scholarly journals Multi-scale model analysis of boundary layer ozone over East Asia

2009 ◽  
Vol 9 (10) ◽  
pp. 3277-3301 ◽  
Author(s):  
M. Lin ◽  
T. Holloway ◽  
T. Oki ◽  
D. G. Streets ◽  
A. Richter

Abstract. This study employs the regional Community Multiscale Air Quality (CMAQ) model to examine seasonal and diurnal variations of boundary layer ozone (O3) over East Asia. We evaluate the response of model simulations of boundary layer O3 to the choice of chemical mechanisms, meteorological fields, boundary conditions, and model resolutions. Data obtained from surface stations, aircraft measurements, and satellites are used to advance understanding of O3 chemistry and mechanisms over East Asia and evaluate how well the model represents the observed features. Satellite measurements and model simulations of summertime rainfall are used to assess the impact of the Asian monsoon on O3 production. Our results suggest that summertime O3 over Central Eastern China is highly sensitive to cloud cover and monsoonal rainfall over this region. Thus, accurate simulation of the East Asia summer monsoon is critical to model analysis of atmospheric chemistry over China. Examination of hourly summertime O3 mixing ratios from sites in Japan confirms the important role of diurnal boundary layer fluctuations in controlling ground-level O3. By comparing five different model configurations with observations at six sites, the specific mechanisms responsible for model behavior are identified and discussed. In particular, vertical mixing, urban chemistry, and dry deposition depending on boundary layer height strongly affect model ability to capture observed behavior. Central Eastern China appears to be the most sensitive region in our study to the choice of chemical mechanisms. Evaluation with TRACE-P aircraft measurements reveals that neither the CB4 nor the SAPRC99 mechanisms consistently capture observed behavior of key photochemical oxidants in springtime. However, our analysis finds that SAPRC99 performs somewhat better in simulating mixing ratios of H2O2 (hydrogen peroxide) and PAN (peroxyacetyl nitrate) at flight altitudes below 1 km. The high level of uncertainty associated with O3 production in Central Eastern China poses a major problem for regional air quality management. This highly polluted, densely populated region would greatly benefit from comprehensive air quality monitoring and the development of model chemical mechanisms appropriate to this unique atmospheric environment.

2018 ◽  
Vol 57 (12) ◽  
pp. 2789-2816 ◽  
Author(s):  
Richard T. McNider ◽  
Arastoo Pour-Biazar ◽  
Kevin Doty ◽  
Andrew White ◽  
Yuling Wu ◽  
...  

AbstractHigh mixing ratios of ozone along the shores of Lake Michigan have been a recurring theme over the last 40 years. Models continue to have difficulty in replicating ozone behavior in the region. Although emissions and chemistry may play a role in model performance, the complex meteorological setting of the relatively cold lake in the summer ozone season and the ability of the physical model to replicate this environment may contribute to air quality modeling errors. In this paper, several aspects of the physical atmosphere that may affect air quality, along with potential paths to improve the physical simulations, are broadly examined. The first topic is the consistent overwater overprediction of ozone. Although overwater measurements are scarce, special boat and ferry ozone measurements over the last 15 years have indicated consistent overprediction by models. The roles of model mixing and lake surface temperatures are examined in terms of changing stability over the lake. From an analysis of a 2009 case, it is tentatively concluded that excessive mixing in the meteorological model may lead to an underestimate of mixing in offline chemical models when different boundary layer mixing schemes are used. This is because the stable boundary layer shear, which is removed by mixing in the meteorological model, can no longer produce mixing when mixing is rediagnosed in the offline chemistry model. Second, air temperature has an important role in directly affecting chemistry and emissions. Land–water temperature contrasts are critical to lake and land breezes, which have an impact on mixing and transport. Here, satellite-derived skin temperatures are employed as a path to improve model temperature performance. It is concluded that land surface schemes that adjust moisture based on surface energetics are important in reducing temperature errors.


2008 ◽  
Vol 8 (24) ◽  
pp. 7543-7555 ◽  
Author(s):  
Y. J. He ◽  
I. Uno ◽  
Z. F. Wang ◽  
P. Pochanart ◽  
J. Li ◽  
...  

