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Black carbon (BC) is one of the most important climate forcers with severe health effects. Large uncertainties in radiative forcing estimation and health impact assessment arise from the fact that there is no standardized method to measure BC mass concentration. This study presents a 2-year comparison of three state-of-the-art BC measurement techniques at the high-altitude research station Pic du Midi (PDM) located in the French Pyrenees at an altitude of 2877 m above sea level. A recently upgraded Aethalometer AE33, a thermal-optical analyser Sunset and a single-particle soot photometer SP2 were deployed to measure simultaneously the mass concentration of equivalent black carbon (MeBC), elemental carbon (MEC) and refractory black carbon (MrBC), respectively. Significant deviations in the response of the instruments were observed. All techniques responded to seasonal variations in the atmospheric changes in BC levels and exhibited good correlation during the whole study period. This indicates that the different instruments quantified the same particle type despite the fact that they are based on different physical principles. However the slopes and correlation coefficients varied between instrument pairs. The largest biases were observed for the AE33 with MeBC values that were around 2 times greater than MrBC and MEC values. The principal reasons of such large discrepancy were explained by the mass absorption cross section (MAC) that was too low and C values recommended by the AE33 manufacturer and applied to the absorption coefficients measured by the AE33. In addition, the long-range transport of dust particles at PDM in spring caused significant increases in the bias between AE33 and SP2 by up to a factor 8. The Sunset MEC measurements agreed within around 17 % with the SP2 MrBC values. The largest overestimations of MEC were observed when the total carbon concentrations were below 25 µgCcm-2 , which is probably linked to the incorrect determination of the organic carbon (OC)–EC split point. Another cause of the discrepancy between instruments was found to be the limited detection range of the SP2, which did not allow for the total detection of fine rBC particles. The procedure used to estimate the missing mass fraction of rBC not covered by the measurement range of the SP2 was found to be critical. We found that a time-dependent correction based on fitting the observed rBC size distribution with a multimodal lognormal distribution is needed to accurately estimate MrBC over a larger size range. [ABSTRACT FROM AUTHOR]

The Aethalometer is a widely used instrument for black carbon (BC) mass concentration and light absorption coefficient (babs) measurements around the world. However, field intercomparison of the two popular models, dual-spot (AE33) and single-spot (AE31) Aethalometers, remains limited; in addition, the difference in secondary brown carbon (BrCsec) light absorption estimation between the two models is largely unknown. We performed full-year collocated AE33 and AE31 measurements in a megacity in southern China – Guangzhou. The babs values agree well between the two Aethalometers (R2 > 0.95), with AE33 / AE31 slopes ranging from 0.87 to 1.04 for seven wavelengths. AE33 consistently exhibits lower limits of detection (LODs) than AE31 for time resolutions of 2 to 60 min. The AE33 / AE31 slope for equivalent BC (eBC) was 1.2, implying the need for site-specific post-correction. The absorption Ångström exponent (AAE) obtained from different approaches does not agree very well between the two models, with the biggest discrepancy found in AAE880/950. The estimated BrCsec light absorption at 370 nm (babs370_BrCsec) was calculated using the minimum- R -squared (MRS) method for both Aethalometers. The babs370_BrCsec comparison yields a slope of 0.78 and an R2 of 0.72 between the two models, implying a non-negligible inter-instrument difference. This study highlights the high consistency in babs but less so in AAE between AE31 and AE33 and reveals site-specific correction for eBC estimation and non-negligible difference in BrCsec estimation. The results are valuable for data continuity in long-term Aethalometer measurements when transitioning from the older (AE31) to the newer (AE33) model, as anticipated in permanent global-climate and air-quality stations. [ABSTRACT FROM AUTHOR]

Currently, emissions from internal combustion vehicles are not properly monitored throughout their life cycle. In particular, a small share of vehicles (< 20 %) with malfunctioning after-treatment systems and old vehicles with outdated engine technology are responsible for the majority (60 %–90 %) of traffic-related emissions. Remote emission sensing (RES) is a method used for screening emissions from a large number of in-use vehicles. Commercial open-path RES systems are capable of providing emission factors for many gaseous compounds, but they are less accurate and reliable for particulate matter (PM). Point sampling (PS) is an extractive RES method where a portion of the exhaust is sampled and then analyzed. So far, PS studies have been predominantly conducted on a rather small scale and have mainly analyzed heavy-duty vehicles (HDVs), which have high exhaust flow rates. In this work, we present a comprehensive PS system that can be used for large-scale screening of PM and gas emissions, largely independent of the vehicle type. The data analysis framework developed here is capable of processing data from thousands of vehicles. The core of the data analysis is our peak detection algorithm (TUG-PDA), which determines and separates emissions down to a spacing of just a few seconds between vehicles. We present a detailed evaluation of the main influencing factors on PS measurements by using about 100 000 vehicle records collected from several measurement locations, mainly in urban areas. We show the capability of the emission screening by providing real-world black carbon (BC), particle number (PN) and nitrogen oxide (NOx) emission trends for various vehicle categories such as diesel and petrol passenger cars or HDVs. Comparisons with open-path RES and PS studies show overall good agreement and demonstrate the applicability even for the latest Euro emission standards, where current open-path RES systems reach their limits. [ABSTRACT FROM AUTHOR]

