Particle Light Absorption Research Articles

Wintertime Diurnal Variation in Absorption Coefficient of Brown Carbon Associated with the Molecular Marker of Levoglucosan

This study investigated the aerosol particle properties and light absorption properties of brown carbon (BrC) by utilizing a seven-wavelength aethalometer, and analyzed NH4+, NO3−, SO42−, K+, K, organic carbon, elemental carbon, levoglucosan, and mannosan in PM2.5. The research was conducted in a rural area of Jeonnam, South Korea, during the winter season. In addition, the dithiothreitol assay-oxidative potential normalized to 9,10-phenanthrenequinone (QDTT-OP) was investigated throughout the study period. The absorption coefficient was found to be 2.6 to 5.6 times higher at 370 nm compared to 880 nm, suggesting the presence of light-absorbing substances in addition to black carbon (BC) particles. The estimated absorption coefficient of BrC370 was 29.9% of the total light absorption coefficient at 370 nm. Furthermore, BrC370 exhibited a strong affinity with levoglucosan while showing a weak correlation with K+, confirming the suitability of levoglucosan as a tracer for biomass burning. The QDTT-OP was 5.3 nM m−3, and highly correlated with the carbonaceous components levoglucosan and mannosan, suggesting a relatively high contribution of biomass combustion emissions to oxidative potential. Further research should be conducted to assess the health risks associated with future PM2.5 exposure related to biomass burning in the atmosphere.

Significant contribution of fractal morphology to aerosol light absorption in polluted environments dominated by black carbon (BC)

In recent years, researchers have emphasized the use of fractal aggregate morphology instead of the core-shell morphology in global climate models for estimating black carbon (BC) forcing. This study confirms that fractal morphology plays an important role in reducing the overestimation of aerosol light absorption calculations in the case of an urban polluted environment. During periods of high anthropogenic BC emissions at Delhi, the particle light absorption is overestimated by 50 to 200% by assumptions of both external mixing and internal core-shell mixing. While incorporating the aggregate morphology model into light absorption simulations is beneficial in such cases, it comes with a high computational burden. To address this, we propose a metric known as morphology index (MI). This index distributes the weightage between the two extreme cases of core-shell and fractal aggregate to obtain accurate particle light absorption. Long-range transported aerosols were estimated to have an MI of 0.78, and fresh local emissions had an MI of 0.48. A BC-based aerosol classification approach was developed to determine the most relevant particle size mode for light absorption. The method is based on patterns found between the correlations of the BC mass concentrations and aerosol number concentrations at the different particles sizes (BC-size correlation spectra). BC-size correlation spectra are introduced as a concept that may be used (i) independently to understand the size-dependent heterogeneous distribution of aerosol light absorption and (ii) in conjunction with MI to accurately model the optical properties of aerosols in different BC regimes.

Contribution of brown carbon to light absorption in emissions of European residential biomass combustion appliances

Abstract. Residential biomass combustion significantly contributes to light-absorbing carbonaceous aerosols in the atmosphere, impacting the earth's radiative balance at regional and global levels. This study investigates the contribution of brown carbon (BrC) to the total particulate light absorption in the wavelength range of 370–950 nm (BrC370–950) and the particulate absorption Ångström exponents (AAE470/950) in 15 different European residential combustion appliances using a variety of wood-based fuels. BrC370–950 was estimated to be from 1 % to 21 % for wood log stoves and 10 % for a fully automatized residential pellet boiler. Correlations between the ratio of organic to elemental carbon (OC / EC) and BrC370–950 indicated that a one-unit increase in OC / EC corresponded to approximately a 14 % increase in BrC370–950. Additionally, BrC370–950 was clearly influenced by the fuel moisture content and the combustion efficiency, while the effect of the combustion appliance type was less prominent. AAE470/950 of wood log combustion aerosols ranged from 1.06 to 1.61. By examining the correlation between AAE470/950 and OC / EC, an AAE470/950 close to unity was found for pure black carbon (BC) particles originating from residential wood combustion. This supports the common assumption used to differentiate light absorption caused by BC and BrC. Moreover, diesel aerosols exhibited an AAE470/950 of 1.02, with BrC contributing only 0.66 % to the total absorption, aligning with the assumption employed in source apportionment. These findings provide important data to assess the BrC from residential wood combustion with different emission characteristics and confirm that BrC can be a major contributor to particulate UV and near-UV light absorption for northern European wood stove emissions with relatively high OC / EC ratios.