Abstract. The impact of the East Asia monsoon on the seasonal behavior of O3 in the boundary layer of Eastern China and the west Pacific region was analyzed for 2004–2006 by means of full-year nested chemical transport model simulations and continuous observational data obtained from three inland mountain sites in central and eastern China and three oceanic sites in the west Pacific region. The basic common features of O3 seasonal behaviors over all the monitoring sites are the pre- and post-monsoon peaks with a summer trough. Such bimodal seasonal patterns of O3 are predominant over the region with strong summer monsoon penetration, and become weaker or even disappear outside the monsoon region. The seasonal/geographical distribution of the pre-defined monsoon index indicated that the East Asia summer monsoon is responsible for the bimodal seasonal O3 pattern, and also partly account for the differences in the O3 seasonal variations between the inland mountain and oceanic sites. Over the inland mountain sites, the O3 concentration increased gradually from the beginning of the year, reached a maximum in June, decreased rapidly to the summer valley in July or August, and then peaked in September or October, thereafter decreased gradually again. Over the oceanic sites, O3 abundance showed a similar increasing trend beginning in January, but then decreased gradually from the end of March, followed by a wide trough with the minimum in July and August and a small peak in October or November. A sensitivity analysis performed by setting China-emission to zero revealed that the chemically produced O3 from China-emission contributed substantially to the O3 abundance, particularly the pre- and post-monsoon O3 peaks, over China mainland. We found that China-emission contributed more than 40% to total boundary layer O3 during summertime (60–70% in July) and accounted for about 40 ppb of each peak value over the inland region if without considering the effect of the nonlinear chemical productions. In contrast, over the oceanic region in the high monsoon index zone, the contribution of China-emission to total boundary layer O3 was always less than 20% (<10 ppb), and less than 10% in summer.


2007 ◽  
Vol 7 (5) ◽  
pp. 1451-1469 ◽  
Author(s):  
S. Morin ◽  
J. Savarino ◽  
S. Bekki ◽  
S. Gong ◽  
J. W. Bottenheim

Abstract. We report the first measurements of the oxygen isotope anomaly of atmospheric inorganic nitrate from the Arctic. Nitrate samples and complementary data were collected at Alert, Nunavut, Canada (82°30 ' N, 62°19 ' W) in spring 2004. Covering the polar sunrise period, characterized by the occurrence of severe boundary layer ozone depletion events (ODEs), our data show a significant correlation between the variations of atmospheric ozone (O3) mixing ratios and Δ17O of nitrate (Δ17O(NO−3)). This relationship can be expressed as: Δ17O(NO−3)/‰, =(0.15±0.03)×O3/(nmol mol–1)+(29.7±0.7), with R2=0.70(n=12), for Δ17O(NO−3) ranging between 29 and 35 ‰. We derive mass-balance equations from chemical reactions operating in the Arctic boundary layer, that describe the evolution of Δ17O(NO−3) as a function of the concentrations of reactive species and their isotopic characteristics. Changes in the relative importance of O3, RO2 and BrO in the oxidation of NO during ODEs, and the large isotope anomalies of O3 and BrO, are the driving force for the variability in the measured Δ17O(NO−3) . BrONO2 hydrolysis is found to be a dominant source of nitrate in the Arctic boundary layer, in agreement with recent modeling studies.


2021 ◽  
Author(s):  
Drew C. Pendergrass ◽  
Daniel J. Jacob ◽  
Shixian Zhai ◽  
Jhoon Kim ◽  
Ja-Ho Koo ◽  
...  

Abstract. We use 2011–2019 aerosol optical depth (AOD) observations from the Geostationary Ocean Color Imager (GOCI) instrument over East Asia to infer 24-h daily surface fine particulate matter (PM2.5) concentrations at continuous 6x6 km2 resolution over eastern China, South Korea, and Japan. This is done with a random forest (RF) algorithm applied to the gap-filled GOCI AODs and other data and trained with PM2.5 observations from the three national networks. The predicted 24-h PM2.5 concentrations for sites entirely withheld from training in a ten-fold crossvalidation procedure correlate highly with network observations (R2 = 0.89) with single-value precision of 26–32 % depending on country. Prediction of annual mean values has R2 = 0.96 and single-value precision of 12 %. The RF algorithm is only moderately successful for diagnosing local exceedances of the National Ambient Air Quality Standard (NAAQS) because these exceedances are typically within the single-value precisions of the RF, and also because of RF smoothing of extreme PM2.5 concentrations. The area-weighted and population-weighted trends of RF PM2.5 concentrations for eastern China, South Korea, and Japan show steady 2015–2019 declines consistent with surface networks, but the surface networks in eastern China and South Korea underestimate population exposure. Further examination of RF PM2.5 fields for South Korea identifies hotspots where surface network sites were initially lacking and shows 2015–2019 PM2.5 decreases across the country except for flat concentrations in the Seoul metropolitan area. Inspection of monthly PM2.5 time series in Beijing, Seoul, and Tokyo shows that the RF algorithm successfully captures observed seasonal variations of PM2.5 even though AOD and PM2.5 often have opposite seasonalities. Application of the RF algorithm to urban pollution episodes in Seoul and Beijing demonstrates high skill in reproducing the observed day-to-day variations in air quality as well as spatial patterns on the 6 km scale. Comparison to a CMAQ simulation for the Korean peninsula demonstrates the value of the continuous RF PM2.5 fields for testing air quality models, including over North Korea where they offer a unique resource.


