scholarly journals Tropospheric ozone production and chemical regime analysis during the COVID-19 lockdown over Europe

2021 ◽  
Author(s):  
Clara M. Nussbaumer ◽  
Andrea Pozzer ◽  
Ivan Tadic ◽  
Lenard Röder ◽  
Florian Obersteiner ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Tropospheric Ozone ◽  
Ozone Production ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
Secondary Pollutants ◽  
Tropopause Region ◽  
Research Aircraft ◽  
Business As Usual ◽  
Atmospheric Trace Gas

Abstract. The COVID-19 (Coronavirus disease 2019) European lockdowns have lead to a significant reduction in the emissions of primary pollutants such as NO (nitric oxide) and NO2 (nitrogen dioxide). As most photochemical processes are related to nitrogen oxide (NOx ≡ NO + NO2) chemistry, this event has presented an exceptional opportunity to investigate its effects on air quality and secondary pollutants, such as tropospheric ozone (O3). In this study, we present the effects of the COVID-19 lockdown on atmospheric trace gas concentrations, net ozone production rates (NOPR) and the dominant chemical regime throughout the troposphere based on three different research aircraft campaigns across Europe. These are the UTOPIHAN campaigns in 2003 and 2004, the HOOVER campaigns in 2006 and 2007 and the BLUESKY campaign in 2020, the latter performed during the COVID-19 lockdown. We present in situ observations and simulation results from the ECHAM5/MESSy Atmospheric Chemistry model which allows for scenario calculations with business as usual emissions during the BLUESKY campaign, referred to as "no-lockdown scenario". We show that the COVID-19 lockdown reduced NO and NO2 mixing ratios in the upper troposphere by around 55 % compared to the no-lockdown scenario due to reduced air traffic. O3 production and loss terms reflected this reduction with a deceleration in O3 cycling due to reduced mixing ratios of NOx while NOPRs were largely unaffected. We also study the role of methyl peroxyradicals forming HCHO (αCH3O2) to show that the COVID-19 lockdown shifted the chemistry in the upper troposphere/tropopause region to a NOx limited regime during BLUESKY. In comparison, we find a VOC limited regime to be dominant during UTOPIHAN.

scholarly journals Characterising the seasonal and geographical variability in tropospheric ozone, stratospheric influence and recent changes

2019 ◽  
Vol 19 (6) ◽  
pp. 3589-3620 ◽  
Author(s):  
Ryan S. Williams ◽  
Michaela I. Hegglin ◽  
Brian J. Kerridge ◽  
Patrick Jöckel ◽  
Barry G. Latter ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Tropospheric Ozone ◽  
Radiative Forcing ◽  
Lower Stratosphere ◽  
Climate Model ◽  
Stratospheric Ozone ◽  
Data Availability ◽  
Ozone Production ◽  
Upper Troposphere ◽  
The World

