Multi-model study of mercury dispersion in the atmosphere: vertical and interhemispheric distribution of mercury species

Abstract. Atmospheric chemistry and transport of mercury play a key role in the global mercury cycle. However, there are still considerable knowledge gaps concerning the fate of mercury in the atmosphere. This is the second part of a model intercomparison study investigating the impact of atmospheric chemistry and emissions on mercury in the atmosphere. While the first study focused on ground-based observations of mercury concentration and deposition, here we investigate the vertical and interhemispheric distribution and speciation of mercury from the planetary boundary layer to the lower stratosphere. So far, there have been few model studies investigating the vertical distribution of mercury, mostly focusing on single aircraft campaigns. Here, we present a first comprehensive analysis based on various aircraft observations in Europe, North America, and on intercontinental flights. The investigated models proved to be able to reproduce the distribution of total and elemental mercury concentrations in the troposphere including interhemispheric trends. One key aspect of the study is the investigation of mercury oxidation in the troposphere. We found that different chemistry schemes were better at reproducing observed oxidized mercury patterns depending on altitude. High concentrations of oxidized mercury in the upper troposphere could be reproduced with oxidation by bromine while elevated concentrations in the lower troposphere were better reproduced by OH and ozone chemistry. However, the results were not always conclusive as the physical and chemical parameterizations in the chemistry transport models also proved to have a substantial impact on model results.

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Multi-model study of mercury dispersion in the atmosphere: Vertical distribution of mercury species

10.5194/acp-2016-1074 ◽

2016 ◽

Cited By ~ 2

Author(s):

Johannes Bieser ◽

Franz Slemr ◽

Jesse Ambrose ◽

Carl Brenninkmeijer ◽

Steve Brooks ◽

...

Keyword(s):

Vertical Distribution ◽

Atmospheric Chemistry ◽

Lower Troposphere ◽

Elemental Mercury ◽

Mercury Species ◽

Substantial Impact ◽

Model Studies ◽

Model Study ◽

The Impact ◽

The Vertical Distribution

Abstract. Atmospheric chemistry and transport of mercury play a key role in the global mercury cycle. However, there are still considerable knowledge gaps concerning the fate of mercury in the atmosphere. This is the second part of a model inter-comparison study investigating the impact of atmospheric chemistry and emissions on mercury in the atmosphere. While the first study focused on ground based observations of mercury concentration and deposition, here we investigate the vertical distribution and speciation of mercury from the planetary boundary layer to the lower stratosphere. So far, there have been few model studies investigating the vertical distribution of mercury, mostly focusing on single aircraft campaigns. Here, we present a first comprehensive analysis based on various aircraft observations in Europe, North America, and on inter-continental flights. The investigated models proved to be able to reproduce the distribution of total and elemental mercury concentrations in the troposphere including inter-hemispheric trends. One key aspect of the study is the investigation of mercury oxidation in the troposphere. We found that different chemistry schemes were better at reproducing observed oxidized mercury (RM) patterns depending on altitude. High RM concentrations in the upper troposphere could be reproduced with oxidation by bromine while elevated concentrations in the lower troposphere were better reproduced by OH and ozone chemistry. However, the results were not always conclusive as the physical and chemical parametrizations in the chemistry transport models also proved to have a substantial impact on model results.

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Atmospheric impacts of short-lived chlorinated species over the recent past: a chemistry-climate perspective

10.5194/egusphere-egu21-12824 ◽

2021 ◽

Author(s):

Ewa Bednarz ◽

Ryan Hossaini ◽

Luke Abraham ◽

Peter Braesicke ◽

Martyn Chipperfield

Keyword(s):

