerosol–cloud interactions.

Global Distribution of the Phase State and Mixing Times within Secondary Organic Aerosol Particles in the Troposphere Based on Room-Temperature Viscosity Measurements

Information on the global distributions of secondary organic aerosol (SOA) phase state and mixing times within SOA is needed to predict the impact of SOA on air quality, climate, and atmospheric chemistry; nevertheless, such information is rare. In this study, we developed parameterizations for viscosity as a function of relative humidity (RH) and temperature based on room-temperature viscosity data for simulated pine tree SOA and toluene SOA. The viscosity parameterizations were then used together with tropospheric RH and temperature fields to predict the SOA phase state and mixing times of water and organic molecules within SOA in the troposphere for 200 nm particles. Based on our results, the glassy state can often occur, and the mixing times of water can often exceed 1 h within SOA at altitudes >6 km. Furthermore, the mixing times of organic molecules within SOA can often exceed 1 h throughout most of the free troposphere (i.e., ≳1 km in altitude). In most of the planetary boundary layer (i.e., ≲1 km in altitude), the glassy state is not important, and the mixing times of water and organic molecules are less than 1 h. Our results are qualitatively consistent with the results from Shiraiwa et al. (Nat. Commun., 2017), although there are quantitative differences. Additional studies are needed to better understand the reasons for these differences.

Transport-driven aerosol differences above and below the canopy of a mixed deciduous forest

Abstract. Exchanges of energy and mass between the surrounding air and plant surfaces occur below, within, and above a forest's vegetative canopy. The canopy also can lead to vertical gradients in light, trace gases, oxidant availability, turbulent mixing, and properties and concentrations of organic aerosol (OA). In this study, a high-resolution time-of-flight aerosol mass spectrometer was used to measure non-refractory submicron aerosol composition and concentration above (30 m) and below (6 m) a forest canopy in a mixed deciduous forest at the Program for Research on Oxidants: PHotochemistry, Emissions, and Transport tower in northern Michigan during the summer of 2016. Three OA factors are resolved using positive matrix factorization: more-oxidized oxygenated organic aerosol (MO-OOA), isoprene-epoxydiol-derived organic aerosol (IEPOX-OA), and 91Fac (a factor characterized with a distinct fragment ion at m/z 91) from both the above- and the below-canopy inlets. MO-OOA was most strongly associated with long-range transport from more polluted regions to the south, while IEPOX-OA and 91Fac were associated with shorter-range transport and local oxidation chemistry. Overall vertical similarity in aerosol composition, degrees of oxidation, and diurnal profiles between the two inlets was observed throughout the campaign, which implies that rapid in-canopy transport of aerosols is efficient enough to cause relatively consistent vertical distributions of aerosols at this scale. However, four distinct vertical gradient episodes are identified for OA, with vertical concentration differences (above-canopy minus below-canopy concentrations) in total OA of up to 0.8 µg m−3, a value that is 42 % of the campaign average OA concentration of 1.9 µg m−3. The magnitude of these differences correlated with concurrent vertical differences in either sulfate aerosol or ozone. These differences are likely driven by a combination of long-range transport mechanisms, canopy-scale mixing, and local chemistry. These results emphasize the importance of including vertical and horizontal transport mechanisms when interpreting trace gas and aerosol data in forested environments.

Coupling interactive fire with atmospheric composition and climate in the UK Earth System Model

Abstract. Fire constitutes a key process in the Earth system (ES), being driven by climate as well as affecting the climate by changing atmospheric composition and impacting the terrestrial carbon cycle. However, studies on the effects of fires on atmospheric composition, radiative forcing and climate have been limited to date, as the current generation of ES models (ESMs) does not include fully atmosphere–composition–vegetation coupled fires feedbacks. The aim of this work is to develop and evaluate a fully coupled fire–composition–climate ES model. For this, the INteractive Fires and Emissions algoRithm for Natural envirOnments (INFERNO) fire model is coupled to the atmosphere-only configuration of the UK's Earth System Model (UKESM1). This fire–atmosphere interaction through atmospheric chemistry and aerosols allows for fire emissions to influence radiation, clouds and generally weather, which can consequently influence the meteorological drivers of fire. Additionally, INFERNO is updated based on recent developments in the literature to improve the representation of human and/or economic factors in the anthropogenic ignition and suppression of fire. This work presents an assessment of the effects of interactive fire coupling on atmospheric composition and climate compared to the standard UKESM1 configuration that uses prescribed fire emissions. Results show a similar performance when using the fire–atmosphere coupling (the “online” version of the model) when compared to the offline UKESM1 that uses prescribed fire. The model can reproduce observed present-day global fire emissions of carbon monoxide (CO) and aerosols, despite underestimating the global average burnt area. However, at a regional scale, there is an overestimation of fire emissions over Africa due to the misrepresentation of the underlying vegetation types and an underestimation over equatorial Asia due to a lack of representation of peat fires. Despite this, comparing model results with observations of CO column mixing ratio and aerosol optical depth (AOD) show that the fire–atmosphere coupled configuration has a similar performance when compared to UKESM1. In fact, including the interactive biomass burning emissions improves the interannual CO atmospheric column variability and consequently its seasonality over the main biomass burning regions – Africa and South America. Similarly, for aerosols, the AOD results broadly agree with the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Aerosol Robotic Network (AERONET) observations.