Changing climatic controls on the greenhouse gas balance of thermokarst bogs during succession after permafrost thaw.

Permafrost thaw in northern peatlands causes collapse of permafrost peat plateaus and thermokarst bog development, with potential impacts on atmospheric greenhouse gas exchange. Here, we measured methane and carbon dioxide fluxes over 3 years (including winters) using static chambers along two permafrost thaw transects in northwestern Canada, spanning young (~30 years since thaw), intermediate and mature thermokarst bogs (~200 years since thaw). Young bogs were wetter, warmer and had more hydrophilic vegetation than mature bogs. Methane emissions increased with wetness and soil temperature (40 cm depth) and modelled annual estimates were greatest in the young bog during the warmest year and lowest in the mature bog during the coolest year (21 and 7 g C-CH4 m-2 year-1, respectively). The dominant control on net ecosystem exchange (NEE) in the mature bog (between +20 and -54 g C-CO2 m-2 year-1) was soil temperature (5 cm), causing net CO2 loss due to higher ecosystem respiration (ER) in warmer years. In contrast, wetness controlled NEE in the young and intermediate bogs (between +55 and -95 g C-CO2 m-2 year-1), where years with periodic inundation at the beginning of the growing season caused greater reduction in gross primary productivity than in ER leading to CO2 loss. Winter fluxes (November-April) represented 16% of annual ER and 38% of annual CH4 emissions. Our study found NEE of thermokarst bogs to be close to neutral and rules out large CO2 losses under current conditions. However, high CH4 emissions after thaw caused a positive net radiative forcing effect. While wet conditions favouring high CH4 emissions only persist for the initial young bog period, we showed that continued climate warming with increased ER, and thus, CO2 losses from the mature bog can cause net positive radiative forcing which would last for centuries after permafrost thaw.

Towards climate neutrality in the Spanish N-fertilizer sector: A study based on radiative forcing.

Agricultural systems in the 21st Century face the double challenge of achieving climate neutrality while maintaining food security. Synthetic fertilizers rich in nitrogen (N-fertilizers) boost agricultural production at the expense of increasing climate impact. Public policies, such as the Farm-to-Fork (F2F) Strategy, aim to reduce the extensive use of N-fertilizers with the ultimate goal of achieving a climate neutral European Union (EU). However, the strong link between N-fertilizers and GHG emissions (i.e., CO2, CH4 and, especially, N2O) highlights the need to better understand the climate impact of this sector. The present study conducts a climate impact analysis of Spanish N-fertilizer sector for two periods: (i) from 1960 to 2020 using real data and (ii) from 2021 to 2100 considering five forecasted scenarios. The scenarios range from business-as-usual practices to a full accomplishment of the goals pursued by the EU's F2F strategy. The system's climate stability and neutrality are analysed for the different scenarios based on radiative forcing (RF) metrics. Additionally, the study evaluates the short-term impact of the EU decarbonization goals on the climate impact of the Spanish N-fertilizer sector. The results of the study illustrate that the long-lasting climate impact of N2O and CO2 emissions compromise the capacity of N-fertilizer sector to achieve climate stability and approach climate neutrality. However, the decarbonisation of transport and N-fertilizer production activities is an important driver to substantially reduce the life cycle CH4 and CO2 emissions in the Spanish N-fertilizer sector. The results also highlight that more severe reductions on N-cycles than those suggested by the EU's F2F are required, especially to reduce the long-lasting N2O emissions in the N-fertilizer sector. Overall, the study concludes that using RF-based metrics increases robustness and transparency of climate assessments, which is necessary for a higher integration of climate science within public policymaking.

Assessment of Black Carbon, optical properties and aerosol radiative forcing at Pranmati basin Himalayan critical zone observatory.

