Seasonal characteristics of tropospheric ozone production and mixing ratios over East Asia: A global three-dimensional chemical transport model analysis

Abstract. Tropospheric ozone is important for the Earth’s climate and air quality. It is produced during the oxidation of organics in the presence of nitrogen oxides. Due to the range of organic species emitted and the chain like nature of their oxidation, this chemistry is complex and understanding the role of different processes (emission, deposition, chemistry) is difficult. We demonstrate a new methodology for diagnosing ozone production based on the processing of bonds contained within emitted molecules, the fate of which is determined by the conservation of spin of the bonding electrons. Using this methodology to diagnose ozone production in the GEOS-Chem chemical transport model, we demonstrate its advantages over the standard diagnostic. We show that the number of bonds emitted, their chemistry and lifetime, and feedbacks on OH are all important in determining the ozone production within the model and its sensitivity to changes. This insight may allow future model-model comparisons to better identify the root causes of model differences.

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Biomass burning influence on high latitude tropospheric ozone and reactive nitrogen in summer 2008: a multi-model analysis based on POLMIP simulations

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-14-24573-2014 ◽

2014 ◽

Vol 14 (17) ◽

pp. 24573-24621 ◽

Cited By ~ 9

Author(s):

S. R. Arnold ◽

L. K. Emmons ◽

S. A. Monks ◽

K. S. Law ◽

D. A. Ridley ◽

...

Keyword(s):

Biomass Burning ◽

High Latitude ◽

Tropospheric Ozone ◽

Transport Model ◽

Chemical Transport ◽

Ozone Production ◽

The Arctic ◽

Vertical Position ◽

Chemical Transport Model ◽

Fire Emissions

Abstract. We have evaluated tropospheric ozone enhancement in air dominated by biomass burning emissions at high laititudes (> 50˚ N) in July 2008, using 10 global chemical transport model simulations from the POLMIP multi-model comparison exercise. In model air masses dominated by fire emissions, Δ O3/ΔCO values ranged between 0.039 and 0.196 ppbv ppbv−1 (mean: 0.113 ppbv ppbv−1) in freshly fire-influenced air, and between 0.140 and 0.261 ppbv ppbv−1 (mean: 0.193 ppbv) in more aged fire-influenced air. These values are in broad agreement with the range of observational estimates from the literature. Model ΔPAN/ΔCO enhancement ratios show distinct groupings according to the meteorological data used to drive the models. ECMWF-forced models produce larger ΔPAN/ΔCO values (4.44–6.28 pptv ppbv−1) than GEOS5-forced models (2.02–3.02 pptv ppbv−1), which we show is likely linked to differences efficiency of vertical transport during poleward export from mid-latitude source regions. Simulations of a large plume of biomass burning and anthropogenic emissions exported from Asia towards the Arctic using a Lagrangian chemical transport model show that 4 day net ozone change in the plume is sensitive to differences in plume chemical composition and plume vertical position among the POLMIP models. In particular, Arctic ozone evolution in the plume is highly sensitive to initial concentrations of PAN, as well as oxygenated VOCs (acetone, acetaldehyde), due to their role in producing the peroxyacetyl radical PAN precursor. Vertical displacement is also important due to its effects on the stability of PAN, and subsequent effect on NOx abundance. In plumes where net ozone production is limited, we find that the lifetime of ozone in the plume is sensitive to hydrogen peroxide loading, due to the production of HO2 from peroxide photolysis, and the key role of HO2 + O3 in controlling ozone loss. Overall, our results suggest that emissions from biomass burning lead to large-scale photochemical enhancement in high latitude tropospheric ozone during summer.