Far-field signature of fire in low gravity: Influence of ambient oxygen content and pressure on size distribution of smoke particles

Fire detection in space habitats is hindered by the unique characteristics of smoke particles released by weakly buoyant flames. For the first time, non-invasive measurements of particle concentration, size, and light absorption properties are performed in the downstream flow of a flame spreading in microgravity. The studied flame spreads over Low Density PolyEthylene (LDPE) coated Nickel/Chrome (NiCr) wires in an opposed oxidizer flow. The far-field signature can then be contrasted with previous measurements performed over the same configurations and related to the morphology of soot particles sampled in and behind the flame.Following measurements regarding the impact of gravity, the influence of ambient pressure and oxygen content on the characteristics of the particles is reported in microgravity. Increased pressure boosts the soot production rate, leading to higher concentration levels of particles detected for any class of particle size. Higher pressure also causes larger aggregates that exhibit a higher level of polydispersity among the constituting primary particles. This tends to enhance light absorption, more specifically at larger particle size. Less intuitively, increased oxygen content accelerates the pyrolysis rate, therefore hastening soot particles’ maturity, and ultimately increasing the detected soot concentration. In addition, enhanced oxygen content reduces organic carbon within particles, boosting light absorption regardless of the particle size. The far-field signature and its sensitivity to the ambient conditions are in decent agreement with observations of soot particles collected at the trailing edge of the flame. As a result, combining higher oxygen content and lower pressure in future space habitats as projected by the main space agencies can cancel out the effect on the detection threshold of a given flame if this threshold only includes the concentration level.

Applicability of aethalometers for monitoring diesel particulate matter concentrations and exposure in underground mines

Occupational exposure to diesel exhaust is regulated by legislation in Europe owing to its carcinogenic effects on humans. In underground mines, exposure to diesel exhaust requires regular monitoring. In this work, we investigate the usage of aethalometer AE33 and portable micro-aethalometer MA200 to assess occupational exposure to diesel exhaust in two underground mines. These instruments provide continuous data on wavelength-dependent particle light absorption, and based on this, equivalent black carbon (eBC) particle concentrations and potential sources. Both aethalometers correlated well with the thermal-optical elemental carbon analysis. Time-resolved aethalometer data revealed work-activity-dependent eBC concentration patterns that can be beneficial for identifying work phases that are significant for occupational exposure. In particular, high eBC peak exposures were observed for workers near load haul dumping areas. The diesel soot mass absorption cross-sections determined were similar for both mines. The absorption Ångström exponent determined from the aethalometer data was suitable for detecting and assessing the contributions of other potential sources to eBC concentrations, such as tobacco smoke, which is often prevalent in work environments. Overall, the portable micro-aethalometers proved to be suitable for monitoring occupational diesel exhaust exposure and can be useful for designing targeted exposure prevention measures in mining environments.

Impact of 2020 COVID-19 lockdowns on particulate air pollution across Europe

Abstract. To fight against the first wave of coronavirus disease 2019 (COVID-19) in 2020, lockdown measures were implemented in most European countries. These lockdowns had well-documented effects on human mobility. We assessed the impact of the lockdown implementation and relaxation on air pollution by comparing daily particulate matter (PM), nitrogen dioxide (NO2) and ozone (O3) concentrations, as well as particle number size distributions (PNSDs) and particle light absorption coefficient in situ measurement data, with values that would have been expected if no COVID-19 epidemic had occurred at 28 sites across Europe for the period 17 February–31 May 2020. Expected PM, NO2 and O3 concentrations were calculated from the 2020 Copernicus Atmosphere Monitoring Service (CAMS) ensemble forecasts, combined with 2019 CAMS ensemble forecasts and measurement data. On average, lockdown implementations did not lead to a decrease in PM2.5 mass concentrations at urban sites, while relaxations resulted in a +26 ± 21 % rebound. The impacts of lockdown implementation and relaxation on NO2 concentrations were more consistent (−29 ± 17 and +31 ± 30 %, respectively). The implementation of the lockdown measures also induced statistically significant increases in O3 concentrations at half of all sites (+13 % on average). An enhanced oxidising capacity of the atmosphere could have boosted the production of secondary aerosol at those places. By comparison with 2017–2019 measurement data, a significant change in the relative contributions of wood and fossil fuel burning to the concentration of black carbon during the lockdown was detected at 7 out of 14 sites. The contribution of particles smaller than 70 nm to the total number of particles significantly also changed at most of the urban sites, with a mean decrease of −7 ± 5 % coinciding with the lockdown implementation. Our study shows that the response of PM2.5 and PM10 mass concentrations to lockdown measures was not systematic at various sites across Europe for multiple reasons, the relationship between road traffic intensity and particulate air pollution being more complex than expected.