The study aimed to understand the optical properties of Black Carbon (BC) and radiative forcing over a data deficient Himalayan region focusing on critical zone observatory employing ground-based measurements by Aethalometer for BC and satellite retrieval techniques for optical properties during mid-May-June 2022 and January-May 2023. BC mass concentration ranged from 0.18 to 4.43 µgm-3, exhibit a mean of 1.47 ± 0.83 µgm-3 with higher summer concentration (1.51 ± 0.94 µgm-3) than winter (1.39 ± 0.61 µgm-3). The average Absorption Ångström Exponent observed to be significantly higher than unity (1.77 ± 0.31) over the studied high-altitude Himalayan region, suggesting the dominance of biomass-burning aerosol. Higher aethalometer derived compensation parameter (K) in winter suggesting locally originated BC while, lower K value in summer suggesting aged BC transported from Indo-Gangetic Plains. Optical properties calculated from "Optical Properties of Aerosol and Cloud" (OPAC) model are used in the "Santa Barbara DISORT Atmospheric Radiative Transfer" (SBDART) model to calculate the aerosol Direct Radiative Force (DRF). The entire studied period is characterized by the predominance of absorbing aerosols, particularly BC, increasing Aerosol Optical Depth, Asymmetric Parameters and decreasing Single Scattering Albedo, leading to a considerable increase in atmospheric radiative forcing (+0.9 Wm-2, top of atmosphere) and Heating Rate (0.36 KDay-1). The mean radiative forcing within atmosphere during summer was higher (+14.29 Wm-2) relative to the winter (+12.00 Wm-2), emphasizing the impact of absorbing aerosols on regional warming and potential glacier melting in the Himalayas at a faster rate. Urgent policy consideration for the reduction of absorbing aerosols is highlighted, recognizing the critical roles of Black Carbon in the changing behaviour of Critical Zone observatory. The study's data serve as a valuable resource to understanding and addressing uncertainties in climate models, aiding effective policy implementation for Black Carbon reduction.

Field evidence of brown carbon absorption enhancement linked to organic nitrogen formation in Indo-Gangetic Plain.

Atmospheric brown carbon (BrC), a short-lived climate forcer, absorbs solar radiation and is a substantial contributor to the warming of the Earth's atmosphere. BrC composition, its absorption properties, and their evolution are poorly represented in climate models, especially during atmospheric aqueous events such as fog and clouds. These aqueous events, especially fog, are quite prevalent during wintertime in Indo-Gangetic Plain (IGP) and involve several stages (e.g., activation, formation, and dissipation, etc.), resulting in a large variation of relative humidity (RH) in the atmosphere. The huge RH variability allowed us to examine the evolution of water-soluble brown carbon (WS-BrC) diurnally and as a function of aerosol liquid water content (ALWC) and RH in this study. We explored links between the evolution of WS-BrC mass absorption efficiency at 365 nm (MAEWS-BrC-365) and chemical characteristics, viz., low-volatility organics and water-soluble organic nitrogen (WSON) to water-soluble organic carbon (WSOC) ratio (org-N/C), in the field (at Kanpur in central IGP) for the first time worldwide. We observed that WSON formation governed enhancement in MAEWS-BrC-365 diurnally (except during the afternoon) in the IGP. During the afternoon, the WS-BrC photochemical bleaching dwarfed the absorption enhancement caused by WSON formation. Further, both MAEWS-BrC-365 and org-N/C ratio increased with a decrease in ALWC and RH in this study, signifying that evaporation of fog droplets or bulk aerosol particles accelerated the formation of nitrogen-containing organic chromophores, resulting in the enhancement of WS-BrC absorptivity. The direct radiative forcing of WS-BrC relative to that of elemental carbon (EC) was ∼19 % during wintertime in Kanpur, and âˆ¼ 40 % of this contribution was in the UV-region. These findings highlight the importance of further examining the links between the evolution of BrC absorption behavior and chemical composition in the field and incorporating it in the BrC framework of climate models to constrain the predictions.

Synergies and trade-offs between provisioning and climate-regulating ecosystem services in reindeer herding ecosystems.

