scholarly journals Contribution of Asian emissions to upper tropospheric CO over the remote Pacific

2021 ◽  
Author(s):  
Linda Smoydzin ◽  
Peter Hoor

Abstract. We use CO data from the MOPITT satellite instrument from 2000–2019 to compose a climatology of severe pollution events in the mid- and upper troposphere over the northern-hemispheric (NH-) Pacific. To link each individual pollution event detected by MOPITT with a CO source region, we performed trajectory calculations using MPTRAC, a lagrangian transport model. To analyse transport pathways and uplift mechanisms we combine MOPITT data, the trajectory calculations and ERA-Interim reanalysis data. Events of elevated CO which we detect at level between 500 hPa and 300 hPa over the NH-Pacific throughout the year, occur with a surprisingly high regularity and frequency (70 % of all days during winter, 80 % respectively during spring). Our study further indicates, that the spatial coverage of individual upper tropospheric pollution cluster increased in spring time during the 20 years we analysed. The position of upper tropospheric pollution plumes show a strong seasonal cycle. During winter, most pollution events are detected over the north-eastern and central NH-Pacific, during spring over the central NH-Pacific and during summer over the western NH-Pacific. We detect most pollution episodes during spring. Trajectory simulations reveal China as the major CO-source region throughout the year. The contribution of other source regions shows a strong seasonal cycle: NE-Asia is a significant CO-source region during winter and summer while India and SE-Asia are important source regions mainly during spring.

2020 ◽  
Author(s):  
Nikos Daskalakis ◽  
Maria Kanakidou ◽  
Mihalis Vrekoussis ◽  
Laura Gallardo

<p>Carbon Monoxide (CO) is an important atmospheric trace gas, and among the key O<sub>3</sub> precursors in the troposphere, alongside NO<sub>x</sub> and VOCs. It is among the most important sinks of OH radical in the atmosphere, which controls lifetime of CH<sub>4</sub> — a major greenhouse gas. Biomass burning sources contribute about 25% to the global emissions of CO, with the remaining CO being either emitted from anthropogenic sources, or being chemically formed in the atmosphere. Because of CO tropospheric lifetime is about two months; it can be transported in the atmosphere thus its sources have a hemispheric impact on atmospheric composition.</p><p>The extent of the impact of biomass burning to remote areas of the world through long range transport is here investigated using the global 3-dimensional chemistry transport model TM4-ECPL. For this, tagged biomass burning CO tracers from the 13 different HTAP (land) source regions are used in the model in order to evaluate the contribution of each source region to the CO concentrations in the 170 HTAP receptor regions that originate from biomass burning. The global simulations cover the period 1994—2015 in order to derive climatological transport patterns for CO and assess the contribution of each of the source regions to each of the receptor regions in the global troposphere. The CO simulations are evaluated by comparison with satellite observations from MOPITT and ground based observations from WDCGG. We show the significant impact of biomass burning emissions to the most remote regions of the world.</p>


2011 ◽  
Vol 51 (2) ◽  
pp. 715 ◽  
Author(s):  
Peter Southgate ◽  
Keith Sircombe ◽  
Christopher Lewis

A pilot study to determine if zircons present in reservoir facies of the North West Shelf can be used to identify provenance and sediment transport pathways has analysed samples from three wells: Guardian–1 and Hijinx–1 (Carnarvon Basin), and Burnside–1 (Browse Basin). Operating companies Chevron, Santos and Hess collected 3–5 kg of cuttings from sandstone bodies intersected in the three wells. Samples were sent to Geoscience Australia for zircon separation and analysis at the Geochronology Laboratory on a sensitive high-resolution ion microprobe (SHRIMP). To provide a statistically meaningful representation of ages in each sample, 70–80 grains were randomly selected for analysis. During the past 20 years, Geoscience Australia and the state geological surveys of WA, NT, Queensland and SA, together with the ANU, UWA and Curtin University, have analysed zircons found in igneous and sedimentary rocks that outcrop in WA and central Australia. This analysis has been done to determine the ages of emplacement, extrusion or maximum depositional ages. This dataset permits the ages of potential onshore provenance areas to be differentiated; hence, correlations can be made between zircons contained within the transported sands and their potential source regions from onshore Australia. In this extended abstract, the spectrum of ages in each sample will be shown, and potential provenance and sediment transport pathways will be discussed. The abstract concludes with the outline of a 2–3 year project to obtain a dataset that will provide a regional stratigraphic and spatial coverage of the North West Shelf for provenance studies.