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A new diagnostic for tropospheric ozone production

Atmospheric Chemistry and Physics ◽

10.5194/acp-17-13669-2017 ◽

2017 ◽

Vol 17 (22) ◽

pp. 13669-13680 ◽

Cited By ~ 4

Author(s):

Peter M. Edwards ◽

Mathew J. Evans

Keyword(s):

Air Quality ◽

Tropospheric Ozone ◽

Transport Model ◽

Chemical Transport ◽

Ozone Production ◽

Chemical Transport Model ◽

Organic Species ◽

Earth’S Climate ◽

Oxidation Of Organics

Abstract. Tropospheric ozone is important for the Earth's climate and air quality. It is produced during the oxidation of organics in the presence of nitrogen oxides. Due to the range of organic species emitted and the chain-like nature of their oxidation, this chemistry is complex and understanding the role of different processes (emission, deposition, chemistry) is difficult. We demonstrate a new methodology for diagnosing ozone production based on the processing of bonds contained within emitted molecules, the fate of which is determined by the conservation of spin of the bonding electrons. Using this methodology to diagnose ozone production in the GEOS-Chem chemical transport model, we demonstrate its advantages over the standard diagnostic. We show that the number of bonds emitted, their chemistry and lifetime, and feedbacks on OH are all important in determining the ozone production within the model and its sensitivity to changes. This insight may allow future model–model comparisons to better identify the root causes of model differences.

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Trends in Global Tropospheric Ozone Inferred from a Composite Record of TOMS/OMI/MLS/OMPS Satellite Measurements and the MERRA-2 GMI Simulation

10.5194/acp-2018-716 ◽

2018 ◽

Cited By ~ 1

Author(s):

Jerry R. Ziemke ◽

Luke D. Oman ◽

Sarah A. Strode ◽

Anne R. Douglass ◽

Mark A. Olsen ◽

...

Keyword(s):

East Asia ◽

Tropospheric Ozone ◽

Transport Model ◽

Central Africa ◽

Chemical Transport ◽

Chemical Transport Model ◽

Ozone Monitoring Instrument ◽

Satellite Measurements ◽

Ozone Trends ◽

Ne Pacific

Abstract. Past studies have suggested that ozone in the troposphere has increased globally throughout much of the 20th century due to increases in anthropogenic emissions and transport. We show by combining satellite measurements with a chemical transport model that during the last four decades tropospheric ozone does indeed indicate increases that are global in nature, yet still highly regional. Satellite ozone measurements from Nimbus-7 and Earth Probe Total Ozone Mapping Spectrometer (TOMS) are merged with ozone measurements from Aura Ozone Monitoring Instrument/Microwave Limb Sounder (OMI/MLS) to determine trends in tropospheric ozone for 1979–2016. Both TOMS (1979–2005) and OMI/MLS (2005–2016) depict large increases in tropospheric ozone from the Near East to India/East Asia and further eastward over the Pacific Ocean. The 38-year merged satellite record shows total net change over this region of about +6 to +7 Dobson Units (DU) (i.e., ~ 15–20 % of average background ozone), with the largest increase (~ 4 DU) occurring during the 2005–2016 Aura period. The Global Modeling Initiative (GMI) chemical transport model with time-varying emissions is included to evaluate tropospheric ozone trends for 1980–2016. The GMI simulation for the combined record also depicts greatest increases of +6 to +7 DU over India/east Asia, identical to the satellite measurements. In regions of significant increases in TCO the trends are a factor of 2–2.5 larger for the Aura record when compared to the earlier TOMS record; for India/east Asia the trends in TCO for both GMI and satellite measurements are ~ +3 DU-decade−1 or greater during 2005–2016 compared to about +1.2 to +1.4 DU-decade−1 for 1979–2016. The GMI simulation and satellite data also reveal a tropospheric ozone increase of ~ +4 to +5 DU for the 38-year record over central Africa and the tropical Atlantic Ocean. Both the GMI simulation and satellite-measured tropospheric ozone during the latter Aura time period show increases of ~ +3 DU-decade−1 over the NH Atlantic and NE Pacific.

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Trends in global tropospheric ozone inferred from a composite record of TOMS/OMI/MLS/OMPS satellite measurements and the MERRA-2 GMI simulation

Atmospheric Chemistry and Physics ◽

10.5194/acp-19-3257-2019 ◽

2019 ◽

Vol 19 (5) ◽

pp. 3257-3269 ◽

Cited By ~ 24

Author(s):

Jerry R. Ziemke ◽

Luke D. Oman ◽

Sarah A. Strode ◽

Anne R. Douglass ◽

Mark A. Olsen ◽

...

