scholarly journals Characterizing sources of high surface ozone events in the southwestern US with intensive field measurements and two global models

2020 ◽  
Vol 20 (17) ◽  
pp. 10379-10400
Author(s):  
Li Zhang ◽  
Meiyun Lin ◽  
Andrew O. Langford ◽  
Larry W. Horowitz ◽  
Christoph J. Senff ◽  
...  

Abstract. The detection and attribution of high background ozone (O3) events in the southwestern US is challenging but relevant to the effective implementation of the lowered National Ambient Air Quality Standard (NAAQS; 70 ppbv). Here we leverage intensive field measurements from the Fires, Asian, and Stratospheric Transport−Las Vegas Ozone Study (FAST-LVOS) in May–June 2017, alongside high-resolution simulations with two global models (GFDL-AM4 and GEOS-Chem), to study the sources of O3 during high-O3 events. We show possible stratospheric influence on 4 out of the 10 events with daily maximum 8 h average (MDA8) surface O3 above 65 ppbv in the greater Las Vegas region. While O3 produced from regional anthropogenic emissions dominates pollution events in the Las Vegas Valley, stratospheric intrusions can mix with regional pollution to push surface O3 above 70 ppbv. GFDL-AM4 captures the key characteristics of deep stratospheric intrusions consistent with ozonesondes, lidar profiles, and co-located measurements of O3, CO, and water vapor at Angel Peak, whereas GEOS-Chem has difficulty simulating the observed features and underestimates observed O3 by ∼20 ppbv at the surface. On days when observed MDA8 O3 exceeds 65 ppbv and the AM4 stratospheric ozone tracer shows 20–40 ppbv enhancements, GEOS-Chem simulates ∼15 ppbv lower US background O3 than GFDL-AM4. The two models also differ substantially during a wildfire event, with GEOS-Chem estimating ∼15 ppbv greater O3, in better agreement with lidar observations. At the surface, the two models bracket the observed MDA8 O3 values during the wildfire event. Both models capture the large-scale transport of Asian pollution, but neither resolves some fine-scale pollution plumes, as evidenced by aerosol backscatter, aircraft, and satellite measurements. US background O3 estimates from the two models differ by 5 ppbv on average (greater in GFDL-AM4) and up to 15 ppbv episodically. Uncertainties remain in the quantitative attribution of each event. Nevertheless, our multi-model approach tied closely to observational analysis yields some process insights, suggesting that elevated background O3 may pose challenges to achieving a potentially lower NAAQS level (e.g., 65 ppbv) in the southwestern US.

2019 ◽  
Author(s):  
Li Zhang ◽  
Meiyun Lin ◽  
Andrew O. Langford ◽  
Larry W. Horowitz ◽  
Christoph J. Senff ◽  
...  

Abstract. The detection and attribution of high background ozone (O3) events in the southwestern U.S. is challenging but relevant to the effective implementation of the lowered National Ambient Air Quality Standard (NAAQS; 70 ppbv). Here we leverage intensive field measurements from the Fires, Asian, and Stratospheric TransportLas Vegas Ozone Study (FAST-LVOS) in MayJune 2017, alongside high-resolution simulations with two global models (GFDL-AM4 and GEOS-Chem), to pinpoint the sources of O3 during high-O3 events. We show stratospheric influence on four out of the ten events with daily maximum 8-hour average (MDA8) surface O3 above 65 ppbv in the greater Las Vegas region. While O3 produced from regional anthropogenic emissions dominates pollution in the Las Vegas Valley, stratospheric intrusions can mix with regional pollution to push surface O3 above 70 ppbv. GFDL-AM4 captures the key characteristics of deep stratospheric intrusions consistent with ozonesondes, lidar profiles, and co-located measurements of O3, CO, and water vapor at Angel Peak, whereas GEOS-Chem has difficulty simulating the observed features and underestimates observed O3 by ~ 20 ppbv at the surface. The two models also differ substantially during a wildfire event, with GEOS-Chem estimating ~ 15 ppbv greater O3, in better agreement with lidar observations. At the surface, the two models bracket the observed MDA8 O3 values during the wildfire event. Both models capture the large-scale transport of Asian pollution, but neither resolves some fine-scale pollution plumes, as evidenced from aerosol backscatter, aircraft, and satellite measurements. U.S. background O3 estimates from the two models differ by 5 ppbv on average and up to 15 ppbv episodically. Our multi-model approach tied closely to observational analysis yields process insights, suggesting that elevated background O3 may pose challenges to achieving a potentially lower NAAQS level (e.g., 65 ppbv) in the southwestern U.S.


