scholarly journals Changes in the aerosol direct radiative forcing from 2001 to 2015: observational constraints and regional mechanisms

Author(s):  
Fabien Paulot ◽  
David Paynter ◽  
Paul Ginoux ◽  
Vaishali Naik ◽  
Larry Horowitz

Abstract. We present observation and model-based estimates of the changes in the direct shortwave effect of aerosols under clear-sky (SDRECS) from 2001 to 2015. Observation-based estimates are obtained from changes in the outgoing shortwave clear-sky radiation (Rsutcs) measured by the Clouds and the Earth's Radiant Energy System (CERES), accounting for the effect of variability in surface albedo, water vapor, and ozone. We find increases in SDRECS (i.e., less radiation scattered to space by aerosols) over Western Europe (0.7–1 W m−2 dec−1) and the Eastern US (0.9–1.8 W m−2 dec−1), decreases over India (−0.5– −1.9 W m−2 dec−1) and no significant change over Eastern China. Comparisons with the GFDL chemistry climate model AM3, driven by CMIP6 historical emissions, show that changes in SDRECS over Western Europe and the Eastern US are well captured, which largely reflects the mature understanding of the sulfate budget in these regions. In contrast, the model overestimates the trends in SDRECS over India and Eastern China. Over China, this bias can be partly attributed to the decline of SO2 emissions after 2007, which is not captured by the CMIP6 emissions. In both India and Eastern China, we find much larger contributions of nitrate and black carbon to changes in SDRECS than in the US and Europe, which highlights the need to better constrain their precursors and chemistry. Globally, our model shows that changes in the all-sky aerosol direct forcing between 2001 and 2015 (+0.03 W m−2) are dominated by black carbon (+0.12 W m−2) with significant offsets from nitrate (−0.03 W m−2) and sulfate (−0.03 W m−2). Changes in the sulfate (+7 %) and nitrate (+60 %) all-sky direct forcing between 2001 and 2015 are only weakly related to changes in the emissions of their precursors (−12.5 % and 19 % for SO2 and NH3, respectively), due mostly to chemical non linearities.

2018 ◽  
Vol 18 (17) ◽  
pp. 13265-13281 ◽  
Author(s):  
Fabien Paulot ◽  
David Paynter ◽  
Paul Ginoux ◽  
Vaishali Naik ◽  
Larry W. Horowitz

Abstract. We present estimates of changes in the direct aerosol effects (DRE) and its anthropogenic component (DRF) from 2001 to 2015 using the GFDL chemistry–climate model AM3 driven by CMIP6 historical emissions. AM3 is evaluated against observed changes in the clear-sky shortwave direct aerosol effect (DREswclr) derived from the Clouds and the Earth's Radiant Energy System (CERES) over polluted regions. From 2001 to 2015, observations suggest that DREclrsw increases (i.e., less radiation is scattered to space by aerosols) over western Europe (0.7–1 W m−2 decade−1) and the eastern US (0.9–1.4 W m−2 decade−1), decreases over India (−1 to −1.6 W m−2 decade−1), and does not change significantly over eastern China. AM3 captures these observed regional changes in DREclrsw well in the US and western Europe, where they are dominated by the decline of sulfate aerosols, but not in Asia, where the model overestimates the decrease of DREclrsw. Over India, the model bias can be partly attributed to a decrease of the dust optical depth, which is not captured by our model and offsets some of the increase of anthropogenic aerosols. Over China, we find that the decline of SO2 emissions after 2007 is not represented in the CMIP6 emission inventory. Accounting for this decline, using the Modular Emission Inventory for China, and for the heterogeneous oxidation of SO2 significantly reduces the model bias. For both India and China, our simulations indicate that nitrate and black carbon contribute more to changes in DREclrsw than in the US and Europe. Indeed, our model suggests that black carbon (+0.12 W m−2) dominates the relatively weak change in DRF from 2001 to 2015 (+0.03 W m−2). Over this period, the changes in the forcing from nitrate and sulfate are both small and of the same magnitude (−0.03 W m−2 each). This is in sharp contrast to the forcing from 1850 to 2001 in which forcings by sulfate and black carbon largely cancel each other out, with minor contributions from nitrate. The differences between these time periods can be well understood from changes in emissions alone for black carbon but not for nitrate and sulfate; this reflects non-linear changes in the photochemical production of nitrate and sulfate associated with changes in both the magnitude and spatial distribution of anthropogenic emissions.


