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Long-term measurements of the mass concentration of black carbon (BC) in the atmosphere (MBC) with well-constrained accuracy are indispensable to quantify its emission, transport, and deposition. The aerosol light absorption coefficient (babs), usually measured by a filter-based absorption photometer, including an Aethalometer (AE), is often used to estimate MBC. The measured babs is converted to MBC by assuming a value for the mass absorption cross section (MAC). Previously, we derived the MAC for AE (MAC (AE)) from measured babs and independently measured MBC values at two sites in the Arctic. MBC was measured with a filter-based absorption photometer with a heated inlet (COSMOS). The accuracy of the COSMOS-derived MBC (MBC (COSMOS)) was within about 15%. Here, we obtained additional MAC (AE) measurements to improve understanding of its variability and uncertainty. We measured babs (AE) and MBC (COSMOS) at Alert (2018–2020), Barrow (2012–2022), Ny-Ålesund (2012–2019), and Pallas (2019–2022). At Pallas, we also obtained four-wavelength photoacoustic aerosol absorption spectrometer (PAAS-4λ) measurements of babs. babs (AE) and MBC (COSMOS) were tightly correlated; the average MAC (AE) at the four sites was 11.4 ± 1.2 m2 g−1 (mean ± 1σ) at 590 nm and 7.76 ± 0.73 m2 g−1 at 880 nm. The spatial variability of MAC (AE) was about 11% (1σ), and its year-to-year variability was about 18%. We compared MAC (AE) in the Arctic with values at mid-latitudes, measured by previous studies, and with values obtained by using other types of filter-based absorption photometer, and PAAS-4λ. Copyright © 2024 American Association for Aerosol Research [ABSTRACT FROM AUTHOR]

Representing mixing state of black carbon (BC) is challenging for global climate models (GCMs). The Community Atmosphere Model version 6 (CAM6) with the four‐mode version of the Modal Aerosol Module (MAM4) represents aerosols as fully internal mixtures with uniform composition within each aerosol mode, resulting in high degree of internal mixing of BC with non‐BC species and large mass ratio of coating to BC (RBC, the mass ratio of non‐BC species to BC in BC‐containing particles). To improve BC mixing state representation, we coupled a machine learning (ML) model of BC mixing state index trained on particle‐resolved simulations to the CAM6 with MAM4 (MAM4‐ML). In MAM4‐ML, we use RBC to partition accumulation mode particles into two new modes, BC‐free particles and BC‐containing particles. We adjust RBC to make the modeled BC mixing state index (χmode) match the one predicted by the ML model (χML). On a global average, the mass fraction of BC‐containing particles in accumulation mode decreases from 100% (MAM4‐default) to 48% (MAM4‐ML). The globally averaged χmode decreases from 78% (MAM4‐default) to 63% (MAM4‐ML, 19% reduction) and agrees well with χML (66%). The RBC decreases by 52% for accumulation mode and better agrees with observations. The hygroscopicity drops by 9% for BC‐containing particles in accumulation mode, leading to a 20% reduction in the BC activation fraction. The surface BC concentration increases most (6.9%) in the Arctic, and the BC burden increases by 4%, globally. Our study highlights the application of the ML model for improving key aerosol processes in GCMs. Plain Language Summary: Black carbon (BC) mixing state is an important property for assessing impacts of BC on human health and climate. It describes how BC is distributed among the particle population and within individual particles. Due to computational costs, global climate models (GCMs) consider aerosols as either external mixtures (e.g., bulk models) or fully internal mixtures with uniform composition within a certain size range (e.g., an aerosol bin in sectional models or an aerosol mode in modal models). To improve BC mixing state representation, we coupled a machine learning (ML) model learned from particle‐resolved simulations to the online simulations of the Community Atmosphere Model version 6 (CAM6) with the four‐mode version of the Modal Aerosol Module (MAM4‐ML). We used the mass ratio of coating to BC (RBC) to determine the mass fraction of BC‐free particles and BC‐containing particles, and we adjusted RBC to make the modeled BC mixing state match ML model. The MAM4‐ML model reduces the degree of internal mixture of BC substantially. In addition, MAM4‐ML RBC is reduced by 52%, leading to a 20% reduction in BC activation fraction and a 4% increase in BC burden. This study proposes a method for the application of the ML to improve GCMs. Key Points: Machine learning model trained on particle‐resolved simulations has been coupled to CAM6 MAM4 to improve BC mixing state representationThe BC mixing state index is reduced by 19%, and the mass ratio of coating to BC is reduced by 52%, in better agreement with observationsDue to the drop in hygroscopicity of BC‐containing aerosol (9%), BC activation fraction decreased by 20%, and BC burden increased by 4% [ABSTRACT FROM AUTHOR]

A warming Arctic is expected to exacerbate wildfires in Siberia, potentially creating a critical feedback to the Arctic climate change. However, our understanding of these fire-climate interactions remains limited. This study investigated changes in East Siberian wildfires and their influence on fire emissions, aerosol optical depth (AOD), and the surface clear-sky insolation across the Siberian Arctic from 2000 to 2020 using satellite observations. Our analysis reveals a substantial increase in wildfires, with fire counts doubling (a 114% increase) and fire radiative power surging by 8.4 × 106 MW compared to the early 21st century. Over 93% of this increase occurred during the boreal summer months. These intensified wildfires led to a significant rise in aerosol emission (organic carbon, PM2.5, and black carbon) exceeding 75% in East Siberia. Consequently, fire-season AOD in the Siberian Arctic increased by 33% (6.0 × 10−2), with 85% (5.1 × 10−2) attributable to wildfire changes. The wildfire-associated increase in AOD resulted in enhanced clear-sky dimming of 4.1 ± 3.2 W m−2 across the Siberian Arctic from 2000 to 2020. These findings suggest a critical feedback mechanism: a warming Arctic drives increased wildfires in Siberia, which in turn significantly impact the Arctic surface radiative budget through enhanced clear-sky dimming. Future simulations and projections for the Arctic should prioritize incorporating the feedback effects of intensifying wildfires. • Active fire points in East Siberia increased by 114% from 2000 to 2020, nearly doubled. • Fire-season AOD in the Siberian Arctic increased by 33% during the study period. • Wildfires increase could explain 85% of the elevated AOD in the Siberian Arctic. • Wildfire-induced AOD increase led to a 4.1 W m−2 clear-sky dimming in the Siberian Arctic. [ABSTRACT FROM AUTHOR]