scholarly journals Quantifying uncertainties due to chemistry modeling – evaluation of tropospheric composition simulations in the CAMS model

2019 ◽  
Author(s):  
Vincent Huijnen ◽  
Andrea Pozzer ◽  
Joaquim Arteta ◽  
Guy Brasseur ◽  
Idir Bouarar ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Model Uncertainty ◽  
Tropospheric Ozone ◽  
Trace Gas ◽  
Chemical Production ◽  
Chemistry Modeling ◽  
Gas Products ◽  
Forecasting System ◽  
Field Campaigns ◽  
Secondary Chemical

Abstract. We report on an evaluation of tropospheric ozone and its precursor gases in three atmospheric chemistry versions as implemented in ECMWF’s Integrated Forecasting System (IFS), referred to as IFS(CB05BASCOE), IFS(MOZART) and IFS(MOCAGE). While the model versions were forced with the same overall meteorology, emissions, transport and deposition schemes, they vary largely in their parameterizations describing atmospheric chemistry, including the organics degradation, heterogeneous chemistry and photolysis, as well as chemical solver. The model results from the three chemistry versions are compared against a range of aircraft field campaigns, ozone sondes and satellite observations, which provides quantification of the overall model uncertainty driven by the chemistry parameterizations. We find that they produce similar patterns and magnitudes for carbon monoxide (CO) and ozone (O3), as well as a range of non-methane hydrocarbons (NMHCs), with averaged differences for O3 (CO) within 10 % (20 %) throughout the troposphere. Most of the divergence in the magnitude of NMHCs can be explained by differences in OH concentrations, which can reach up to 50 % particularly at high latitudes. Also comparatively large discrepancies between model versions exist for NO2, SO2 and HNO3, which are strongly influenced by secondary chemical production and loss. Other, common biases in CO and NMHCs are mainly attributed to uncertainties in their emissions. This configuration of having various chemistry versions within IFS provides a quantification of uncertainties induced by chemistry modeling in the main CAMS global trace gas products beyond those that are constrained by data-assimilation.

scholarly journals Quantifying uncertainties due to chemistry modelling – evaluation of tropospheric composition simulations in the CAMS model (cycle 43R1)

2019 ◽  
Vol 12 (4) ◽  
pp. 1725-1752 ◽  
Author(s):  
Vincent Huijnen ◽  
Andrea Pozzer ◽  
Joaquim Arteta ◽  
Guy Brasseur ◽  
Idir Bouarar ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Tropospheric Ozone ◽  
Trace Gas ◽  
Chemical Production ◽  
Weather Forecasts ◽  
Medium Range ◽  
Gas Products ◽  
Forecasting System ◽  
Field Campaigns ◽  
Secondary Chemical

Abstract. We report on an evaluation of tropospheric ozone and its precursor gases in three atmospheric chemistry versions as implemented in the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecasting System (IFS), referred to as IFS(CB05BASCOE), IFS(MOZART) and IFS(MOCAGE). While the model versions were forced with the same overall meteorology, emissions, transport and deposition schemes, they vary largely in their parameterisations describing atmospheric chemistry, including the organics degradation, heterogeneous chemistry and photolysis, as well as chemical solver. The model results from the three chemistry versions are compared against a range of aircraft field campaigns, surface observations, ozone-sondes and satellite observations, which provides quantification of the overall model uncertainty driven by the chemistry parameterisations. We find that they produce similar patterns and magnitudes for carbon monoxide (CO) and ozone (O3), as well as a range of non-methane hydrocarbons (NMHCs), with averaged differences for O3 (CO) within 10 % (20 %) throughout the troposphere. Most of the divergence in the magnitude of CO and NMHCs can be explained by differences in OH concentrations, which can reach up to 50 %, particularly at high latitudes. There are also comparatively large discrepancies between model versions for NO2, SO2 and HNO3, which are strongly influenced by secondary chemical production and loss. Other common biases in CO and NMHCs are mainly attributed to uncertainties in their emissions. This configuration of having various chemistry versions within IFS provides a quantification of uncertainties induced by chemistry modelling in the main CAMS global trace gas products beyond those that are constrained by data assimilation.