The mixing state of black carbon (BC) aerosols, which is the diameter ratio of coated particle to BC core (Dp/Dc), can be retrieved by the single-particle soot photometer (SP2). However, the retrieved Dp/Dc contains errors, because the core–shell model and Mie scattering calculation are normally employed in the retrieval principle of SP2 and the spherical core–shell structure seriously deviated from the real morphology of coated BC. In this study, fractal models are constructed to represent thinly and thickly coated BC particles for optical simulations, the differential scattering cross-sections are selected as references to conduct optical retrieval of particle diameter (Dp) based on Mie theory, just like the retrieval principle of SP2, and the volume equivalent diameter of BC core (Dc) is the same for fractal and spherical models. Then, the retrieval errors of the mixing state (Dp/Dc) of BC are investigated from numerical aspects, and the estimation accuracy of BC radiative forcing is analyzed through the simple forcing efficiency (SFE) equation with SP2 retrieval results taken into consideration. Results show that SP2 retrieved Dp/Dc based on Mie theory underestimates the realistic Dp/Dc of coated BC at most particle sizes. The retrieval errors of Dp/Dc of thinly coated BC for both single particles and particle groups are larger than those of thickly coated BC. In addition, evaluation errors of radiative forcing of coated BC caused by retrieval errors of SP2 are up to about 55 % and 95 % at 1064 and 532 nm , respectively. This study provides meaningful referential understandings of the retrieved Dp/Dc of SP2 based on Mie scattering. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is a component of particulate matter, emitted from the incomplete combustion of carbonaceous fuels. The presence of BC in the atmosphere can disrupt the atmospheric radiation budget, and exposure to BC can adversely affect human health. Multi-wavelength light-absorption-based dual-spot aethalometers can be used to quantify the source and characteristics of BC from traffic or biomass-burning-based sources. However, aethalometer measurements are affected by artifacts such as aerosol loading and light scattering; hence, they often need correction to reduce measurement uncertainty. This work assesses the performance of the recently developed portable aethalometer (MA300, AethLabs). Due to their portability and ease of usage, MA300s can be suitable for mobile and personal exposure monitoring. Here, we evaluate BC concentration and source apportionment accuracy of three MA300 units relative to a widely used aethalometer, the AE33 (Magee Scientific). Synchronous field measurements were performed at a major traffic intersection during regular and wildfire-smoke-affected days in Vancouver, Canada. We find that MA300-reported BC mass concentrations were strongly correlated (Slope range between 0.73 and 1.01, with R2 = 0.9) compared to the reference instrument, yet there is visible instrumental variability in the normalized concentrations (5 %) across three units. The mean absolute error of MA300-reported BC concentrations ranged between 0.44–0.98 µ g m -3 , with the highest deviations observed in wildfire-smoke-affected polluted days. From the aerosol light absorption measurement perspective, MA300s tend to underestimate the absorption coefficients (babs) across the five wavelengths. UV channel light absorption results were subjected to the highest amount of noise and were found to be consistently underestimating in all the MA300 units, leading to systematic bias in source apportionment analysis. Absorption Ångström exponent values from the MA300 units were able to capture the variability of aerosol sources within a day, with a mean value of 1.15 during clean days and 1.46 during wildfire-smoke-affected days. We investigated the application of the latest non-linear aethalometer correction protocols in the MA300 and found that flow fluctuations enhanced noise across all channels, compared to onboard instrument correction. We also identify that the UV (λ = 370 nm) channel absorption measurements are most sensitive to instrumental artifacts during the wildfire-smoke-affected period. Hence, as an alternative to traditional UV and IR (λ = 880 nm)-based BC source apportionment methods, in this work, we tested the blue (λ = 470 nm) and IR wavelengths for BC source apportionment calculation. When the blue–IR-based source apportionment technique is adopted instead of the UV–IR, there is a 10 % (on average) decrease in the percentage difference of the apportioned components from the reference monitor. [ABSTRACT FROM AUTHOR]

