scholarly journals Calibrating a global atmospheric chemistry transport model using Gaussian process emulation and ground-level concentrations of ozone and carbon monoxide

2021 ◽  
Author(s):  
Edmund Ryan ◽  
Oliver Wild

Abstract. Atmospheric chemistry transport models are important tools to investigate the local, regional and global controls on atmospheric composition and air quality. To ensure that these models represent the atmosphere adequately it is important to compare their outputs with measurements. However, ground based measurements of atmospheric composition are typically sparsely distributed and representative of much smaller spatial scales than those resolved in models, and thus direct comparison incurs uncertainty. In this study, we investigate the feasibility of using observations of one or more atmospheric constituents to estimate parameters in chemistry transport models and to explore how these estimates and their uncertainties depend upon representation errors and the level of spatial coverage of the measurements. We apply Gaussian process emulation to explore the model parameter space and use monthly averaged ground-level concentrations of ozone (O3) and carbon monoxide (CO) from across Europe and the US. Using synthetic observations we find that the estimates of parameters with greatest influence on O3 and CO are unbiased, and the associated parameter uncertainties are low even at low spatial coverage or with high representation error. Using reanalysis data, we find that estimates of the most influential parameter – corresponding to the dry deposition process – are closer to its expected value using both O3 and CO data than using O3 alone. This is remarkable because it shows that while CO is largely unaffected by dry deposition, the additional constraints it provides are valuable for achieving unbiased estimates of the dry deposition parameter. In summary, these findings identify the level of spatial representation error and coverage needed to achieve good parameter estimates and highlight the benefits of using multiple constraints to calibrate atmospheric chemistry models.

2021 ◽  
Vol 14 (9) ◽  
pp. 5373-5391
Author(s):  
Edmund Ryan ◽  
Oliver Wild

Abstract. Atmospheric chemistry transport models are important tools to investigate the local, regional and global controls on atmospheric composition and air quality. To ensure that these models represent the atmosphere adequately, it is important to compare their outputs with measurements. However, ground based measurements of atmospheric composition are typically sparsely distributed and representative of much smaller spatial scales than those resolved in models; thus, direct comparison incurs uncertainty. In this study, we investigate the feasibility of using observations of one or more atmospheric constituents to estimate parameters in chemistry transport models and to explore how these estimates and their uncertainties depend upon representation errors and the level of spatial coverage of the measurements. We apply Gaussian process emulation to explore the model parameter space and use monthly averaged ground-level concentrations of ozone (O3) and carbon monoxide (CO) from across Europe and the US. Using synthetic observations, we find that the estimates of parameters with greatest influence on O3 and CO are unbiased, and the associated parameter uncertainties are low even at low spatial coverage or with high representation error. Using reanalysis data, we find that estimates of the most influential parameter – corresponding to the dry deposition process – are closer to its expected value using both O3 and CO data than using O3 alone. This is remarkable because it shows that while CO is largely unaffected by dry deposition, the additional constraints it provides are valuable for achieving unbiased estimates of the dry deposition parameter. In summary, these findings identify the level of spatial representation error and coverage needed to achieve good parameter estimates and highlight the benefits of using multiple constraints to calibrate atmospheric chemistry transport models.


2018 ◽  
Vol 18 (21) ◽  
pp. 16155-16172 ◽  
Author(s):  
Laura E. Revell ◽  
Andrea Stenke ◽  
Fiona Tummon ◽  
Aryeh Feinberg ◽  
Eugene Rozanov ◽  
...  

