Aerosol Absorption Coefficient Research Articles

Improving the sectional Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) aerosols of the Weather Research and Forecasting-Chemistry (WRF-Chem) model with the revised Gridpoint Statistical Interpolation system and multi-wavelength aerosol optical measurements: the dust aerosol observation campaign at Kashi, near the Taklimakan Desert, northwestern China

Abstract. The Gridpoint Statistical Interpolation data assimilation (DA) system was developed for the four size bin sectional Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) aerosol mechanism in the Weather Research and Forecasting-Chemistry (WRF-Chem) model. The forward and tangent linear operators for the aerosol optical depth (AOD) analysis were derived from WRF-Chem aerosol optical code. We applied three-dimensional variational DA to assimilate the multi-wavelength AOD, ambient aerosol scattering coefficient, and aerosol absorption coefficient, measured by the sun–sky photometer, nephelometer, and aethalometer, respectively. These measurements were undertaken during a dust observation field campaign at Kashi in northwestern China in April 2019. The results showed that the DA analyses decreased the model aerosols' low biases; however, it had some deficiencies. Assimilating the surface particle concentration increased the coarse particles in the dust episodes, but AOD and the coefficients for aerosol scattering and absorption were still lower than those observed. Assimilating aerosol scattering coefficient separately from AOD improved the two optical quantities. However, it caused an overestimation of the particle concentrations at the surface. Assimilating the aerosol absorption coefficient yielded the highest positive bias in the surface particle concentration, aerosol scattering coefficient, and AOD. The positive biases in the DA analysis were caused by the forward operator underestimating aerosol mass scattering and absorption efficiency. As compensation, the DA system increased particle concentrations excessively to fit the observed optical values. The best overall improvements were obtained from the simultaneous assimilation of the surface particle concentration and AOD. The assimilation did not substantially change the aerosol chemical fractions. After DA, the clear-sky aerosol radiative forcing at Kashi was −10.4 W m−2 at the top of the atmosphere, which was 55 % higher than the radiative forcing value before DA.

Assessment of the COVID-19 Lockdown Effects on Spectral Aerosol Scattering and Absorption Properties in Athens, Greece

COVID-19 is evolving into one of the worst pandemics in recent history, claiming a death toll of over 1.5 million as of December 2020. In an attempt to limit the expansion of the pandemic in its initial phase, nearly all countries imposed restriction measures, which resulted in an unprecedented reduction of air pollution. This study aims to assess the impact of the lockdown effects due to COVID-19 on in situ measured aerosol properties, namely spectral-scattering (bsca) and absorption (babs) coefficients, black carbon (BC) concentrations, single-scattering albedo (SSA), scattering and absorption Ångström exponents (SAE, AAE) in Athens, Greece. Moreover, a comparison is performed with the regional background site of Finokalia, Crete, for a better assessment of the urban impact on observed differences. The study examines pre-lockdown (1–22 March 2020), lockdown (23 March–3 May 2020) and post-lockdown (4–31 May 2020) periods, while the aerosol properties are also compared with a 3–4 year preceding period (2016/2017–2019). Comparison of meteorological parameters in Athens, between the lockdown period and respective days in previous years, showed only marginal variation, which is not deemed sufficient in order to justify the notable changes in aerosol concentrations and optical properties. The largest reduction during the lockdown period was observed for babs compared to the pre-lockdown (−39%) and to the same period in previous years (−36%). This was intensified during the morning traffic hours (−60%), reflecting the large decrease in vehicular emissions. Furthermore, AAE increased during the lockdown period due to reduced emissions from fossil-fuel combustion, while a smaller (−21%) decrease was observed for bsca along with slight increases (6%) in SAE and SSA values, indicating that scattering aerosol properties were less affected by the decrease in vehicular emissions, as they are more dependent on regional sources and atmospheric processing. Nighttime BC emissions related to residential wood-burning were slightly increased during the lockdown period, with respect to previous-year means. On the contrary, aerosol and pollution changes during the lockdown period at Finokalia were low and highly sensitive to natural sources and processes.