Keyword(s):

East Asia ◽

Tropospheric Ozone ◽

Transport Model ◽

Central Africa ◽

Chemical Transport ◽

Chemical Transport Model ◽

Ozone Monitoring Instrument ◽

Satellite Measurements ◽

Ozone Trends ◽

Ne Pacific

Abstract. Past studies have suggested that ozone in the troposphere has increased globally throughout much of the 20th century due to increases in anthropogenic emissions and transport. We show, by combining satellite measurements with a chemical transport model, that during the last four decades tropospheric ozone does indeed indicate increases that are global in nature, yet still highly regional. Satellite ozone measurements from Nimbus-7 and Earth Probe Total Ozone Mapping Spectrometer (TOMS) are merged with ozone measurements from the Aura Ozone Monitoring Instrument/Microwave Limb Sounder (OMI/MLS) to determine trends in tropospheric ozone for 1979–2016. Both TOMS (1979–2005) and OMI/MLS (2005–2016) depict large increases in tropospheric ozone from the Near East to India and East Asia and further eastward over the Pacific Ocean. The 38-year merged satellite record shows total net change over this region of about +6 to +7 Dobson units (DU) (i.e., ∼15 %–20 % of average background ozone), with the largest increase (∼4 DU) occurring during the 2005–2016 Aura period. The Global Modeling Initiative (GMI) chemical transport model with time-varying emissions is used to aid in the interpretation of tropospheric ozone trends for 1980–2016. The GMI simulation for the combined record also depicts the greatest increases of +6 to +7 DU over India and East Asia, very similar to the satellite measurements. In regions of significant increases in tropospheric column ozone (TCO) the trends are a factor of 2–2.5 larger for the Aura record when compared to the earlier TOMS record; for India and East Asia the trends in TCO for both GMI and satellite measurements are ∼+3 DU decade−1 or greater during 2005–2016 compared to about +1.2 to +1.4 DU decade−1 for 1979–2005. The GMI simulation and satellite data also reveal a tropospheric ozone increases in ∼+4 to +5 DU for the 38-year record over central Africa and the tropical Atlantic Ocean. Both the GMI simulation and satellite-measured tropospheric ozone during the latter Aura time period show increases of ∼+3 DU decade−1 over the N Atlantic and NE Pacific.

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Biomass burning influence on high-latitude tropospheric ozone and reactive nitrogen in summer 2008: a multi-model analysis based on POLMIP simulations

Atmospheric Chemistry and Physics ◽

10.5194/acp-15-6047-2015 ◽

2015 ◽

Vol 15 (11) ◽

pp. 6047-6068 ◽

Cited By ~ 25

Author(s):

S. R. Arnold ◽

L. K. Emmons ◽

S. A. Monks ◽

K. S. Law ◽

D. A. Ridley ◽

...

Keyword(s):

Biomass Burning ◽

High Latitude ◽

Tropospheric Ozone ◽

Transport Model ◽

Chemical Transport ◽

Ozone Production ◽

The Arctic ◽

Vertical Position ◽

Chemical Transport Model ◽

Fire Emissions

Abstract. We have evaluated tropospheric ozone enhancement in air dominated by biomass burning emissions at high latitudes (> 50° N) in July 2008, using 10 global chemical transport model simulations from the POLMIP multi-model comparison exercise. In model air masses dominated by fire emissions, ΔO3/ΔCO values ranged between 0.039 and 0.196 ppbv ppbv−1 (mean: 0.113 ppbv ppbv−1) in freshly fire-influenced air, and between 0.140 and 0.261 ppbv ppbv−1 (mean: 0.193 ppbv) in more aged fire-influenced air. These values are in broad agreement with the range of observational estimates from the literature. Model ΔPAN/ΔCO enhancement ratios show distinct groupings according to the meteorological data used to drive the models. ECMWF-forced models produce larger ΔPAN/ΔCO values (4.47 to 7.00 pptv ppbv−1) than GEOS5-forced models (1.87 to 3.28 pptv ppbv−1), which we show is likely linked to differences in efficiency of vertical transport during poleward export from mid-latitude source regions. Simulations of a large plume of biomass burning and anthropogenic emissions exported from towards the Arctic using a Lagrangian chemical transport model show that 4-day net ozone change in the plume is sensitive to differences in plume chemical composition and plume vertical position among the POLMIP models. In particular, Arctic ozone evolution in the plume is highly sensitive to initial concentrations of PAN, as well as oxygenated VOCs (acetone, acetaldehyde), due to their role in producing the peroxyacetyl radical PAN precursor. Vertical displacement is also important due to its effects on the stability of PAN, and subsequent effect on NOx abundance. In plumes where net ozone production is limited, we find that the lifetime of ozone in the plume is sensitive to hydrogen peroxide loading, due to the production of HOx from peroxide photolysis, and the key role of HO2 + O3 in controlling ozone loss. Overall, our results suggest that emissions from biomass burning lead to large-scale photochemical enhancement in high-latitude tropospheric ozone during summer.