Abstract. The stratospheric contribution to tropospheric ozone (O3) has been a subject of much debate in recent decades but is known to have an important influence. Recent improvements in diagnostic and modelling tools provide new evidence that the stratosphere has a much larger influence than previously thought. This study aims to characterise the seasonal and geographical distribution of tropospheric ozone, its variability, and its changes and provide quantification of the stratospheric influence on these measures. To this end, we evaluate hindcast specified-dynamics chemistry–climate model (CCM) simulations from the European Centre for Medium-Range Weather Forecasts – Hamburg (ECHAM)/Modular Earth Submodel System (MESSy) Atmospheric Chemistry (EMAC) model and the Canadian Middle Atmosphere Model (CMAM), as contributed to the International Global Atmospheric Chemistry – Stratosphere-troposphere Processes And their Role in Climate (IGAC-SPARC) (IGAC–SPARC) Chemistry Climate Model Initiative (CCMI) activity, together with satellite observations from the Ozone Monitoring Instrument (OMI) and ozone-sonde profile measurements from the World Ozone and Ultraviolet Radiation Data Centre (WOUDC) over a period of concurrent data availability (2005–2010). An overall positive, seasonally dependent bias in 1000–450 hPa (∼0–5.5 km) sub-column ozone is found for EMAC, ranging from 2 to 8 Dobson units (DU), whereas CMAM is found to be in closer agreement with the observations, although with substantial seasonal and regional variation in the sign and magnitude of the bias (∼±4 DU). Although the application of OMI averaging kernels (AKs) improves agreement with model estimates from both EMAC and CMAM as expected, comparisons with ozone-sondes indicate a positive ozone bias in the lower stratosphere in CMAM, together with a negative bias in the troposphere resulting from a likely underestimation of photochemical ozone production. This has ramifications for diagnosing the level of model–measurement agreement. Model variability is found to be more similar in magnitude to that implied from ozone-sondes in comparison with OMI, which has significantly larger variability. Noting the overall consistency of the CCMs, the influence of the model chemistry schemes and internal dynamics is discussed in relation to the inter-model differences found. In particular, it is inferred that CMAM simulates a faster and shallower Brewer–Dobson circulation (BDC) compared to both EMAC and observational estimates, which has implications for the distribution and magnitude of the downward flux of stratospheric ozone over the most recent climatological period (1980–2010). Nonetheless, it is shown that the stratospheric influence on tropospheric ozone is significant and is estimated to exceed 50 % in the wintertime extratropics, even in the lower troposphere. Finally, long-term changes in the CCM ozone tracers are calculated for different seasons. An overall statistically significant increase in tropospheric ozone is found across much of the world but particularly in the Northern Hemisphere and in the middle to upper troposphere, where the increase is on the order of 4–6 ppbv (5 %–10 %) between 1980–1989 and 2001–2010. Our model study implies that attribution from stratosphere–troposphere exchange (STE) to such ozone changes ranges from 25 % to 30 % at the surface to as much as 50 %–80 % in the upper troposphere–lower stratosphere (UTLS) across some regions of the world, including western Eurasia, eastern North America, the South Pacific and the southern Indian Ocean. These findings highlight the importance of a well-resolved stratosphere in simulations of tropospheric ozone and its implications for the radiative forcing, air quality and oxidation capacity of the troposphere.

scholarly journals Comparisons of observed and modeled OH and HO2concentrations during the ambient measurement period of the HOxComp field campaign

2012 ◽  
Vol 12 (5) ◽  
pp. 2567-2585 ◽  
Author(s):  
Y. Kanaya ◽  
A. Hofzumahaus ◽  
H.-P. Dorn ◽  
T. Brauers ◽  
H. Fuchs ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Chemical Mechanism ◽  
Ozone Production ◽  
High Yield ◽  
Base Case ◽  
Peroxy Radicals ◽  
Field Campaign ◽  
Mixing Ratios ◽  
Measurement Mode ◽  
Single Instrument