Source-Based Size-Resolved Optical Properties of Carbonaceous Aerosols

In this study, the source-based optical properties of polydisperse carbonaceous aerosols were determined from PM2.5 concentrations measured at a Global Atmospheric Watch station in South Korea. The extinction and absorption coefficients of carbonaceous aerosols were calculated using the Mie theory and assuming a lognormal size distribution. Based on the mass concentration from the EPA’s Positive Matrix Factorization (PMF) receptor model, which considers five source identification and apportionment factors (biogenic source, local biomass burning, secondary organic aerosol, transported biomass burning, and mixed sources), the source-based size-resolved mass extinction and absorption efficiencies were estimated for each source using a multilinear regression model. The results show that the source-based optical properties depend on the aerosol size and physicochemical characteristics of the chemical compounds. The long-range transport of biomass burning (LBB) aerosol, which has a mass concentration of 20%, holds a 12.1–23.1% total extinction efficiency—depending on the size and refractive index—in the range of 0.1–0.5 μm in geometric mean diameter and humic-like substances (HULIS) imaginary refractive index of 0.006–0.3. Biogenic sources of aerosols with small diameters have higher mass absorption efficiencies (MAE) than other sources, depending on the size and refractive index.

Detailed characterization of the CAPS single-scattering albedo monitor (CAPS PMssa) as a field-deployable instrument for measuring aerosol light absorption with the extinction-minus-scattering method

Abstract. The CAPS PMssa monitor is a recently commercialized instrument designed to measure aerosol single-scattering albedo (SSA) with high accuracy (Onasch et al., 2015). The underlying extinction and scattering coefficient measurements made by the instrument also allow calculation of aerosol absorption coefficients via the extinction-minus-scattering (EMS) method. Care must be taken with EMS measurements due to the occurrence of large subtractive error amplification, especially for the predominantly scattering aerosols that are typically found in the ambient atmosphere. Practically this means that although the CAPS PMssa can measure scattering and extinction coefficients with high accuracy (errors on the order of 1 %–10 %), the corresponding errors in EMS-derived absorption range from ∼10 % to greater than 100 %. Therefore, we examine the individual error sources in detail with the goal of constraining these as tightly as possible. Our main focus is on the correction of the scattered light truncation effect (i.e., accounting for the near-forward and near-backward scattered light that is undetectable by the instrument), which we show to be the main source of underlying error in atmospheric applications. We introduce a new, modular framework for performing the truncation correction calculation that enables the consideration of additional physical processes such as reflection from the instrument's glass sampling tube, which was neglected in an earlier truncation model. We validate the truncation calculations against comprehensive laboratory measurements. It is demonstrated that the process of glass tube reflection must be considered in the truncation calculation, but that uncertainty still remains regarding the effective length of the optical cavity. Another important source of uncertainty is the cross-calibration constant that quantitatively links the scattering coefficient measured by the instrument to its extinction coefficient. We present measurements of this constant over a period of ∼5 months that demonstrate that the uncertainty in this parameter is very well constrained for some instrument units (2 %–3 %) but higher for others. We then use two example field datasets to demonstrate and summarize the potential and the limitations of using the CAPS PMssa for measuring absorption. The first example uses mobile measurements on a highway road to highlight the excellent responsiveness and sensitivity of the instrument, which enables much higher time resolution measurements of relative absorption than is possible with filter-based instruments. The second example from a stationary field site (Cabauw, the Netherlands) demonstrates how truncation-related uncertainties can lead to large biases in EMS-derived absolute absorption coefficients. Nevertheless, we use a subset of fine-mode-dominated aerosols from the dataset to show that under certain conditions and despite the remaining truncation uncertainties, the CAPS PMssa can still provide consistent EMS-derived absorption measurements, even for atmospheric aerosols with high SSA. Finally, we present a detailed list of recommendations for future studies that use the CAPS PMssa to measure absorption with the EMS method. These recommendations could also be followed to obtain accurate measurements (i.e., errors less than 5 %–10 %) of SSA and scattering and extinction coefficients with the instrument.