Atmospheric Chemistry ◽

Climate Model ◽

Stratospheric Ozone ◽

Lower Boundary ◽

Montreal Protocol ◽

Recent Past ◽

Substantial Impact ◽

Ozone Depleting Substances ◽

The Impact

The emissions of most long-lived halogenated ozone-depleting substances (ODSs) are now decreasing, owing to controls on their production introduced by Montreal Protocol and its amendments. However, short-lived halogenated compounds can also have substantial impact on atmospheric chemistry, including stratospheric ozone, particularly if emitted near climatological uplift regions. It has recently become evident that emissions of some chlorinated very short-lived species (VSLSs), such as chloroform (CHCl3) and dichloromethane (CH2Cl2), could be larger than previously believed and increasing, particularly in Asia. While these may exert a significant influence on atmospheric chemistry and climate, their impacts remain poorly characterised.&#160;&#160;We address this issue using the UM-UKCA chemistry-climate model (CCM). While not only the first, to our knowledge, model study addressing this problem using a CCM, it is also the first such study employing a whole atmosphere model, thereby simulating the tropospheric Cl-VSLSs emissions and the resulting stratospheric impacts in a fully consistent manner. We use a newly developed Double-Extended Stratospheric-Tropospheric (DEST) chemistry scheme, which includes emissions of all major chlorinated and brominated VSLSs alongside an extended treatment of long-lived ODSs.&#160;We examine the impacts of rising Cl-VSLSs emissions on atmospheric chlorine tracers and ozone, including their long-term trends. We pay particular attention to the role of &#8216;nudging&#8217;, as opposed to the free-running model set up, for the simulated Cl-VSLSs impacts, thereby demostrating the role of atmospheric dynamics in modulating the atmospheric responses to Cl-VSLSs. In addition, we employ novel estimates of Cl-VSLS emissions over the recent past and compare the results with the simulations that prescribe Cl-VSLSs using simple lower boundary conditions. This allows us to demonstrate the impact such choice has on the dominant location and seasonality of the Cl-VSLSs transport into the stratosphere.

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On the impact of future climate change on tropopause folds and tropospheric ozone

Atmospheric Chemistry and Physics ◽

10.5194/acp-19-14387-2019 ◽

2019 ◽

Vol 19 (22) ◽

pp. 14387-14401 ◽

Cited By ~ 2

Author(s):

Dimitris Akritidis ◽

Andrea Pozzer ◽

Prodromos Zanis

Keyword(s):

Atmospheric Chemistry ◽

Tropospheric Ozone ◽

Eastern Mediterranean ◽

Stratospheric Ozone ◽

Lower Troposphere ◽

Future Climate Change ◽

Identification Algorithm ◽

The Future ◽

Projected Changes ◽

The Impact

Abstract. Using a transient simulation for the period 1960–2100 with the state-of-the-art ECHAM5/MESSy Atmospheric Chemistry (EMAC) global model and a tropopause fold identification algorithm, we explore the future projected changes in tropopause folds, stratosphere-to-troposphere transport (STT) of ozone, and tropospheric ozone under the RCP6.0 scenario. Statistically significant changes in tropopause fold frequencies from 1970–1999 to 2070–2099 are identified in both hemispheres, regionally exceeding 3 %, and are associated with the projected changes in the position and intensity of the subtropical jet streams. A strengthening of ozone STT is projected for the future in both hemispheres, with an induced increase in transported stratospheric ozone tracer throughout the whole troposphere, reaching up to 10 nmol mol−1 in the upper troposphere, 8 nmol mol−1 in the middle troposphere, and 3 nmol mol−1 near the surface. Notably, the regions exhibiting the largest changes of ozone STT at 400 hPa coincide with those with the highest fold frequency changes, highlighting the role of the tropopause folding mechanism in STT processes under a changing climate. For both the eastern Mediterranean and Middle East (EMME) and Afghanistan (AFG) regions, which are known as hotspots of fold activity and ozone STT during the summer period, the year-to-year variability of middle-tropospheric ozone with stratospheric origin is largely explained by the short-term variations in ozone at 150 hPa and tropopause fold frequency. Finally, ozone in the lower troposphere is projected to decrease under the RCP6.0 scenario during MAM (March, April, and May) and JJA (June, July, and August) in the Northern Hemisphere and during DJF (December, January, and February) in the Southern Hemisphere, due to the decline of ozone precursor emissions and the enhanced ozone loss from higher water vapour abundances, while in the rest of the troposphere ozone shows a remarkable increase owing mainly to the STT strengthening and the stratospheric ozone recovery.

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The impact of traffic emissions on atmospheric ozone and OH: results from QUANTIFY

Atmospheric Chemistry and Physics ◽

10.5194/acp-9-3113-2009 ◽

2009 ◽

Vol 9 (9) ◽

pp. 3113-3136 ◽

Cited By ~ 116

Author(s):

P. Hoor ◽

J. Borken-Kleefeld ◽

D. Caro ◽

O. Dessens ◽

O. Endresen ◽

...