2015 ◽  
Vol 15 (4) ◽  
pp. 4427-4461 ◽  
Author(s):  
T. P. Canty ◽  
L. Hembeck ◽  
T. P. Vinciguerra ◽  
D. C. Anderson ◽  
D. L. Goldberg ◽  
...  

Abstract. Regulatory air quality models, such as the Community Multiscale Air Quality model (CMAQ), are used by federal and state agencies to guide policy decisions that determine how to best achieve adherence with National Ambient Air Quality Standards for surface ozone. We use observations of ozone and its important precursor NO2 to test the representation of the photochemistry and emission of ozone precursors within CMAQ. Observations of tropospheric column NO2 from the Ozone Monitoring Instrument (OMI), retrieved by two independent groups, show that the model overestimates urban NO2 and underestimates rural NO2 under all conditions examined for July and August 2011 in the US Northeast. The overestimate of the urban to rural ratio of tropospheric column NO2 for this baseline run of CMAQ (CB05 mechanism, mobile NOx emissions from the National Emissions Inventory; isoprene emissions from MEGAN v2.04) suggests this model may under estimate the importance of interstate transport of NOx. This CMAQ simulation leads to a considerable overestimate of the 2 month average of 8 h daily maximum surface ozone in the US Northeast, as well as an overestimate of 8 h ozone at AQS sites during days when the state of Maryland experienced NAAQS exceedances. We have implemented three changes within CMAQ motivated by OMI NO2 as well as aircraft observations obtained in July 2011 during the NASA DISCOVER-AQ campaign: (a) the modeled lifetime of organic nitrates within CB05 has been reduced by a factor of 10, (b) emissions of NOx from mobile sources has been reduced by a factor of 2, and (c) isoprene emissions have been reduced by using MEGAN v2.10 rather than v2.04. Compared to the baseline simulation, the CMAQ run using all three of these changes leads to a considerably better simulation of the ratio of urban to rural column NO2, better agreement with the 2 month average of daily 8 h maximum ozone in the US Northeast, fewer number of false positives of an ozone exceedance throughout the domain, as well as an unbiased simulation of surface ozone at ground based AQS sites in Maryland that experienced an ozone exceedance during July and August 2007. These modifications to CMAQ may provide a framework for use in studies focused on achieving future adherence to specific air quality standards for surface ozone by reducing emission of NOx from various anthropogenic sectors.


2021 ◽  
Vol 880 (1) ◽  
pp. 012004
Author(s):  
H Mahidin ◽  
M T Latif ◽  
A Hamdan ◽  
J Salleh ◽  
D Dominick ◽  
...  