Three-wavelength measurement of aerosol absorption using a multi-resonator coupled photoacoustic spectrometer.

Aerosol optical absorption measurements are important for the prediction of climate change, as aerosols directly disturb Earth's radiation balance by absorbing or scattering solar radiation. Although photoacoustic spectroscopy is commonly recognized as one of the best candidates to measure the absorption of aerosols, multi-wavelength measurements of aerosols optical absorption remain challenging. Here, a method based on photoacoustic spectroscopy that can simultaneously measure the aerosol absorption characteristics of three wavelengths (404, 637 and 805 nm) is proposed. In the three-wavelength photoacoustic spectrometer (TW-PAS), a photoacoustic cell with three acoustic resonators operating at different resonant frequencies was designed for offering multi-laser (multi-wavelength) operation simultaneously, and only one microphone was used to measure the acoustic signals of all resonators. The performance of TW-PAS was demonstrated and evaluated by measuring and analyzing the wavelength-dependent absorption coefficients of carbonaceous aerosols, which shows good agreement with previously reported results. The developed TW-PAS exhibits high potential for classifying and quantifying different types of light-absorbing aerosols by analyzing its absorption wavelength dependence characteristics.

Applicability of benchtop multi-wavelength polar photometers to off-line measurements of the Multi-Angle Absorption Photometer (MAAP) samples

In this study, the applicability of a benchtop polar photometer (PP_UniMI) to retrieve multi-wavelength aerosol absorption coefficient data by off-line measurements of the Multi-Angle Absorption Photometer (MAAP) sample spots is presented. MAAP is a widespread single wavelength online instrument providing the aerosol absorption coefficient and the equivalent black carbon concentration. In this work, MAAP samples collected during four different campaigns were analysed off-line with PP_UniMI.First of all, data from PP_UniMI and MAAP were compared to investigate contributions to measurement uncertainties. In particular, the role of the following assumptions performed in the MAAP was investigated:1) reconstructing angular distribution of light scattered by filter samples from measurements at three fixed angles using analytical functions;2) setting the fraction of the back-scattered radiation by the blank filter (BM) at a fixed value BM = 0.7;3) assuming a fixed value for the asymmetry factor g = 0.75.Samples collected at several sites showed an agreement within 5% when data from the two instruments were retrieved using the same approximations (i.e. backscattered radiation from the filter matrix BM set at a fixed value, phase functions reconstructed by analytical functions from measurements at 3 angles, same asymmetry factor) in the data retrieval algorithm. Conversely, larger differences (14% on average) between off-line measurements and averaged MAAP data were obtained when the high-angular resolved information available by PP_UniMI was exploited. By analysing the role of MAAP assumptions for σap retrieval, it resulted that fixing BM = 0.7 was the main responsible for the detected differences. Indeed, high-angular resolved off-line measurements by PP_UniMI allow to directly measure BM, obtaining BM = 0.88 on white spots. It is noteworthy that the observed results were similar at all investigated sites, so they proved to be independent of the aerosol type and can likely be attributed to instrumental effects. Moreover, a sensitivity test was carried out also to check the impact of the fixed value used for the asymmetry factor (set at g = 0.75 in both instruments). Varying g values within the typical range for ambient aerosol (0.50–0.75) the estimate of aerosol absorbance ABS (directly obtained from PP_UniMI measurements and linked to σap) was affected by 8% at most, thus being a minor source of uncertainty in the calculation. The effect of the variability in blank spots used for off-line analyses was also evaluated and resulted in a contribution smaller than 3% to the uncertainty of the methodology employed.Finally, the possibility of exploiting multi-wavelength assessment of absorption coefficients is an added value of PP_UniMI; indeed, it allows to estimate the contribution of different aerosol sources and components to the absorption coefficient using MAAP tapes used in present or past campaigns.