Abstract. Previous multi-model intercomparisons have shown that chemistry–climate models exhibit significant biases in tropospheric ozone compared with observations. We investigate annual-mean tropospheric column ozone in 15 models participating in the SPARC–IGAC (Stratosphere–troposphere Processes And their Role in Climate–International Global Atmospheric Chemistry) Chemistry-Climate Model Initiative (CCMI). These models exhibit a positive bias, on average, of up to 40 %–50 % in the Northern Hemisphere compared with observations derived from the Ozone Monitoring Instrument and Microwave Limb Sounder (OMI/MLS), and a negative bias of up to ∼30 % in the Southern Hemisphere. SOCOLv3.0 (version 3 of the Solar-Climate Ozone Links CCM), which participated in CCMI, simulates global-mean tropospheric ozone columns of 40.2 DU – approximately 33 % larger than the CCMI multi-model mean. Here we introduce an updated version of SOCOLv3.0, “SOCOLv3.1”, which includes an improved treatment of ozone sink processes, and results in a reduction in the tropospheric column ozone bias of up to 8 DU, mostly due to the inclusion of N2O5 hydrolysis on tropospheric aerosols. As a result of these developments, tropospheric column ozone amounts simulated by SOCOLv3.1 are comparable with several other CCMI models. We apply Gaussian process emulation and sensitivity analysis to understand the remaining ozone bias in SOCOLv3.1. This shows that ozone precursors (nitrogen oxides (NOx), carbon monoxide, methane and other volatile organic compounds, VOCs) are responsible for more than 90 % of the variance in tropospheric ozone. However, it may not be the emissions inventories themselves that result in the bias, but how the emissions are handled in SOCOLv3.1, and we discuss this in the wider context of the other CCMI models. Given that the emissions data set to be used for phase 6 of the Coupled Model Intercomparison Project includes approximately 20 % more NOx than the data set used for CCMI, further work is urgently needed to address the challenges of simulating sub-grid processes of importance to tropospheric ozone in the current generation of chemistry–climate models.


2014 ◽  
Vol 14 (17) ◽  
pp. 9295-9316 ◽  
Author(s):  
O. Stein ◽  
M. G. Schultz ◽  
I. Bouarar ◽  
H. Clark ◽  
V. Huijnen ◽  
...  

Abstract. Despite the developments in the global modelling of chemistry and of the parameterization of the physical processes, carbon monoxide (CO) concentrations remain underestimated during Northern Hemisphere (NH) winter by most state-of-the-art chemistry transport models. The consequential model bias can in principle originate from either an underestimation of CO sources or an overestimation of its sinks. We address both the role of surface sources and sinks with a series of MOZART (Model for Ozone And Related Tracers) model sensitivity studies for the year 2008 and compare our results to observational data from ground-based stations, satellite observations, and vertical profiles from measurements on passenger aircraft. In our base case simulation using MACCity (Monitoring Atmospheric Composition and Climate project) anthropogenic emissions, the near-surface CO mixing ratios are underestimated in the Northern Hemisphere by more than 20 ppb from December to April, with the largest bias of up to 75 ppb over Europe in January. An increase in global biomass burning or biogenic emissions of CO or volatile organic compounds (VOCs) is not able to reduce the annual course of the model bias and yields concentrations over the Southern Hemisphere which are too high. Raising global annual anthropogenic emissions with a simple scaling factor results in overestimations of surface mixing ratios in most regions all year round. Instead, our results indicate that anthropogenic CO and, possibly, VOC emissions in the MACCity inventory are too low for the industrialized countries only during winter and spring. Reasonable agreement with observations can only be achieved if the CO emissions are adjusted seasonally with regionally varying scaling factors. A part of the model bias could also be eliminated by exchanging the original resistance-type dry deposition scheme with a parameterization for CO uptake by oxidation from soil bacteria and microbes, which reduces the boreal winter dry deposition fluxes. The best match to surface observations, satellite retrievals, and aircraft observations was achieved when the modified dry deposition scheme was combined with increased wintertime road traffic emissions over Europe and North America (factors up to 4.5 and 2, respectively). One reason for the apparent underestimation of emissions may be an exaggerated downward trend in the Representative Concentration Pathway (RCP) 8.5 scenario in these regions between 2000 and 2010, as this scenario was used to extrapolate the MACCity emissions from their base year 2000. This factor is potentially amplified by a lack of knowledge about the seasonality of emissions. A methane lifetime of 9.7 yr for our basic model and 9.8 yr for the optimized simulation agrees well with current estimates of global OH, but we cannot fully exclude a potential effect from errors in the geographical and seasonal distribution of OH concentrations on the modelled CO.