Abstract Sarawak Region of Malaysia is currently experiencing a high demand for capital needs such as transformation forest to plantations, economic development, and improving transportation systems. Those land cover changes will increase primary pollutant emissions and trigger surface O3 formation. Surface O3 is a secondary pollutant and a significant greenhouse gas contributing to climate change and declining air quality. In this study, variations in surface O3 concentrations at urban and suburban sites in Sarawak were explored using the Malaysian Department of Environment data spanning a two-year cycle (2018-2019). The primary aim of this study is to ascertain the variation of surface O3 concentrations reported at four monitoring stations in Sarawak, namely Kuching (SQ1) (Urban), Sibu (SQ2) (Suburban), Bintulu (SQ3) (Suburban), and Miri (SQ4) (Suburban). The study also analysed the relationship between O3 distribution and nitrogen oxides (NO and NO2). The findings showed that O3 concentrations observed in the region during the study period were lower than the maximum permissible value of 100 ppbv suggested by the Malaysian Ambient Air Quality Standard (2020). SQ4 (Miri) at suburban sites recorded the highest average surface O3 concentrations with an hourly average and daily maximum O3 concentration of 15.7 and 89.5 ppbv, respectively. Temperatures, UV exposure, and wind speed all impact the concentration of surface O3 in Sarawak. In all stations, concentrations of O3 were inversely linked with NO, NO2, and relative humidity (RH). This research will assist the relevant agency in forecast, monitor, and mitigate the level of O3 in the ambient environment, especially in the Sarawak Region.


2020 ◽  
Author(s):  
Chaitri Roy ◽  
Suvarna Fadnavis ◽  
Sabin Thazhe Purayil

<p>Ozone in the upper troposphere is a dominant radiative constituent.  In this study, we investigate ozone variability due to stratospheric intrusions in the upper troposphere over India, and its associated radiative impacts during monsoon breaks co-occurring with El Niño. For this purpose, we use the ECHAM5-HAMMOZ, Global-Chemistry-climate model simulations, and ERA-Interim reanalysis data. Our analysis shows that during El Niño deep stratospheric intrusions, occurring at the North India - Tibetan Plateau (NI-TP) region and the western edge of the monsoon anticyclone, lead to an enormous increase in ozone amounts (~160 ppb) in the upper troposphere over India. These intrusions elevate the surface ozone levels by ~20 ppb and ozone radiative forcing by ~0.33 W m<sup>-2</sup> at the top of the atmosphere (TOA). </p><p>Interestingly, the stratospheric intrusions are associated with a wave train composed of cyclonic and anticyclonic circulation in the upper troposphere, emanating from El-Niño region in the east Pacific, traversing towards NI-TP locale. The wave train transports extra-tropical cold air mass, producing an anomalous cooling of ~2 - 3 K in the upper troposphere over NI-TP. The cold wave train induces Rossby wave breaking (RWB), which facilitates stratospheric intrusions, thereby enhancing subsidence over NI-TP region. Additionally, this severe cold subsidence over North India during break days may further intensify the deficit rainfall condition during break days.</p>


2016 ◽  
Vol 113 (40) ◽  
pp. 11131-11136 ◽  
Author(s):  
Mang Lin ◽  
Lin Su ◽  
Robina Shaheen ◽  
Jimmy C. H. Fung ◽  
Mark H. Thiemens

The extent to which stratospheric intrusions on synoptic scales influence the tropospheric ozone (O3) levels remains poorly understood, because quantitative detection of stratospheric air has been challenging. Cosmogenic 35S mainly produced in the stratosphere has the potential to identify stratospheric air masses at ground level, but this approach has not yet been unambiguously shown. Here, we report unusually high 35S concentrations (7,390 atoms m−3; ∼16 times greater than annual average) in fine sulfate aerosols (aerodynamic diameter less than 0.95 µm) collected at a coastal site in southern California on May 3, 2014, when ground-level O3 mixing ratios at air quality monitoring stations across southern California (43 of 85) exceeded the recently revised US National Ambient Air Quality Standard (daily maximum 8-h average: 70 parts per billion by volume). The stratospheric origin of the significantly enhanced 35S level is supported by in situ measurements of air pollutants and meteorological variables, satellite observations, meteorological analysis, and box model calculations. The deep stratospheric intrusion event was driven by the coupling between midlatitude cyclones and Santa Ana winds, and it was responsible for the regional O3 pollution episode. These results provide direct field-based evidence that 35S is an additional sensitive and unambiguous tracer in detecting stratospheric air in the boundary layer and offer the potential for resolving the stratospheric influences on the tropospheric O3 level.


