scholarly journals Measurement report: The importance of biomass burning in light extinction and direct radiative effect of urban aerosol during the COVID-19 lockdown in China

2021 ◽  
Author(s):  
Jie Tian ◽  
Qiyuan Wang ◽  
Huikun Liu ◽  
Yongyong Ma ◽  
Suixin Liu ◽  
...  

Abstract. To mitigate climate change in China, a better understanding of optical properties of aerosol is required due to the complexity in emission sources. Here, an intensive real-time measurement was conducted in an urban area of China before and during the lockdown of Coronavirus Disease 2019 (COVID-19), to explore the impacts of anthropogenic activities on aerosol light extinction and direct radiative effect (DRE). The mean light extinction coefficient (bext) reduced from 774.7 ± 298.1 Mm−1 during the normal period to 544.3 ± 179.4 Mm−1 during the lockdown period. The generalized addictive model analysis indicated that the large decline of bext (29.7 %) was entirely attributed to the sharp reductions in anthropogenic emissions. Chemical calculation of bext based on the ridge regression analysis showed that organic aerosol (OA) was the largest contributor to bext in both periods (45.1–61.4 %), and contributions of two oxygenated OAs to bext increased by 3.0–14.6 % during the lockdown. A hybrid environmental receptor model combining with chemical and optical variables identified six sources of bext. It was found that bext from traffic-related emission, coal combustion, fugitive dust, nitrate plus secondary OA (SOA) source, and sulfate plus SOA source decreased by 21.4–97.9 % in the lockdown, whereas bext from biomass burning increased by 27.1 % mainly driven by undiminished needs of residential cooking and heating. The atmospheric radiative transfer model was further used to illustrate that biomass burning instead of traffic-related emission became the largest positive effect (10.0 ± 10.9 W m−2) on aerosol DRE in the atmosphere during the lockdown. Our study provides insights into aerosol bext and DRE from anthropogenic sources, and the results implied the importance of biomass burning for tackling climate change in China in the future.

2017 ◽  
Author(s):  
Xuan Wang ◽  
Colette L. Heald ◽  
Jiumeng Liu ◽  
Rodney J. Weber ◽  
Pedro Campuzano-Jost ◽  
...  

Abstract. Organic aerosols (OA) that strongly absorbs solar radiation in the near-UV are referred to as brown carbon (BrC). However the sources, evolution, and optical properties of BrC remain highly uncertain, and contribute significantly to uncertainty in the estimate of the global direct radiative effect (DRE) of aerosols. Previous modeling studies of BrC optical properties and DRE have been unable to fully evaluate model performance due to the lack of direct measurements of BrC absorption. In this study, we develop a global model simulation (GEOS-Chem) of BrC and test it against BrC absorption measurements from two aircraft campaigns in the continental U.S. (SEAC4RS and DC3). To our knowledge, this is the first study to compare simulated BrC absorption with direct ambient measurements. We show that the BrC absorption properties from biomass burning estimated based on previous laboratory measurements overestimate the aircraft measurements of ambient BrC absorption. In addition, applying a photochemical scheme to simulate bleaching/degradation of BrC improves model skill. The airborne observations are consistent with a mass absorption coefficient (MAC) of freshly emitted biomass burning OA of 0.57 m2 g−1 at 365 nm with an absorption Ångström exponents (AAE) = 3.1 for 300 & 600 wavelengths pair, coupled with a 1 day whitening e-folding time. Using the GEOS-Chem chemical transport model integrated with the RRTMG radiative transfer model, we estimate that the top-of-atmosphere all-sky direct radiative effect (DRE) of OA is −0.350 Wm−2, 10 % higher than that without consideration of BrC absorption. Therefore, our best estimate of the absorption DRE of BrC is +0.042 Wm−2. We suggest that the DRE of BrC has been overestimated previously due to the lack of observational constraints from direct measurements and omission of the effects of photochemical whitening.


2021 ◽  
Author(s):  
Filippo Calì Quaglia ◽  
Daniela Meloni ◽  
Alcide Giorgio di Sarra ◽  
Tatiana Di Iorio ◽  
Virginia Ciardini ◽  
...  

