scholarly journals Observation of ozone enhancement in the lower troposphere over East Asia from a space-borne ultraviolet spectrometer

2015 ◽  
Vol 15 (2) ◽  
pp. 2013-2054 ◽  
Author(s):  
S. Hayashida ◽  
X. Liu ◽  
A. Ono ◽  
K. Yang ◽  
K. Chance

Abstract. We report observations from space using ultraviolet (UV) radiance for significant enhancement of ozone in the lower troposphere over Central and Eastern China (CEC). The recent retrieval products of the Ozone Monitoring Instrument (OMI) onboard the Earth Observing System (EOS)/Aura satellite revealed the spatial and temporal variation of ozone distributions in multiple layers in the troposphere. We compared the OMI-derived ozone over Beijing with airborne measurements by the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) program. The correlation between OMI and MOZAIC ozone in the lower troposphere was reasonable, which assured the reliability of OMI ozone retrievals in the lower troposphere under enhanced ozone conditions. The ozone enhancement was clearly observed over CEC, with Shandong Province as its center, and most notable in June in any given year. Similar seasonal variations were observed throughout the nine-year OMI measurement period of 2005 to 2013. The ozone enhancement in June was associated with the enhancement of carbon monoxide (CO) and hotspots, which is consistent with previous studies of in-situ measurements such those made by the MTX2006 campaign. A considerable part of this ozone enhancement could be attributed to the emissions of ozone precursors from open crop residue burning (OCRB) after the winter wheat harvest, in addition to emissions from industrial activities and automobiles. The ozone distribution presented in this study is also consistent with some model studies that apply emissions from OCRB. The lower tropospheric ozone distribution is first shown from OMI retrieval in this study, and the results will be useful in clarifying any unknown factors that influence ozone distribution by comparison with model simulations.

2015 ◽  
Vol 15 (17) ◽  
pp. 9865-9881 ◽  
Author(s):  
S. Hayashida ◽  
X. Liu ◽  
A. Ono ◽  
K. Yang ◽  
K. Chance

Abstract. We report observations from space using ultraviolet (UV) radiance for significant enhancement of ozone in the lower troposphere over central and eastern China (CEC). The recent retrieval products of the Ozone Monitoring Instrument (OMI) onboard the Earth Observing System (EOS) Aura satellite revealed the spatial and temporal variation of ozone distributions in multiple layers in the troposphere. We compared the OMI-derived ozone over Beijing with airborne measurements by the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC) program. The correlation between OMI and MOZAIC ozone in the lower troposphere was reasonable, which assured the reliability of OMI ozone retrievals in the lower troposphere under enhanced ozone conditions. The ozone enhancement was clearly observed over CEC, with Shandong Province as its center, and was most notable in June in any given year. Similar seasonal variations were observed throughout the 9-year OMI measurement period of 2005 to 2013. A considerable part of this ozone enhancement could be attributed to the emissions of ozone precursors from industrial activities and automobiles, and possibly from open crop residue burning (OCRB) after the winter wheat harvest. The ozone distribution presented in this study is also consistent with some model studies. The lower tropospheric ozone distribution is first shown from OMI retrieval in this study, and the results will be useful in clarifying any unknown factors that influence ozone distribution by comparison with model simulations.


2010 ◽  
Vol 10 (4) ◽  
pp. 1671-1687 ◽  
Author(s):  
J.-D. Paris ◽  
A. Stohl ◽  
P. Ciais ◽  
P. Nédélec ◽  
B. D. Belan ◽  
...  