Photochemical transformation and secondary aerosol formation potential of Euro6 gasoline and diesel passenger car exhaust emissions

Traffic remains a major source of urban air pollution although emission regulations have led to significant reductions in exhaust emissions of new vehicles. In this work the photochemical transformation of exhaust emissions from gasoline and diesel passenger vehicles compliant with the current European ‘Euro6’ emission standard and operated with traditional and alternative fuels was investigated using an environmental chamber. By assessing four different engine operation conditions, we show that vehicle operation notably affects the exhaust composition and secondary aerosol formation potential. For the gasoline vehicle, secondary aerosols dominate the total particulate emissions. In contrast, we observe no substantial secondary aerosol formation for exhaust emissions of a Euro6-level diesel vehicle. High engine load operation and cold start of the gasoline vehicle led to 11–470-fold particulate mass enhancement, while for moderate driving conditions the enhancement ratio was below 2. High aerosol enhancements also led to strong increases in particle light absorption. The results underline the necessity for future directives to include the emission components leading to secondary pollution, in addition to the freshly emitted pollutants. The link observed between secondary organic aerosol (SOA) formation and gaseous aromatic hydrocarbon emissions suggests that monitoring and limiting these gaseous species can provide an indirect regulation for SOA. Additionally, ammonia released as a byproduct of the gasoline vehicle is confirmed as an important precursor for secondary aerosols.

Importance of size representation and morphology in modelling optical properties of black carbon: comparison between laboratory measurements and model simulations

Abstract. Black carbon (BC) from incomplete combustion of biomass or fossil fuels is the strongest absorbing aerosol component in the atmosphere. Optical properties of BC are essential in climate models for quantification of their impact on radiative forcing. The global climate models, however, consider BC to be spherical particles, which causes uncertainties in their optical properties. Based on this, an increasing number of model-based studies provide databases and parameterization schemes for the optical properties of BC, using more realistic fractal aggregate morphologies. In this study, the reliability of the different modelling techniques of BC was investigated by comparing them to laboratory measurements. The modelling techniques were examined for bare BC particles in the first step and for BC particles with organic material in the second step. A total of six morphological representations of BC particles were compared, three each for spherical and fractal aggregate morphologies. In general, the aggregate representation performed well for modelling the particle light absorption coefficient σabs, single-scattering albedo SSA, and mass absorption cross-section MACBC for laboratory-generated BC particles with volume mean mobility diameters dp,V larger than 100 nm. However, for modelling Ångström absorption exponent AAE, it was difficult to suggest a method due to size dependence, although the spherical assumption was in better agreement in some cases. The BC fractal aggregates are usually modelled using monodispersed particles, since their optical simulations are computationally expensive. In such studies, the modelled optical properties showed a 25 % uncertainty in using the monodisperse size method. It is shown that using the polydisperse size distribution in combination with fractal aggregate morphology reduces the uncertainty in measured σabs to 10 % for particles with dp,V between 60–160 nm. Furthermore, the sensitivities of the BC optical properties to the various model input parameters such as the real and imaginary parts of the refractive index (mre and mim), the fractal dimension (Df), and the primary particle radius (app) of an aggregate were investigated. When the BC particle is small and rather fresh, the change in the Df had relatively little effect on the optical properties. There was, however, a significant relationship between app and the particle light scattering, which increased by a factor of up to 6 with increasing total particle size. The modelled optical properties of BC are well aligned with laboratory-measured values when the following assumptions are used in the fractal aggregate representation: mre between 1.6 and 2, mim between 0.50 and 1, Df from 1.7 to 1.9, and app between 10 and 14 nm. Overall, this study provides experimental support for emphasizing the importance of an appropriate size representation (polydisperse size method) and an appropriate morphological representation for optical modelling and parameterization scheme development of BC.

