Light-absorbing Carbonaceous Aerosols Research Articles

Long-term spatial distribution and implication of black and brown carbon in the Tibetan Plateau

Black carbon (BC) and brown carbon (BrC) over the high-altitude Tibetan Plateau (TP) can significantly influence regional and global climate change as well as glacial melting. However, obtaining plateau-scale in situ observations is challenging due to its high altitude. By integrating reanalysis data with on-site measurements, the spatial distribution of BC and BrC can be accurately estimated using the random forest algorithm (RF). In our study, the on-site observations of BC and BrC were successively conducted at four sites from 2018 to 2021. Ground-level BC and BrC concentrations were then obtained at a spatial resolution of 0.25° × 0.25° for three periods (including Periods-1980, 2000, and 2020) using RF and multi-source data. The highest annual concentrations of BC (1363.9 ± 338.7 ng/m3) and BrC (372.1 ± 96.2 ng/m3) were observed during Period-2000. BC contributed a dominant proportion of carbonaceous aerosol, with concentrations 3–4 times higher than those of BrC across the three periods. The ratios of BrC to BC decreased from Period-1980 to Period-2020, indicating the increasing importance of BC over the TP. Spatial distributions of plateau-scale BC and BrC concentrations showed heightened levels in the southeastern TP, particularly during Period-2000. These findings significantly enhance our understanding of the spatio-temporal distribution of light-absorbing carbonaceous aerosol over the TP.

Assessment of light-absorbing carbonaceous aerosol origins and properties at the ATOLL site in northern France

Abstract. Understanding the lifecycle of light-absorbing carbonaceous aerosols, from emission to deposition, is critical for assessing their climate impact. This study integrated multi-year aerosol observations from the ATOLL (ATmospheric Observations in liLLe, northern France) platform, with air mass back trajectories and emission inventory as a newly developed “INTERPLAY” (IN-siTu obsERvations, hysPLit, And emission inventorY) approach. Applied to black carbon (BC), the method apportioned source contributions (shipping, vehicular, residential heating, industrial) and studied aerosol aging effects, notably on the brown carbon (BrC) component. Results estimate that, throughout the year, vehicular traffic dominated BC (31 %), followed by shipping (25 %, of which one-third was from canals/rivers) and residential heating (21 %). Comparing INTERPLAY results with the aethalometer model highlights that the “residential sector” BC can be entirely apportioned to BC from wood burning (BCwb), notably in winter, while vehicular traffic corresponds to only about 41 % of BC fossil fuel (BCff) at the ATOLL site, the rest being apportioned to shipping (33 %) and industrial (23 %) emissions. Thus, vehicular traffic and BCff should not be used interchangeably, particularly in regions near intense maritime traffic. Concerning BrC, our analysis confirms a dominant role of residential heating. Focusing on winter, results suggest a considerable decrease in the BrC component only 24 h after emission, with fresh residential emissions being responsible for 72 % of BrC absorption at ATOLL. The results from this study allow for an improved understanding of sources and atmospheric dynamics of light-absorbing carbonaceous aerosols in northern France, being crucial for both source abatement strategies as well as a better assessment of their climate impact.

Predicted Concentrations and Optical Properties of Brown Carbon from Biomass Burning over Europe.

Black carbon (BC) and brown carbon (BrC) are light-absorbing carbonaceous aerosol components that can contribute to radiative forcing and thus affect the climate. In this study, we focus on the modification of aerosol optical properties associated with BrC emissions from biomass burning. BrC is simulated with the introduction of three new species in the three-dimensional chemical transport model PMCAMx-SR, two primary-absorbing (inert and reactive BrC) species, and one "photobleached" BrC species. 10% of the emitted BrC is assumed to be inert, and the rest to be reactive and able to undergo photobleaching. The scattering and absorption coefficients of the aerosol for different wavelengths are estimated by using Mie theory. BrC causes a 5-15% increase of the aerosol optical depth at 550 nm in regions affected by fires and can increase light absorption by up to 12% compared to when there is no BrC. During major biomass burning events, the absorption of BrC can reach up to 13% of that of BC at 550 nm and 25% at 440 nm. The ability of the model to reproduce measured absorption is improved when BrC is added to the light-absorbing components.