Gaining knowledge on source contribution to aerosol optical absorption properties and organics by receptor modelling

In this source apportionment study, an original approach based on receptor modelling was tested to relate primary and secondary organic aerosol (OA) contributions - estimated from ACSM (Aerosol Chemical Speciation Monitor) measurements - to their emission sources. Moreover, thanks to the coupling of optical and chemical variables as input to the receptor model, information such as the impact of mineral dust to the aerosol absorption in the atmosphere and estimates for the absorption Ångström exponent (α) of the sources were retrieved.An advanced source apportionment study using the Multilinear Engine (ME-2) was performed on data collected during February 2017 in Rome (Italy), in the frame of the CARE (Carbonaceous Aerosol in Rome and Environs) experiment. A complete chemical characterisation (elements, non-refractory components, and carbonaceous components) was carried out, and the aerosol absorption coefficients bap(λ) at 7 wavelengths (370, 470, 520, 590, 660, 880, and 950 nm) were retrieved by an Aethalometer AE33; all these variables (chemical + optical) were used as input to the receptor model. The final constrained solution consisted of nine factors which were assigned to major sources impacting on the investigated site (hereafter sources are referred to as: biomass burning, nitrate and aged aerosol, traffic exhaust, sulphate, mineral dust, marine aerosol, traffic non-exhaust, local source, and polluted marine aerosol), comprising both local urban sources and contributions from long-range transport. The bootstrap analysis supported the goodness of the solution.Total OA concentration from ACSM was apportioned by our receptor model and afterwards compared with HOA (hydrocarbon-like organic aerosol), BBOA (biomass burning-like organic aerosol), and OOA (oxygenated organic aerosol) concentrations obtained as results from an independent source apportionment study previously performed. As an original result of this work, insights on OA contributions were thus retrieved: (1) the contribution of organic aerosol assigned by ME-2 to the traffic exhaust source was fully comparable to HOA assessed by ACSM data analysis; (2) our source apportionment results gave the relevant indication that the OOA apportionment made on ACSM data likely includes a secondary OA contribution due to biomass burning.Other relevant results came from bap apportionment obtained by our multi-variable source apportionment approach: traffic exhaust was the main contributor to aerosol absorption in the atmosphere, but mineral dust contribution was also notable when a not negligible mineral dust transport episode was registered at the measurement site. In addition, source dependent optical absorption parameters (i.e. the absorption Ångström exponent - α - and the mass absorption cross section at different wavelengths) were retrieved without any a-priori assumption.In perspective, our modelling approach paves the way to more powerful source apportionment approaches which have the potential of providing much more insights on aerosol properties and sources.

Impact of the COVID-19 pandemic and control measures on air quality and aerosol light absorption in Southwestern China

China has been performing nationwide social lockdown by releasing the Level 1 response to major public health emergencies (RMPHE) to struggle against the COVID-19 (SARS-CoV-2) outbreak since late January 2020. During the Level 1 RMPHE, social production and public transport were maintained at minimal levels, and residents stayed in and worked from home. The universal impact of anthropogenic activities on air pollution can be evaluated by comparing it with air quality under such extreme conditions. We investigated the concentration of both gaseous and particulate pollutants and aerosol light absorption at different levels of (RMPHE) in an urban area of southwestern China. During the lockdown, PM2.5, PM10, SO2, NOx, and BC decreased by 30–50%, compared to the pre-Level 1 RMPHE period. Meanwhile, the decrease of NOx caused the rise of O3 by up to 2.3 times due to the volatile organic compounds (VOCs) limitation. The aerosol light absorption coefficient at multiple wavelengths decreased by 50%, and AAE decreased by 20% during the Level 1 RMPHE. BrC played essential roles in light absorption after the RMPHE was announced, accounting for 54.0% of the aerosol absorption coefficient at 370 nm. Moreover, the lockdown down-weighted the fraction of fossil fuel in BC concentrations to 0.43 (minima). This study characterizes air pollution at the most basic level and can provide policymakers with references for the “baseline.”