Keyword(s):

Atmospheric Chemistry ◽

Lower Troposphere ◽

Local Maximum ◽

Traffic Emissions ◽

Transport Sector ◽

Maximum Effect ◽

Ship Emissions ◽

Emission Data ◽

Global Emission ◽

The Impact

Abstract. To estimate the impact of emissions by road, aircraft and ship traffic on ozone and OH in the present-day atmosphere six different atmospheric chemistry models have been used. Based on newly developed global emission inventories for road, ship and aircraft emission data sets each model performed sensitivity simulations reducing the emissions of each transport sector by 5%. The model results indicate that on global annual average lower tropospheric ozone responds most sensitive to ship emissions (50.6%±10.9% of the total traffic induced perturbation), followed by road (36.7%±9.3%) and aircraft exhausts (12.7%±2.9%), respectively. In the northern upper troposphere between 200–300 hPa at 30–60° N the maximum impact from road and ship are 93% and 73% of the maximum effect of aircraft, respectively. The latter is 0.185 ppbv for ozone (for the 5% case) or 3.69 ppbv when scaling to 100%. On the global average the impact of road even dominates in the UTLS-region. The sensitivity of ozone formation per NOx molecule emitted is highest for aircraft exhausts. The local maximum effect of the summed traffic emissions on the ozone column predicted by the models is 0.2 DU and occurs over the northern subtropical Atlantic extending to central Europe. Below 800 hPa both ozone and OH respond most sensitively to ship emissions in the marine lower troposphere over the Atlantic. Based on the 5% perturbation the effect on ozone can exceed 0.6% close to the marine surface (global zonal mean) which is 80% of the total traffic induced ozone perturbation. In the southern hemisphere ship emissions contribute relatively strongly to the total ozone perturbation by 60%–80% throughout the year. Methane lifetime changes against OH are affected strongest by ship emissions up to 0.21 (± 0.05)%, followed by road (0.08 (±0.01)%) and air traffic (0.05 (± 0.02)%). Based on the full scale ozone and methane perturbations positive radiative forcings were calculated for road emissions (7.3±6.2 mWm−2) and for aviation (2.9±2.3 mWm−2). Ship induced methane lifetime changes dominate over the ozone forcing and therefore lead to a net negative forcing (−25.5±13.2 mWm−2).

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Finite element analysis of the impact of the properties of dental wedge materials on functional features

Archives of Materials Science and Engineering ◽

10.5604/01.3001.0015.5930 ◽

2021 ◽

Vol 112 (1) ◽

pp. 32-41

Author(s):

M. Czerwiński ◽

J. Żmudzki ◽

K. Kwieciński ◽

M. Kowalczyk

Keyword(s):

Finite Element Analysis ◽

Finite Element ◽

High Plasticity ◽

Element Analysis ◽

Expanded Polytetrafluoroethylene ◽

Model Studies ◽

Model Study ◽

The Matrix ◽

Functional Features ◽

The Impact

Purpose: Defect of the interproximal wall of the tooth is filled with use the shaped matrix and wedge which seals bottom margin during filling. Better fit of the wedge and equalization of the pressure forces on the matrix is achieved by the compliance of the wedge structure through cuts and perforations and the use of silicone materials and unidirectionally expanded polytetrafluoroethylene (ePTFE). The work presents a methodology for model studies of the mechanics of dental wedges in order to evaluate and compare the impact of wedge materials on functional features. The hypothesis of the work was that the mechanical properties of ePTFE determine the effectiveness of the dental wedge. Design/methodology/approach: Effect of modulus of elasticity and friction coefficient of wedge and matrix materials on the functional features of the wedge was studied on the way Finite Element Analysis (FEA). Simulation included contact sliding between wedge and matrix what was simulated in nonlinear large displacements regime. The sealing evaluation criterion was the pressure distribution between the wedge and matrix below the lower edge of the defect. Displacement values were the criterion for the loss of convexity as a result of matrix deformation. Findings: The material for the wedge should be characterized by a low coefficient of friction, low elasticity (ensuring high compliance of the wedge) and at the same time the ability to large permanent deformations, which allows for plastic shaping of the matrix from the side of the defect in order to achieve the required wall convexity and the tangent point. Research limitations/implications: Results show tendency of phenomena in limitation to model simplification of the interdental gap and the ideal adhesion of the matrix to the tooth and linear elasticity of materials. Practical implications: The material that best meets the requirements is unidirectionally expanded polytetrafluoroethylene, which has one of the lowest coefficients of friction and very high plasticity necessary to shape the matrix from the inside of the cavity. Originality/value: Methodology of model study and criteria of functional characteristics of dental wedge was presented.

