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  • 1
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 24 ( 2018-12-18), p. 17963-17978
    Abstract: Abstract. Reactive nitrogen (N) emissions have increased over the last 150 years as a result of greater fossil fuel combustion and food production. The resulting increase in N deposition can alter the function of ecosystems, but characterizing its ecological impacts remains challenging, in part because of uncertainties in model-based estimates of N dry deposition. Here, we use the Geophysical Fluid Dynamics Laboratory (GFDL) atmospheric chemistry–climate model (AM3) coupled with the GFDL land model (LM3) to estimate dry deposition velocities. We leverage the tiled structure of LM3 to represent the impact of physical, hydrological, and ecological heterogeneities on the surface removal of chemical tracers. We show that this framework can be used to estimate N deposition at more ecologically relevant scales (e.g., natural vegetation, water bodies) than from the coarse-resolution global model AM3. Focusing on North America, we show that the faster removal of N over forested ecosystems relative to cropland and pasture implies that coarse-resolution estimates of N deposition from global models systematically underestimate N deposition to natural vegetation by 10 % to 30 % in the central and eastern US. Neglecting the sub-grid scale heterogeneity of dry deposition velocities also results in an underestimate (overestimate) of the amount of reduced (oxidized) nitrogen deposited to water bodies. Overall, changes in land cover associated with human activities are found to slow down the removal of N from the atmosphere, causing a reduction in the dry oxidized, dry reduced, and total (wet+dry) N deposition over the contiguous US of 8 %, 26 %, and 6 %, respectively. We also find that the reduction in the overall rate of removal of N associated with land-use change tends to increase N deposition on the remaining natural vegetation and facilitate N export to Canada. We show that sub-grid scale differences in the surface removal of oxidized and reduced nitrogen imply that projected near-term (2010–2050) changes in oxidized (−47 %) and reduced (+40 %) US N emissions will cause opposite changes in N deposition to water bodies (increase) and natural vegetation (decrease) in the eastern US, with potential implications for acidification and ecosystems.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 2
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 20, No. 1 ( 2020-01-08), p. 281-301
    Abstract: Abstract. The top-of-atmosphere (TOA) outgoing longwave flux over the 9.6 µm ozone band is a fundamental quantity for understanding chemistry–climate coupling. However, observed TOA fluxes are hard to estimate as they exhibit considerable variability in space and time that depend on the distributions of clouds, ozone (O3), water vapor (H2O), air temperature (Ta), and surface temperature (Ts). Benchmarking present-day fluxes and quantifying the relative influence of their drivers is the first step for estimating climate feedbacks from ozone radiative forcing and predicting radiative forcing evolution. To that end, we constructed observational instantaneous radiative kernels (IRKs) under clear-sky conditions, representing the sensitivities of the TOA flux in the 9.6 µm ozone band to the vertical distribution of geophysical variables, including O3, H2O, Ta, and Ts based upon the Aura Tropospheric Emission Spectrometer (TES) measurements. Applying these kernels to present-day simulations from the Chemistry-Climate Model Initiative (CCMI) project as compared to a 2006 reanalysis assimilating satellite observations, we show that the models have large differences in TOA flux, attributable to different geophysical variables. In particular, model simulations continue to diverge from observations in the tropics, as reported in previous studies of the Atmospheric Chemistry Climate Model Intercomparison Project (ACCMIP) simulations. The principal culprits are tropical middle and upper tropospheric ozone followed by tropical lower tropospheric H2O. Five models out of the eight studied here have TOA flux biases exceeding 100 mW m−2 attributable to tropospheric ozone bias. Another set of five models have flux biases over 50 mW m−2 due to H2O. On the other hand, Ta radiative bias is negligible in all models (no more than 30 mW m−2). We found that the atmospheric component (AM3) of the Geophysical Fluid Dynamics Laboratory (GFDL) general circulation model and Canadian Middle Atmosphere Model (CMAM) have the lowest TOA flux biases globally but are a result of cancellation of opposite biases due to different processes. Overall, the multi-model ensemble mean bias is -133±98 mW m−2, indicating that they are too atmospherically opaque due to trapping too much radiation in the atmosphere by overestimated tropical tropospheric O3 and H2O. Having too much O3 and H2O in the troposphere would have different impacts on the sensitivity of TOA flux to O3 and these competing effects add more uncertainties on the ozone radiative forcing. We find that the inter-model TOA outgoing longwave radiation (OLR) difference is well anti-correlated with their ozone band flux bias. This suggests that there is significant radiative compensation in the calculation of model outgoing longwave radiation.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2020
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 3
