Black carbon aerosols over Indian Ocean have unique source fingerprint and optical characteristics during monsoon season.

Effects of aerosols such as black carbon (BC) on climate and buildup of the monsoon over the Indian Ocean are insufficiently quantified. Uncertain contributions from various natural and anthropogenic sources impede our understanding. Here, we use observations over 5 y of BC and its isotopes at a remote island observatory in northern Indian Ocean to constrain loadings and sources during little-studied monsoon season. Carbon-14 data show a highly variable yet largely fossil (65 ± 15%) source mixture. Combining carbon-14 with carbon-13 reveals the impact of African savanna burning, which occasionally approach 50% (48 ± 9%) of the total BC loadings. The BC mass-absorption cross-section for this regime is 7.6 ± 2.6 m2/g, with higher values during savanna fire input. Taken together, the combustion sources, longevity, and optical properties of BC aerosols over summertime Indian Ocean are different than the more-studied winter aerosol, with implications for chemical transport and climate model simulations of the Indian monsoon.

Observational Evidence of Large Contribution from Primary Sources for Carbon Monoxide in the South Asian Outflow.

South Asian air is among the most polluted in the world, causing premature death of millions and asserting a strong perturbation of the regional climate. A central component is carbon monoxide (CO), which is a key modulator of the oxidizing capacity of the atmosphere and a potent indirect greenhouse gas. While CO concentrations are declining elsewhere, South Asia exhibits an increasing trend for unresolved reasons. In this paper, we use dual-isotope (δ13C and δ18O) fingerprinting of CO intercepted in the South Asian outflow to constrain the relative contributions from primary and secondary CO sources. Results show that combustion-derived primary sources dominate the wintertime continental CO fingerprint (fprimary ∼ 79 ± 4%), significantly higher than the global estimate (fprimary ∼ 55 ± 5%). Satellite-based inventory estimates match isotope-constrained fprimary-CO, suggesting observational convergence in source characterization and a prospect for model-observation reconciliation. This "ground-truthing" emphasizes the pressing need to mitigate incomplete combustion activities for climate/air quality benefits in South Asia.

Atmospheric Black Carbon Loadings and Sources over Eastern Sub-Saharan Africa Are Governed by the Regional Savanna Fires.

Vast black carbon (BC) emissions from sub-Saharan Africa are perceived to warm the regional climate, impact rainfall patterns, and impair human respiratory health. However, the magnitudes of these perturbations are ill-constrained, largely due to limited ground-based observations and uncertainties in emissions from different sources. This paper reports multiyear concentrations of BC and other key PM2.5 aerosol constituents from the Rwanda Climate Observatory, serving as a regional receptor site. We find a strong seasonal cycle for all investigated chemical species, where the maxima coincide with large-scale upwind savanna fires. BC concentrations show notable interannual variability, with no clear long-term trend. The Δ14C and δ13C signatures of BC unambiguously show highly elevated biomass burning contributions, up to 93 ± 3%, with a clear and strong savanna burning imprint. We further observe a near-equal contribution from C3 and C4 plants, irrespective of air mass source region or season. In addition, the study provides improved relative emission factors of key aerosol components, organic carbon (OC), K+, and NO3-, in savanna-fires-influenced background atmosphere. Altogether, we report quantitative source constraints on Eastern Africa BC emissions, with implications for parameterization of satellite fire and bottom-up emission inventories as well as regional climate and chemical transport modeling.

Rivers across the Siberian Arctic unearth the patterns of carbon release from thawing permafrost.

Climate warming is expected to mobilize northern permafrost and peat organic carbon (PP-C), yet magnitudes and system specifics of even current releases are poorly constrained. While part of the PP-C will degrade at point of thaw to CO2 and CH4 to directly amplify global warming, another part will enter the fluvial network, potentially providing a window to observe large-scale PP-C remobilization patterns. Here, we employ a decade-long, high-temporal resolution record of 14C in dissolved and particulate organic carbon (DOC and POC, respectively) to deconvolute PP-C release in the large drainage basins of rivers across Siberia: Ob, Yenisey, Lena, and Kolyma. The 14C-constrained estimate of export specifically from PP-C corresponds to only 17 ± 8% of total fluvial organic carbon and serves as a benchmark for monitoring changes to fluvial PP-C remobilization in a warming Arctic. Whereas DOC was dominated by recent organic carbon and poorly traced PP-C (12 ± 8%), POC carried a much stronger signature of PP-C (63 ± 10%) and represents the best window to detect spatial and temporal dynamics of PP-C release. Distinct seasonal patterns suggest that while DOC primarily stems from gradual leaching of surface soils, POC reflects abrupt collapse of deeper deposits. Higher dissolved PP-C export by Ob and Yenisey aligns with discontinuous permafrost that facilitates leaching, whereas higher particulate PP-C export by Lena and Kolyma likely echoes the thermokarst-induced collapse of Pleistocene deposits. Quantitative 14C-based fingerprinting of fluvial organic carbon thus provides an opportunity to elucidate large-scale dynamics of PP-C remobilization in response to Arctic warming.

