scholarly journals Hydrological controls on the tropospheric ozone greenhouse gas effect

Elem Sci Anth ◽  
2017 ◽  
Vol 5 ◽  
Author(s):  
Le Kuai ◽  
Kevin W. Bowman ◽  
Helen M. Worden ◽  
Robert L. Herman ◽  
Susan S. Kulawik

The influence of the hydrological cycle in the greenhouse gas (GHG) effect of tropospheric ozone (O3) is quantified in terms of the O3 longwave radiative effect (LWRE), which is defined as the net reduction of top-of-atmosphere flux due to total tropospheric O3 absorption. The O3 LWRE derived from the infrared spectral measurements by Aura’s Tropospheric Emission Spectrometer (TES) show that the spatiotemporal variation of LWRE is relevant to relative humidity, surface temperature, and tropospheric O3 column. The zonally averaged subtropical LWRE is ~0.2 W m–2 higher than the zonally averaged tropical LWRE, generally due to lower water vapor concentrations and less cloud coverage at the downward branch of the Hadley cell in the subtropics. The largest values of O3 LWRE over the Middle East (>1 W/m2) are further due to large thermal contrasts and tropospheric ozone enhancements from atmospheric circulation and pollution. Conversely, the low O3 LWRE over the Inter-Tropical Convergence Zone (on average 0.4 W m–2) is due to strong water vapor absorption and cloudiness, both of which reduce the tropospheric O3 absorption in the longwave radiation. These results show that changes in the hydrological cycle due to climate change could affect the magnitude and distribution of ozone radiative forcing.

2018 ◽  
Author(s):  
Steven Turnock ◽  
Oliver Wild ◽  
Frank Dentener ◽  
Yanko Davila ◽  
Louisa Emmons ◽  
...  

Abstract. This study quantifies future changes in tropospheric ozone (O3) using a simple parameterisation of source-receptor relationships based on simulations from a range of models participating in the Task Force on Hemispheric Transport of Air Pollutants (TF-HTAP) experiments. Surface and tropospheric O3 changes are calculated globally and across 16 regions from perturbations in precursor emissions (NOx, CO, VOCs) and methane (CH4) abundance. A source attribution is provided for each source region along with an estimate of uncertainty based on the spread of the results from the models. Tests against model simulations using HadGEM2-ES confirm that the approaches used within the parameterisation are valid. The O3 response to changes in CH4 abundance is slightly larger in TF-HTAP Phase 2 than in the TF-HTAP Phase 1 assessment (2010) and provides further evidence that controlling CH4 is important for limiting future O3 concentrations. Different treatments of chemistry and meteorology in models remains one of the largest uncertainties in calculating the O3 response to perturbations in CH4 abundance and precursor emissions, particularly over the Middle East and South Asian regions. Emission changes for the future ECLIPSE scenarios and a subset of preliminary Shared Socio-economic Pathways (SSPs) indicate that surface O3 concentrations will increase by 1 to 8 ppbv in 2050 across different regions. Source attribution analysis highlights the growing importance of CH4 in the future under current legislation. A global tropospheric O3 radiative forcing of +0.07 W m−2 from 2010 to 2050 is predicted using the ECLIPSE scenarios and SSPs, based solely on changes in CH4 abundance and tropospheric O3 precursor emissions and neglecting any influence of climate change. Current legislation is shown to be inadequate in limiting the future degradation of surface ozone air quality and enhancement of near-term climate warming. More stringent future emission controls provide a large reduction in both surface O3 concentrations and O3 radiative forcing. The parameterisation provides a simple tool to highlight the different impacts and associated uncertainties of local and hemispheric emission control strategies on both surface air quality and the near-term climate forcing by tropospheric O3.