Secondary organic aerosol formation from atmospheric reactions of anisole and associated health effects

Anisole (methoxybenzene) represents an important marker compound of lignin pyrolysis and a starting material for many chemical products. In this study, secondary organic aerosols (SOA) formed by anisole via various atmospheric processes, including homogeneous photooxidation with varying levels of OH• and NOx and subsequent heterogeneous NO3• dark reactions, were investigated. The yields of anisole SOA, particle-bound organoperoxides, particle-induced oxidative potential (OP), and cytotoxicity were characterized in view of the atmospheric fate of the anisole precursor. Anisole SOA yields ranged between 0.12 and 0.35, depending on the reaction pathways and aging degrees. Chemical analysis of the SOA suggests that cleavage of the benzene ring is the main reaction channel in the photooxidation of anisole to produce low-volatility, highly oxygenated small molecules.Fresh anisole SOA from OH• photooxidation are more light-absorbing and have higher OP and organoperoxide content. The high correlation between SOA OP and organoperoxide content decreases exponentially with the degree of OH• aging. However, the contribution of organoperoxides to OP is minor (<4%), suggesting that other, non-peroxide oxidizers play a central role in anisole SOA OP. The particle-induced OP and particulate organoperoxides yield both reach a maximum value after ∼2 days’ of photooxidation, implicating the potential long impact of anisole during atmospheric transport. NOx-involved photooxidation and nighttime NO3• reactions facilitate organic nitrate formation and enhance particle light absorption. High NOx levels suppress anisole SOA formation and organoperoxides yield in photooxidation, with decreased aerosol OP and cellular oxidative stress. In contrast, nighttime aging significantly increases the SOA toxicity and reactive oxygen species (ROS) generation in lung cells. These dynamic properties and the toxicity of anisole SOA advocate consideration of the complicated and consecutive aging processes in depicting the fate of VOCs and assessing the related effects in the atmosphere.

Characteristics and evolution of brown carbon in western United States wildfires

Abstract. Brown carbon (BrC) associated with aerosol particles in western United States wildfires was measured between July and August 2019 aboard the NASA DC-8 research aircraft during the Fire Influence on Regional to Global Environments and Air Quality (FIREX-AQ) study. Two BrC measurement methods are investigated, highly spectrally resolved light absorption in solvent (water and methanol) extracts of particles collected on filters and in situ bulk aerosol particle light absorption measured at three wavelengths (405, 532 and 664 nm) with a photoacoustic spectrometer (PAS). A light-absorption closure analysis for wavelengths between 300 and 700 nm was performed. The combined light absorption of particle pure black carbon material, including enhancements due to internally mixed materials, plus soluble BrC and a Mie-predicted factor for conversion of soluble BrC to aerosol particle BrC, was compared to absorption spectra from a power law fit to the three PAS wavelengths. For the various parameters used, at a wavelength of roughly 400 nm they agreed, at lower wavelengths the individual component-predicted particle light absorption significantly exceeded the PAS and at higher wavelengths the PAS absorption was consistently higher but more variable. Limitations with extrapolation of PAS data to wavelengths below 405 nm and missing BrC species of low solubility that more strongly absorb at higher wavelengths may account for the differences. Based on measurements closest to fires, the emission ratio of PAS-measured BrC at 405 nm relative to carbon monoxide (CO) was on average 0.13 Mm−1 ppbv−1; emission ratios for soluble BrC are also provided. As the smoke moved away from the burning regions, the evolution over time of BrC was observed to be highly complex; BrC enhancement, depletion or constant levels with age were all observed in the first 8 h after emission in different plumes. Within 8 h following emissions, 4-nitrocatechol, a well-characterized BrC chromophore commonly found in smoke particles, was largely depleted relative to the bulk BrC. In a descending plume where temperature increased by 15 K, 4-nitrocatechol dropped, possibly due to temperature-driven evaporation, but bulk BrC remained largely unchanged. Evidence was found for reactions with ozone, or related species, as a pathway for secondary formation of BrC under both low and high oxides of nitrogen (NOx) conditions, while BrC was also observed to be bleached in regions of higher ozone and low NOx, consistent with complex behaviors of BrC observed in laboratory studies. Although the evolution of smoke in the first hours following emission is highly variable, a limited number of measurements of more aged smoke (15 to 30 h) indicate a net loss of BrC. It is yet to be determined how the near-field BrC evolution in smoke affects the characteristics of smoke over longer timescales and spatial scales, where its environmental impacts are likely to be greater.