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 22, No. 18 ( 2022-09-21), p. 12221-12239
    Abstract: Abstract. Anthropogenic aerosols exert a cooling influence that offsets part of the greenhouse gas warming. Due to their short tropospheric lifetime of only several days, the aerosol forcing responds quickly to emissions. Here, we present and discuss the evolution of the aerosol forcing since 2000. There are multiple lines of evidence that allow us to robustly conclude that the anthropogenic aerosol effective radiative forcing (ERF) – both aerosol–radiation interactions (ERFari) and aerosol–cloud interactions (ERFaci) – has become less negative globally, i.e. the trend in aerosol effective radiative forcing changed sign from negative to positive. Bottom-up inventories show that anthropogenic primary aerosol and aerosol precursor emissions declined in most regions of the world; observations related to aerosol burden show declining trends, in particular of the fine-mode particles that make up most of the anthropogenic aerosols; satellite retrievals of cloud droplet numbers show trends in regions with aerosol declines that are consistent with these in sign, as do observations of top-of-atmosphere radiation. Climate model results, including a revised set that is constrained by observations of the ocean heat content evolution show a consistent sign and magnitude for a positive forcing relative to the year 2000 due to reduced aerosol effects. This reduction leads to an acceleration of the forcing of climate change, i.e. an increase in forcing by 0.1 to 0.3 W m−2, up to 12 % of the total climate forcing in 2019 compared to 1750 according to the Intergovernmental Panel on Climate Change (IPCC).
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2022
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 4
    Online Resource
    Online Resource
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 1 ( 2018-01-12), p. 339-355
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 1 ( 2018-01-12), p. 339-355
    Abstract: Abstract. Current estimates of agricultural ammonia (NH3) emissions in China differ by more than a factor of 2, hindering our understanding of their environmental consequences. Here we apply both bottom-up statistical and top-down inversion methods to quantify NH3 emissions from agriculture in China for the year 2008. We first assimilate satellite observations of NH3 column concentration from the Tropospheric Emission Spectrometer (TES) using the GEOS-Chem adjoint model to optimize Chinese anthropogenic NH3 emissions at the 1∕2°  ×  2∕3° horizontal resolution for March–October 2008. Optimized emissions show a strong summer peak, with emissions about 50 % higher in summer than spring and fall, which is underestimated in current bottom-up NH3 emission estimates. To reconcile the latter with the top-down results, we revisit the processes of agricultural NH3 emissions and develop an improved bottom-up inventory of Chinese NH3 emissions from fertilizer application and livestock waste at the 1∕2°  ×  2∕3° resolution. Our bottom-up emission inventory includes more detailed information on crop-specific fertilizer application practices and better accounts for meteorological modulation of NH3 emission factors in China. We find that annual anthropogenic NH3 emissions are 11.7 Tg for 2008, with 5.05 Tg from fertilizer application and 5.31 Tg from livestock waste. The two sources together account for 88 % of total anthropogenic NH3 emissions in China. Our bottom-up emission estimates also show a distinct seasonality peaking in summer, consistent with top-down results from the satellite-based inversion. Further evaluations using surface network measurements show that the model driven by our bottom-up emissions reproduces the observed spatial and seasonal variations of NH3 gas concentrations and ammonium (NH4+) wet deposition fluxes over China well, providing additional credibility to the improvements we have made to our agricultural NH3 emission inventory.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 5
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 3 ( 2018-02-16), p. 2341-2361
    Abstract: Abstract. Widespread efforts to abate ozone (O3) smog have significantly reduced emissions of nitrogen oxides (NOx) over the past 2 decades in the Southeast US, a place heavily influenced by both anthropogenic and biogenic emissions. How reactive nitrogen speciation responds to the reduction in NOx emissions in this region remains to be elucidated. Here we exploit aircraft measurements from ICARTT (July–August 2004), SENEX (June–July 2013), and SEAC4RS (August–September 2013) and long-term ground measurement networks alongside a global chemistry–climate model to examine decadal changes in summertime reactive oxidized nitrogen (RON) and ozone over the Southeast US. We show that our model can reproduce the mean vertical profiles of major RON species and the total (NOy) in both 2004 and 2013. Among the major RON species, nitric acid (HNO3) is dominant (∼ 42–45 %), followed by NOx (31 %), total peroxy nitrates (ΣPNs; 14 %), and total alkyl nitrates (ΣANs; 9–12 %) on a regional scale. We find that most RON species, including NOx, ΣPNs, and HNO3, decline proportionally with decreasing NOx emissions in this region, leading to a similar decline in NOy. This linear response might be in part due to the nearly constant summertime supply of biogenic VOC emissions in this region. Our model captures the observed relative change in RON and surface ozone from 2004 to 2013. Model sensitivity tests indicate that further reductions of NOx emissions will lead to a continued decline in surface ozone and less frequent high-ozone events.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 6