2011 ◽  
Vol 11 (4) ◽  
pp. 1549-1564 ◽  
Author(s):  
A. K. Halse ◽  
M. Schlabach ◽  
S. Eckhardt ◽  
A. Sweetman ◽  
K. C. Jones ◽  
...  

Abstract. Passive air samplers (PAS) were deployed at 86 European background sites during summer 2006 in order (i) to gain further insight into spatial patterns of persistent organic pollutants (POPs) in European background air and, (ii) to evaluate PAS as an alternative sampling technique under EMEP (Co-operative programme for monitoring and evaluation of the long-range transmissions of air pollutants in Europe). The samples were analyzed for selected PCBs, HCHs, DDTs, HCB, PAHs and chlordanes, and air concentrations were calculated on the basis of losses of performance reference compounds. Air concentrations of PCBs were generally lowest in more remote areas of northern Europe with elevated levels in more densely populated areas. γ-HCH was found at elevated levels in more central parts of Europe, whereas α-HCH, β-HCH and DDTs showed higher concentrations in the south-eastern part. There was no clear spatial pattern in the concentrations for PAHs, indicative of influence by local sources, rather than long range atmospheric transport (LRAT). HCB was evenly distributed across Europe, while the concentrations of chlordanes were typically low or non-detectable. A comparison of results obtained on the basis of PAS and active air sampling (AAS) illustrated that coordinated PAS campaigns have the potential serve as useful inter-comparison exercises within and across existing monitoring networks. The results also highlighted limitations of the current EMEP measurement network with respect to spatial coverage. We finally adopted an existing Lagrangian transport model (FLEXPART) as recently modified to incorporate key processes relevant for POPs to evaluate potential source regions affecting observed concentrations at selected sites. Using PCB-28 as an example, the model predicted concentrations which agreed within a factor of 3 with PAS measurements for all except 1 out of the 17 sites selected for this analysis.


2017 ◽  
Author(s):  
Jenny A. Fisher ◽  
Lee T. Murray ◽  
Dylan B. A. Jones ◽  
Nicholas M. Deutscher

Abstract. Carbon monoxide (CO) simulation in atmospheric chemistry models is frequently used for source-receptor analysis, emission inversion, interpretation of observations, and chemical forecasting due to its computational efficiency and ability to quantitatively link simulated CO burdens to sources. While several methods exist for modelling CO source attribution, most are inappropriate for regions where the CO budget is dominated by secondary production rather than direct emissions. Here, we introduce a major update to the linear CO-only capability in the GEOS-Chem chemical transport model that for the first time allows source-region tagging of secondary CO produced from oxidation of non-methane volatile organic compounds. Our updates also remove fundamental inconsistencies between the CO-only simulation and the standard full chemistry simulation by using consistent CO production rates in both. We find that relative to the standard chemistry simulation, CO in the original CO-only simulation was overestimated by more than 100 ppb in the model surface layer and underestimated in outflow regions. The improved CO-only simulation largely resolves these discrepancies by improving both the magnitude and location of secondary production. Despite large differences between the original and improved simulations, however, model evaluation with the global dataset used to benchmark GEOS-Chem shows negligible change to the model's ability to match the observations. This suggests that the current GEOS-Chem benchmark is not well suited to evaluate model changes in regions influenced by biogenic emissions and chemistry, and expanding the dataset to include observations from biogenic source regions (including those from recent aircraft campaigns) should be a priority for the GEOS-Chem community. Using Australasia as a case study, we show that the new ability to geographically tag secondary CO production provides significant added value for interpreting observations and model results in regions where primary CO emissions are low. Secondary production dominates the CO budget across much of the world, especially in the southern hemisphere, and we recommend future model-observation and multi-model comparisons implement this capability to provide a more complete understanding of CO sources and their variability.


2017 ◽  
Vol 10 (11) ◽  
pp. 4129-4144 ◽  
Author(s):  
Jenny A. Fisher ◽  
Lee T. Murray ◽  
Dylan B. A. Jones ◽  
Nicholas M. Deutscher