Formation and Evolution of Catechol-Derived SOA Mass, Composition, Volatility, and Light Absorption

Phenolic compounds emitted from wildfires contribute to secondary organic aerosol (SOA) and brown carbon (BrC) upon oxidation initiated by hydroxyl (OH) and nitrate radicals (NO3). We conducted a set of laboratory chamber experiments to study catechol oxidation by OH and NO3 with a focus on the associated SOA formation and evolution under conditions relevant to fresh wildfire plumes. Oxidation products in both gas and particle phases as well as SOA volatility were measured using an iodide-adduct high-resolution time-of-flight chemical ionization mass spectrometer coupled with the filter inlet for gases and aerosols (FIGAERO-CIMS). Nitrocatechol (C6H5NO4) was the dominant particle-phase compound in both OH-initiated and NO3-initiated oxidation and was strongly associated with particle light absorption at 405 nm, consistent with BrC. Maximum SOA mass yields, ranging from 0.1 to 1.6 for the OH- and NO3-driven experiments, respectively, varied with the net formation of nitrocatechol. Gas–particle partitioning measurements implied the effective saturation vapor concentration, c*, of nitrocatechol is 12 μg m–3 for the OH-initiated experiment and 2.4 μg m–3 for the NO3-initiated experiments, both far lower than group contribution method estimates, which ranged from 1.8 × 102 to 8.5 × 108 μg m–3. In extended photochemical aging experiments, wall-loss-corrected photochemical lifetimes of BrC in the chamber were 17.4 ± 0.8 and 12.4 ± 0.1 h, while particulate nitrocatechol had lifetimes of 21 ± 8 and 6.9 ± 0.6 h for OH-initiated and NO3-initiated conditions, respectively. Implications for phenolic-derived SOA and BrC evolution in wildfire plumes are discussed.

Aerosol particle properties at a remote tropical rainforest in Borneo

This paper aims to investigate aerosol particle properties and their seasonal variabilities at a remote tropical forest site. It also attempts to study the relationship between aerosol particles and dynamic atmospheric processes that modulate aerosol variability. Mass concentrations for particles smaller than 10 μm aerodynamic diameter (PM10) and optical aerosol particle properties were measured at Danum Valley tropical rainforest in Borneo Island. The particle mass concentrations were measured using a Tapered Element Oscillating Microbalance (TEOM). Measurements of aerosol particle optical properties, i.e., the particle light absorption and scattering coefficients, were conducted using a Multi-Angle Absorption Photometer (MAAP) and nephelometer, respectively. The single scattering albedo (SSA) and scattering Angstrom exponent (SAE) were calculated from the aerosol scattering and absorption coefficients. The results showed that the daily average of PM10 mass concentrations was 12.3 μgm−3, while the particle light absorption coefficients at wavelength 637 nm and scattering coefficients at wavelength 525 nm were reported as 2.7 Mm−1 and 21.7 Mm−1, respectively. The daily average SSA and SAE recorded were 0.89 and 1.44, respectively. The SSA showed no seasonal variations while higher SAE was observed during the dry season due to the influence of biomass burning originating from the southern region of Borneo. The wavelet analysis showed strong intra-seasonal cycles (12–20 and 32–64 days) which suggest the influence of Quasi-BiWeekly (QBW) oscillation and Madden-Julian Oscillation (MJO) on the aerosol variability over the tropics. The analysis also showed seasonal and annual variability bands, generally associated with the dry and wet seasons over the region.

Influence of organic aerosol molecular composition on particle absorptive properties in autumn Beijing