Abstract. A photochemical box model constrained by ancillary observations was used to simulate OH and HO2 concentrations for three days of ambient observations during the HOxComp field campaign held in Jülich, Germany in July 2005. Daytime OH levels observed by four instruments were fairly well reproduced to within 33% by a base model run (Regional Atmospheric Chemistry Mechanism with updated isoprene chemistry adapted from Master Chemical Mechanism ver. 3.1) with high R2 values (0.72–0.97) over a range of isoprene (0.3–2 ppb) and NO (0.1–10 ppb) mixing ratios. Daytime HO2(*) levels, reconstructed from the base model results taking into account the sensitivity toward speciated RO2 (organic peroxy) radicals, as recently reported from one of the participating instruments in the HO2 measurement mode, were 93% higher than the observations made by the single instrument. This also indicates an overprediction of the HO2 to OH recycling. Together with the good model-measurement agreement for OH, it implies a missing OH source in the model. Modeled OH and HO2(*) could only be matched to the observations by addition of a strong unknown loss process for HO2(*) that recycles OH at a high yield. Adding to the base model, instead, the recently proposed isomerization mechanism of isoprene peroxy radicals (Peeters and Müller, 2010) increased OH and HO2(*) by 28% and 13% on average. Although these were still only 4% higher than the OH observations made by one of the instruments, larger overestimations (42–70%) occurred with respect to the OH observations made by the other three instruments. The overestimation in OH could be diminished only when reactive alkanes (HC8) were solely introduced to the model to explain the missing fraction of observed OH reactivity. Moreover, the overprediction of HO2(*) became even larger than in the base case. These analyses imply that the rates of the isomerization are not readily supported by the ensemble of radical observations. One of the measurement days was characterized by low isoprene concentrations (∼0.5 ppb) and OH reactivity that was well explained by the observed species, especially before noon. For this selected period, as opposed to the general behavior, the model tended to underestimate HO2(*). We found that this tendency is associated with high NOx concentrations, suggesting that some HO2 production or regeneration processes under high NOx conditions were being overlooked; this might require revision of ozone production regimes.

scholarly journals OH and HO<sub>2</sub> radical chemistry in a midlatitude forest: Measurements and model comparisons

2019 ◽  
Author(s):  
Michelle L. Lew ◽  
Pamela S. Rickly ◽  
Brandon P. Bottorff ◽  
Sofia Sklaveniti ◽  
Thierry Léonardis ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Global Climate ◽  
Oxidation Products ◽  
Chemical Mechanism ◽  
Ozone Production ◽  
Peroxy Radicals ◽  
Mixing Ratios ◽  
Photolysis Rates ◽  
Model Predictions ◽  
Ho2 Radical

Abstract. Reactions of the hydroxyl (OH) and peroxy radicals (HO2 and RO2) play a central role in the chemistry of the atmosphere. In addition to controlling the lifetimes of many trace gases important to issues of global climate change, OH radical reactions initiate the oxidation of volatile organic compounds (VOCs) which can lead to the production of ozone and secondary organic aerosols in the atmosphere. Previous measurements of these radicals in forest environments characterized by high mixing ratios of isoprene and low mixing ratios of nitrogen oxides (NOx) have shown serious discrepancies with modeled concentrations. These results bring into question our understanding of the atmospheric chemistry of isoprene and other biogenic VOCs under low NOx conditions. During the summer of 2015, OH and HO2 radical concentrations as well as total OH reactivity were measured using Laser-Induced Fluorescence - Fluorescence Assay by Gas Expansion (LIF-FAGE) techniques as part of the Indiana Radical, Reactivity and Ozone Production Intercomparison (IRRONIC). This campaign took place in a forested area near the Indiana University, Bloomington campus characterized by high mixing ratios of isoprene and low mixing ratios of NOx. Supporting measurements of photolysis rates, VOCs, NOx, and other species were used to constrain a zero-dimensional box model based on the Regional Atmospheric Chemistry Mechanism (RACM2) and the Master Chemical Mechanism (MCM). Using an OH chemical scavenger technique, the study revealed the presence of an interference with the LIF-FAGE measurements of OH that increased with both ambient concentrations of ozone and temperature. Subtraction of the interference resulted in measured OH concentrations that were in better agreement with model predictions, although the model still underestimated the measured concentrations, likely due to an underestimation of the concentration of NO at this site. Measurements of HO2 radical concentrations during the campaign included a fraction of isoprene-based peroxy radicals (HO2* = HO2 + αRO2) and were found to agree with model predictions. On average, the measured reactivity was consistent with that calculated from measured OH sinks to within 20 %, with modeled oxidation products accounting for the missing reactivity, although significant missing reactivity (approximately 40 % of the total measured reactivity) was observed on some days.

scholarly journals A Multi-sensor Upper Tropospheric Ozone Product (MUTOP) based on TES ozone and GOES water vapor: derivation