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Future impact of traffic emissions on atmospheric ozone and OH based on two scenarios

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-12-20975-2012 ◽

2012 ◽

Vol 12 (8) ◽

pp. 20975-21012

Author(s):

Ø. Hodnebrog ◽

T. K. Berntsen ◽

O. Dessens ◽

M. Gauss ◽

V. Grewe ◽

...

Keyword(s):

Atmospheric Chemistry ◽

Radiative Forcing ◽

Road Traffic ◽

North Atlantic Ocean ◽

Lower Troposphere ◽

Traffic Emissions ◽

Transport Sector ◽

Atmospheric Ozone ◽

The Future ◽

The Impact

Abstract. The future impact of traffic emissions on atmospheric ozone and OH has been investigated separately for the three sectors AIRcraft, maritime SHIPping and ROAD traffic. To reduce uncertainties we present results from an ensemble of six different atmospheric chemistry models, each simulating the atmospheric chemical composition in a possible high emission scenario (A1B), and with emissions from each transport sector reduced by 5% to estimate sensitivities. Our results are compared with optimistic future emission scenarios (B1 and B1 ACARE), presented in a companion paper, and with the recent past (year 2000). Present-day activity indicates that anthropogenic emissions so far evolve closer to A1B than the B1 scenario. As a response to expected changes in emissions, AIR and SHIP will have increased impacts on atmospheric O3 and OH in the future while the impact of ROAD traffic will decrease substantially as a result of technological improvements. In 2050, maximum aircraft-induced O3 occurs near 80° N in the UTLS region and could reach 9 ppbv in the zonal mean during summer. Emissions from ship traffic have their largest O3 impact in the maritime boundary layer with a maximum of 6 ppbv over the North Atlantic Ocean during summer in 2050. The O3 impact of road traffic emissions in the lower troposphere peaks at 3 ppbv over the Arabian Peninsula, much lower than the impact in 2000. Radiative Forcing (RF) calculations show that the net effect of AIR, SHIP and ROAD combined will change from a~marginal cooling of −0.38 ± 13 mW m−2 in 2000 to a relatively strong cooling of −32 ± 8.9 (B1) or −31 ± 20 mW m−2 (A1B) in 2050, when taking into account RF due to changes in O3, CH4 and CH4-induced O3. This is caused both by the enhanced negative net RF from SHIP, which will change from −20 ± 5.4 mW m−2 in 2000 to −31 ± 4.8 (B1) or −40 ± 11 mW m−2 (A1B) in 2050, and from reduced O3 warming from ROAD, which is likely to turn from a positive net RF of 13 ± 7.9 mW m−2 in 2000 to a slightly negative net RF of −2.9 ± 1.7 (B1) or −3.3 ± 3.8 (A1B) mW m−2 in the middle of this century. The negative net RF from ROAD is temporary and induced by the strong decline in ROAD emissions prior to 2050, which only affects the methane cooling term due to the longer lifetime of CH4 compared to O3. The O3 RF from AIR in 2050 is strongly dependent on scenario and ranges from 19 ± 6.8 (B1 ACARE) to 62 ± 13.6 mW m−2 (A1B). There is also a considerable span in the net RF from AIR in 2050, ranging from −0.54 ± 4.6 (B1 ACARE) to 12 ± 11 (A1B) mW m−2 compared to 6.5 ± 2.1 mW m−2 in 2000.

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Improved characterisation of the impact of chlorinated VSLSs on atmospheric chemistry and climate: past, present and future

10.5194/egusphere-egu2020-10611 ◽

2020 ◽

Author(s):

Ewa Bednarz ◽

Ryan Hossaini ◽

Luke Abraham ◽

Martyn Chipperfield

Keyword(s):