Author(s):  
K. L. Chan ◽  
K. Qin

In this study, we present a quantitative estimation of the impacts of biomass burning emissions from different source regions to the local air quality in Hong Kong in 2014 using global chemistry transport model simulations, sun photometer measurements, satellite observations and local monitoring network data. This study focuses on two major biomass burning pollutants, black carbon aerosols and carbon monoxide (CO). The model simulations of atmospheric black carbon and CO show excellent agreement with sun photometer aerosol optical depth (AOD) measurements, satellite CO columns observations and local monitoring stations data. From the model simulation results, we estimated that biomass burning contributes 12&amp;thinsp;% of total black carbon and 16&amp;thinsp;% of atmospheric CO in Hong Kong on annual average. South East Asia shows the largest influence to the black carbon and CO levels in Hong Kong, accounts for 11&amp;thinsp;% of the total atmospheric black carbon and 8&amp;thinsp;% of CO. Biomass burning in North East Asia and Africa also show significant impacts to Hong Kong. Elevated levels of atmospheric black carbon aerosols and CO were observed during springtime (March and April) which is mainly due to the enhancement of biomass burning contributions. Black carbon and CO originating from biomass burning sources are estimated to contribute 40&amp;thinsp;% of atmospheric black carbon and 28&amp;thinsp;% of CO in Hong Kong during March 2014. An investigation focusing on the biomass burning pollution episode during springtime suggests the intensified biomass burning activities in the Indochinese Peninsula are the major sources of black carbon and CO in Hong Kong during the time.


2021 ◽  
Author(s):  
Haiyue Tan ◽  
Lin Zhang ◽  
Xiao Lu ◽  
Yuanhong Zhao ◽  
Bo Yao ◽  
...  

Abstract. China, being one of the major emitters of greenhouse gases, has taken strong actions to tackle climate change, e.g., to achieve carbon neutrality by 2060. It also becomes important to better understand the changes in the atmospheric mixing ratio and emissions of CH4, the second most important human-influenced greenhouse gas, in China. Here we analyze the sources contributing to the atmospheric CH4 mixing ratio and their trends in China over 2007–2018 using the GEOS-Chem model simulations driven by two commonly used global anthropogenic emission inventories: the Emissions Database for Global Atmospheric Research (EDGAR v4.3.2) and the Community Emissions Data System (CEDS). The model results are interpreted with an ensemble of surface, aircraft, and satellite observations of CH4 mixing ratios over China and the Pacific region. The EDGAR and CEDS estimates show considerable differences reflecting large uncertainties in estimates of Chinese CH4 emissions. Chinese CH4 emission estimates based on EDGAR and natural sources increase from 46.7 Tg per annum (Tg a−1) in 1980 to 69.8 Tg a−1 in 2012 with an increase rate of 0.7 Tg a−2, and estimates with CEDS increase from 32.9 Tg a−1 in 1980 and 76.7 Tg a−1 in 2014 (a much stronger trend of 1.3 Tg a−2 over the period). Both surface, aircraft, and satellite measurements indicate CH4 increase rates of 7.0–8.4 ppbv a−1 over China in the recent decade. We find that the model simulation using the CEDS inventory and interannually varying OH levels can best reproduce these observed CH4 mixing ratios and trends over China. Model results over China are sensitive to the global OH level, with a 10 % increase in the global tropospheric volume-weighted mean OH concentration presenting a similar effect to that of a 47 Tg a−1 decrease in global CH4 emissions. We further apply a tagged tracer simulation to quantify the source contributions from different emission sectors and regions. We find that domestic CH4 emissions account for 11.4 % of the mean surface mixing ratio and drive 68.3 % of the surface trend (mainly via the energy sector) in China over 2007–2018. We emphasize that intensive CH4 measurements covering eastern China will help better assess the driving factors of CH4 mixing ratios and support the emission mitigation in China.