Black carbon (BC) aerosol typically has two major sources in the urban environment: traffic and domestic biomass burning, which has a significant contribution to urban air pollution during the heating season. Traffic emissions have been widely studied by both laboratory experiments (individual vehicle emission) and real-world measurement campaigns (fleet emission). However, emission information from biomass burning is limited, especially an insufficiency of experimental results from real-world studies. In this work, the black carbon burden in the urban atmosphere was apportioned to fossil fuel (FF) and biomass burning (BB) related components using the Aethalometer source apportionment model. Applying the BC source apportionment information, the combustion-related CO 2 was apportioned by multilinear regression analysis, supposing that both CO 2 components should be correlated with their corresponding BC component. The combination of the Aethalometer model with the multilinear regression analysis (AM-MLR) provided the source-specific emission ratios (ERs) as the slopes of the corresponding BC–CO 2 regressions. Based on the ER values, the source-specific emission factors (EFs) were determined using the carbon content of the corresponding fuel. The analysis was carried out on a 3-month-long BC and CO 2 dataset collected at three monitoring locations in Ljubljana, Slovenia, between December 2019 and March 2020. The measured mean site-specific concentration values were in the 3560–4830 ng m -3 and 458–472 ppm ranges for BC and CO 2 , respectively. The determined average EFs for BC were 0.39 and 0.16 g(kg fuel) -1 for traffic and biomass burning, respectively. It was also concluded that the traffic-related BC component dominates the black carbon concentration (55 %–64 % depending on the location), while heating has the major share in the combustion-related CO 2 (53 %–62 % depending on the location). The method gave essential information on the source-specific emission factors of BC and CO 2 , enabling better characterization of urban anthropogenic emissions and the respective measures that may change the anthropogenic emission fingerprint. [ABSTRACT FROM AUTHOR]

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 MAC BC 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. [ABSTRACT FROM AUTHOR]

Black carbon (BC) is an important atmospheric component with strong light absorption. Many attempts have been made to measure BC mass size distribution (BCMSD) for its significant impact on climate and public health. Larger-coverage BCMSD, ranging from upper submicron particles sizes to larger than 1 µm , contributes to a substantial proportion of total BC mass and absorption. However, the current time resolution of larger-coverage BCMSD measurement was limited to 1 d, which was insufficient to characterize variation of larger-coverage BCMSD. In this study, a new method to determine equivalent BCMSD (eBCMSD) was proposed from size-resolved absorption coefficient measured by an aerodynamic aerosol classifier in tandem with an aethalometer. The proposed method could measure larger-coverage eBCMSD with a time resolution as high as 1 h and was validated by comparing the measurement results with refractory BCMSD (rBCMSD) measured by a differential mobility analyzer in tandem with a single-particle soot photometer (DMA–SP2) for particle sizes larger than 300 nm during a field measurement in the Yangtze River Delta. Bulk refractory BC mass concentration (mrBC,bulk) by DMA–SP2 was underestimated by 33 % compared to bulk equivalent BC mass concentration (meBC,bulk) by this method because of the limited size range of measurement for DMA–SP2. Uncertainty analysis of this method was performed with respect to mass absorption cross-section (MAC), transfer function inversion, number fraction of BC-containing particle and instrumental noise. The results indicated that MAC was the main uncertainty source, leading to meBC,bulk values that varied from -20 % to 28 %. With the advantage of a wide size coverage up to 1.5 µm , high time resolution, easy operation and low cost, this method is expected to have wide applications in field measurement for better estimating the radiative properties and climate effects of BC. [ABSTRACT FROM AUTHOR]

A new regulatory standard for non-volatile particulate matter (nvPM) mass-based emissions from aircraft engines has been adopted by the International Civil Aviation Organisation. One of the instruments used for the regulatory nvPM mass emissions measurements in aircraft engine certification tests is the Artium Technologies LII 300, which is based on laser-induced incandescence. The LII 300 response has been shown in some cases to vary with the type of black carbon particle measured. Hence it is important to identify a suitable black carbon emission source for instrument calibration. In this study, the relationship between the nvPM emissions produced by different engine sources and the response of the LII 300 instrument utilising the auto-compensating laser-induced incandescence (AC-LII) method was investigated. Six different sources were used, including a turboshaft helicopter engine, a diesel generator, an intermediate pressure test rig of a single-sector combustor, an auxiliary power unit gas turbine engine, a medium-sized diesel engine, and a downsized turbocharged direct-injection gasoline engine. Optimum LII 300 laser fluence levels were determined for each source and operating condition evaluated. It was found that an optimised laser fluence can be valid for real-time measurements from a variety of sources, where the mass concentration was independent of laser fluence levels covering the typical operating ranges for the various sources. However, it is important to perform laser fluence sweeps to determine the optimum fluence range as differences were observed in the laser fluence required between sources and fuels. We discuss the measurement merits, variability, and best practices in the real-time quantification of nvPM mass concentration using the LII 300 instrument and compare that with other diagnostic techniques, namely absorption-based methods such as photoacoustic spectroscopy (using a photoacoustic extinctiometer, PAX, and a micro soot sensor, MSS) and thermal-optical analysis (TOA). Particle size distributions were also measured using a scanning mobility particle sizer (SMPS). Overall, the LII 300 provides robust and consistent results when compared with the other diagnostic techniques across multiple engine sources and fuels. The results from this study will inform the development of updated calibration protocols to ensure repeatable and reproducible measurements of nvPM mass emissions from aircraft engines using the LII 300. [ABSTRACT FROM AUTHOR]