Wintertime Air Quality in Megacity Dhaka, Bangladesh Strongly Affected by Influx of Black Carbon Aerosols from Regional Biomass Burning.

Clean air is a key parameter for a sustainable society, and currently, megacity Dhaka has among the worst air qualities in the world. This results from poorly constrained contributions of a variety of sources from both local emissions and regional influx from the highly polluted Indo-Gangetic Plain, impacting the respiratory health of the 21 million inhabitants in the Greater Dhaka region. An important component of the fine particulate matter (PM2.5) is black carbon (BC) aerosols. In this study, we investigated the combustion sources of BC using a dual carbon isotope (δ13C and Δ14C) in Dhaka during the high-loading winter period of 2013/14 (regular and lockdown/hartal period) in order to guide mitigation policies. On average, BC (13 ± 6 µg m-3) contributed about 9% of the PM2.5 (145 ± 79 µg m-3) loadings. The relative contribution from biomass combustion under regular conditions was 44 ± 1% (with the rest from fossil combustion), while during periods of politically motivated large-scale lockdown of business and traffic, the biomass burning contribution increased to 63 ± 1%. To reduce the severe health impact of BC and other aerosol pollution in Dhaka, mitigation should therefore target regional-scale biomass/agricultural burning in addition to local traffic.

Observed and Modeled Black Carbon Deposition and Sources in the Western Russian Arctic 1800-2014.

Black carbon (BC) particles contribute to climate warming by heating the atmosphere and reducing the albedo of snow/ice surfaces. The available Arctic BC deposition records are restricted to the Atlantic and North American sectors, for which previous studies suggest considerable spatial differences in trends. Here, we present first long-term BC deposition and radiocarbon-based source apportionment data from Russia using four lake sediment records from western Arctic Russia, a region influenced by BC emissions from oil and gas production. The records consistently indicate increasing BC fluxes between 1800 and 2014. The radiocarbon analyses suggest mainly (∼70%) biomass sources for BC with fossil fuel contributions peaking around 1960-1990. Backward calculations with the atmospheric transport model FLEXPART show emission source areas and indicate that modeled BC deposition between 1900 and 1999 is largely driven by emission trends. Comparison of observed and modeled data suggests the need to update anthropogenic BC emission inventories for Russia, as these seem to underestimate Russian BC emissions and since 1980s potentially inaccurately portray their trend. Additionally, the observations may indicate underestimation of wildfire emissions in inventories. Reliable information on BC deposition trends and sources is essential for design of efficient and effective policies to limit climate warming.

Source Quantification of South Asian Black Carbon Aerosols with Isotopes and Modeling.

Black carbon (BC) aerosols perturb climate and impoverish air quality/human health-affecting ∼1.5 billion people in South Asia. However, the lack of source-diagnostic observations of BC is hindering the evaluation of uncertain bottom-up emission inventories (EIs) and thereby also models/policies. Here, we present dual-isotope-based (Δ14C/δ13C) fingerprinting of wintertime BC at two receptor sites of the continental outflow. Our results show a remarkable similarity in contributions of biomass and fossil combustion, both from the site capturing the highly populated highly polluted Indo-Gangetic Plain footprint (IGP; Δ14C-fbiomass = 50 ± 3%) and the second site in the N. Indian Ocean representing a wider South Asian footprint (52 ± 6%). Yet, both sites reflect distinct δ13C-fingerprints, indicating a distinguishable contribution of C4-biomass burning from peninsular India (PI). Tailored-model-predicted season-averaged BC concentrations (700 ± 440 ng m-3) match observations (740 ± 250 ng m-3), however, unveiling a systematically increasing model-observation bias (+19% to -53%) through winter. Inclusion of BC from open burning alone does not reconcile predictions (fbiomass = 44 ± 8%) with observations. Direct source-segregated comparison reveals regional offsets in anthropogenic emission fluxes in EIs, overestimated fossil-BC in the IGP, and underestimated biomass-BC in PI, which contributes to the model-observation bias. This ground-truthing pinpoints uncertainties in BC emission sources, which benefit both climate/air-quality modeling and mitigation policies in South Asia.