2010 ◽  
Vol 10 (12) ◽  
pp. 30055-30087 ◽  
Author(s):  
S. R. Felker ◽  
J. L. Moody ◽  
A. J. Wimmers ◽  
G. Osterman ◽  
K. Bowman
Keyword(s):  
Water Vapor ◽  
Potential Vorticity ◽  
Tropospheric Ozone ◽  
Forecast Model ◽  
Scientific Basis ◽  
Specific Humidity ◽  
Upper Troposphere ◽  
Weather Patterns ◽  
Mixing Ratios ◽  
Spatial Coverage

Abstract. The Tropospheric Emission Spectrometer (TES), a hyperspectral infrared instrument on the Aura satellite, retrieves a vertical profile of tropospheric ozone. However, polar-orbiting instruments like TES provide limited nadir-view coverage. This work illustrates the value of these observations when taken in context with information about synoptic-scale weather patterns. The goal of this study is to create map-view products of upper troposphere (UT) ozone through the integration of TES ozone measurements with two synoptic dynamical tracers of stratospheric influence: specific humidity derived from the GOES Imager, and potential vorticity from an operational forecast model. As a mixing zone between tropospheric and stratospheric reservoirs, the upper troposphere (UT) exhibits a complex chemical makeup. Determination of ozone mixing ratios in this layer is especially difficult without direct in-situ measurement. However, it is well understood that UT ozone is correlated with dynamical tracers like low specific humidity and high potential vorticity. Blending the advantages of two remotely sensed quantities (GOES water vapor and TES ozone) is at the core of the Multi-sensor Upper Tropospheric Ozone Product (MUTOP). Our approach results in the temporal and spatial coverage of a geostationary platform, a major improvement over individual polar overpasses, while retaining TES's ability to characterize UT ozone. Results suggest that over 70% of TES-observed UT ozone variability can be explained by correlation with the two dynamical tracers. MUTOP reproduces TES retrievals across the GOES-West domain with a root mean square error (RMSE) of 19.2 ppbv. There are several advantages to this multi-sensor derived product approach: (1) it is calculated from 2 operational fields (GOES specific humidity and GFS PV), so the layer-average ozone can be created and used in near real-time; (2) the product provides the spatial resolution and coverage of a geostationary platform as it depicts the distribution of dynamically driven ozone in the UT; and (3) the 6 h temporal resolution of the imagery allows for the visualization of rapid movement of this dynamically-driven ozone in the UT. This paper presents the scientific basis and methodology behind the creation of this unique ozone product, as well as a statistical comparison of the derived product to a set of coincident TES observations.

scholarly journals Measurements of NO, NO<sub>y</sub>, N<sub>2</sub>O, and O<sub>3</sub> during SPURT: implications for transport and chemistry in the lowermost stratosphere

2005 ◽  
Vol 5 (5) ◽  
pp. 8649-8688 ◽  
Author(s):  
M. I. Hegglin ◽  
D. Brunner ◽  
Th. Peter ◽  
P. Hoor ◽  
H. Fischer ◽  
...  
Keyword(s):  
Atmospheric Transport ◽  
Potential Temperature ◽  
Transport Processes ◽  
Ozone Production ◽  
Data Set ◽  
Latitude Range ◽  
Mixing Ratios ◽  
Tropical Tropopause ◽  
Tropopause Region ◽  
Extratropical Tropopause