2017 ◽  
Author(s):  
Antara Banerjee ◽  
Amanda C. Maycock ◽  
John A. Pyle

Abstract. The ozone radiative forcings (RFs) resulting from projected changes in climate, ozone-depleting substances (ODSs), non-methane ozone precursor emissions and methane between the years 2000 and 2100 are calculated using simulations from the UM-UKCA chemistry-climate model. Projected measures to improve air-quality through reductions in tropospheric ozone precursor emissions present a co-benefit for climate, with a net global mean ozone RF of −0.09 Wm−2. This is opposed by a positive ozone RF of 0.07 Wm−2 due to future decreases in ODSs, which is mainly driven by an increase in tropospheric ozone through stratosphere-to-troposphere exchange. An increase in methane abundance by more than a factor of two (as projected by the RCP8.5 scenario) is found to drive an ozone RF of 0.19 Wm−2, which would greatly outweigh the climate benefits of tropospheric non-methane ozone precursor reductions. A third of the ozone RF due to the projected increase in methane results from increases in stratospheric ozone. The sign of the ozone RF due to future changes in climate (including the radiative effects of greenhouse gas concentrations, sea surface temperatures and sea ice changes) is shown to be dependent on the greenhouse gas emissions pathway, with a positive RF (0.06 Wm−2) for RCP4.5 and a negative RF (−0.07 Wm−2) for the RCP8.5 scenario. This dependence arises from differences in the contribution to RF from stratospheric ozone changes.


2013 ◽  
Vol 13 (8) ◽  
pp. 4057-4072 ◽  
Author(s):  
K. W. Bowman ◽  
D. T. Shindell ◽  
H. M. Worden ◽  
J.F. Lamarque ◽  
P. J. Young ◽  
...  

Abstract. We use simultaneous observations of tropospheric ozone and outgoing longwave radiation (OLR) sensitivity to tropospheric ozone from the Tropospheric Emission Spectrometer (TES) to evaluate model tropospheric ozone and its effect on OLR simulated by a suite of chemistry-climate models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean of ACCMIP models show a persistent but modest tropospheric ozone low bias (5–20 ppb) in the Southern Hemisphere (SH) and modest high bias (5–10 ppb) in the Northern Hemisphere (NH) relative to TES ozone for 2005–2010. These ozone biases have a significant impact on the OLR. Using TES instantaneous radiative kernels (IRK), we show that the ACCMIP ensemble mean tropospheric ozone low bias leads up to 120 mW m−2 OLR high bias locally but zonally compensating errors reduce the global OLR high bias to 39 ± 41 m Wm−2 relative to TES data. We show that there is a correlation (R2 = 0.59) between the magnitude of the ACCMIP OLR bias and the deviation of the ACCMIP preindustrial to present day (1750–2010) ozone radiative forcing (RF) from the ensemble ozone RF mean. However, this correlation is driven primarily by models whose absolute OLR bias from tropospheric ozone exceeds 100 m Wm−2. Removing these models leads to a mean ozone radiative forcing of 394 ± 42 m Wm−2. The mean is about the same and the standard deviation is about 30% lower than an ensemble ozone RF of 384 ± 60 m Wm−2 derived from 14 of the 16 ACCMIP models reported in a companion ACCMIP study. These results point towards a profitable direction of combining satellite observations and chemistry-climate model simulations to reduce uncertainty in ozone radiative forcing.


2017 ◽  
Vol 17 (2) ◽  
pp. 1557-1569 ◽  
Author(s):  
Tomás Sherwen ◽  
Mat J. Evans ◽  
Lucy J. Carpenter ◽  
Johan A. Schmidt ◽  
Loretta J. Mickley

Abstract. Tropospheric ozone (O3) is a global warming gas, but the lack of a firm observational record since the preindustrial period means that estimates of its radiative forcing (RFTO3) rely on model calculations. Recent observational evidence shows that halogens are pervasive in the troposphere and need to be represented in chemistry-transport models for an accurate simulation of present-day O3. Using the GEOS-Chem model we show that tropospheric halogen chemistry is likely more active in the present day than in the preindustrial. This is due to increased oceanic iodine emissions driven by increased surface O3, higher anthropogenic emissions of bromo-carbons, and an increased flux of bromine from the stratosphere. We calculate preindustrial to present-day increases in the tropospheric O3 burden of 113 Tg without halogens but only 90 Tg with, leading to a reduction in RFTO3 from 0.43 to 0.35 Wm−2. We attribute  ∼ 50 % of this reduction to increased bromine flux from the stratosphere,  ∼ 35 % to the ocean–atmosphere iodine feedback, and  ∼ 15 % to increased tropospheric sources of anthropogenic halogens. This reduction of tropospheric O3 radiative forcing due to halogens (0.087 Wm−2) is greater than that from the radiative forcing of stratospheric O3 (∼ 0.05 Wm−2). Estimates of RFTO3 that fail to consider halogen chemistry are likely overestimates (∼ 25 %).