Unravelling the ozone-weather relationship: the role of vegetation and radical reactions

2021 ◽  
Author(s):  
Tamara Emmerichs ◽  
Bruno Franco ◽  
Catherine Wespes ◽  
Simon Rosanka ◽  
Domenico Taraborrelli
Keyword(s):  
Atmospheric Chemistry ◽  
Tropospheric Ozone ◽  
Surface Ozone ◽  
Air Pollutant ◽  
Tropospheric Chemistry ◽  
Peroxy Radicals ◽  
Chemical Production ◽  
Global Models ◽  
Near Surface

<p>Near-surface ozone is a harmful air pollutant, which is not only controlled by chemical production and loss processes.  The major removal process of near-surface ozone is dry deposition accounting for 20 % of the total tropospheric ozone loss. Due to its significance, parameterizations used in atmospheric chemistry models represent a major source of uncertainty for tropospheric ozone simulations. This uncertainty might be one of the reasons why global models tend to overestimate ozone, when compared to observations. The model used in this study, the global atmospheric model ECHAM5/MESSy (EMAC), is no exception. Like most global models, EMAC employs a “resistances in series” scheme, which is hardly sensitive to local meteorological conditions (e.g. humidity) and lacks non-stomatal deposition. In this study, these missing features have been implemented in EMAC affecting not only the deposition of ozone but also the removal of ozone precursors, resulting in lower chemical production of ozone.</p><p>Furthermore, near-surface ozone may be significantly impacted by water vapour forming complexes with peroxy radicals. The role of water in the reaction of HO<sub>2</sub> radical with itself and nitrogen oxides is known from the literature. However, in current models only the former is considered by assuming a linear dependence on water concentrations. Recent experimental evidence for the significant role of water on the kinetics of one of the most important reaction for ozone chemistry, namely NO<sub>2</sub> + OH, has been published. Here, the available kinetic data for the HO<sub>x</sub> + NO<sub>x</sub> reactions have been critically re-assessed and included in EMAC to test its global significance. Additionally, we considered the representation of isoprene and nitrous acid (HONO) as important oxidants for lower tropospheric chemistry. Namely, for isoprene emissions we added a drought stress factor which enables a higher sensitivity to meteorology leading to reduced emissions. Also, we firstly implemented soil emissions of HONO which is known as a missing source in models. The implications of these modifications on the global tropospheric composition are analysed, focusing on near-surface ozone and related precursors. The improved representation of ozone in EMAC is demonstrated using measurements from the Infrared Atmospheric Sounding Interferometers (IASI), the Tropospheric Ozone Assessment Report (TOAR) database and from the Trajectory-mapped Ozonesonde dataset for the Stratosphere and Troposphere (TOST). The overall changes might help to reduce the uncertainty and overestimation of models predicting near-surface ozone.</p>

scholarly journals The influence of weather-driven processes on tropospheric ozone

2021 ◽  
Author(s):  
Tamara Emmerichs ◽  
Bruno Franco ◽  
Catherine Wespes ◽  
Vinod Kumar ◽  
Andrea Pozzer ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Dry Deposition ◽  
Tropospheric Ozone ◽  
Surface Ozone ◽  
Air Pollutant ◽  
Chemical Production ◽  
Ozone Monitoring Instrument ◽  
Near Surface ◽  
The Impact