2019 ◽  
Author(s):  
Cheng Gong ◽  
Yadong Lei ◽  
Yimian Ma ◽  
Xu Yue ◽  
Hong Liao

Abstract. Ozone-vegetation feedback is essential to tropospheric ozone (O3) concentrations. The O3 stomatal uptake damages leaf photosynthesis and stomatal conductance and, in turn, influences O3 dry deposition. Further, O3 directly influences isoprene emissions, an important precursor of O3. The effects of O3 on vegetation further alter local meteorological fields and indirectly influence O3 concentrations. In this study, we apply a fully coupled chemistry-carbon-climate global model (ModelE2-YIBs) to evaluate changes in O3 concentrations caused by O3–vegetation interactions. Different parameterizations and sensitivities of the effect of O3 damage on photosynthesis, stomatal conductance, and isoprene emissions (IPE) are implemented in the model. The results show that O3-induced inhibition of stomatal conductance increases surface O3 on average by + 2.1 (+ 1.4) ppbv in eastern China, + 1.6 (− 0.5) ppbv in the eastern U.S., and + 1.3 (+ 1.0) ppbv in western Europe at high (low) damage sensitivity. Such positive feedback is dominated by reduced O3 dry deposition, in addition to the increased temperature and decreased relative humidity from weakened transpiration. Including the effect of O3 damage on IPE slightly reduces surface O3 concentrations by influencing precursors. However, the reduced IPE weakens surface shortwave radiative forcing of secondary organic aerosols leading to increased temperature and O3 concentrations in the eastern U.S. This study highlights the importance of interactions between O3 and vegetation with regard to O3 concentrations and the resultant air quality.


2020 ◽  
Vol 20 (6) ◽  
pp. 3841-3857 ◽  
Author(s):  
Cheng Gong ◽  
Yadong Lei ◽  
Yimian Ma ◽  
Xu Yue ◽  
Hong Liao

Abstract. Ozone–vegetation feedback is essential to tropospheric ozone (O3) concentrations. The O3 stomatal uptake damages leaf photosynthesis and stomatal conductance and, in turn, influences O3 dry deposition. Further, O3 directly influences isoprene emissions, an important precursor of O3. The effects of O3 on vegetation further alter local meteorological fields and indirectly influence O3 concentrations. In this study, we apply a fully coupled chemistry–carbon–climate global model (ModelE2-YIBs) to evaluate changes in O3 concentrations caused by O3–vegetation interactions. Different parameterizations and sensitivities of the effect of O3 damage on photosynthesis, stomatal conductance, and isoprene emissions (IPE) are implemented in the model. The results show that O3-induced inhibition of stomatal conductance increases surface O3 on average by +2.1 ppbv (+1.2 ppbv) in eastern China, +1.8 ppbv (−0.3 ppbv) in the eastern US, and +1.3 ppbv (+1.0 ppbv) in western Europe at high (low) damage sensitivity. Such positive feedback is dominated by reduced O3 dry deposition in addition to the increased temperature and decreased relative humidity from weakened transpiration. Including the effect of O3 damage on IPE slightly reduces surface O3 concentrations by influencing precursors. However, the reduced IPE weaken surface shortwave radiative forcing of secondary organic aerosols, leading to increased temperature and O3 concentrations in the eastern US. This study highlights the importance of interactions between O3 and vegetation with regard to O3 concentrations and the resultant air quality.


2020 ◽  
Vol 80 (2) ◽  
pp. 147-163
Author(s):  
X Liu ◽  
Y Kang ◽  
Q Liu ◽  
Z Guo ◽  
Y Chen ◽  
...  

