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Brown carbon light absorptivity is associated with organic aerosol volatility and elemental carbon concentrations.

 

Wildfires emit large amounts of black carbon and light-absorbing organic carbon, known as brown carbon, into the atmosphere. These particles perturb Earth’s radiation budget through absorption of incoming shortwave radiation. It is generally thought that brown carbon loses its absorptivity after emission in the atmosphere due to sunlight-driven photochemical bleaching. Consequently, the atmospheric warming effect exerted by brown carbon remains highly variable and poorly represented in climate models compared with that of the relatively nonreactive black carbon. Given that wildfires are predicted to increase globally in the coming decades, it is increasingly important to quantify these radiative impacts. Here we present measurements of ensemble-scale and particle-scale shortwave absorption in smoke plumes from wildfires in the western United States. We find that a type of dark brown carbon contributes three-quarters of the short visible light absorption and half of the long visible light absorption. This strongly absorbing organic aerosol species is water insoluble, resists daytime photobleaching and increases in absorptivity with night-time atmospheric processing. Our findings suggest that parameterizations of brown carbon in climate models need to be revised to improve the estimation of smoke aerosol radiative forcing and associated warming.

 

Abstract. Black carbon (BC) is one of the dominant absorbing aerosol species in the atmosphere. It normally has complex fractal-like structures due to the aggregation process during combustion. A wide range of aerosol–radiation interactions (ARIs) of BC have been reported throughout experimental and modeling studies. One reason for the large discrepancies among multiple studies is the application of the oversimplified spherical morphology for BC in ARI estimates. In current climate models, the Mie theory is commonly used to calculate the optical properties of spherical BC aerosols. Here, we employ a regional chemical transport model coupled with a radiative transfer code that utilizes the non-spherical BC optical simulations to re-evaluate the effects of particles' morphologies on BC shortwave ARI, and the wavelength range of 0.3–4.0 µm was considered. Anthropogenic activities and wildfires are two major sources of BC emissions. Therefore, we choose the typical polluted area in eastern China, which is dominated by anthropogenic emissions, and the fire region in the northwest US, which is dominated by fire emissions in this study. A 1-month simulation in eastern China and a 7 d simulation in the fire region in the northwest US were performed. The fractal BC model generally presents a larger clear-sky ARI compared to the spherical BC model. Assuming BC particles are externally mixed with other aerosols, the relative differences in the time-averaged clear-sky ARI between the fractal model with a fractal dimension (Df) of 1.8 and the spherical model are 12.1 %–20.6 % and 10.5 %–14.9 % for typical polluted urban cities in China and fire sites in the northwest US, respectively. Furthermore, the regional-mean clear-sky ARI is also significantly affected by the BC morphology, and relative differences of 17.1 % and 38.7 % between the fractal model with a Df of 1.8 and the spherical model were observed in eastern China and the northwest US, respectively. However, the existence of clouds would weaken the BC morphological effects. The time-averaged all-sky ARI relative differences between the fractal model with a Df of 1.8 and the spherical model are 4.9 %–6.4 % and 9.0 %–11.3 % in typical urban polluted cities and typical fire sites, respectively. Besides, for the regional-mean all-sky ARI, the relative differences between the fractal model and the spherical model are less than 7.3 % and 16.8 % in the polluted urban area in China and the fire region in the US, respectively. The results imply that current climate modeling may significantly underestimate the BC ARI uncertainties as the morphological effects on BC ARI are ignored in most climate models. 

Abstract. Measurement of light absorption of solar radiation byaerosols is vital for assessing direct aerosol radiative forcing, whichaffects local and global climate. Low-cost and easy-to-operate filter-basedinstruments, such as the Particle Soot Absorption Photometer (PSAP), that collect aerosols on a filter and measure light attenuation through thefilter are widely used to infer aerosol light absorption. However,filter-based absorption measurements are subject to artifacts that aredifficult to quantify. These artifacts are associated with the presence ofthe filter medium and the complex interactions between the filter fibers and accumulated aerosols. Various correction algorithms have been introduced to correct for the filter-based absorption coefficient measurements toward predicting the particle-phase absorption coefficient (Babs). However, the inability of these algorithms to incorporate into their formulations the complex matrix of influencing parameters such as particle asymmetry parameter, particle size, and particle penetration depth results in prediction of particle-phase absorption coefficients with relatively low accuracy. The analytical forms of corrections also suffer from a lack of universal applicability: different corrections are required for rural andurban sites across the world. In this study, we analyzed and compared 3 months of high-time-resolution ambient aerosol absorption data collectedsynchronously using a three-wavelength photoacoustic absorption spectrometer (PASS) and PSAP. Both instruments were operated on the same sampling inletat the Department of Energy's Atmospheric Radiation Measurement program's Southern Great Plains (SGP) user facility in Oklahoma. We implemented the two mostcommonly used analytical correction algorithms, namely, Virkkula (2010) and the average of Virkkula (2010) and Ogren (2010)–Bond et al. (1999) as well as a random forest regression (RFR) machine learning algorithm to predict Babs values from the PSAP's filter-based measurements. The predicted Babs was compared against the reference Babs measured by the PASS. The RFR algorithm performed the best by yielding the lowest root mean squareerror of prediction. The algorithm was trained using input datasets from the PSAP (transmission and uncorrected absorption coefficient), a co-locatednephelometer (scattering coefficients), and the Aerosol Chemical Speciation Monitor (mass concentration of non-refractory aerosol particles). A revisedform of the Virkkula (2010) algorithm suitable for the SGP site has beenproposed; however, its performance yields approximately 2-fold errors when compared to the RFR algorithm. To generalize the accuracy and applicabilityof our proposed RFR algorithm, we trained and tested it on a dataset oflaboratory measurements of combustion aerosols. Input variables to thealgorithm included the aerosol number size distribution from the Scanning Mobility Particle Sizer, absorption coefficients from the filter-basedTricolor Absorption Photometer, and scattering coefficients from amultiwavelength nephelometer. The RFR algorithm predicted Babs values within 5 % of the reference Babs measured by the multiwavelength PASS during the laboratory experiments. Thus, we show that machine learningapproaches offer a promising path to correct for biases in long-termfilter-based absorption datasets and accurately quantify their variabilityand trends needed for robust radiative forcing determination.