Reindeer (Rangifer tarandus) pastoralism utilizes vast boreo-arctic taiga and tundra as grazing land. Highly fluctuating population sizes pose major challenges to the economy and livelihood of indigenous herder communities. In this study we investigated the effect of population fluctuations on core provisioning and regulating ecosystem services in two Sámi reindeer herding districts with contrasting fluctuation trends. We compared 50-year long time series on herd size, meat production, forage productivity, carbon footprint, and CO2-equivalence metrics for surface albedo change based on the radiative forcing concept. Our results show, for both districts, that the economic benefits from the provisioning services were higher than the costs from the regulating services. Still, there were major contrasts; the district with moderate and stable reindeer density gained nearly the double on provisioning services per unit area. The costs from increasing heat absorption due to reduction in surface albedo caused by replacement of high-reflective lichens with low-reflective woody plants, was 10.5 times higher per unit area in the district with large fluctuations. Overall, the net economic benefits per unit area were 237 % higher in the district with stable reindeer density. These results demonstrate that it is possible to minimize trade-offs between economic benefits from reindeer herding locally and global economic costs in terms of climate-regulating services by minimizing fluctuations in herds that are managed at sustainable densities.

Aerosol radiative forcing of forest fires unprecedented in South Korea (2022) captured by Korean geostationary satellites, GK-2A AMI and GK-2B GEMS.

The worst forest fires in Korean history broke out on March 4, 2022 and lasted for ten days. In order to monitor the catastrophic forest fires, Geostationary Korea Multi-Purpose Satellite (GK)-2 A Advanced Meteorological Imager (AMI) and GK-2B Geostationary Environment Monitoring Spectrometer (GEMS) data were used in this study. Aerosol optical depth (AOD) irretrievable for the biomass-burning aerosols produced with water vapor classified as could-contaminated, was reconstructed by ultraviolet aerosol index (UVAI). Afterward, aerosol radiative forcing (ARF) at TOA was finally estimated by the correlation of AOD and surface albedo with ARF. Most of the aerosols drifted toward the East Sea by the prevailing westerly winds, and caused a cooling effect on the atmosphere with a maximum daily average radiative forcing of -69.28 Wm-2. Furthermore, the fire-prone conditions for the unprecedented forest fires were discussed in detail as following aspects; 1) the most severe drought caused by a "triple-dip" La Niña; 2) pressure patterns and topographical features that generate strong winds; 3) coniferous forests prone to fires; and 4) increased human activity following the nationwide COVID-19 vaccination. This study demonstrated that the rapid and effective ARF estimation based on the satellite remote sensing can contribute to a better understanding of ARF in the Earth's radiation budget for the global forest fires that will be more frequent, intense, and longer-lasting due to the human-caused climate and environment changes.

Freshwater wetland restoration and conservation are long-term natural climate solutions.

Freshwater wetlands have a disproportionately large influence on the global carbon cycle, with the potential to serve as long-term carbon sinks. Many of the world's freshwater wetlands have been destroyed or degraded, thereby affecting carbon-sink capacity. Ecological restoration of degraded wetlands is thus becoming an increasingly sought-after natural climate solution. Yet the time required to revert a degraded wetland from a carbon source to sink remains largely unknown. Moreover, increased methane (CH4) and nitrous oxide (N2O) emissions might complicate the climate benefit that wetland restoration may represent. We conducted a global meta-analysis to evaluate the benefits of wetland restoration in terms of net ecosystem carbon and greenhouse gas balance. Most studies (76 %) investigated the benefits of wetland restoration in peatlands (bogs, fens, and peat swamps) in the northern hemisphere, whereas the effects of restoration in non-peat wetlands (freshwater marshes, non-peat swamps, and riparian wetlands) remain largely unexplored. Despite higher CH4 emissions, most restored (77 %) and all natural peatlands were net carbon sinks, whereas most degraded peatlands (69 %) were carbon sources. Conversely, CH4 emissions from non-peat wetlands were similar across degraded, restored, and natural non-peat wetlands. When considering the radiative forcings and atmospheric lifetimes of the different greenhouse gases, the average time for restored wetlands to have a net cooling effect on the climate after restoration is 525 years for peatlands and 141 years for non-peat wetlands. The radiative benefit of wetland restoration does, therefore, not meet the timeframe set by the Paris Agreement to limit global warming by 2100. The conservation and protection of natural freshwater wetlands should be prioritised over wetland restoration as those ecosystems already play a key role in climate change mitigation.