The regional climate model RegCM version 4.6, developed by the European Centre for Medium-Range Weather Forecasts Reanalysis, was used to simulate the radiation budget over China. Clouds and the Earth’s Radiant Energy System (CERES) satellite data were utilized to evaluate the simulation results based on 4 radiative components: net shortwave (NSW) radiation at the surface of the earth and top of the atmosphere (TOA) under all-sky and clear-sky conditions. The performance of the model for low-value areas of NSW was superior to that for high-value areas. NSW at the surface and TOA under all-sky conditions was significantly underestimated; the spatial distribution of the bias was negative in the north and positive in the south, bounded by 25°N for the annual and seasonal averaged difference maps. Compared with the all-sky condition, the simulation effect under clear-sky conditions was significantly better, which indicates that the cloud fraction is the key factor affecting the accuracy of the simulation. In particular, the bias of the TOA NSW under the clear-sky condition was <±10 W m-2 in the eastern areas. The performance of the model was better over the eastern monsoon region in winter and autumn for surface NSW under clear-sky conditions, which may be related to different levels of air pollution during each season. Among the 3 areas, the regional average biases overall were largest (negative) over the Qinghai-Tibet alpine region and smallest over the eastern monsoon region.


2021 ◽  
Vol 4 (1) ◽  
Author(s):  
Zhili Wang ◽  
Lei Lin ◽  
Yangyang Xu ◽  
Huizheng Che ◽  
Xiaoye Zhang ◽  
...  

AbstractAnthropogenic aerosol (AA) forcing has been shown as a critical driver of climate change over Asia since the mid-20th century. Here we show that almost all Coupled Model Intercomparison Project Phase 6 (CMIP6) models fail to capture the observed dipole pattern of aerosol optical depth (AOD) trends over Asia during 2006–2014, last decade of CMIP6 historical simulation, due to an opposite trend over eastern China compared with observations. The incorrect AOD trend over China is attributed to problematic AA emissions adopted by CMIP6. There are obvious differences in simulated regional aerosol radiative forcing and temperature responses over Asia when using two different emissions inventories (one adopted by CMIP6; the other from Peking university, a more trustworthy inventory) to driving a global aerosol-climate model separately. We further show that some widely adopted CMIP6 pathways (after 2015) also significantly underestimate the more recent decline in AA emissions over China. These flaws may bring about errors to the CMIP6-based regional climate attribution over Asia for the last two decades and projection for the next few decades, previously anticipated to inform a wide range of impact analysis.


2016 ◽  
Author(s):  
Yu Hao Mao ◽  
Hong Liao

Abstract. We applied a global three-dimensional chemical transport model (GEOS-Chem) to examine the impacts of the East Asian monsoon on the interannual variations of mass concentrations and direct radiative forcing (DRF) of black carbon (BC) over eastern China (110–125° E, 20–45° N). With emissions fixed at the year 2010 levels, model simulations were driven by the Goddard Earth Observing System (GEOS-4) meteorological fields for 1986–2006 and the Modern Era Retrospective-analysis for Research and Applications (MERRA) meteorological fields for 1980–2010. During the period of 1986–2006, simulated JJA and DJF surface BC concentrations were higher in MERRA than in GEOS-4 by 0.30 µg m−3 (44 %) and 0.77 µg m−3 (54 %), respectively, because of the generally weaker precipitation in MERRA. We found that the strength of the East Asian summer monsoon (EASM, (East Asian winter monsoon, EAWM)) negatively correlated with simulated JJA (DJF) surface BC concentrations (r = –0.7 (–0.7) in GEOS-4 and –0.4 (–0.7) in MERRA), mainly by the changes in atmospheric circulation. Relative to the five strongest EASM years, simulated JJA surface BC concentrations in the five weakest monsoon years were higher over northern China (110–125° E, 28–45° N) by 0.04–0.09 µg m−3 (3–11 %), but lower over southern China (110–125° E, 20–27° N) by 0.03–0.04 µg m−3 (10–11 %). Compared to the five strongest EAWM years, simulated DJF surface BC concentrations in the five weakest monsoon years were higher by 0.13–0.15 µg m−3 (5–8 %) in northern China and by 0.04–0.10 µg m−3 (3–12 %) in southern China. The resulting JJA (DJF) mean all-sky DRF of BC at the top of the atmosphere were 0.04 W m−2 (3 %, (0.03 W m−2, 2 %)) higher in northern China but 0.06 W m−2 (14 %, (0.03 W m−2, 3 %)) lower in southern China. In the weakest monsoon years, the weaker vertical convection led to the lower BC concentrations above 1–2 km in southern China, and therefore the lower BC DRF in the region. The differences in vertical profiles of BC between the weakest and strongest EASM years (1998–1997) and EAWM years (1990–1996) reached up to –0.09 µg m−3 (–46 %) and –0.08 µg m−3 (–11 %) at 1–2 km in eastern China.