<p>Extended and intense wildfires occurred in Northern Canada and, unexpectedly, on the Greenlandic West coast during summer 2017. The thick smoke plume emitted into the atmosphere was transported to the high Arctic, producing one of the largest impacts ever observed in the region. Evidence of Canadian and Greenlandic wildfires was recorded at the Thule High Arctic Atmospheric Observatory (THAAO, 76.5°N, 68.8°W, www.thuleatmos-it.it) by a suite of instruments managed by ENEA, INGV, Univ. of Florence, and NCAR. Ground-based observations of the radiation budget have allowed quantification of the surface radiative forcing at THAAO. </p><p>Excess biomass burning chemical tracers such as CO, HCN, H2CO, C2H6, and NH3 were  measured in the air column above Thule starting from August 19 until August 23. The aerosol optical depth (AOD) reached a peak value of about 0.9 on August 21, while an enhancement of wildfire compounds was  detected in PM10. The measured shortwave radiative forcing was -36.7 W/m2 at 78° solar zenith angle (SZA) for AOD=0.626.</p><p>MODTRAN6.0 radiative transfer model (Berk et al., 2014) was used to estimate the aerosol radiative effect and the heating rate profiles at 78° SZA. Measured temperature profiles, integrated water vapour, surface albedo, spectral AOD and aerosol extinction profiles from CALIOP onboard CALIPSO were used as model input. The peak  aerosol heating rate (+0.5 K/day) was  reached within the aerosol layer between 8 and 12 km, while the maximum radiative effect (-45.4 W/m2) is found at 3 km, below the largest aerosol layer.</p><p>The regional impact of the event that occurred on August 21 was investigated using a combination of atmospheric radiative transfer modelling with measurements of AOD and ground surface albedo from MODIS. The aerosol properties used in the radiative transfer model were constrained by in situ measurements from THAAO. Albedo data over the ocean have been obtained from Jin et al. (2004). Backward trajectories produced through HYSPLIT simulations (Stein et al., 2015) were also employed to trace biomass burning plumes.</p><p>The radiative forcing efficiency (RFE) over land and ocean was derived, finding values spanning from -3 W/m2 to -132 W/m2, depending on surface albedo and solar zenith angle. The fire plume covered a vast portion of the Arctic, with large values of the daily shortwave RF (< -50 W/m2) lasting for a few days. This large amount of aerosol is expected to influence cloud properties in the Arctic, producing significant indirect radiative effects.</p>


2021 ◽  
Author(s):  
Elisa Bergas-Massó ◽  
María Gonçalves Ageitos ◽  
Stelios Myriokefalitakis ◽  
Twan van Noije ◽  
Ron Miller ◽  
...  

<p>Atmospheric deposition of soluble iron (Fe) to the ocean has an impact on oceanic primary productivity, thus on carbon dioxide uptake. Understanding how anthropogenic activity influences the atmospheric Fe cycle is key to project ocean biogeochemical cycles and has been barely explored.</p><p>In this study, we assess past, present, and future soluble Fe deposition to the ocean, accounting for natural and anthropogenic sources, using an advanced atmospheric Fe cycle module implemented into the EC-Earth3 Earth System Model. This version of the model considers primary emissions of insoluble and soluble Fe forms associated with dust minerals, and anthropogenic and biomass burning combustion aerosols. Fe solubilization processes in the atmosphere include 1)  proton-promoted, 2)  oxalate-promoted (with oxalate calculated on-line), and 3) photo-reductive Fe dissolution. We run time-slice simulations using the atmosphere-chemistry model configuration constrained by past, present, and future ocean states. The necessary sea surface temperature and sea ice concentration climatologies are obtained from EC-Earth3 CMIP6 coupled model experiments. Future projections rely on three CMIP6 scenarios representing different socio-economic pathways and end-of-the-century forcing levels: SSP1-2.6, SSP2-4.5, and SSP3-7.0. </p><p>Our setup allows us to estimate the soluble Fe deposition into the ocean while quantifying the contribution from dust, biomass burning, and anthropogenic combustion sources separately under a range of scenarios. Our preliminary results suggest nearly a 50% increase in soluble Fe deposition for the present time since the industrial revolution, attributed to increased atmospheric acidity and oxalate concentrations that result in a more efficient atmospheric processing. Future projections of soluble Fe show a high correlation between anthropogenic activity and solubility of deposited Fe, scenarios with higher anthropogenic emissions consistently yield a higher fraction of soluble over total deposited Fe. Our results also suggest diverging trends for the different ocean basins. Disentangling the factors that drive those differences in regions where Fe is known to be the limiting nutrient, such as the North Pacific or the Southern Ocean, is fundamental to improve our understanding of the atmospheric Fe cycle and its consequences for  the ocean biogeochemistry.  </p>


2016 ◽  
Author(s):  
C. Di Biagio ◽  
P. Formenti ◽  
L. Doppler ◽  
C. Gaimoz ◽  
N. Grand ◽  
...  