Abstract. Near-surface ozone is an harmful air pollutant, which is determined to a considerable extent by weather-controlled processes, and may be significantly impacted by water vapour forming complexes with peroxy radicals. The role of water in the reaction of HO2 radical with nitrogen oxides is known from the literature, and in current models the water complex is considered by assuming a linear dependence on water concentrations. In fact, recent experimental evidence has been published, showing the significant role of water on the kinetics of one of the most important reaction for ozone chemistry, namely NO2 + OH. Here, the available kinetic data for the HOx + NOx reactions have been included in the atmospheric chemistry model ECHAM5/MESSy (EMAC) to test its global significance. Among the modified kinetics, the newly added HNO3 channel from HO2 + NO, dominates, significantly reducing NO2. A major removal process of near-surface ozone is dry deposition accounting for 20 % of the total tropospheric ozone loss mostly occurring over vegetation. However, parameterizations for modelling dry deposition represent a major source of uncertainty for tropospheric ozone simulations. This potentially belongs to the reasons why global models, such as EMAC used here, overestimate ozone with respect to observations. In fact, the employed parameterization is hardly sensitive to local meteorological conditions (e.g., humidity) and lacks non-stomatal deposition. In this study, a dry deposition scheme including these features have been used in EMAC, affecting not only the deposition of ozone but of its precursors, resulting in lower chemical production of ozone. Additionally, we improved the emissions of isoprene and nitrous acid (HONO). Namely, for isoprene emissions we have accounted for the impact of drought stress which confers a higher model sensitivity to meteorology leading to reduced annual emissions down to 32 %. For HONO, we have implemented soil emissions, which depend on soil moisture and thus on precipitation. We estimate for the first time a global source strength of 7 Tg(N) a−1. Furthermore, the usage of a parameterization for the production of lightning NOx that depends on cloud top height contributes to a more realistic representation of NO2 columns over remote oceans with respect to the satellite measurements of the Ozone Monitoring Instrument (OMI). The combination of all the model modifications reduces the simulated global ozone burden by ≈ 20 % to 337 Tg, which is in better agreement with recent estimates. By comparing simulation results with measurements from the Infrared Atmospheric Sounding Interferometer (IASI) and the Tropospheric Ozone Assessment Report (TOAR) databases (of 2009) we demonstrate an overall reduction of the ozone bias by a factor of 2.

scholarly journals Tropospheric ozone in CMIP6 simulations

2021 ◽  
Vol 21 (5) ◽  
pp. 4187-4218
Author(s):  
Paul T. Griffiths ◽  
Lee T. Murray ◽  
Guang Zeng ◽  
Youngsub Matthew Shin ◽  
N. Luke Abraham ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Tropospheric Ozone ◽  
Climate Models ◽  
Climate Model ◽  
Decadal Variability ◽  
Stratospheric Ozone ◽  
Ozone Production ◽  
Model Intercomparison ◽  
Chemical Production ◽  
Intercomparison Project

Abstract. The evolution of tropospheric ozone from 1850 to 2100 has been studied using data from Phase 6 of the Coupled Model Intercomparison Project (CMIP6). We evaluate long-term changes using coupled atmosphere–ocean chemistry–climate models, focusing on the CMIP Historical and ScenarioMIP ssp370 experiments, for which detailed tropospheric-ozone diagnostics were archived. The model ensemble has been evaluated against a suite of surface, sonde and satellite observations of the past several decades and found to reproduce well the salient spatial, seasonal and decadal variability and trends. The multi-model mean tropospheric-ozone burden increases from 247 ± 36 Tg in 1850 to a mean value of 356 ± 31 Tg for the period 2005–2014, an increase of 44 %. Modelled present-day values agree well with previous determinations (ACCENT: 336 ± 27 Tg; Atmospheric Chemistry and Climate Model Intercomparison Project, ACCMIP: 337 ± 23 Tg; Tropospheric Ozone Assessment Report, TOAR: 340 ± 34 Tg). In the ssp370 experiments, the ozone burden increases to 416 ± 35 Tg by 2100. The ozone budget has been examined over the same period using lumped ozone production (PO3) and loss (LO3) diagnostics. Both ozone production and chemical loss terms increase steadily over the period 1850 to 2100, with net chemical production (PO3-LO3) reaching a maximum around the year 2000. The residual term, which contains contributions from stratosphere–troposphere transport reaches a minimum around the same time before recovering in the 21st century, while dry deposition increases steadily over the period 1850–2100. Differences between the model residual terms are explained in terms of variation in tropopause height and stratospheric ozone burden.