Abstract. We present measurements of NO, NOy, O3, and N2O within the lowermost stratosphere (LMS) over Europe obtained during the SPURT project. The measurements cover each of the four seasons during two years between November 2001 and July 2003, and probe the entire altitude and latitude range of the LMS: from 5° N to 85° N equivalent latitude, and from 290 to 375 K potential temperature. The measurements represent a comprehensive data set of these tracers and reveal atmospheric transport processes that influence tracer distributions in the LMS. Mean mixing ratios of stratospheric tracers in equivalent latitude-potential temperature coordinates show a clear seasonal cycle related to the Brewer-Dobson circulation with highest values in spring and lowest values in autumn. Vertical profiles show strong gradients at the extratropical tropopause suggesting that vertical (cross-isentropic) mixing is reduced above the tropopause. Mixing along isentropes is also strongly reduced since pronounced meridional gradients are found on potential temperature surfaces in the LMS. Concurrent large gradients in PV in the vertical and in the meridional direction horizontally suggest the presence of a transport and mixing barrier. Well above the tropopause distinguished seasonal cycles were found in the correlation slopes ΔO3/ΔN2O and ΔNOy/ΔN2O. Smallest slopes found during spring indicate chemically aged stratospheric air originating from high altitudes and latitudes. The slopes are larger in summer and autumn suggesting that a substantial fraction of air takes a 'short-cut' from the tropical tropopause region into the extratropical LMS. The comparison of measured NO with critical NO values at which net ozone production changes from negative to positive implies a net ozone production up to 20 K above the local tropopause in winter, increasing during spring and summer to up to 50 K in autumn. Above this height NO values favor ozone destruction.

scholarly journals Hydrogen cyanide in the upper troposphere: GEM-AQ simulation and comparison with ACE-FTS observations

2009 ◽  
Vol 9 (1) ◽  
pp. 2165-2194 ◽  
Author(s):  
A. Lupu ◽  
J. W. Kaminski ◽  
L. Neary ◽  
J. C. McConnell ◽  
K. Toyota ◽  
...  
Keyword(s):  
Southern Hemisphere ◽  
Atmospheric Chemistry ◽  
Hydrogen Cyanide ◽  
Weather Forecasting ◽  
Boreal Summer ◽  
Air Quality Model ◽  
Quality Model ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
The Tropics

Abstract. We investigate the spatial and temporal distribution of hydrogen cyanide (HCN) in the upper troposphere through numerical simulations and comparison with observations from a space-based instrument. To perform the simulations, we used the Global Environmental Multiscale Air Quality model (GEM-AQ), which is based on the three-dimensional global multiscale model developed by the Meteorological Service of Canada for operational weather forecasting. The model was run for the period 2004–2006 on a 1.5°×1.5° global grid with 28 hybrid vertical levels from the surface up to 10 hPa. Objective analysis data from the Canadian Meteorological Centre were used to update the meteorological fields every 24 h. Fire emission fluxes of gas species were generated by using year-specific inventories of carbon emissions with 8-day temporal resolution from the Global Fire Emission Database (GFED) version 2. The model output is compared with HCN profiles measured by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) instrument onboard the Canadian SCISAT-1 satellite. High values of up to a few ppbv are observed in the tropics in the Southern Hemisphere; the enhancement in HCN volume mixing ratios in the upper troposphere is most prominent in October. Low upper-tropospheric mixing ratios of less than 100 pptv are mostly recorded at middle and high latitudes in the Southern Hemisphere in May–July. Mixing ratios in Northern Hemisphere peak in the boreal summer. The amplitude of the seasonal variation is less pronounced than in the Southern Hemisphere. Our model results show that in the upper troposphere GEM-AQ performs well globally for all seasons, except at Northern high and middle latitudes in summer, where the model has a large negative bias, and in the tropics in winter and spring, where it exhibits large positive bias. This may reflect inaccurate emissions or possible inaccuracies in the emission profile. The model is able to explain most of the observed variability in the upper troposphere HCN field, including the interannual variations in the observed mixing ratio. The estimated average global emission equals 1.3 Tg N yr−1. The average atmospheric burden is 0.53 Tg N, and the corresponding lifetime is 4.9 months.