Direct radiative forcing of light-absorbing carbonaceous aerosols in China

China is an important emitter of light-absorbing carbonaceous aerosols (LACs), including black carbon (BC) and brown carbon (BrC). Currently, there are large uncertainties in model-estimated direct radiative forcing (DRF) of LACs, partially due to the poor understanding of the emissions and optical properties of LACs. In this study, we estimated the DRF of LACs over China during the implementation of the Air Pollution Prevention and Control Action Plan (APPCAP) using the global chemical transport model (GEOS-Chem) coupled with the Rapid Radiative Transfer Model of GCMs (RRTMG). We updated the refractive index of BC, includedbiomass burning (BB) sources, biofuel (BF) and coal combustion (CC) sources in the residential sector as BrC emission sources and the optical properties were updated, which were not fully considered in the previous model studies. Our results showed that model could reasonably capture the spatial and temporal variations of LACs in China with the correlation coefficients between model simulated and Aerosol Robotic Network (AERONET) observed daily absorption aerosol optical depth (AAOD) of LACs at 440 nm above 0.63 and the corresponding values of the normalized mean bias within ±30%. The simulated annual mean LACs AAOD at 440 nm in China was 0.016 (0.021) in 2017 (2014) and BrC contributed about 20% (21%). The estimated annual mean clear-sky LACs DRF at the top of the atmosphere in China was 1.02 W m−2 in 2017 and 1.38 W m−2 in 2014, and the contribution of BrC was about 10% and 11%, respectively, which was dominated by the BF sources (46% in 2017 and 44% in 2014) and the BB sources (38% in 2017 and 43% in 2014), with CC sources being low (16% in 2017 and 13% in 2014). The annual mean AAOD and DRF of LACs in China decreased by 0.005 and 0.36 W m−2 from 2014 to 2017, which were largely attributed to the reductions of anthropogenic emissions during the implementation of APPCAP. Our results would improve the understanding of the light absorption capacity and climate effects of LACs in China.

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.

Light absorption properties and source contributions of black and brown carbon in Guangxi, southern China

Black carbon (BC) and brown carbon aerosols (BrC) are primary light-absorbing carbonaceous aerosols that significantly influence the global and regional radiation balance, as well as air quality. Guangxi Zhuang Autonomous Region, as a primarily agricultural province of China and neighbouring Southeast Asia, is subjected to both local emissions and pollution transport from Southeast Asian biomass burning. To investigate the light absorption properties and source contributions of BC and BrC in this region, observations from a 7-wavelength Aethalometer are employed to estimate the light absorption properties of BC and BrC over the period from March to December 2020 in Nanning, China. This study focuses on analysing the absorption contributions of BC and BrC to the total absorption of carbonaceous aerosols, identifying their emission sources, and exploring the impact of long-range transport of biomass burning (BB) from Southeast Asia on BC and BrC based on backward trajectory and weighted concentration-weighted trajectories (WCWT) model. Our results show that the absorption Ångström exponent (AAE) of light-absorbing carbonaceous aerosols varies from 0.54 to 2.08, reflecting the presence of different absorbing aerosol sources with specific optical properties. The average absorption coefficients of BC and BrC at 370 nm, denoted as babs,BC(370) and babs,BrC(370), are 42.25 Mm−1 and 9.63 Mm−1, respectively, with the highest value observed in winter. The average absorption of BrC contributes 19% to the total absorption from light-absorbing carbonaceous aerosols, and this contribution decreases for high babs,BrC(370) values, with the highest value in summer at 20%. For the BC source apportionment using a site-specific AAE, fossil fuel combustion (FF) contributes 57%, with its highest proportion in summer (62%). Meanwhile, biomass burning (BB) accounts for 43%, with the greatest contribution in winter (58%). These results highlight the considerable role of BB in Guangxi. In terms of the BrC sources, secondary BrC (BrCsec) is responsible for 32% of the total light absorption of BrC at 370 nm, and is particularly characterized by a much higher level of 35% at night, meaning the dominant role of BrCsec in Nanning. The relative contribution of babs,BrC,sec(370) increases with a higher contribution of babs,BrC(370) to aerosol absorption. Compared with the BrCsec, primary BrC values are higher in spring and winter, due to the increased emissions from biomass burning. Based on the analysis of backward trajectory and WCWT, the increase in BC and BrC during March and April is mainly influenced by the long-range transport of BB from Southeast Asian countries, e.g., Laos and Thailand. Overall, the contributions of BB and FF emissions to BC are comparable in Guangxi, while BrC mainly formed from primary sources is significantly impacted by both local emissions and the long-range transport of BB. Studying the optical characteristics and emission sources in this region can promote the understanding of the radiative effect of light-absorbing carbonaceous aerosols under the joint contributions from biomass burning and industrial emissions.