2014 ◽  
Vol 7 (5) ◽  
pp. 2503-2516 ◽  
Author(s):  
K. Klingmüller ◽  
B. Steil ◽  
C. Brühl ◽  
H. Tost ◽  
J. Lelieveld

Abstract. The modelling of aerosol radiative forcing is a major cause of uncertainty in the assessment of global and regional atmospheric energy budgets and climate change. One reason is the strong dependence of the aerosol optical properties on the mixing state of aerosol components, such as absorbing black carbon and, predominantly scattering sulfates. Using a new column version of the aerosol optical properties and radiative-transfer code of the ECHAM/MESSy atmospheric-chemistry–climate model (EMAC), we study the radiative transfer applying various mixing states. The aerosol optics code builds on the AEROPT (AERosol OPTical properties) submodel, which assumes homogeneous internal mixing utilising the volume average refractive index mixing rule. We have extended the submodel to additionally account for external mixing, partial external mixing and multilayered particles. Furthermore, we have implemented the volume average dielectric constant and Maxwell Garnett mixing rule. We performed regional case studies considering columns over China, India and Africa, corroborating much stronger absorption by internal than external mixtures. Well-mixed aerosol is a good approximation for particles with a black-carbon core, whereas particles with black carbon at the surface absorb significantly less. Based on a model simulation for the year 2005, we calculate that the global aerosol direct radiative forcing for homogeneous internal mixing differs from that for external mixing by about 0.5 W m−2.


2011 ◽  
Vol 11 (8) ◽  
pp. 24085-24125 ◽  
Author(s):  
E. M. Leibensperger ◽  
L. J. Mickley ◽  
D. J. Jacob ◽  
W.-T. Chen ◽  
J. H. Seinfeld ◽  
...  

Abstract. We use the GEOS-Chem chemical transport model combined with the GISS general circulation model to calculate the aerosol direct and indirect (warm cloud) radiative forcings from US anthropogenic sources over the 1950–2050 period, based on historical emission inventories and future projections from the IPCC A1B scenario. The aerosol simulation is evaluated with observed spatial distributions and 1980–2010 trends of aerosol concentrations and wet deposition in the contiguous US. The radiative forcing from US anthropogenic aerosols is strongly localized over the eastern US. We find that it peaked in 1970–1990, with values over the eastern US (east of 100° W) of −2.0 W m−2 for direct forcing including contributions from sulfate (−2.0 W m−2), nitrate (−0.2 W m−2), organic carbon (−0.2 W m−2), and black carbon (+0.4 W m−2). The aerosol indirect effect is of comparable magnitude to the direct forcing. We find that the forcing declined sharply from 1990 to 2010 (by 0.8 W m−2 direct and 1.0 W m−2 indirect), mainly reflecting decreases in SO2 emissions, and project that it will continue declining post-2010 but at a much slower rate since US SO2 emissions have already declined by almost 60 % from their peak. This suggests that much of the warming effect of reducing US anthropogenic aerosol sources may have already been realized by 2010, however some additional warming is expected through 2020. The small positive radiative forcing from US BC emissions (+0.3 W m−2 over the eastern US in 2010) suggests that an emission control strategy focused on BC would have only limited climate benefit.