Spectrally refined unbiased Monte Carlo estimate of the Earth's global radiative cooling.

The Earth's radiative cooling is a key driver of climate. Determining how it is affected by greenhouse gas concentration is a core question in climate-change sciences. Due to the complexity of radiative transfer processes, current practices to estimate this cooling require the development and use of a suite of radiative transfer models whose accuracy diminishes as we move from local, instantaneous estimates to global estimates over the whole globe and over long periods of time (decades). Here, we show that recent advances in nonlinear Monte Carlo methods allow a paradigm shift: a completely unbiased estimate of the Earth's infrared cooling to space can be produced using a single model, integrating the most refined spectroscopic models of molecular gas energy transitions over a global scale and over years, all at a very low computational cost (a few seconds).

Inverse effects of aerosol radiative forcing on heavy PM2.5 pollution of local accumulation and regional transport over Central China.

Regional transport of air pollutants is a crucial factor influencing atmospheric environment, and aerosol radiative forcing (ARF) feedback to atmospheric boundary layer (ABL) structure and ambient air pollution is yet to be comprehensively understood over the receptor region of regional transport. By simulating meteorology and air pollutants during a heavy PM2.5 pollution event with WRF-Chem model, we quantitatively investigated the ARF and ABL interaction for PM2.5 pollution over the Twain-Hu Basin (THB), a key receptor region of regional transport over central China. Driven by northerly winds, PM2.5 was transported from upstream north China to downstream THB accompanied by high PM2.5 levels in the free troposphere. The ARF exacerbated local PM2.5 accumulation by up to 20 µg m-3 and inhibited the impact of regional transport on PM2.5 levels in the ABL with reducing near-surface PM2.5 concentrations of 5 µg m-3 over the THB. The ARF-intensified air temperature inversion at the top of ABL was unfavorable for the transported air pollutants crossing the ABL top to the near-surface layer, thus weakening the impact of regional PM2.5 transport on air quality in the receptor region. Meanwhile, the ARF of transported PM2.5 induced updrafts in the free troposphere, promoting vertical mixing of air pollutants with positive feedback on increasing secondary PM2.5 concentrations in the free troposphere. The ARF induced more and less secondary PM2.5 formations respectively in the free troposphere and the near-surface layer during the regional transport period of air pollution. These results enhance our comprehension of aerosol-meteorology feedback in regional changes of atmospheric environment with inverse effects of ARF on PM2.5 pollution of local accumulation and regional transport.

Sources, variability, long-term trends, and radiative forcing of aerosols in the Arctic: implications for Arctic amplification.

Atmospheric pollution in the Arctic has been an important driver for the ongoing climate change there. Increase in the Arctic aerosols causes the phenomena of Arctic haze and Arctic amplification. Our analysis of aerosol optical depth (AOD), black carbon (BC), and dust using ground-based, satellite, and reanalysis data in the Arctic for the period 2003-2019 shows that the lowest amount of all these is found in Greenland and Central Arctic. There is high AOD, BC, and dust in the northern Eurasia and parts of North America. All aerosols show their highest values in spring. Significant positive trends in AOD (> 0.003 year-1) and BC (0.0002-0.0003 year-1) are found in the northwestern America and northern Asia. Significant negative trends are observed for dust (- 0.0001 year-1) around Central Arctic. Seasonal analysis of AOD, BC, and dust reveals an increasing trend in summer and decreasing trend in spring in the Arctic. The major sources of aerosols are the nearby Europe, Russia, and North America regions, as assessed using the potential source contribution function (PSCF). Anthropogenic emissions from the transport, energy, and household sectors along with natural sources such as wildfires contribute to the positive trends of aerosols in the Arctic. These increasing aerosols in the Arctic influence Arctic amplification through radiative effects. Here, we find that the net aerosol radiative forcing is high in Central Arctic, Greenland, Siberia, and Canadian Arctic, about 2-4 W/m2, which can influence the regional temperature. Therefore, our study can assist policy decisions for the mitigation of Arctic haze and Arctic amplification in this environmental fragile region of the Earth.