Recent updates to the atmospheric chemistry modeling of the ECMWF IFS in support to CAMS

2021 ◽  
Author(s):  
Vincent Huijnen ◽  
Jason Williams ◽  
Idir Bouarar ◽  
Sophie Belamari ◽  
Simon Chabrillat ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Stratospheric Ozone ◽  
Tropospheric Chemistry ◽  
Atmospheric Composition ◽  
Aerosol Formation ◽  
Chemistry Modeling ◽  
Forecasting System ◽  
Isoprene Oxidation ◽  
Reactive Gases ◽  
Monitoring Service

<p>The Integrated Forecasting System (IFS) of ECMWF is the core of the Copernicus Atmosphere Monitoring Service (CAMS) which provides global analyses and forecasts of atmospheric composition, namely reactive gases, aerosol and greenhouse gases. With respect to the atmospheric chemistry component, the operational system currently relies on a modified version of the CB05 chemistry scheme for the troposphere, combined with the Cariolle scheme to describe stratospheric ozone. In an alternative, more recent configuration also stratospheric ozone chemistry is included based on the BASCOE chemistry module. Alternative atmospheric chemistry modules which can be employed are based on MOZART and MOCAGE chemistry. <br>Recently, further revisions to the modified CB05 tropospheric chemistry scheme have been developed, focusing both on inorganic and organic chemistry, with the aim of improving the quality of existing air-quality products, and the development of new products. On major update is a revision of the isoprene oxidation scheme based on those employed in existing chemistry transport models, as well as inclusion of the basic chemistry describing C8 and C9 aromatics degradation. <br>An example of a new product derived from these updates include a description of global distribution of glyoxal, while this also resulted in an improved modeling of OH recycling particularly over tropical forests. Also we support improved secondary organic aerosol formation due to gaseous anthropogenic, biogenic and biomass burning sources.<br>In this contribution we provide an overview of these revisions, and provide a first quantification of their uncertainties, by comparing products to observations and to those from alternative chemistry modules.</p>

scholarly journals Tropospheric Ozone Assessment Report

Elem Sci Anth ◽  
2020 ◽  
Vol 8 (1) ◽  
Author(s):  
A. T. Archibald ◽  
J. L. Neu ◽  
Y. F. Elshorbany ◽  
O. R. Cooper ◽  
P. J. Young ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Tropospheric Ozone ◽  
Climate Model ◽  
Ozone Production ◽  
Climate Modelling ◽  
Model Intercomparison ◽  
Chemical Production ◽  
Intercomparison Project ◽  
Near Term ◽  
Review Model

Our understanding of the processes that control the burden and budget of tropospheric ozone has changed dramatically over the last 60 years. Models are the key tools used to understand these changes, and these underscore that there are many processes important in controlling the tropospheric ozone budget. In this critical review, we assess our evolving understanding of these processes, both physical and chemical. We review model simulations from the International Global Atmospheric Chemistry Atmospheric Chemistry and Climate Model Intercomparison Project and Chemistry Climate Modelling Initiative to assess the changes in the tropospheric ozone burden and its budget from 1850 to 2010. Analysis of these data indicates that there has been significant growth in the ozone burden from 1850 to 2000 (approximately 43 ± 9%) but smaller growth between 1960 and 2000 (approximately 16 ± 10%) and that the models simulate burdens of ozone well within recent satellite estimates. The Chemistry Climate Modelling Initiative model ozone budgets indicate that the net chemical production of ozone in the troposphere plateaued in the 1990s and has not changed since then inspite of increases in the burden. There has been a shift in net ozone production in the troposphere being greatest in the northern mid and high latitudes to the northern tropics, driven by the regional evolution of precursor emissions. An analysis of the evolution of tropospheric ozone through the 21st century, as simulated by Climate Model Intercomparison Project Phase 5 models, reveals a large source of uncertainty associated with models themselves (i.e., in the way that they simulate the chemical and physical processes that control tropospheric ozone). This structural uncertainty is greatest in the near term (two to three decades), but emissions scenarios dominate uncertainty in the longer term (2050–2100) evolution of tropospheric ozone. This intrinsic model uncertainty prevents robust predictions of near-term changes in the tropospheric ozone burden, and we review how progress can be made to reduce this limitation.

scholarly journals Drivers of changes in stratospheric and tropospheric ozone between year 2000 and 2100

2016 ◽  
Vol 16 (5) ◽  
pp. 2727-2746 ◽  
Author(s):  
Antara Banerjee ◽  
Amanda C. Maycock ◽  
Alexander T. Archibald ◽  
N. Luke Abraham ◽  
Paul Telford ◽  
...  
Keyword(s):  
Climate Change ◽  
Greenhouse Gases ◽  
Tropospheric Ozone ◽  
Climate Forcing ◽  
Atmospheric Response ◽  
Chemical Production ◽  
The United Kingdom ◽  
Ozone Precursor ◽  
Ozone Depleting Substances ◽  
Year 2000

