scholarly journals CO source contribution analysis for California during ARCTAS-CARB

2011 ◽  
Vol 11 (2) ◽  
pp. 3627-3661 ◽  
Author(s):  
G. G. Pfister ◽  
J. Avise ◽  
C. Wiedinmyer ◽  
D. P. Edwards ◽  
L. K. Emmons ◽  
...  

Abstract. Air pollution is of concern in many parts of California and is impacted by both local emissions and also by pollution inflow from the Pacific. In this study, we use the regional chemical transport model WRF-Chem V3.2 to examine the CO budget over California. We include model CO tracers for different emission sources in the model, which allow estimating the relative importance of local sources versus pollution inflow on the distribution of CO at the surface and in the free troposphere. The focus of our study is on the 15 June–15 July 2008 time period, which coincides with the aircraft deployment of the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission over California. Model simulations are evaluated using these aircraft observations as well as satellite retrievals and surface observations of CO. Evaluation results show that the model overall predicts the observed CO fields well, but points towards an underestimate of CO from the fires in Northern California, which had a strong influence during the study period, and towards a slight overestimate of CO from pollution inflow and local anthropogenic sources. The analysis of the CO budget over California reveals that inflow of CO explains on average 53 ± 21% of surface CO during the study period, compared to 22 ± 18% for local anthropogenic sources and 18 ± 22% for fires. In the free troposphere, the average CO contributions are estimated as 78 ± 16% for CO inflow, 6 ± 4% for CO from local anthropogenic sources and 11 ± 13% for CO from fires.

2011 ◽  
Vol 11 (15) ◽  
pp. 7515-7532 ◽  
Author(s):  
G. G. Pfister ◽  
J. Avise ◽  
C. Wiedinmyer ◽  
D. P. Edwards ◽  
L. K. Emmons ◽  
...  

Abstract. Air pollution is of concern in many parts of California and is impacted by both local emissions and also by pollution inflow from the North Pacific Ocean. In this study, we use the regional chemical transport model WRF-Chem V3.2 together with the global Model for OZone and Related Chemical Tracers to examine the CO budget over California. We include model CO tracers for different emission sources in the models, which allow estimation of the relative importance of local sources versus pollution inflow on the distribution of CO at the surface and in the free troposphere. The focus of our study is on the 15 June–15 July 2008 time period, which coincides with the aircraft deployment of the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) mission over California. Model simulations are evaluated using these aircraft observations as well as satellite retrievals and surface observations of CO. Evaluation results show that the model overall predicts the observed CO fields well, but points towards an underestimate of CO from the fires in Northern California, which had a strong influence during the study period, and towards a slight overestimate of CO from pollution inflow and local anthropogenic sources. The analysis of the CO budget over California reveals that inflow of CO explains on average 99 ± 11 ppbV of surface CO during the study period, compared to 61 ± 95 ppbV for local anthropogenic direct emissions of CO and 84 ± 194 ppbV for fires. In the free troposphere, the average CO contributions are estimated as 96 ± 7 ppbV for CO inflow, 8 ± 9 ppbV for CO from local anthropogenic sources and 18 ± 13 ppbV for CO from fires. Accounting for the low bias in the CO fire emission inventory, the fire impact during the study period might have been up to a factor 4 higher than the given estimates.


2015 ◽  
Vol 15 (1) ◽  
pp. 99-112 ◽  
Author(s):  
Z. Jiang ◽  
J. R. Worden ◽  
D. B. A. Jones ◽  
J.-T. Lin ◽  
W. W. Verstraeten ◽  
...  

Abstract. Rapid industrialization in Asia in the last two decades has resulted in a significant increase in Asian ozone (O3) precursor emissions with likely a corresponding increase in the export of O3 and its precursors. However, the relationship between this increasing O3, the chemical environment, O3 production efficiency, and the partitioning between anthropogenic and natural precursors is unclear. In this work, we use satellite measurements of O3, CO and NO2 from TES (Tropospheric Emission Spectrometer), MOPITT (Measurement of Pollution In The Troposphere) and OMI (Ozone Monitoring Instrument) to quantify O3 precursor emissions for 2006 and their impact on free tropospheric O3 over northeastern Asia, where pollution is typically exported globally due to strong westerlies. Using the GEOS-Chem (Goddard Earth Observing System Chemistry) global chemical transport model, we test the modeled seasonal and interannual variation of O3 based on prior and updated O3 precursor emissions where the updated emissions of CO and NOx are based on satellite measurements of CO and NO2. We show that the observed TES O3 variability and amount are consistent with the model for these updated emissions. However, there is little difference in the modeled ozone between the updated and prior emissions. For example, for the 2006 June time period, the prior and posterior NOx emissions were 14% different over China but the modeled ozone in the free troposphere was only 2.5% different. Using the adjoint of GEOS-Chem we partition the relative contributions of natural and anthropogenic sources to free troposphere O3 in this region. We find that the influence of lightning NOx in the summer is comparable to the contribution from surface emissions but smaller for other seasons. China is the primary contributor of anthropogenic CO, emissions and their export during the summer. While the posterior CO emissions improved the comparison between model and TES by 32%, on average, this change also had only a small effect on the free tropospheric ozone. Our results show that the influence of India and southeastern Asia emissions on O3 pollution export to the northwestern Pacific is sizeable, comparable with Chinese emissions in winter, about 50% of Chinese emissions in spring and fall, and approximately 20% of the emissions in the summer.