Atmospheric Chemistry ◽

Climate Model ◽

Stratospheric Ozone ◽

Montreal Protocol ◽

Recent Past ◽

Substantial Impact ◽

Emissions Scenarios ◽

Ozone Depleting Substances ◽

The Impact ◽

Future Emissions

The emissions of most long-lived halogenated ozone-depleting substances (ODSs) are now decreasing, owing to controls on their production introduced by Montreal Protocol and its amendments. However, short-lived halogenated compounds can also have substantial impact on atmospheric chemistry, including stratospheric ozone, particularly if emitted near climatological uplift regions. It has recently become evident that emissions of some chlorinated very short-lived species (VSLSs), such as chloroform (CHCl3) and dichloromethane (CH2Cl2), could be larger than previously believed and increasing, particularly in Asia. While these may exert a significant influence on atmospheric chemistry and climate, their impacts remain poorly characterised.&#160;We address this issue using the UM-UKCA chemistry-climate model. We use a newly developed Double-Extended Stratospheric-Tropospheric (DEST) chemistry scheme, which includes emissions of all major chlorinated and brominated VSLSs alongside an extended treatment of long-lived ODSs. Employing novel estimates of Cl-VSLS emissions we show model results regarding the atmospheric impacts of chlorinated VSLSs over the recent past (2000-present), with a focus on stratospheric ozone and HCl trends. Finally, we introduce our plans regarding examining the impacts of chlorinated VSLSs under a range of potential future emissions scenarios; the results of which will be directly relevant for the next WMO/UNEP assessment.

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Future impact of traffic emissions on atmospheric ozone and OH based on two scenarios

Atmospheric Chemistry and Physics ◽

10.5194/acp-12-12211-2012 ◽

2012 ◽

Vol 12 (24) ◽

pp. 12211-12225 ◽

Cited By ~ 10

Author(s):

Ø. Hodnebrog ◽

T. K. Berntsen ◽

O. Dessens ◽

M. Gauss ◽

V. Grewe ◽

...

Keyword(s):

Atmospheric Chemistry ◽

Radiative Forcing ◽

Road Traffic ◽

North Atlantic Ocean ◽

Lower Troposphere ◽

Traffic Emissions ◽

Transport Sector ◽

Atmospheric Ozone ◽

The Future ◽

The Impact

Abstract. The future impact of traffic emissions on atmospheric ozone and OH has been investigated separately for the three sectors AIRcraft, maritime SHIPping and ROAD traffic. To reduce uncertainties we present results from an ensemble of six different atmospheric chemistry models, each simulating the atmospheric chemical composition in a possible high emission scenario (A1B), and with emissions from each transport sector reduced by 5% to estimate sensitivities. Our results are compared with optimistic future emission scenarios (B1 and B1 ACARE), presented in a companion paper, and with the recent past (year 2000). Present-day activity indicates that anthropogenic emissions so far evolve closer to A1B than the B1 scenario. As a response to expected changes in emissions, AIR and SHIP will have increased impacts on atmospheric O3 and OH in the future while the impact of ROAD traffic will decrease substantially as a result of technological improvements. In 2050, maximum aircraft-induced O3 occurs near 80° N in the UTLS region and could reach 9 ppbv in the zonal mean during summer. Emissions from ship traffic have their largest O3 impact in the maritime boundary layer with a maximum of 6 ppbv over the North Atlantic Ocean during summer in 2050. The O3 impact of road traffic emissions in the lower troposphere peaks at 3 ppbv over the Arabian Peninsula, much lower than the impact in 2000. Radiative forcing (RF) calculations show that the net effect of AIR, SHIP and ROAD combined will change from a marginal cooling of −0.44 ± 13 mW m−2 in 2000 to a relatively strong cooling of −32 ± 9.3 (B1) or −32 ± 18 mW m−2 (A1B) in 2050, when taking into account RF due to changes in O3, CH4 and CH4-induced O3. This is caused both by the enhanced negative net RF from SHIP, which will change from −19 ± 5.3 mW m−2 in 2000 to −31 ± 4.8 (B1) or −40 ± 9 mW m−2 (A1B) in 2050, and from reduced O3 warming from ROAD, which is likely to turn from a positive net RF of 12 ± 8.5 mW m−2 in 2000 to a slightly negative net RF of −3.1 ± 2.2 (B1) or −3.1 ± 3.4 (A1B) mW m−2 in the middle of this century. The negative net RF from ROAD is temporary and induced by the strong decline in ROAD emissions prior to 2050, which only affects the methane cooling term due to the longer lifetime of CH4 compared to O3. The O3 RF from AIR in 2050 is strongly dependent on scenario and ranges from 19 ± 6.8 (B1 ACARE) to 61 ± 14 mW m−2 (A1B). There is also a considerable span in the net RF from AIR in 2050, ranging from −0.54 ± 4.6 (B1 ACARE) to 12 ± 11 (A1B) mW m−2 compared to 6.6 ± 2.2 mW m−2 in 2000.