Abstract. Organic aerosol (OA) is a major component of fine particulate matter (PM), affecting air quality, human health, and the climate. The absorptive and reflective behavior of OA components contributes to determining particle optical properties and thus their effects on the radiative budget of the troposphere. There is limited knowledge on the influence of the molecular composition of OA on particle optical properties in the polluted urban environment. In this study, we characterized the molecular composition of oxygenated OA collected on filter samples in the autumn of 2018 in Beijing, China, with a filter inlet for gases and aerosols coupled to a high-resolution time-of-flight chemical ionization mass spectrometer (FIGAERO–CIMS). Three haze episodes occurred during our sampling period with daily maximum concentrations of OA of 50, 30, and 55 µg m−3. We found that the signal intensities of dicarboxylic acids and sulfur-containing compounds increased during the two more intense haze episodes, while the relative contributions of wood-burning markers and other aromatic compounds were enhanced during the cleaner periods. We further assessed the optical properties of oxygenated OA components by combining detailed chemical composition measurements with collocated particle light absorption measurements. We show that light absorption enhancement (Eabs) of black carbon (BC) was mostly related to more oxygenated OA (e.g., dicarboxylic acids), likely formed in aqueous-phase reactions during the intense haze periods with higher relative humidity, and speculate that they might contribute to lensing effects. Aromatics and nitro-aromatics (e.g., nitrocatechol and its derivatives) were mostly related to a high light absorption coefficient (babs) consistent with light-absorbing (brown) carbon (BrC). Our results provide information on oxygenated OA components at the molecular level associated with BrC and BC particle light absorption and can serve as a basis for further studies on the effects of anthropogenic OA on radiative forcing in the urban environment.

Measurement report: Comparison of airborne, in situ measured, lidar-based, and modeled aerosol optical properties in the central European background – identifying sources of deviations

Abstract. A unique data set derived from remote sensing, airborne, and ground-based in situ measurements is presented. This measurement report highlights the known complexity of comparing multiple aerosol optical parameters examined with different approaches considering different states of humidification and atmospheric aerosol concentrations. Mie-theory-based modeled aerosol optical properties are compared with the respective results of airborne and ground-based in situ measurements and remote sensing (lidar and photometer) performed at the rural central European observatory at Melpitz, Germany. Calculated extinction-to-backscatter ratios (lidar ratios) were in the range of previously reported values. However, the lidar ratio is a function of the aerosol type and the relative humidity. The particle lidar ratio (LR) dependence on relative humidity was quantified and followed the trend found in previous studies. We present a fit function for the lidar wavelengths of 355, 532, and 1064 nm with an underlying equation of fLR(RH, γ(λ))=fLR(RH=0,λ)×(1-RH)-γ(λ), with the derived estimates of γ(355 nm) = 0.29 (±0.01), γ(532 nm) = 0.48 (±0.01), and γ(1064 nm) = 0.31 (±0.01) for central European aerosol. This parameterization might be used in the data analysis of elastic-backscatter lidar observations or lidar-ratio-based aerosol typing efforts. Our study shows that the used aerosol model could reproduce the in situ measurements of the aerosol particle light extinction coefficients (measured at dry conditions) within 13 %. Although the model reproduced the in situ measured aerosol particle light absorption coefficients within a reasonable range, we identified many sources for significant uncertainties in the simulations, such as the unknown aerosol mixing state, brown carbon (organic material) fraction, and the unknown aerosol mixing state wavelength-dependent refractive index. The modeled ambient-state aerosol particle light extinction and backscatter coefficients were smaller than the measured ones. However, depending on the prevailing aerosol conditions, an overlap of the uncertainty ranges of both approaches was achieved.

Wildfires and wood stoves: Woodsmoke toxicity and chemical characterization study in the north-western United States

PM2.5 is the most monitored air pollutant for which EPA has set national ambient air quality standards (NAAQS). As such, it is the pollutant on which the Air Quality Index (AQI) is most often based. PM2.5 and PM10 are the only criteria pollutant whose composition, and therefore toxicity varies. The PM2.5 AQI does not account for chemical composition. In areas where woodsmoke is the dominant PM2.5 source, coemitted hazardous air pollutants (HAPs) could impact community health differently than indicated by PM2.5 based AQI. PM2.5, carbon monoxide (CO), and particle light absorption were measured continuously from August 2018 through May 2019 in a suburban community where woodsmoke contributed the majority of ambient PM2.5. Air samples were also collected at least every 6 days at the site and analyzed for a suite of hazardous air pollutants (HAPs). EPA's positive matrix factorization (PMF) model 5.0 was used to identify the primary source contributors to local air pollution and apportion what fraction of each pollutant was from woodsmoke. Both measurements and the PMF model result showed significant chemical distinction between wood stove and wildfire smoke. Wildfire smoke contained significantly less CO and organic compounds than wood stove smoke relative to measured PM2.5. Comparing select HAPs to ambient CO concentration indicated atmospheric oxidation depleted PAHs in the wildfire smoke, although the relative amount of UV absorbing organic carbon did not change. HAPs most strongly associated with wood combustion were assessed relative to their individual cancerous and non-cancerous screening levels, as well as the PM2.5 and CO NAAQS.

