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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]