    Online Resource
    Online Resource
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 14 ( 2018-07-17), p. 10157-10175
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 14 ( 2018-07-17), p. 10157-10175
    Abstract: Abstract. Northern India (23–31° N, 68–90° E) is one of the most densely populated and polluted regions in world. Accurately modeling pollution in the region is difficult due to the extreme conditions with respect to emissions, meteorology, and topography, but it is paramount in order to understand how future changes in emissions and climate may alter the region's pollution regime. We evaluate the ability of a developmental version of the new-generation NOAA GFDL Atmospheric Model, version 4 (AM4) to simulate observed wintertime fine particulate matter (PM2.5) and its relationship to meteorology over Northern India. We compare two simulations of GFDL-AM4 nudged to observed meteorology for the period 1980–2016 driven by pollutant emissions from two global inventories developed in support of the Coupled Model Intercomparison Project Phases 5 (CMIP5) and 6 (CMIP6), and compare results with ground-based observations from India's Central Pollution Control Board (CPCB) for the period 1 October 2015–31 March 2016. Overall, our results indicate that the simulation with CMIP6 emissions produces improved concentrations of pollutants over the region relative to the CMIP5-driven simulation. While the particulate concentrations simulated by AM4 are biased low overall, the model generally simulates the magnitude and daily variability of observed total PM2.5. Nitrate and organic matter are the primary components of PM2.5 over Northern India in the model. On the basis of correlations of the individual model components with total observed PM2.5 and correlations between the two simulations, meteorology is the primary driver of daily variability. The model correctly reproduces the shape and magnitude of the seasonal cycle of PM2.5, but the simulated diurnal cycle misses the early evening rise and secondary maximum found in the observations. Observed PM2.5 abundances are by far the highest within the densely populated Indo-Gangetic Plain, where they are closely related to boundary layer meteorology, specifically relative humidity, wind speed, boundary layer height, and inversion strength. The GFDL AM4 model reproduces the overall observed pollution gradient over Northern India as well as the strength of the meteorology–PM2.5 relationship in most locations.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 7
    Online Resource
    Online Resource
    Copernicus GmbH ; 2018
    In:  Atmospheric Chemistry and Physics Vol. 18, No. 17 ( 2018-09-14), p. 13265-13281
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 18, No. 17 ( 2018-09-14), p. 13265-13281
    Abstract: 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.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2018
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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  • 8
    In: Atmospheric Chemistry and Physics, Copernicus GmbH, Vol. 21, No. 2 ( 2021-01-27), p. 1105-1126
    Abstract: Abstract. Feedbacks play a fundamental role in determining the magnitude of the response of the climate system to external forcing, such as from anthropogenic emissions. The latest generation of Earth system models includes aerosol and chemistry components that interact with each other and with the biosphere. These interactions introduce a complex web of feedbacks that is important to understand and quantify. This paper addresses multiple pathways for aerosol and chemical feedbacks in Earth system models. These focus on changes in natural emissions (dust, sea salt, dimethyl sulfide, biogenic volatile organic compounds (BVOCs) and lightning) and changes in reaction rates for methane and ozone chemistry. The feedback terms are then given by the sensitivity of a pathway to climate change multiplied by the radiative effect of the change. We find that the overall climate feedback through chemistry and aerosols is negative in the sixth Coupled Model Intercomparison Project (CMIP6) Earth system models due to increased negative forcing from aerosols in a climate with warmer surface temperatures following a quadrupling of CO2 concentrations. This is principally due to increased emissions of sea salt and BVOCs which are sensitive to climate change and cause strong negative radiative forcings. Increased chemical loss of ozone and methane also contributes to a negative feedback. However, overall methane lifetime is expected to increase in a warmer climate due to increased BVOCs. Increased emissions of methane from wetlands would also offset some of the negative feedbacks. The CMIP6 experimental design did not allow the methane lifetime or methane emission changes to affect climate, so we found a robust negative contribution from interactive aerosols and chemistry to climate sensitivity in CMIP6 Earth system models.
    Type of Medium: Online Resource
    ISSN: 1680-7324
    Language: English
    Publisher: Copernicus GmbH
    Publication Date: 2021
    detail.hit.zdb_id: 2092549-9
    detail.hit.zdb_id: 2069847-1
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