2018 ◽  
Vol 18 (12) ◽  
pp. 8727-8744 ◽  
Author(s):  
Stefano Galmarini ◽  
Ioannis Kioutsioukis ◽  
Efisio Solazzo ◽  
Ummugulsum Alyuz ◽  
Alessandra Balzarini ◽  
...  

Abstract. In this study we introduce a hybrid ensemble consisting of air quality models operating at both the global and regional scale. The work is motivated by the fact that these different types of models treat specific portions of the atmospheric spectrum with different levels of detail, and it is hypothesized that their combination can generate an ensemble that performs better than mono-scale ensembles. A detailed analysis of the hybrid ensemble is carried out in the attempt to investigate this hypothesis and determine the real benefit it produces compared to ensembles constructed from only global-scale or only regional-scale models. The study utilizes 13 regional and 7 global models participating in the Hemispheric Transport of Air Pollutants phase 2 (HTAP2)–Air Quality Model Evaluation International Initiative phase 3 (AQMEII3) activity and focuses on surface ozone concentrations over Europe for the year 2010. Observations from 405 monitoring rural stations are used for the evaluation of the ensemble performance. The analysis first compares the modelled and measured power spectra of all models and then assesses the properties of the mono-scale ensembles, particularly their level of redundancy, in order to inform the process of constructing the hybrid ensemble. This study has been conducted in the attempt to identify that the improvements obtained by the hybrid ensemble relative to the mono-scale ensembles can be attributed to its hybrid nature. The improvements are visible in a slight increase of the diversity (4 % for the hourly time series, 10 % for the daily maximum time series) and a smaller improvement of the accuracy compared to diversity. Root mean square error (RMSE) improved by 13–16 % compared to G and by 2–3 % compared to R. Probability of detection (POD) and false-alarm rate (FAR) show a remarkable improvement, with a steep increase in the largest POD values and smallest values of FAR across the concentration ranges. The results show that the optimal set is constructed from an equal number of global and regional models at only 15 % of the stations. This implies that for the majority of the cases the regional-scale set of models governs the ensemble. However given the high degree of redundancy that characterizes the regional-scale models, no further improvement could be expected in the ensemble performance by adding yet more regional models to it. Therefore the improvement obtained with the hybrid set can confidently be attributed to the different nature of the global models. The study strongly reaffirms the importance of an in-depth inspection of any ensemble of opportunity in order to extract the maximum amount of information and to have full control over the data used in the construction of the ensemble.


2020 ◽  
Vol 20 (21) ◽  
pp. 13455-13466
Author(s):  
Zhihao Shi ◽  
Lin Huang ◽  
Jingyi Li ◽  
Qi Ying ◽  
Hongliang Zhang ◽  
...  

Abstract. Meteorological conditions play important roles in the formation of ozone (O3) and fine particulate matter (PM2.5). China has been suffering from serious regional air pollution problems, characterized by high concentrations of surface O3 and PM2.5. In this study, the Community Multiscale Air Quality (CMAQ) model was used to quantify the sensitivity of surface O3 and PM2.5 to key meteorological parameters in different regions of China. Six meteorological parameters were perturbed to create different meteorological conditions, including temperature (T), wind speed (WS), absolute humidity (AH), planetary boundary layer height (PBLH), cloud liquid water content (CLW) and precipitation (PCP). Air quality simulations under the perturbed meteorological conditions were conducted in China in January and July of 2013. The changes in O3 and PM2.5 concentrations due to individual meteorological parameters were then quantified. T has a great influence on the daily maximum 8 h average O3 (O3-8 h) concentrations, which leads to O3-8 h increases by 1.7 in January in Chongqing and 1.1 ppb K−1 in July in Beijing. WS, AH, and PBLH have a smaller but notable influence on O3-8 h with maximum change rates of 0.3 ppb %−1, −0.15 ppb %−1, and 0.14 ppb %−1, respectively. T, WS, AH, and PBLH have important effects on PM2.5 formation of both in January and July. In general, PM2.5 sensitivities are negative to T, WS, and PBLH and positive to AH in most regions of China. The sensitivities in January are much larger than in July. PM2.5 sensitivity to T, WS, PBLH, and AH in January can be up to −5 µg m−3 K−1, −3 µg m−3 %−1, −1 µg m−3 %−1, and +0.6 µg m−3 %−1, respectively, and in July it can be up to −2 µg m−3 K−1, −0.4 µg m−3 %−1, −0.14 µg m−3 %−1, and +0.3 µg m−3 %−1, respectively. Other meteorological factors (CLW and PCP) have negligible effects on O3-8 h (less than 0.01 ppb %−1) and PM2.5 (less than 0.01 µg m−3 %−1). The results suggest that surface O3 and PM2.5 concentrations can change significantly due to changes in meteorological parameters, and it is necessary to consider these effects when developing emission control strategies in different regions of China.