Abstract. Carbon monoxide (CO) simulation in atmospheric chemistry models is frequently used for source–receptor analysis, emission inversion, interpretation of observations, and chemical forecasting due to its computational efficiency and ability to quantitatively link simulated CO burdens to sources. While several methods exist for modeling CO source attribution, most are inappropriate for regions where the CO budget is dominated by secondary production rather than direct emissions. Here, we introduce a major update to the linear CO-only capability in the GEOS-Chem chemical transport model that for the first time allows source–region tagging of secondary CO produced from oxidation of non-methane volatile organic compounds. Our updates also remove fundamental inconsistencies between the CO-only simulation and the standard full chemistry simulation by using consistent CO production rates in both. We find that relative to the standard chemistry simulation, CO in the original CO-only simulation was overestimated by more than 100 ppb in the model surface layer and underestimated in outflow regions. The improved CO-only simulation largely resolves these discrepancies by improving both the magnitude and location of secondary production. Despite large differences between the original and improved simulations, however, model evaluation with the global dataset used to benchmark GEOS-Chem shows negligible change to the model's ability to match the observations. This suggests that the current GEOS-Chem benchmark is not well suited to evaluate model changes in regions influenced by biogenic emissions and chemistry, and expanding the dataset to include observations from biogenic source regions (including those from recent aircraft campaigns) should be a priority for the GEOS-Chem community. Using Australasia as a case study, we show that the new ability to geographically tag secondary CO production provides significant added value for interpreting observations and model results in regions where primary CO emissions are low. Secondary production dominates the CO budget across much of the world, especially in the Southern Hemisphere, and we recommend future model–observation and multi-model comparisons implement this capability to provide a more complete understanding of CO sources and their variability.


2019 ◽  
Author(s):  
Kunal Bali ◽  
Sagnik Dey ◽  
Dilip Ganguly ◽  
Krik R. Smith

Abstract. Estimating ambient PM2.5 (fine particulate matter) concentrations in India over many years is challenging because spatial coverage of ground-based monitoring, while better recently, is still inadequate and satellite-based assessment lacks temporal continuity. Here we analyze MERRA-2 reanalysis aerosol products to estimate PM2.5 at hourly scale to fill the space-time sampling gap. MERRA-2 PM2.5 are calibrated and validated (r = 0.94, slope of the regression = 0.99) against coincident in-situ measurements. We present the first space-time variability of ambient PM2.5 diurnal pattern in India for an 18-year (2000–2017) period. Diurnal amplitude is found to be quite large (> 30 μg m−3) in the Indo-Gangetic Basin (IGB) and western arid regions of India. PM2.5 is found to decrease over the western dust source region and increase over the Himalayan foothills and parts of IGB and central India primarily in the morning and evening hours. This increasing trend at an annual scale is primarily governed by a large increase in concentration during Oct–Feb that can be attributed to a combination of the rise in emission and declining boundary layer height. Our results suggest that the satellite-based concentration estimates (typically representative of late morning to early afternoon hours) are lower (magnitude depends on the place and season) than the 24-hour average concentration in most parts of India. In the future, the integration of reanalysis data in concentration modeling may assist in reducing the uncertainty in estimates of air pollution concentration patterns in India and elsewhere.


2010 ◽  
Vol 10 (3) ◽  
pp. 1345-1359 ◽  
Author(s):  
G. G. Pfister ◽  
L. K. Emmons ◽  
D. P. Edwards ◽  
A. Arellano ◽  
T. Campos ◽  
...  

Abstract. We analyze the transport of pollution across the Pacific during the NASA INTEX-B (Intercontinental Chemical Transport Experiment Part B) campaign in spring 2006 and examine how this year compares to the time period for 2000 through 2006. In addition to aircraft measurements of carbon monoxide (CO) collected during INTEX-B, we include in this study multi-year satellite retrievals of CO from the Measurements of Pollution in the Troposphere (MOPITT) instrument and simulations from the chemistry transport model MOZART-4. Model tracers are used to examine the contributions of different source regions and source types to pollution levels over the Pacific. Additional modeling studies are performed to separate the impacts of inter-annual variability in meteorology and dynamics from changes in source strength. Interannual variability in the tropospheric CO burden over the Pacific and the US as estimated from the MOPITT data range up to 7% and a somewhat smaller estimate (5%) is derived from the model. When keeping the emissions in the model constant between years, the year-to-year changes are reduced (2%), but show that in addition to changes in emissions, variable meteorological conditions also impact transpacific pollution transport. We estimate that about 1/3 of the variability in the tropospheric CO loading over the contiguous US is explained by changes in emissions and about 2/3 by changes in meteorology and transport. Biomass burning sources are found to be a larger driver for inter-annual variability in the CO loading compared to fossil and biofuel sources or photochemical CO production even though their absolute contributions are smaller. Source contribution analysis shows that the aircraft sampling during INTEX-B was fairly representative of the larger scale region, but with a slight bias towards higher influence from Asian contributions.