2020 ◽  
Vol 163 (3) ◽  
pp. 1427-1442 ◽  
Author(s):  
Steven J Smith ◽  
Jean Chateau ◽  
Kalyn Dorheim ◽  
Laurent Drouet ◽  
Olivier Durand-Lasserve ◽  
...  

AbstractThe relatively short atmospheric lifetimes of methane (CH4) and black carbon (BC) have focused attention on the potential for reducing anthropogenic climate change by reducing Short-Lived Climate Forcer (SLCF) emissions. This paper examines radiative forcing and global mean temperature results from the Energy Modeling Forum (EMF)-30 multi-model suite of scenarios addressing CH4 and BC mitigation, the two major short-lived climate forcers. Central estimates of temperature reductions in 2040 from an idealized scenario focused on reductions in methane and black carbon emissions ranged from 0.18–0.26 °C across the nine participating models. Reductions in methane emissions drive 60% or more of these temperature reductions by 2040, although the methane impact also depends on auxiliary reductions that depend on the economic structure of the model. Climate model parameter uncertainty has a large impact on results, with SLCF reductions resulting in as much as 0.3–0.7 °C by 2040. We find that the substantial overlap between a SLCF-focused policy and a stringent and comprehensive climate policy that reduces greenhouse gas emissions means that additional SLCF emission reductions result in, at most, a small additional benefit of ~ 0.1 °C in the 2030–2040 time frame.


2019 ◽  
Vol 19 (7) ◽  
pp. 4877-4897 ◽  
Author(s):  
Sandro Vattioni ◽  
Debra Weisenstein ◽  
David Keith ◽  
Aryeh Feinberg ◽  
Thomas Peter ◽  
...  

Abstract. Stratospheric sulfate geoengineering (SSG) could contribute to avoiding some of the adverse impacts of climate change. We used the SOCOL-AER global aerosol–chemistry–climate model to investigate 21 different SSG scenarios, each with 1.83 Mt S yr−1 injected either in the form of accumulation-mode H2SO4 droplets (AM H2SO4), gas-phase SO2 or as combinations of both. For most scenarios, the sulfur was continuously emitted at an altitude of 50 hPa (≈20 km) in the tropics and subtropics. We assumed emissions to be zonally and latitudinally symmetric around the Equator. The spread of emissions ranged from 3.75∘ S–3.75∘ N to 30∘ S–30∘ N. In the SO2 emission scenarios, continuous production of tiny nucleation-mode particles results in increased coagulation, which together with gaseous H2SO4 condensation, produces coarse-mode particles. These large particles are less effective for backscattering solar radiation and have a shorter stratospheric residence time than AM H2SO4 particles. On average, the stratospheric aerosol burden and corresponding all-sky shortwave radiative forcing for the AM H2SO4 scenarios are about 37 % larger than for the SO2 scenarios. The simulated stratospheric aerosol burdens show a weak dependence on the latitudinal spread of emissions. Emitting at 30∘ N–30∘ S instead of 10∘ N–10∘ S only decreases stratospheric burdens by about 10 %. This is because a decrease in coagulation and the resulting smaller particle size is roughly balanced by faster removal through stratosphere-to-troposphere transport via tropopause folds. Increasing the injection altitude is also ineffective, although it generates a larger stratospheric burden, because enhanced condensation and/or coagulation leads to larger particles, which are less effective scatterers. In the case of gaseous SO2 emissions, limiting the sulfur injections spatially and temporally in the form of point and pulsed emissions reduces the total global annual nucleation, leading to less coagulation and thus smaller particles with increased stratospheric residence times. Pulse or point emissions of AM H2SO4 have the opposite effect: they decrease the stratospheric aerosol burden by increasing coagulation and only slightly decrease clear-sky radiative forcing. This study shows that direct emission of AM H2SO4 results in higher radiative forcing for the same sulfur equivalent mass injection strength than SO2 emissions, and that the sensitivity to different injection strategies varies for different forms of injected sulfur.


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