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Creators/Authors contains: "Chen, L.‐W. Antony"

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  1. Brown carbon (BrC) plays an important role in global radiative budget but there have been few studies on BrC in Arctic despite rapid warming and increasing wildfires in this region. Here we investigate the optical properties of BrC from boreal fires in Alaska summer, with two sets of measurements from PILS-LWCC-TOC (Particle-Into-Liquid-Sampler – Liquid-Waveguide Capillary flow-through optical Cell - Total-Organic-Carbon analyzer) and filter measurements. We show that during intense wildfires, the mass absorption coefficient at 365 nm (MAC365) from water soluble organic carbon (WSOC) remained stable at ∼1 m2 g−1. With all plumes sampled and derived transport time, we show a decrease of MAC365 with plume age, with a shorter photobleaching lifetime (∼11 h) at 365 nm compared to 405 nm (∼20 h). The total absorption by organic aerosols measured from filters at 365 nm is higher than the absorption by WSOC by a factor 2–3, suggesting a dominant role of insoluble organic carbon. Overall BrC dominates absorption in the near-ultraviolet and visible radiation during wildfire season in Alaska summer. 
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  2. As the importance of non-tailpipe particles (NTP) over tailpipe emissions from urban traffic has been increasing, there is a need to evaluate NTP contributions to ambient particulate matter (PM) using representative source profiles. The Brake and Tire Wear Study conducted in Los Angeles, California in the winter of 2020 collected 64 PM2.5 and 64 PM10 samples from 32 pairs of downwind-upwind measurements at two near-road locations (I-5 in Anaheim and I-710 in Long Beach). These samples were characterized for inorganic and organic markers and, along with locally-developed brake wear, tire wear, and road dust source profiles, subject to source apportionment using the effective-variance chemical mass balance (EV-CMB) model. Model results highlighted the dominance of resuspended dust in both PM2.5 (23–33%) and PM10 (32–53%). Brake and tire wear contributed more to PM2.5 than tailpipe exhausts (diesel + gasoline) for I-5 (29–30% vs. 19–21%) while they were comparable for I-710 (15–17% vs. 15–19%). For PM10, the brake and tire wear contributions were 2–3 times the exhaust contributions. Different fleet compositions on and near I-5 and I-710 appeared to influence the relative importance of NTP and exhaust sources. The downwind-upwind differences in source contributions were often insignificant, consistent with small and/or nearly equal impacts of adjacent highway traffic emissions on the downwind and upwind sites. The utility of sole markers, such as barium and zinc, to predict brake and tire wear abundances in ambient PM is evaluated. 
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  3. Brown carbon (BrC) has a substantial direct radiative effect, but current estimates of its impact on radiative balance are highly uncertain due to a lack of measurements of its light-absorbing properties, such as mass absorption efficiency (MAE). Here, we present a new analytical paradigm based on a Bayesian inference (BI) model that takes multiwavelength aethalometer measurements and total carbon data to resolve the concentrations of black carbon and BrC, and MAEs of BrC on a sample-by-sample basis. Hourly MAEs, unattainable in previous studies, can now be calculated, enabling the first-time observation of the darkening-bleaching dynamics of BrC in response to photochemical transformation. We demonstrate the application of this BI model to analyze measurements collected over one year (2021–2022) in Hong Kong. Diel variations in MAE370 nm of BrC reveal a darkening-to-bleaching transition occurring between 8 and 10 o’clock when the solar irradiance ranges from 30 to 400 W m–2. Furthermore, we consistently observe an increase in MAE370 nm of BrC with nitrogen oxide concentrations, suggesting the enhanced formation of nitrogenous organics. This BI model-based data analysis would bring forth a breakthrough in amassing observation data of BrC and its MAEs in diverse ambient environments and with high time resolution. 
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