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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.more » « less
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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.more » « less
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