Siberian Arctic black carbon sources constrained by model and observation.

Black carbon (BC) in haze and deposited on snow and ice can have strong effects on the radiative balance of the Arctic. There is a geographic bias in Arctic BC studies toward the Atlantic sector, with lack of observational constraints for the extensive Russian Siberian Arctic, spanning nearly half of the circum-Arctic. Here, 2 y of observations at Tiksi (East Siberian Arctic) establish a strong seasonality in both BC concentrations (8 ng⋅m-3 to 302 ng⋅m-3) and dual-isotope-constrained sources (19 to 73% contribution from biomass burning). Comparisons between observations and a dispersion model, coupled to an anthropogenic emissions inventory and a fire emissions inventory, give mixed results. In the European Arctic, this model has proven to simulate BC concentrations and source contributions well. However, the model is less successful in reproducing BC concentrations and sources for the Russian Arctic. Using a Bayesian approach, we show that, in contrast to earlier studies, contributions from gas flaring (6%), power plants (9%), and open fires (12%) are relatively small, with the major sources instead being domestic (35%) and transport (38%). The observation-based evaluation of reported emissions identifies errors in spatial allocation of BC sources in the inventory and highlights the importance of improving emission distribution and source attribution, to develop reliable mitigation strategies for efficient reduction of BC impact on the Russian Arctic, one of the fastest-warming regions on Earth.

Quantifying Degradative Loss of Terrigenous Organic Carbon in Surface Sediments Across the Laptev and East Siberian Sea.

Ongoing permafrost thaw in the Arctic may remobilize large amounts of old organic matter. Upon transport to the Siberian shelf seas, this material may be degraded and released to the atmosphere, exported off-shelf, or buried in the sediments. While our understanding of the fate of permafrost-derived organic matter in shelf waters is improving, poor constraints remain regarding degradation in sediments. Here we use an extensive data set of organic carbon concentrations and isotopes (n = 109) to inventory terrigenous organic carbon (terrOC) in surficial sediments of the Laptev and East Siberian Seas (LS + ESS). Of these ~2.7 Tg terrOC about 55% appear resistant to degradation on a millennial timescale. A first-order degradation rate constant of 1.5 kyr-1 is derived by combining a previously established relationship between water depth and cross-shelf sediment-terrOC transport time with mineral-associated terrOC loadings. This yields a terrOC degradation flux of ~1.7 Gg/year from surficial sediments during cross-shelf transport, which is orders of magnitude lower than earlier estimates for degradation fluxes of dissolved and particulate terrOC in the water column of the LS + ESS. The difference is mainly due to the low degradation rate constant of sedimentary terrOC, likely caused by a combination of factors: (i) the lower availability of oxygen in the sediments compared to fully oxygenated waters, (ii) the stabilizing role of terrOC-mineral associations, and (iii) the higher proportion of material that is intrinsically recalcitrant due to its chemical/molecular structure in sediments. Sequestration of permafrost-released terrOC in shelf sediments may thereby attenuate the otherwise expected permafrost carbon-climate feedback.

Remobilization of Old Permafrost Carbon to Chukchi Sea Sediments During the End of the Last Deglaciation.

Climate warming is expected to destabilize permafrost carbon (PF-C) by thaw-erosion and deepening of the seasonally thawed active layer and thereby promote PF-C mineralization to CO2 and CH4. A similar PF-C remobilization might have contributed to the increase in atmospheric CO2 during deglacial warming after the last glacial maximum. Using carbon isotopes and terrestrial biomarkers (Δ14C, δ13C, and lignin phenols), this study quantifies deposition of terrestrial carbon originating from permafrost in sediments from the Chukchi Sea (core SWERUS-L2-4-PC1). The sediment core reconstructs remobilization of permafrost carbon during the late Allerød warm period starting at 13,000 cal years before present (BP), the Younger Dryas, and the early Holocene warming until 11,000 cal years BP and compares this period with the late Holocene, from 3,650 years BP until present. Dual-carbon-isotope-based source apportionment demonstrates that Ice Complex Deposit-ice- and carbon-rich permafrost from the late Pleistocene (also referred to as Yedoma)-was the dominant source of organic carbon (66 ± 8%; mean ± standard deviation) to sediments during the end of the deglaciation, with fluxes more than twice as high (8.0 ± 4.6 g·m-2·year-1) as in the late Holocene (3.1 ± 1.0 g·m-2·year-1). These results are consistent with late deglacial PF-C remobilization observed in a Laptev Sea record, yet in contrast with PF-C sources, which at that location were dominated by active layer material from the Lena River watershed. Release of dormant PF-C from erosion of coastal permafrost during the end of the last deglaciation indicates vulnerability of Ice Complex Deposit in response to future warming and sea level changes.