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Review comments for manuscript titled “Seasonal variation of fine- and coarse-mode nitrates and related aerosols over East Asia: Synergetic observations and chemical transport model analysis” by: I. Uno et al.

10.5194/acp-2017-447-rc1 ◽

2017 ◽

Author(s):

Anonymous

Keyword(s):

Seasonal Variation ◽

East Asia ◽

Transport Model ◽

Chemical Transport ◽

Model Analysis ◽

Chemical Transport Model ◽

Coarse Mode

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The UIUC three-dimensional stratospheric chemical transport model: Description and evaluation of the simulated source gases and ozone

Journal of Geophysical Research Atmospheres ◽

10.1029/1999jd900138 ◽

1999 ◽

Vol 104 (D9) ◽

pp. 11755-11781 ◽

Cited By ~ 67

Author(s):

Eugene V. Rozanov ◽

Vladimir A. Zubov ◽

Michael E. Schlesinger ◽

Fanglin Yang ◽

Natalia G. Andronova

Keyword(s):

Transport Model ◽

Three Dimensional ◽

Chemical Transport ◽

Model Description ◽

Chemical Transport Model ◽

Simulated Source

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Implementation of state-of-the-art ternary new-particle formation scheme to the regional chemical transport model PMCAMx-UF in Europe

Geoscientific Model Development ◽

10.5194/gmd-9-2741-2016 ◽

2016 ◽

Vol 9 (8) ◽

pp. 2741-2754 ◽

Cited By ~ 8

Author(s):

Elham Baranizadeh ◽

Benjamin N. Murphy ◽

Jan Julin ◽

Saeed Falahat ◽

Carly L. Reddington ◽

...

Keyword(s):

Transport Model ◽

Three Dimensional ◽

Chemical Transport ◽

Particle Formation ◽

Radiative Transfer Model ◽

Transfer Model ◽

New Particle Formation ◽

Chemical Transport Model ◽

Order Of Magnitude ◽

Adjustment Scheme

Abstract. The particle formation scheme within PMCAMx-UF, a three-dimensional chemical transport model, was updated with particle formation rates for the ternary H2SO4–NH3–H2O pathway simulated by the Atmospheric Cluster Dynamics Code (ACDC) using quantum chemical input data. The model was applied over Europe for May 2008, during which the EUCAARI-LONGREX (European Aerosol Cloud Climate and Air Quality Interactions–Long-Range Experiment) campaign was carried out, providing aircraft vertical profiles of aerosol number concentrations. The updated model reproduces the observed number concentrations of particles larger than 4 nm within 1 order of magnitude throughout the atmospheric column. This agreement is encouraging considering the fact that no semi-empirical fitting was needed to obtain realistic particle formation rates. The cloud adjustment scheme for modifying the photolysis rate profiles within PMCAMx-UF was also updated with the TUV (Tropospheric Ultraviolet and Visible) radiative-transfer model. Results show that, although the effect of the new cloud adjustment scheme on total number concentrations is small, enhanced new-particle formation is predicted near cloudy regions. This is due to the enhanced radiation above and in the vicinity of the clouds, which in turn leads to higher production of sulfuric acid. The sensitivity of the results to including emissions from natural sources is also discussed.

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