2020 ◽  
Vol 20 (10) ◽  
pp. 5899-5909 ◽  
Author(s):  
Yucong Miao ◽  
Huizheng Che ◽  
Xiaoye Zhang ◽  
Shuhua Liu

Abstract. Rapid urbanization and industrialization have led to deterioration of air quality in the Beijing–Tianjin–Hebei (BTH) region due to high loadings of PM2.5. Heavy aerosol pollution frequently occurs in winter, in close relation to the planetary boundary layer (PBL) meteorology. To unravel the physical processes that influence PBL structure and aerosol pollution in BTH, this study combined long-term observational data analyses, synoptic pattern classification, and meteorology–chemistry coupled simulations. During the winter of 2017 and 2018, Beijing and Tangshan often experienced heavy PM2.5 pollution simultaneously, accompanied by strong thermal inversion aloft. These concurrences of pollution in different cities were primarily regulated by the large-scale synoptic conditions. Using principal component analysis with geopotential height fields at the 850 hPa level during winter, two typical synoptic patterns associated with heavy pollution in BTH were identified. One pattern is characterized by a southeast-to-north pressure gradient across BTH, and the other is associated with high pressure in eastern China. Both synoptic types feature warmer air temperature at 1000 m a.g.l., which could suppress the development of the PBL. Under these unfavorable synoptic conditions, aerosols can modulate PBL structure through the radiative effect, which was examined using numerical simulations. The aerosol radiative effect can significantly lower the daytime boundary layer height through cooling the surface layer and heating the upper part of the PBL, leading to the deterioration of air quality. This PBL–aerosol feedback is sensitive to the aerosol vertical structure, which is more effective when the synoptic pattern can distribute more aerosols to the upper PBL.


2010 ◽  
Vol 3 (1) ◽  
pp. 169-188 ◽  
Author(s):  
K. W. Appel ◽  
S. J. Roselle ◽  
R. C. Gilliam ◽  
J. E. Pleim

Abstract. This paper presents a comparison of the operational performances of two Community Multiscale Air Quality (CMAQ) model v4.7 simulations that utilize input data from the 5th-generation Mesoscale Model (MM5) and the Weather Research and Forecasting (WRF) meteorological models. Two sets of CMAQ model simulations were performed for January and August 2006. One set utilized MM5 meteorology (MM5-CMAQ) and the other utilized WRF meteorology (WRF-CMAQ), while all other model inputs and options were kept the same. For January, predicted ozone (O3) mixing ratios were higher in the Southeast and lower Mid-west regions in the WRF-CMAQ simulation, resulting in slightly higher bias and error as compared to the MM5-CMAQ simulations. The higher predicted O3 mixing ratios are attributed to less dry deposition of O3 in the WRF-CMAQ simulation due to differences in the calculation of the vegetation fraction between the MM5 and WRF models. The WRF-CMAQ results showed better performance for particulate sulfate (SO42−), similar performance for nitrate (NO3−), and slightly worse performance for nitric acid (HNO3), total carbon (TC) and total fine particulate (PM2.5) mass than the corresponding MM5-CMAQ results. For August, predictions of O3 were notably higher in the WRF-CMAQ simulation, particularly in the southern United States, resulting in increased model bias. Concentrations of predicted particulate SO42− were lower in the region surrounding the Ohio Valley and higher along the Gulf of Mexico in the WRF-CMAQ simulation, contributing to poorer model performance. The primary causes of the differences in the MM5-CMAQ and WRF-CMAQ simulations appear to be due to differences in the calculation of wind speed, planetary boundary layer height, cloud cover and the friction velocity (u∗) in the MM5 and WRF model simulations, while differences in the calculation of vegetation fraction and several other parameters result in smaller differences in the predicted CMAQ model concentrations. The performance for SO42−, NO3− and NH4+ wet deposition was similar for both simulations for January and August.


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