Atmospheric particles have several impacts on health and the environment, especially in urban areas. Parts of those particles are not fresh and have undergone atmospheric chemical and physical processes. Due to a lack of representativeness of experimental conditions and experimental artifacts such as particle wall losses in chambers, there are uncertainties on the effects of physical processes (condensation, nucleation and coagulation) and their role in particle evolution from modern vehicles. This study develops a new method to correct wall losses, accounting for size dependence and experiment-to-experiment variations. It is applied to the evolution of fresh diesel exhaust particles to characterize the physical processes which they undergo. The correction method is based on the black carbon decay and a size-dependent coefficient to correct particle distributions. Six diesel passenger cars, Euro 3 to Euro 6, were driven on a chassis dynamometer with Artemis Urban cold start and Artemis Motorway cycles. Exhaust was injected in an 8 m 3 chamber with Teflon walls. The physical evolution of particles was characterized during 6 to 10 h. Increase in particle mass is observed even without photochemical reactions due to the presence of intermediate-volatility organic compounds and semi-volatile organic compounds. These compounds were quantified at emission and induce a particle mass increase up to 17 % h -1 , mainly for the older vehicles (Euro 3 and Euro 4). Condensation is 4 times faster when the available particle surface is multiplied by 6.5. If initial particle number concentration is below [8–9] × 10 4 cm -3 , a nucleation mode seems to be present but not measured by a scanning mobility particle sizer (SMPS). The growth of nucleation-mode particles results in an increase in measured [PN]. Above this threshold, particle number concentration decreases due to coagulation, up to - 27 % h -1. Under those conditions, the chamber and experimental setup are well suited to characterizing and quantifying the process of coagulation. [ABSTRACT FROM AUTHOR]

Long-term measurements of atmospheric mass concentrations of black carbon (BC) are needed to investigate changes in its emission, transport, and deposition. However, depending on instrumentation, parameters related to BC such as aerosol absorption coefficient (babs) have been measured instead. Most ground-based measurements of babs in the Arctic have been made by filter-based absorption photometers, including particle soot absorption photometers (PSAPs), continuous light absorption photometers (CLAPs), Aethalometers, and multi-angle absorption photometers (MAAPs). The measured babs can be converted to mass concentrations of BC (MBC) by assuming the value of the mass absorption cross section (MAC; MBC= babs/ MAC). However, the accuracy of conversion of babs to MBC has not been adequately assessed. Here, we introduce a systematic method for deriving MAC values from babs measured by these instruments and independently measured MBC. In this method, MBC was measured with a filter-based absorption photometer with a heated inlet (COSMOS). COSMOS-derived MBC (MBC (COSMOS)) is traceable to a rigorously calibrated single particle soot photometer (SP2), and the absolute accuracy of MBC (COSMOS) has been demonstrated previously to be about 15 % in Asia and the Arctic. The necessary conditions for application of this method are a high correlation of the measured babs with independently measured MBC and long-term stability of the regression slope, which is denoted as MAC cor (MAC derived from the correlation). In general, babs – MBC (COSMOS) correlations were high (r2= 0.76–0.95 for hourly data) at Alert in Canada, Ny-Ålesund in Svalbard, Barrow (NOAA Barrow Observatory) in Alaska, Pallastunturi in Finland, and Fukue in Japan and stable for up to 10 years. We successfully estimated MAC cor values (10.8–15.1 m 2 g -1 at a wavelength of 550 nm for hourly data) for these instruments, and these MAC cor values can be used to obtain error-constrained estimates of MBC from babs measured at these sites even in the past, when COSMOS measurements were not made. Because the absolute values of MBC at these Arctic sites estimated by this method are consistent with each other, they are applicable to the study of spatial and temporal variation in MBC in the Arctic and to evaluation of the performance of numerical model calculations. [ABSTRACT FROM AUTHOR]