2004 ◽  
Vol 4 (6) ◽  
pp. 7917-7984 ◽  
Author(s):  
R. Lang ◽  
M. G. Lawrence

Abstract. This study examines two key parameters of the hydrological cycle, water vapor (WV) and precipitation rates (PR), as modelled by the chemistry transport model MATCH (Model of Atmospheric Transport and Chemistry) driven by National Centers for Environmental Prediction (NCEP) reanalysis data (NRA). For model output evaluation we employ WV total column data from the Global Ozone Monitoring Experiment (GOME) on ERS-2, which is the only instrument capable measuring WV on a global scale and over all surface types with a substantial data record from 1995 to the present. We find that MATCH and NRA WV and PR distributions are closely related, but that significant regional differences in both parameters exist in magnitude and distribution patterns when compared to the observations. We also find that WV residual patterns between model and observations show remarkable similarities to residuals observed in the PR when comparing MATCH and NRA output to observations comprised by the Global Precipitation Climatology Project (GPCP). We conclude that deficiencies in model parameters shared by MATCH and NRA, like, for example, in the evapotranspiration rates, are likely to lead to the observed differences. Regional differences between MATCH modelled WV columns and the observations can be as large as 2 cm on the basis of a three years monthly average. Differences in the global mean WV values are, however, below 1 mm. Regional differences in the PR between MATCH and GPCP can be above 5 mm per day and MATCH computes on average a higher PR than what has been observed. As a consequence, this leads to shorter model WV residence times by about 1 day as compared to NRA data and the observations. We find that MATCH has problems in modelling the WV content in regions of strong upward convection like, for example, along the Inter Tropical Convergence Zone, where it appears to be generally too dry as compared to the observations. The study therefore suggests that a too rapid conversion of WV to precipitate in MATCH, especially in instances of strong convection, leads to regionally too dry model results and in turn to generally too low WV residence times. The study additionally demonstrates the value of the GOME WV record for model evaluation.


2009 ◽  
Vol 9 (2) ◽  
pp. 5505-5547 ◽  
Author(s):  
J. Joiner ◽  
M. R. Schoeberl ◽  
A. P. Vasilkov ◽  
L. Oreopoulos ◽  
S. Platnick ◽  
...  

Abstract. Estimates of the radiative forcing due to anthropogenically-produced tropospheric O3 are derived primarily from models. Here, we use tropospheric ozone and cloud data from several instruments in the A-train constellation of satellites as well as information from the GEOS-5 Data Assimilation System to accurately estimate the radiative effect of tropospheric O3 for January and July 2005. Since we cannot distinguish between natural and anthropogenic sources with the satellite data, our derived radiative effect reflects the unadjusted (instantaneous) effect of the total tropospheric O3 rather than the anthropogenic component. We improve upon previous estimates of tropospheric ozone mixing ratios from a residual approach using the NASA Earth Observing System (EOS) Aura Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) by incorporating cloud pressure information from OMI. We focus specifically on the magnitude and spatial structure of the cloud effect on both the short- and long-wave radiative budget. The estimates presented here can be used to evaluate the various aspects of model-generated radiative forcing. For example, our derived cloud impact is to reduce the radiative effect of tropospheric ozone by ~16%. This is centered within the published range of model-produced cloud effect on instantaneous radiative forcing.


2020 ◽  
Vol 20 (1) ◽  
pp. 281-301 ◽  
Author(s):  
Le Kuai ◽  
Kevin W. Bowman ◽  
Kazuyuki Miyazaki ◽  
Makoto Deushi ◽  
Laura Revell ◽  
...  

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.