Amplified drying in South Asian summer monsoon precipitation due to anthropogenic sulfate aerosols.

A declining trend in Indian summer monsoon precipitation (ISMP) in the latter half of the 20th century is a scientifically challenging and societally relevant research issue. Heavy aerosol loading over India is one of the key factors in modulating the ISMP. Using the state-of-the-state-of-the-art chemistry-climate model, ECHAM6-HAMMOZ, the impacts of South Asian anthropogenic sulfate aerosols on the Indian summer monsoon precipitation were investigated against: (1) 2010 La Niña (excess monsoon), (2) 2015 El Niño (deficit monsoon) in comparison to (3) normal monsoon 2016. Sensitivity simulations were designed with 48% enhancement in South Asian SO2 emissions based on a trend estimated from Ozone Monitoring Instrument (OMI) satellite observations during 2006-2017. The model simulations showed that sulfate aerosols reduce ISMP by 27.5%-43.3 %, while simulations without sulfate loading enhanced ISMP by 23% in 2010 La Niña and reduction by 35% in 2015 El Niño. This paper reports that sulfate aerosols loading over India reduce precipitation by aerosol-induced direct and indirect effects by inducing atmospheric cooling, weakening in the convection, and reduction in moisture transport to Indian landmass. This paper emphasizes the necessity of alternate use of energy to reduce sulfate aerosol emissions to solve water issues in South Asia.

Dual carbon isotope-based brown carbon aerosol characteristics at a high-altitude site in the northeastern Himalayas: Role of biomass burning.

PM2.5 samples (n = 34) were collected from January to April 2017 over Shillong (25.7°N, 91.9°E; 1064 m amsl), a high-altitude site situated in the northeastern Himalaya. The main aim was to understand the sources, characteristics, and optical properties of local vs long-range transported carbonaceous aerosols (CA) using chemical species and dual carbon isotopes (13C and 14C). Percentage biomass burning (BB)/biogenic fraction (fbio, calculated from 14C) varied from 67 to 92 % (78 ± 7) and correlated well with primary BB tracers like f60, and K+, suggesting BB as a considerable source. Rain events are shown to reduce the fbio fraction, indicating majority of BB-derived CA are transported. Further, δ13C (-26.6 ± 0.4) variability was very low over Shillong, suggesting it's limitations in source apportionment over the study region, if used alone. Average ratio of absorption coefficient of methanol-soluble BrC (BrCMS) to water-soluble BrC (BrCWS) at 365 nm was 1.8, indicating a significant part of BrC was water-insoluble. A good positive correlation between fbio and mass absorption efficiency of BrCWS and BrCMS at 365 nm with the higher slope for BrCMS suggests BB derived water-insoluble BrC was more absorbing. Relative radiative forcing (RRF, 300 to 2500 nm) of BrCWS and BrCMS with respect to EC were 11 ± 5 % and 23 ± 16 %, respectively. Further, the RRF of BrCMS was up to 60 %, and that of BrCWS was up to 22 % with respect to EC for the samples with fbio ≥ 0.85 (i.e., dominated by BB), reflecting the importance of BB in BrC RRF estimation.

Photovoltaic fields largely outperform afforestation efficiency in global climate change mitigation strategies.

Suppression of carbon emissions through photovoltaic (PV) energy and carbon sequestration through afforestation provides complementary climate change mitigation (CCM) strategies. However, a quantification of the "break-even time" (BET) required to offset the warming impacts of the reduced surface reflectivity of incoming solar radiation (albedo effect) is needed, though seldom accounted for in CCM strategies. Here, we quantify the CCM potential of PV fields and afforestation, considering atmospheric carbon reductions, solar panel life cycle analysis (LCA), surface energy balance, and land area required across different climatic zones, with a focus on drylands, which offer the main remaining land area reserves for forestation aiming climate change mitigation (Rohatyn S, Yakir D, Rotenberg E, Carmel Y. Limited climate change mitigation potential through forestation of the vast dryland regions. 2022. Science 377:1436-1439). Results indicate a BET of PV fields of ∼2.5 years but >50× longer for dryland afforestation, even though the latter is more efficient at surface heat dissipation and local surface cooling. Furthermore, PV is ∼100× more efficient in atmospheric carbon mitigation. While the relative efficiency of afforestation compared with PV fields significantly increases in more mesic climates, PV field BET is still ∼20× faster than in afforestation, and land area required greatly exceeds availability for tree planting in a sufficient scale. Although this analysis focusing purely on the climatic radiative forcing perspective quantified an unambiguous advantage for the PV strategy over afforestation, both approaches must be combined and complementary, depending on climate zone, since forests provide crucial ecosystem, climate regulation, and even social services.