Bias in quantification of light absorption enhancement of black carbon aerosol coated with low-volatility brown carbon

Brown carbon (BrC) is an optically defined class of organic carbon (OC) which strongly absorbs light at shorter visible and ultraviolet-A (UVA) wavelengths. Both light absorbing and non-absorbing OC have been found to coat black carbon (BC) and could modulate the optical properties of BC. Thermodenuders are conventionally used in conjunction with instruments measuring particle light absorption, such as photoacoustic spectrometers, to parametrize enhanced BC light absorption (Eabs) due to OC. This method can introduce unquantified measurement artifacts because thermodenuders do not remove low-volatility compounds at the temperatures they are commonly operated at and due to temperature-dependent loss of particles within the instrument. These artifacts could lead to errors in accurately estimating Eabs for coated BC particles. The value of Eabs can also be estimated by comparing the mass absorption cross-section (MAC) of coated BC aerosol to literature-based MAC values of uncoated BC. In this study, we use two integrated photoacoustic-nephelometer spectrometers, operating at wavelengths of 375 nm and 532 nm, respectively, to quantify the differences and errors associated with measuring Eabs using these two methods. Our results indicate differences ranging from 25% to 65% for Eabs measured using both methods at 375 nm. We observed little to no enhancement at either wavelength using the thermodenuder method. In contrast, the Eabs value increased with the OC/BC ratio at 375 nm using the literature-based MAC method. The difference between the two methods was attributed to the presence of low-volatility brown carbon, and these results were corroborated using discrete dipole approximation calculations. Theoretical calculations predicted that these low-volatility OC could have values of the imaginary part of the refractive index up to 0.32 at a wavelength of 375 nm, which is in line with previous studies that found large absorption by low-volatility organics.Copyright © 2021 American Association for Aerosol Research

Using correlations between observed equivalent black carbon and aerosol size distribution to derive size resolved BC mass concentration: a method applied on long-term observations performed at Zeppelin station, Ny-Ålesund, Svalbard

The aim of this study was to explore particle size dependent properties by combining long-term observations of equivalent black carbon (eBC) and number size distributions to investigate their correlation as function of particle size. The work was conducted in two main parts. The first part consisted of a short laboratory experiment to compare observed total particle light absorption (σabs) with that observed according to particle size by using a combination of a Differential Mobility Analyzer (DMA) and a Particle Soot Absorption Photometer (PSAP). The laboratory study confirmed strong similarities between the observed and derived σabs. In the second part the statistical approach using correlation between the σabs and the dN of each bin of the number size distribution was tested on long-term data ranging from 2002 to 2010 observed at Zeppelin station, Ny-Ålesund Svalbard. The data was clustered according to the number size distribution and grouped in four major categories: Washout, Nucleation, Intermediate and Polluted. Each category presented different features with respect to the derived eBC mass distributions, the Intermediate category showed similarities to the few available Single Particle Soot Photometer (SP2) observations in the Arctic. Overall, the statistical distribution of eBC, according to particle size, presented a larger dynamical range in the location of the mode(s). To check for consistency, the eBC mass distributions were transformed into number based eBC size distribution and compared to the observed total number size distribution. Whereas the Washout, Nucleation and Intermediate categories presented plausible number distributions, the Polluted category displayed a mode at small sizes (about 50 nm) that was significantly exaggerated.

Mass-specific light absorption coefficients of mineral particles in aqueous suspension for the ultraviolet to near-infrared radiation spectral region (200-2500 nm).

Light absorption by in-water suspended natural particles in the near-infrared radiation (NIR; 780-3000 nm) region has received little attention. Minerogenic matter is thought to be one source for NIR light absorption in aquatic environments. Here, mass-specific particulate light absorption coefficients of several particulate single minerals and mineral samples for the spectral range of 200-2500 nm are presented. The current methodology allows very sensitive measurements of particle suspension with a detection limit of about 2×10-6m2g-1 for the mass-specific absorption coefficient. Except for one, all mineral materials examined possessed significant light absorption throughout the full spectral range considered. The spectra revealed absorption features of specific elements (like iron) and from water structures (H2O, O-H bonds) in the mineral or crystal structure that have been known from reflectance measurements of minerals. The specific absorption in the NIR was as high as 0.02m2g-1 for laterite earths samples, but also below the detection limit for a steatite sample in a narrow spectral region (1600-1800 nm). The specific absorption by mineral particles in the NIR was, hence, highly variable from strong absorbing black minerals (magnetite) to low absorbing white clays. The information in the absorption coefficient spectrum can be used not only to identify specific mineral in natural particle assemblages but also to quantify their contribution to total particulate absorption in the NIR.