High mass absorption efficiency of carbonaceous aerosols during the biomass burning season in Chiang Mai of northern Thailand

Abstract Southeast Asia is one of the major regions of biomass burning in the world. To investigate the light absorption properties of carbonaceous aerosols produced from biomass burning, mass concentrations of PM2.5 and its major chemical compositions were obtained by filter sampling, and aerosol absorption coefficient (bap) at 370 nm (bap-370nm) and at 880 nm (bap-880nm) were synchronously determined for the sampled filters using a transmissometer in urban Chiang Mai of Northern Thailand during the dry season in 2019. On campaign average, the reconstructed PM2.5 mass from the measured chemical components accounted for 99% of the measured PM2.5 mass, in which organic matters (OM) accounted for 64 ± 10%. Hardwood burning was identified as the dominant source of carbonaceous aerosols. The measured aerosol absorption Angstrom exponent (AAE) at 370–880 nm (AAE370–880nm) was 1.71 ± 0.24. Mass absorption efficiency (MAE) of elemental carbon (EC) and organic carbon (OC) was estimated using a multiple linear regression model between bap and mass concentrations of EC and OC, resulting in campaign-average values of 8.11 m2 g−1 and 0.24 m2 g−1 at 880 nm and 21.06 m2 g−1 and 2.57 m2 g−1 at 370 nm, respectively, which were evidently larger than those in other cities worldwide. The contributions of EC to bap in 370–880 nm spectrum region ranged from 49 ± 5% to 79 ± 3%, and those of OC ranged from 51 ± 5% to 21 ± 3%. Results from this study suggested a potentially significant impact of carbonaceous aerosols on direct radiative forcings in the dry season over Southeast Asia and downwind regions.

Estimating contributions of black and brown carbon to solar absorption from aethalometer and AERONET measurements in the highly polluted Kathmandu Valley, Nepal

We estimated the individual contributions of black carbon (BC) and brown carbon (BrC) to the aerosol absorption coefficient (σap) and absorption aerosol optical depth (AAOD) in the highly polluted Kathmandu Valley, Nepal, by applying the absorption Ångström exponent (AÅE) method to multi-wavelength aethalometer and AERONET sun/sky radiometer measurements. The elevated σap levels observed during the winter and pre-monsoon periods were primarily due to increased usage of diesel generators and low-grade fuel/coal. The AAODBC and AAODBrC values were substantially higher during the pre-monsoon period, almost two-fold higher than winter levels, due to seasonally increased biomass-burning activities from agricultural residue burning and forest fires. The overall contribution of BC to σap was approximately 80%–95%, whereas BrC accounted for 5%–20% at 520 nm. However, the BrC contribution to σap at 370 nm was substantially higher during the winter, ranging from 29.3% to 34.0%. The portioning of AERONET measurements indicates that BC contributed 80% (69%) while BrC contributed 20% (31%) to AAOD of carbonaceous aerosols at 520 nm (370 nm). Although the observation principles and techniques are completely independent, the BC and BrC absorption for simultaneous daytime data points shows a strong correlation between surface aethalometer-based and column AERONET-based estimates. The contributions of BC and BrC to absorption in Kathmandu Valley are similar to those observed under open biomass and garbage-burning conditions; however, the BrC absorption at both 370 and 520 nm is approximately 2- to 3-fold higher than those observed for urban areas in East Asia.

Differing effects of escalating pollution on absorption and scattering efficiencies of aerosols: Toward co-beneficial air quality enhancement and climate protection measures