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Organic pollutants from Indonesian peatland fires: regional influences and its impact on lower the stratospheric composition

10.5194/egusphere-egu21-10203 ◽

2021 ◽

Author(s):

Simon Rosanka ◽

Bruno Franco ◽

Lieven Clarisse ◽

Pierre-François Coheur ◽

Andreas Wahner ◽

...

Keyword(s):

Biomass Burning ◽

Lower Troposphere ◽

Atmospheric Model ◽

Chemical Production ◽

Global Atmospheric Model ◽

Reservoir Species ◽

Upward Transport ◽

High Concentrations ◽

Stratospheric Composition ◽

The Impact

In 2015, the particularly strong dry season in Indonesia, caused by an exceptional strong El Ni&#241;o, led to severe peatland fires. Due to the high carbon content of peatland, these fires are characterised by high volatile organic compound (VOC) biomass burning emissions. The resulting primary and secondary pollutants are efficiently transported to the upper troposphere/lower stratosphere (UTLS) by the developing Asian monsoon anticyclone (ASMA) and the general upward transport in the intertropical convergence zone (ITCZ). In this study, we assess the importance of these VOC emissions for the composition of the lower troposphere and the UTLS by performing multiple chemistry simulations using the global atmospheric model ECHAM/MESSy (EMAC). In a first step, we find that EMAC properly captures the exceptional strength of the Indonesian fires based on the comparison of modelled columns of the biomass burning marker hydrogen cyanide (HCN) to spaceborne measurements from the Infrared Atmospheric Sounding Interferometer (IASI). In the lower troposphere, the increase in VOC levels is higher in Indonesia compared to other biomass burning regions. This directly impacts the oxidation capacity and leads to a high reduction in hydroxyl radicals (OH) and nitrogen oxides (NOx). In general, an increase in ozone (O3) is predicted close to the peatland fires. However, particular high concentrations of phenols lead to an O3 depletion in eastern Indonesia. By employing the detailed in-cloud OVOC oxidation scheme J&#252;lich Aqueous-phase Mechanism of Organic Chemistry (JAMOC), we find that the predicted changes are dampened and that by ignoring these processes, global models tend to overestimate the impact of such extreme pollution events. The upward transport in the ASMA and the ITCZ leads to elevated VOC concentrations in the UTLS region. This also results in a depletion of lower stratospheric O3. We find that this is caused by a high destruction of O3 by phenoxy radicals and by the increased formation of NOx reservoir species, which dampen the chemical production of O3.

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Sensitivity of tropospheric ozone to halogen chemistry in the chemistry-climate model LMDZ-INCA vNMHC

10.5194/gmd-2021-388 ◽

2021 ◽

Author(s):

Cyril Caram ◽

Sophie Szopa ◽

Anne Cozic ◽

Slimane Bekki ◽

Carlos Cuevas ◽

...

Keyword(s):

Atmospheric Chemistry ◽

Tropospheric Ozone ◽

Climate Models ◽

Marine Boundary Layer ◽

Climate Model ◽

Chemical System ◽

Model Studies ◽

Halogen Chemistry ◽

The Impact

Abstract. The atmospheric chemistry of halogenated species (Cl, Br, I) participates in the global chemical sink of tropospheric ozone and perturbs the oxidizing capacity of the troposphere, notably influencing the atmospheric lifetime of methane. Global chemistry-climate models are commonly used to assess the global budget of ozone, its sensitivity to emissions of its precursors, and to project its long-term evolution. Here, we report on the implementation of tropospheric halogens chemistry in the chemistry-climate model LMDZ-INCA and its effects on the tropospheric ozone budget. Overall, the results show that the model simulates satisfactorily the impact of halogens on the photooxidizing system in the troposphere, in particular in the marine boundary layer. To elucidate the mechanisms and quantify the effects, standard metrics representative of the behavior of the tropospheric chemical system (Ox, HOx, NOx, CH4, and NMVOCs) are computed with and without halogen chemistry. Tropospheric halogens in the LMDZ-INCA model lead to a decrease of 22 % in the ozone burden, 8 % in OH, and 33 % in NOx. Additional sensitivity simulations show that the inclusion of halogens chemistry makes ozone more sensitive to perturbations in CH4, NOx, and NMVOCs. Consistent with other global model studies, the sensitivity of the tropospheric ozone burden to changes from pre-industrial to present-day emissions is found to be ~20 % lower when tropospheric halogens are taken into account.

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