Abstract. We analysed results of three intensive aircraft campaigns above Siberia (April and September 2006, August 2007) with a total of ~70 h of continuous CO2, CO and O3 measurements. The flight route consists of consecutive ascents and descents between Novosibirsk (55° N, 82° E) and Yakutsk (62° N, 129° E). We performed retroplume calculations with the Lagrangian particle dispersion model FLEXPART for many short segments along the flight tracks. To reduce the extremely rich information on source regions provided by the model calculation into a small number of distinct cases, we performed a statistical clustering – to our knowledge for the first time – into potential source regions of the footprint emission sensitivities obtained from the model calculations. This technique not only worked well to separate source region influences but also resulted in clearly distinct tracer concentrations for the various clusters obtained. High CO and O3 concentrations were found associated with agricultural fire plumes originating from Kazakhstan in September 2006. A statistical analysis indicates that summer uptake of CO2 is largely explained (~50% of variance) by air mass exposure to uptake by Siberian and sub-arctic ecosystems. This resulted in an average 5 to 10 ppm difference with overlaying air masses. Stratosphere-troposphere exchange is found to strongly influence the observed O3 mixing ratios in spring, but not in summer. European emissions contributed to high O3 concentrations above Siberia in April 2006 and August 2007, while emissions from North Eastern China also contributed to higher O3 mixing ratios in summer, but tend to lower mixing ratios in spring, when the airmass aerosol burden is important. In the lower troposphere, large-scale deposition processes in the boreal and sub-arctic boundary layer is a large O3 sink, resulting in a ~20 ppb difference with overlaying air masses. Lagrangian footprint clustering is very promising and could also be advantageously applied to the interpretation of ground based measurements including calculation of tracers' sources and sinks.


2021 ◽  
Author(s):  
Phuc Thi Minh Ha ◽  
Yugo Kanaya ◽  
Fumikazu Taketani ◽  
Maria Dolores Andrés Hernández ◽  
Benjamin Schreiner ◽  
...  

Abstract. Nitrous acid (HONO) is an important atmospheric gas given its contribution to the cycles of NOx and HOx, but its role in global atmospheric photochemistry is not fully understood. This study, for the first time, implemented three pathways of HONO formation in the chemistry-climate model CHASER (MIROC-ESM) to explore three physical phenomena: gas-phase kinetic reactions (GRs), direct emission (EM), and heterogeneous reactions on cloud/aerosol particles (HRs). We evaluated the simulations by the atmospheric measurements from the OMI (Ozone Monitoring Instrument), EANET (Acid Deposition Monitoring Network in eastern Asia) / EMEP (European Monitoring and Evaluation Programme) ground-based stationary observations, observations from the ship R/V Mirai, and aircraft-based measurements by ATom1 (atmospheric tomography) and EMeRGe-Asia-2018 (Effect of Megacities on the Transport and Transformation of Pollutants on the Regional to Global scales). We showed that the inclusion of the HONO chemistry in the modeling process reduces the model bias against the measurements for PM2.5, NO3−/HNO3, NO2, OH, O3, and CO, especially in the lower troposphere and the North Pacific (NP) region. We found that the retrieved global abundance of tropospheric HONO was 1.4 TgN. Of the three source pathways, HRs and EM contributed 63 % and 26 % to the net HONO production, respectively. We also observed that, reactions on the aerosol surfaces contributed larger amounts of HONO (51 %) than those on the cloud surfaces (12 %). The model exhibited significant negative biases for daytime HONO in the Asian off-coast region, compared with the airborne measurements by EMeRGe-Asia-2018, indicating the existence of unknown daytime HONO sources. Strengthening of aerosol uptake of NO2 near-surface and in the middle troposphere, cloud uptake, and direct HONO emission are all potential yet-unknown HONO sources. We also found that the simulated HONO abundance and its impact on NOx-O3 chemistry are sensitive to the yield of the heterogeneous conversion of NO2 to HONO (vs. HNO3). Inclusion of HONO reduces global tropospheric NOx (NO + NO2) levels by 20.4 %, thereby weakening the tropospheric oxidizing capacity, which in turn, increases CH4 lifetime (13 %) and CO abundance (8 %). HRs on the surfaces of cloud particles, which have been neglected in previous modeling studies, are the main drivers of these impacts. This effect is particularly salient for the substantial reductions of levels of OH (40–67 %) and O3 (30–45 %) in the NP region during summer given the significant reduction of NOx level (50–95 %). In contrast, HRs on aerosol surfaces in China (Beijing) enhance OH and O3 winter mean levels by 600–1700 % and 10–33 %, respectively, with regards to their minima in winter. Overall, our findings suggest that a global model that does not consider HONO heterogeneous mechanisms (especially HRs on cloud particle surfaces) may erroneously predict the effect of HONO in remote areas and polluted regions.