2017 ◽  
Author(s):  
David P. Edwards ◽  
Helen M. Worden ◽  
Doreen Neil ◽  
Gene Francis ◽  
Tim Valle ◽  
...  

Abstract. The CHRONOS space mission concept provides time-resolved abundance for emissions and transport studies of the highly variable and highly uncertain air pollutants carbon monoxide and methane, with sub-hourly revisit rate at fine (~ 4 km) horizontal spatial resolution across a North American domain. CHRONOS can provide complete synoptic air pollution maps (snapshots) of the continental domain with fewer than 10 minutes of observations. This rapid mapping enables visualization of air pollution transport simultaneously across the entire continent and enables a sentinel-like capability for monitoring evolving, or unanticipated, air pollution sources in multiple locations at the same time with high temporal resolution. CHRONOS uses a compact imaging gas filter correlation radiometer for these observations, with heritage from more than 17 years of scientific data and algorithm advances by the science teams for the MOPITT instrument on NASA's Terra spacecraft in low Earth orbit. To achieve continental-scale sub-hourly sampling, the CHRONOS mission would be conducted from geostationary orbit, with the instrument hosted on a communications or meteorological platform. CHRONOS observations would contribute to an integrated observing system for atmospheric composition using surface, suborbital and satellite data with atmospheric chemistry models, as defined by the Committee on Earth Observing Satellites. Addressing the U.S. National Academy's 2007 Decadal Survey direction to characterize diurnal changes in tropospheric composition, CHRONOS observations would find direct societal applications for air quality management and forecasting to protect public health.


2018 ◽  
Vol 11 (2) ◽  
pp. 1061-1085 ◽  
Author(s):  
David P. Edwards ◽  
Helen M. Worden ◽  
Doreen Neil ◽  
Gene Francis ◽  
Tim Valle ◽  
...  

Abstract. The CHRONOS space mission concept provides time-resolved abundance for emissions and transport studies of the highly variable and highly uncertain air pollutants carbon monoxide and methane, with sub-hourly revisit rate at fine (∼ 4 km) horizontal spatial resolution across a North American domain. CHRONOS can provide complete synoptic air pollution maps (snapshots) of the continental domain with less than 10 min of observations. This rapid mapping enables visualization of air pollution transport simultaneously across the entire continent and enables a sentinel-like capability for monitoring evolving, or unanticipated, air pollution sources in multiple locations at the same time with high temporal resolution. CHRONOS uses a compact imaging gas filter correlation radiometer for these observations, with heritage from more than 17 years of scientific data and algorithm advances by the science teams for the Measurements of Pollution in the Troposphere (MOPITT) instrument on NASA's Terra spacecraft in low Earth orbit. To achieve continental-scale sub-hourly sampling, the CHRONOS mission would be conducted from geostationary orbit, with the instrument hosted on a communications or meteorological platform. CHRONOS observations would contribute to an integrated observing system for atmospheric composition using surface, suborbital and satellite data with atmospheric chemistry models, as defined by the Committee on Earth Observing Satellites. Addressing the U.S. National Academy's 2007 decadal survey direction to characterize diurnal changes in tropospheric composition, CHRONOS observations would find direct societal applications for air quality management and forecasting to protect public health.


2020 ◽  
Vol 20 (6) ◽  
pp. 3945-3963
Author(s):  
Frank Roux ◽  
Hannah Clark ◽  
Kuo-Ying Wang ◽  
Susanne Rohs ◽  
Bastien Sauvage ◽  
...  