2016 ◽  
Author(s):  
Lei Zhu ◽  
Daniel J. Jacob ◽  
Patrick S. Kim ◽  
Jenny A. Fisher ◽  
Karen Yu ◽  
...  

Abstract. Formaldehyde (HCHO) column data from satellites are widely used as a proxy for emissions of volatile organic compounds (VOCs), but validation of the data has been extremely limited. Here we use highly accurate HCHO aircraft observations from the NASA SEAC4RS campaign over the Southeast US in August–September 2013 to validate and intercompare six operational and research retrievals of HCHO columns from four different satellite instruments (OMI, GOME2A, GOME2B and OMPS) and three different research groups. The GEOS-Chem chemical transport model provides a common intercomparison platform. We find that all retrievals capture the HCHO maximum over Arkansas and Louisiana, reflecting high emissions of biogenic isoprene, and are consistent in their spatial variability over the Southeast US (r = 0.4–0.8 on a 0.5° × 0.5° grid) as well as their day-to-day variability (r = 0.5–0.8). However, all satellite retrievals are biased low in the mean by 20–51 %, which would lead to corresponding bias in estimates of isoprene emissions from the satellite data. The smallest bias is for OMI-BIRA, which has the highest corrected slant columns and the lowest scattering weights in its air mass factor (AMF) calculation. Correcting the assumed HCHO vertical profiles (shape factors) used in the AMF calculation would further reduce the bias in the OMI-BIRA data. We conclude that current satellite HCHO data provide a reliable proxy for isoprene emission variability but with a low mean bias due both to the corrected slant columns and the scattering weights used in the retrievals.


2011 ◽  
Vol 11 (10) ◽  
pp. 27887-27911
Author(s):  
K. J. Wecht ◽  
D. J. Jacob ◽  
S. C. Wofsy ◽  
E. A. Kort ◽  
J. R. Worden ◽  
...  

Abstract. We validate satellite methane observations from the Tropospheric Emission Spectrometer (TES) with 151 aircraft vertical profiles over the Pacific from the HIAPER Pole-to-Pole Observation (HIPPO) program. We find that a collocation window of ±750 km and ±24 h does not introduce significant error in comparing TES and aircraft profiles. We validate both the TES standard product (V004) and an experimental product with two pieces of information in the vertical (V005). We determine a V004 mean bias of 65.7 ppb with residual standard deviation of 44.2 ppb. For V005 we determine mean biases (residual standard deviations) in the lower and upper troposphere of 18.2 (31.1) and 49.4 (33.2) ppb, respectively. TES errors show no significant dependence on latitude or surface type. Even when V005 cannot retrieve two pieces of information it still performs better than V004. An observation system simulation experiment (OSSE) with the GEOS-Chem chemical transport model (CTM) and its adjoint shows that TES V004 has only limited value for constraining methane sources. Our successful validation of V005 encourages its production as a standard retrieval to replace V004.


2012 ◽  
Vol 12 (4) ◽  
pp. 1823-1832 ◽  
Author(s):  
K. J. Wecht ◽  
D. J. Jacob ◽  
S. C. Wofsy ◽  
E. A. Kort ◽  
J. R. Worden ◽  
...  

Abstract. We validate satellite methane observations from the Tropospheric Emission Spectrometer (TES) with 151 aircraft vertical profiles over the Pacific from the HIAPER Pole-to-Pole Observation (HIPPO) program. We find that a collocation window of ±750 km and ±24 h does not introduce significant error in comparing TES and aircraft profiles. We validate both the TES standard product (V004) and an experimental product with two pieces of information in the vertical (V005). We determine a V004 mean bias of 65.8 ppb and random instrument error of 43.3 ppb. For V005 we determine a mean bias of 42.3 ppb and random instrument error of 26.5 ppb in the upper troposphere, and mean biases (random instrument errors) in the lower troposphere of 28.8 (28.7) and 16.9 (28.9) ppb at high and low latitudes respectively. Even when V005 cannot retrieve two pieces of information it still performs better than V004. An observation system simulation experiment (OSSE) with the GEOS-Chem chemical transport model (CTM) and its adjoint shows that TES V004 has only limited value for constraining methane sources. Our successful validation of V005 encourages its production as a standard retrieval to replace V004.