Optical Properties of Individual Tar Balls in the Free Troposphere.

Tar balls are brown carbonaceous particles that are highly viscous, spherical, amorphous, and light absorbing. They are believed to form in biomass burning smoke plumes during transport in the troposphere. Tar balls are also believed to have a significant impact on the Earth's radiative balance, but due to poorly characterized optical properties, this impact is highly uncertain. Here, we used two nighttime samples to investigate the chemical composition and optical properties of individual tar balls transported in the free troposphere to the Climate Observatory "Ottavio Vittori" on Mt. Cimone, Italy, using multimodal microspectroscopy. In our two samples, tar balls contributed 50% of carbonaceous particles by number. Of those tar balls, 16% were inhomogeneously mixed with other constituents. Using electron energy loss spectroscopy, we retrieved the complex refractive index (RI) for a wavelength range from 200 to 1200 nm for both inhomogeneously and homogeneously mixed tar balls. We found no significant difference in the average RI of inhomogeneously and homogeneously mixed tar balls (1.40-0.03i and 1.36-0.03i at 550 nm, respectively). Furthermore, we estimated the top of the atmosphere radiative forcing using the Santa Barbara DISORT Atmospheric Radiative Transfer model and found that a layer of only tar balls with an optical depth of 0.1 above vegetation would exert a positive radiative forcing ranging from 2.8 W m-2 (on a clear sky day) to 9.5 W m-2 (when clouds are below the aerosol layer). Understanding the optical properties of tar balls can help reduce uncertainties associated with the contribution of biomass-burning aerosol in current climate models.

A gradual increase of aerosol pollution in the Third Pole during the past four decades: Implication for regional climate change.

We analyse the long-term (1980-2020) changes in aerosols over the Third Pole (TP) and assess the changes in radiative forcing (RF) using satellite, ground-based and reanalysis data. The annual mean aerosol optical depth (AOD) varies from 0.06 to 0.24, with the highest values of around 0.2 in the north and southwest TP, which are dominated by dust from Taklimakan and Thar deserts, respectively. However, Organic Carbon (OC), Black Carbon (BC) and sulphate aerosols have significant contributions to the total AOD in the south and east TP. High amounts of dust are observed in spring and summer, but BC in winter. Trajectory analysis reveals that the air mass originated from East and South Asia carries BC and OC, whereas the air from South Asia, Central Asia and Middle East brings dust to TP. Significant positive trends in AOD is found in TP, with high values of about 0.002/yr in the eastern and southern TP. There is a gradual increase in BC and OC concentrations during 1980-2020, but the change from 2000 is phenomenal. The RF at the top of the atmosphere varies from -10 to 2 W/m2 in TP, and high positive RF of about 2 W/m2 is estimated in Pamir, Karakoram and Nyainquentanglha mountains, where the massive glacier mass exists. The RF has increased in much of TP during recent decades (2001-2020) with respect to previous decades (1981-2000), which can be due to the rise in BC and dust during the latter period. Therefore, the positive trend in BC and its associated change in RF can amplify the regional warming, and thus, the melting of glaciers or ice in TP. This is a great concern as it is directly connected to the water security of many South Asian countries.

Impacts of haze and nitrogen oxide alleviation on summertime ozone formation: A modeling study over the Yangtze River Delta, China.