Mass and Light Absorption Properties of Atmospheric Carbonaceous Aerosols over the Outflow Regions of Indo-Gangetic Plain

The uncertainty associated with carbonaceous aerosols in climate models becomes an obstacle to evaluating their harmful environmental effects. Brown Carbon (BrC) has recently become an eye-catching carbonaceous aerosol in ambient air because of its strong light absorption properties. The optical properties of soluble BrC are well studied in South Asia, one of the largest emitters. However, the absorption property of strong light-absorbing insoluble BrC is highly uncertain because of their complex mixing. Besides, the simultaneous apportionment of light-absorbing carbonaceous aerosol constituents as a function of wavelengths is seldom explored. The present study aims to study mass as well as apportionment of absorption properties of Black Carbon (BC) and different BrC chromophores using a multi-wavelength thermal-optical carbon analyzer over the least explored Eastern part of India to fill the knowledge gap. The output suggested that the primary emission sources dominate the carbonaceous aerosol mass; thus, the primary emission reductions will be helpful in improving the local air quality. The BrC is the dominant light-absorbing carbonaceous aerosol in the ultraviolet wavelengths. Besides, significant light absorption by BrC chromophores in near-infrared wavelengths (up to ∼50% of total aerosol absorption) suggested the absorption by BrC in longer wavelengths cannot be neglected. The insoluble fraction of BrC (Tar-BrC), which has a property identical to BC, contributes significantly to light absorption and is more than 50% of total absorption by aerosols in shorter ≤635 nm wavelengths. The present study also revealed that the contribution of Tar-BrC is more pronounced in the Indo-Gangetic Plain (IGP) outflow region than in the IGP emission source regions.

Aerosol absorption using in situ filter-based photometers and ground-based sun photometry in the Po Valley urban atmosphere

Abstract. Light-absorbing aerosols (LAAs) are short-lived climate forcers with a significant impact on Earth's radiative balance. LAAs include dust aerosols, black carbon (BC) and organic light-absorbing carbonaceous aerosol (collectively termed brown carbon, BrC), which have also been proven to be highly toxic. In this study, aerosol absorption at five wavelengths (ranging from ultraviolet to infrared) was monitored continuously using filter-based photometers during two winter seasons in 2020 and 2021 in the city of Modena (southern central Po Valley, northern Italy), at two regulatory air quality monitoring sites, along with other pollutants (coarse particulate matter, PM10; fine particulate matter, PM2.5; O3; NO; NO2; and C6H6) and the vehicular traffic rate. The aerosol optical depth (AOD) and other column aerosol optical properties were concurrently monitored at four wavelengths by an AErosol RObotic NETwork (AERONET) sun photometer under urban background conditions within Modena. In situ absorption levels were apportioned to both sources (fossil fuel and biomass burning) and species (BC and BrC), while columnar absorption was apportioned to BC, BrC and mineral dust. The combined analysis of the atmospheric aerosol and gas measurements and of the meteorological conditions (in situ and from the ERA5 reanalysis) identified the location of potential urban sources of BC and BrC, most likely related to traffic and biomass burning. In situ data show different diurnal/weekly patterns for BrC from biomass burning and BC from traffic, with minor differences between the background and the urban traffic conditions. AERONET version 3 absorption aerosol optical depth (AAOD) retrievals at four wavelengths allowed the estimation of the absorptive direct radiative effect due to LAAs over the same period under the reasonable assumption that the AOD signal is concentrated within the mixing layer. AERONET retrievals showed a modest correlation of columnar absorption with planetary boundary layer (PBL)-scaled in situ observations, although the correlation improved significantly during a desert dust transport event that affected both in situ aerosol and columnar absorption, particularly in the blue spectrum range. A low correlation occurred between the contribution of BrC to aerosol absorption for the in situ and the columnar observations, with the BrC contribution being generally larger for in situ observations. Finally, evidence of a highly layered atmosphere during the study period, featuring significant spatial mixing and modest vertical mixing, was shown by ERA5-based atmospheric temperature profiles and by the large correlation of concurrent AERONET AOD retrievals in Modena and in Ispra (on the northwestern side of the Po Valley, ca. 225 km from Modena).