ISOPRENE EMISSION ESTIMATE IN REGION CONTAINING EUCALYPTUS FOREST AND ITS RELATIONSHIP WITH LOCAL TROPOSPHERIC OZONE: CASE STUDY

2014 ◽  
Vol 32 (2) ◽  
pp. 207
Author(s):  
Ana Paula Dos Santos Zepka ◽  
Kelly Ribeiro
Keyword(s):  
Atmospheric Chemistry ◽  
Tropospheric Ozone ◽  
Chemical Compounds ◽  
Biogenic Emissions ◽  
Mixing Ratios ◽  
Eucalyptus Forest ◽  
Emission Estimate ◽  
Time Required ◽  
Commercial Forest

ABSTRACT. In order to study the biogenic emissions of isoprene by a commercial eucalyptus forest and its relationship with the local tropospheric ozone, two intensivesurveys were conducted in Fibria Celulose e Papel company, Cac¸apava, Vale do Paraíba, São Paulo State, Brazil. The samples were analyzed for isoprene via thermaldesorption gas chromatography. Ozone was monitored using a UV Photometric O3 Analyzer, Model 49i. The highest mixing ratios of isoprene were detected at noonand ranged from the maximum of 8.3 ppbv on November 29, 2010 to 3.5 ppbv on June 30, 2011. On the evaluated days, it was observed that isoprene and ozone peakedwith about two hours delay; this is explained by the time required for the isoprene to react with other precursors and, in the presence of sunlight, to form ozone. Duringthe winter days when both temperature and photosynthetic active radiation are lower, the emission of isoprene was also 65% lower than in the summer. Based on themaximum ozone (27.9 ppbv) detected, the atmosphere in this region is considered clean according to Conselho Nacional do Meio Ambiente (CONAMA) stipulates amaximum of 81.5 ppbv of ozone for good air quality.Keywords: commercial forest, chemical compounds, atmospheric chemistry. RESUMO. Com o objetivo de estudar a emissão de isopreno biogênico por floresta comercial de eucalipto e sua relação com o ozônio troposférico local, foramrealizadas duas campanhas intensivas na companhia Fibria Celulose e Papel, em Caçapava, no Vale do Paraíba Paulista. As amostras coletadas de isopreno foramanalisadas por cromatografia gasosa via dessorção térmica. O ozônio foi monitorado pelo Analisador UV Photometric O3, Modelo 49i. Ao meio-dia foram detectadasas maiores razões de mistura de isopreno, variando do máximo de 8,3 ppbv em 29 de novembro de 2010 a 3,5 ppbv em 30 de junho de 2011. Nos dias avaliados,observou-se que o ozônio apresentou pico máximo atrasado em cerca de duas horas em relação ao máximo de isopreno, o que é justificável devido ao tempo necessário para que este gás reaja com outros precursores, e que na presença de luz solar levem à formação de ozônio. Durante os dias avaliados de inverno, com temperaturae radiação fotossinteticamente ativa menores, a emissão de isopreno foi 65% menor do que na semana estudada do verão. Baseado no máximo detectado de ozônio(27,9 ppbv), a atmosfera dessa região é considerada limpa de acordo com o Conselho Nacional do Meio Ambiente (CONAMA) que estipula o máximo de 81,5 ppbv de ozônio para um ar de boa qualidade.Palavras-chave: floresta comercial, compostos químicos, química atmosférica.

scholarly journals Reactive nitrogen, ozone and ozone production in the Arctic troposphere and the impact of stratosphere-troposphere exchange

2011 ◽  
Vol 11 (24) ◽  
pp. 13181-13199 ◽  
Author(s):  
Q. Liang ◽  
J. M. Rodriguez ◽  
A. R. Douglass ◽  
J. H. Crawford ◽  
J. R. Olson ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Stratospheric Ozone ◽  
Arctic Region ◽  
Ozone Production ◽  
The Arctic ◽  
Subsequent Formation ◽  
Air Masses ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
The Impact