2014 ◽  
Vol 14 (1) ◽  
pp. 283-299 ◽  
Author(s):  
V. F. Sofieva ◽  
J. Tamminen ◽  
E. Kyrölä ◽  
T. Mielonen ◽  
P. Veefkind ◽  
...  

Abstract. A new ozone climatology, based on ozonesonde and satellite measurements, spanning the altitude region between the earth's surface and ~60 km is presented (TpO3 climatology). This climatology is novel in that the ozone profiles are categorized according to calendar month, latitude and local tropopause heights. Compared to the standard latitude–month categorization, this presentation improves the representativeness of the ozone climatology in the upper troposphere and the lower stratosphere (UTLS). The probability distribution of tropopause heights in each latitude–month bin provides additional climatological information and allows transforming/comparing the TpO3 climatology to a standard climatology of zonal mean ozone profiles. The TpO3 climatology is based on high-vertical-resolution measurements of ozone from the satellite-based Stratospheric Aerosol and Gas Experiment II (in 1984 to 2005) and from balloon-borne ozonesondes from 1980 to 2006. The main benefits of the TpO3 climatology are reduced standard deviations on climatological ozone profiles in the UTLS, partial characterization of longitudinal variability, and characterization of ozone profiles in the presence of double tropopauses. The first successful application of the TpO3 climatology as a priori in ozone profile retrievals from Ozone Monitoring Instrument on board the Earth Observing System (EOS) Aura satellite shows an improvement of ozone precision in UTLS of up to 10% compared with the use of conventional climatologies. In addition to being advantageous for use as a priori in satellite retrieval algorithms, the TpO3 climatology might be also useful for validating the representation of ozone in climate model simulations.


2016 ◽  
Author(s):  
Johannes Bieser ◽  
Franz Slemr ◽  
Jesse Ambrose ◽  
Carl Brenninkmeijer ◽  
Steve Brooks ◽  
...  

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.


2017 ◽  
Vol 10 (11) ◽  
pp. 4121-4134 ◽  
Author(s):  
Peter R. Colarco ◽  
Santiago Gassó ◽  
Changwoo Ahn ◽  
Virginie Buchard ◽  
Arlindo M. da Silva ◽  
...  

Abstract. We provide an analysis of the commonly used Ozone Monitoring Instrument (OMI) aerosol index (AI) product for qualitative detection of the presence and loading of absorbing aerosols. In our analysis, simulated top-of-atmosphere (TOA) radiances are produced at the OMI footprints from a model atmosphere and aerosol profile provided by the NASA Goddard Earth Observing System (GEOS-5) Modern-Era Retrospective Analysis for Research and Applications aerosol reanalysis (MERRAero). Having established the credibility of the MERRAero simulation of the OMI AI in a previous paper we describe updates in the approach and aerosol optical property assumptions. The OMI TOA radiances are computed in cloud-free conditions from the MERRAero atmospheric state, and the AI is calculated. The simulated TOA radiances are fed to the OMI near-UV aerosol retrieval algorithms (known as OMAERUV) is compared to the MERRAero calculated AI. Two main sources of discrepancy are discussed: one pertaining to the OMI algorithm assumptions of the surface pressure, which are generally different from what the actual surface pressure of an observation is, and the other related to simplifying assumptions in the molecular atmosphere radiative transfer used in the OMI algorithms. Surface pressure assumptions lead to systematic biases in the OMAERUV AI, particularly over the oceans. Simplifications in the molecular radiative transfer lead to biases particularly in regions of topography intermediate to surface pressures of 600 and 1013.25 hPa. Generally, the errors in the OMI AI due to these considerations are less than 0.2 in magnitude, though larger errors are possible, particularly over land. We recommend that future versions of the OMI algorithms use surface pressures from readily available atmospheric analyses combined with high-spatial-resolution topographic maps and include more surface pressure nodal points in their radiative transfer lookup tables.