Light absorption properties of black and brown carbon during the prescribed burning season at an urban background site in Brisbane, Australia

Light-absorbing carbonaceous aerosols primarily comprise black carbon (BC) and brown carbon (BrC), and they play a key role in atmospheric radiative forcing and global climate. Here, we present the light absorption, potential sources, and health risks of BC and BrC during the prescribed burning season at an urban background site in Brisbane based on the measurements with a seven-wavelength aethalometer. The enhancements in light absorption at 880 nm were potentially governed by the transport of prescribed burning emissions. Source apportionment results revealed that fossil-fuel (FF) combustion contributed more to the total equivalent BC (eBC) (67%) over the entire measurement period as compared to biomass burning (BB). The percentages of secondary BrC to BrC for BB- and FF-dominated periods were 60% and 21%, respectively, indicating the greater potential of BB emissions to form secondary BrC compared to FF emissions. The diurnal trend showed that the peaks of secondary BrC occurred at nighttime with high relative humidity, implying that the formation of secondary BrC was potentially associated with aqueous reactions. Potential source contribution function (PSCF) results suggested that air masses originating from southern and northern Brisbane were the potential pollution sources, where BB and traffic emissions were dominant. In addition, the health risks of eBC (based on equivalent numbers of passively smoked cigarettes) remarkably increased for periods with elevated eBC emissions, potentially originating from prescribed burns. These findings contribute to our understanding of the impact of BB on the light absorption properties of BC and BrC and could serve as a reference for government officials when performing prescribed burns with reduced environmental and health effects.

Revisiting the Absorption Spectra of Polycyclic Aromatic Hydrocarbons over Porto (Portugal) by TD-DFT Calculations

Brown carbon is a type of strong light-absorbing carbonaceous aerosol associated with radiative forcing. Nevertheless, the difficulty in correlating the chemical composition of brown carbon with its light absorption properties impairs the proper elucidation of its role in radiative forcing. Here, we have used a time-dependent density functional theory (TD-DFT)-based procedure to revisit the “real-world” absorption spectra of polycyclic aromatic hydrocarbons (PAHs) over the city of Porto, in Portugal, while correcting the spectra for their quantity in PM10 particulate matter. Our aim is to, by comparing these new results with those obtained previously regarding PM2.5 data, evaluate the role of different groupings of particulate matter in the light absorption of brown carbon. The results indicate that irrespective of the absorption spectra corresponding to their PM10 or PM2.5 data, the studied PAHs should contribute to radiative forcing by light absorption at UVA and (sub)visible wavelengths. However, the identity of the individual PAH species that contribute the most for the considered wavelengths can be quite different. Thus, different groupings of particulate matter appear to provide distinct contributions to light absorption and radiative forcing over the same location, even when considering the same class of molecular compounds.