2019 ◽  
Author(s):  
Le Kuai ◽  
Kevin W. Bowman ◽  
Helen Worden ◽  
Kazuyuki Miyazaki ◽  
Susan Kulawik ◽  
...  

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 its evolution. To that end, we construct observational instantaneous radiative kernels (IRKs) 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 Inter-comparison Project (ACCMIP) simulations. The principal culprits are tropical mid and upper tropospheric ozone followed by tropical lower tropospheric H2O. Five models out of the eight studied here have TOA flux biases exceeding 100 mWm−2 attributable to tropospheric ozone bias. Another set of five models flux biases over 50 mWm−2 due to H2O. On the other hand, Ta radiative bias is negligible in all models (no more than 30 mWm−2). We found that AM3 and CMAM have the lowest TOA flux biases globally but are a result of cancellation of difference processes. Overall, the multi-model ensemble mean bias is −132.9 ± 98 mWm−2, indicating that they are too atmospherically opaque thereby reducing sensitivity of TOA flux to ozone and potentially an underestimate of ozone radiative forcing. We find that the inter-model TOA 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.


2012 ◽  
Vol 12 (7) ◽  
pp. 16493-16514 ◽  
Author(s):  
G.-J. Roelofs

Abstract. The dominant removal mechanism for atmospheric aerosol is activation of particles to cloud droplets and subsequent wet deposition in precipitation. The atmospheric lifetime of aerosol is thus closely coupled to the atmospheric cycling time of water vapor. Changes of hydrological cycle characteristics resulting from climate change therefore directly affect aerosol lifetime, and thus the radiative forcing exerted by aerosol. This study expresses the coupling between water vapor and aerosol lifetimes and their temperature sensitivities in fundamental equations and in terms of the efficiency of processing of air by precipitating clouds. Based on climate model simulations these temperature sensitivities are estimated to be on the order of +5.3% K−1, but this may be an overestimation. Generally, shifting spatial and temporal patterns of aerosol (precursor) emissions and precipitation, and changes in aerosol activation efficiency probably influence aerosol lifetimes more than climate change itself, resulting in a wide range of simulated aerosol lifetime sensitivities between aerosol-climate models. It is possible that the climate sensitivity of models plays a role. It can be argued that climate sensitivity is intrinsically coupled with the simulated (temperature sensitivity of the) aerosol lifetime through the distribution of water vapor and aerosol between the lower and upper troposphere. This implies a fundamental relation between various feedback forcings (water vapor, lapse rate, cloud) and the aerosol forcing, illustrating the key role of the hydrological cycle in different aspects of the climate system.


2011 ◽  
Vol 11 (10) ◽  
pp. 27637-27659
Author(s):  
M. A. Pfeffer ◽  
J. E. Kristjansson ◽  
F. Stordal ◽  
T. Berntsen ◽  
J. Fast

Abstract. Aerosol-cloud-water vapor interactions in clean maritime air have been described for different aerosol sources using the WRF-Chem atmospheric model. The simulations were made over the Lesser Antilles in the region of the RICO measurement campaign where the clouds are low, patchy, typical trade-wind cumuli. In this very clean air, sea salt and DMS are found to have greater effects than anthropogenic pollution on the cloud droplets' effective radii and longwave and shortwave outgoing top of atmosphere radiation. The changes in radiation due to each aerosol source are a function of how each source influences aerosol concentration, cloud droplet number concentration, cloud droplet sizes, and water vapor concentration. Changes in outgoing shortwave radiation are due predominantly to changes in the clouds, followed by the direct aerosol effect which is about 2/3 as important, followed by the effects of water vapor which is in turn about 2/3 as important as the direct effect. Changes in outgoing longwave radiation are due predominantly to changes in the clouds, with changes in water vapor being about 1/10 as important. The simulated changes in water vapor concentration are due to the competing effects of aerosol particles being able to both enhance condensation of available water vapor and enhance evaporation of smaller droplets. These changes are independent of precipitation effects as there is essentially no drizzle in the domain. It is expected that the indirect radiative forcing of aerosols via water vapor may be stronger in dirtier and more strongly convective conditions.


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