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.


2011 ◽  
Vol 11 (17) ◽  
pp. 9253-9269 ◽  
Author(s):  
J. Angelbratt ◽  
J. Mellqvist ◽  
D. Simpson ◽  
J. E. Jonson ◽  
T. Blumenstock ◽  
...  

Abstract. Trends in the CO andC2H6 partial columns ~0–15 km) have been estimated from four European ground-based solar FTIR (Fourier Transform InfraRed) stations for the 1996–2006 time period. The CO trends from the four stations Jungfraujoch, Zugspitze, Harestua and Kiruna have been estimated to −0.45 ± 0.16% yr−1, −1.00 ± 0.24% yr−1, −0.62 ± 0.19 % yr−1 and −0.61 ± 0.16% yr−1, respectively. The corresponding trends for C2H6 are −1.51 ± 0.23% yr−1, −2.11 ± 0.30% yr−1, −1.09 ± 0.25% yr−1 and −1.14 ± 0.18% yr−1. All trends are presented with their 2-σ confidence intervals. To find possible reasons for the CO trends, the global-scale EMEP MSC-W chemical transport model has been used in a series of sensitivity scenarios. It is shown that the trends are consistent with the combination of a 20% decrease in the anthropogenic CO emissions seen in Europe and North America during the 1996–2006 period and a 20% increase in the anthropogenic CO emissions in East Asia, during the same time period. The possible impacts of CH4 and biogenic volatile organic compounds (BVOCs) are also considered. The European and global-scale EMEP models have been evaluated against the measured CO and C2H6 partial columns from Jungfraujoch, Zugspitze, Bremen, Harestua, Kiruna and Ny-Ålesund. The European model reproduces, on average the measurements at the different sites fairly well and within 10–22% deviation for CO and 14–31% deviation for C2H6. Their seasonal amplitude is captured within 6–35% and 9–124% for CO and C2H6, respectively. However, 61–98% of the CO and C2H6 partial columns in the European model are shown to arise from the boundary conditions, making the global-scale model a more suitable alternative when modeling these two species. In the evaluation of the global model the average partial columns for 2006 are shown to be within 1–9% and 37–50% of the measurements for CO and C2H6, respectively. The global model sensitivity for assumptions made in this paper is also analyzed.


2012 ◽  
Vol 12 (1) ◽  
pp. 623-689 ◽  
Author(s):  
G. W. Mann ◽  
K. S. Carslaw ◽  
D. A. Ridley ◽  
D. V. Spracklen ◽  
K. J. Pringle ◽  
...  

Abstract. A global modal aerosol microphysics module (GLOMAP-mode) is evaluated and improved by comparing against a sectional version (GLOMAP-bin) and observations in the same 3-D global offline chemistry transport model. With both schemes, the model captures the main features of the global particle size distribution, with sub-micron aerosol approximately unimodal in continental regions and bi-modal in marine regions. Initial bin-mode comparisons showed that various size distribution parameter settings (mode widths and inter-modal separation sizes) resulted in clear biases compared to the sectional scheme. By adjusting these parameters in the modal scheme, much better agreement is achieved against the bin scheme and observations. Surface mass of sulphate, sea-salt, black carbon (BC) and organic carbon (OC) are, on the annual mean, within 25 % in the two schemes in nearly all regions. On the annual mean, surface level concentrations of condensation nuclei (CN), cloud condensation nuclei (CCN), surface area density and condensation sink also compare within 25 % in most regions. However, marine CCN concentrations between 30° N and 30° S are systematically higher in the modal scheme, by 25–60 %, which we attribute to differences in size-resolved particle growth or cloud-processing. Larger differences also exist in regions or seasons dominated by biomass burning and in free-troposphere and high-latitude regions. Indeed, in the free-troposphere, GLOMAP-mode BC is a factor 2–4 higher than GLOMAP-bin, likely due to differences in size-resolved scavenging. Nevertheless, in most parts of the atmosphere, we conclude that bin-mode differences are much less than model-observation differences, although some processes are missing in these runs which may pose a bigger challenge to modal schemes (e.g. boundary layer nucleation, ultra-fine sea-spray). The findings here underline the need for a spectrum of complexity in global models, with size-resolved aerosol properties predicted by modal schemes needing to be continually benchmarked and improved against freely evolving sectional schemes and observations.