Vertical Distribution of Bio-Optical Properties of the Azov – Black Sea Basin Waters in April – May, 2019

Purpose. The work is aimed at investigating spatial distribution of the chlorophyll a concentration and the spectral light absorption coefficients by all optically active components in the Azov and Black seas in spring, when the seawater hydrophysical structure changes. Methods and Results. The data collected in the 106th scientific cruise of R/V Professor Vodyanitsky in April 19 – May 10, 2019 were used. The chlorophyll a concentration was measured by the spectrophotometric method. The spectral light absorption coefficients were determined in accordance with the NASA protocol 2018. The optical measurements were performed using the dual-beam spectrophotometer Lambda 35 (PerkinElmer). It was shown that in the surface layer of the Black Sea, the chlorophyll a concentration varied from 0.21 to 1.2 mg/m3. At some stations in the deep-water region, the increased values of this parameter were observed in the lower part of the euphotic zone that was associated with the beginning of seasonal water stratification due to the surface water heating. At these stations, the phytoplankton absorption spectra were more smoothed in the lower part of the euphotic zone than those in the upper layer. In the deep-water region, the non-algal particles contribution to the total particulate light absorption at wavelength 438 nm changed with depth from 40 ± 15 % at the surface to 29 ± 12 % near the bottom of the euphotic zone; whereas in the coastal waters this parameter was almost unchangeable within the water column (54 ± 11 %). No significant change of the colored dissolved organic matter contribution to the total light absorption with depth was revealed (69% on average). In the Sea of Azov, vertical distribution both of the chlorophyll a concentration (6.2 mg/m3 on average) and the spectral light absorption coefficients by all the optically active components was uniform. The non-algal particles contribution to the particulate light absorption was 40 ± 14 %, and the colored dissolved organic matter contribution to the total light absorption constituted 52 ± 6 %. Conclusions. New data on spatial distribution of the chlorophyll a concentration and the spectral light absorption coefficients by the optically active components in the Black and Azov seas were obtained for the spring period when the seawater hydrophysical characteristics changed.

The Evolution of Icelandic Volcano Emissions, as Observed From Space in the Era of NASA's Earth Observing System (EOS)

AbstractVolcanoes are natural phenomena that have global environmental impacts. Satellite remote sensing can help classify volcanic eruptions and track the dispersion of emissions. We assess multiple volcanic eruptions in Iceland (Eyjafjallajökull 2010, Grímsvötn 2011, and Holuhraun 2014–2015), using space‐borne observations to infer information about the geological dynamics of each volcano and the properties and evolution of plume particles. We derive qualitative constraints on plume particle size, shape, and light‐absorption characteristics from Multiangle Imaging SpectroRadiometer (MISR) space‐borne imagery. With the MISR Research Algorithm (RA), we distinguish sulfate/water‐dominated volcanic plumes from Holuhraun and ash‐dominated plumes from Eyjafjallajökull and Grímsvötn, and even identify subtler changes in ash particle size and light‐absorption within plumes. Additionally, plume heights are retrieved geometrically from MISR. These are combined with surface thermal anomalies from the MODerate resolution Imaging Spectroradiometer (MODIS) and SO2 concentrations derived from the Ozone Monitoring Instrument (OMI) to synthesize eruption remote‐sensing chronologies. Signals related to differences in particle properties are identified and linked to evolving magma composition at Eyjafjallajökull. The results illustrate the potential to distinguish qualitative differences in eruptive magma composition based on particle light absorption and plume profile from remote‐sensing. For the sulfate‐rich Holuhraun plumes, the influence of aerosol hygroscopic growth during transport is inferred from such data. Three processes appear to dominate plume evolution in Iceland: downwind aerosol formation, particle hydration, and particle deposition. This work demonstrates enhanced MISR capabilities and, more generally, remote‐sensing analysis that can be applied globally, especially where suborbital volcano observations are limited or entirely absent.