Comparison of black carbon, primary and secondary brown carbon light absorption and direct solar absorption at the foothill and summit of Mt. Hua, China

Atmospheric black carbon (BC), primary and secondary brown carbon (BrCpri and BrCsec) are the light-absorbing carbonaceous aerosol components. The vertical changes in the BC and BrC distributions are not generally known. Here, we presented a study of the spectral light absorption properties, direct solar absorption, and potential source areas of BC and BrC at the foothill (375 m a.s.l.) and summit (2060 m a.s.l.) of Mt. Hua, China. More than tripled BC and BrC light absorption coefficient were observed at the foothill compared to the summit. The dominant carbonaceous light-absorbing was attributed to BC with the percentages of 77 % (foothill) and 79 % (summit), respectively. The light absorption coefficient and direct solar absorption of BrCpri were much higher than those of BrCsec at foothill, especially in winter. The enhancing contributions of BrCsec light absorption coefficient and direct solar absorption were observed with high RH and visibility at the summit. The light absorption properties of BC, BrCpri, and BrCsec may be attributed to the emissions, meteorological conditions, and photochemical oxidation. The inferred potential source spatial distributions of BC and BrCpri showed different patterns at the foothill and summit. The results underlined the primary emission effects (including BC and BrCpri) at the foothill and the importance of BrCsec at the summit, respectively.

Sizing response of the Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) and Laser Aerosol Spectrometer (LAS) to changes in submicron aerosol composition and refractive index

Abstract. We evaluate the sensitivity of the size calibrations of two commercially available, high-resolution optical particle sizers to changes in aerosol composition and complex refractive index (RI). The Droplet Measurement Technologies Ultra-High Sensitivity Aerosol Spectrometer (UHSAS) and the TSI, Inc. Laser Aerosol Spectrometer (LAS) are two commonly used instruments for measuring the portion of the aerosol size distribution with diameters larger than nominally 60–90 nm. Both instruments illuminate particles with a laser and relate the single-particle light scattering intensity and count rate measured over a wide range of angles to the size-dependent particle concentration. While the optical block geometry and flow system are similar for each instrument, a significant difference between the two models is the laser wavelength (1054 nm for the UHSAS and 633 nm for the LAS) and intensity (about 100 times higher for the UHSAS), which may affect the way each instrument sizes non-spherical or absorbing aerosols. Here, we challenge the UHSAS and LAS with laboratory-generated, mobility-size-classified aerosols of known chemical composition to quantify changes in the optical size response relative to that of ammonium sulfate (RI of 1.52+0i at 532 nm) and NIST-traceable polystyrene latex spheres (PSLs with RI of 1.59+0i at 589 nm). Aerosol inorganic salt species are chosen to cover the real refractive index range of 1.32 to 1.78, while chosen light-absorbing carbonaceous aerosols include fullerene soot, nigrosine dye, humic acid, and fulvic acid standards. The instrument response is generally in good agreement with the electrical mobility diameter. However, large undersizing deviations are observed for the low-refractive-index fluoride salts and the strongly absorbing nigrosine dye and fullerene soot particles. Polydisperse size distributions for both fresh and aged wildfire smoke aerosols from the recent Fire Influence on Regional to Global Environments Experiment and Air Quality (FIREX-AQ) and the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex) airborne campaigns show good agreement between both optical sizers and contemporaneous electrical mobility sizing and particle time-of-flight mass spectrometric measurements. We assess the instrument uncertainties by interpolating the laboratory response curves using previously reported RIs and size distributions for multiple aerosol type classifications. These results suggest that, while the optical sizers may underperform for strongly absorbing laboratory compounds and fresh tailpipe emissions measurements, sampling aerosols within the atmospherically relevant range of refractive indices are likely to be sized to better than ±10 %–20 % uncertainty over the submicron aerosol size range when using instruments calibrated with ammonium sulfate.