2021 ◽  
Author(s):  
Emily Dowd ◽  
Christopher Wilson ◽  
Martyn Chipperfield ◽  
Manuel Gloor

<p>Methane (CH<sub>4</sub>) is the second most important atmospheric greenhouse gas after carbon dioxide. Global concentrations of CH<sub>4</sub> have been rising in the last decade and our understanding of what is driving the increase remains incomplete. Natural sources, such as wetlands, contribute to the uncertainty of the methane budget. However, anthropogenic sources, such as fossil fuels, present an opportunity to mitigate the human contribution to climate change on a relatively short timescale, since CH<sub>4</sub> has a much shorter lifetime than carbon dioxide. Therefore, it is important to know the relative contributions of these sources in different regions.</p><p>We have investigated the inter-annual variation (IAV) and rising trend of CH<sub>4</sub> concentrations using a global 3-D chemical transport model, TOMCAT. We independently tagged several regional natural and anthropogenic CH<sub>4</sub> tracers in TOMCAT to identify their contribution to the atmospheric CH<sub>4</sub> concentrations over the period 2009 – 2018. The tagged regions were selected based on the land surface types and the predominant flux sector within each region and include subcontinental regions, such as tropical South America, boreal regions and anthropogenic regions such as Europe. We used surface CH<sub>4</sub> fluxes derived from a previous TOMCAT-based atmospheric inversion study (Wilson et al., 2020). These atmospheric inversions were constrained by satellite and surface flask observations of CH<sub>4</sub>, giving optimised monthly estimates for fossil fuel and non-fossil fuel emissions on a 5.6° horizontal grid. During the study period, the total optimised CH<sub>4</sub> flux grew from 552 Tg/yr to 593 Tg/yr. This increase in emissions, particularly in the tropics, contributed to the increase in atmospheric CH<sub>4 </sub>concentrations and added to the imbalance in the CH<sub>4</sub> budget. We will use the results of the regional tagged tracers to quantify the contribution of regional methane emissions at surface observation sites, and to quantify the contributions of the natural and anthropogenic emissions from the tagged regions to the IAV and the rising methane concentrations.</p><p>Wilson, C., Chipperfield, M. P., Gloor, M., Parker, R. J., Boesch, H., McNorton, J., Gatti, L. V., Miller, J. B., Basso, L. S., and Monks, S. A.: Large and increasing methane emissions from Eastern Amazonia derived from satellite data, 2010–2018, Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2020-1136, in review, 2020.</p>


2021 ◽  
Author(s):  
Kazuki Kamezaki ◽  
Shohei Hattori ◽  
Naohiro Yoshida

<p>Carbonyl sulfide (OCS), the most abundant sulfur-containing gas in the ambient atmosphere, possesses great potential for tracer of the carbon cycle. Sulfur isotopic composition (<sup>34</sup>S/<sup>32</sup>S ratio, δ<sup>34</sup>S) on OCS is a feasible tool to evaluate the OCS budget. We applied the sulfur isotope measurement for the tropospheric OCS cycle and distinguished OCS sources from oceanic and anthropogenic emissions.</p><p> </p><p>Here, we present a developed measurement system of δ<sup>34</sup>S of OCS and the result of latitudinal (north-south) observations of OCS within Japan using the method. The OCS sampling system was carried to three sampling sites in Japan: Miyakojima (24°8’N, 125°3’E), Yokohama (35°5’N, 139°5’E), and Otaru (43°1’N, 141°2’E). The observed δ<sup>34</sup>Sof OCS ranging from 9.7 to 14.5‰ reflects the tropospheric OCS cycle. Particularly in winter, latitudinal decreases in δ<sup>34</sup>Svalues were found to be correlated with increases in OCS concentrations, resulting in an intercept of (4.7 ± 0.8)‰ in the Keeling plot approach. This trend suggests the transport of anthropogenic OCS emissions from the Asian continent to the western Pacific by the Asian monsoon outflow.</p><p> </p><p>The estimated background δ<sup>34</sup>S of OCS in eastern Asia is consistent with the δ<sup>34</sup>S of OCS previously reported in Israel and the Canary Islands, suggesting that the background δ<sup>34</sup>S of OCS in the Northern Hemisphere ranges from 12.0 to 13.5‰. Our constructed sulfur isotopic mass balance of OCS revealed that anthropogenic sources, not merely oceanic sources, account for much of the missing source of atmospheric OCS. This sulfur isotopic constraint on atmospheric OCS is an important step together with isotopic characterizations and analysis using a chemical transport model, will enable detailed quantitative OCS budget and estimation of gross primary production.</p>


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