Abstract. Pollution aerosols strongly influence the composition of the Western Mediterranean basin, but at present little is known on their optical properties. We report in this study in situ observations of the single scattering albedo (ω) of pollution aerosol plumes measured over the Western Mediterranean basin during the TRAQA (TRansport and Air QuAlity) airborne campaign in summer 2012. Cases of pollution export from different source regions around the basin and at different altitudes between ~160 and 3500 m above sea level have been sampled during the flights. Data from this study show a large variability of ω, with values between 0.84–0.98 at 370 nm and 0.70–0.99 at 950 nm. The single scattering albedo generally decreases with the wavelength, with some exception associated to the mixing of pollution with sea spray over the sea surface. Lowest values of ω (0.84–0.70 between 370 and 950 nm) are measured in correspondence of a fresh plume possibly linked to ship emissions over the basin. The range of variability of ω observed in this study seems to be independent of the source region around the basin, as well as of the altitude and ageing time of the plumes. The observed variability of ω reflects in a large variability for the complex refractive index of pollution aerosols, which is estimated to span in the large range 1.41–1.75 and 0.002–0.068 for the real and the imaginary parts, respectively, between 370 and 950 nm. Radiative calculations in clear-sky conditions have been performed with the GAME radiative transfer model to test the sensitivity of the aerosol shortwave Direct Radiative Effect (DRE) to the variability of ω as observed in this study. Results from the calculations suggest up to a 50 % and 30 % change of the forcing efficiency (FE), i.e. the DRE per unit of optical depth, at the surface (−160÷−235 Wm−2 τ−1 at 60° solar zenith angle) and at the Top-Of-Atmosphere (−137÷−92 5 Wm−2 τ−1) for ω varying between its maximum and minimum value. This induces a change of up to an order of magnitude (+23÷+143 Wm−2 τ−1) for the radiative effect within the atmosphere.


2014 ◽  
Vol 14 (11) ◽  
pp. 5513-5527 ◽  
Author(s):  
C. L. Heald ◽  
D. A. Ridley ◽  
J. H. Kroll ◽  
S. R. H. Barrett ◽  
K. E. Cady-Pereira ◽  
...  

Abstract. The direct radiative effect (DRE) of aerosols, which is the instantaneous radiative impact of all atmospheric particles on the Earth's energy balance, is sometimes confused with the direct radiative forcing (DRF), which is the change in DRE from pre-industrial to present-day (not including climate feedbacks). In this study we couple a global chemical transport model (GEOS-Chem) with a radiative transfer model (RRTMG) to contrast these concepts. We estimate a global mean all-sky aerosol DRF of −0.36 Wm−2 and a DRE of −1.83 Wm−2 for 2010. Therefore, natural sources of aerosol (here including fire) affect the global energy balance over four times more than do present-day anthropogenic aerosols. If global anthropogenic emissions of aerosols and their precursors continue to decline as projected in recent scenarios due to effective pollution emission controls, the DRF will shrink (−0.22 Wm−2 for 2100). Secondary metrics, like DRE, that quantify temporal changes in both natural and anthropogenic aerosol burdens are therefore needed to quantify the total effect of aerosols on climate.


2018 ◽  
Vol 18 (2) ◽  
pp. 635-653 ◽  
Author(s):  
Xuan Wang ◽  
Colette L. Heald ◽  
Jiumeng Liu ◽  
Rodney J. Weber ◽  
Pedro Campuzano-Jost ◽  
...  