Contribution of brown carbon to the light absorption and radiative effect of carbonaceous aerosols from biomass burning emissions in Chiang Mai, Thailand

Chiang Mai suffers from adverse haze associated with heavy biomass burning (BB) during almost every dry season (February to April). As an important source of light-absorbing carbonaceous aerosols (black carbon and brown carbon), BB can have strong radiative effects on local and regional climate. However, studies on characterizing the impacts of BB aerosols on climate in Chiang Mai are quite limited. In this study, we use a global chemical transport model (GEOS-Chem) coupled with the rapid radiative transfer model for GCMs (RRTMG) to estimate the radiative forcing (RF) of BB aerosols in Chiang Mai. Brown carbon (BrC) is included as an absorber and treated as an individual tracer in the model. To our best knowledge, this is the first study to estimate the BrC RF in Chiang Mai. As evaluated, our simulations that were assigned with medium- and high-absorbing kBrC (BrC imaginary refractive index) well reproduces the absorption coefficient of ambient BrC in Chiang Mai. Based on our estimations, 33–40% of total carbonaceous aerosol absorption at 440 nm is attributed to BrC and 60–67% to BC during dry season. As estimated, BrC contributes 14 ± 3% to the instantaneous RF of total carbonaceous aerosol (IRFCAs) at the top of atmosphere (TOA) and 16 ± 3% to IRFCAs at surface. Moreover, including BrC in model strengthens (reduces) the surface (TOA) cooling effect of total organic carbon by 9 ± 5% (9 ± 3%), indicating the warming effect of BrC in the atmosphere in Chiang Mai.

Polarimetric sensitivity of light-absorbing carbonaceous aerosols over ocean: A theoretical assessment

Visible-light-absorbing carbonaceous aerosols within the boundary layer affect the radiance and polarization states of the radiation at the top of the atmosphere. Remote sensing from suborbital and satellite-based platforms utilizes these radiance and polarization signals to retrieve the key properties of these aerosols. Recent retrieval algorithms have shown a progressive trend toward including multi-angular and multi-spectral polarimetric measurements to produce better retrieval accuracy in comparison to those using measurements based on a single viewing angle. Here, we perform a theoretical investigation of the top of atmosphere (TOA) radiance-related reflectance factor (bidirectional reflectance factor (BRF)) and the two types of polarimetry-related factors (polarized bidirectional reflectance factor (pBRF) and the degree of linear polarization (DoLP)) for different types of atmospheric light-absorbing carbonaceous aerosols as a function of particle size distribution. We selected three polarimetric bands corresponding to those utilized by NASA's Airborne Multiangle SpectroPolarimetric Imager (AirMSPI)—near-UV (470 nm), visible (660 nm), and near-infrared (865 nm)—for our simulations which were performed over ocean surface using the successive order of scattering (SOS) algorithm coupled to a Lorenz-Mie aerosol optics model. The analysis of particle phase matrix elements indicates a close relationship between the angular dependencies of DoLP and associated phase matrix components at the shortest polarimetric band (470 nm). Using Jacobian analysis, we find that the radiance- and polarimetry-related reflectance factors of weakly light-absorbing aerosols, such as brown carbon, are more sensitive to changes in particle size and imaginary refractive index in comparison with those of black carbon, which is strongly light-absorbing. Our results suggest that the DoLP data could be used by future retrieval algorithms for reliably estimating microphysical properties of absorbing carbonaceous aerosols with imaginary refractive index less than 0.4.

Elemental and water-insoluble organic carbon in Svalbard snow: a synthesis of observations during 2007–2018