Isotope-Based Source Apportionment of EC Aerosol Particles during Winter High-Pollution Events at the Zeppelin Observatory, Svalbard.

Black carbon (BC) aerosol particles contribute to climate warming of the Arctic, yet both the sources and the source-related effects are currently poorly constrained. Bottom-up emission inventory (EI) approaches are challenged for BC in general and the Arctic in particular. For example, estimates from three different EI models on the fractional contribution to BC from biomass burning (north of 60° N) vary between 11% and 68%, each acknowledging large uncertainties. Here we present the first dual-carbon isotope-based (Δ(14)C and δ(13)C) source apportionment of elemental carbon (EC), the mass-based correspondent to optically defined BC, in the Arctic atmosphere. It targeted 14 high-loading and high-pollution events during January through March of 2009 at the Zeppelin Observatory (79° N; Svalbard, Norway), with these representing one-third of the total sampling period that was yet responsible for three-quarters of the total EC loading. The top-down source-diagnostic (14)C fingerprint constrained that 52 ± 15% (n = 12) of the EC stemmed from biomass burning. Including also two samples with 95% and 98% biomass contribution yield 57 ± 21% of EC from biomass burning. Significant variability in the stable carbon isotope signature indicated temporally shifting emissions between different fossil sources, likely including liquid fossil and gas flaring. Improved source constraints of Arctic BC both aids better understanding of effects and guides policy actions to mitigate emissions.

Regionally-varying combustion sources of the January 2013 severe haze events over eastern China.

Thick haze plagued northeastern China in January 2013, strongly affecting both regional climate and human respiratory health. Here, we present dual carbon isotope constrained (Δ(14)C and δ(13)C) source apportionment for combustion-derived black carbon aerosol (BC) for three key hotspot regions (megacities): North China Plain (NCP, Beijing), the Yangtze River Delta (YRD, Shanghai), and the Pearl River Delta (PRD, Guangzhou) for January 2013. BC, here quantified as elemental carbon (EC), is one of the most health-detrimental components of PM2.5 and a strong climate warming agent. The results show that these severe haze events were equally affected (∼ 30%) by biomass combustion in all three regions, whereas the sources of the dominant fossil fuel component was dramatically different between north and south. In the NCP region, coal combustion accounted for 66% (46-74%, 95% C.I.) of the EC, whereas, in the YRD and PRD regions, liquid fossil fuel combustion (e.g., traffic) stood for 46% (18-66%) and 58% (38-68%), respectively. Taken together, these findings suggest the need for a regionally-specific description of BC sources in climate models and regionally-tailored mitigation to combat severe air pollution events in East Asia.

Source Apportionment of Polycyclic Aromatic Hydrocarbons in Central European Soils with Compound-Specific Triple Isotopes (δ(13)C, Δ(14)C, and δ(2)H).

This paper reports the first study applying a triple-isotope approach for source apportionment of polycyclic aromatic hydrocarbons (PAHs). The (13)C/(12)C, (14)C/(12)C, and (2)H/(1)H isotope ratios of PAHs were determined in forest soils from mountainous areas of the Czech Republic, European Union. Statistical modeling applying a Bayesian Markov chain Monte Carlo (MCMC) framework to the environmental triple isotope PAH data and an end-member PAH isotope database allowed comprehensive accounting of uncertainties and quantitative constraints on the PAH sources among biomass combustion, liquid fossil fuel combustion, and coal combustion at low and high temperatures. The results suggest that PAHs in this central European region had a clear predominance of coal combustion sources (75 ± 6%; uncertainties represent 1 SD), mainly coal pyrolysis at low temperature (∼650 °C; 61 ± 8%). Combustion of liquid fossil fuels and biomass represented 16 ± 3 and 9 ± 3% of the total PAH burden (∑PAH14), respectively. Although some soils were located close to potential PAH point sources, the source distribution was within a narrow range throughout the region. These observation-based top-down constraints on sources of environmental PAHs provide a reference for both improved bottom-up emission inventories and guidance for efforts to mitigate PAH emissions.