The strict emission control measures have profoundly changed the air pollution in the Yangtze River Delta (YRD) region, China. However, the impacts of decreasing fine particulates (PM2.5) and nitrogen oxide (NOx) on summer ozone (O3) formation still remain disputable. We perform simulations in the 2018 summer over the YRD using the WRF-Chem model that considers the aerosol radiative forcing (ARF) and HO2 heterogeneous loss on aerosol surface. The model reasonably reproduces the measured spatiotemporal surface O3 and PM2.5 concentrations and aerosol compositions. Model sensitivity experiments show that the NOx mitigation during recent years changes daytime O3 formation in summer from the transition regime to the NOx-sensitive regime in the YRD. The decreasing NOx emission generally weakens O3 formation and lowers ambient O3 levels in summer during recent years, except for some urban centers of megacities. While, the haze alleviation characterized by a decline in ambient PM2.5 concentration in the past years largely counteracts the daytime O3 decrease caused by NOx mitigation, largely contributing to the persistently high levels of summertime O3. The counteracting effect is dominantly attributed to the attenuated ARF and minorly contributed by the suppressed HO2 uptake and heterogeneous loss on aerosol surface. These results highlight that the repeated O3 pollution in the YRD is closely associated with NOx and haze alleviation and more efforts must be taken to achieve lower O3 levels.

Sulfur hexafluoride in the marine atmosphere and surface seawater of the Western Pacific and Eastern Indian Ocean.

Sulfur hexafluoride (SF6) is a powerful greenhouse gas with a high global warming potential. While SF6 emissions from urban areas have been extensively studied, our knowledge about SF6 concentrations in the oceanic atmosphere and its air-sea exchange remains limited. Herein, the concentrations of SF6 in the atmosphere and surface seawater of the WPO (Western Pacific Ocean) and EIO (Eastern Indian Ocean) were comprehensively characterized from 2019 to 2022 in the first long-term study. The mean mixing ratios of SF6 over the WPO and EIO during 2019-2020 (2021-2022) were 10.9 (11.2) and 10.9 (11.1) ppt, respectively. The atmospheric SF6 concentration over the WPO and EIO increased at rates of 0.40 ± 0.06 and 0.58 ± 0.28 ppt yr-1, respectively, surpassing previously reported annual growth rates. The faster growth was primarily attributed to the influence of polluted air masses originating from eastern Asian countries, particularly Japan, Northeast China, and India. This might explain why the radiative forcing caused by SF6 in the study region was higher than the global average. The concentrations of SF6 in the surface seawater of the WPO and EIO ranged from 0.33 to 2.54 fmol kg-1, and the distribution was affected by atmospheric concentrations and ocean currents. Estimated air-sea fluxes revealed that the ocean acted as a significant sink of atmospheric SF6, and the preliminary estimation suggested oceanic uptake accounts for about 7% of annual global SF6 emissions. Based on these findings, we tentatively suggest that the strength of the ocean as a sink of SF6 may warrant reassessment. The global oceanic uptake of SF6 has the potential to reduce its global abundance and environmental impacts.

Optical source apportionment of aqueous brown carbon (BrC) on a daytime and nighttime basis in the eastern Indo-Gangetic Plain (IGP) and insights from 13C and 15N isotopic signatures.