Abstract. Light-absorbing carbonaceous aerosols emitted by biomass or fossil fuel combustion can contribute to amplifying Arctic climate warming by lowering the albedo of snow. The Svalbard archipelago, being near to Europe and Russia, is particularly affected by these pollutants, and improved knowledge of their distribution in snow is needed to assess their impact. Here we present and synthesize new data obtained on Svalbard between 2007 and 2018, comprising measurements of elemental (EC) and water-insoluble organic carbon (WIOC) in snow from 37 separate sites. We used these data, combined with meteorological data and snowpack modeling, to investigate the variability of EC and WIOC deposition in Svalbard snow across latitude, longitude, elevation and time. Overall, EC concentrations (CsnowEC) ranged from <1.0 to 266.6 ng g−1, while WIOC concentrations (CsnowWIOC) ranged from <1 to 9426 ng g−1, with the highest values observed near Ny-Ålesund. Calculated snowpack loadings (LsnowEC, LsnowWIOC) on glaciers surveyed in spring 2016 were 0.1 to 2.6 mg m−2 and 2 to 173 mg m−2, respectively. The median CsnowEC and the LsnowEC on those glaciers were close to or lower than those found in earlier (2007–2009), comparable surveys. Both LsnowEC and LsnowWIOC increased with elevation and snow accumulation, with dry deposition likely playing a minor role. Estimated area-averaged snowpack loads across Svalbard were 1.1 mg EC m−2 and 38.3 mg WIOC m−2 for the 2015–2016 winter. An ∼11-year long dataset of spring surface snow measurements from the central Brøgger Peninsula was used to quantify the interannual variability of EC and WIOC deposition in snow. In most years, CsnowEC and CsnowWIOC at Ny-Ålesund (50 m a.s.l.) were 2–5 times higher than on the nearby Austre Brøggerbreen glacier (456 m a.s.l.), and the median EC/WIOC in Ny-Ålesund was 6 times higher, suggesting a possible influence of local EC emission from Ny-Ålesund. While no long-term trends between 2011 and 2018 were found, CsnowEC and CsnowWIOC showed synchronous variations at Ny-Ålesund and Austre Brøggerbreen. When compared with data from other circum-Arctic sites obtained by comparable methods, the median CsnowEC on Svalbard falls between that found in central Greenland (lowest) and those in continental sectors of European Arctic (northern Scandinavia, Russia and Siberia; highest), which is consistent with large-scale patterns of BC in snow reported by surveys based on other methods.

Substantial decreases of light absorption, concentrations and relative contributions of fossil fuel to light-absorbing carbonaceous aerosols attributed to the COVID-19 lockdown in east China.

To prevent spreads of Coronavirus disease-2019 (COVID-19), China adopted the lockdown measures in late January 2020, providing a platform to study the response of air quality and atmospheric chemical and physical properties to strict reduced emissions. In this study, the continuous measurements of aerosol light absorption were conducted in Nanjing, east China, from January 3 to March 31, 2020. Our results showed that the contribution of black carbon (BC) to light absorption at the different wavelengths was more than 75% and the rest light absorption was contributed by brown carbon (BrC), which was mainly originated from primary emissions. Secondary BrC absorption, which was mainly produced by photochemical oxidation, constituted a minor fraction (2–7%) of the total absorption. Compared with the sampling in the pre-lockdown, the significant decreases of BC (43%) and secondary BrC absorption (31%) were found during the lockdown period, resulting in a substantial decrease of solar energy absorbance by 36% on a local scale. The control measures also changed the diurnal variations of light absorption. Due to the reduced emissions, the relative fraction of fossil fuel to BC also dropped from 78% in the pre-lockdown to 71% in the lockdown. The concentrations of BC, PM2.5 and NO2 decreased 1.1 μg m−3, 33 μg m−3 and 9.1 ppb whereas O3 concentration increased 9.0 ppb during the COVID-19 lockdown period. The decreased concentrations of BC, PM2.5 and NO2 were mainly contributed by both emission reduction (51–64%) and meteorological conditions (36–49%). Our results highlighted that the balance of control measures in alleviation of particulate matter (PM) and O3 pollution, and meteorology should be seriously considered for improvement of air quality in this urban city of China.