Abstract. Organic aerosols (OA) that strongly absorb solar radiation in the near-UV are referred to as brown carbon (BrC). The sources, evolution, and optical properties of BrC remain highly uncertain and contribute significantly to uncertainty in the estimate of the global direct radiative effect (DRE) of aerosols. Previous modeling studies of BrC optical properties and DRE have been unable to fully evaluate model performance due to the lack of direct measurements of BrC absorption. In this study, we develop a global model simulation (GEOS-Chem) of BrC and test it against BrC absorption measurements from two aircraft campaigns in the continental US (SEAC4RS and DC3). To the best of our knowledge, this is the first study to compare simulated BrC absorption with direct aircraft measurements. We show that BrC absorption properties estimated based on previous laboratory measurements agree with the aircraft measurements of freshly emitted BrC absorption but overestimate aged BrC absorption. In addition, applying a photochemical scheme to simulate bleaching/degradation of BrC improves model skill. The airborne observations are therefore consistent with a mass absorption coefficient (MAC) of freshly emitted biomass burning OA of 1.33 m2 g−1 at 365 nm coupled with a 1-day whitening e-folding time. Using the GEOS-Chem chemical transport model integrated with the RRTMG radiative transfer model, we estimate that the top-of-the-atmosphere all-sky direct radiative effect (DRE) of OA is −0.344 Wm−2, 10 % higher than that without consideration of BrC absorption. Therefore, our best estimate of the absorption DRE of BrC is +0.048 Wm−2. We suggest that the DRE of BrC has been overestimated previously due to the lack of observational constraints from direct measurements and omission of the effects of photochemical whitening.


Atmosphere ◽  
2021 ◽  
Vol 12 (10) ◽  
pp. 1254
Author(s):  
Marios-Bruno Korras-Carraca ◽  
Antonis Gkikas ◽  
Christos Matsoukas ◽  
Nikolaos Hatzianastassiou

We assess the 40-year climatological clear-sky global direct radiative effect (DRE) of five main aerosol types using the MERRA-2 reanalysis and a spectral radiative transfer model (FORTH). The study takes advantage of aerosol-speciated, spectrally and vertically resolved optical properties over the period 1980–2019, to accurately determine the aerosol DREs, emphasizing the attribution of the total DREs to each aerosol type. The results show that aerosols radiatively cool the Earth’s surface and heat its atmosphere by 7.56 and 2.35 Wm−2, respectively, overall cooling the planet by 5.21 Wm−2, partly counterbalancing the anthropogenic greenhouse global warming during 1980–2019. These DRE values differ significantly in terms of magnitude, and even sign, among the aerosol types (sulfate and black carbon aerosols cool and heat the planet by 1.88 and 0.19 Wm−2, respectively), the hemispheres (larger NH than SH values), the surface cover type (larger land than ocean values) or the seasons (larger values in local spring and summer), while considerable inter-decadal changes are evident. These DRE differences are even larger by up to an order of magnitude on a regional scale, highlighting the important role of the aerosol direct radiative effect for local and global climate.


2021 ◽  
Vol 13 (24) ◽  
pp. 4992
Author(s):  
Nicolas Nesme ◽  
Rodolphe Marion ◽  
Olivier Lezeaux ◽  
Stéphanie Doz ◽  
Claude Camy-Peyret ◽  
...  

Methane (CH4) is one of the most contributing anthropogenic greenhouse gases (GHGs) in terms of global warming. Industry is one of the largest anthropogenic sources of methane, which are currently only roughly estimated. New satellite hyperspectral imagers, such as PRISMA, open up daily temporal monitoring of industrial methane sources at a spatial resolution of 30 m. Here, we developed the Characterization of Effluents Leakages in Industrial Environment (CELINE) code to inverse images of the Korpezhe industrial site. In this code, the in-Scene Background Radiance (ISBR) method was combined with a standard Optimal Estimation (OE) approach. The ISBR-OE method avoids the use of a complete and time-consuming radiative transfer model. The ISBR-OEM developed here overcomes the underestimation issues of the linear method (LM) used in the literature for high concentration plumes and controls a posteriori uncertainty. For the Korpezhe site, using the ISBR-OEM instead of the LM -retrieved CH4 concentration map led to a bias correction on CH4 mass from 4 to 16% depending on the source strength. The most important CH4 source has an estimated flow rate ranging from 0.36 ± 0.3 kg·s−1 to 4 ± 1.76 kg·s−1 on nine dates. These local and variable sources contribute to the CH4 budget and can better constrain climate change models.