Chaperone proteostasis in Parkinson's disease: stabilization of the Hsp70/alpha-synuclein complex by Hip.

The ATP-dependent protein chaperone heat-shock protein 70 (Hsp70) displays broad anti-aggregation functions and has a critical function in preventing protein misfolding pathologies. According to in vitro and in vivo models of Parkinson's disease (PD), loss of Hsp70 activity is associated with neurodegeneration and the formation of amyloid deposits of alpha-synuclein (alphaSyn), which constitute the intraneuronal inclusions in PD patients known as Lewy bodies. Here, we show that Hsp70 depletion can be a direct result of the presence of aggregation-prone polypeptides. We show a nucleotide-dependent interaction between Hsp70 and alphaSyn, which leads to the aggregation of Hsp70, in the presence of ADP along with alphaSyn. Such a co-aggregation phenomenon can be prevented in vitro by the co-chaperone Hip (ST13), and the hypothesis that it might do so also in vivo is supported by studies of a Caenorhabditis elegans model of alphaSyn aggregation. Our findings indicate that a decreased expression of Hip could facilitate depletion of Hsp70 by amyloidogenic polypeptides, impairing chaperone proteostasis and stimulating neurodegeneration.

Source forensics of black carbon aerosols from China.

The limited understanding of black carbon (BC) aerosol emissions from incomplete combustion causes a poorly constrained anthropogenic climate warming that globally may be second only to CO2 and regionally, such as over East Asia, the dominant driver of climate change. The relative contribution to atmospheric BC from fossil fuel versus biomass combustion is important to constrain as fossil BC is a stronger climate forcer. The source apportionment is the underpinning for targeted mitigation actions. However, technology-based "bottom-up" emission inventories are inconclusive, largely due to uncertain BC emission factors from small-scale/household combustion and open burning. We use "top-down" radiocarbon measurements of atmospheric BC from five sites including three city sites and two regional sites to determine that fossil fuel combustion produces 80 ± 6% of the BC emitted from China. This source-diagnostic radiocarbon signal in the ambient aerosol over East Asia establishes a much larger role for fossil fuel combustion than suggested by all 15 BC emission inventory models, including one with monthly resolution. Our results suggest that current climate modeling should refine both BC emission strength and consider the stronger radiative absorption associated with fossil-fuel-derived BC. To mitigate near-term climate effects and improve air quality in East Asia, activities such as residential coal combustion and city traffic should be targeted.

Aerosol demasking enhances climate warming over South Asia.

Anthropogenic aerosols mask the climate warming caused by greenhouse gases (GHGs). In the absence of observational constraints, large uncertainties plague the estimates of this masking effect. Here we used the abrupt reduction in anthropogenic emissions observed during the COVID-19 societal slow-down to characterize the aerosol masking effect over South Asia. During this period, the aerosol loading decreased substantially and our observations reveal that the magnitude of this aerosol demasking corresponds to nearly three-fourths of the CO2-induced radiative forcing over South Asia. Concurrent measurements over the northern Indian Ocean unveiled a ~7% increase in the earth's surface-reaching solar radiation (surface brightening). Aerosol-induced atmospheric solar heating decreased by ~0.4 K d-1. Our results reveal that under clear sky conditions, anthropogenic emissions over South Asia lead to nearly 1.4 W m-2 heating at the top of the atmosphere during the period March-May. A complete phase-out of today's fossil fuel combustion to zero-emission renewables would result in rapid aerosol demasking, while the GHGs linger on.

A rationally designed six-residue swap generates comparability in the aggregation behavior of α-synuclein and ß-synuclein.

The aggregation process of α-synuclein, a protein closely associated with Parkinson's disease, is highly sensitive to sequence variations. It is therefore of great importance to understand the factors that define the aggregation propensity of specific mutational variants as well as their toxic behavior in the cellular environment. In this context, we investigated the extent to which the aggregation behavior of α-synuclein can be altered to resemble that of ß-synuclein, an aggregation-resistant homologue of α-synuclein not associated with disease, by swapping residues between the two proteins. Because of the vast number of possible swaps, we have applied a rational design procedure to single out a mutational variant, called α2ß, in which two short stretches of the sequence in the NAC region have been replaced in α-synuclein from ß-synuclein. We find not only that the aggregation rate of α2ß is close to that of ß-synuclein, being much lower than that of α-synuclein, but also that α2ß effectively changes the cellular toxicity of α-synuclein to a value similar to that of ß-synuclein upon exposure of SH-SY5Y cells to preformed oligomers. Remarkably, control experiments on the corresponding mutational variant of ß-synuclein, called ß2α, confirmed that the mutations that we have identified also shift the aggregation behavior of this protein toward that of α-synuclein. These results demonstrate that it is becoming possible to control in quantitative detail the sequence code that defines the aggregation behavior and toxicity of α-synuclein.