Study of Temporal Variations of Equivalent Black Carbon in a Coastal City in Northwest Spain Using an Atmospheric Aerosol Data Management Software

Light-absorbing carbonaceous aerosols (including black carbon (BC)) pose serious health issues and play significant roles in atmospheric radiative properties. Two-year measurements (2015–2016) of aerosol light absorption, combined with measurements of sub-micrometric particles, were continuously conducted in A Coruña (northwest (NW) Spain) to determine their light absorption properties: absorption coefficients (σabs) and the absorption Ångström exponent (AAE). The mean and standard deviation of equivalent black carbon (eBC) during the period of study were 0.85 ± 0.83 µg m−3, which are lower than other values measured in urban areas of Spain and Europe. High eBC concentrations found in winter are associated with an increase in emissions from anthropogenic sources in combination with lower mixing layer heights and frequent stagnant conditions. The pronounced diurnal variability suggests a strong influence from local sources. AAE had an average value of 1.26 ± 0.22 which implies that both fossil fuel combustion and biomass burning influenced optical aerosol properties. This also highlights biomass combustion in suburban areas, where the use of wood for domestic heating is encouraged, as an important source of eBC. All data treatment was gathered using SCALA© as atmospheric aerosol data management support software program.

Influence of Meteorological Conditions and Fire Hotspots on PM0.1 in Northern Thailand during Strong Haze Episodes and Carbonaceous Aerosol Characterization

ABSTRACT Northern Thailand has long been severely affected by haze from biomass burning containing fine and ultrafine aerosols in the dry period. The carbonaceous PM0.1 comprising elemental carbon (EC) and organic carbon (OC) collected during the haze and non-haze periods in Chiang Mai, Thailand was investigated. The PM0.1 levels during the haze periods were about 3 times higher than the non-haze periods, a significant increase. PM0.1 concentration was strongly correlated with atmospheric relative humidity and the number of forest fire hotspots. Carbonaceous aerosol characteristics in PM0.1 were analyzed with the thermal/optical transmittance (TOT) method following the IMPROVE protocol. The concentrations of OC and EC, distribution of OC and EC and OC/EC ratios in PM0.1 were evaluated. Average OC and EC mass concentrations in PM0.1 were 6.8 ± 2.7 and 1.4 ± 0.5 µg m–3 during the haze periods, significantly higher than those during the non-haze periods; 1.9 ± 0.9 and 0.5 ± 0.2 µg m–3. The OC/EC ratio increased linearly with the number of hotspots. This indicated significant contribution from biomass burning to the PM0.1. This was strongly supported by the 48-hr backward trajectory simulation, that indicated both domestic and transboundary aerosol transports. Because both organic and elemental carbon are the light-absorbing carbonaceous aerosols, the increase during the haze periods contributed to regional air quality and climate. This study enhances the understanding of PM0.1 behavior in Chiang Mai, Thailand, during the haze periods in upper southeast Asia.

Optical source apportionment and radiative effect of light-absorbing carbonaceous aerosols in a tropical marine monsoon climate zone: the importance of ship emissions

Abstract. Source-specific optical properties of light-absorbing carbonaceous (LAC) aerosols in the atmosphere are poorly understood because they are generated by various sources. In this study, a receptor model combining multi-wavelength absorption and chemical species was used to explore the source-specific optical properties of LAC aerosols in a tropical marine monsoon climate zone. The results showed that biomass burning and ship emissions were the dominant contributors to average aerosol light absorption. The source-specific absorption Ångström exponent (AAE) indicated that black carbon (BC) was the dominant LAC aerosol in ship and motor vehicle emissions. Moreover, brown carbon (BrC) was present in biomass-burning emissions. The source-specific mass absorption cross section (MAC) showed that BC from ship emissions had a stronger light-absorbing capacity compared to emissions from biomass burning and motor vehicles. The BrC MAC derived from biomass burning was also smaller than the BC MAC and was highly dependent on wavelength. Furthermore, radiative effect assessment indicated a comparable atmospheric forcing and heating capacity of LAC aerosols between biomass burning and ship emissions. This study provides insights into the optical properties of LAC aerosols from various sources. It also sheds more light on the radiative effects of LAC aerosols generated by ship emissions.

Characterization of light-absorbing aerosols from a laboratory combustion source with two different photoacoustic techniques

In this study, we characterized a variety of light-absorbing carbonaceous aerosols generated from a controlled combustion system using two different photoacoustic measurement techniques: the RGB-DP...