2021 ◽  
Author(s):  
Babak Jahani ◽  
Hendrik Andersen ◽  
Josep Calbó ◽  
Josep-Abel González ◽  
Jan Cermak

Abstract. This study presents an approach for quantification of cloud-aerosol transition zone broadband longwave radiative effects at the top of the atmosphere (TOA) during daytime over the ocean, based on satellite observations and radiative transfer simulation. Specifically, we used several products from MODIS (Moderate Resolution Imaging Spectroradiometer) and CERES (Clouds and the Earth’s Radiant Energy System) sensors for identification and selection of CERES footprints with horizontally homogeneous transition zone and clear-sky conditions. For the selected transition zone footprints, radiative effect was calculated as the difference between the instantaneous CERES TOA upwelling broadband longwave radiance observations and corresponding clear-sky radiance simulations. The clear-sky radiances were simulated using the Santa Barbara DISORT Atmospheric Radiative Transfer model fed by the hourly ERA5 reanalysis (fifth generation ECMWF reanalysis) atmospheric and surface data. The CERES radiance observations corresponding to the clear-sky footprints detected were also used for validating the simulated clear-sky radiances. We tested this approach using the radiative measurements made by the MODIS and CERES instruments onboard Aqua platform over the south-eastern Atlantic Ocean during August 2010. For the studied period and domain, transition zone radiative effect (given in flux units) is on average equal to 8.0 ± 3.7 W m−2 (heating effect; median: 5.4 W m−2), although cases with radiative effects as large as 50 W m−2 were found.


2017 ◽  
Author(s):  
Annemarie Fraser ◽  
Ashu Dastoor ◽  
Andrei Ryjkov

Abstract. Wildfire frequency has increased in past four decades in Canada, and is expected to increase in future as a result of climate change (Wotton et al., 2010). Mercury (Hg) emissions from biomass burning are known to be significant; however, the impact of biomass burning on air concentration and deposition fluxes in Canada has not been previously quantified. We use estimates of burned biomass from FINN (Fire Inventory from NCAR) and vegetation-specific Emission Factors (EFs) of mercury to investigate the spatiotemporal variability of Hg emissions in Canada. We use Environment and Climate Change Canada's GEM-MACH-Hg (Global Environmental Multi-scale, Modelling Air quality and Chemistry model, mercury version) to quantify the impact of biomass burning in Canada on spatiotemporal variability of air concentrations and deposition fluxes of mercury in Canada. We use North American gaseous elemental mercury (GEM) observations (2010–2015), GEM-MACH-Hg, and an inversion technique to optimize the emission factors for GEM for five vegetation types represented in North American fires to constrain the biomass burning impacts of mercury. We use three biomass burning Hg emissions scenarios in Canada to conduct three sets of model simulations for 2010–2015: two scenarios where Hg is emitted only as GEM using literature or optimized EFs, and a third scenario where Hg is emitted as GEM using literature EFs and particle bound mercury (PBM) emitted using the average GEM/PBM ratio from lab measurements. The three biomass burning emission scenarios represent the range of possible values for the impacts of Hg emissions from biomass burning in Canada on Hg concentration and deposition. We find total biomass burning Hg emissions to be highly variable from year to year, and estimate average 2010–2015 total atmospheric biomass burning emissions of Hg in Canada to be between 6–14 t during the biomass burning season (i.e., from May to September), which is 3–7 times the mercury emission from anthropogenic sources in Canada for this period. On average, 65 % of the emissions occur in the provinces west of Ontario. We find that while emissions from biomass burning have a small impact on surface air concentrations of GEM averaged over individual provinces/territories, the impact at individual sites can be as high as 95 % during burning events. We estimate average annual mercury deposition from biomass burning in Canada to be between 0.3–2.8 t, compared to 0.14 t of mercury deposition from anthropogenic sources during the biomass burning season in Canada. Compared to the biomass burning emissions, the relative impact of fires on mercury deposition is shifted eastward, with on average 54 % of the deposition occurring in provinces west of Ontario. While the relative contribution of Canadian biomass burning to the total mercury deposition over each province/territory is no more than 9 % between 2010–2015, the local contribution in some locations (including areas downwind of biomass burning) can be as high as 80 % (e.g. northwest of Great Slave Lake in 2014) from May-September. We find that northern Alberta and Saskatchewan, central British Columbia, and the area around Great Slave Lake in the Northwest Territories are at greater risk of mercury contamination from biomass burning. GEM is considered to be the dominant mercury species emitted from biomass burning; however, there remains an uncertainty in the speciation of mercury released from biomass burning. We find that the impact of biomass burning emissions on mercury deposition is significantly affected by the uncertainty in speciation of emitted mercury because PBM is more readily deposited closer to the emission sources than GEM; an addition of ~ 18 % of mercury emission from biomass burning in the form of PBM in the model increases the 6 year average deposition by ~ 4 times.


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