2007 ◽  
Vol 7 (20) ◽  
pp. 5357-5370 ◽  
Author(s):  
B. Sauvage ◽  
F. Gheusi ◽  
V. Thouret ◽  
J.-P. Cammas ◽  
J. Duron ◽  
...  

Abstract. A meso-scale model was used to understand and describe the dynamical processes driving high ozone concentrations observed during both dry and monsoon season in monthly climatologies profiles over Lagos (Nigeria, 6.6° N, 3.3° E), obtained with the MOZAIC airborne measurements (ozone and carbon monoxide). This study focuses on ozone enhancements observed in the upper-part of the lower troposphere, around 3000 m. Two individual cases have been selected in the MOZAIC dataset as being representative of the climatological ozone enhancements, to be simulated and analyzed with on-line Lagrangian backtracking of air masses. This study points out the role of baroclinic low-level circulations present in the Inter Tropical Front (ITF) area. Two low-level thermal cells around a zonal axis and below 2000 m, in mirror symmetry to each other with respect to equator, form near 20° E and around 5° N and 5° S during the (northern hemisphere) dry and wet seasons respectively. They are caused by surface gradients – the warm dry surface being located poleward of the ITF and the cooler wet surface equatorward of the ITF. A convergence line exists between the poleward low-level branch of each thermal cell and the equatorward low-level branch of the Hadley cell. Our main conclusion is to point out this line as a preferred location for fire products – among them ozone precursors – to be uplifted and injected into the lower free troposphere. The free tropospheric transport that occurs then depends on the hemisphere and season. In the NH dry season, the AEJ allows transport of ozone and precursors westward to Lagos. In the NH monsoon (wet) season, fire products are transported from the southern hemisphere to Lagos by the southeasterly trade that surmounts the monsoon layer. Additionally ozone precursors uplifted by wet convection in the ITCZ can also mix to the ones uplifted by the baroclinic cell and be advected up to Lagos by the trade flow.


2018 ◽  
Vol 18 (22) ◽  
pp. 16345-16361 ◽  
Author(s):  
Derong Zhou ◽  
Ke Ding ◽  
Xin Huang ◽  
Lixia Liu ◽  
Qiang Liu ◽  
...  

Abstract. Anthropogenic fossil fuel (FF) combustion, biomass burning (BB) and desert dust are the main sources of air pollutants around the globe but are particularly intensive and important for air quality in Asia in spring. In this study, we investigate the vertical distribution, transport characteristics, source contribution and meteorological feedback of these aerosols in a unique pollution episode that occurred in eastern Asia based on various measurement data and modeling methods. In this episode, the Yangtze River Delta (YRD) in eastern China experienced persistent air pollution, dramatically changing from secondary fine particulate pollution to dust pollution in late March 2015. The Eulerian and Lagrangian models were conducted to investigate the vertical structure, transport characteristics and mechanisms of the multi-scale, multisource and multiday air pollution episode. The regional polluted continental aerosols mainly accumulated near the surface, mixed with dust aerosol downwash from the upper planetary boundary layer (PBL) and middle–lower troposphere (MLT), and further transported by large-scale cold fronts and warm conveyor belts. BB smoke from Southeast Asia was transported by westerlies around the altitude of 3 km from southern China, was further mixed with dust and FF aerosols in eastern China and experienced long-range transport over the Pacific. These pollutants could all be transported to the YRD region and cause a structure of multilayer pollution there. These pollutants could also cause significant feedback with MLT meteorology and then enhance local anthropogenic pollution. This study highlights the importance of intensive vertical measurement in eastern China and the downwind Pacific Ocean and raises the need for quantitative understanding of environmental and climate impacts of these pollution sources.


2004 ◽  
Vol 4 (3) ◽  
pp. 3285-3332 ◽  
Author(s):  
B. Sauvage ◽  
V. Thouret ◽  
J.-P. Cammas ◽  
F. Gheusi ◽  
G. Athier ◽  
...  