This study reports day-night and seasonal variations of aqueous brown carbon (BrCaq) and constituent humic-like substances (HULIS) (neutral and acidic HULIS: HULIS-n and HULIS-a) from the eastern Indo-Gangetic Plain (IGP) of India during 2019-2020. This is followed by the application of the receptor model positive matrix factorization (PMF) for optical source apportionment of BrCaq and the use of stable isotopic ratios (δ13C and δ15N) to understand atmospheric processing. Nighttime BrCaq absorption and mass absorption efficiencies (MAE) were enhanced by 40-150 % and 50-190 %, respectively, compared to the daytime across seasons, possibly as a combined effect from daytime photobleaching, dark-phase secondary formation, and increased nighttime emissions. MAE250 nm/MAE365 nm (i.e., E2/E3) ratios and Angstrom Exponents revealed that BrCaq and HULIS-n were relatively more aromatic and conjugated during the biomass burning-dominated periods while BrCaq and HULIS-a were comprised mostly of non-conjugated aliphatic structures from secondary processes during the photochemistry-dominated summer. The relative radiative forcing of BrCaq with respect to elemental carbon (EC) was 10-12 % in the post-monsoon and winter in the 300-400 nm range. Optical source apportionment using PMF revealed that BrCaq absorption at 300, 365 and 420 nm wavelengths in the eastern IGP is mostly from biomass burning (60-75 %), followed by combined marine and fossil fuel-derived sources (24-31 %), and secondary processes (up to 10 %). Source-specific MAEs at 365 nm were estimated to be the highest for the combined marine and fossil fuel source (1.34 m2 g-1) followed by biomass burning (0.78 m2 g-1) and secondary processing (0.13 m2 g-1). Finally, δ13C and δ15N isotopic analysis confirmed the importance of summertime photochemistry and wintertime NO3--dominated chemistry in constraining BrC characteristics. Overall, the quantitative apportionment of BrCaq sources and processing reported here can be expected to lead to targeted source-specific measurements and a better understanding of BrC climate forcing in the future.

Response of Arctic Black Carbon Contamination and Climate Forcing to Global Supply Chain Relocation.

Black carbon (BC) plays a vital role in Arctic warming. Extensive investigations have been conducted to elucidate the source-receptor relationships of BC between the Arctic and mid-/high-latitude sources. However, it is unclear to what extent source relocation under globalization could disturb Arctic BC contamination and climate forcing from anthropogenic BC emissions. Here, we show that the global supply chain (GSC) relocation featured by the southward shift of industries from high-latitude developed countries to low-latitude developing countries markedly reduces the BC burden in the Arctic using a global chemical transport model (GEOS-Chem) and a multiregional input-output analysis (MRIO). We find that Arctic annual mean BC concentration associated with the GSC relocation drops by ∼15% from the case without the GSC relocation. The total net BC level declines 7% over the entire Arctic and 16% in the European Arctic. We also observed markedly declining BC deposition as well as direct and snow albedo radiative forcing in the Arctic. We show that the Arctic BC burden would be further reduced by decreasing BC emissions in China, attributable to its emission reduction and ongoing shift of the GSC from China to southern and southeastern Asia.

Evaluation and uncertainty analysis of Himawari-8 hourly aerosol product version 3.1 and its influence on surface solar radiation before and during the COVID-19 outbreak.

The hourly Himawari-8 version 3.1 (V31) aerosol product has been released and incorporates an updated Level 2 algorithm that uses forecast data as an a priori estimate. However, there has not been a thorough evaluation of V31 data across a full-disk scan, and V31 has yet to be applied in the analysis of its influence on surface solar radiation (SSR). This study firstly investigates the accuracy of V31 aerosol products, which includes three categories of aerosol optical depth (AOD) (AODMean, AODPure, and AODMerged) as well as the corresponding Ångström exponent (AE), using ground-based measurements from the AERONET and SKYNET. Results indicate that V31 AOD products are more consistent with ground-based measurements compared to previous products (V30). The highest correlation and lowest error were seen in the AODMerged, with a correlation coefficient of 0.8335 and minimal root mean square error of 0.1919. In contrast, the AEMerged shows a larger discrepancy with measurements unlike the AEMean and AEPure. Error analysis reveals that V31 AODMerged has generally stable accuracy across various ground types and geometrical observation angles, however, there are higher uncertainties in areas with high aerosol loading, particularly for fine aerosols. The temporal analysis shows that V31 AODMerged performs better compared to V30, particularly in the afternoon. Finally, the impacts of aerosols on SSR based on the V31 AODMerged are investigated through the development of a sophisticated SSR estimation algorithm in the clear sky. Results demonstrate that the estimated SSR is significant consistency with those of well-known CERES products, with preservation of 20 times higher spatial resolution. The spatial analysis reveals a significant reduction of AOD in the North China Plain before and during the COVID-19 outbreak, resulting in an average 24.57 W m-2 variation of the surface shortwave radiative forcing in clear sky daytime.