Abstract. A stratosphere-resolving configuration of the Met Office's Unified Model (UM) with the United Kingdom Chemistry and Aerosols (UKCA) scheme is used to investigate the atmospheric response to changes in (a) greenhouse gases and climate, (b) ozone-depleting substances (ODSs) and (c) non-methane ozone precursor emissions. A suite of time-slice experiments show the separate, as well as pairwise, impacts of these perturbations between the years 2000 and 2100. Sensitivity to uncertainties in future greenhouse gases and aerosols is explored through the use of the Representative Concentration Pathway (RCP) 4.5 and 8.5 scenarios. The results highlight an important role for the stratosphere in determining the annual mean tropospheric ozone response, primarily through stratosphere–troposphere exchange (STE) of ozone. Under both climate change and reductions in ODSs, increases in STE offset decreases in net chemical production and act to increase the tropospheric ozone burden. This opposes the effects of projected decreases in ozone precursors through measures to improve air quality, which act to reduce the ozone burden. The global tropospheric lifetime of ozone (τO3) does not change significantly under climate change at RCP4.5, but it decreases at RCP8.5. This opposes the increases in τO3 simulated under reductions in ODSs and ozone precursor emissions. The additivity of the changes in ozone is examined by comparing the sum of the responses in the single-forcing experiments to those from equivalent combined-forcing experiments. Whilst the ozone responses to most forcing combinations are found to be approximately additive, non-additive changes are found in both the stratosphere and troposphere when a large climate forcing (RCP8.5) is combined with the effects of ODSs.

scholarly journals Impact of uncertainties in inorganic chemical rate constants on tropospheric composition and ozone radiative forcing

2017 ◽  
Author(s):  
Ben Newsome ◽  
Mat Evans
Keyword(s):  
Rate Constant ◽  
Atmospheric Chemistry ◽  
Rate Constants ◽  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Transport Model ◽  
Surface Ozone ◽  
Photolysis Rates ◽  
The Impact ◽  
Chemical Rate

Abstract. Chemical rate constants determine the composition of the atmosphere and how this composition has changed over time. They are central to our understanding of climate change and air quality degradation. Atmospheric chemistry models, whether online or offline, box, regional or global use these rate constants. Expert panels synthesise laboratory measurements, making recommendations for the rate constants that should be used. This results in very similar or identical rate constants being used by all models. The inherent uncertainties in these recommendations are, in general, therefore ignored. We explore the impact of these uncertainties on the composition of the troposphere using the GEOS-Chem chemistry transport model. Based on the JPL and IUPAC evaluations we assess 50 mainly inorganic rate constants and 10 photolysis rates, through simulations where we increase the rate of the reactions to the 1σ upper value recommended by the expert panels. We assess the impact on 4 standard metrics: annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime. Uncertainty in the rate constants for NO2 + OH    M →  HNO3, OH + CH4 → CH3O2 + H2O and O3 + NO → NO2 + O2 are the three largest source of uncertainty in these metrics. We investigate two methods of assessing these uncertainties, addition in quadrature and a Monte Carlo approach, and conclude they give similar outcomes. Combining the uncertainties across the 60 reactions, gives overall uncertainties on the annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime of 11, 12, 17 and 17 % respectively. These are larger than the spread between models in recent model inter-comparisons. Remote regions such as the tropics, poles, and upper troposphere are most uncertain. This chemical uncertainty is sufficiently large to suggest that rate constant uncertainty should be considered when model results disagree with measurement. Calculations for the pre-industrial allow a tropospheric ozone radiative forcing to be calculated of 0.412 ± 0.062 Wm−2. This uncertainty (15 %) is comparable to the inter-model spread in ozone radiative forcing found in previous model-model inter-comparison studies where the rate constants used in the models are all identical or very similar. Thus the uncertainty of tropospheric ozone radiative forcing should expanded to include this additional source of uncertainty. These rate constant uncertainties are significant and suggest that refinement of supposedly well known chemical rate constants should be considered alongside other improvements to enhance our understanding of atmospheric processes.

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