Abstract. We use aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission to examine the distributions and source attributions of O3 and NOy in the Arctic and sub-Arctic region. Using a number of marker tracers, we distinguish various air masses from the background troposphere and examine their contributions to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has a mean O3 of ~60 ppbv and NOx of ~25 pptv throughout spring and summer with CO decreasing from ~145 ppbv in spring to ~100 ppbv in summer. These observed mixing ratios are not notably different from the values measured during the 1988 ABLE-3A and the 2002 TOPSE field campaigns despite the significant changes in emissions and stratospheric ozone layer in the past two decades that influence Arctic tropospheric composition. Air masses associated with stratosphere-troposphere exchange are present throughout the mid and upper troposphere during spring and summer. These air masses, with mean O3 concentrations of 140–160 ppbv, are significant direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin displays net O3 formation in the Arctic due to its sustainable, high NOx (75 pptv in spring and 110 pptv in summer) and NOy (~800 pptv in spring and ~1100 pptv in summer). The air masses influenced by the stratosphere sampled during ARCTAS-B also show conversion of HNO3 to PAN. This active production of PAN is the result of increased degradation of ethane in the stratosphere-troposphere mixed air mass to form CH3CHO, followed by subsequent formation of PAN under high NOx conditions. These findings imply that an adequate representation of stratospheric NOy input, in addition to stratospheric O3 influx, is essential to accurately simulate tropospheric Arctic O3, NOx and PAN in chemistry transport models. Plumes influenced by recent anthropogenic and biomass burning emissions observed during ARCTAS show highly elevated levels of hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contain O3 higher than that in the Arctic tropospheric background except some aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.

scholarly journals Impact of the new HNO<sub>3</sub>-forming channel of the HO<sub>2</sub>+NO reaction on tropospheric HNO<sub>3</sub>, NO<sub>x</sub>, HO<sub>x</sub> and ozone

2008 ◽  
Vol 8 (14) ◽  
pp. 4061-4068 ◽  
Author(s):  
D. Cariolle ◽  
M. J. Evans ◽  
M. P. Chipperfield ◽  
N. Butkovskaya ◽  
A. Kukui ◽  
...  
Keyword(s):  
Southern Hemisphere ◽  
Atmospheric Chemistry ◽  
Tropospheric Ozone ◽  
Transport Model ◽  
Chemical Transport Model ◽  
Temperature Dependent ◽  
Upper Troposphere ◽  
The Mean ◽  
The Tropics ◽  
The Impact

Abstract. We have studied the impact of the recently observed reaction NO+HO2→HNO3 on atmospheric chemistry. A pressure and temperature-dependent parameterisation of this minor channel of the NO+HO2→NO2+OH reaction has been included in both a 2-D stratosphere-troposphere model and a 3-D tropospheric chemical transport model (CTM). Significant effects on the nitrogen species and hydroxyl radical concentrations are found throughout the troposphere, with the largest percentage changes occurring in the tropical upper troposphere (UT). Including the reaction leads to a reduction in NOx everywhere in the troposphere, with the largest decrease of 25% in the tropical and Southern Hemisphere UT. The tropical UT also has a corresponding large increase in HNO3 of 25%. OH decreases throughout the troposphere with the largest reduction of over 20% in the tropical UT. The mean global decrease in OH is around 13%, which is very large compared to the impact that typical photochemical revisions have on this modelled quantity. This OH decrease leads to an increase in CH4 lifetime of 5%. Due to the impact of decreased NOx on the OH:HO2 partitioning, modelled HO2 actually increases in the tropical UT on including the new reaction. The impact on tropospheric ozone is a decrease in the range 5 to 12%, with the largest impact in the tropics and Southern Hemisphere. Comparison with observations shows that in the region of largest changes, i.e. the tropical UT, the inclusion of the new reaction tends to degrade the model agreement. Elsewhere the model comparisons are not able to critically assess the impact of including this reaction. Only small changes are calculated in the minor species distributions in the stratosphere.

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