2015 ◽  
Vol 15 (19) ◽  
pp. 10965-10982 ◽  
Author(s):  
T. P. Canty ◽  
L. Hembeck ◽  
T. P. Vinciguerra ◽  
D. C. Anderson ◽  
D. L. Goldberg ◽  
...  

Abstract. Regulatory air quality models, such as the Community Multiscale Air Quality model (CMAQ), are used by federal and state agencies to guide policy decisions that determine how to best achieve adherence with National Ambient Air Quality Standards for surface ozone. We use observations of ozone and its important precursor NO2 to test the representation of the photochemistry and emission of ozone precursors within CMAQ. Observations of tropospheric column NO2 from the Ozone Monitoring Instrument (OMI), retrieved by two independent groups, show that the model overestimates urban NO2 and underestimates rural NO2 under all conditions examined for July and August 2011 in the US Northeast. The overestimate of the urban to rural ratio of tropospheric column NO2 for this baseline run of CMAQ (CB05 mechanism, mobile NOx emissions from the National Emissions Inventory; isoprene emissions from MEGAN v2.04) suggests this model may underestimate the importance of interstate transport of NOx. This CMAQ simulation leads to a considerable overestimate of the 2-month average of 8 h daily maximum surface ozone in the US Northeast, as well as an overestimate of 8 h ozone at AQS sites during days when the state of Maryland experienced NAAQS exceedances. We have implemented three changes within CMAQ motivated by OMI NO2 as well as aircraft observations obtained in July 2011 during the NASA DISCOVER-AQ campaign: (a) the modeled lifetime of organic nitrates within CB05 has been reduced by a factor of 10, (b) emissions of NOx from mobile sources has been reduced by a factor of 2, and (c) isoprene emissions have been reduced by using MEGAN v2.10 rather than v2.04. Compared to the baseline simulation, the CMAQ run using all three of these changes leads to considerably better simulation of column NO2 in both urban and rural areas, better agreement with the 2-month average of daily 8 h maximum ozone in the US Northeast, fewer number of false positives of an ozone exceedance throughout the domain, as well as an unbiased simulation of surface ozone at ground-based AQS sites in Maryland that experienced an ozone exceedance during July and August 2007. These modifications to CMAQ may provide a framework for use in studies focused on achieving future adherence to specific air quality standards for surface ozone by reducing emission of NOx from various anthropogenic sectors.