Abstract. The research infrastructure IAGOS (In-Service Aircraft for a Global Observing System) equips commercial aircraft with instruments to monitor the composition of the atmosphere during flights around the world. In this article, we use data from two China Airlines aircraft based in Taipei (Taiwan) which provided daily measurements of ozone, carbon monoxide and water vapour throughout the summer of 2016. We present time series, from the surface to the upper troposphere, of ozone, carbon monoxide and relative humidity near Taipei, focusing on periods influenced by the passage of typhoons. We examine landing and take-off profiles in the vicinity of tropical cyclones using ERA-5 reanalyses to elucidate the origin of the anomalies in the vertical distribution of these chemical species. Results indicate a high ozone content in the upper- to middle-troposphere track of the storms. The high ozone mixing ratios are generally correlated with potential vorticity and anti-correlated with relative humidity, suggesting stratospheric origin. These results suggest that tropical cyclones participate in transporting air from the stratosphere to troposphere and that such transport could be a regular feature of typhoons. After the typhoons passed Taiwan, the tropospheric column was filled with substantially lower ozone mixing ratios due to the rapid uplift of marine boundary layer air. At the same time, the relative humidity increased, and carbon monoxide mixing ratios fell. Locally, therefore, the passage of typhoons has a positive effect on air quality at the surface, cleansing the atmosphere and reducing the mixing ratios of pollutants such as CO and O3.


2008 ◽  
Vol 8 (20) ◽  
pp. 6037-6050 ◽  
Author(s):  
M. G. Lawrence ◽  
M. Salzmann

Abstract. Global chemistry-transport models (CTMs) and chemistry-GCMs (CGCMs) generally simulate vertical tracer transport by deep convection separately from the advective transport by the mean winds, even though a component of the mean transport, for instance in the Hadley and Walker cells, occurs in deep convective updrafts. This split treatment of vertical transport has various implications for CTM simulations. In particular, it has led to a misinterpretation of several sensitivity simulations in previous studies in which the parameterized convective transport of one or more tracers is neglected. We describe this issue in terms of simulated fluxes and fractions of these fluxes representing various physical and non-physical processes. We then show that there is a significant overlap between the convective and large-scale mean advective vertical air mass fluxes in the CTM MATCH, and discuss the implications which this has for interpreting previous and future sensitivity simulations, as well as briefly noting other related implications such as numerical diffusion.


2021 ◽  
Author(s):  
Tamsin Edwards ◽  

<p><strong>The land ice contribution to global mean sea level rise has not yet been predicted with ice sheet and glacier models for the latest set of socio-economic scenarios (SSPs), nor with coordinated exploration of uncertainties arising from the various computer models involved. Two recent international projects (ISMIP6 and GlacierMIP) generated a large suite of projections using multiple models, but mostly used previous generation scenarios and climate models, and could not fully explore known uncertainties. </strong></p><p><strong>Here we estimate probability distributions for these projections for the SSPs using Gaussian Process emulation of the ice sheet and glacier model ensembles. We model the sea level contribution as a function of global mean surface air temperature forcing and (for the ice sheets) model parameters, with the 'nugget' allowing for multi-model structural uncertainty. Approximate independence of ice sheet and glacier models is assumed, because a given model responds very differently under different setups (such as initialisation). </strong></p><p><strong>We find that limiting global warming to 1.5</strong>°<strong>C </strong><strong>would halve the land ice contribution to 21<sup>st</sup> century </strong><strong>sea level rise</strong><strong>, relative to current emissions pledges: t</strong><strong>he median decreases from 25 to 13 cm sea level equivalent (SLE) by 2100. However, the Antarctic contribution does not show a clear response to emissions scenario, due to competing processes of increasing ice loss and snowfall accumulation in a warming climate. </strong></p><p><strong>However, under risk-averse (pessimistic) assumptions for climate and Antarctic ice sheet model selection and ice sheet model parameter values, Antarctic ice loss could be five times higher, increasing the median land ice contribution to 42 cm SLE under current policies and pledges, with the 95<sup>th</sup> percentile exceeding half a metre even under 1.5</strong>°<strong>C warming. </strong></p><p><strong>Gaussian Process emulation can therefore be a powerful tool for estimating probability density functions from multi-model ensembles and testing the sensitivity of the results to assumptions.</strong></p>


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