Abstract The mass absorption efficiency (MAE) and mass scattering efficiency (MSE) of aerosols are critical to their light extinction capacity. In winter in northern China, episodes of clear air and heavy haze alternately occur due to the high primary emission and secondary formation of aerosols, coupled with changing weather conditions. These occurrences facilitate detailed investigation of how significant changes in the pollution level impact the MAE and MSE, they also enable the determination of whether current air quality improvement measures are also beneficial to the mitigation of climate change, to avoid climatic side effects of attempts to clean the air. In the present study, a one-month observation campaign was conducted in Beijing, China, during the 2016–2017 winter season. A photoacoustic extinctiometer, which is an in situ measurement instrument, was used to investigate the aerosol absorption coefficient ( σ a ) and scattering coefficient ( σ s ) at an infra-red wavelength of 870 nm. The MAE and MSE were found to vary differently with increasing pollution level. A positive correlation between the particulate matter concentration (PM2.5) and the MAE was observed for PM2.5 σ a and σ s , increasing from 0.827 ± 0.018 (average ± standard deviation) for a bottom particulate matter concentration group of (0, 25] μg m−3 to 0.924 ± 0.007 for a top particulate matter concentration group of (300, 400] μg m−3, indicating a positive correlation between the SSA and PM2.5. These observations suggest a risk of current clean air measures weakening or eliminating the cooling effect of ambient aerosols in northern China. It seems that no previous study has involved the simultaneous acquisition of σ a and σ s at the same wavelength with the purpose of determining how increasing air pollution differently impacts the MAE and MSE. Practical measures that can be used to decrease the black carbon-to-PM2.5 ratio include phasing out or reducing black carbon-rich sources and promoting technologies that decrease the black carbon-to-organic carbon ratio.

Investigation of aerosol absorption with dual-polarization lidar observations.

Polarization lidar has been widely used in recent decades to observe the vertical structures of aerosols and clouds in the atmosphere. We developed a dual-polarization lidar system that can detect polarization measurements simultaneously at 355 nm and 532 nm. Dust events and haze episodes over northern China in 2014 were observed by the developed lidar. The results showed that the dust-dominated aerosol depolarization ratios at 532 nm were larger than those at 355 nm, but those of the air pollutants were smaller, indicating that this tool could provide a more accurate classification of aerosols. Moreover, we found a good relationship between the absorption coefficient of aerosols and the ratio of depolarization ratios at 532 nm and 355 nm for dust aerosols. Our results imply that aerosol absorption from polarization measurements may be determined by lidar at the ultraviolet and visible wavelengths.

The Contribution of Black Carbon and Non-BC Absorbers on Aerosol Absorption Coefficient in Nanjing, China

An aethalometer was employed in a 1-year campaign (November 2014–November 2015) in Nanjing, China, that aimed to estimate the contributions of black carbon (BC; annual average ± std = 4.0 ± 3.3 µg m–3) and non-BC absorbers, such as brown carbon, to the aerosol absorption coefficient. We applied two methods: 1) the traditional calculation from the aethalometer data, assuming an absorption Ångström exponent (AAE) of unity for BC (“AE method”), which provided an overall average of 27.2% for the non-BC contribution, and 2) a recently developed method based on the wavelength dependence of AAE (the “WDA method”), which indicated the existence of non-BC absorbers in 25.3% of the samples on average. We utilized trajectory and source area analyses and, in agreement with the results from other studies in this region, verified biomass burning emission sources, mainly to the northwest of the measurement site.

Spatial and Temporal Variability of Carbonaceous Aerosol Absorption in the Po Valley

Knowledge gaps in the optical properties of carbonaceous aerosols account for a significant fraction of the uncertainty of aerosol - light interactions in climate models. Both black carbon (BC) and brown carbon (BrC) can display a range of optical properties in ambient aerosol due to different sources and chemical transformation pathways. This study investigates the optical absorption properties of BC and BrC at an urban and a rural site in the Po Valley (Italy), a known European pollution hot spot. We observed spatial and seasonal variability of aerosol absorption coefficients, with the highest values measured in winter at the urban site of Milan (12 Mm–1 on average) and the lowest values in summer at the rural site of Motta Visconti (3 Mm–1 on average). The average aerosol Absorption Ångström Exponent (AAE) measured during the two experiments across the 370–880 nm wavelength range was 1.1 and 1.2 at the urban and the rural site, respectively. The observed AAE values in winter (the average AAE during the two winter campaigns was 1.2) are consistent with the contribution of wood burning BrC, as confirmed by macro-tracer analysis. The BC mass absorption cross section (MACBC) did not show a specific seasonal or spatial variability across the two sites and maintained an average value of 10 ± 5 m2 g–1 at 880 nm. The optical properties of BrC, investigated off-line after extraction of organic aerosol (OA) indicate that wood burning was the dominant BrC source in winter, while secondary organic aerosol (SOA) from other anthropogenic emissions was the main source of BrC in summer.