2010 ◽  
Vol 10 (22) ◽  
pp. 11305-11322 ◽  
Author(s):  
T. Nagashima ◽  
T. Ohara ◽  
K. Sudo ◽  
H. Akimoto

Abstract. We estimated the source-receptor relationship for surface O3 in East Asia during the early 2000s using a method that tags O3 tracers according to their region of chemical production (tagged tracer method) with a global chemical transport model. The estimation demonstrated the importance of intracontinental transport of O3 inside East Asia as well as of the transport of O3 from distant source regions. The model well simulated the absolute concentration and seasonal variation of surface O3 in East Asia and demonstrated significant seasonal differences in the origin of surface O3. In the cold season (October to March), more than half of surface O3 in East Asia is attributable to the O3 transported from distant sources outside of East Asia. In the warm season (April to September), most of the surface O3 is attributable to O3 created within East Asia in most areas of East Asia. In spring the contribution of domestically created O3 accounted for 20% of the surface O3 in Japan and the Korean Peninsula, 40% in the North China Plain, and around 50% in the southern part of China, and the domestic contribution increased greatly in summer. The contributions of O3 created in China and the Korean Peninsula to O3 in Japan were estimated at about 10% and 5%, respectively. We also demonstrated a large contribution (20%) from China to the Korean Peninsula. In the northern and southern parts of China, large contributions of over 10% from East Siberia and the Indochina Peninsula, respectively, were identified. The contribution from intercontinental transport increased with latitude; it was 21% in Northeast China and 13% in Japan and the Korean Peninsula in spring. As for the hourly mean of surface O3, domestically created O3 was the main contributor in most areas of East Asia, except for the low O3 class (<30 ppbv), and accounted for more than 50% in the very high O3 class (>90 ppbv). The mean relative contribution of O3 created in China to O3 in central Japan was about 10% in every class, but that created in the Korean Peninsula was significant in all except the low O3 class. We identified the substantial impact of foreign sources on Japan's ambient air quality standard in the high O3 class (60–90 ppbv) in spring.


2020 ◽  
Vol 20 (6) ◽  
pp. 3739-3776 ◽  
Author(s):  
Rebecca H. Schwantes ◽  
Louisa K. Emmons ◽  
John J. Orlando ◽  
Mary C. Barth ◽  
Geoffrey S. Tyndall ◽  
...  

Abstract. Ozone is a greenhouse gas and air pollutant that is harmful to human health and plants. During the summer in the southeastern US, many regional and global models are biased high for surface ozone compared to observations. Past studies have suggested different solutions including the need for updates to model representation of clouds, chemistry, ozone deposition, and emissions of nitrogen oxides (NOx) or biogenic hydrocarbons. Here, due to the high biogenic emissions in the southeastern US, more comprehensive and updated isoprene and terpene chemistry is added into CESM/CAM-chem (Community Earth System Model/Community Atmosphere Model with full chemistry) to evaluate the impact of chemistry on simulated ozone. Comparisons of the model results with data collected during the Studies of Emissions Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS) field campaign and from the US EPA (Environmental Protection Agency) CASTNET (Clean Air Status and Trends Network) monitoring stations confirm the updated chemistry improves simulated surface ozone, ozone precursors, and NOx reservoir compounds. The isoprene and terpene chemistry updates reduce the bias in the daily maximum 8 h average (MDA8) surface ozone by up to 7 ppb. In the past, terpene oxidation in particular has been ignored or heavily reduced in chemical schemes used in many regional and global models, and this study demonstrates that comprehensive isoprene and terpene chemistry is needed to reduce surface ozone model biases. Sensitivity tests were performed in order to evaluate the impact of lingering uncertainties in isoprene and terpene oxidation on ozone. Results suggest that even though isoprene emissions are higher than terpene emissions in the southeastern US, remaining uncertainties in isoprene and terpene oxidation have similar impacts on ozone due to lower uncertainties in isoprene oxidation. Additionally, this study identifies the need for further constraints on the aerosol uptake of organic nitrates derived from isoprene and terpenes in order to reduce uncertainty in simulated ozone. Although the updates to isoprene and terpene chemistry greatly reduce the ozone bias in CAM-chem, a large bias remains. Evaluation against SEAC4RS field campaign results suggests future improvements to horizontal resolution and cloud parameterizations in CAM-chem may be particularly important for further reducing this bias.


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