Systolic Blood Pressure Response to Exercise in Endurance Athletes in Relation to Oxygen Uptake, Work Rate and Normative Values.

Work rate has a direct impact on the systolic blood pressure (SBP) during aerobic exercise, which may be challenging in the evaluation of the SBP response in athletes reaching high work rates. We aimed to investigate the exercise SBP response in endurance athletes in relation to oxygen uptake (VO2), work rate and to recent reference equations for exercise SBP in the general population. Endurance athletes with a left-ventricular end-diastolic diameter above the reference one performed a maximal bicycle cardiopulmonary exercise test. The increase in SBP during exercise was divided by the increase in VO2 (SBP/VO2 slope) and in Watts, respectively (SBP/W slope). The maximum SBP (SBPmax) and the SBP/W slope were compared to the predicted values. In total, 27 athletes (59% men) were included; mean age, 40 ± 10 years; mean VO2max, 50 ± 5 mL/kg/min. The mean SBP/VO2 slope was 29.8 ± 10.2 mm Hg/L/min, and the mean SBP/W slope was 0.27 ± 0.08 mm Hg/W. Compared to the predicted normative values, athletes had, on average, a 12.2 ± 17.6 mm Hg higher SBPmax and a 0.12 ± 0.08 mm Hg/W less steep SBP/W slope (p < 0.01 and p < 0.001, respectively). In conclusion, the higher SBPmax values and the less steep SBP/W slope highlight the importance of considering work rate when interpreting the SBP response in endurance athletes and suggest a need for specific normative values in athletes to help clinicians distinguish physiologically high maximal blood pressure from a pathological blood pressure response.

14C characteristics of organic carbon in the atmosphere and at glacier region of the Tibetan Plateau.

As an important component of carbonaceous aerosols (CA), organic carbon (OC) exerts a strong, yet insufficiently constrained perturbation of the climate. In this study, we reported sources of OC based on its natural abundance radiocarbon (14C) fingerprinting in aerosols and water-insoluble organic carbon (WIOC) in snowpits across the Tibetan Plateau (TP) - one of the remote regions in the world and a freshwater reservoir for billions of people. Overall, the proportions from 14C-based non-fossil fuel contribution (fnon-fossil) for OC in aerosols was 74 ± 10%, while for WIOC in snowpits was 81 ± 10%, both of which were significantly higher than that of elemental carbon (EC). These indicated sources of OC (WIOC) and EC were different at remote TP. Spatially, high fnon-fossil of WIOC of snowpit samples appeared at the inner part of the TP, indicating the important contribution of local non-fossil sources. Therefore, local non-fossil sources rather than long-range transportation OC dominants its total amount of the TP. In addition, the contribution of local non-fossil sourced WIOC increased during the monsoon period because heavy precipitation removed a high ratio of long-range transportation WIOC. The results of this study showed that not only OC and EC but also their different fuel sources should be treated separately in models to investigate their sources and atmospheric transportation.

Large contribution of fossil-derived components to aqueous secondary organic aerosols in China.

Incomplete understanding of the sources of secondary organic aerosol (SOA) leads to large uncertainty in both air quality management and in climate change assessment. Chemical reactions occurring in the atmospheric aqueous phase represent an important source of SOA mass, yet, the effects of anthropogenic emissions on the aqueous SOA (aqSOA) are not well constrained. Here we use compound-specific dual-carbon isotopic fingerprints (δ13C and Δ14C) of dominant aqSOA molecules, such as oxalic acid, to track the precursor sources and formation mechanisms of aqSOA. Substantial stable carbon isotope fractionation of aqSOA molecules provides robust evidence for extensive aqueous-phase processing. Contrary to the paradigm that these aqSOA compounds are largely biogenic, radiocarbon-based source apportionments show that fossil precursors produced over one-half of the aqSOA molecules. Large fractions of fossil-derived aqSOA contribute substantially to the total water-soluble organic aerosol load and hence impact projections of both air quality and anthropogenic radiative forcing. Our findings reveal the importance of fossil emissions for aqSOA with effects on climate and air quality.