Exploiting multi-wavelength aerosol absorption coefficients in a multi-time resolution source apportionment study to retrieve source-dependent absorption parameters

Abstract. In this paper, a new methodology coupling aerosol optical and chemical parameters in the same source apportionment study is reported. In addition to results on source contributions, this approach provides information such as estimates for the atmospheric absorption Ångström exponent (α) of the sources and mass absorption cross sections (MACs) for fossil fuel emissions at different wavelengths. A multi-time resolution source apportionment study using the Multilinear Engine (ME-2) was performed on a PM10 dataset with different time resolutions (24, 12, and 1 h) collected during two different seasons in Milan (Italy) in 2016. Samples were optically analysed by an in-house polar photometer to retrieve the aerosol absorption coefficient bap (in Mm−1) at four wavelengths (λ=405, 532, 635, and 780 nm) and were chemically characterized for elements, ions, levoglucosan, and carbonaceous components. The dataset joining chemically speciated and optical data was the input for the multi-time resolution receptor model; this approach was proven to strengthen the identification of sources, thus being particularly useful when important chemical markers (e.g. levoglucosan, elemental carbon) are not available. The final solution consisted of eight factors (nitrate, sulfate, resuspended dust, biomass burning, construction works, traffic, industry, aged sea salt); the implemented constraints led to a better physical description of factors and the bootstrap analysis supported the goodness of the solution. As for bap apportionment, consistent with what was expected, biomass burning and traffic were the main contributors to aerosol absorption in the atmosphere. A relevant feature of the approach proposed in this work is the possibility of retrieving a lot of other information about optical parameters; for example, in contrast to the more traditional approach used by optical source apportionment models, here we obtained source-dependent α values without any a priori assumption (α biomass burning =1.83 and α fossil fuels =0.80). In addition, the MACs estimated for fossil fuel emissions were consistent with literature values. It is worth noting that the approach presented here can also be applied using more common receptor models (e.g. EPA PMF instead of multi-time resolution ME-2) if the dataset comprises variables with the same time resolution as well as optical data retrieved by widespread instrumentation (e.g. an Aethalometer instead of in-house instrumentation).

Observation-based estimates of the mass absorption cross-section of black and brown carbon and their contribution to aerosol light absorption in East Asia

In this study, we estimated the contribution of black carbon (BC) and brown carbon (BrC) to aerosol light absorption from surface in-situ and aerosol robotic network (AERONET) columnar observations. The mass absorption cross-section (MAC) of BC (MACBC) was estimated to be 6.4 ± 1.5 m2 g−1 at 565 nm from in-situ aerosol measurements at Gosan Climate Observatory (GCO), Korea, in January 2014, which was lower than those observed in polluted urban areas. A BrC MAC of 0.62 ± 0.06 m2 g−1 (565 nm) in our estimate is approximately ten times lower than MACBC at 565 nm. The contribution of BC and BrC to the carbonaceous aerosol absorption coefficient at 565 nm from the in-situ measurements was estimated at 88.1 ± 7.4% and 11.9 ± 7.4%, respectively at GCO. Similarly, the contribution of BC and BrC to the absorption aerosol optical depth (AAOD) for carbonaceous aerosol (CA), constrained by AERONET observations at 14 sites over East Asia by using different spectral dependences of the absorption (i.e., absorption Ångström exponent) of BC and BrC, was 84.9 ± 2.8% and 15.1 ± 2.8% at 565 nm, respectively. The contribution of BC to CA AAOD was greater in urban sites than in the background areas, whereas the contribution of BrC to CA AAOD was higher in background sites. The overall contribution of BC to CA AAOD decreased by 73%–87% at 365 nm, and increased to 93%–97% at 860 nm. The contribution of BrC to CA AAOD decreased significantly with increasing wavelength from approximately 17% at 365 nm to 4% at 860 nm.