2015 ◽  
Vol 28 (17) ◽  
pp. 6823-6840 ◽  
Author(s):  
Froila M. Palmeiro ◽  
David Barriopedro ◽  
Ricardo García-Herrera ◽  
Natalia Calvo

Abstract Sudden stratospheric warmings (SSWs) are characterized by a pronounced increase of the stratospheric polar temperature during the winter season. Different definitions have been used in the literature to diagnose the occurrence of SSWs, yielding discrepancies in the detected events. The aim of this paper is to compare the SSW climatologies obtained by different methods using reanalysis data. The occurrences of Northern Hemisphere SSWs during the extended-winter season and the 1958–2014 period have been identified for a suite of eight representative definitions and three different reanalyses. Overall, and despite the differences in the number and exact dates of occurrence of SSWs, the main climatological signatures of SSWs are not sensitive to the considered reanalysis. The mean frequency of SSWs is 6.7 events decade−1, but it ranges from 4 to 10 events, depending on the method. The seasonal cycle of events is statistically indistinguishable across definitions, with a common peak in January. However, the multidecadal variability is method dependent, with only two definitions displaying minimum frequencies in the 1990s. An analysis of the mean signatures of SSWs in the stratosphere revealed negligible differences among methods compared to the large case-to-case variability within a given definition. The stronger and more coherent tropospheric signals before and after SSWs are associated with major events, which are detected by most methods. The tropospheric signals of minor SSWs are less robust, representing the largest source of discrepancy across definitions. Therefore, to obtain robust results, future studies on stratosphere–troposphere coupling should aim to minimize the detection of minor warmings.


2017 ◽  
Vol 17 (11) ◽  
pp. 6663-6678 ◽  
Author(s):  
Shreeya Verma ◽  
Julia Marshall ◽  
Mark Parrington ◽  
Anna Agustí-Panareda ◽  
Sebastien Massart ◽  
...  

Abstract. Airborne observations of greenhouse gases are a very useful reference for validation of satellite-based column-averaged dry air mole fraction data. However, since the aircraft data are available only up to about 9–13 km altitude, these profiles do not fully represent the depth of the atmosphere observed by satellites and therefore need to be extended synthetically into the stratosphere. In the near future, observations of CO2 and CH4 made from passenger aircraft are expected to be available through the In-Service Aircraft for a Global Observing System (IAGOS) project. In this study, we analyse three different data sources that are available for the stratospheric extension of aircraft profiles by comparing the error introduced by each of them into the total column and provide recommendations regarding the best approach. First, we analyse CH4 fields from two different models of atmospheric composition – the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecasting System for Composition (C-IFS) and the TOMCAT/SLIMCAT 3-D chemical transport model. Secondly, we consider scenarios that simulate the effect of using CH4 climatologies such as those based on balloons or satellite limb soundings. Thirdly, we assess the impact of using a priori profiles used in the satellite retrievals for the stratospheric part of the total column. We find that the models considered in this study have a better estimation of the stratospheric CH4 as compared to the climatology-based data and the satellite a priori profiles. Both the C-IFS and TOMCAT models have a bias of about −9 ppb at the locations where tropospheric vertical profiles will be measured by IAGOS. The C-IFS model, however, has a lower random error (6.5 ppb) than TOMCAT (12.8 ppb). These values are well within the minimum desired accuracy and precision of satellite total column XCH4 retrievals (10 and 34 ppb, respectively). In comparison, the a priori profile from the University of Leicester Greenhouse Gases Observing Satellite (GOSAT) Proxy XCH4 retrieval and climatology-based data introduce larger random errors in the total column, being limited in spatial coverage and temporal variability. Furthermore, we find that the bias in the models varies with latitude and season. Therefore, applying appropriate bias correction to the model fields before using them for profile extension is expected to further decrease the error contributed by the stratospheric part of the profile to the total column.


2012 ◽  
Vol 27 (3) ◽  
pp. 263-271 ◽  
Author(s):  
Monica Cristina Damião Mendes ◽  
Iracema F. A. Cavalcanti ◽  
Dirceu Luis Herdies

An assessment of blocking episodes over the Southern Hemisphere, selected from the Era-40 and NCEP/NCAR reanalysis are presented in this study. Blocking can be defined by an objective index based on two 500 hPa geopotential height meridional gradients. The seasonal cycle and preferential areas of occurrence are well reproduced by the two data sets. In both reanalysis used in this study, South Pacific and Oceania were the preferred regions for blocking occurrence, followed by the Atlantic Ocean. However the results revealed differences in frequencies of occurrences, which may be related to the choice of assimilation scheme employed to produce the reanalysis data sets. It is important to note that the ERA 40 and NCEP/NCAR reanalysis were produced using consistent models and assimilation schemes throughout the whole reanalyzed period, which are different for each set.


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