Abstract. We analyze MOZAIC ozone observations recorded over Equatorial Africa, from April 1997 to March 2003 to give the first ozone climatology of this region. The monthly mean vertical profiles have been systematically analyzed with monthly mean ECMWF data using a Lagrangian-model (LAGRANTO). We assess the roles played by the dynamical features of Equatorial Africa and the intense biomass burning sources within the region in defining the ozone distribution. The lower troposphere exhibits layers of enhanced ozone during the biomass burning season in each hemisphere (boreal winter in the northern tropics and boreal summer in the southern tropics). The monthly mean vertical profiles of ozone are clearly influenced by the local dynamical situation. Over the Gulf of Guinea during boreal winter, the ozone profile is characterized by systematically high ozone below 650 hPa. This is due to the high stability caused by the Harmattan winds in the lower troposphere and the blocking Saharan anticyclone in the middle troposphere that prevents any efficient vertical mixing. In contrast, Central African enhancements are not only found in the lower troposphere but throughout the troposphere. The boreal summer ozone maximum in the lower troposphere of Central Africa continues up to November in the middle troposphere due to the influx of air masses laden with biomass burning products from Brazil and Southern Africa. Despite its southern latitude, Central Africa during the boreal winter is also under the influence of the northern tropical fires. This phenomenon is known as the "ozone paradox". However, the tropospheric ozone columns calculated from the MOZAIC data give evidence that the Tropical Tropospheric Ozone Column (TTOC) maximum over Africa swings from West Africa in DJF to Central Africa in JJA. This contrasts with studies based on TOMS satellite data. A rough assessment of the regional ozone budget shows that the northern tropics fires in boreal winter might contribute up to 20% of the global photochemical ozone production. This study gives the first detailed picture of the ozone distribution over Equatorial Africa that should be used to validate both global models over this region and future satellite products.


2016 ◽  
Author(s):  
Can Li ◽  
Nickolay A. Krotkov ◽  
Simon Carn ◽  
Yan Zhang ◽  
Robert J. D. Spurr ◽  
...  

Abstract. Since the fall of 2004, the Ozone Monitoring Instrument (OMI) has been providing global monitoring of volcanic SO2 emissions, helping to understand their climate impacts and to mitigate aviation hazards. Here we introduce a new generation OMI volcanic SO2 dataset based on a principal component analysis (PCA) retrieval technique. To reduce retrieval noise and artifacts as seen in the current operational linear fit (LF) algorithm, the new algorithm, OMSO2VOLCANO, uses characteristic features extracted directly from OMI radiances in the spectral fitting, thereby helping to minimize interferences from various geophysical processes (e.g., O3 absorption) and measurement details (e.g., wavelength shift). To solve the problem of low bias for large SO2 total columns in the LF product, the OMSO2VOLCANO algorithm employs a table lookup approach to estimate SO2 Jacobians (i.e., the instrument sensitivity to a perturbation in the SO2 column amount) and iteratively adjusts the spectral fitting window to exclude shorter wavelengths where the SO2 absorption signals are saturated. To first order, the effects of clouds and aerosols are accounted for using a simple Lambertian equivalent reflectivity approach. As with the LF algorithm, OMSO2VOLCANO provides total column retrievals based on a set of pre-defined SO2 profiles from the lower troposphere to the lower stratosphere, including a new profile peaked at 13 km for plumes in the upper troposphere. Examples given in this study indicate that the new dataset shows significant improvement over the LF product, with at least 50 % reduction in retrieval noise over the remote Pacific. For large eruptions such as Kasatochi in 2008 (~ 1700 kt total SO2) and Sierra Negra in 2005 (> 1100 DU maximal SO2), OMSO2VOLCANO generally agrees well with other algorithms that also utilize the full spectral content of satellite measurements, while the LF algorithm tends to underestimate SO2. We also demonstrate that, despite the coarser spatial and spectral resolution of the Suomi National Polar-orbiting Partnership (Suomi-NPP) Ozone Mapping and Profiler Suite (OMPS) instrument, application of the new PCA algorithm to OMPS data produces highly consistent retrievals between OMI and OMPS. The new PCA algorithm is therefore capable of continuing the volcanic SO2 data record well into the future using current and future hyperspectral UV satellite instruments.


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