Intra-regional transport of black carbon between the south edge of the North China Plain and central China during winter haze episodes

Abstract. Black carbon (BC), which is formed from the incomplete combustion of fuel sources (mainly fossil fuel, biofuel and open biomass burning), is a chemically inert optical absorber in the atmosphere. It has significant impacts on global climate, regional air quality and human health. During transportation, its physical and chemical characteristics as well as its sources change dramatically. To investigate the properties of BC (i.e., mass concentration, sources and optical properties) during intra-regional transport between the southern edge of the North China Plain (SE-NCP) and central China (CC), simultaneous BC observations were conducted in a megacity (Wuhan – WH) in CC, in three borderline cities (Xiangyang – XY, Suixian – SX and Hong'an – HA; from west to east) between the SE-NCP and CC, and in a city (Luohe – LH) in the SE-NCP during typical winter haze episodes. Using an Aethalometer, the highest equivalent BC (eBC) mass concentrations and the highest aerosol absorption coefficients (σabs) were found in LH in the SE-NCP, followed by the borderline cities (XY, SX and HA) and WH. The levels, sources, optical properties (i.e., σabs and absorption Ångström exponent, AAE) and geographic origins of eBC were different between clean and polluted periods. Compared with clean days, higher eBC levels (26.4 %–163 % higher) and σabs (18.2 %–236 % higher) were found during pollution episodes due to the increased combustion of fossil fuels (increased by 51.1 %–277 %), which was supported by the decreased AAE values (decreased by 7.40 %–12.7 %). The conditional bivariate probability function (CBPF) and concentration-weighted trajectory (CWT) results showed that the geographic origins of biomass burning (BCbb) and fossil fuel (BCff) combustion-derived BC were different. Air parcels from the south dominated for border sites during clean days, with contributions of 46.0 %–58.2 %, whereas trajectories from the northeast showed higher contributions (37.5 %–51.2 %) during pollution episodes. At the SE-NCP site (LH), transboundary influences from the south (CC) exhibited a more frequent impact (with air parcels from this direction comprising 47.8 % of all parcels) on the ambient eBC levels during pollution episodes. At WH, eBC was mainly from the northeast transport route throughout the observation period. Two transportation cases showed that the mass concentrations of eBC, BCff and σabs all increased, from upwind to downwind, whereas AAE decreased. This study highlights that intra-regional prevention and control for dominant sources at each specific site should be considered in order to improve the regional air quality.

Aerosol optical properties under different pollution levels in the Pearl River Delta (PRD) region of China

To clarify the aerosol hygroscopic growth and optical properties of the Pearl River Delta (PRD) region, integrated observations were conducted in Heshan City of Guangdong Province from October 19 to November 17, 2014. The concentrations and chemical compositions of PM2.5, aerosol optical properties and meteorological parameters were measured. The mean value of PM2.5 increased from less than 35 (excellent) to 35-75 μg/m3 (good) and then to greater than 75 μg/m3 (pollution), corresponding to mean PM2.5 values of 24.9, 51.2, and 93.3 μg/m3, respectively. The aerosol scattering hygroscopic growth factor (f(RH = 80%)) values were 2.0, 2.12, and 2.18 for the excellent, good, and pollution levels, respectively. The atmospheric extinction coefficient (σext) and the absorption coefficient of aerosols (σap) increased, and the single scattering albedo (SSA) decreased from the excellent to the pollution levels. For different air mass sources, under excellent and good levels, the land air mass from northern Heshan had lower f(RH) and σsp values. In addition, the mixed aerosol from the sea and coastal cities had lower f(RH) and showed that the local sources of coastal cities have higher scattering characteristics in pollution periods.

Complex refractive index, single scattering albedo, and mass absorption coefficient of secondary organic aerosols generated from oxidation of biogenic and anthropogenic precursors

Refractive index and optical properties of biogenic and anthropogenic secondary organic aerosol (SOA) particles were investigated. Aerosol precursors, namely longifolene, α-pinene, 1-methylnaphthal...

Correction

This article refers to:Multiple scattering correction factor estimation for aethalometer aerosol absorption coefficient measurement